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 - Schick, Daniel A1 - Herzog, Marc A1 - Wen, Haidan A1 - Chen, Pice A1 - Adamo, Carolina A1 - Gaal, Peter A1 - Schlom, Darrell G. A1 - Evans, Paul G. A1 - Li, Yuelin A1 - Bargheer, Matias T1 - Localized excited charge carriers generate ultrafast inhomogeneous strain in the multiferroic BiFeO3 JF - Physical review letters N2 - We apply ultrafast x-ray diffraction with femtosecond temporal resolution to monitor the lattice dynamics in a thin film of multiferroic BiFeO3 after above-band-gap photoexcitation. The sound-velocity limited evolution of the observed lattice strains indicates a quasi-instantaneous photoinduced stress which decays on a nanosecond time scale. This stress exhibits an inhomogeneous spatial profile evidenced by the broadening of the Bragg peak. These new data require substantial modification of existing models of photogenerated stresses in BiFeO3: the relevant excited charge carriers must remain localized to be consistent with the data. Y1 - 2014 U6 - https://doi.org/10.1103/PhysRevLett.112.097602 SN - 0031-9007 SN - 1079-7114 VL - 112 IS - 9 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Herzog, Marc A1 - Schick, Daniel A1 - Leitenberger, Wolfram A1 - Shayduk, Roman A1 - van der Veen, Renske M. A1 - Milne, Christopher J. A1 - Johnson, Steven Lee A1 - Vrejoiu, Ionela A1 - Bargheer, Matias T1 - Tailoring interference and nonlinear manipulation of femtosecond x-rays JF - New journal of physics : the open-access journal for physics N2 - We present ultrafast x-ray diffraction (UXRD) experiments on different photoexcited oxide superlattices. All data are successfully simulated by dynamical x-ray diffraction calculations based on a microscopic model, that accounts for the linear response of phonons to the excitation laser pulse. Some Bragg reflections display a highly nonlinear strain dependence. The origin of linear and two distinct nonlinear response phenomena is discussed in a conceptually simpler model using the interference of envelope functions that describe the diffraction efficiency of the average constituent nanolayers. The combination of both models facilitates rapid and accurate simulations of UXRD experiments. Y1 - 2012 U6 - https://doi.org/10.1088/1367-2630/14/1/013004 SN - 1367-2630 VL - 14 IS - 1 PB - IOP Publ. Ltd. CY - Bristol ER - TY - JOUR A1 - Schick, Daniel A1 - Bojahr, Andre A1 - Herzog, Marc A1 - von Korff Schmising, Clemens A1 - Shayduk, Roman A1 - Leitenberger, Wolfram A1 - Gaa, P. A1 - Bargheer, Matias T1 - Normalization schemes for ultrafast x-ray diffraction using a table-top laser-driven plasma source JF - Review of scientific instruments : a monthly journal devoted to scientific instruments, apparatus, and techniques N2 - We present an experimental setup of a laser-driven x-ray plasma source for femtosecond x-ray diffraction. Different normalization schemes accounting for x-ray source intensity fluctuations are discussed in detail. We apply these schemes to measure the temporal evolution of Bragg peak intensities of perovskite superlattices after ultrafast laser excitation. Y1 - 2012 U6 - https://doi.org/10.1063/1.3681254 SN - 0034-6748 VL - 83 IS - 2 PB - American Institute of Physics CY - Melville ER - TY - THES A1 - Pudell, Jan-Etienne T1 - Lattice dynamics T1 - Gitterdynamik BT - observed with x-ray diffraction BT - beobachtet mit Röntgenbeugung N2 - In this thesis I summarize my contribution to the research field of ultrafast structural dynamics in condensend matter. It consists of 17 publications that cover the complex interplay between electron, magnon, and phonon subsystems in solid materials and the resulting lattice dynamics after ultrafast photoexcitation. The investigation of such dynamics is necessary for the physical understanding of the processes in materials that might become important in the future as functional materials for technological