@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} } @article{PenaCamargoThiesbrummelHempeletal.2022, author = {Pena-Camargo, Francisco and Thiesbrummel, Jarla and Hempel, Hannes and Musiienko, Artem and Le Corre, Vincent M. and Diekmann, Jonas and Warby, Jonathan and Unold, Thomas and Lang, Felix and Neher, Dieter and Stolterfoht, Martin}, title = {Revealing the doping density in perovskite solar cells and its impact on device performance}, series = {Applied physics reviews}, volume = {9}, journal = {Applied physics reviews}, number = {2}, publisher = {AIP Publishing}, address = {Melville}, issn = {1931-9401}, doi = {10.1063/5.0085286}, pages = {11}, year = {2022}, abstract = {Traditional inorganic semiconductors can be electronically doped with high precision. Conversely, there is still conjecture regarding the assessment of the electronic doping density in metal-halide perovskites, not to mention of a control thereof. This paper presents a multifaceted approach to determine the electronic doping density for a range of different lead-halide perovskite systems. Optical and electrical characterization techniques, comprising intensity-dependent and transient photoluminescence, AC Hall effect, transfer-length-methods, and charge extraction measurements were instrumental in quantifying an upper limit for the doping density. The obtained values are subsequently compared to the electrode charge per cell volume under short-circuit conditions ( CUbi/eV), which amounts to roughly 10(16) cm(-3). This figure of merit represents the critical limit below which doping-induced charges do not influence the device performance. The experimental results consistently demonstrate that the doping density is below this critical threshold 10(12) cm(-3), which means << CUbi / e V) for all common lead-based metal-halide perovskites. Nevertheless, although the density of doping-induced charges is too low to redistribute the built-in voltage in the perovskite active layer, mobile ions are present in sufficient quantities to create space-charge-regions in the active layer, reminiscent of doped pn-junctions. These results are well supported by drift-diffusion simulations, which confirm that the device performance is not affected by such low doping densities.}, language = {en} } @article{MatternReppertZeuschneretal.2022, author = {Mattern, Maximilian and Reppert, Alexander von and Zeuschner, Steffen Peer and Pudell, Jan-Etienne and K{\"u}hne, F. and Diesing, Detlef and Herzog, Marc and Bargheer, Matias}, title = {Electronic energy transport in nanoscale Au/Fe hetero-structures in the perspective of ultrafast lattice dynamics}, series = {Applied physics letters}, volume = {120}, journal = {Applied physics letters}, number = {9}, publisher = {AIP Publishing}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/5.0080378}, pages = {5}, year = {2022}, abstract = {We study the ultrafast electronic transport of energy in a photoexcited nanoscale Au/Fe hetero-structure by modeling the spatiotemporal profile of energy densities that drives transient strain, which we quantify by femtosecond x-ray diffraction. This flow of energy is relevant for intrinsic demagnetization and ultrafast spin transport. We measured lattice strain for different Fe layer thicknesses ranging from few atomic layers to several nanometers and modeled the spatiotemporal flow of energy densities. The combination of a high electron-phonon coupling coefficient and a large Sommerfeld constant in Fe is found to yield electronic transfer of nearly all energy from Au to Fe within the first hundreds of femtoseconds.}, language = {en} } @article{LeCorreDiekmannPenaCamargoetal.2022, author = {Le Corre, Vincent M. and Diekmann, Jonas and Pe{\~n}a-Camargo, Francisco and Thiesbrummel, Jarla and Tokmoldin, Nurlan and Gutierrez-Partida, Emilio and Peters, Karol Pawel and Perdig{\´o}n-Toro, Lorena and Futscher, Moritz H. and Lang, Felix and Warby, Jonathan and Snaith, Henry J. and Neher, Dieter and Stolterfoht, Martin}, title = {Quantification of efficiency losses due to mobile ions in Perovskite solar cells via fast hysteresis measurements}, series = {Solar RRL}, volume = {6}, journal = {Solar RRL}, number = {4}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {2367-198X}, doi = {10.1002/solr.202100772}, pages = {10}, year = {2022}, abstract = {Perovskite