TY - JOUR A1 - Robrade, Jan A1 - Oskinova, Lidia M. A1 - Schmitt, J. H. M. M. A1 - Leto, Paolo A1 - Trigilio, C. T1 - Outstanding X-ray emission from the stellar radio pulsar CU Virginis JF - Astronomy and astrophysics : an international weekly journal N2 - Context. Among the intermediate-mass magnetic chemically peculiar (MCP) stars, CU Vir is one of the most intriguing objects. Its 100% circularly polarized beams of radio emission sweep the Earth as the star rotates, thereby making this strongly magnetic star the prototype of a class of nondegenerate stellar radio pulsars. While CU Vir is well studied in radio, its high-energy properties are not known. Yet, X-ray emission is expected from stellar magnetospheres and confined stellar winds. Aims. Using X-ray data we aim to test CU Vir for intrinsic X-ray emission and investigate mechanisms responsible for its generation. Methods. We present X-ray observations performed with XMM-Newton and Chandra and study obtained X-ray images, light curves, and spectra. Basic X-ray properties are derived from spectral modelling and are compared with model predictions. In this context we investigate potential thermal and nonthermal X-ray emission scenarios. Results. We detect an X-ray source at the position of CU Vir. With LX approximate to 3 x 10(28) erg s(-1) it is moderately X-ray bright, but the spectrum is extremely hard compared to other Ap stars. Spectral modelling requires multi-component models with predominant hot plasma at temperatures of about T-X = 25MK or, alternatively, a nonthermal spectral component. Both types of model provide a virtually equivalent description of the X-ray spectra. The Chandra observation was performed six years later than those by XMM-Newton, yet the source has similar X-ray flux and spectrum, suggesting a steady and persistent X-ray emission. This is further confirmed by the X-ray light curves that show only mild X-ray variability. Conclusions. CU Vir is also an exceptional star at X-ray energies. To explain its full X-ray properties, a generating mechanism beyond standard explanations, like the presence of a low-mass companion or magnetically confined wind-shocks, is required. Magnetospheric activity might be present or, as proposed for fast-rotating strongly magnetic Bp stars, the X-ray emission of CU Vir is predominantly auroral in nature. KW - individual: CU Vir KW - stars: activity KW - stars: chemically peculiar KW - stars: magnetic field KW - X-rays: stars Y1 - 2018 U6 - https://doi.org/10.1051/0004-6361/201833492 SN - 1432-0746 VL - 619 PB - EDP Sciences CY - Les Ulis ER - TY - JOUR A1 - Leto, Paolo A1 - Trigilio, C. A1 - Oskinova, Lidia M. A1 - Ignace, R. A1 - Buemi, C. S. A1 - Umana, G. A1 - Ingallinera, A. A1 - Leone, Francesco A1 - Phillips, N. M. A1 - Agliozzo, Claudia A1 - Todt, Helge Tobias A1 - Cerrigone, L. T1 - A combined multiwavelength VLA/ALMA/Chandra study unveils the complex magnetosphere of the B-type star HR5907 JF - Monthly notices of the Royal Astronomical Society N2 - We present new radio/millimeter measurements of the hot magnetic star HR5907 obtained with the VLA and ALMA interferometers. We find that HR5907 is the most radio luminous early type star in the cm-mm band among those presently known. Its multi-wavelength radio light curves are strongly variable with an amplitude that increases with radio frequency. The radio emission can be explained by the populations of the non-thermal electrons accelerated in the current sheets on the outer border of the magnetosphere of this fast-rotating magnetic star. We classify HR5907 as another member of the growing class of strongly magnetic fast-rotating hot stars where the gyro-synchrotron emission mechanism efficiently operates in their magnetospheres. The new radio observations of HR5907 are combined with archival X-ray data to study the physical condition of its magnetosphere. The X-ray spectra of HR5907 show tentative evidence for the presence of non-thermal spectral component. We suggest that non-thermal X-rays originate a stellar X-ray aurora due to streams of non-thermal electrons impacting on the stellar surface. Taking advantage of the relation between the spectral indices of the X-ray power-law spectrum and the non-thermal electron energy distributions, we perform 3-D modelling of the radio emission for HR5907. The wavelength-dependent radio light curves probe magnetospheric layers at different heights above the stellar surface. A detailed comparison between simulated and observed radio light curves leads us to conclude that the stellar magnetic field of HR 5907 is likely non-dipolar, providing further indirect evidence of the complex magnetic field topology of HR5907. KW - stars: chemically peculiar KW - stars: early-type KW - stars: individual: HR 5907 KW - stars: magnetic field KW - radio continuum: stars KW - X-rays: stars Y1 - 2018 U6 - https://doi.org/10.1093/mnras/sty244 SN - 0035-8711 SN - 1365-2966 VL - 476 IS - 1 SP - 562 EP - 579 PB - Oxford Univ. Press CY - Oxford ER - TY - JOUR A1 - Oskinova, Lidia M. A1 - Bulik, Tomasz A1 - Gomez-Moran, Ada Nebot T1 - Infrared outbursts as potential tracers of common-envelope events in high-mass X-ray binary formation JF - Astronomy and astrophysics : an international weekly journal N2 - Context. Classic massive binary evolutionary scenarios predict that a transitional common-envelope (CE) phase could be preceded as well as succeeded by the evolutionary stage when a binary consists of a compact object and a massive star, that is, a high-mass X-ray binary (HMXB). The observational manifestations of common envelope are poorly constrained. We speculate that its ejection might be observed in some cases as a transient event at mid-infrared (IR) wavelengths. Aims. We estimate the expected numbers of CE ejection events and HMXBs per star formation unit rate, and compare these theoretical estimates with observations. Methods. We compiled a list of 85 mid-IR transients of uncertain nature detected by the Spitzer Infrared Intensive Transients Survey and searched for their associations with X-ray, optical, and UV sources. Results. Confirming our theoretical estimates, we find that only one potential HMXB may be plausibly associated with an IR-transient and tentatively propose that X-ray source NGC4490-X40 could be a precursor to the SPIRITS 16az event. Among other interesting sources, we suggest that the supernova remnant candidate [BWL2012] 063 might be associated with SPIRITS 16ajc. We also find that two SPIRITS events are likely associated with novae, and seven have potential optical counterparts. Conclusions. The massive binary evolutionary scenarios that involve CE events do not contradict currently available observations of IR transients and HMXBs in star-forming galaxies. KW - X-rays: binaries KW - stars: massive KW - infrared: general KW - infrared: galaxies Y1 - 2018 U6 - https://doi.org/10.1051/0004-6361/201832925 SN - 0004-6361 SN - 1432-0746 VL - 613 PB - EDP Sciences CY - Les Ulis ER - TY - JOUR A1 - González-Galán, Ana A1 - Oskinova, Lidia M. A1 - Popov, Sergei B. A1 - Haberl, F. A1 - Kühnel, M. A1 - Gallagher, John S. A1 - Schurch, Matthew A1 - Guerrero, Martín A. T1 - A multiwavelength study of SXP 1062, the long-period X-ray pulsar associated with a supernova remnant JF - Monthly notices of the Royal Astronomical Society N2 - SXP 1062 is a Be X-ray binary (BeXB) located in the Small Magellanic Cloud. It hosts a long-period X-ray pulsar and is likely associated with the supernova remnant MCSNR J0127−7332. In this work we present a multiwavelength view on SXP 1062 in different luminosity regimes. We consider monitoring campaigns in optical (OGLE survey) and X-ray (Swift telescope). During these campaigns a tight coincidence of X-ray and optical outbursts is observed. We interpret this as typical Type I outbursts as often detected in BeXBs at periastron passage of the neutron star (NS). To study different X-ray luminosity regimes in depth, during the source quiescence we observed it with XMM–Newton while Chandra observations followed an X-ray outburst. Nearly simultaneously with Chandra observations in X-rays, in optical the RSS/SALT telescope obtained spectra of SXP 1062. On the basis of our multiwavelength campaign we propose a simple scenario where the disc of the Be star is observed face-on, while the orbit of the NS is inclined with respect to the disc. According to the model of quasi-spherical settling accretion our estimation of the magnetic field of the pulsar in SXP 1062 does not require an extremely strong magnetic field at the present time. KW - stars: neutron KW - pulsars: individual: SXP 1062 KW - galaxies: individual: Small Magellanic Cloud KW - X-rays: binaries Y1 - 2017 U6 - https://doi.org/10.1093/mnras/stx3127 SN - 0035-8711 SN - 1365-2966 VL - 475 IS - 2 SP - 2809 EP - 2821 PB - Oxford University Press CY - Oxford ER - TY - JOUR A1 - Martinez-Chicharro, M. A1 - Torrejon, J. M. A1 - Oskinova, Lidia M. A1 - Furst, F. A1 - Postnov, K. A1 - Rodes-Roca, J. J. A1 - Hainich, Rainer A1 - Bodaghee, A. T1 - Evidence of Compton cooling during an X-ray flare supports a neutron star nature of the compact object in 4U1700-37 JF - Monthly notices of the Royal Astronomical Society N2 - Based on new Chandra X-ray telescope data, we present empirical evidence of plasma Compton cooling during a flare in the non-pulsating massive X-ray binary 4U1700-37. This behaviour might be explained by quasi-spherical accretion on to a slowly rotating magnetized neutron star (NS). In quiescence, the NS in 4U1700-37 is surrounded by a hot radiatively cooling shell. Its presence is supported by the detection of mHz quasi-periodic oscillations likely produced by its convection cells. The high plasma temperature and the relatively low X-ray luminosity observed during the quiescence, point to a small emitting area similar to 1 km, compatible with a hotspot on an NS surface. The sudden transition from a radiative to a significantly more efficient Compton cooling regime triggers an episode of enhanced accretion resulting in a flare. During the flare, the plasma temperature drops quickly. The predicted luminosity for such transitions, similar to 3 x 10(35) erg s(-1), is very close to the luminosity of 4U1700-37 during quiescence. The transition may be caused by the accretion of a clump in the stellar wind of the donor star. Thus, a magnetized NS nature of the compact object is strongly favoured. KW - stars: individual: 4U1700-37 KW - V*V884 Sco KW - X-rays: binaries Y1 - 2017 U6 - https://doi.org/10.1093/mnrasl/slx165 SN - 0035-8711 SN - 1365-2966 VL - 473 IS - 1 SP - L74 EP - L78 PB - Oxford Univ. Press CY - Oxford ER - TY - JOUR A1 - Torrejon, J. M. A1 - Reig, Pablo A1 - Fürst, F. A1 - Martinez-Chicharro, M. A1 - Postnov, K. A1 - Oskinova, Lidia M. T1 - NuSTAR rules out a cyclotron line in the accreting magnetar candidate 4U2206+54 JF - Monthly notices of the Royal Astronomical Society N2 - Based on our new NuSTAR X-ray telescope data, we rule out any cyclotron line up to 60 keV in the spectra of the high-mass X-ray binary 4U2206+54. In particular, we do not find any evidence of the previously claimed line around 30 keV, independently of the source flux, along the spin pulse. The spin period