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 - Shoaee, Safa A1 - Stolterfoht, Martin A1 - Neher, Dieter T1 - The Role of Mobility on Charge Generation, Recombination, and Extraction in Polymer-Based Solar Cells JF - dvanced energy materials N2 - Organic semiconductors are of great interest for a broad range of optoelectronic applications due to their solution processability, chemical tunability, highly scalable fabrication, and mechanical flexibility. In contrast to traditional inorganic semiconductors, organic semiconductors are intrinsically disordered systems and therefore exhibit much lower charge carrier mobilities-the Achilles heel of organic photovoltaic cells. In this progress review, the authors discuss recent important developments on the impact of charge carrier mobility on the charge transfer state dissociation, and the interplay of free charge extraction and recombination. By comparing the mobilities on different timescales obtained by different techniques, the authors highlight the dispersive nature of these materials and how this reflects on the key processes defining the efficiency of organic photovoltaics. KW - charge generation KW - charge recombination KW - extraction KW - mobility KW - organic solar cells KW - polymer:fullerene bulk heterojunction Y1 - 2018 U6 - https://doi.org/10.1002/aenm.201703355 SN - 1614-6832 SN - 1614-6840 VL - 8 IS - 28 PB - Wiley-VCH CY - Weinheim ER - TY - GEN A1 - Reppert, Alexander von A1 - Puddell, J. A1 - Koc, A. A1 - Reinhardt, M. A1 - Leitenberger, Wolfram A1 - Dumesnil, K. A1 - Zamponi, Flavio A1 - Bargheer, Matias T1 - Persistent nonequilibrium dynamics of the thermal energies in the spin and phonon systems of an antiferromagnet N2 - We present a temperature and fluence dependent Ultrafast X-Ray Diffraction study of a laser-heated antiferromagnetic dysprosium thin film. The loss of antiferromagnetic order is evidenced by a pronounced lattice contraction. We devise a method to determine the energy flow between the phonon and spin system from calibrated Bragg peak positions in thermal equilibrium. Reestablishing the magnetic order is much slower than the cooling of the lattice, especially around the Néel temperature. Despite the pronounced magnetostriction, the transfer of energy from the spin system to the phonons in Dy is slow after the spin-order is lost. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 272 Y1 - 2016 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-98710 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 - GEN 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 T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe 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. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1137 Y1 - 2021 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-499761 SN - 1866-8372 IS - 1137 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 - Kleinpeter, Erich A1 - Koch, Andreas T1 - The 13 C chemical shift and the anisotropy effect of the carbene electron-deficient centre BT - simple means to characterize the electron distribution of carbenes JF - Magnetic resonance in chemistry N2 - Both the C-13 chemical shift and the calculated anisotropy effect (spatial magnetic properties) of the electron-deficient centre of stable, crystalline, and structurally characterized carbenes have been employed to unequivocally characterize potential resonance contributors to the present mesomerism (carbene, ylide, betaine, and zwitter ion) and to determine quantitatively the electron deficiency of the corresponding carbene carbon atom. Prior to that, both structures and C-13 chemical shifts were calculated and compared with the experimental delta(C-13)/ppm values and geometry parameters (as a quality criterion for obtained structures). KW - C-13 chemical shift KW - carbenes KW - zwitterions KW - carbene electron deficiency KW - nucleus-independent chemical shifts (NICS) KW - through space NMR shieldings KW - (TSNMRS) Y1 - 2019 U6 - https://doi.org/10.1002/mrc.4979 SN - 0749-1581 SN - 1097-458X VL - 58 IS - 3 SP - 280 EP - 292 PB - Wiley CY - Hoboken ER - TY - JOUR A1 - Kleinpeter, Erich A1 - Koch, Andreas T1 - Quantification of sigma-acceptor and pi-donor stabilization in O, S and Hal analogues of N-heterocyclic carbenes (NHCs) on the magnetic criterion JF - The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment & general theory N2 - The spatial magnetic properties, through-space NMR shieldings (TSNMRSs), of stable O, S and Hal analogues of N-heterocyclic carbenes (NHCs) have been calculated using the GIAO perturbation method employing the nucleus-independent chemical shift (NICS) concept and the results visualized as iso-chemical-shielding surfaces (ICSSs) of various sizes and directions. The TSNMRS values (actually the anisotropy effects measurable in H-1 NMR spectroscopy) are employed to qualify and quantify the position of the present mesomeric equilibria (carbenes <-> ylides). The results are confirmed by geometry (bond angles and bond lengths), IR spectra, UV spectra, and C-13 chemical shifts of the electron-deficient carbon centers. Y1 - 2021 U6 - https://doi.org/10.1021/acs.jpca.1c05257 SN - 1089-5639 SN - 1520-5215 VL - 125 IS - 33 SP - 7235 EP - 7245 PB - American Chemical Society CY - Washington ER - TY - THES A1 - Bojahr, Andre T1 - Hypersound interaction studied by time-resolved inelastic light and x-ray scattering T1 - Wechselwirkende Hyperschallwellen untersucht mittels zeitaufgelöster inelastischer Licht- und Röntgenstreuung N2 - This publications-based thesis summarizes my contribution to the scientific field of ultrafast structural dynamics. It consists of 16 publications, about the generation, detection and coupling of coherent gigahertz longitudinal acoustic phonons, also called hypersonic waves. To generate such high frequency phonons, femtosecond near infrared laser pulses were used to heat nanostructures composed of perovskite oxides on an ultrashort timescale. As a consequence the heated regions of such a nanostructure expand and a high frequency acoustic phonon pulse is generated. To detect such coherent acoustic sound pulses I use ultrafast variants of optical Brillouin and x-ray scattering. Here an incident optical or x-ray photon is scattered by the excited sound wave in the sample. The scattered light intensity measures the occupation of the phonon modes. The central part of this work is the investigation of coherent high amplitude phonon wave packets which can behave nonlinearly, quite similar to shallow water waves which show a steepening of wave fronts or solitons well known as tsunamis. Due to the high amplitude of the acoustic wave packets in the solid, the acoustic properties can change significantly in the vicinity of the sound pulse. This may lead to a shape change of the pulse. I have observed by time-resolved Brillouin scattering, that a single cycle hypersound pulse shows a wavefront steepening. I excited hypersound pulses with strain amplitudes until 1% which I have calibrated by ultrafast x-ray diffraction (UXRD). On the basis of this first experiment we developed the idea of the nonlinear mixing of narrowband phonon wave packets which we call "nonlinear phononics" in analogy with the nonlinear optics, which summarizes a kaleidoscope of surprising optical phenomena showing up at very high electric fields. Such phenomena are for instance Second Harmonic Generation, four-wave-mixing or solitons. But in case of excited coherent phonons the wave packets have usually very broad spectra which make it nearly impossible to look at elementary scattering processes between phonons with certain momentum and energy. For that purpose I tested different techniques to excite narrowband phonon wave packets which mainly consist of phonons with a certain momentum and frequency. To this end epitaxially grown metal films on a dielectric substrate were excited with a train of laser pulses. These excitation pulses drive the metal film to oscillate with the frequency given by their inverse temporal displacement and send a hypersonic wave of this frequency into the substrate. The monochromaticity of these wave packets was proven by ultrafast optical Brillouin and x-ray scattering. Using the excitation of such narrowband phonon wave packets I was able to observe the Second Harmonic Generation (SHG) of coherent phonons as a first example of nonlinear wave mixing of nanometric phonon wave packets. N2 - Diese publikationsbasierte Dissertation fasst meinen Beitrag zum Forschungsgebiet der ultraschnellen Strukturdynamik zusammen. Diese Arbeit besteht aus 16 Publikationen aus den Bereichen der Erzeugung, Detektion und Kopplung von kohärenten Gigahertz