semiconductors differ from most inorganic and organic semiconductors due to the presence of mobile ions in the material. Although the phenomenon is intensively investigated, important questions such as the exact impact of the mobile ions on the steady-state power conversion efficiency (PCE) and stability remain. Herein, a simple method is proposed to estimate the efficiency loss due to mobile ions via "fast-hysteresis" measurements by preventing the perturbation of mobile ions out of their equilibrium position at fast scan speeds (approximate to 1000 V s(-1)). The "ion-free" PCE is between 1\% and 3\% higher than the steady-state PCE, demonstrating the importance of ion-induced losses, even in cells with low levels of hysteresis at typical scan speeds (approximate to 100mv s(-1)). The hysteresis over many orders of magnitude in scan speed provides important information on the effective ion diffusion constant from the peak hysteresis position. The fast-hysteresis measurements are corroborated by transient charge extraction and capacitance measurements and numerical simulations, which confirm the experimental findings and provide important insights into the charge carrier dynamics. The proposed method to quantify PCE losses due to field screening induced by mobile ions clarifies several important experimental observations and opens up a large range of future experiments.}, language = {en} } @article{ZeiskeSandbergZarrabietal.2022, author = {Zeiske, Stefan and Sandberg, Oskar J. and Zarrabi, Nasim and Wolff, Christian Michael and Raoufi, Meysam and Pe{\~n}a-Camargo, Francisco and Gutierrez-Partida, Emilio and Meredith, Paul and Stolterfoht, Martin and Armin, Ardalan}, title = {Static disorder in lead halide perovskites}, series = {The journal of physical chemistry letters}, volume = {13}, journal = {The journal of physical chemistry letters}, number = {31}, publisher = {American Chemical Society}, address = {Washington}, issn = {1948-7185}, doi = {10.1021/acs.jpclett.2c01652}, pages = {7280 -- 7285}, year = {2022}, abstract = {In crystalline and amorphous semiconductors, the temperature-dependent Urbach energy can be determined from the inverse slope of the logarithm of the absorption spectrum and reflects the static and dynamic energetic disorder. Using recent advances in the sensitivity of photocurrent spectroscopy methods, we elucidate the temperature-dependent Urbach energy in lead halide perovskites containing different numbers of cation components. We find Urbach energies at room temperature to be 13.0 +/- 1.0, 13.2 +/- 1.0, and 13.5 +/- 1.0 meV for single, double, and triple cation perovskite. Static, temperature-independent contributions to the Urbach energy are found to be as low as 5.1 ?+/- 0.5, 4.7 +/- 0.3, and 3.3 +/- 0.9 meV for the same systems. Our results suggest that, at a low temperature, the dominant static disorder in perovskites is derived from zero-point phonon energy rather than structural disorder. This is unusual for solution-processed semiconductors but broadens the potential application of perovskites further to quantum electronics and devices.}, language = {en} } @article{MarinBeloquiZhangGuoetal.2022, author = {Marin-Beloqui, Jose and Zhang, Guanran and Guo, Junjun and Shaikh, Jordan and Wohrer, Thibaut and Hosseini, Seyed Mehrdad and Sun, Bowen and Shipp, James and Auty, Alexander J. and Chekulaev, Dimitri and Ye, Jun and Chin, Yi-Chun and Sullivan, Michael B. and Mozer, Attila J. and Kim, Ji-Seon and Shoaee, Safa and Clarke, Tracey M.}, title = {Insight into the origin of trapping in polymer/fullerene blends with a systematic alteration of the fullerene to higher adducts}, series = {Journal of physical chemistry C}, volume = {126}, journal = {Journal of physical chemistry C}, number = {5}, publisher = {American Chemical Society}, address = {Washington}, issn = {1932-7447}, doi = {10.1021/acs.jpcc.1c10378}, pages = {2708 -- 2719}, year = {2022}, abstract = {The bimolecular recombination characteristics of conjugated polymer poly[(4,4'-bis(2-ethylhexyl)dithieno[3,2-b:2',3'-d]silole)-2,6-diyl-alt-(2,5-bis 3-tetradecylthiophen-2-y1 thiazolo 5,4-d thiazole)-2,5diy1] (PDTSiTTz) blended with the fullerene series PC60BM, ICMA, ICBA, and ICTA have been investigated using microsecond and femtosecond transient absorption spectroscopy, in conjunction with