TY  - JOUR
A1  - Wolf, Thomas J. A.
A1  - Parrish, Robert M.
A1  - Myhre, Rolf H.
A1  - Martinez, Todd J.
A1  - Koch, Henrik
A1  - Gühr, Markus
T1  - Observation of Ultrafast Intersystem Crossing in Thymine by Extreme Ultraviolet Time-Resolved Photoelectron Spectroscopy
JF  - The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment & general theory
N2  - We studied the photoinduced ultrafast relaxation dynamics of the nucleobase thymine using gas-phase time-resolved photoelectron spectroscopy. By employing extreme ultraviolet pulses from high harmonic generation for photoionization, we substantially extend our spectral observation window with respect to previous studies. This enables us to follow relaxation of the excited state population all the way to low-lying electronic states including the ground state. In thymine, we observe relaxation from the optically bright (1)pi pi* state of thymine to a dark (1)n pi* state within 80 +/- 30 fs. The (1)n pi* state relaxes further within 3.5 +/- 0.3 ps to a low-lying electronic state. By comparison with quantum chemical simulations, we can unambiguously assign its spectroscopic signature to the (3)pi pi* state. Hence, our study draws a comprehensive picture of the relaxation mechanism of thymine including ultrafast intersystem crossing to the triplet manifold.
Y1  - 2019
U6  - https://doi.org/10.1021/acs.jpca.9b05573
SN  - 1089-5639
SN  - 1520-5215
VL  - 123
IS  - 32
SP  - 6897
EP  - 6903
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Nikolis, Vasileios C.
A1  - Mischok, Andreas
A1  - Siegmund, Bernhard
A1  - Kublitski, Jonas
A1  - Jia, Xiangkun
A1  - Benduhn, Johannes
A1  - Hörmann, Ulrich
A1  - Neher, Dieter
A1  - Gather, Malte C.
A1  - Spoltore, Donato
A1  - Vandewal, Koen
T1  - Strong light-matter coupling for reduced photon energy losses in organic photovoltaics
JF  - Nature Communications
N2  - Strong light-matter coupling can re-arrange the exciton energies in organic semiconductors. Here, we exploit strong coupling by embedding a fullerene-free organic solar cell (OSC) photo-active layer into an optical microcavity, leading to the formation of polariton peaks and a red-shift of the optical gap. At the same time, the open-circuit voltage of the device remains unaffected. This leads to reduced photon energy losses for the low-energy polaritons and a steepening of the absorption edge. While strong coupling reduces the optical gap, the energy of the charge-transfer state is not affected for large driving force donor-acceptor systems. Interestingly, this implies that strong coupling can be exploited in OSCs to reduce the driving force for electron transfer, without chemical or microstructural modifications of the photoactive layer. Our work demonstrates that the processes determining voltage losses in OSCs can now be tuned, and reduced to unprecedented values, simply by manipulating the device architecture.
Y1  - 2019
U6  - https://doi.org/10.1038/s41467-019-11717-5
SN  - 2041-1723
VL  - 10
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Caprioglio, Pietro
A1  - Wolff, Christian Michael
A1  - Marquez, Jose A.