has increased significantly, since the last observation, up to 5750 +/- 10 s, confirming the rapid spin-down rate (nu)over dot = -1.8 x 10(-14) Hz s(-1). This behaviour might be explained by the presence of a strongly magnetized neutron star (B-s > several times 10(13) G) accreting from the slow wind of its main-sequence O9.5 companion. KW - Stars: individual: 4U2206+54, BD+53 2790 KW - X-rays: binaries Y1 - 2018 U6 - https://doi.org/10.1093/mnras/sty1628 SN - 0035-8711 SN - 1365-2966 VL - 479 IS - 3 SP - 3366 EP - 3372 PB - Oxford Univ. Press CY - Oxford ER - TY - JOUR A1 - Massa, Derck A1 - Oskinova, Lidia M. A1 - Prinja, Raman A1 - Ignace, Richard T1 - Coordinated UV and X-Ray Spectroscopic Observations of the O-type Giant xi Per BT - the Connection between X-Rays and Large-scale Wind Structure JF - The astrophysical journal : an international review of spectroscopy and astronomical physics N2 - We present new, contemporaneous Hubble Space Telescope STIS and XMM-Newton observations of the O7. III(n) ((f)) star xi Per. We supplement the new data with archival IUE spectra, to analyze the variability of the wind lines and X-ray flux of xi Per. The variable wind of this star is known to have a 2.086-day periodicity. We use a simple, heuristic spot model that fits the low-velocity (near-surface) IUE wind line variability very well, to demonstrate that the low-velocity absorption in the new STIS spectra of N IV lambda 1718 and Si IV lambda 1402 vary with the same 2.086-day period. It is remarkable that the period and amplitude of the STIS data agree with those of the IUE spectra obtained 22 yr earlier. We also show that the time variability of the new XMM-Newton fluxes is also consistent with the 2.086-day period. Thus, our new, multiwavelength coordinated observations demonstrate that the mechanism that causes the UV wind line variability is also responsible for a significant fraction of the X-rays in single O stars. The sequence of events for the multiwavelength light-curve minima is Si IV lambda 1402, N IV lambda 1718, and X-ray flux, each separated by a phase of about 0.06 relative to the 2.086-day period. Analysis of the X-ray fluxes shows that they become softer as they weaken. This is contrary to expectations if the variability is caused by periodic excess absorption. Furthermore, the high-resolution X-ray spectra suggest that the individual emission lines at maximum are more strongly blueshifted. If we interpret the low-velocity wind line light curves in terms of our model, it implies that there are two bright regions, i.e., regions with less absorption, separated by 180 degrees, on the surface of the star. We note that the presence and persistence of two spots separated by 180 degrees suggest that a weak dipole magnetic field is responsible for the variability of the UV wind line absorption and X-ray flux in xi Per. KW - stars: activity KW - stars: early-type KW - stars: winds, outflows KW - ultraviolet: stars KW - X-rays: stars Y1 - 2019 U6 - https://doi.org/10.3847/1538-4357/ab0283 SN - 0004-637X SN - 1538-4357 VL - 873 IS - 1 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Oskinova, Lidia M. A1 - Feldmeier, Achim A1 - Hamann, Wolf-Rainer T1 - High-resolution X-ray spectroscopy of bright O-type stars JF - Monthly notices of the Royal Astronomical Society N2 - Archival X-ray spectra of the four prominent single, non-magnetic O stars zeta Pup, zeta Ori, xi Per and zeta Oph, obtained in high resolution with Chandra HETGS/MEG have been studied. The resolved X-ray emission line profiles provide information about the shocked, hot gas which emits the X-radiation, and about the bulk of comparably cool stellar wind material which partly absorbs this radiation. In this paper, we synthesize X-ray line profiles with a model of a clumpy stellar wind. We find that the geometrical shape of the wind inhomogeneities is important: better agreement with the observations can be achieved with radially compressed clumps than with spherical clumps. The parameters of the model, i.e. chemical abundances, stellar radius, mass-loss rate and terminal wind velocity, are taken from existing analyses of UV and optical spectra of the programme stars. On this basis, we also calculate the continuum-absorption coefficient of the cool-wind material, using the Potsdam Wolf-Rayet (POWR) model atmosphere code. The radial location of X-ray emitting gas is restricted from analysing the FIR line ratios of helium-like ions. The only remaining free parameter of our model is the typical distance between the clumps; here, we assume that at any point in the wind there is one clump passing by per one dynamical time-scale of the wind. The total emission in a model line is scaled to the observation. There is a good agreement between synthetic and observed line profiles. We conclude that the X-ray emission line profiles in O stars can be explained by hot plasma embedded in a cool wind which is highly clumped in the form of radially compressed shell fragments. KW - stars : individual : zeta Pup KW - stars : individual : zeta Ori KW - stars : individual : xi Per KW - stars : individual : zeta Oph KW - X-rays : stars Y1 - 2006 U6 - https://doi.org/10.1111/j.1365-2966.2006.10858.x SN - 0035-8711 VL - 372 SP - 313 EP - 326 PB - Oxford University Press CY - Oxford ER - TY - JOUR A1 - Hainich, Rainer A1 - Oskinova, Lidia M. A1 - Shenar, Tomer A1 - Marchant Campos, Pablo A1 - Eldridge, J. J. A1 - Sander, Andreas Alexander Christoph A1 - Hamann, Wolf-Rainer A1 - Langer, Norbert A1 - Todt, Helge Tobias T1 - Observational properties of massive black hole binary progenitors JF - Astronomy and astrophysics : an international weekly journal N2 - Context: The first directly detected gravitational waves (GW 150914) were emitted by two coalescing black holes (BHs) with masses of ≈ 36 M⊙ and ≈ 29 M⊙. Several scenarios have been proposed to put this detection into an astrophysical context. The evolution of an isolated massive binary system is among commonly considered models. Aims: Various groups have performed detailed binary-evolution calculations that lead to BH merger events. However, the question remains open as to whether binary systems with the predicted properties really exist. The aim of this paper is to help observers to close this gap by providing spectral characteristics of massive binary BH progenitors during a phase where at least one of the companions is still non-degenerate. Methods: Stellar evolution models predict fundamental stellar parameters. Using these as input for our stellar atmosphere code (Potsdam Wolf-Rayet), we compute a set of models for selected evolutionary stages of massive merging BH progenitors at different metallicities. Results: The synthetic spectra obtained from our atmosphere calculations reveal that progenitors of massive BH merger events start their lives as O2-3V stars that evolve to early-type blue supergiants before they undergo core-collapse during the Wolf-Rayet phase. When the primary has collapsed, the remaining system will appear as a wind-fed high-mass X-ray binary. Based on our atmosphere models, we provide feedback parameters, broad band magnitudes, and spectral templates that should help to identify such binaries in the future. Conclusions: While the predicted parameter space for massive BH binary progenitors is partly realized in nature, none of the known massive binaries match our synthetic spectra of massive BH binary progenitors exactly. Comparisons of empirically determined mass-loss rates with those assumed by evolution calculations reveal significant differences. The consideration of the empirical mass-loss rates in evolution calculations will possibly entail a shift of the maximum in the predicted binary-BH merger rate to higher metallicities, that is, more candidates should be expected in our cosmic neighborhood than previously assumed. KW - gravitational waves KW - binaries: close KW - stars: early-type KW - stars: atmospheres KW - stars: winds KW - outflows KW - stars: mass-loss Y1 - 2018 U6 - https://doi.org/10.1051/0004-6361/201731449 SN - 1432-0746 VL - 609 PB - EDP Sciences CY - Les Ulis ER - TY - JOUR A1 - Fulmer, Leah M. A1 - Gallagher, John S. A1 - Hamann, Wolf-Rainer A1 - Oskinova, Lidia M. A1 - Ramachandran, Varsha T1 - Testing massive star evolution, star-formation history, and feedback at low metallicity BT - photometric analysis of OB stars in the SMC Wing JF - Astronomy and astrophysics : an international weekly journal N2 - Context. The supergiant ionized shell SMC-SGS 1 (DEM 167), which is located in the outer Wing of the Small Magellanic Cloud (SMC), resembles structures that originate from an energetic star-formation event and later stimulate star formation as they expand into the ambient medium. However, stellar populations within and surrounding SMC-SGS 1 tell a different story. Aims. We present a photometric study of the stellar population encompassed by SMC-SGS 1 in order to trace the history of such a large structure and its potential influence on star formation within the low-density, low-metallicity environment of the SMC. Methods. For a stellar population that is physically associated with SMC-SGS 1, we combined near-ultraviolet (NUV) photometry from the Galaxy Evolution Explorer with archival optical (V-band) photometry from the ESO Danish 1.54 m Telescope. Given their colors and luminosities, we estimated stellar ages and masses by matching observed photometry to theoretical stellar isochrone models. Results. We find that the investigated region supports an active, extended star-formation event spanning similar to 25-40 Myr ago, as well as continued star formation into the present. Using a standard initial mass function, we infer a lower bound on the stellar mass from this period of similar to 3 x 10(4) M-circle dot, corresponding to a star-formation intensity of similar to 6 x 10(-3) M-circle dot kpc(-2) yr(-1). Conclusions. The spatial and temporal distributions of young stars encompassed by SMC-SGS 1 imply a slow, consistent progression of star formation over millions of years. Ongoing star formation, both along the edge and interior to SMC-SGS 1, suggests a combined stimulated and stochastic mode of star formation within the SMC Wing. We note that a slow expansion of the shell within this low-density environment may preserve molecular clouds within the volume of the shell, leaving them to form stars even after nearby stellar feedback expels local gas and dust. KW - galaxies KW - stellar content KW - stars KW - formation KW - individual KW - Small KW - Magellanic Cloud Y1 - 2020 U6 - https://doi.org/10.1051/0004-6361/201834314 SN - 0004-6361 SN - 1432-0746 VL - 633 PB - EDP Sciences CY - Les Ulis ER - TY - JOUR A1 - Toalá, Jesús Alberto A1 - Bowman, Dominic A1 - Van Reeth, Timothy A1 - Todt, Helge Tobias A1 - Dsilva, Karan A1 - Shenar, Tomer A1 - Koenigsberger, Gloria Suzanne A1 - Estrada-Dorado, Sandino A1 - Oskinova, Lidia M. A1 - Hamann, Wolf-Rainer T1 - Multiple variability time-scales of the early nitrogen-rich Wolf-Rayet star WR 7 JF - Monthly notices of the Royal Astronomical Society N2 - We present the analysis of the optical variability of the early, nitrogen-rich Wolf-Rayet (WR) star WR 7. The analysis of multisector Transiting