applications, for example in data storage applications, information processing, sensors, or energy harvesting. In this work I present ultrafast x-ray diffraction (UXRD) experiments based on the optical pump – x-ray probe technique revealing the time-resolved lattice strain. To study these dynamics the samples (mainly thin film heterostructures) are excited by femtosecond near-infrared or visible light pulses. The induced strain dynamics caused by stresses of the excited subsystems are measured in a pump-probe scheme with x-ray diffraction (XRD) as a probe. The UXRD setups used during my thesis are a laser-driven table-top x-ray source and large-scale synchrotron facilities with dedicated time-resolved diffraction setups. The UXRD experiments provide quantitative access to heat reservoirs in nanometric layers and monitor the transient responses of these layers with coupled electron, magnon, and phonon subsystems. In contrast to optical probes, UXRD allows accessing the material-specific information, which is unavailable for optical light due to the detection of multiple indistinguishable layers in the range of the penetration depth. In addition, UXRD facilitates a layer-specific probe for layers buried opaque heterostructures to study the energy flow. I extended this UXRD technique to obtain the driving stress profile by measuring the strain dynamics in the unexcited buried layer after excitation of the adjacent absorbing layers with femtosecond laser pulses. This enables the study of negative thermal expansion (NTE) in magnetic materials, which occurs due to the loss of the magnetic order. Part of this work is the investigation of stress profiles which are the source of coherent acoustic phonon wave packets (hypersound waves). The spatiotemporal shape of these stress profiles depends on the energy distribution profile and the ability of the involved subsystems to produce stress. The evaluation of the UXRD data of rare-earth metals yields a stress profile that closely matches the optical penetration profile: In the paramagnetic (PM) phase the photoexcitation results in a quasi-instantaneous expansive stress of the metallic layer whereas in the antiferromagnetic (AFM) phase a quasi-instantaneous contractive stress and a second contractive stress contribution rising on a 10 ps time scale adds to the PM contribution. These two time scales are characteristic for the magnetic contribution and are in agreement with related studies of the magnetization dynamics of rare-earth materials. Several publications in this thesis demonstrate the scientific progress in the field of active strain control to drive a second excitation or engineer an ultrafast switch. These applications of ultrafast dynamics are necessary to enable control of functional material properties via strain on ultrafast time scales. For this thesis I implemented upgrades of the existing laser-driven table-top UXRD setup in order to achieve an enhancement of x-ray flux to resolve single digit nanometer thick layers. Furthermore, I developed and built a new in-situ time-resolved magneto-optic Kerr effect (MOKE) and optical reflectivity setup at the laser-driven table-top UXRD setup to measure the dynamics of lattice, electrons and magnons under the same excitation conditions. N2 - In dieser Doktoarbeit sind meine Beiträge zum Forschungsgebiet der ltraschnellen Strukturdynamik in kondensierter Materie zusammegefasst. Sie besteht aus 17 Publikationen, welche dieWechselwirkung zwischen Elektron-, Magnon- und Phononsystem in Festkörpern, sowie die dadurch verursachte Gitterdynamik nach ultraschneller optischer Anregung diskutieren. Die Untersuchung dieser Dynamik ist erforderlich für das physikalische Verständnis der Prozesse in Materialien, die in Zukunft als Funktionsmaterialien für technologische Anwendungen, z.B. in der Datenspeicherung und Informationsverarbeitung, sowie bei Sensoren und der Energiegewinnung, wichtig