@article{BrinkmannBeckerZimmermannetal.2022, author = {Brinkmann, Kai Oliver and Becker, Tim and Zimmermann, Florian and Kreusel, Cedric and Gahlmann, Tobias and Theisen, Manuel and Haeger, Tobias and Olthof, Selina and T{\"u}ckmantel, Christian and G{\"u}nster, M. and Maschwitz, Timo and G{\"o}belsmann, Fabian and Koch, Christine and Hertel, Dirk and Caprioglio, Pietro and Pe{\~n}a-Camargo, Francisco and Perdig{\´o}n-Toro, Lorena and Al-Ashouri, Amran and Merten, Lena and Hinderhofer, Alexander and Gomell, Leonie and Zhang, Siyuan and Schreiber, Frank and Albrecht, Steve and Meerholz, Klaus and Neher, Dieter and Stolterfoht, Martin and Riedl, Thomas}, title = {Perovskite-organic tandem solar cells with indium oxide interconnect}, series = {Nature}, volume = {604}, journal = {Nature}, number = {7905}, publisher = {Nature Research}, address = {Berlin}, issn = {0028-0836}, doi = {10.1038/s41586-022-04455-0}, pages = {280 -- 286}, year = {2022}, abstract = {Multijunction solar cells can overcome the fundamental efficiency limits of single-junction devices. The bandgap tunability of metal halide perovskite solar cells renders them attractive for multijunction architectures(1). Combinations with silicon and copper indium gallium selenide (CIGS), as well as all-perovskite tandem cells, have been reported(2-5). Meanwhile, narrow-gap non-fullerene acceptors have unlocked skyrocketing efficiencies for organic solar cells(6,7). Organic and perovskite semiconductors are an attractive combination, sharing similar processing technologies. Currently, perovskite-organic tandems show subpar efficiencies and are limited by the low open-circuit voltage (V-oc) of wide-gap perovskite cells(8) and losses introduced by the interconnect between the subcells(9,10). Here we demonstrate perovskite-organic tandem cells with an efficiency of 24.0 per cent (certified 23.1 per cent) and a high V-oc of 2.15 volts. Optimized charge extraction layers afford perovskite subcells with an outstanding combination of high V-oc and fill factor. The organic subcells provide a high external quantum efficiency in the near-infrared and, in contrast to paradigmatic concerns about limited photostability of non-fullerene cells(11), show an outstanding operational stability if excitons are predominantly generated on the non-fullerene acceptor, which is the case in our tandems. The subcells are connected by an ultrathin (approximately 1.5 nanometres) metal-like indium oxide layer with unprecedented low optical/electrical losses. This work sets a milestone for perovskite-organic tandems, which outperform the best p-i-n perovskite single junctions(12) and are on a par with perovskite-CIGS and all-perovskite multijunctions(13).}, language = {en} } @misc{BullaCoughlinDhawanetal.2022, author = {Bulla, Mattia and Coughlin, Michael W. and Dhawan, Suhail and Dietrich, Tim}, title = {Multi-messenger constraints on the Hubble constant through combination of gravitational waves, gamma-ray bursts and kilonovae from neutron star mergers}, series = {Universe : open access journal}, volume = {8}, journal = {Universe : open access journal}, number = {5}, publisher = {MDPI}, address = {Basel}, issn = {2218-1997}, doi = {10.3390/universe8050289}, pages = {21}, year = {2022}, abstract = {The simultaneous detection of gravitational waves and light from the binary neutron star merger GW170817 led to independent measurements of distance and redshift, providing a direct estimate of the Hubble constant H-0 that does not rely on a cosmic distance ladder, nor assumes a specific cosmological model. By using gravitational waves as "standard sirens", this approach holds promise to arbitrate the existing tension between the H-0 value inferred from the cosmic microwave background and those obtained from local measurements. However, the known degeneracy in the gravitational-wave analysis between distance and inclination of the source led to a H-0 value from GW170817 that was not precise enough to resolve the existing tension. In this review, we summarize recent works exploiting the viewing-angle dependence of the electromagnetic signal, namely the associated short gamma-ray burst and kilonova, to constrain the system inclination and improve on H-0. We outline the key ingredients of the different methods, summarize the results obtained in the aftermath of GW170817 and discuss the possible systematics introduced by each of these methods.