electroluminescence measurements and ambient photoemission spectroscopy. The non-Langevin polymer PDTSiTTz allows an inspection of intrinsic bimolecular recombination rates uninhibited by diffusion, while the low oscillator strengths of fullerenes allow polymer features to dominate, and we compare our results to those of the well-known polymer Si-PCPDTBT. Using mu s-TAS, we have shown that the trap -limited decay dynamics of the PDTSiTTz polaron becomes progressively slower across the fullerene series, while those of Si-PCPDTBT are invariant. Electroluminescence measurements showed an unusual double peak in pristine PDTSiTTz, attributed to a low energy intragap charge transfer state, likely interchain in nature. Furthermore, while the pristine PDTSiTTz showed a broad, low-intensity density of states, the ICBA and ICTA blends presented a virtually identical DOS to Si-PCPDTBT and its blends. This has been attributed to a shift from a delocalized, interchain highest occupied molecular orbital (HOMO) in the pristine material to a dithienosilole-centered HOMO in the blends, likely a result of the bulky fullerenes increasing interchain separation. This HOMO localization had a side effect of progressively shifting the polymer HOMO to shallower energies, which was correlated with the observed decrease in bimolecular recombination rate and increased "trap" depth. However, since the density of tail states remained the same, this suggests that the traditional viewpoint of "trapping" being dominated by tail states may not encompass the full picture and that the breadth of the DOS may also have a strong influence on bimolecular recombination.}, language = {en} } @article{MayerLeverPicconietal.2022, author = {Mayer, Dennis and Lever, Fabiano and Picconi, David and Metje, Jan and Ališauskas, Skirmantas and Calegari, Francesca and D{\"u}sterer, Stefan and Ehlert, Christopher and Feifel, Raimund and Niebuhr, Mario and Manschwetus, Bastian and Kuhlmann, Marion and Mazza, Tommaso and Robinson, Matthew Scott and Squibb, Richard James and Trabattoni, Andrea and Wallner, M{\aa}ns and Saalfrank, Peter and Wolf, Thomas J. A. and G{\"u}hr, Markus}, title = {Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy}, series = {Nature Communications}, volume = {13}, journal = {Nature Communications}, publisher = {Springer Nature}, address = {Berlin}, issn = {2041-1723}, doi = {10.1038/s41467-021-27908-y}, pages = {9}, year = {2022}, abstract = {The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The method allows us to discover that a major part of the population relaxes to the molecular ground state within 220-250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states.}, language = {en} } @article{PetrovSingerCoughlinetal.2022, author = {Petrov, Polina and Singer, Leo P. and Coughlin, Michael W. and Kumar, Vishwesh and Almualla, Mouza and Anand, Shreya and Bulla, Mattia and Dietrich, Tim and Foucart, Francois and Guessoum, Nidhal}, title = {Data-driven expectations for electromagnetic counterpart searches based on LIGO/Virgo public alerts}, series = {The astrophysical journal : an international review of spectroscopy and astronomical physics; part 1}, volume = {924}, journal = {The astrophysical journal : an international review of spectroscopy and astronomical physics; part 1}, number = {2}, publisher = {Institute of Physics Publ.}, address = {London}, issn = {1538-4357}, doi = {10.3847/1538-4357/ac366d}, pages = {10}, year = {2022}, abstract = {Searches for electromagnetic counterparts of gravitational-wave signals have redoubled since the first detection in 2017 of a binary neutron star merger with a gamma-ray burst, optical/infrared kilonova, and panchromatic afterglow. Yet, one LIGO/Virgo observing run later, there has not yet been a second, secure identification of an electromagnetic counterpart. This is not surprising given that the localization uncertainties of events in LIGO and Virgo's third observing run, O3, were much larger than predicted. We explain this by showing that improvements in data analysis that now allow LIGO/Virgo to detect weaker and hence more poorly localized events have increased the overall number of detections, of which well-localized, gold-plated events make up a smaller proportion overall. We present simulations of the next two LIGO/Virgo/KAGRA observing runs, O4 and O5, that are grounded in the statistics of O3 public alerts. To illustrate the significant impact that the updated predictions can have, we study the follow-up strategy for the Zwicky Transient Facility. Realistic and timely forecasting of gravitational-wave localization accuracy is paramount given the large commitments of telescope time and the need to prioritize which events are followed up. We include a data release of our simulated localizations as a public proposal planning resource for astronomers.