TY  - JOUR
A1  - Jiang, Wei
A1  - Tao, Chen
A1  - Stolterfoht, Martin
A1  - Jin, Hui
A1  - Stephen, Meera
A1  - Lin, Qianqian
A1  - Nagiri, Ravi C. R.
A1  - Burn, Paul L.
A1  - Gentle, Ian R.
T1  - Hole-transporting materials for low donor content organic solar cells
BT  - charge transport and device performance
JF  - Organic electronics : physics, materials and applications
N2  - Low donor content solar cells are an intriguing class of photovoltaic device about which there is still considerable discussion with respect to their mode of operation. We have synthesized a series of triphenylamine-based materials for use in low donor content devices with the electron accepting [6,6]-phenyl-C71-butyric acid methyl ester (PC(7)0BM). The triphenylamine-based materials absorb light in the near UV enabling the PC(7)0BM to be be the main light absorbing organic semiconducting material in the solar cell. It was found that the devices did not operate as classical Schottky junctions but rather photocurrent was generated by hole transfer from the photo-excited PC(7)0BM to the triphenylamine-based donors. We found that replacing the methoxy surface groups with methyl groups on the donor material led to a decrease in hole mobility for the neat films, which was due to the methyl substituted materials having the propensity to aggregate. The thermodynamic drive to aggregate was advantageous for the performance of the low donor content (6 wt%) films. It was found that the 6 wt% donor devices generally gave higher performance than devices containing 50 wt% of the donor.
KW  - photoexcited hole transfer
KW  - photocurrent generation
KW  - synthesis
KW  - hole
KW  - mobility
KW  - low donor content
KW  - Schottky junction
Y1  - 2020
U6  - https://doi.org/10.1016/j.orgel.2019.105480
SN  - 1566-1199
SN  - 1878-5530
VL  - 76
PB  - Elsevier
CY  - Amsterdam
ER  - 
TY  - JOUR
A1  - Kirchartz, Thomas
A1  - Márquez, José A.
A1  - Stolterfoht, Martin
A1  - Unold, Thomas
T1  - Photoluminescence-based characterization of halide perovskites for photovoltaics
JF  - Advanced Energy Materials
N2  - Photoluminescence spectroscopy is a widely applied characterization technique for semiconductor materials in general and halide perovskite solar cell materials in particular. It can give direct information on the recombination kinetics and processes as well as the internal electrochemical potential of free charge carriers in single semiconductor layers, layer stacks with transport layers, and complete solar cells. The correct evaluation and interpretation of photoluminescence requires the consideration of proper excitation conditions, calibration and application of the appropriate approximations to the rather complex theory, which includes radiative recombination, non-radiative recombination, interface recombination, charge transfer, and photon recycling. In this article, an overview is given of the theory and application to specific halide perovskite compositions, illustrating the variables that should be considered when applying photoluminescence analysis in these materials.
KW  - metal halide perovskites
KW  - numerical simulations
KW  - photoluminescence
KW  - photon recycling
Y1  - 2020
U6  - https://doi.org/10.1002/aenm.201904134
SN  - 1614-6832
SN  - 1614-6840
VL  - 10
IS  - 26
SP  - 1
EP  - 21
PB  - Wiley
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Yazmaciyan, Aren
A1  - Stolterfoht, Martin
A1  - Burn, Paul L.
A1  - Lin, Qianqian
A1  - Meredith, Paul
A1  - Armin, Ardalan
T1  - Recombination losses above and below the transport percolation threshold in bulk heterojunction organic solar cells
JF  - Advanced energy materials
N2  - Achieving the highest power conversion efficiencies in bulk heterojunction organic solar cells requires a morphology that delivers electron and hole percolation pathways for optimized transport, plus sufficient donor:acceptor contact area for near unity charge transfer state formation. This is a significant structural challenge, particularly in semiconducting polymer:fullerene systems. This balancing act in the model high efficiency PTB7:PC70BM blend is studied by tuning the donor:acceptor ratio, with a view to understanding the recombination loss mechanisms above and below the fullerene transport percolation threshold. The internal quantum efficiency is found to be strongly correlated to the slower carrier mobility in agreement with other recent studies. Furthermore, second-order recombination losses dominate the shape of the current density-voltage curve in efficient blend combinations, where the fullerene phase is percolated. However, below the charge transport percolation threshold, there is an electric-field dependence of first-order losses, which includes electric-field-dependent photogeneration. In the intermediate regime, the fill factor appears to be limited by both first- and second-order losses. These findings provide additional basic understanding of the interplay between the bulk heterojunction morphology and the order of recombination in organic solar cells. They also shed light on the limitations of widely used transport models below the percolation threshold.