}, language = {en} } @phdthesis{Buechner2022, author = {B{\"u}chner, Robby}, title = {Understanding local electronic structure variations in bio-inspired aromatic molecules}, doi = {10.25932/publishup-55319}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-553192}, school = {Universit{\"a}t Potsdam}, pages = {viii, 111}, year = {2022}, abstract = {In this thesis, the dependencies of charge localization and itinerance in two classes of aromatic molecules are accessed: pyridones and porphyrins. The focus lies on the effects of isomerism, complexation, solvation, and optical excitation, which are concomitant with different crucial biological applications of specific members of these groups of compounds. Several porphyrins play key roles in the metabolism of plants and animals. The nucleobases, which store the genetic information in the DNA and RNA are pyridone derivatives. Additionally, a number of vitamins are based on these two groups of substances. This thesis aims to answer the question of how the electronic structure of these classes of molecules is modified, enabling the versatile natural functionality. The resulting insights into the effect of constitutional and external factors are expected to facilitate the design of new processes for medicine, light-harvesting, catalysis, and environmental remediation. The common denominator of pyridones and porphyrins is their aromatic character. As aromaticity was an early-on topic in chemical physics, the overview of relevant theoretical models in this work also mirrors the development of this scientific field in the 20th century. The spectroscopic investigation of these compounds has long been centered on their global, optical transition between frontier orbitals. The utilization and advancement of X-ray spectroscopic methods characterizing the local electronic structure of molecular samples form the core of this thesis. The element selectivity of the near-edge X-ray absorption fine structure (NEXAFS) is employed to probe the unoccupied density of states at the nitrogen site, which is key for the chemical reactivity of pyridones and porphyrins. The results contribute to the growing database of NEXAFS features and their interpretation, e.g., by advancing the debate on the porphyrin N K-edge through systematic experimental and theoretical arguments. Further, a state-of-the-art laser pump - NEXAFS probe scheme is used to characterize the relaxation pathway of a photoexcited porphyrin on the atomic level. Resonant inelastic X-ray scattering (RIXS) provides complementary results by accessing the highest occupied valence levels including symmetry information. It is shown that RIXS is an effective experimental tool to gain detailed information on charge densities of individual species in tautomeric mixtures. Additionally, the hRIXS and METRIXS high-resolution RIXS spectrometers, which have been in part commissioned in the course of this thesis, will gain access to the ultra-fast and thermal chemistry of pyridones, porphyrins, and many other compounds. With respect to both classes of bio-inspired aromatic molecules, this thesis establishes that even though pyridones and porphyrins differ largely by their optical absorption bands and hydrogen bonding abilities, they all share a global stabilization of local constitutional changes and relevant external perturbation. It is because of this wide-ranging response that pyridones and porphyrins can be applied in a manifold of biological and technical processes.}, language = {en} } @article{BuechnerdaCruzGroveretal.2022, author = {B{\"u}chner, Robby and da Cruz, Vinicius Vaz and Grover, Nitika and Charisiadis, Asterios and Fondell, Mattis and Haverkamp, Robert and Senge, Mathias O. and F{\"o}hlisch, Alexander}, title = {Fundamental electronic changes upon intersystem crossing in large aromatic photosensitizers: free base 5,10,15,20-tetrakis(4-carboxylatophenyl)porphyrin}, series = {Physical chemistry, chemical physics : a journal of European Chemical Societies}, volume = {24}, journal = {Physical chemistry, chemical physics : a journal of European Chemical Societies}, number = {12}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {1463-9076}, doi = {10.1039/d1cp05420a}, pages = {7505 -- 7511}, year = {2022}, abstract = {Free base 5,10,15,20-tetrakis(4-carboxylatophenyl)porphyrin stands for the class of powerful porphyrin photosensitizers for singlet oxygen generation and light-harvesting. The atomic level selectivity of dynamic UV pump - N K-edge probe X-ray absorption spectroscopy in combination with time-dependent density functional theory (TD-DFT) gives direct access to the crucial excited molecular states within the unusual relaxation pathway. The efficient intersystem crossing, that is El-Sayed forbidden and not facilitated by a heavy atom is confirmed to be the result of the long singlet excited state lifetime (Q(x) 4.9 ns) and thermal effects. Overall, the interplay of stabilization by conservation of angular momenta and vibronic relaxation drive the de-excitation in these chromophores.