Exoplanet Survey Satellite (TESS) light curves and high-resolution spectroscopic observations confirm multiperiodic variability that is modulated on time-scales of years. We detect a dominant period of 2.6433 +/- 0.0005 d in the TESS sectors 33 and 34 light curves in addition to the previously reported high-frequency features from sector 7. We discuss the plausible mechanisms that may be responsible for such variability in WR 7, including pulsations, binarity, co-rotating interaction regions (CIRs), and clumpy winds. Given the lack of strong evidence for the presence of a stellar or compact companion, we suggest that WR 7 may pulsate in quasi-coherent modes in addition to wind variability likely caused by CIRs on top of stochastic low-frequency variability. WR 7 is certainly a worthy target for future monitoring in both spectroscopy and photometry to sample both the short (less than or similar to 1 d) and long (greater than or similar to 1000 d) variability time-scales. KW - stars: atmospheres KW - stars: evolution KW - stars: individual: WR 7 KW - stars: winds KW - outflows KW - stars: Wolft-Rayet Y1 - 2022 U6 - https://doi.org/10.1093/mnras/stac1455 SN - 0035-8711 SN - 1365-2966 VL - 514 IS - 2 SP - 2269 EP - 2277 PB - Oxford University Press CY - Oxford ER - TY - JOUR A1 - Oskinova, Lidia M. A1 - Schaerer, Daniel T1 - Ionization of He II in star-forming galaxies by X-rays from cluster winds and superbubbles JF - Astronomy and astrophysics : an international weekly journal N2 - The nature of the sources powering nebular He II emission in star-forming galaxies remains debated, and various types of objects have been considered, including Wolf-Rayet stars, X-ray binaries, and Population III stars. Modern X-ray observations show the ubiquitous presence of hot gas filling star-forming galaxies. We use a collisional ionization plasma code to compute the specific He II ionizing flux produced by hot gas and show that if its temperature is not too high (less than or similar to 2.5 MK), then the observed levels of soft diffuse X-ray radiation could explain He II ionization in galaxies. To gain a physical understanding of this result, we propose a model that combines the hydrodynamics of cluster winds and hot superbubbles with observed populations of young massive clusters in galaxies. We find that in low-metallicity galaxies, the temperature of hot gas is lower and the production rate of He II ionizing photons is higher compared to high-metallicity galaxies. The reason is that the slower stellar winds of massive stars in lower-metallicity galaxies input less mechanical energy in the ambient medium. Furthermore, we show that ensembles of star clusters up to similar to 10-20 Myr old in galaxies can produce enough soft X-rays to induce nebular He II emission. We discuss observations of the template low-metallicity galaxy I Zw 18 and suggest that the He II nebula in this galaxy is powered by a hot superbubble. Finally, appreciating the complex nature of stellar feedback, we suggest that soft X-rays from hot superbubbles are among the dominant sources of He II ionizing flux in low-metallicity star-forming galaxies. KW - galaxies KW - ISM KW - high-redshift KW - bubbles KW - X-rays Y1 - 2022 U6 - https://doi.org/10.1051/0004-6361/202142520 SN - 0004-6361 SN - 1432-0746 VL - 661 PB - EDP Sciences CY - Les Ulis ER - TY - JOUR A1 - Tönjes, Ralf A1 - Kori, Hiroshi T1 - Phase and frequency linear response theory for hyperbolic chaotic oscillators JF - Chaos : an interdisciplinary journal of nonlinear science N2 - We formulate a linear phase and frequency response theory for hyperbolic flows, which generalizes phase response theory for autonomous limit cycle oscillators to hyperbolic chaotic dynamics. The theory is based on a shadowing conjecture, stating the existence of a perturbed trajectory shadowing every unperturbed trajectory on the system attractor for any small enough perturbation of arbitrary duration and a corresponding unique time isomorphism, which we identify as phase such that phase shifts between the unperturbed trajectory and its perturbed shadow are well defined. The phase sensitivity function is the solution of an adjoint linear equation and can be used to estimate the average change of phase velocity to small time dependent or independent perturbations. These changes in frequency are experimentally accessible, giving a convenient way to define and measure phase response curves for chaotic oscillators. The shadowing trajectory and the phase can be constructed explicitly in the tangent space of an unperturbed trajectory using co-variant Lyapunov vectors. It can also be used to identify the limits of the regime of linear response. Y1 - 2022 U6 - https://doi.org/10.1063/5.0064519 SN - 1054-1500 SN - 1089-7682 VL - 32 IS - 4 PB - AIP Publishing CY - Melville ER - TY - JOUR A1 - Zheng, Chunming A1 - Tönjes, Ralf A1 - Pikovskij, Arkadij T1 - Transition to synchrony in a three-dimensional swarming model with helical trajectories JF - Physical review : E, Statistical, nonlinear and soft matter physics N2 - We investigate the transition from incoherence to global collective motion in a three-dimensional swarming model of agents with helical trajectories, subject to noise and global coupling. Without noise this model was recently proposed as a generalization of the Kuramoto model and it was found that alignment of the velocities occurs discontinuously for arbitrarily small attractive coupling. Adding noise to the system resolves this singular limit and leads to a continuous transition, either to a directed collective motion or to center-of-mass rotations. Y1 - 2021 U6 - https://doi.org/10.1103/PhysRevE.104.014216 SN - 2470-0045 SN - 2470-0053 VL - 104 IS - 1 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Tönjes, Ralf A1 - Pikovsky, Arkady T1 - Low-dimensional description for ensembles of identical phase oscillators subject to Cauchy noise JF - Physical review : E, Statistical, nonlinear and soft matter physics N2 - We study ensembles of globally coupled or forced identical phase oscillators subject to independent white Cauchy noise. We demonstrate that if the oscillators are forced in several harmonics, stationary synchronous regimes can be exactly described with a finite number of complex order parameters. The corresponding distribution of phases is a product of wrapped Cauchy distributions. For sinusoidal forcing, the Ott-Antonsen low-dimensional reduction is recovered. Y1 - 2020 U6 - https://doi.org/10.1103/PhysRevE.102.052315 SN - 2470-0045 SN - 2470-0053 VL - 102 IS - 5 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Gong, Chen Chris A1 - Zheng, Chunming A1 - Tönjes, Ralf A1 - Pikovskij, Arkadij T1 - Repulsively coupled Kuramoto-Sakaguchi phase oscillators ensemble subject to common noise JF - Chaos : an interdisciplinary journal of nonlinear science N2 - We consider the Kuramoto-Sakaguchi model of identical coupled phase oscillators with a common noisy forcing. While common noise always tends to synchronize the oscillators, a strong repulsive coupling prevents the fully synchronous state and leads to a nontrivial distribution of oscillator phases. In previous numerical simulations, the formation of stable multicluster states has been observed in this regime. However, we argue here that because identical phase oscillators in the Kuramoto-Sakaguchi model form a partially integrable system according to the Watanabe-Strogatz theory, the formation of clusters is impossible. Integrating with various time steps reveals that clustering is a numerical artifact, explained by the existence of higher order Fourier terms in the errors of the employed numerical integration schemes. By monitoring the induced change in certain integrals of motion, we quantify these errors. We support these observations by showing, on the basis of the analysis of the corresponding Fokker-Planck equation, that two-cluster states are non-attractive. On the other hand, in ensembles of general limit cycle oscillators, such as Van der Pol oscillators, due to an anharmonic phase response function as well as additional amplitude dynamics, multiclusters can occur naturally. Published under license by AIP Publishing. Y1 - 2019 U6 - https://doi.org/10.1063/1.5084144 SN - 1054-1500 SN - 1089-7682 VL - 29 IS - 3 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Gong, Chen Chris A1 - Tönjes, Ralf A1 - Pikovsky, Arkady T1 - Coupled Möbius maps as a tool to model Kuramoto phase synchronization JF - Physical review : E, Statistical, nonlinear and soft matter physics N2 - We propose Mobius maps as a tool to model synchronization phenomena in coupled phase oscillators. Not only does the map provide fast computation of phase synchronization, it also reflects the underlying group structure of the sinusoidally coupled continuous phase dynamics. We study map versions of various known continuous-time collective dynamics, such as the synchronization transition in the Kuramoto-Sakaguchi model of nonidentical oscillators, chimeras in two coupled populations of identical phase oscillators, and Kuramoto-Battogtokh chimeras on a ring, and demonstrate similarities and differences between the iterated map models and their known continuous-time counterparts. Y1 - 2020 U6 - https://doi.org/10.1103/PhysRevE.102.022206 SN - 2470-0045 SN - 2470-0053 SN - 1063-651X SN - 2470-0061 SN - 1550-2376 VL - 102 IS - 2 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Zheng, Chunming A1 - Tönjes, Ralf T1 - Noise-induced swarming of active particles JF - Physical review : E, Statistical, nonlinear and soft matter physics N2 - We report on the effect of spatially correlated noise on the velocities of self-propelled particles. Correlations in the random forces acting on self-propelled particles can induce directed collective motion, i.e., swarming. Even with repulsive coupling in the velocity directions, which favors a disordered state, strong correlations in the fluctuations can align the velocities locally leading to a macroscopic, turbulent velocity field. On the other hand, while spatially correlated noise is aligning the velocities locally, the swarming transition to globally directed motion is inhibited when the correlation length of the noise is nonzero, but smaller than the system size. We analyze the swarming transition in d-dimensional space in a mean field model of globally coupled velocity vectors. Y1 - 2022 U6 - https://doi.org/10.1103/PhysRevE.106.064601 SN - 2470-0045 SN - 2470-0053 VL - 106 IS - 6 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Pasechnik, Sergey V. A1 - Shmeleva, Dina A1 - Saidgaziev, Ayvr Sh. A1 - Kharlamov, Semen A1 - Vasilieva, Aleksandra A. A1 - Santer, Svetlana T1 - Shear flows induced by electro-osmotic pumps in optofluidic liquid crystal cell for modulation of visible light and THz irradiation JF - Liquid Crystals and their Application : Russian Journal N2 - The work is devoted to the use of electrokinetic phenomena in liquid crystals to create a new class of microfluidics devices - optofluidics, designed to control electromagnetic radiation, including the THz frequency range. To achieve the goal, an optical method is used to study changes in the orientational structure in LC layers caused by