A1  - Nordmann, Joleik
A1  - Zhang, Shanshan
A1  - Rothhardt, Daniel
A1  - Hörmann, Ulrich
A1  - Amir, Yohai
A1  - Redinger, Alex
A1  - Kegelmann, Lukas
A1  - Zu, Fengshuo
A1  - Albrecht, Steve
A1  - Koch, Norbert
A1  - Kirchartz, Thomas
A1  - Saliba, Michael
A1  - Unold, Thomas
A1  - Neher, Dieter
T1  - The impact of energy alignment and interfacial recombination on the internal and external open-circuit voltage of perovskite solar cells
JF  - Energy & environmental science
N2  - Charge transport layers (CTLs) are key components of diffusion controlled perovskite solar cells, however, they can induce additional non-radiative recombination pathways which limit the open circuit voltage (V-OC) of the cell. In order to realize the full thermodynamic potential of the perovskite absorber, both the electron and hole transport layer (ETL/HTL) need to be as selective as possible. By measuring the photoluminescence yield of perovskite/CTL heterojunctions, we quantify the non-radiative interfacial recombination currents in pin- and nip-type cells including high efficiency devices (21.4%). Our study comprises a wide range of commonly used CTLs, including various hole-transporting polymers, spiro-OMeTAD, metal oxides and fullerenes. We find that all studied CTLs limit the V-OC by inducing an additional non-radiative recombination current that is in most cases substantially larger than the loss in the neat perovskite and that the least-selective interface sets the upper limit for the V-OC of the device. Importantly, the V-OC equals the internal quasi-Fermi level splitting (QFLS) in the absorber layer only in high efficiency cells, while in poor performing devices, the V-OC is substantially lower than the QFLS. Using ultraviolet photoelectron spectroscopy and differential charging capacitance experiments we show that this is due to an energy level mis-alignment at the p-interface. The findings are corroborated by rigorous device simulations which outline important considerations to maximize the V-OC. This work highlights that the challenge to suppress non-radiative recombination losses in perovskite cells on their way to the radiative limit lies in proper energy level alignment and in suppression of defect recombination at the interfaces.
Y1  - 2019
U6  - https://doi.org/10.1039/c9ee02020a
SN  - 1754-5692
SN  - 1754-5706
VL  - 12
IS  - 9
SP  - 2778
EP  - 2788
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  - 
TY  - JOUR
A1  - Le Corre, Vincent M.
A1  - Stolterfoht, Martin
A1  - Perdigón-Toro, Lorena
A1  - Feuerstein, Markus
A1  - Wolff, Christian Michael
A1  - Gil-Escrig, Lidon
A1  - Bolink, Henk J.
A1  - Neher, Dieter
A1  - Koster, L. Jan Anton
T1  - Charge Transport Layers Limiting the Efficiency of Perovskite Solar Cells: How To Optimize Conductivity, Doping, and Thickness
JF  - ACS Applied Energy Materials
N2  - Perovskite solar cells (PSCs) are one of the main research topics of the photovoltaic community; with efficiencies now reaching up to 24%, PSCs are on the way to catching up with classical inorganic solar cells. However, PSCs have not yet reached their full potential. In fact, their efficiency is still limited by nonradiative recombination, mainly via trap-states and by losses due to the poor transport properties of the commonly used transport layers (TLs). Indeed, state-of-the-art TLs (especially if organic) suffer from rather low mobilities, typically within 10(-5) and 10(-2) cm(-2) V-1 s(-1), when compared to the high mobilities, 1-10 cm(-2) V-1 s(-1), measured for perovskites. This work presents a comprehensive analysis of the effect of the mobility, thickness, and doping density of the transport layers based on combined experimental and modeling results of two sets of devices made of a solution-processed high-performing triple-cation (PCE approximate to 20%). The results are also cross-checked on vacuum-processed MAPbI(3) devices. From this analysis, general guidelines on how to optimize a TL are introduced and especially a new and simple formula to easily calculate the amount of doping necessary to counterbalance the low mobility of the TLs.
KW  - perovskite solar cells
KW  - transport layers
KW  - conductivity
KW  - doping
KW  - charge transport
Y1  - 2019
U6  - https://doi.org/10.1021/acsaem.9b00856
SN  - 2574-0962
VL  - 2
IS  - 9
SP  - 6280
EP  - 6287
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Tubiana, C.
A1  - Rinaldi, G.
A1  - Guettler, C.
A1  - Snodgrass, C.
A1  - Shi, X.
A1  - Hu, X.
A1  - Marschall, R.
A1  - Fulle, M.
A1  - Bockeele-Morvan, D.
A1  - Naletto, G.
A1  - Capaccioni, F.
A1  - Sierks, H.
A1  - Arnold, G.