werden könnten. In dieser Arbeit präsentiere ich Experimente, welche ultraschneller Röntgenbeugung (UXRD) als Technik nutzen. Sie basiert auf der Anrege-Abfrage-Technik: Die Dynamik in der Probe (hauptsächlich Dünnfilm-Heterostrukturen) wird durch Femtosekunden-Lichtpulse im nahen Infrarot oder im sichtbaren Bereich angeregt. Die Dehnung des Materials, welche die Spannung (Druck) der angeregten Teilsysteme hervorruft, wird mit Röntgenbeugung als Abfrage gemessen. Während meiner Doktorandentätigkeit habe ich zwei Arten von Aufbauten zur UXRD genutzt: lasergetriebene laborbasierte Röntgenquellen und Synchrotronstrahlungsquellen mit zugehörigen zeitaufgelösten Messinstrumenten. Mit den UXRD-Experimenten kann die gespeicherte Energie unterschiedlicher gekoppelter Teilsysteme, wie Elektronen, Mangonen und Phononen, einer nur wenige Nanometer dicken Schicht gemessen werden. Im Vergleich zu optischenMesstechniken bietet UXRD den Zugriff auf materialspezifische Informationen, die für optisches Licht aufgrund der Detektion mehrerer nicht unterscheidbarer Schichten im Bereich der Eindringtiefe nicht zur Verfügung steht. Darüber hinaus lässt sich mit UXRD eine für optische Detektion verdeckte Schicht als schichtspezifische Sonde nutzen, um den Energietransport zu untersuchen. Dieses Prinzip wurde dazu genutzt, um das treibende Spannungsprofil mittels der Dehnungsdynamik in einer angrenzenden, optisch nicht angeregten Schicht zu messen. Dies ermöglichte die Untersuchung der Dichteanomalie in magnetischen Materialen, die durch den Verlust der magnetischen Ordnung entsteht. Ebenfalls Teil dieser Arbeit ist die Untersuchung von Spannungsprofilen als Quelle von kohärenten akustischen Phononen (Hyperschallwellen). Das raumzeitliche Profil des Spannungsprofils hängt von der Energieverteilung innerhalb der Teilsysteme und ihrer Fähigkeit ab, Energie in Dehnung umzusetzen. Die Auswertung von UXRD Experimenten an Metallen der Seltenen Erden ergab ein Spannungsprofil, dass dem Absorptionsprofil der optischen Anregung entsprach: In der paramagnetischen Phase erzeugte es einen instantanen expansiven Druck, wohingegen in der antiferromagnetischen Phase ein instantaner und ein auf einer 10 ps Zeitskala ansteigender kontrahierender Druck zusätzlich auftritt. Die beiden charakteristischen Zeitskalen in der antiferromagnetischen Phase sind in Übereinstimmung mit verschiedenen Studien der Demagnetisierungsdynamik in den Metallen der Seltenen Erden. Einige Publikationen dieser Arbeit beschäftigen sich mit Feld der aktiven Dehnungskontrolle. Dies ermöglich die Kontrolle von Funktionsmaterialen via Dehnung auf ultraschnellen Zeitskalen. Im Rahmen meiner Doktorandentätigkeit habe ich den lasergetriebenen UXRD Aufbau optimiert, um mit dem hohen Röntgenfluss Experimente mit nur einigen Nanometer dicken Schichten zu ermöglichen. Diese Maschine habe ich um einen zeitaufgelösten Aufbau zur in situ Messung der Reflektivität und Magnetisierungsdynamik mittels magnetooptischem Kerr-Effekt ergänzt. Dies ermöglicht die gleichzeitige Messung von Gitter-, Elektronen- und Magnonendynamik unter derselben Anregebedingung. KW - ultrafast x-ray diffraction KW - ultraschnelle Röntgendiffraktion KW - lattice dynamics KW - Gitterdynamik KW - nanoscale heat transfer KW - nanoskaliger Wärmetransport KW - ultrafast magnetism KW - ultraschneller Magnetimus KW - mechanical and acoustical properties KW - mechanische und akustische Eigenschaften Y1 - 2020 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-484453 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 - Haseeb, Haider T1 - Charge and heat transport across interfaces in nanostructured porous silicon T1 - Ladungs- und Wärmetransport über Grenzflächen in nanostrukturiertem porösem Silizium N2 - This thesis discusses heat and charge transport phenomena in single-crystalline Silicon penetrated by nanometer-sized pores, known as mesoporous Silicon (pSi). Despite the