a shear flow generated by electroosmotic pumps. Simula-tion of LC behaviour in an experimental cell containing electroosmotic pumps and flat layers of a nematic liquid crystal is fulfilled. The experimental depend-ences of the intensity of polarized radiation passing through flat LC layers on the control voltage applied to the electroosmotic pump and the results of calcu-lations of the hydrodynamic and mechano-optical characteristics of the experi-mental LC cell are presented. The propagation of THz irradiation across the multilayer structure of the optofluidic cell is considered taking into account the minimum number of re-reflections of waves from different layers and the ab-sorption of THz irradiation in a propylene and a liquid crystal. N2 - Работа посвящена использованию электрокинетических явлений в жидких кристаллах для создания нового класса микрофлюидных устройств – опто- флюидики, предназначенных для управления электромагнитным излуче- нием, в том числе терагерцового диапазона частот. Для достижения цели оптическим методом исследуются изменения ориентационной структуры в слоях ЖК, вызванные сдвиговым течением, генерируемым электроосмоти- ческими насосами. Проведено моделирование поведения ЖК в эксперимен- тальной ячейке, содержащей электроосмотические насосы и плоские слои нематического жидкого кристалла. Представлены экспериментальные за- висимости интенсивности поляризованного излучения, проходящего через плоские слои ЖК, от управляющего напряжения, подаваемого на электро- осмотический насос, и результаты расчетов гидродинамических и механо- оптических характеристик экспериментальной ЖК-ячейки. Рассмотрено распространение ТГц излучения по многослойной структуре оптофлюид- ной ячейки с учетом минимального числа переотражений волн от разных слоев и поглощения ТГц излучения в пропилене и жидком кристалле. KW - nematic liquid crystal KW - terahertz range KW - electrokinetic phenomena KW - osmotic flow KW - director configuration KW - optical irradiation intensity KW - E7 KW - polypropylene Y1 - 2022 U6 - https://doi.org/10.18083/LCAppl.2022.3.49 SN - 1991-3966 SN - 2499–9644 VL - 22 IS - 3 SP - 49 EP - 57 PB - Nanomaterials Research Institute CY - Ivanovo ER - TY - JOUR A1 - Pick, Leonie A1 - Effenberger, Frederic A1 - Zhelavskaya, Irina A1 - Korte, Monika T1 - A Statistical Classifier for Historical Geomagnetic Storm Drivers Derived Solely From Ground-Based Magnetic Field Measurements JF - Earth and Space Science N2 - Solar wind observations show that geomagnetic storms are mainly driven by interplanetary coronal mass ejections (ICMEs) and corotating or stream interaction regions (C/SIRs). We present a binary classifier that assigns one of these drivers to 7,546 storms between 1930 and 2015 using ground‐based geomagnetic field observations only. The input data consists of the long‐term stable Hourly Magnetospheric Currents index alongside the corresponding midlatitude geomagnetic observatory time series. This data set provides comprehensive information on the global storm time magnetic disturbance field, particularly its spatial variability, over eight solar cycles. For the first time, we use this information statistically with regard to an automated storm driver identification. Our supervised classification model significantly outperforms unskilled baseline models (78% accuracy with 26[19]% misidentified interplanetary coronal mass ejections [corotating or stream interaction regions]) and delivers plausible driver occurrences with regard to storm intensity and solar cycle phase. Our results can readily be used to advance related studies fundamental to space weather research, for example, studies connecting galactic cosmic ray modulation and geomagnetic disturbances. They are fully reproducible by means of the underlying open‐source software (Pick, 2019, http://doi.org/10.5880/GFZ.2.3.2019.003) KW - geomagnetic observatory data KW - geomagnetic storm drivers KW - historical geomagnetic storms KW - supervised machine learning Y1 - 2019 U6 - https://doi.org/10.1029/2019EA000726 SN - 2333-5084 VL - 6 SP - 2000 EP - 2015 PB - American Geophysical Union CY - Malden, Mass. ER - TY - JOUR A1 - Karamzadeh Toularoud, Nasim A1 - Heimann, Sebastian A1 - Dahm, Torsten A1 - Krüger, Frank T1 - Application based seismological array design by seismicity scenario modelling JF - Geophysical journal international N2 - The design of an array configuration is an important task in array seismology during experiment planning. Often the array response function (ARF), which depends on the relative position of array stations and frequency content of the incoming signals, is used as the array design criterion. In practice, additional constraints and parameters have to be taken into account, for example, land ownership, site-specific noise levels or characteristics of the seismic sources under investigation. In this study, a flexible array design framework is introduced that implements a customizable scenario modelling and optimization scheme by making use of synthetic seismograms. Using synthetic seismograms to evaluate array performance makes it possible to consider additional constraints. We suggest to use synthetic array beamforming as an array design criterion instead of the ARF. The objective function of the optimization scheme is defined according to the monitoring goals, and may consist of a number of subfunctions. The array design framework is exemplified by designing a seven-station small-scale array to monitor earthquake swarm activity in Northwest Bohemia/Vogtland in central Europe. Two subfunctions are introduced to verify the accuracy of horizontal slowness estimation; one to suppress aliasing effects due to possible secondary lobes of synthetic array beamforming calculated in horizontal slowness space and the other to reduce the event’s mislocation caused by miscalculation of the horizontal slowness vector. Subsequently, a weighting technique is applied to combine the subfunctions into one single scalar objective function to use in the optimization process. KW - Array Seismology KW - Array design KW - Seismicity modelling Y1 - 2018 SN - 0956-540X SN - 1365-246X VL - 216 IS - 3 SP - 1711 EP - 1727 PB - Oxford Univ. Press CY - Oxford ER - TY - JOUR A1 - Li, Tian-yi A1 - Benduhn, Johannes A1 - Qiao, Zhi A1 - Liu, Yuan A1 - Li, Yue A1 - Shivhare, Rishi A1 - Jaiser, Frank A1 - Wang, Pei A1 - Ma, Jie A1 - Zeika, Olaf A1 - Neher, Dieter A1 - Mannsfeld, Stefan C. B. A1 - Ma, Zaifei A1 - Vandewal, Koen A1 - Leo, Karl T1 - Effect of H- and J-Aggregation on the Photophysical and Voltage Loss of Boron Dipyrromethene Small Molecules in Vacuum-Deposited Organic Solar Cells JF - The journal of physical chemistry letters N2 - An understanding of the factors limiting the open-circuit voltage (V-oc) and related photon energy loss mechanisms is critical to increase the power conversion efficiency (PCE) of small-molecule organic solar cells (OSCs), especially those with near-infrared (NIR) absorbers. In this work, two NIR boron dipyrromethene (BODIPY) molecules are characterized for application in planar (PHJ) and bulk (BHJ) heterojunction OSCs. When two H atoms are substituted by F atoms on the peripheral phenyl rings of the molecules, the molecular aggregation type in the thin film changes from the H-type to J-type. For PHJ devices, the nonradiative voltage loss of 0.35 V in the J-aggregated BODIPY is lower than that of 0.49 V in the H-aggregated device. In BHJ devices with a nonradiative voltage loss of 0.35 V, a PCE of 5.5% is achieved with an external quantum efficiency (EQE) maximum of 68% at 700 nm. Y1 - 2019 U6 - https://doi.org/10.1021/acs.jpclett.9b01222 SN - 1948-7185 VL - 10 IS - 11 SP - 2684 EP - 2691 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Yang, Xiao Hui A1 - Jaiser, Frank A1 - Stiller, Burkhard A1 - Neher, Dieter A1 - Galbrecht, Frank A1 - Scherf, Ullrich T1 - Efficient polymer electrophosphoreseent devices with interfacial layers JF - Advanced functional materials N2 - It is shown that several polymers can form insoluble interfacial layers on a poly (ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) layer after annealing of the double-layer structure. The thickness of the interlayer is dependent on the characteristics of the underlying PEDOT.PSS and the molecular weight of the polymers. It is further shown that the electronic structures of the interlayer polymers have a significant effect on the properties of red-light-emitting polymer-based electrophosphorescent devices. Upon increasing the highest occupied molecular orbital and lowest unoccupied molecular orbital positions, a significant increase in current density and device efficiency is observed. This is attributed to efficient blocking of electrons in combination with direct injection of holes from the interlayer to the phosphorescent dye. Upon proper choice of the interlayer polymer, efficient red, polymer-based electrophosphorescent devices with a peak luminance efficiency of 5.5 cd A(-1) (external quantum efficiency = 6 %) and a maximum power-conversion efficiency of 5 Im W-1 can be realized. Y1 - 2006 U6 - https://doi.org/10.1002/adfm.200500834 SN - 1616-301X SN - 1616-3028 VL - 16 IS - 16 SP - 2156 EP - 2162 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Kurpiers, Jona A1 - Ferron, Thomas A1 - Roland, Steffen A1 - Jakoby, Marius A1 - Thiede, Tobias A1 - Jaiser, Frank A1 - Albrecht, Steve A1 - Janietz, Silvia A1 - Collins, Brian A. A1 - Howard, Ian A. A1 - Neher, Dieter T1 - Probing the pathways of free charge generation in organic bulk heterojunction solar cells JF - Nature Communications N2 - The fact that organic solar cells perform efficiently despite the low dielectric constant of most photoactive blends initiated a long-standing debate regarding the dominant pathways of free charge formation. Here, we address this issue through the accurate measurement of the activation energy for free charge photogeneration over a wide range of photon energy, using the method of time-delayed collection field. For our prototypical low bandgap polymer:fullerene blends, we find that neither the temperature nor the field dependence of free charge generation depend on the excitation energy, ruling out an appreciable contribution to free charge generation though hot carrier pathways. On the other hand, activation energies are on the order of the room temperature thermal energy for all studied blends. We conclude that charge generation in such devices proceeds through thermalized charge transfer states, and that thermal energy is sufficient to separate most of these states into free charges. Y1 - 2018 U6 - https://doi.org/10.1038/s41467-018-04386-3 SN - 2041-1723 VL - 9 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Sarhan, Radwan Mohamed A1 - Koopman, Wouter-Willem Adriaan A1 - Pudell, Jan-Etienne A1 - Stete, Felix A1 - Rössle, Matthias A1 - Herzog, Marc A1 - Schmitt, Clemens Nikolaus Zeno A1 - Liebig, Ferenc A1 - Koetz, Joachim A1 - Bargheer, Matias T1 - Scaling up nanoplasmon catalysis BT - the role of heat dissipation JF - The journal of physical chemistry : C, Nanomaterials and interfaces N2 - Nanoscale heating by optical excitation of plasmonic nanoparticles offers a new perspective of controlling chemical