KW  - bulk heterojunctions
KW  - charge transport
KW  - organic solar cells
KW  - percolation threshold
KW  - recombination losses
Y1  - 2018
U6  - https://doi.org/10.1002/aenm.201703339
SN  - 1614-6832
SN  - 1614-6840
VL  - 8
IS  - 18
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Wolff, Christian Michael
A1  - Amir, Yohai
A1  - Paulke, Andreas
A1  - Perdigón-Toro, Lorena
A1  - Caprioglio, Pietro
A1  - Neher, Dieter
T1  - Approaching the fill factor Shockley-Queisser limit in stable, dopant-free triple cation perovskite solar cells
JF  - Energy & Environmental Science
N2  - Perovskite solar cells now compete with their inorganic counterparts in terms of power conversion efficiency, not least because of their small open-circuit voltage (V-OC) losses. A key to surpass traditional thin-film solar cells is the fill factor (FF). Therefore, more insights into the physical mechanisms that define the bias dependence of the photocurrent are urgently required. In this work, we studied charge extraction and recombination in efficient triple cation perovskite solar cells with undoped organic electron/hole transport layers (ETL/HTL). Using integral time of flight we identify the transit time through the HTL as the key figure of merit for maximizing the fill factor (FF) and efficiency. Complementarily, intensity dependent photocurrent and V-OC measurements elucidate the role of the HTL on the bias dependence of non-radiative and transport-related loss channels. We show that charge transport losses can be completely avoided under certain conditions, yielding devices with FFs of up to 84%. Optimized cells exhibit power conversion efficiencies of above 20% for 6 mm(2) sized pixels and 18.9% for a device area of 1 cm(2). These are record efficiencies for hybrid perovskite devices with dopant-free transport layers, highlighting the potential of this device technology to avoid charge-transport limitations and to approach the Shockley-Queisser limit.
Y1  - 2017
U6  - https://doi.org/10.1039/c7ee00899f
SN  - 1754-5692
SN  - 1754-5706
VL  - 10
SP  - 1530
EP  - 1539
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  - 
TY  - JOUR
A1  - Wang, Qiong
A1  - Smith, Joel A.
A1  - Skroblin, Dieter
A1  - Steele, Julian A.
A1  - Wolff, Christian Michael
A1  - Caprioglio, Pietro
A1  - Stolterfoht, Martin
A1  - Köbler, Hans
A1  - Turren-Cruz, Silver-Hamill
A1  - Li, Meng
A1  - Gollwitzer, Christian
A1  - Neher, Dieter
A1  - Abate, Antonio
T1  - Managing phase purities and crystal orientation for high-performance and photostable cesium lead halide perovskite solar cells
JF  - Solar RRL
N2  - Inorganic perovskites with cesium (Cs+) as the cation have great potential as photovoltaic materials if their phase purity and stability can be addressed. Herein, a series of inorganic perovskites is studied, and it is found that the power conversion efficiency of solar cells with compositions CsPbI1.8Br1.2, CsPbI2.0Br1.0, and CsPbI2.2Br0.8 exhibits a high dependence on the initial annealing step that is found to significantly affect the crystallization and texture behavior of the final perovskite film. At its optimized annealing temperature, CsPbI1.8Br1.2 exhibits a pure orthorhombic phase and only one crystal orientation of the (110) plane. Consequently, this allows for the best efficiency of up to 14.6% and the longest operational lifetime, T-S80, of approximate to 300 h, averaged of over six solar cells, during the maximum power point tracking measurement under continuous light illumination and nitrogen atmosphere. This work provides essential progress on the enhancement of photovoltaic performance and stability of CsPbI3 - xBrx perovskite solar cells.
KW  - cesium lead halides
KW  - crystal orientation
KW  - inorganic perovskites
KW  - ISOS-L-1I protocol
KW  - phase purity
KW  - photostability
Y1  - 2020
VL  - 4
IS  - 9
PB  - WILEY-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Lang, Felix
T1  - All-perovskite tandems get flexible
JF  - Nature energy
N2  - Flexible all-perovskite tandem photovoltaics open up new opportunities for application compared to rigid devices, yet their performance lags behind. Now, researchers show that molecule-bridged interfaces mitigate charge recombination and crack formation, improving the efficiency and mechanical reliability of flexible devices.
Y1  - 2022
U6  - https://doi.org/10.1038/s41560-022-01087-6
SN  - 2058-7546
VL  - 7
IS  - 8
SP  - 688
EP  - 689
PB  - Nature Publishing Group
CY  - London
ER  - 
TY  - JOUR
A1  - Pisoni, Stefano
A1  - Stolterfoht, Martin
A1  - Lockinger, Johannes
A1  - Moser, Thierry
A1  - Jiang, Yan
A1  - Caprioglio, Pietro
A1  - Neher, Dieter
A1  - Buecheler, Stephan
A1  - Tiwari, Ayodhya N.