A1  - Barucci, M. A.
A1  - Bertaux, J-L
A1  - Bertini, I
A1  - Bodewits, D.
A1  - Capria, M. T.
A1  - Ciarniello, M.
A1  - Cremonese, G.
A1  - Crovisier, J.
A1  - Da Deppo, V
A1  - Debei, S.
A1  - De Cecco, M.
A1  - Deller, J.
A1  - De Sanctis, M. C.
A1  - Davidsson, B.
A1  - Doose, L.
A1  - Erard, S.
A1  - Filacchione, G.
A1  - Fink, U.
A1  - Formisano, M.
A1  - Fornasier, S.
A1  - Gutierrez, P. J.
A1  - Ip, W-H
A1  - Ivanovski, S.
A1  - Kappel, David
A1  - Keller, H. U.
A1  - Kolokolova, L.
A1  - Koschny, D.
A1  - Krueger, H.
A1  - La Forgia, F.
A1  - Lamy, P. L.
A1  - Lara, L. M.
A1  - Lazzarin, M.
A1  - Levasseur-Regourd, A. C.
A1  - Lin, Z-Y
A1  - Longobardo, A.
A1  - Lopez-Moreno, J. J.
A1  - Marzari, F.
A1  - Migliorini, A.
A1  - Mottola, S.
A1  - Rodrigo, R.
A1  - Taylor, F.
A1  - Toth, I
A1  - Zakharov, V
T1  - Diurnal variation of dust and gas production in comet 67P/Churyumov-Gerasimenko at the inbound equinox as seen by OSIRIS and VIRTIS-M on board Rosetta
JF  - Astronomy and astrophysics : an international weekly journal
N2  - Context. On 27 April 2015, when comet 67P/Churyumov-Gerasimenko was at 1.76 au from the Sun and moving toward perihelion, the OSIRIS and VIRTIS-M instruments on board the Rosetta spacecraft simultaneously observed the evolving dust and gas coma during a complete rotation of the comet. Aims. We aim to characterize the spatial distribution of dust, H2O, and CO2 gas in the inner coma. To do this, we performed a quantitative analysis of the release of dust and gas and compared the observed H2O production rate with the rate we calculated using a thermophysical model. Methods. For this study we selected OSIRIS WAC images at 612 nm (dust) and VIRTIS-M image cubes at 612 nm, 2700 nm (H2O emission band), and 4200 nm (CO2 emission band). We measured the average signal in a circular annulus to study the spatial variation around the comet, and in a sector of the annulus to study temporal variation in the sunward direction with comet rotation, both at a fixed distance of 3.1 km from the comet center. Results. The spatial correlation between dust and water, both coming from the sunlit side of the comet, shows that water is the main driver of dust activity in this time period. The spatial distribution of CO2 is not correlated with water and dust. There is no strong temporal correlation between the dust brightness and water production rate as the comet rotates. The dust brightness shows a peak at 0 degrees subsolar longitude, which is not pronounced in the water production. At the same epoch, there is also a maximum in CO2 production. An excess of measured water production with respect to the value calculated using a simple thermophysical model is observed when the head lobe and regions of the southern hemisphere with strong seasonal variations are illuminated (subsolar longitude 270 degrees-50 degrees). A drastic decrease in dust production when the water production (both measured and from the model) displays a maximum occurs when typical northern consolidated regions are illuminated and the southern hemisphere regions with strong seasonal variations are instead in shadow (subsolar longitude 50 degrees-90 degrees). Possible explanations of these observations are presented and discussed.
KW  - comets: general
KW  - comets: individual: 67P/Churyumov-Gerasimenko
KW  - methods: data analysis
Y1  - 2019
U6  - https://doi.org/10.1051/0004-6361/201834869
SN  - 1432-0746
VL  - 630
PB  - EDP Sciences
CY  - Les Ulis
ER  - 
TY  - JOUR
A1  - Rinaldi, G.
A1  - Formisano, M.