longitudinal-akustischen Phononen, auch Hyperschallwellen genannt. Um solch hochfrequente Phononen zu erzeugen, werden Femtosekunden nahinfrarot Laserpulse benutzt, um Nanostrukturen auf einer ultraschnellen Zeitskala zu erhitzen. Die aufgeheizten Regionen der Nanostruktur dehnen sich aufgrund der hohen Temperatur aus und ein hochfrequenter Schallpuls wird generiert. Um solche akustischen Pulse zu detektieren benutze ich ultraschnelle Varianten der Brillouin- und Röntgenstreuung. Dabei wird ein einfallendes optisches oder Röntgenphoton an der erzeugten Schallwelle gestreut. Die gemessene Streuintensität ist hierbei ein Maß für die Besetzung einzelner Phononenzustände. Der zentrale Teil dieser Arbeit ist die Untersuchung von kohärenten Phonon-Wellenpaketen mit sehr hoher Amplitude. Diese Wellenpakete können sich nichtlinear verhalten, sehr ähnlich zu Flachwasserwellen bei denen nichtlineare Effekte in Form eines Aufsteilens der Wellenfronten oder der Existenz von Solitonen, bekannt als Tsunamis, äußern. Durch die hohe Amplitude der akustischen Wellenpakete können sich die akustischen Eigenschaften des Festkörpers in der Umgebung des Schallpulses signifikant ändern, welches sich dann in einer Formänderung des Schallpulses widerspiegelt. Ich konnte mittels zeitaufgelöster Brillouinstreuung das Aufsteilen der Wellenfronten eines Hyperschallpulses bestehend aus einem einzigen Oszillationszyklus beobachten. Hierbei wurden Hyperschallwellen mit einer Dehnungsamplitude von bis zu 1% angeregt, wobei ich diesen Wert mittels ultraschneller Röntgenbeugung kalibrieren konnte. Mit diesem ersten Experiment als Basis entwickelten wir die Idee der nichtlinearen Wellenmischung von schmalbandigen Phonon-Wellenpaketen unter dem Titel "nichtlineare Phononik" in Analogie zur nichtlinearen Optik, welche sich aus einer Reihe von verblüffenden optischen Phänomenen bei sehr hohen elektrischen Feldstärken zusammensetzt. Solche Phänomene sind z. B. die optische Frequenzverdopplung, das Vier-Wellen-Mischen oder Solitone. Nur sind im Falle von kohärenten Phononen die erzeugten Spektren sehr breitbandig, was die Untersuchung von spezifischen Phononen mit festem Impuls und definierter Frequenz fast unmöglich macht. Aus diesem Grund testete ich verschiedene Methoden um schmalbandige Phonon-Wellenpakete anzuregen, welche im Wesentlichen aus Phononen bestimmten Impulses und definierter Frequenz bestehen. Dafür wurden schließ lich epitaktisch auf ein dielektrisches Substrat aufgewachsene Metallfilme mit einen Laserpulszug angeregt. Hier sorgen die Lichtpulse für eine periodische Oszillation des Metalfilms, wobei die Anregefrequenz durch den inversen zeitlichen Abstand der Lichtpulse gegeben ist. Diese periodische Oszillation sendet dann ein Hyperschallwellenpaket eben dieser Frequenz ins Substrat. Die Monochromie dieser Wellenpakete konnte dabei mittels ultraschneller Brillouin- und Röntgenstreuung bestätigt werden. Durch die Benutzung dieser schmalbandigen Phonon-Wellenpakete war es mir möglich, die Frequenzverdopplung (SHG) von kohärenten Phononen zu beobachten, was ein erstes Beispiel für die nichtlineare Wellenmischung von nanometrischen Phonon-Wellenpaketen ist. KW - hypersound KW - nonlinear acoustics KW - ultrafast KW - Brillouin scattering KW - x-ray diffraction KW - self-steepening KW - second-harmonic generation KW - Phononen KW - Wechselwirkung KW - Anharmonizität KW - nichtlineare Wellenmischung KW - zweite Harmonische KW - Phononenstreuung KW - nichlineare Phononik Y1 - 2016 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-93860 ER - TY - THES A1 - Maerten, Lena T1 - Spectroscopic perspectives on ultrafast coupling phenomena in perovskite oxides T1 - Spektroskopische Untersuchung ultraschneller Kopplungsphänomene in Perowskit-Oxiden N2 - In this thesis, I study ultrafast dynamics in perovskite oxides using time resolved broadband spectroscopy. I focus on the observation of coherent phonon propagation by time resolved Brillouin scattering: following the excition of metal transducer films with a femtosecond infrared pump pulse, coherent phonon dynamics in the GHz frequency range are triggered. Their propagation is monitored using a delayed white light probe pulse. The technique is illustrated on various thin films and multilayered samples. I apply the technique to investigate the linear and nonlinear acoustic response in bulk