T1  - On the origin of open-circuit voltage losses in flexible n-i-p perovskite solar cells
JF  - Science and technology of advanced materials : STAM
N2  - The possibility to manufacture perovskite solar cells (PSCs) at low temperatures paves the way to flexible and lightweight photovoltaic (PV) devices manufactured via high-throughput roll-to-roll processes. In order to achieve higher power conversion efficiencies, it is necessary to approach the radiative limit via suppression of non-radiative recombination losses. Herein, we performed a systematic voltage loss analysis for a typical low-temperature processed, flexible PSC in n-i-p configuration using vacuum deposited C-60 as electron transport layer (ETL) and two-step hybrid vacuum-solution deposition for CH3NH3PbI3 perovskite absorber. We identified the ETL/absorber interface as a bottleneck in relation to non-radiative recombination losses, the quasi-Fermi level splitting (QFLS) decreases from similar to 1.23 eV for the bare absorber, just similar to 90 meV below the radiative limit, to similar to 1.10 eV when C-60 is used as ETL. To effectively mitigate these voltage losses, we investigated different interfacial modifications via vacuum deposited interlayers (BCP, B4PyMPM, 3TPYMB, and LiF). An improvement in QFLS of similar to 30-40 meV is observed after interlayer deposition and confirmed by comparable improvements in the open-circuit voltage after implementation of these interfacial modifications in flexible PSCs. Further investigations on absorber/hole transport layer (HTL) interface point out the detrimental role of dopants in Spiro-OMeTAD film (widely employed HTL in the community) as recombination centers upon oxidation and light exposure. [GRAPHICS] .
KW  - Perovskite solar cell
KW  - flexible
KW  - interface engineering
KW  - non-radiative recombination
KW  - quasi-Fermi level splitting
Y1  - 2019
U6  - https://doi.org/10.1080/14686996.2019.1633952
SN  - 1468-6996
SN  - 1878-5514
VL  - 20
SP  - 786
EP  - 795
PB  - Taylor & Francis
CY  - Abingdon
ER  - 
TY  - JOUR
A1  - Samson, Stephanie
A1  - Rech, Jeromy
A1  - Perdigón-Toro, Lorena
A1  - Peng, Zhengxing
A1  - Shoaee, Safa
A1  - Ade, Harald
A1  - Neher, Dieter
A1  - Stolterfoht, Martin
A1  - You, Wei
T1  - Organic solar cells with large insensitivity to donor polymer molar mass across all acceptor classes
JF  - ACS applied polymer materials
N2  - Donor polymer number-average molar mass (M-n) has long been known to influence organic photovoltaic (OPV) performance via changes in both the polymer properties and the resulting bulk heterojunction morphology. The exact nature of these M-n effects varies from system to system, although there is generally some intermediate M-n that results in optimal performance. Interestingly, our earlier work with the difluorobenzotriazole (FTAZ)-based donor polymer, paired with either N2200 (polymer acceptor) or PC61BM (fullerene acceptor), PcBm demonstrated <10% variation in power conversion efficiency and a consistent morphology over a large span of M-n (30 kg/mol to over 100 kg/mol). Would such insensitivity to polymer M-n still hold true when prevailing small molecular acceptors were used with FTAZ? To answer this question, we explored the impact of FTAZ on OPVs with ITIC, a high-performance small-molecule fused-ring electron acceptor (FREA). By probing the photovoltaic characteristics of the resulting OPVs, we show that a similar FTAZ mn insensitivity is also found in the FTAZ:ITIC system. This study highlights a single-donor polymer which, when paired with an archetypal fullerene, polymer, and FREA, results in systems that are largely insensitive to donor M. Our results may have implications in polymer batch-to-batch reproducibility, in particular, relaxing the need for tight M-n control during synthesis.
KW  - polymer solar cells
KW  - conjugated polymers
KW  - fullerenes
KW  - fluorination
KW  - molecular weight
KW  - non-fullerene acceptors
KW  - power conversion efficiency
Y1  - 2020
U6  - https://doi.org/10.1021/acsapm.0c01041
SN  - 2637-6105
VL  - 2
IS  - 11
SP  - 5300
EP  - 5308
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Le Corre, Vincent M.