A1  - Kappel, David
A1  - Capaccioni, F.
A1  - Bockelee-Morvan, D.
A1  - Cheng, Y-C
A1  - Vincent, J-B
A1  - Deshapriya, P.
A1  - Arnold, G.
A1  - Capria, M. T.
A1  - Ciarniello, M.
A1  - De Sanctis, M. C.
A1  - Doose, L.
A1  - Erard, S.
A1  - Federico, C.
A1  - Filacchione, G.
A1  - Fink, U.
A1  - Leyrat, C.
A1  - Longobardo, A.
A1  - Magni, G.
A1  - Mighorini, A.
A1  - Mottola, S.
A1  - Naletto, G.
A1  - Raponi, A.
A1  - Taylor, F.
A1  - Tosi, F.
A1  - Tozzi, G. P.
A1  - Salatti, M.
T1  - Analysis of night-side dust activity on comet 67P observed by VIRTIS-M
BT  - a new method to constrain the thermal inertia on the surface
JF  - Astronomy and astrophysics : an international weekly journal
N2  - On 2015 July 18, near perihelion at a heliocentric distance of 1.28 au, the Visible InfraRed Thermal Imaging Spectrometer (VIRTIS-M) on board the Rosetta spacecraft had the opportunity of observing dust activity in the inner coma with a view of the night side (shadowed side) of comet 67P/Churyumov-Gerasimenko. At the time of the measurements we present here, we observe a dust plume that originates on the far side of the nucleus. We are able to identify the approximate location of its source at the boundary between the Hapi and Anuket regions, and we find that it has been in darkness for some hours before the observation. Assuming that this time span is equal to the conductive time scale, we obtain a thermal inertia in the range 25-36 W K-1 m(-2) s(-1/2). These thermal inertia values can be used to verify with a 3D finite-element method (REM) numerical code whether the surface and subsurface temperatures agree with the values found in the literature. We explored three different configurations: (1) a layer of water ice mixed with dust beneath a dust mantle of 5 mm with thermal inertia of 36 J m(-2) K-1 S-0.5 ; (2) the same structure, but with thermal inertia of 100 J m(-2) K-1 S-0.5; (3) an ice-dust mixture that is directly exposed. Of these three configurations, the first seems to be the most reasonable, both for the low thermal inertia and for the agreement with the surface and subsurface temperatures that have been found for the comet 67P/Churyumov-Gerasimenko. The spectral properties of the plume show that the visible dust color ranged from 16 +/- 4.8%/100 nm to 13 +/- 2.6%/100 nm, indicating that this plume has no detectable color gradient. The morphology of the plume can be classified as a narrow jet that has an estimated total ejected mass of between 6 and 19 tons when we assume size distribution indices between -2.5 and -3.
KW  - comets: general
KW  - comets: individual: 67P/Churyumov-Gerasimenko
KW  - infrared: planetary systems
Y1  - 2019
U6  - https://doi.org/10.1051/0004-6361/201834907
SN  - 1432-0746
VL  - 630
PB  - EDP Sciences
CY  - Les Ulis
ER  - 
TY  - JOUR
A1  - Schaffenroth, Veronika
A1  - Barlow, Brad N.
A1  - Geier, Stephan
A1  - Vuckovic, Maja
A1  - Kilkenny, D.
A1  - Wolz, M.
A1  - Kupfer, Thomas
A1  - Heber, Ulrich
A1  - Drechsel, H.
A1  - Kimeswenger, S.
A1  - Marsh, T.
A1  - Wolf, M.
A1  - Pelisoli, Ingrid Domingos
A1  - Freudenthal, Joseph
A1  - Dreizler, S.
A1  - Kreuzer, S.
A1  - Ziegerer, E.