SrTiO_3, which displays a ferroelastic phase transition from a cubic to a tetragonal structural phase at T_a=105 K. In the linear regime, I observe a coupling of the observed acoustic phonon mode to the softening optic modes describing the phase transition. In the nonlinear regime, I find a giant slowing down of the sound velocity in the low temperature phase that is only observable for a strain amplitude exceeding the tetragonality of the material. It is attributed to a coupling of the high frequency phonons to ferroelastic domain walls in the material. I propose a new mechanism for the coupling of strain waves to the domain walls that is only effective for high amplitude strain. A detailed study of the phonon attenuation across a wide temperature range shows that the phonon attenuation at low temperatures is influenced by the domain configuration, which is determined by interface strain. Preliminary measurements on magnetic-ferroelectric multilayers reveal that the excitation fluence needs to be carefully controlled when dynamics at phase transitions are studied. N2 - In dieser Doktorarbeit untersuche ich ultraschnelle Dynamik in perovskitischen Oxiden mittels zeitaufgelöster optischer Spektroskopie. Der Schwerpunkt liegt dabei auf Phononendynamik, die mithilfe von zeitaufgelöster Brillouin-Streuung sichtbar gemacht wird: durch die Anregung einer metallischen Transducer-Schicht mit einem ultrakurzen Anregepuls wird eine kohärente Phononendynamik im GHz Frequenzbereich erzeugt. Die Ausbreitung der Schallpulse wird mit einem Weißlicht-Abfragepuls aufgezeichnet. Diese Methode wird am Beispiel verschiedener Dünnschicht- und Übergitterproben illustriert. Die Methode und das gewonnene Verständnis wende ich an, um lineare und nichtlineare akustische Eigenschaften an einem SrTiO_3-Kristall zu untersuchen. Dieser weist einen ferroelastischen Phasenübergang von kubischer zu tetragonaler Kristallstruktur bei T_a=105 K auf. Im linearen Regime beobachte ich eine Kopplung der untersuchten akustischen Mode an eine weichwerdende optische Mode, welche den Phasenübergang charakterisiert. Im nichtlinearen Regime tritt eine gigantische Verlangsamung der Schallgeschwindigkeit unterhalb von T_a auf, wenn die induzierte Gitterverzerrung die Tetragonalität des Materials übersteigt. Dies kann auf eine Kopplung der hochfrequenten akustischen Mode an ferroelastische Domänenwände bei tiefen Temperaturen zurückgeführt werden. Ich entwickle einen neuen Mechanismus, der die Kopplung der Verzerrungswelle an die Domänenwände beschreibt. Eine detaillierte Untersuchung der Phononendämpfung in SrTiO_3 über einen weiten Temperaturbereich zeigt, dass diese bei tiefen Temperaturen durch die Domänenkonfiguration beeinflusst ist. Die Domänenkonfiguration ist durch Verzerrungen an der Kristall-Transducer Grenzfläche bestimmt. Erste Untersuchungen an magnetisch-ferroelektrischen Übergittern zeigen, dass die Anregungsfluenz vorsichtig eingestellt werden muss, um die Dynamik an Phasenübergängen zu untersuchen. KW - coherent phonons KW - phonon dynamics KW - time resolved KW - Brillouin scattering KW - perovskite oxides KW - optical spectroscopy KW - hypersound propagation KW - phonon damping KW - domain wall motion KW - phonon backfolding KW - superlattice dispersion KW - kohärente Phononen KW - Phononen Dynamik KW - zeitaufgelöst KW - Brillouin Streuung KW - Perowskit-Oxide KW - optische Spektroskopie KW - Hyperschall Propagation KW - Phononen Dämpfung KW - Domänenwandbewegung KW - Phononen Rückfaltung KW - Übergitter Dispersion Y1 - 2015 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-77623 ER - TY - JOUR A1 - Shayduk, Roman A1 - Hallmann, Jörg A1 - Rodriguez-Fernandez, Angel A1 - Scholz, Markus A1 - Lu, Wei A1 - Bösenberg, Ulrike A1 - Möller, Johannes A1 - Zozulya, Alexey A1 - Jiang, Man A1 - Wegner, Ulrike A1 - Secareanu, Radu-Costin A1 - Palmer, Guido A1 - Emons, Moritz A1 - Lederer, Max A1 - Volkov, Sergey A1 - Lindfors-Vrejoiu, Ionela A1 - Schick, Daniel A1 - Herzog, Marc A1 - Bargheer, Matias A1 - Madsen, Anders T1 - Femtosecond x-ray diffraction study of multi-THz coherent phonons in SrTiO3 JF - Applied physics letters N2 - We report generation of ultra-broadband longitudinal acoustic coherent phonon wavepackets in SrTiO3 (STO) with frequency components extending throughout the first Brillouin zone. The wavepackets are