}, language = {en} } @article{PerdigonToroLeQuangPhuongElleretal.2022, author = {Perdig{\´o}n-Toro, Lorena and Le Quang Phuong, and Eller, Fabian and Freychet, Guillaume and Saglamkaya, Elifnaz and Khan, Jafar and Wei, Qingya and Zeiske, Stefan and Kroh, Daniel and Wedler, Stefan and Koehler, Anna and Armin, Ardalan and Laquai, Frederic and Herzig, Eva M. and Zou, Yingping and Shoaee, Safa and Neher, Dieter}, title = {Understanding the role of order in Y-series non-fullerene solar cells to realize high open-circuit voltages}, series = {Advanced energy materials}, volume = {12}, journal = {Advanced energy materials}, number = {12}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1614-6832}, doi = {10.1002/aenm.202103422}, pages = {13}, year = {2022}, abstract = {Non-fullerene acceptors (NFAs) as used in state-of-the-art organic solar cells feature highly crystalline layers that go along with low energetic disorder. Here, the crucial role of energetic disorder in blends of the donor polymer PM6 with two Y-series NFAs, Y6, and N4 is studied. By performing temperature-dependent charge transport and recombination studies, a consistent picture of the shape of the density of state distributions for free charges in the two blends is developed, allowing an analytical description of the dependence of the open-circuit voltage V-OC on temperature and illumination intensity. Disorder is found to influence the value of the V-OC at room temperature, but also its progression with temperature. Here, the PM6:Y6 blend benefits substantially from its narrower state distributions. The analysis also shows that the energy of the equilibrated free charge population is well below the energy of the NFA singlet excitons for both blends and possibly below the energy of the populated charge transfer manifold, indicating a down-hill driving force for free charge formation. It is concluded that energetic disorder of charge-separated states has to be considered in the analysis of the photovoltaic properties, even for the more ordered PM6:Y6 blend.}, language = {en} } @article{DoerriesChechkinSchumeretal.2022, author = {Doerries, Timo J. and Chechkin, Aleksei and Schumer, Rina and Metzler, Ralf}, title = {Rate equations, spatial moments, and concentration profiles for mobile-immobile models with power-law and mixed waiting time distributions}, series = {Physical review : E, Statistical, nonlinear and soft matter physics}, volume = {105}, journal = {Physical review : E, Statistical, nonlinear and soft matter physics}, number = {1}, publisher = {The American Institute of Physics}, address = {Woodbury, NY}, issn = {2470-0045}, doi = {10.1103/PhysRevE.105.014105}, pages = {24}, year = {2022}, abstract = {We present a framework for systems in which diffusion-advection transport of a tracer substance in a mobile zone is interrupted by trapping in an immobile zone. Our model unifies different model approaches based on distributed-order diffusion equations, exciton diffusion rate models, and random-walk models for multirate mobile-immobile mass transport. We study various forms for the trapping time dynamics and their effects on the tracer mass in the mobile zone. Moreover, we find the associated breakthrough curves, the tracer density at a fixed point in space as a function of time, and the mobile and immobile concentration profiles and the respective moments of the transport. Specifically, we derive explicit forms for the anomalous transport dynamics and an asymptotic power-law decay of the mobile mass for a Mittag-Leffler trapping time distribution. In our analysis we point out that even for exponential trapping time densities, transient anomalous transport is observed. Our results have direct applications in geophysical contexts, but also in biological, soft matter, and solid state systems.}, language = {en} }