A1  - Feuerstein, Markus
A1  - Caprioglio, Pietro
A1  - Koster, Lambert Jan Anton
A1  - Neher, Dieter
T1  - Voltage-Dependent Photoluminescence and How It Correlates with the Fill Factor and Open-Circuit Voltage in Perovskite Solar Cells
JF  - Acs energy letters
N2  - Optimizing the photoluminescence (PL) yield of a solar cell has long been recognized as a key principle to maximize the power conversion efficiency. While PL measurements are routinely applied to perovskite films and solar cells under open circuit conditions (V-OC), it remains unclear how the emission depends on the applied voltage. Here, we performed PL(V) measurements on perovskite cells with different hole transport layer thicknesses and doping concentrations, resulting in remarkably different fill factors (FFs). The results reveal that PL(V) mirrors the current-voltage (JV) characteristics in the power-generating regime, which highlights an interesting correlation between radiative and nonradiative recombination losses. In particular, high FF devices show a rapid quenching of PL(V) from open-circuit to the maximum power point. We conclude that, while the PL has to be maximized at V-OC at lower biases < V-OC the PL must be rapidly quenched as charges need to be extracted prior to recombination.
Y1  - 2019
U6  - https://doi.org/10.1021/acsenergylett.9b02262
SN  - 2380-8195
VL  - 4
IS  - 12
SP  - 2887
EP  - 2892
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Zhang, Shanshan
A1  - Stolterfoht, Martin
A1  - Armin, Ardalan
A1  - Lin, Qianqian
A1  - Zu, Fengshuo
A1  - Sobus, Jan
A1  - Jin, Hui
A1  - Koch, Norbert
A1  - Meredith, Paul
A1  - Burn, Paul L.
A1  - Neher, Dieter
T1  - Interface Engineering of Solution-Processed Hybrid Organohalide Perovskite Solar Cells
JF  - ACS applied materials & interfaces
N2  - Engineering the interface between the perovskite absorber and the charge-transporting layers has become an important method for improving the charge extraction and open-circuit voltage (V-OC) of hybrid perovskite solar cells. Conjugated polymers are particularly suited to form the hole-transporting layer, but their hydrophobicity renders it difficult to solution-process the perovskite absorber on top. Herein, oxygen plasma treatment is introduced as a simple means to change the surface energy and work function of hydrophobic polymer interlayers for use as p-contacts in perovskite solar cells. We find that upon oxygen plasma treatment, the hydrophobic surfaces of different prototypical p-type polymers became sufficiently hydrophilic to enable subsequent perovskite junction processing. In addition, the oxygen plasma treatment also increased the ionization potential of the polymer such that it became closer to the valance band energy of the perovskite. It was also found that the oxygen plasma treatment could increase the electrical conductivity of the p-type polymers, facilitating more efficient charge extraction. On the basis of this concept, inverted MAPbI(3) perovskite devices with different oxygen plasma-treated polymers such as P3HT, P3OT, polyTPD, or PTAA were fabricated with power conversion efficiencies of up to 19%.
KW  - organohalide lead perovskites
KW  - solar cells
KW  - surface wetting
KW  - work function
KW  - oxygen plasma
KW  - transport layer
Y1  - 2018
U6  - https://doi.org/10.1021/acsami.8b02503
SN  - 1944-8244
VL  - 10
IS  - 25
SP  - 21681
EP  - 21687
PB  - American Chemical Society
CY  - Washington
ER  - 
TY  - JOUR
A1  - Stolterfoht, Martin
A1  - Wolff, Christian Michael
A1  - Marquez, Jose A.
A1  - Zhang, Shanshan
A1  - Hages, Charles J.
A1  - Rothhardt, Daniel
A1  - Albrecht, Steve
A1  - Burn, Paul L.
A1  - Meredith, Paul
A1  - Unold, Thomas
A1  - Neher, Dieter
T1  - Visualization and suppression of interfacial recombination for high-efficiency large-area pin perovskite solar cells
JF  - Nature Energy
N2  - The performance of perovskite solar cells is predominantly limited by non-radiative recombination, either through trap-assisted recombination in the absorber layer or via minority carrier recombination at the perovskite/transport layer interfaces. Here, we use transient and absolute photoluminescence imaging to visualize all non-radiative recombination pathways in planar pintype perovskite solar cells with undoped organic charge transport layers. We find significant quasi-Fermi-level splitting losses (135 meV) in the perovskite bulk, whereas interfacial recombination results in an additional free energy loss of 80 meV at each individual interface, which limits the open-circuit voltage (V-oc) of the complete cell to similar to 1.12 V. Inserting ultrathin interlayers between the perovskite and transport layers leads to a substantial reduction of these interfacial losses at both the p and n contacts. Using this knowledge and approach, we demonstrate reproducible dopant-free 1 cm(2) perovskite solar cells surpassing 20% efficiency (19.83% certified) with stabilized power output, a high V-oc (1.17 V) and record fill factor (>81%).