reactions, where heat is not spatially uniform as in conventional macroscopic heating but strong temperature gradients exist around microscopic hot spots. In nanoplasmonics, metal particles act as a nanosource of light, heat, and energetic electrons driven by resonant excitation of their localized surface plasmon resonance. As an example of the coupling reaction of 4-nitrothiophenol into 4,4′-dimercaptoazobenzene, we show that besides the nanoscopic heat distribution at hot spots, the microscopic distribution of heat dictated by the spot size of the light focus also plays a crucial role in the design of plasmonic nanoreactors. Small sizes of laser spots enable high intensities to drive plasmon-assisted catalysis. This facilitates the observation of such reactions by surface-enhanced Raman scattering, but it challenges attempts to scale nanoplasmonic chemistry up to large areas, where the excess heat must be dissipated by one-dimensional heat transport. KW - Gold KW - Raman spectroscopy KW - Silicon KW - Irradiation KW - Lasers Y1 - 2019 U6 - https://doi.org/10.1021/acs.jpcc.8b12574 SN - 1932-7447 VL - 123 IS - 14 SP - 9352 EP - 9357 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Sini, Gjergji A1 - Schubert, Marcel A1 - Risko, Chad A1 - Roland, Steffen A1 - Lee, Olivia P. A1 - Chen, Zhihua A1 - Richter, Thomas V. A1 - Dolfen, Daniel A1 - Coropceanu, Veaceslav A1 - Ludwigs, Sabine A1 - Scherf, Ullrich A1 - Facchetti, Antonio A1 - Frechet, Jean M. J. A1 - Neher, Dieter T1 - On the Molecular Origin of Charge Separation at the Donor-Acceptor Interface JF - Advanced energy materials N2 - Fullerene-based acceptors have dominated organic solar cells for almost two decades. It is only within the last few years that alternative acceptors rival their dominance, introducing much more flexibility in the optoelectronic properties of these material blends. However, a fundamental physical understanding of the processes that drive charge separation at organic heterojunctions is still missing, but urgently needed to direct further material improvements. Here a combined experimental and theoretical approach is used to understand the intimate mechanisms by which molecular structure contributes to exciton dissociation, charge separation, and charge recombination at the donor-acceptor (D-A) interface. Model systems comprised of polythiophene-based donor and rylene diimide-based acceptor polymers are used and a detailed density functional theory (DFT) investigation is performed. The results point to the roles that geometric deformations and direct-contact intermolecular polarization play in establishing a driving force ( energy gradient) for the optoelectronic processes taking place at the interface. A substantial impact for this driving force is found to stem from polymer deformations at the interface, a finding that can clearly lead to new design approaches in the development of the next generation of conjugated polymers and small molecules. KW - donor-acceptor interfaces KW - energy gradients KW - geometrical deformations KW - nonfullerene acceptors KW - organic photovoltaics KW - photocurrent generation KW - polymer solar cells Y1 - 2018 U6 - https://doi.org/10.1002/aenm.201702232 SN - 1614-6832 SN - 1614-6840 VL - 8 IS - 12 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Ullbrich, Sascha A1 - Benduhn, Johannes A1 - Jia, Xiangkun A1 - Nikolis, Vasileios C. A1 - Tvingstedt, Kristofer A1 - Piersimoni, Fortunato A1 - Roland, Steffen A1 - Liu, Yuan A1 - Wu, Jinhan A1 - Fischer, Axel A1 - Neher, Dieter A1 - Reineke, Sebastian A1 - Spoltore, Donato A1 - Vandewal, Koen T1 - Emissive and charge-generating donor-acceptor interfaces for organic optoelectronics with low voltage losses JF - Nature materials N2 - Intermolecular charge-transfer states at the interface between electron donating (D) and accepting (A) materials are crucial for the operation of organic solar cells but can also be exploited for organic light-emitting diodes(1,2). Non-radiative charge-transfer state decay is dominant in state-of-the-art D-A-based organic solar cells and is responsible for large voltage losses and relatively low power-conversion efficiencies as well as electroluminescence external quantum yields in the 0.01-0.0001% range(3,4). In contrast, the electroluminescence external quantum yield reaches up to 16% in D-A-based organic light-emitting diodes(5-7). Here, we show that proper control of charge-transfer state properties allows simultaneous occurrence of a high photovoltaic and emission quantum yield within a single, visible-light-emitting D-A system. This leads to ultralow-emission turn-on voltages as well as significantly reduced voltage losses upon solar illumination. These results unify the description of the electro-optical properties of charge-transfer states in organic optoelectronic devices and foster the use of organic D-A blends in energy conversion applications involving visible and ultraviolet photons(8-11). KW - Electronics, photonics and device physics KW - Optoelectronic devices and components KW - Photonic devices KW - Solar energy and photovoltaic technology Y1 - 2019 U6 - https://doi.org/10.1038/s41563-019-0324-5 SN - 1476-1122 SN - 1476-4660 VL - 18 IS - 5 SP - 459 EP - 464 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Ran, Niva A. A1 - Love, John A. A1 - Heiber, Michael C. A1 - Jiao, Xuechen A1 - Hughes, Michael P. A1 - Karki, Akchheta A1 - Wang, Ming A1 - Brus, Viktor V. A1 - Wang, Hengbin A1 - Neher, Dieter A1 - Ade, Harald A1 - Bazan, Guillermo C. A1 - Thuc-Quyen Nguyen, T1 - Charge generation and recombination in an organic solar cell with low energetic offsets JF - dvanced energy materials N2 - Organic bulk heterojunction (BHJ) solar cells require energetic offsets between the donor and acceptor to obtain high short-circuit currents (J(SC)) and fill factors (FF). However, it is necessary to reduce the energetic offsets to achieve high open-circuit voltages (V-OC). Recently, reports have highlighted BHJ blends that are pushing at the accepted limits of energetic offsets necessary for high efficiency. Unfortunately, most of these BHJs have modest FF values. How the energetic offset impacts the solar cell characteristics thus remains poorly understood. Here, a comprehensive characterization of the losses in a polymer:fullerene BHJ blend, PIPCP:phenyl-C61-butyric acid methyl ester (PC61BM), that achieves a high V-OC (0.9 V) with very low energy losses (E-loss = 0.52 eV) from the energy of absorbed photons, a respectable J(SC) (13 mA cm(-2)), but a limited FF (54%) is reported. Despite the low energetic offset, the system does not suffer from field-dependent generation and instead it is characterized by very fast nongeminate recombination and the presence of shallow traps. The charge-carrier losses are attributed to suboptimal morphology due to high miscibility between PIPCP and PC61BM. These results hold promise that given the appropriate morphology, the J(SC), V-OC, and FF can all be improved, even with very low energetic offsets. KW - energetic offset KW - fill factor KW - morphology KW - organic solar cells KW - recombination Y1 - 2018 U6 - https://doi.org/10.1002/aenm.201701073 SN - 1614-6832 SN - 1614-6840 VL - 8 IS - 5 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Hosseini, Seyed Mehrdad A1 - Roland, Steffen A1 - Kurpiers, Jona A1 - Chen, Zhiming A1 - Zhang, Kai A1 - Huang, Fei A1 - Armin, Ardalan A1 - Neher, Dieter A1 - Shoaee, Safa T1 - Impact of Bimolecular Recombination on the Fill Factor of Fullerene and Nonfullerene-Based Solar Cells BT - A Comparative Study of Charge Generation and Extraction JF - The journal of physical chemistry : C, Nanomaterials and interfaces N2 - Power conversion efficiencies of donor/acceptor organic solar cells utilizing nonfullerene acceptors have now increased beyond the record of their fullerene-based counterparts. There remain many fundamental questions regarding nanomorphology, interfacial states, charge generation and extraction, and losses in these systems. Herein, we present a comparative study of bulk heterojunction solar cells composed of a recently introduced naphthothiadiazole-based polymer (NT812) as the electron donor and two different acceptor molecules, namely, [6,6]-phenyl-C71-butyric acid methyl ester (PCBM)[70] and 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2′,3′-d′]-s-indaceno[1,2-b:5,6-b′]dithiophene (ITIC). A comparison between the photovoltaic performance of these two types of solar cells reveals that the open-circuit voltage (Voc) of the NT812:ITIC-based solar cell is larger, but the fill factor (FF) is lower than that of the NT812:PCBM[70] device. We find the key reason behind this reduced FF in the ITIC-based device to be faster nongeminate recombination relative to the NT812:PCBM[70] system. Y1 - 2019 U6 - https://doi.org/10.1021/acs.jpcc.8b11669 SN - 1932-7447 VL - 123 IS - 11 SP - 6823 EP - 6830 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Roland, Steffen A1 - Yan, Liang A1 - Zhang, Qianqian A1 - Jiao, Xuechen A1 - Hunt, Adrian A1 - Ghasemi, Masoud A1 - Ade, Harald A1 - You, Wei A1 - Neher, Dieter T1 - Charge Generation and Mobility-Limited Performance of Bulk Heterojunction Solar Cells with a Higher Adduct Fullerene JF - The journal of physical chemistry : C, Nanomaterials and interfaces N2 - Alternative electron acceptors are being actively explored in order to advance the development of bulk-heterojunction (BHJ) organic solar cells (OSCs). The indene-C-60 bisadduct (ICBA) has been regarded as a promising candidate, as it provides high open-circuit voltage in BHJ solar cells; however, the photovoltaic performance of such ICBA-based devices is often inferior when compared to cells with the omnipresent PCBM electron acceptor. Here, by pairing the high performance polymer (FTAZ) as the donor with either PCBM or ICBA as the acceptor, we explore the physical mechanism behind the reduced performance of the ICBA-based device. Time delayed collection field (TDCF) experiments reveal reduced, yet field-independent free charge generation in the FTAZ:ICBA system, explaining the overall lower photocurrent in its cells. Through the analysis of the photoluminescence, photogeneration, and electroluminescence, we find that the lower generation efficiency is neither caused by inefficient exciton splitting, nor do we find evidence for significant energy back-transfer from the CT state to singlet excitons. In fact, the increase in open circuit voltage when replacing PCBM by ICBA is entirely caused by the increase in the CT energy, related to the shift in the LUMO energy, while changes in the radiative and nonradiative recombination losses are nearly absent. On the other hand, space charge limited current (SCLC) and bias-assisted charge extraction (BACE) measurements consistently reveal a severely lower electron mobilitiy in the FTAZ:ICBA blend. Studies of the blends with resonant soft X-ray scattering (R-SoXS), grazing incident wide-angle X-ray scattering (GIWAXS), and scanning transmission X-ray microscopy (STXM) reveal very little differences in the mesoscopic morphology but significantly less nanoscale molecular ordering of the fullerene domains in the ICBA based blends, which we propose as the