extensive attention given to it as a thermoelectric material of interest, studies on microscopic thermal and electronic transport beyond its macroscopic characterizations are rarely reported. In contrast, this work reports the interplay of both. PSi samples synthesized by electrochemical anodization display a temperature dependence of specific heat 𝐶𝑝 that deviates from the characteristic 𝑇^3 behaviour (at 𝑇<50𝐾). A thorough analysis reveals that both 3D and 2D Einstein and Debye modes contribute to this specific heat. Additional 2D Einstein modes (~3 𝑚𝑒𝑉) agree reasonably well with the boson peak of SiO2 in pSi pore walls. 2D Debye modes are proposed to account for surface acoustic modes causing a significant deviation from the well-known 𝑇^3 dependence of 𝐶𝑝 at 𝑇<50𝐾. A novel theoretical model gives insights into the thermal conductivity of pSi in terms of porosity and phonon scattering on the nanoscale. The thermal conductivity analysis utilizes the peculiarities of the pSi phonon dispersion probed by the inelastic neutron scattering experiments. A phonon mean-free path of around 10 𝑛𝑚 extracted from the presented model is proposed to cause the reduced thermal conductivity of pSi by two orders of magnitude compared to p-doped bulk Silicon. Detailed analysis indicates that compound averaging may cause a further 10-50% reduction. The percolation threshold of 65% for thermal conductivity of pSi samples is subsequently determined by employing theoretical effective medium models. Temperature-dependent electrical conductivity measurements reveal a thermally activated transport process. A detailed analysis of the activation energy 𝐸𝐴𝜎 in the thermally activated transport exhibits a Meyer Neldel compensation rule between different samples that originates in multi-phonon absorption upon carrier transport. Activation energies 𝐸𝐴𝑆 obtained from temperature-dependent thermopower measurements provide further evidence for multi-phonon assisted hopping between localized states as a dominant charge transport mechanism in pSi, as they systematically differ from the determined 𝐸𝐴𝜎 values. N2 - Diese Dissertation befasst sich mit Wärme- und Ladungstransportphänomenen in mesoporösem Silizium (pSi) oder etwas genauer in einkristallinem Silizium, welches mit nanometergroßen Poren durchsetzt ist. Trotz der großen Aufmerksamkeit, die diesem thermoelektrischen Material zuteil wird, wird nur selten über Studien zum mikroskopischen thermischen und elektronischen Transport jenseits seiner makroskopischen Charakterisierung berichtet. Im Gegensatz dazu wird in dieser Studie das Zusammenspiel von beidem untersucht. PSi-Proben, die durch elektrochemische Anodisierung synthetisiert wurden, zeigen eine Temperaturabhängigkeit der spezifischen Wärme 𝐶𝑝, die vom charakteristischen 𝑇3 Verhalten (bei 𝑇<50𝐾) abweicht. Eine gründliche Analyse zeigt, dass sowohl 3D- als auch 2D-Einstein- und Debye-Moden zu dieser spezifischen Wärme beitragen. Zusätzliche 2D-Einstein-Moden (~3 𝑚𝑒𝑉) stimmen gut mit dem Bosonen-Peak von SiO2 in teilweise oxidierten pSi-Porenwänden überein. 2D-Debye-Moden werden vorgeschlagen, um akustische Oberflächenmoden zu erklären, die eine signifikante Abweichung von der bekannten 𝑇3Abhängigkeit von 𝐶𝑝 bei 𝑇<50𝐾 verursachen. Ein neuartiges theoretisches Modell gibt Einblicke in die Wärmeleitfähigkeit von pSi in Bezug auf Porosität und Phononenstreuung auf der Nanoskala. Die Analyse der Wärmeleitfähigkeit nutzt die Besonderheiten der pSi-Phononendispersion, die durch Experimente mit inelastischer Neutronenstreuung untersucht wurden. Ein mittlerer freier Weg der Phononen von etwa 10 𝑛𝑚, der aus dem vorgestellten Modell extrahiert wurde, wird als Ursache für die um zwei Größenordnungen geringere Wärmeleitfähigkeit von pSi im Vergleich zu p-dotiertem Silizium vorgeschlagen. Eine detaillierte Analyse zeigt, dass die Porosität selbst eine weitere Verringerung der Wärmeleitfähigkeit um 