KW  - Energy science and technology
KW  - Solar cells
Y1  - 2018
U6  - https://doi.org/10.1038/s41560-018-0219-8
SN  - 2058-7546
VL  - 3
IS  - 10
SP  - 847
EP  - 854
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Schulze, Patricia S. C.
A1  - Bett, Alexander J.
A1  - Bivour, Martin
A1  - Caprioglio, Pietro
A1  - Gerspacher, Fabian M.
A1  - Kabaklı, Özde Ş.
A1  - Richter, Armin
A1  - Stolterfoht, Martin
A1  - Zhang, Qinxin
A1  - Neher, Dieter
A1  - Hermle, Martin
A1  - Hillebrecht, Harald
A1  - Glunz, Stefan W.
A1  - Goldschmidt, Jan Christoph
T1  - 25.1% high-efficiency monolithic perovskite silicon tandem solar cell with a high bandgap perovskite absorber
JF  - Solar RRL
N2  - Monolithic perovskite silicon tandem solar cells can overcome the theoretical efficiency limit of silicon solar cells. This requires an optimum bandgap, high quantum efficiency, and high stability of the perovskite. Herein, a silicon heterojunction bottom cell is combined with a perovskite top cell, with an optimum bandgap of 1.68 eV in planar p-i-n tandem configuration. A methylammonium-free FA(0.75)Cs(0.25)Pb(I0.8Br0.2)(3) perovskite with high Cs content is investigated for improved stability. A 10% molarity increase to 1.1 m of the perovskite precursor solution results in approximate to 75 nm thicker absorber layers and 0.7 mA cm(-2) higher short-circuit current density. With the optimized absorber, tandem devices reach a high fill factor of 80% and up to 25.1% certified efficiency. The unencapsulated tandem device shows an efficiency improvement of 2.3% (absolute) over 5 months, showing the robustness of the absorber against degradation. Moreover, a photoluminescence quantum yield analysis reveals that with adapted charge transport materials and surface passivation, along with improved antireflection measures, the high bandgap perovskite absorber has the potential for 30% tandem efficiency in the near future.
KW  - heterojunction silicon solar cells
KW  - interfaces
KW  - perovskite solar cells
KW  - tandem solar cells
KW  - thin films
Y1  - 2020
VL  - 4
IS  - 7
PB  - John Wiley & Sons, Inc.
CY  - New Jersey
ER  - 
TY  - JOUR
A1  - Zu, Fengshuo
A1  - Warby, Jonathan
A1  - Stolterfoht, Martin
A1  - Li, Jinzhao
A1  - Shin, Dongguen
A1  - Unger, Eva
A1  - Koch, Norbert
T1  - Photoinduced energy-level realignment at interfaces between organic semiconductors and metal-halide perovskites
JF  - Physical review letters
N2  - In contrast to the common conception that the interfacial energy-level alignment is affixed once the interface is formed, we demonstrate that heterojunctions between organic semiconductors and metal-halide perovskites exhibit huge energy-level realignment during photoexcitation. Importantly, the photoinduced level shifts occur in the organic component, including the first molecular layer in direct contact with the perovskite. This is caused by charge-carrier accumulation within the organic semiconductor under illumination and the weak electronic coupling between the junction components.
Y1  - 2021
U6  - https://doi.org/10.1103/PhysRevLett.127.246401
SN  - 0031-9007
SN  - 1079-7114
VL  - 127
IS  - 24
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Raoufi, Meysam
A1  - Hörmann, Ulrich
A1  - Ligorio, Giovanni
A1  - Hildebrandt, Jana
A1  - Pätzel, Michael
A1  - Schultz, Thorsten
A1  - Perdigón-Toro, Lorena
A1  - Koch, Norbert
A1  - List-Kratochvil, Emil
A1  - Hecht, Stefan
A1  - Neher, Dieter
T1  - Simultaneous effect of ultraviolet radiation and surface modification on the work function and hole injection properties of ZnO thin films
JF  - Physica Status Solidi.  A , Applications and materials science
N2  - The combined effect of ultraviolet (UV) light soaking and self-assembled monolayer deposition on the work function (WF) of thin ZnO layers and on the efficiency of hole injection into the prototypical conjugated polymer poly(3-hexylthiophen-2,5-diyl) (P3HT) is systematically investigated. It is shown that the WF and injection efficiency depend strongly on the history of UV light exposure. Proper treatment of the ZnO layer enables ohmic hole injection into P3HT, demonstrating ZnO as a potential anode material for organic optoelectronic devices. The results also suggest that valid conclusions on the energy-level alignment at the ZnO/organic interfaces may only be drawn if the illumination history is precisely known and controlled. This is inherently problematic when comparing electronic data from ultraviolet photoelectron spectroscopy (UPS) measurements carried out under different or ill-defined illumination conditions.