main cause for the lower generation efficiency and smaller electron mobility. Calculations of the JV curves with an analytical model, using measured values, show good agreement with the experimentally determined JV characteristics, proving that these devices suffer from slow carrier extraction, resulting in significant bimolecular recombination losses. Therefore, this study highlights the importance of high charge carrier mobility for newly synthesized acceptor materials, in addition to having suitable energy levels. Y1 - 2017 U6 - https://doi.org/10.1021/acs.jpcc.7b02288 SN - 1932-7447 VL - 121 SP - 10305 EP - 10316 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Benduhn, Johannes A1 - Tvingstedt, Kristofer A1 - Piersimoni, Fortunato A1 - Ullbrich, Sascha A1 - Fan, Yeli A1 - Tropiano, Manuel A1 - McGarry, Kathryn A. A1 - Zeika, Olaf A1 - Riede, Moritz K. A1 - Douglas, Christopher J. A1 - Barlow, Stephen A1 - Marder, Seth R. A1 - Neher, Dieter A1 - Spoltore, Donato A1 - Vandewal, Koen T1 - Intrinsic non-radiative voltage losses in fullerene-based organic solar cells JF - Nature Energy N2 - Organic solar cells demonstrate external quantum efficiencies and fill factors approaching those of conventional photovoltaic technologies. However, as compared with the optical gap of the absorber materials, their open-circuit voltage is much lower, largely due to the presence of significant non-radiative recombination. Here, we study a large data set of published and new material combinations and find that non-radiative voltage losses decrease with increasing charge-transfer-state energies. This observation is explained by considering non-radiative charge-transfer-state decay as electron transfer in the Marcus inverted regime, being facilitated by a common skeletal molecular vibrational mode. Our results suggest an intrinsic link between non-radiative voltage losses and electron-vibration coupling, indicating that these losses are unavoidable. Accordingly, the theoretical upper limit for the power conversion efficiency of single-junction organic solar cells would be reduced to about 25.5% and the optimal optical gap increases to (1.45-1.65) eV, that is, (0.2-0.3) eV higher than for technologies with minimized non-radiative voltage losses. Y1 - 2017 U6 - https://doi.org/10.1038/nenergy.2017.53 SN - 2058-7546 VL - 2 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Hofacker, Andreas A1 - Neher, Dieter T1 - Dispersive and steady-state recombination in organic disordered semiconductors JF - Physical review : B, Condensed matter and materials physics N2 - Charge carrier recombination in organic disordered semiconductors is strongly influenced by the thermalization of charge carriers in the density of states (DOS). Measurements of recombination dynamics, conducted under transient or steady-state conditions, can easily be misinterpreted when a detailed understanding of the interplay of thermalization and recombination is missing. To enable adequate measurement analysis, we solve the multiple-trapping problem for recombining charge carriers and analyze it in the transient and steady excitation paradigm for different DOS distributions. We show that recombination rates measured after pulsed excitation are inherently time dependent since recombination gradually slows down as carriers relax in the DOS. When measuring the recombination order after pulsed excitation, this leads to an apparent high-order recombination at short times. As times goes on, the recombination order approaches an asymptotic value. For the Gaussian and the exponential DOS distributions, this asymptotic value equals the recombination order of the equilibrated system under steady excitation. For a more general DOS distribution, the recombination order can also depend on the carrier density, under both transient and steady-state conditions. We conclude that transient experiments can provide rich information about recombination in and out of equilibrium and the underlying DOS occupation provided that consistent modeling of the system is performed. Y1 - 2017 U6 - https://doi.org/10.1103/PhysRevB.96.245204 SN - 2469-9950 SN - 2469-9969 VL - 96 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Mechau, Norman A1 - Saphiannikova, Marina A1 - Neher, Dieter T1 - Molecular tracer diffusion in thin azobenzene polymer layers JF - Applied physics letters N2 - Translational diffusion of fluorescent tracer molecules in azobenzene polymer layers is studied at different temperatures and under illumination using the method of fluorescence recovery after photobleaching. Diffusion is clearly observed in the dark above the glass transition temperature, while homogeneous illumination at 488 nm and 100 mW/cm(2) does not cause any detectable diffusion of the dye molecules within azobenzene layers. This implies that the viscosity of azobenzene layers remains nearly unchanged under illumination with visible light in the absence of internal or external forces. (c) 2006 American Institute of Physics. Y1 - 2006 U6 - https://doi.org/10.1063/1.2405853 SN - 0003-6951 VL - 89 IS - 25 PB - Elsevier CY - Melville ER - TY - JOUR A1 - Alqahtani, Obaid A1 - Babics, Maxime A1 - Gorenflot, Julien A1 - Savikhin, Victoria A1 - Ferron, Thomas A1 - Balawi, Ahmed H. A1 - Paulke, Andreas A1 - Kan, Zhipeng A1 - Pope, Michael A1 - Clulow, Andrew J. A1 - Wolf, Jannic A1 - Burn, Paul L. A1 - Gentle, Ian R. A1 - Neher, Dieter A1 - Toney, Michael F. A1 - Laquai, Frederic A1 - Beaujuge, Pierre M. A1 - Collins, Brian A. T1 - Mixed Domains Enhance Charge Generation and Extraction in Bulk-Heterojunction Solar Cells with Small-Molecule Donors JF - Advanced energy materials N2 - The interplay between nanomorphology and efficiency of polymer-fullerene bulk-heterojunction (BHJ) solar cells has been the subject of intense research, but the generality of these concepts for small-molecule (SM) BHJs remains unclear. Here, the relation between performance; charge generation, recombination, and extraction dynamics; and nanomorphology achievable with two SM donors benzo[1,2-b:4,5-b]dithiophene-pyrido[3,4-b]-pyrazine BDT(PPTh2)(2), namely SM1 and SM2, differing by their side-chains, are examined as a function of solution additive composition. The results show that the additive 1,8-diiodooctane acts as a plasticizer in the blends, increases domain size, and promotes ordering/crystallinity. Surprisingly, the system with high domain purity (SM1) exhibits both poor exciton harvesting and severe charge trapping, alleviated only slightly with increased crystallinity. In contrast, the system consisting of mixed domains and lower crystallinity (SM2) shows both excellent exciton harvesting and low charge recombination losses. Importantly, the onset of large, pure crystallites in the latter (SM2) system reduces efficiency, pointing to possible differences in the ideal morphologies for SM-based BHJ solar cells compared with polymer-fullerene devices. In polymer-based systems, tie chains between pure polymer crystals establish a continuous charge transport network, whereas SM-based active layers may in some cases require mixed domains that enable both aggregation and charge percolation to the electrodes. KW - charge transport KW - domain purity KW - microscopy KW - mixed domains KW - organic solar cells KW - photovoltaic devices KW - resonant X-ray scattering KW - small molecules KW - transient spectroscopy Y1 - 2018 U6 - https://doi.org/10.1002/aenm.201702941 SN - 1614-6832 SN - 1614-6840 VL - 8 IS - 19 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Liu, Ji-Cai A1 - Ignatova, Nina A1 - Kimberg, Victor A1 - Krasnov, Pavel A1 - Föhlisch, Alexander A1 - Simon, Marc A1 - Gel'mukhanov, Faris T1 - Time-resolved study of recoil-induced rotation by X-ray pump - X-ray probe spectroscopy JF - Physical chemistry, chemical physics : a journal of European Chemical Societies N2 - Modern stationary X-ray spectroscopy is unable to resolve rotational structure. In the present paper, we propose to use time-resolved two color X-ray pump-probe spectroscopy with picosecond resolution for real-time monitoring of the rotational dynamics induced by the recoil effect. The proposed technique consists of two steps. The first short pump X-ray pulse ionizes the valence electron, which transfers angular momentum to the molecule. The second time-delayed short probe X-ray pulse resonantly excites a 1s electron to the created valence hole. Due to the recoil-induced angular momentum the molecule rotates and changes the orientation of transition dipole moment of core-excitation with respect to the transition dipole moment of the valence ionization, which results in a temporal modulation of the probe X-ray absorption as a function of the delay time between the pulses. We developed an accurate theory of the X-ray pump-probe spectroscopy of the recoil-induced rotation and study how the energy of the photoelectron and thermal dephasing affect the structure of the time-dependent X-ray absorption using the CO molecule as a case-study. We also discuss the feasibility of experimental observation of our theoretical findings, opening new perspectives in studies of molecular rotational dynamics. Y1 - 2022 U6 - https://doi.org/10.1039/d1cp05000a SN - 1463-9076 SN - 1463-9084 VL - 24 IS - 11 SP - 6627 EP - 6638 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Voroshnin, Vladimir A1 - Tarasov, Artem V. A1 - Bokai, Kirill A. A1 - Chikina, Alla A1 - Senkovskiy, Boris V. A1 - Ehlen, Niels A1 - Usachov, Dmitry Yu. A1 - Gruneis, Alexander A1 - Krivenkov, Maxim A1 - Sanchez-Barriga, Jaime A1 - Fedorov, Alexander T1 - Direct spectroscopic evidence of magnetic proximity effect in MoS2 monolayer on graphene/Co JF - ACS nano N2 - A magnetic field modifies optical properties and provides valley splitting in a molybdenum disulfide (MoS2) monolayer. Here we demonstrate a scalable approach to the epitaxial synthesis of MoS2 monolayer on a magnetic graphene/Co system. Using spin- and angle-resolved photoemission spectroscopy we observe a magnetic proximity effect that causes a 20 meV spin-splitting at the (Gamma) over bar point and canting of spins at the (K) over bar point in the valence band toward the in-plane direction of cobalt magnetization. Our density functional theory calculations reveal that the in-plane spin component at (K) over bar is localized on Co atoms in the valence band, while in the conduction band it is localized on the MoS2 layer. The calculations also predict a 16 meV spin-splitting at the (Gamma) over bar point and 8 meV (K) over bar-(K) over bar' valley asymmetry for an out-of-plane magnetization. These findings suggest control over optical transitions in MoS2 via Co magnetization. Our estimations show that the magnetic proximity effect is equivalent to the action of the magnetic field as large as 100 T. KW - magnetic proximity effect KW - MoS2 KW - monolayer KW - graphene KW - spin-resolved KW - ARPES Y1 - 2022 U6 - https://doi.org/10.1021/acsnano.1c10391 SN - 1936-0851 SN - 1936-086X VL - 16 IS - 5 SP - 7448 EP - 7456 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Abiuso, Paolo A1 - Holubec, Viktor A1 - Anders, Janet A1 - Ye, Zhuolin A1 - Cerisola, Federico A1 - Perarnau-Llobet, Marti T1 - Thermodynamics and optimal