}, language = {en} } @misc{CaesarMcCarthyThornalleyetal.2022, author = {Caesar, Levke and McCarthy, Gerard D. and Thornalley, David J. R. and Cahill, Niamh and Rahmstorf, Stefan}, title = {Reply to: Atlantic circulation change still uncertain}, series = {Nature geoscience}, volume = {15}, journal = {Nature geoscience}, number = {3}, publisher = {Nature Publ. Group}, address = {London}, issn = {1752-0894}, doi = {10.1038/s41561-022-00897-3}, pages = {168 -- 170}, year = {2022}, language = {en} } @article{CestnikPikovskij2022, author = {Cestnik, Rok and Pikovskij, Arkadij}, title = {Exact finite-dimensional reduction for a population of noisy oscillators and its link to Ott-Antonsen and Watanabe-Strogatz theories}, series = {Chaos : an interdisciplinary journal of nonlinear science}, volume = {32}, journal = {Chaos : an interdisciplinary journal of nonlinear science}, number = {11}, publisher = {AIP}, address = {Melville}, issn = {1054-1500}, doi = {10.1063/5.0106171}, pages = {15}, year = {2022}, abstract = {Populations of globally coupled phase oscillators are described in the thermodynamic limit by kinetic equations for the distribution densities or, equivalently, by infinite hierarchies of equations for the order parameters. Ott and Antonsen [Chaos 18, 037113 (2008)] have found an invariant finite-dimensional subspace on which the dynamics is described by one complex variable per population. For oscillators with Cauchy distributed frequencies or for those driven by Cauchy white noise, this subspace is weakly stable and, thus, describes the asymptotic dynamics. Here, we report on an exact finite-dimensional reduction of the dynamics outside of the Ott-Antonsen subspace. We show that the evolution from generic initial states can be reduced to that of three complex variables, plus a constant function. For identical noise-free oscillators, this reduction corresponds to the Watanabe-Strogatz system of equations [Watanabe and Strogatz, Phys. Rev. Lett. 70, 2391 (1993)]. We discuss how the reduced system can be used to explore the transient dynamics of perturbed ensembles. Published under an exclusive license by AIP Publishing.}, language = {en} } @article{CestnikPikovsky2022, author = {Cestnik, Rok and Pikovsky, Arkady}, title = {Hierarchy of exact low-dimensional reductions for populations of coupled oscillators}, series = {Physical review letters}, volume = {128}, journal = {Physical review letters}, number = {5}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.128.054101}, pages = {6}, year = {2022}, abstract = {We consider an ensemble of phase oscillators in the thermodynamic limit, where it is described by a kinetic equation for the phase distribution density. We propose an Ansatz for the circular moments of the distribution (Kuramoto-Daido order parameters) that allows for an exact truncation at an arbitrary number of modes. In the simplest case of one mode, the Ansatz coincides with that of Ott and Antonsen [Chaos 18, 037113 (2008)]. Dynamics on the extended manifolds facilitate higher-dimensional behavior such as chaos, which we demonstrate with a simulation of a Josephson junction array. The findings are generalized for oscillators with a Cauchy-Lorentzian distribution of natural frequencies.}, language = {en} } @article{CiarnielloFulleRaponietal.2022, author = {Ciarniello, Mauro and Fulle, Marco and Raponi, Andrea and Filacchione, Gianrico and Capaccioni, Fabrizio and Rotundi, Alessandra and Rinaldi, Giovanna and Formisano, Michelangelo and Magni, Gianfranco and Tosi, Federico and De Sanctis, Maria Cristina and Capria, Maria Teresa and Longobardo, Andrea and Beck, Pierre and Fornasier, Sonia and Kappel, David and Mennella, Vito and Mottola, Stefano and Rousseau, Batiste and Arnold, Gabriele}, title = {Macro and micro structures of pebble-made cometary nuclei reconciled by seasonal evolution}, series = {Nature astronomy}, volume = {6}, journal = {Nature astronomy}, number = {5}, publisher = {Nature Research}, address = {Berlin}, issn = {2397-3366}, doi = {10.1038/s41550-022-01625-y}, pages = {546 -- 553}, year = {2022}, abstract = {Comets evolve due to sublimation of ices embedded inside porous dust, triggering dust emission (that is, erosion) followed by mass loss, mass redistribution and surface modifications. Surface changes were revealed by the Deep Impact and Stardust NExT missions for comet 9P/Tempel 1 (ref.