KW  - charge injection across hybrid interfaces
KW  - energy-level alignments
KW  - hybrid metal oxides
KW  - organic interfaces
Y1  - 2020
U6  - https://doi.org/10.1002/pssa.201900876
SN  - 1862-6300
SN  - 1862-6319
VL  - 217
IS  - 5
SP  - 1
EP  - 6
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Kaa, Johannes M.
A1  - Sternemann, Christian
A1  - Appel, Karen
A1  - Cerantola, Valerio
A1  - Preston, Thomas R.
A1  - Albers, Christian
A1  - Elbers, Mirko
A1  - Libon, Lelia
A1  - Makita, Mikako
A1  - Pelka, Alexander
A1  - Petitgirard, Sylvain
A1  - Plückthun, Christian
A1  - Roddatis, Vladimir
A1  - Sahle, Christoph J.
A1  - Spiekermann, Georg
A1  - Schmidt, Christian
A1  - Schreiber, Anja
A1  - Sakrowski, Robin
A1  - Tolan, Metin
A1  - Wilke, Max
A1  - Zastrau, Ulf
A1  - Konopkova, Zuzana
T1  - Structural and electron spin state changes in an x-ray heated iron carbonate system at the Earth's lower mantle pressures
JF  - Physical review research
N2  - The determination of the spin state of iron-bearing compounds at high pressure and temperature is crucial for our understanding of chemical and physical properties of the deep Earth. Studies on the relationship between the coordination of iron and its electronic spin structure in iron-bearing oxides, silicates, carbonates, iron alloys, and other minerals found in the Earth's mantle and core are scarce because of the technical challenges to simultaneously probe the sample at high pressures and temperatures. We used the unique properties of a pulsed and highly brilliant x-ray free electron laser (XFEL) beam at the High Energy Density (HED) instrument of the European XFEL to x-ray heat and probe samples contained in a diamond anvil cell. We heated and probed with the same x-ray pulse train and simultaneously measured x-ray emission and x-ray diffraction of an FeCO3 sample at a pressure of 51 GPa with up to melting temperatures. We collected spin state sensitive Fe K beta(1,3) fluorescence spectra and detected the sample's structural changes via diffraction, observing the inverse volume collapse across the spin transition. During x-ray heating, the carbonate transforms into orthorhombic Fe4C3O12 and iron oxides. Incipient melting was also observed. This approach to collect information about the electronic state and structural changes from samples contained in a diamond anvil cell at melting temperatures and above will considerably improve our understanding of the structure and dynamics of planetary and exoplanetary interiors.
Y1  - 2022
U6  - https://doi.org/10.1103/PhysRevResearch.4.033042
SN  - 2643-1564
VL  - 4
IS  - 3
PB  - American Physical Society
CY  - College Park
ER  - 
TY  - JOUR
A1  - Zeuschner, Steffen Peer
A1  - Mattern, Maximilian
A1  - Pudell, Jan-Etienne
A1  - Reppert, Alexander von
A1  - Rössle, Matthias
A1  - Leitenberger, Wolfram
A1  - Schwarzkopf, Jutta
A1  - Boschker, Jos
A1  - Herzog, Marc
A1  - Bargheer, Matias
T1  - Reciprocal space slicing
BT  - a time-efficient approach to femtosecond x-ray diffraction
JF  - Structural dynamics
N2  - An experimental technique that allows faster assessment of out-of-plane strain dynamics of thin film heterostructures via x-ray diffraction is presented. In contrast to conventional high-speed reciprocal space-mapping setups, our approach reduces the measurement time drastically due to a fixed measurement geometry with a position-sensitive detector. This means that neither the incident (ω) nor the exit (2θ) diffraction angle is scanned during the strain assessment via x-ray diffraction. Shifts of diffraction peaks on the fixed x-ray area detector originate from an out-of-plane strain within the sample. Quantitative strain assessment requires the determination of a factor relating the observed shift to the change in the reciprocal lattice vector. The factor depends only on the widths of the peak along certain directions in reciprocal space, the diffraction angle of the studied reflection, and the resolution of the instrumental setup. We provide a full theoretical explanation and exemplify the concept with picosecond strain dynamics of a thin layer of NbO2.