T1  - The EREBOS project: Investigating the effect of substellar and low-mass stellar companions on late stellar evolution Survey, target selection, and atmospheric parameters
JF  - Astronomy and astrophysics : an international weekly journal
N2  - Eclipsing post-common-envelope binaries are highly important for resolving the poorly understood, very short-lived common-envelope phase of stellar evolution. Most hot subdwarfs (sdO/Bs) are the bare helium-burning cores of red giants that have lost almost all of their hydrogen envelope. This mass loss is often triggered by common-envelope interactions with close stellar or even substellar companions. Cool companions to hot subdwarf stars such as late-type stars and brown dwarfs are detectable from characteristic light-curve variations - reflection effects and often eclipses. In the recently published catalog of eclipsing binaries in the Galactic Bulge and in the Asteroid Terrestrial-impact Last Alert System (ATLAS) survey, we discovered 125 new eclipsing systems showing a reflection effect seen by visual inspection of the light curves and using a machine-learning algorithm, in addition to the 36 systems previously discovered by the Optical Gravitational Lesing Experiment (OGLE) team. The Eclipsing Reflection Effect Binaries from Optical Surveys (EREBOS) project aims at analyzing all newly discovered eclipsing binaries of the HW Vir type (hot subdwarf + close, cool companion) based on a spectroscopic and photometric follow up to derive the mass distribution of the companions, constrain the fraction of substellar companions, and determine the minimum mass needed to strip off the red-giant envelope. To constrain the nature of the primary we derived the absolute magnitude and the reduced proper motion of all our targets with the help of the parallaxes and proper motions measured by the Gaia mission and compared those to the Gaia white-dwarf candidate catalog. It was possible to derive the nature of a subset of our targets, for which observed spectra are available, by measuring the atmospheric parameter of the primary, confirming that less than 10% of our systems are not sdO/Bs with cool companions but are white dwarfs or central stars of planetary nebula. This large sample of eclipsing hot subdwarfs with cool companions allowed us to derive a significant period distribution for hot subdwarfs with cool companions for the first time showing that the period distribution is much broader than previously thought and is ideally suited to finding the lowest-mass companions to hot subdwarf stars. The comparison with related binary populations shows that the period distribution of HW Vir systems is very similar to WD+dM systems and central stars of planetary nebula with cool companions. In the future, several new photometric surveys will be carried out, which will further increase the sample of this project, providing the potential to test many aspects of common-envelope theory and binary evolution.
KW  - binaries: eclipsing
KW  - brown dwarfs
KW  - binaries: spectroscopic
KW  - binaries: close
KW  - subdwarfs
KW  - surveys
Y1  - 2019
U6  - https://doi.org/10.1051/0004-6361/201936019
SN  - 1432-0746
VL  - 630
PB  - EDP Sciences
CY  - Les Ulis
ER  - 
TY  - JOUR
A1  - Mehrabi, Pedram
A1  - Schulz, Eike C.
A1  - Dsouza, Raison
A1  - Müller-Werkmeister, Henrike
A1  - Tellkamp, Friedjof
A1  - Miller, R. J. Dwayne
A1  - Pai, Emil F.
T1  - Time-resolved crystallography reveals allosteric communication aligned with molecular breathing
JF  - Science
N2  - A comprehensive understanding of protein function demands correlating structure and dynamic changes. Using time-resolved serial synchrotron crystallography, we visualized half-of-the-sites reactivity and correlated molecular-breathing motions in the enzyme fluoroacetate dehalogenase. Eighteen time points from 30 milliseconds to 30 seconds cover four turnover cycles of the irreversible reaction. They reveal sequential substrate binding, covalent-intermediate formation, setup of a hydrolytic water molecule, and product release. Small structural changes of the protein mold and variations in the number and placement of water molecules accompany the various chemical steps of catalysis. Triggered by enzyme-ligand interactions, these repetitive changes in the protein framework’s dynamics and entropy constitute crucial components of the catalytic machinery.