(1)), and a full inventory of the processes modifying cometary nuclei was provided by Rosetta while it escorted comet 67P/Churyumov-Gerasimenko for approximately two years(2-4). Such observations also showed puzzling water-ice-rich spots that stood out as patches optically brighter and spectrally bluer than the average cometary surfaces(5-9). These are up to tens of metres large and indicate macroscopic compositional dishomogeneities apparently in contrast with the structural homogeneity above centimetre scales of pebble-made nuclei(10). Here we show that the occurrence of blue patches determines the seasonal variability of the nucleus colour(4,11,12) and gives insight into the internal structure of comets. We define a new model that links the centimetre-sized pebbles composing the nucleus(10) and driving cometary activity(13,14) to metre-sized water-ice-enriched blocks embedded in a drier matrix. The emergence of blue patches is due to the matrix erosion driven by CO2-ice sublimation that exposes the water-ice-enriched blocks, which in turn are eroded by water-ice sublimation when exposed to sunlight. Our model explains the observed seasonal evolution of the nucleus and reconciles the available data at micro (sub-centimetre) and macro (metre) scales.}, language = {en} } @article{ClarkFreyseYashinaetal.2022, author = {Clark, Oliver J. and Freyse, Friedrich and Yashina, L. V. and Rader, Oliver and Sanchez-Barriga, Jaime}, title = {Robust behavior and spin-texture stability of the topological surface state in Bi2Se3 upon deposition of gold}, series = {npj quantum materials}, volume = {7}, journal = {npj quantum materials}, number = {1}, publisher = {Nature Publishing Group}, address = {London}, issn = {2397-4648}, doi = {10.1038/s41535-022-00443-9}, pages = {7}, year = {2022}, abstract = {The Dirac point of a topological surface state (TSS) is protected against gapping by time-reversal symmetry. Conventional wisdom stipulates, therefore, that only through magnetisation may a TSS become gapped. However, non-magnetic gaps have now been demonstrated in Bi2Se3 systems doped with Mn or In, explained by hybridisation of the Dirac cone with induced impurity resonances. Recent photoemission experiments suggest that an analogous mechanism applies even when Bi2Se3 is surface dosed with Au. Here, we perform a systematic spin- and angle-resolved photoemission study of Au-dosed Bi2Se3. Although there are experimental conditions wherein the TSS appears gapped due to unfavourable photoemission matrix elements, our photon-energy-dependent spectra unambiguously demonstrate the robustness of the Dirac cone against high Au coverage. We further show how the spin textures of the TSS and its accompanying surface resonances remain qualitatively unchanged following Au deposition, and discuss the mechanism underlying the suppression of the spectral weight.}, language = {en} } @article{ClarkWadgaonkarFreyseetal.2022, author = {Clark, Oliver J. and Wadgaonkar, Indrajit and Freyse, Friedrich and Springholz, Gunther and Battiato, Marco and Sanchez-Barriga, Jaime}, title = {Ultrafast thermalization pathways of excited bulk and surface states in the ferroelectric rashba semiconductor GeTe}, series = {Advanced materials}, volume = {34}, journal = {Advanced materials}, number = {24}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {0935-9648}, doi = {10.1002/adma.202200323}, pages = {13}, year = {2022}, abstract = {A large Rashba effect is essential for future applications in spintronics. Particularly attractive is understanding and controlling nonequilibrium properties of ferroelectric Rashba semiconductors. Here, time- and angle-resolved photoemission is utilized to access the ultrafast dynamics of bulk and surface transient Rashba states after femtosecond optical excitation of GeTe. A complex thermalization pathway is observed, wherein three different timescales can be clearly distinguished: intraband thermalization, interband equilibration, and electronic cooling. These dynamics exhibit an unconventional temperature dependence: while the cooling phase speeds up with increasing sample temperature, the opposite happens for interband thermalization. It is demonstrated how, due to the Rashba effect, an interdependence of these timescales on the relative strength of both electron-electron and electron-phonon interactions is responsible for the counterintuitive temperature dependence, with spin-selection constrained interband electron-electron scatterings found both to dominate dynamics away from the Fermi level, and to weaken with increasing temperature. These findings are supported by theoretical calculations within the Boltzmann approach explicitly showing the opposite behavior of all relevant electron-electron and electron-phonon scattering channels with temperature, thus confirming the microscopic mechanism of the experimental findings. The present results are important for future applications of ferroelectric Rashba semiconductors and their excitations in ultrafast spintronics.}, language = {en} }