Y1  - 2020
U6  - https://doi.org/10.1063/4.0000040
SN  - 2329-7778
VL  - 8
IS  - 1
PB  - AIP Publishing LLC
CY  - Melville, NY
ER  - 
TY  - JOUR
A1  - Seroussi, Helene
A1  - Nowicki, Sophie
A1  - Simon, Erika
A1  - Abe-Ouchi, Ayako
A1  - Albrecht, Torsten
A1  - Brondex, Julien
A1  - Cornford, Stephen
A1  - Dumas, Christophe
A1  - Gillet-Chaulet, Fabien
A1  - Goelzer, Heiko
A1  - Golledge, Nicholas R.
A1  - Gregory, Jonathan M.
A1  - Greve, Ralf
A1  - Hoffman, Matthew J.
A1  - Humbert, Angelika
A1  - Huybrechts, Philippe
A1  - Kleiner, Thomas
A1  - Larourl, Eric
A1  - Leguy, Gunter
A1  - Lipscomb, William H.
A1  - Lowry, Daniel
A1  - Mengel, Matthias
A1  - Morlighem, Mathieu
A1  - Pattyn, Frank
A1  - Payne, Anthony J.
A1  - Pollard, David
A1  - Price, Stephen F.
A1  - Quiquet, Aurelien
A1  - Reerink, Thomas J.
A1  - Reese, Ronja
A1  - Rodehacke, Christian B.
A1  - Schlegel, Nicole-Jeanne
A1  - Shepherd, Andrew
A1  - Sun, Sainan
A1  - Sutter, Johannes
A1  - Van Breedam, Jonas
A1  - van de Wal, Roderik S. W.
A1  - Winkelmann, Ricarda
A1  - Zhang, Tong
T1  - initMIP-Antarctica
BT  - an ice sheet model initialization experiment of ISMIP6
JF  - The Cryosphere : TC ; an interactive open access journal of the European Geosciences Union
N2  - Ice sheet numerical modeling is an important tool to estimate the dynamic contribution of the Antarctic ice sheet to sea level rise over the coming centuries. The influence of initial conditions on ice sheet model simulations, however, is still unclear. To better understand this influence, an initial state intercomparison exercise (initMIP) has been developed to compare, evaluate, and improve initialization procedures and estimate their impact on century-scale simulations. initMlP is the first set of experiments of the Ice Sheet Model Intercomparison Project for CMIP6 (ISMIP6), which is the primary Coupled Model Intercomparison Project Phase 6 (CMIP6) activity focusing on the Greenland and Antarctic ice sheets. Following initMlP-Greenland, initMlP-Antarctica has been designed to explore uncertainties associated with model initialization and spin-up and to evaluate the impact of changes in external forcings. Starting from the state of the Antarctic ice sheet at the end of the initialization procedure, three forward experiments are each run for 100 years: a control run, a run with a surface mass balance anomaly, and a run with a basal melting anomaly beneath floating ice. This study presents the results of initMlP-Antarctica from 25 simulations performed by 16 international modeling groups. The submitted results use different initial conditions and initialization methods, as well as ice flow model parameters and reference external forcings. We find a good agreement among model responses to the surface mass balance anomaly but large variations in responses to the basal melting anomaly. These variations can be attributed to differences in the extent of ice shelves and their upstream tributaries, the numerical treatment of grounding line, and the initial ocean conditions applied, suggesting that ongoing efforts to better represent ice shelves in continental-scale models should continue.
Y1  - 2019
U6  - https://doi.org/10.5194/tc-13-1441-2019
SN  - 1994-0416
SN  - 1994-0424
VL  - 13
IS  - 5
SP  - 1441
EP  - 1471
PB  - Copernicus
CY  - Göttingen
ER  - 
TY  - JOUR
A1  - Reese, Ronja
A1  - Albrecht, Torsten
A1  - Mengel, Matthias
A1  - Asay-Davis, Xylar
A1  - Winkelmann, Ricarda
T1  - Antarctic sub-shelf melt rates via PICO
JF  - The Cryosphere : TC ; an interactive open access journal of the European Geosciences Union
N2  - Ocean-induced melting below ice shelves is one of the dominant drivers for mass loss from the Antarctic Ice Sheet at present. An appropriate representation of sub-shelf melt rates is therefore essential for model simulations of marine-based ice sheet evolution. Continental-scale ice sheet models often rely on simple melt-parameterizations, in particular for long-term simulations, when fully coupled ice-ocean interaction becomes computationally too expensive. Such parameterizations can account for the influence of the local depth of the ice-shelf draft or its slope on melting. However, they do not capture the effect of ocean circulation underneath the ice shelf. Here we present the Potsdam Ice-shelf Cavity mOdel (PICO), which simulates the vertical overturning circulation in ice-shelf cavities and thus enables the computation of sub-shelf melt rates consistent with this circulation. PICO is based on an ocean box model that coarsely resolves ice shelf cavities and uses a boundary layer melt formulation. We implement it as a module of the Parallel Ice Sheet Model (PISM) and evaluate its performance under present-day conditions of the Southern Ocean. We identify a set of parameters that yield two-dimensional melt rate fields that qualitatively reproduce the typical pattern of comparably high melting near the grounding line and lower melting or refreezing towards the calving front. PICO captures the wide range of melt rates observed for Antarctic ice shelves, with an average of about 0.1 ma(-1) for cold sub-shelf cavities, for example, underneath Ross or Ronne ice shelves, to 16 ma(-1) for warm cavities such as in the Amundsen Sea region. This makes PICO a computationally feasible and more physical alternative to melt parameterizations purely based on ice draft geometry.