protocols of multidimensional quadratic Brownian systems JF - Journal of physics communications N2 - We characterize finite-time thermodynamic processes of multidimensional quadratic overdamped systems. Analytic expressions are provided for heat, work, and dissipation for any evolution of the system covariance matrix. The Bures-Wasserstein metric between covariance matrices naturally emerges as the local quantifier of dissipation. General principles of how to apply these geometric tools to identify optimal protocols are discussed. Focusing on the relevant slow-driving limit, we show how these results can be used to analyze cases in which the experimental control over the system is partial. KW - stochastic thermodynamics KW - thermodynamic control KW - thermodynamic length KW - overdamped brownian systems Y1 - 2022 U6 - https://doi.org/10.1088/2399-6528/ac72f8 SN - 2399-6528 VL - 6 IS - 6 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Stojkoski, Viktor A1 - Sandev, Trifce A1 - Kocarev, Ljupco A1 - Pal, Arnab T1 - Autocorrelation functions and ergodicity in diffusion with stochastic resetting JF - Journal of physics : A, Mathematical and theoretical N2 - Diffusion with stochastic resetting is a paradigm of resetting processes. Standard renewal or master equation approach are typically used to study steady state and other transport properties such as average, mean squared displacement etc. What remains less explored is the two time point correlation functions whose evaluation is often daunting since it requires the implementation of the exact time dependent probability density functions of the resetting processes which are unknown for most of the problems. We adopt a different approach that allows us to write a stochastic solution for a single trajectory undergoing resetting. Moments and the autocorrelation functions between any two times along the trajectory can then be computed directly using the laws of total expectation. Estimation of autocorrelation functions turns out to be pivotal for investigating the ergodic properties of various observables for this canonical model. In particular, we investigate two observables (i) sample mean which is widely used in economics and (ii) time-averaged-mean-squared-displacement (TAMSD) which is of acute interest in physics. We find that both diffusion and drift-diffusion processes with resetting are ergodic at the mean level unlike their reset-free counterparts. In contrast, resetting renders ergodicity breaking in the TAMSD while both the stochastic processes are ergodic when resetting is absent. We quantify these behaviors with detailed analytical study and corroborate with extensive numerical simulations. Our results can be verified in experimental set-ups that can track single particle trajectories and thus have strong implications in understanding the physics of resetting. KW - autocorrelations KW - ergodicity KW - diffusion KW - stochastic resetting Y1 - 2022 U6 - https://doi.org/10.1088/1751-8121/ac4ce9 SN - 1751-8113 SN - 1751-8121 VL - 55 IS - 10 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Kühn, Danilo A1 - Müller, Moritz A1 - Sorgenfrei, Nomi A1 - Giangrisostomi, Erika A1 - Jay, Raphael Martin A1 - Ovsyannikov, Ruslan A1 - Martensson, Nils A1 - Sanchez-Portal, Daniel A1 - Föhlisch, Alexander T1 - Directional sub-femtosecond charge transfer dynamics and the dimensionality of 1T-TaS2 JF - Scientific reports N2 - For the layered transition metal dichalcogenide 1T-TaS2, we establish through a unique experimental approach and density functional theory, how ultrafast charge transfer in 1T-TaS2 takes on isotropic three-dimensional character or anisotropic two-dimensional character, depending on the commensurability of the charge density wave phases of 1T-TaS2. The X-ray spectroscopic core-hole-clock method prepares selectively in-and out-of-plane polarized sulfur 3p orbital occupation with respect to the 1T-TaS2 planes and monitors sub-femtosecond wave packet delocalization. Despite being a prototypical two-dimensional material, isotropic three-dimensional charge transfer is found in the commensurate charge density wave phase (CCDW), indicating strong coupling between layers. In contrast, anisotropic two-dimensional charge transfer occurs for the nearly commensurate phase (NCDW). In direct comparison, theory shows that interlayer interaction in the CCDW phase - not layer stacking variations - causes isotropic three-dimensional charge transfer. This is presumably a general mechanism for phase transitions and tailored properties of dichalcogenides with charge density waves. Y1 - 2019 U6 - https://doi.org/10.1038/s41598-018-36637-0 SN - 2045-2322 VL - 9 IS - 488 PB - Nature Publ. Group CY - London ER - TY - JOUR A1 - Giangrisostomi, Erika A1 - Ovsyannikov, Ruslan A1 - Sorgenfrei, Nomi A1 - Zhang, Teng A1 - Lindblad, Andreas A1 - Sassa, Yasmine A1 - Cappel, Ute B. A1 - Leitner, Torsten A1 - Mitzner, Rolf A1 - Svensson, Svante A1 - Martensson, Nils A1 - Föhlisch, Alexander T1 - Low Dose Photoelectron Spectroscopy at BESSY II BT - electronic structure of matter in its native state JF - Journal of electron spectroscopy and related phenomena : the international journal on theoretical and experimental aspects of electron spectroscopy N2 - The implementation of a high-transmission, angular-resolved time-of-Right electron spectrometer with a 1.25 MHz pulse selector at the PM4 soft X-ray dipole beamline of the synchrotron BESSY II creates unique capabilities to inquire electronic structure via photoelectron spectroscopy with a minimum of radiation dose. Solid-state samples can be prepared and characterized with standard UHV techniques and rapidly transferred from various preparation chambers to a 4-axis temperature-controlled measurement stage. A synchronized MHz laser system enables excited-state characterization and dynamical studies starting from the picosecond timescale. This article introduces the principal characteristics of the PM4 beamline and LowDosePES end-station. Recent results from graphene, an organic hole transport material for solar cells and the transition metal dichalcogenide MoS2 are presented to demonstrate the instrument performances. Y1 - 2018 U6 - https://doi.org/10.1016/j.elspec.2017.05.011 SN - 0368-2048 SN - 1873-2526 VL - 224 SP - 68 EP - 78 PB - Elsevier CY - Amsterdam ER - TY - JOUR A1 - Pontius, Niko A1 - Beye, Martin A1 - Trabant, Christoph A1 - Mitzner, Rolf A1 - Sorgenfrei, Nomi A1 - Kachel, Torsten A1 - Woestmann, Michael A1 - Roling, Sebastian A1 - Zacharias, Helmut A1 - Ivanov, Rosen A1 - Treusch, Rolf A1 - Buchholz, Marcel A1 - Metcalf, Pete A1 - Schuessler-Langeheine, Christian A1 - Föhlisch, Alexander T1 - Probing the non-equilibrium transient state in magnetite by a jitter-free two-color X-ray pump and X-ray probe experiment JF - Structural dynamics N2 - We present a general experimental concept for jitter-free pump and probe experiments at free electron lasers. By generating pump and probe pulse from one and the same X-ray pulse using an optical split-and-delay unit, we obtain a temporal resolution that is limited only by the X-ray pulse lengths. In a two-color X-ray pump and X-ray probe experiment with sub 70 fs temporal resolution, we selectively probe the response of orbital and charge degree of freedom in the prototypical functional oxide magnetite after photoexcitation. We find electronic order to be quenched on a time scale of (30 +/- 30) fs and hence most likely faster than what is to be expected for any lattice dynamics. Our experimental result hints to the formation of a short lived transient state with decoupled electronic and lattice degree of freedom in magnetite. The excitation and relaxation mechanism for X-ray pumping is discussed within a simple model leading to the conclusion that within the first 10 fs the original photoexcitation decays into low-energy electronic excitations comparable to what is achieved by optical pump pulse excitation. Our findings show on which time scales dynamical decoupling of degrees of freedom in functional oxides can be expected and how to probe this selectively with soft X-ray pulses. Results can be expected to provide crucial information for theories for ultrafast behavior of materials and help to develop concepts for novel switching devices. (C) 2018 Author(s). Y1 - 2018 U6 - https://doi.org/10.1063/1.5042847 SN - 2329-7778 VL - 5 IS - 5 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Kühn, Danilo A1 - Giangrisostomi, Erika A1 - Jay, Raphael Martin A1 - Sorgenfrei, Nomi A1 - Föhlisch, Alexander T1 - The influence of x-ray pulse length on space-charge effects in optical pump/x-ray probe photoemission JF - New journal of physics : the open-access journal for physics N2 - Pump-probe photoelectron spectroscopy (PES) is a versatile tool to investigate the dynamics of transient states of excited matter. Vacuum space-charge effects can mask these dynamics and complicate the interpretation of electron spectra. Here we report on space-charge effects in Au 4f photoemission from a polycrystalline gold surface, excited with moderately intense 90 ps (FWHM) soft x-ray probe pulses, under the influence of the Coulomb forces exerted by a pump electron cloud, which was produced by intense 40 fs laser pulses. The experimentally observed kinetic energy shift and spectral broadening of the Au 4f lines, measured with highly-efficient time-of-flight spectroscopy, are in good agreement with simulations utilizing a mean-field model of the electrostatic pump electron potential. This confirms that the line broadening is predominantly caused by variations in the take-off time of the probe electrons without appreciable influence of local scattering events. Our findings might be of general interest for pump-probe PES with picosecond-pulse-length sources. KW - space-charge effects KW - mean-field model KW - x-ray photoemission KW - electron spectroscopy KW - pump-probe KW - ARTOF Y1 - 2019 U6 - https://doi.org/10.1088/1367-2630/ab2f5c SN - 1367-2630 VL - 21 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Li, Tian-yi A1 - Benduhn, Johannes A1 - Li, Yue A1 - Jaiser, Frank A1 - Spoltore, Donato A1 - Zeika, Olaf A1 - Ma, Zaifei A1 - Neher, Dieter A1 - Vandewal, Koen A1 - Leo, Karl T1 - Boron dipyrromethene (BODIPY) with meso-perfluorinated alkyl substituents as near infrared donors in organic solar cells JF - Journal of materials chemistry : A, Materials for energy and sustainability N2 - Three furan-fused BODIPYs were synthesized with perfluorinated methyl, ethyl and n-propyl groups on the meso-carbon. They were obtained with high yields by reacting the furan-fused 2-carboxylpyrrole in corresponding perfluorinated acid and anhydride. With the increase in perfluorinated alkyl chain length, the molecular packing in the single crystal is influenced, showing increasing stacking distance and decreasing slope angle. All the BODIPYs were characterized as intense absorbers in near infrared region in solid state, peaking at similar to 800 nm with absorption coefficient of over 280 000 cm(-1). Facilitated by high thermal stability, the furan-fused BODIPYs were employed in vacuum-deposited organic solar cells as electron donors. All devices exhibit PCE over 6.0% with the