efficiently generated in STO using femtosecond infrared laser excitation of an atomically flat 1.6 nm-thick epitaxial SrRuO3 film. We use femtosecond x-ray diffraction at the European X-Ray Free Electron Laser Facility to study the dispersion and damping of phonon wavepackets. The experimentally determined damping constants for multi-THz frequency phonons compare favorably to the extrapolation of a simple ultrasound damping model over several orders of magnitude. Y1 - 2022 U6 - https://doi.org/10.1063/5.0083256 SN - 0003-6951 SN - 1077-3118 VL - 120 IS - 20 PB - AIP Publishing CY - Melville ER - TY - JOUR A1 - Deb, Marwan A1 - Popova, Elena A1 - Jaffrès, Henri-Yves A1 - Keller, Niels A1 - Bargheer, Matias T1 - Polarization-dependent subpicosecond demagnetization in iron garnets JF - Physical review : B, covering condensed matter and materials physics N2 - Controlling the magnetization dynamics at the fastest speed is a major issue of fundamental condensed matter physics and its applications for data storage and processing technologies. It requires a deep understanding of the interactions between the degrees of freedom in solids, such as spin, electron, and lattice as well as their responses to external stimuli. In this paper, we systematically investigate the fluence dependence of ultrafast magnetization dynamics induced by below-bandgap ultrashort laser pulses in the ferrimagnetic insulators BixY3-xFe5O12 with 1 xBi 3. We demonstrate subpicosecond demagnetization dynamics in this material followed by a very slow remagnetization process. We prove that this demagnetization results from an ultrafast heating of iron garnets by two-photon absorption (TPA), suggesting a phonon-magnon thermalization time of 0.6 ps. We explain the slow remagnetization timescale by the low phonon heat conductivity in garnets. Additionally, we show that the amplitudes of the demagnetization, optical change, and lattice strain can be manipulated by changing the ellipticity of the pump pulses. We explain this phenomenon considering the TPA circular dichroism. These findings open exciting prospects for ultrafast manipulation of spin, charge, and lattice dynamics in magnetic insulators by ultrafast nonlinear optics. Y1 - 2022 U6 - https://doi.org/10.1103/PhysRevB.106.184416 SN - 2469-9950 SN - 2469-9969 VL - 106 IS - 18 PB - American Institute of Physics, American Physical Society CY - Woodbury, NY ER - TY - JOUR A1 - Deb, Marwan A1 - Popova, Elena A1 - Jaffrès, Henri-Yves A1 - Keller, Niels A1 - Bargheer, Matias T1 - Controlling high-frequency spin-wave dynamics using double-pulse laser excitation JF - Physical review applied N2 - Manipulating spin waves is highly required for the development of innovative data transport and processing technologies. Recently, the possibility of triggering high-frequency standing spin waves in magnetic insulators using femtosecond laser pulses was discovered, raising the question about how one can manipulate their dynamics. Here we explore this question by investigating the ultrafast magnetiza-tion and spin-wave dynamics induced by double-pulse laser excitation. We demonstrate a suppression or enhancement of the amplitudes of the standing spin waves by precisely tuning the time delay between the two pulses. The results can be understood as the constructive or destructive interference of the spin waves induced by the first and second laser pulses. Our findings open exciting perspectives towards generating single-mode standing spin waves that combine high frequency with large amplitude and low magnetic damping. Y1 - 2022 U6 - https://doi.org/10.1103/PhysRevApplied.18.044001 SN - 2331-7019 VL - 18 IS - 4 PB - American Physical Society CY - College Park ER - TY - GEN A1 - Stete, Felix A1 - Koopman, Wouter-Willem Adriaan A1 - Bargheer, Matias T1 - Signatures of strong coupling on nanoparticles BT - revealing absorption anticrossing by tuning the dielectric environment T2 - Quantum Nano-Photonics N2 - The electromagnetic coupling of molecular excitations to plasmonic nanoparticles offers a promising method to manipulate the light-matter interaction at the nanoscale. Plasmonic nanoparticles foster exceptionally high coupling strengths, due to their capacity to strongly concentrate the light-field to sub-wavelength mode volumes. A particularly interesting coupling regime occurs, if the coupling increases