Y1  - 2019
U6  - https://doi.org/10.1126/science.aaw9904
SN  - 0036-8075
SN  - 1095-9203
VL  - 365
IS  - 6458
SP  - 1167
EP  - 1170
PB  - American Assoc. for the Advancement of Science
CY  - Washington
ER  - 
TY  - JOUR
A1  - Deb, Marwan
A1  - Popova, Elena
A1  - Hehn, Michel
A1  - Keller, Niels
A1  - Petit-Watelot, Sebastien
A1  - Bargheer, Matias
A1  - Mangin, Stephane
A1  - Malinowski, Gregory
T1  - Damping of Standing Spin Waves in Bismuth-Substituted Yttrium Iron Garnet as Seen via the Time-Resolved Magneto-Optical Kerr Effect
JF  - Physical review applied
N2  - We investigate spin-wave resonance modes and their damping in insulating thin films of bismuth-substituted yttrium iron garnet by performing femtosecond magneto-optical pump-probe experiments. For large magnetic fields in the range below the magnetization saturation, we find that the damping of high-order standing spin-wave (SSW) modes is about 40 times lower than that for the fundamental one. The observed phenomenon can be explained by considering different features of magnetic anisotropy and exchange fields that, respectively, define the precession frequency for fundamental and high-order SSWs. These results provide further insight into SSWs in iron garnets and may be exploited in many new photomagnonic devices.
Y1  - 2019
U6  - https://doi.org/10.1103/PhysRevApplied.12.044006
SN  - 2331-7019
VL  - 12
IS  - 4
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Pittarello, Lidia
A1  - Goderis, Steven
A1  - Soens, Bastien
A1  - McKibbin, Seann J.
A1  - Giuli, Gabriele
A1  - Bariselli, Federico
A1  - Dias, Bruno
A1  - Helber, Bernd
A1  - Lepore, Giovanni Orazio
A1  - Vanhaecke, Frank
A1  - Köberl, Christian
A1  - Magin, Thierry E.
A1  - Claeys, Philippe
T1  - Meteoroid atmospheric entry investigated with plasma flow experiments: Petrography and geochemistry of the recovered material
JF  - Icarus : international journal of solar system studies
N2  - Melting experiments attempting to reproduce some of the processes affecting asteroidal and cometary material during atmospheric entry have been performed in a high enthalpy facility. For the first time with the specific experimental setup, the resulting material has been recovered, studied, and compared with natural analogues, focusing on the thermal and redox reactions triggered by interaction between the melt and the atmospheric gases under high temperature and low pressure conditions. Experimental conditions were tested across a range of parameters, such as heat flux, experiment duration, and pressure, using two types of sample holders materials, namely cork and graphite. A basalt served as asteroidal analog and to calibrate the experiments, before melting a H5 ordinary chondrite meteorite. The quenched melt recovered after the experiments has been analyzed by mu-XRF, EDS-SEM, EMPA, LA-ICP-MS, and XANES spectroscopy. The glass formed from the basalt is fairly homogeneous, depleted in highly volatile elements (e.g., Na, K), relatively enriched in moderately siderophile elements (e.g., Co, Ni), and has reached an equilibrium redox state with a lower Fe3+/Fe-tot ratio than that in the starting material. Spherical objects, enriched in SiO2, Na2O and K2O, were observed, inferring condensation from the vaporized material. Despite instantaneous quenching, the melt formed from the ordinary chondrite shows extensive crystallization of mostly olivine and magnetite, the latter indicative of oxygen fugacity compatible with presence of both Fe2+ and Fe3+. Similar features have been observed in natural meteorite fusion crusts and in micrometeorites, implying that, at least in terms of maximum temperature reached and chemical reactions, the experiments have successfully reproduced the conditions likely encountered by extraterrestrial material following atmospheric entry.
KW  - Melting experiments
KW  - Atmospheric entry
KW  - Meteorites
KW  - Fusion crust
KW  - Redox
Y1  - 2019
U6  - https://doi.org/10.1016/j.icarus.2019.04.033
SN  - 0019-1035
SN  - 1090-2643
VL  - 331
SP  - 170
EP  - 178
PB  - Elsevier
CY  - San Diego
ER  -