EQE maximum reaching 70% at similar to 790 nm. The chemical modification of the BODIPY donors have certain influence on the active layer morphology, and the highest PCE of 6.4% was obtained with a notably high jsc of 13.6 mA cm(-2). Sensitive EQE and electroluminance studies indicated that the energy losses generated by the formation of a charge transfer state and the radiative recombination at the donor-acceptor interface were comparable in the range of 0.14-0.19 V, while non-radiative recombination energy loss of 0.38 V was the main energy loss route resulting in the moderate V-oc of 0.76 V. Y1 - 2018 U6 - https://doi.org/10.1039/c8ta06261g SN - 2050-7488 SN - 2050-7496 VL - 6 IS - 38 SP - 18583 EP - 18591 PB - Royal Society of Chemistry CY - Cambridge ER - TY - JOUR A1 - Liebig, Ferenc A1 - Sarhan, Radwan Mohamed A1 - Prietzel, Claudia Christina A1 - Thünemann, Andreas F. A1 - Bargheer, Matias A1 - Koetz, Joachim T1 - Undulated Gold Nanoplatelet Superstructures BT - In Situ Growth of Hemispherical Gold Nanoparticles onto the Surface of Gold Nanotriangles JF - Langmuir N2 - Negatively charged flat gold nanotriangles, formed in a vesicular template phase and separated by an AOT-micelle-based depletion flocculation, were reloaded by adding a cationic polyelectrolyte, that is, a hyperbranched polyethylenimine (PEI). Heating the system to 100 degrees C in the presence of a gold chloride solution, the reduction process leads to the formation of gold nanoparticles inside the polymer shell surrounding the nanoplatelets. The gold nanoparticle formation is investigated by UV-vis spectroscopy, small-angle X-ray scattering, and dynamic light scattering measurements in combination with transmission electron microscopy. Spontaneously formed gold clusters in the hyperbranched PEI shell with an absorption maximum at 350 nm grow on the surface of the nanotriangles as hemispherical particles with diameters of similar to 6 nm. High-resolution micrographs show that the hemispherical gold particles are crystallized onto the {111} facets on the bottom and top of the platelet as well as on the edges without a grain boundary. Undulated gold nanoplatelet superstructures with special properties become available, which show a significantly modified performance in SERS-detected photocatalysis regarding both reactivity and enhancement factor. Y1 - 2018 U6 - https://doi.org/10.1021/acs.langmuir.7b02898 SN - 0743-7463 VL - 34 IS - 15 SP - 4584 EP - 4594 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Tchoumba Kwamen, Christelle Larodia A1 - Rössle, Matthias A1 - Leitenberger, Wolfram A1 - Alexe, Marin A1 - Bargheer, Matias T1 - Time-resolved X-ray diffraction study of the structural dynamics in an epitaxial ferroelectric thin Pb(Zr0.2Ti0.8)O-3 film induced by sub-coercive fields JF - Applied physics letters N2 - The electric field-dependence of structural dynamics in a tetragonal ferroelectric lead zirconate titanate thin film is investigated under subcoercive and above-coercive fields using time-resolved X-ray diffraction. The domain nucleation and growth are monitored in real time during the application of an external field to the prepoled thin film capacitor. We propose the observed broadening of the in-plane peak width of the symmetric 002 Bragg reflection as an indicator of the domain disorder and discuss the processes that change the measured peak intensity. Subcoercive field switching results in remnant disordered domain configurations. Published under license by AIP Publishing. Y1 - 2019 U6 - https://doi.org/10.1063/1.5084104 SN - 0003-6951 SN - 1077-3118 VL - 114 IS - 16 PB - American Institute of Physics CY - Melville ER - TY - JOUR A1 - Stete, Felix A1 - Koopman, Wouter-Willem Adriaan A1 - Bargheer, Matias T1 - Signatures of strong coupling on nanoparticles BT - revealing absorption anticrossing by tuning the dielectric environment JF - ACS Photonics N2 - In the strong coupling regime, exciton and plasmon excitations are hybridized into combined system excitations. The correct identification of the coupling regime in these systems is currently debated, from both experimental and theoretical perspectives. In this article we show that the extinction spectra may show a large peak splitting, although the energy loss encoded in the absorption spectra clearly rules out the strong coupling regime. We investigate the coupling of J-aggregate excitons to the localized surface plasmon polaritons on gold nanospheres and nanorods by fine-tuning the plasmon resonance via layer-by-layer deposition of polyelectrolytes. While both structures show a characteristic anticrossing in extinction and scattering experiments, the careful assessment of the systems’ light absorption reveals that strong coupling of the plasmon to the exciton is not present in the nanosphere system. In a phenomenological model of two classical coupled oscillators, a Fano-like regime causes only the resonance of the light-driven oscillator to split up, while the other one still dissipates energy at its original frequency. Only in the strong-coupling limit do both oscillators split up the frequencies at which they dissipate energy, qualitatively explaining our experimental finding. KW - hybrid nanoparticles KW - exciton plasmon coupling KW - layer-by-layer deposition KW - strong coupling KW - absorption measurements Y1 - 2017 U6 - https://doi.org/10.1021/acsphotonics.7b00113 SN - 2330-4022 VL - 4 SP - 1669 EP - 1676 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Mattern, Maximilian A1 - Pudell, Jan-Etienne A1 - Laskin, Gennadii A1 - Reppert, Alexander von A1 - Bargheer, Matias T1 - Analysis of the temperature- and fluence-dependent magnetic stress in laser-excited SrRuO3 JF - Structural dynamics N2 - We use ultrafast x-ray diffraction to investigate the effect of expansive phononic and contractive magnetic stress driving the picosecond strain response of a metallic perovskite SrRuO3 thin film upon femtosecond laser excitation. We exemplify how the anisotropic bulk equilibrium thermal expansion can be used to predict the response of the thin film to ultrafast deposition of energy. It is key to consider that the laterally homogeneous laser excitation changes the strain response compared to the near-equilibrium thermal expansion because the balanced in-plane stresses suppress the Poisson stress on the picosecond timescale. We find a very large negative Grüneisen constant describing the large contractive stress imposed by a small amount of energy in the spin system. The temperature and fluence dependence of the strain response for a double-pulse excitation scheme demonstrates the saturation of the magnetic stress in the high-fluence regime. KW - Thin films KW - Thermodynamic properties KW - Bragg peak KW - Ultrafast X-ray diffraction KW - Thermal effects KW - Phonons KW - Magnetism KW - Lattice dynamics KW - Lasers KW - Perovskites Y1 - 2020 U6 - https://doi.org/10.1063/4.0000072 SN - 2329-7778 VL - 8 IS - 2 PB - AIP Publishing LLC CY - Melville, NY ER - TY - JOUR A1 - Zeuschner, Steffen Peer A1 - Wang, Xi-Guang A1 - Deb, Marwan A1 - Popova, Elena A1 - Malinowski, Gregory A1 - Hehn, Michel A1 - Keller, Niels A1 - Berakdar, Jamal A1 - Bargheer, Matias T1 - Standing spin wave excitation in Bi BT - YIG films via temperature-induced anisotropy changes and magneto-elastic coupling JF - Physical review : B, Condensed matter and materials physics N2 - Based on micromagnetic simulations and experimental observations of the magnetization and lattice dynamics after the direct optical excitation of the magnetic insulator Bi : YIG or indirect excitation via an optically opaque Pt/Cu double layer, we disentangle the dynamical effects of magnetic anisotropy and magneto-elastic coupling. The strain and temperature of the lattice are quantified via modeling ultrafast x-ray diffraction data. Measurements of the time-resolved magneto-optical Kerr effect agree well with the magnetization dynamics simulated according to the excitation via two mechanisms: the magneto-elastic coupling to the experimentally verified strain dynamics and the ultrafast temperature-induced transient change in the magnetic anisotropy. The numerical modeling proves that, for direct excitation, both mechanisms drive the fundamental mode with opposite phase. The relative ratio of standing spin wave amplitudes of higher-order modes indicates that both mechanisms are substantially active. Y1 - 2022 U6 - https://doi.org/10.1103/PhysRevB.106.134401 SN - 2469-9950 SN - 2469-9969 VL - 106 IS - 13 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Liebig, Ferenc A1 - Henning, Ricky A1 - Sarhan, Radwan Mohamed A1 - Prietzel, Claudia Christina A1 - Bargheer, Matias A1 - Koetz, Joachim T1 - A new route to gold nanoflowers JF - Nanotechnology N2 - Catanionic vesicles spontaneously formed by mixing the anionic surfactant bis(2-ethylhexyl)sulfosuccinate sodium salt with the cationic surfactant cetyltrimethylammonium bromide were used as a reducing medium to produce gold clusters, which are embedded and well-ordered into the template phase. The gold clusters can be used as seeds in the growth process that follows by adding ascorbic acid as a mild reducing component. When the ascorbic acid was added very slowly in an ice bath round-edged gold nanoflowers were produced. When the same experiments were performed at room temperature in the presence of Ag+ ions, sharp-edged nanoflowers could be synthesized. The mechanism of nanoparticle formation can be understood to be a non-diffusion-limited Ostwald ripening process of preordered gold nanoparticles embedded in catanionic vesicle fragments. Surface-enhanced Raman scattering experiments show an excellent enhancement factor of 1.7 . 10(5) for the nanoflowers deposited on a silicon wafer. KW - catanionic vesicles KW - gold cluster KW - gold nanoflowers KW - crystal growth KW - HRTEM KW - SEM Y1 - 2018 U6 - https://doi.org/10.1088/1361-6528/aaaffd SN - 0957-4484 SN - 1361-6528 VL - 29 IS - 18 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Pudell, Jan-Etienne A1 - Sander, M. A1 - Bauer, R. A1 - Bargheer, Matias A1 - Herzog, Marc A1 - Gaál, Peter T1 - Full Spatiotemporal Control of Laser-Excited Periodic Surface Deformations JF - Physical review applied N2 - We demonstrate full control of acoustic and thermal periodic deformations at solid surfaces down to subnanosecond time scales and few-micrometer length scales via independent variation of the temporal and spatial phase of two optical transient grating (TG) excitations. For this purpose, we introduce an experimental setup that exerts control of the spatial phase of subsequent time-delayed TG excitations depending on their polarization state. Specific exemplary coherent control cases are discussed theoretically and corresponding experimental data are presented in which time-resolved x-ray reflectivity measures the spatiotemporal surface distortion of nanolayered heterostructures. Finally, we discuss examples where the application of our method may enable the control of functional material properties via tailored spatiotemporal strain fields. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevApplied.12.024036 SN - 2331-7019 VL - 12 IS - 2 PB - American Physical Society CY - College Park ER -