to a level such that the coupling strength surpasses all damping rates in the system. In this so-called strong-coupling regime hybrid light-matter states emerge, which can no more be divided into separate light and matter components. These hybrids unite the features of the original components and possess new resonances whose positions are separated by the Rabi splitting energy h Omega. Detuning the resonance of one of the components leads to an anticrossing of the two arising branches of the new resonances omega(+) and omega(-) with a minimal separation of Omega = omega(+) - omega(-). Y1 - 2018 SN - 978-94-024-1546-9 SN - 978-94-024-1544-5 SN - 978-94-024-1543-8 U6 - https://doi.org/10.1007/978-94-024-1544-5_53 SN - 1871-465X SP - 445 EP - 447 PB - Springer CY - Dordrecht ER - TY - GEN A1 - Stete, Felix A1 - Schossau, Phillip Gerald A1 - Koopman, Wouter-Willem Adriaan A1 - Bargheer, Matias T1 - Size Dependence of the Coupling Strength in Plasmon-Exciton Nanoparticles T2 - Quantum Nano-Photonics N2 - The coupling between molecular excitations and nanoparticles leads to promising applications. It is for example used to enhance the optical cross-section of molecules in surface enhanced Raman scattering, Purcell enhancement or plasmon enhanced dye lasers. In a coupled system new resonances emerge resulting from the original plasmon (ωpl) and exciton (ωex) resonances as ω±=12(ωpl+ωex)±14(ωpl−ωex)2+g2−−−−−−−−−−−−−−−√, (1) where g is the coupling parameter. Hence, the new resonances show a separation of Δ = ω+ − ω− from which the coupling strength can be deduced from the minimum distance between the two resonances, Ω = Δ(ω+ = ω−). Y1 - 2018 SN - 978-94-024-1546-9 SN - 978-94-024-1544-5 SN - 978-94-024-1543-8 U6 - https://doi.org/10.1007/978-94-024-1544-5_26 SN - 1871-465X SP - 381 EP - 383 PB - Springer CY - Dordrecht ER - TY - THES A1 - Born, Artur T1 - Electronic structure, quasi-particle interaction and relaxation in 3d-elements from X-ray spectroscopy Y1 - 2021 ER - TY - THES A1 - Schick, Daniel T1 - Ultrafast lattice dynamics in photoexcited nanostructures : femtosecond X-ray diffraction with optimized evaluation schemes T1 - Ultraschnelle Gitterdynamik in optisch angeregten Nanostrukturen : Femtosekunden-Röntgendiffraktion mit optimierten Auswerteroutinen N2 - Within the course of this thesis, I have investigated the complex interplay between electron and lattice dynamics in nanostructures of perovskite oxides. Femtosecond hard X-ray pulses were utilized to probe the evolution of atomic rearrangement directly, which is driven by ultrafast optical excitation of electrons. The physics of complex materials with a large number of degrees of freedom can be interpreted once the exact fingerprint of ultrafast lattice dynamics in time-resolved X-ray diffraction experiments for a simple model system is well known. The motion of atoms in a crystal can be probed directly and in real-time by femtosecond pulses of hard X-ray radiation in a pump-probe scheme. In order to provide such ultrashort X-ray pulses, I have built up a laser-driven plasma X-ray source. The setup was extended by a stable goniometer, a two-dimensional X-ray detector and a cryogen-free cryostat. The data acquisition routines of the diffractometer for these ultrafast X-ray diffraction experiments were further improved in terms of signal-to-noise ratio and angular resolution. The implementation of a high-speed reciprocal-space mapping technique allowed for a two-dimensional structural analysis with femtosecond temporal resolution. I have studied the ultrafast lattice dynamics, namely the excitation and propagation of coherent phonons, in photoexcited thin films and superlattice structures of the metallic perovskite SrRuO3. Due to the quasi-instantaneous coupling of the lattice to the optically excited electrons in this material a spatially and temporally well-defined thermal stress profile is generated in SrRuO3. This enables understanding the effect of the resulting coherent lattice dynamics in time-resolved X-ray diffraction data in great detail, e.g. the appearance of a transient Bragg peak splitting in both thin films and superlattice structures of SrRuO3. In addition, a comprehensive simulation toolbox to calculate the ultrafast lattice dynamics and the resulting X-ray diffraction response in photoexcited one-dimensional crystalline