Y1  - 2018
U6  - https://doi.org/10.5194/tc-12-1969-2018
SN  - 1994-0416
SN  - 1994-0424
VL  - 12
IS  - 6
SP  - 1969
EP  - 1985
PB  - Copernicus
CY  - Göttingen
ER  - 
TY  - JOUR
A1  - Steffen, Will
A1  - Röckstrom, Johan
A1  - Richardson, Katherine
A1  - Lenton, Timothy M.
A1  - Folke, Carl
A1  - Liverman, Diana
A1  - Summerhayes, Colin P.
A1  - Barnosky, Anthony D.
A1  - Cornell, Sarah E.
A1  - Crucifix, Michel
A1  - Donges, Jonathan
A1  - Fetzer, Ingo
A1  - Lade, Steven J.
A1  - Scheffer, Marten
A1  - Winkelmann, Ricarda
A1  - Schellnhuber, Hans Joachim
T1  - Trajectories of the Earth System in the Anthropocene
JF  - Proceedings of the National Academy of Sciences of the United States of America
N2  - We explore the risk that self-reinforcing feedbacks could push the Earth System toward a planetary threshold that, if crossed, could prevent stabilization of the climate at intermediate temperature rises and cause continued warming on a "Hothouse Earth" pathway even as human emissions are reduced. Crossing the threshold would lead to a much higher global average temperature than any interglacial in the past 1.2 million years and to sea levels significantly higher than at any time in the Holocene. We examine the evidence that such a threshold might exist and where it might be. If the threshold is crossed, the resulting trajectory would likely cause serious disruptions to ecosystems, society, and economies. Collective human action is required to steer the Earth System away from a potential threshold and stabilize it in a habitable interglacial-like state. Such action entails stewardship of the entire Earth System-biosphere, climate, and societies-and could include decarbonization of the global economy, enhancement of biosphere carbon sinks, behavioral changes, technological innovations, new governance arrangements, and transformed social values.
KW  - Earth System trajectories
KW  - climate change
KW  - Anthropocene
KW  - biosphere feedbacks
KW  - tipping elements
Y1  - 2018
U6  - https://doi.org/10.1073/pnas.1810141115
SN  - 0027-8424
VL  - 115
IS  - 33
SP  - 8252
EP  - 8259
PB  - National Acad. of Sciences
CY  - Washington
ER  - 
TY  - JOUR
A1  - Reese, Ronja
A1  - Winkelmann, Ricarda
A1  - Gudmundsson, Gudmundur Hilmar
T1  - Grounding-line flux formula applied as a flux condition in numerical simulations fails for buttressed Antarctic ice streams
JF  - The Cryosphere : TC ; an interactive open access journal of the European Geosciences Union
N2  - Currently, several large-scale ice-flow models impose a condition on ice flux across grounding lines using an analytically motivated parameterisation of grounding-line flux. It has been suggested that employing this analytical expression alleviates the need for highly resolved computational domains around grounding lines of marine ice sheets. While the analytical flux formula is expected to be accurate in an unbuttressed flow-line setting, its validity has hitherto not been assessed for complex and realistic geometries such as those of the Antarctic Ice Sheet. Here the accuracy of this analytical flux formula is tested against an optimised ice flow model that uses a highly resolved computational mesh around the Antarctic grounding lines. We find that when applied to the Antarctic Ice Sheet the analytical expression provides inaccurate estimates of ice fluxes for almost all grounding lines. Furthermore, in many instances direct application of the analytical formula gives rise to unphysical complex-valued ice fluxes. We conclude that grounding lines of the Antarctic Ice Sheet are, in general, too highly buttressed for the analytical parameterisation to be of practical value for the calculation of grounding-line fluxes.
Y1  - 2018
U6  - https://doi.org/10.5194/tc-12-3229-2018
SN  - 1994-0416
SN  - 1994-0424
VL  - 12
IS  - 10
SP  - 3229
EP  - 3242
PB  - Copernicus
CY  - Göttingen
ER  -