structures was developed in this thesis work. With the powerful experimental and theoretical framework at hand, I have studied the excitation and propagation of coherent phonons in more complex material systems. In particular, I have revealed strongly localized charge carriers after above-bandgap femtosecond photoexcitation of the prototypical multiferroic BiFeO3, which are the origin of a quasi-instantaneous and spatially inhomogeneous stress that drives coherent phonons in a thin film of the multiferroic. In a structurally imperfect thin film of the ferroelectric Pb(Zr0.2Ti0.8)O3, the ultrafast reciprocal-space mapping technique was applied to follow a purely strain-induced change of mosaicity on a picosecond time scale. These results point to a strong coupling of in- and out-of-plane atomic motion exclusively mediated by structural defects. N2 - Im Rahmen dieser Arbeit habe ich mich mit den komplexen Wechselwirkungen zwischen Elektronen- und Gitterdynamik in oxidischen Perowskit-Nanostrukturen beschäftigt. Dazu wurden verschiedene Proben mit intensiven, ultrakurzen Laserpulsen angeregt. Um die zeitliche Entwicklung der induzierten atomaren Umordnung zu untersuchen, wurden Femtosekunden-Pulse harter Röntgenstrahlung genutzt. Zunächst wurde die ultraschnelle Gitterdynamik in einfachen Modellsystemen mit zeitaufgelösten Röntgendiffraktionsexperimenten untersucht, um im Anschluss ähnliche Experimente an komplexeren Materialien mit mehreren Freiheitsgraden interpretieren zu können. Die Bewegung der Atome in einem Kristall kann über Anrege-Abtast-Verfahren direkt mit gepulster, harter Röntgenstrahlung gemessen werden. Die Dauer der Röntgenpulse muss dafür einige hundert Femtosekunden kurz sein. Um diese ultrakurzen Röntgenpulse zu erzeugen, habe ich eine lasergetriebene Plasma-Röntgenquelle aufgebaut. Der Aufbau wurde um ein stabiles Goniometer, einen zweidimensionalen Röntgendetektor und einen kryogenfreien Kryostat erweitert und in Bezug auf das Signal-zu-Rausch-Verhältnis und die Winkelauflösung optimiert. Durch die Entwicklung einer schnellen Methode zur Vermessung des reziproken Raums konnte erstmals an solch einer Quelle eine zweidimensionale Strukturanalyse mit Femtosekunden-Zeitauflösung realisiert werden. Die Anregung und Ausbreitung von kohärenten Phononen habe ich in optisch angeregten Dünnfilm- und Übergitterstrukturen untersucht. Eine entscheidende Rolle spielen dabei metallische SrRuO3 Schichten. Durch die quasi-instantane Kopplung des Gitters an die optisch angeregten Elektronen in SrRuO3 wird ein räumlich und zeitlich wohldefiniertes Druckprofil erzeugt. Dadurch kann der Einfluss der resultierenden kohärenten Gitterdynamik auf die zeitaufgelösten Röntgendiffraktionsdaten im Detail verstanden werden. Beobachtet wurde z.B. das Auftreten einer transienten Aufspaltung eines Bragg-Reflexes bei Dünnfilm- und Übergitterstrukturen aus SrRuO3. Außerdem wurde eine umfangreiche Simulationsumgebung entwickelt, mit deren Hilfe die ultraschnelle Dynamik und die dazugehörigen Röntgendiffraktionssignale in optisch angeregten eindimensionalen Kristallstrukturen berechnet werden können. Der von mir entwickelte experimentelle Aufbau sowie das Simulationspaket zur Datenanalyse und -interpretation wurden anschließend für die Untersuchung kohärenter Phononen in komplexeren Materialsystemen eingesetzt. Im Speziellen konnte ich in multiferroischem BiFeO3 eine stark lokalisierte Ladungsträgerverteilung nach einer optischen Femtosekunden-Anregung nachweisen. Sie ist die Ursache für einen quasi-instantanen und räumlich inhomogenen Druck, der die kohärenten Phononen in einem dünnen Film dieses Multiferroikums erzeugt. Außerdem habe ich die ultraschnelle Vermessung des reziproken Raums angewendet, um eine verzerrungsinduzierte Veränderung der Mosaizität in einem strukturell unvollkommenen Film aus ferroelektrischem Pb(Zr0.2Ti0.8)O3 zu verfolgen. Die Ergebnisse deuten auf eine ausschließlich durch strukturelle Defekte vermittelte Kopplung der atomaren Bewegungen parallel und senkrecht zur Flächennormalen des Filmes hin. KW - ultraschnelle Röntgendiffraktion KW - Gitterdynamik KW - Nanostruktur KW - optische Anregung KW - Perowskit KW - ultrafast X-ray diffraction KW - lattice dynamics KW - nanostructure KW - photoexcitation KW - perovskite Y1 - 2013 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus-68827 ER -