10-50% verursachen kann. Die Perkolationsschwelle von 65 % für die Wärmeleitfähigkeit von pSi-Proben wird anschließend mit Hilfe eines theoretischen Ansatzes für effektive Medien bestimmt. Temperaturabhängige Messungen der elektrischen Leitfähigkeit lassen einen thermisch aktivierten Transportprozess erkennen. Eine detaillierte Analyse der Aktivierungsenergie 𝐸𝐴𝜎 im thermisch aktivierten Transport zeigt eine Meyer-Neldel-Kompensationsregel zwischen verschiedenen Proben, die auf Multiphononenabsorption beim Ladungsträgertransport zurückzuführen ist. Aktivierungsenergien 𝐸𝐴𝑆, die aus temperaturabhängigen Seebeck-Messungen gewonnen wurden, liefern weitere Beweise für Multiphononen-unterstütztes Springen zwischen lokalisierten Zuständen als dominanten Ladungstransportmechanismus in pSi, da sie sich systematisch von den ermittelten 𝐸𝐴𝜎 Werten unterscheiden. KW - mesoporous KW - silicon KW - Meyer-Neldel-rule KW - nanomaterials KW - Meyer-Neldel-Regel KW - mesoporös KW - Nanomaterialien KW - Silizium Y1 - 2023 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-611224 ER - TY - JOUR A1 - Deb, Marwan A1 - Popova, Elena A1 - Hehn, Michel A1 - Keller, Niels A1 - Petit-Watelot, Sebastien A1 - Bargheer, Matias A1 - Mangin, Stephane A1 - Malinowski, Gregory T1 - Femtosecond Laser-Excitation-Driven High Frequency Standing Spin Waves in Nanoscale Dielectric Thin Films of Iron Garnets JF - Physical review letters N2 - We demonstrate that femtosecond laser pulses allow triggering high-frequency standing spin-wave modes in nanoscale thin films of a bismuth-substituted yttrium iron garnet. By varying the strength of the external magnetic field, we prove that two distinct branches of the dispersion relation are excited for all the modes. This is reflected in particular at a very weak magnetic field (similar to 33 mT) by a spin dynamics with a frequency up to 15 GHz, which is 15 times higher than the one associated with the ferromagnetic resonance mode. We argue that this phenomenon is triggered by ultrafast changes of the magnetic anisotropy via laser excitation of incoherent and coherent phonons. These findings open exciting prospects for ultrafast photo magnonics. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevLett.123.027202 SN - 0031-9007 SN - 1079-7114 VL - 123 IS - 2 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Sarhan, Radwan Mohamed A1 - Koopman, Wouter-Willem Adriaan A1 - Schuetz, Roman A1 - Schmid, Thomas A1 - Liebig, Ferenc A1 - Koetz, Joachim A1 - Bargheer, Matias T1 - The importance of plasmonic heating for the plasmondriven photodimerization of 4-nitrothiophenol JF - Scientific Reports N2 - Metal nanoparticles form potent nanoreactors, driven by the optical generation of energetic electrons and nanoscale heat. The relative influence of these two factors on nanoscale chemistry is strongly debated. This article discusses the temperature dependence of the dimerization of 4-nitrothiophenol (4-NTP) into 4,4′-dimercaptoazobenzene (DMAB) adsorbed on gold nanoflowers by Surface-Enhanced Raman Scattering (SERS). Raman thermometry shows a significant optical heating of the particles. The ratio of the Stokes and the anti-Stokes Raman signal moreover demonstrates that the molecular temperature during the reaction rises beyond the average crystal lattice temperature of the plasmonic particles. The product bands have an even higher temperature than reactant bands, which suggests that the reaction proceeds preferentially at thermal hot spots. In addition, kinetic measurements of the reaction during external heating of the reaction environment yield a considerable rise of the reaction rate with temperature. Despite this significant heating effects, a comparison of SERS spectra recorded after heating the sample by an external heater to spectra recorded after prolonged illumination shows that the reaction is strictly photo-driven. While in both cases the temperature increase is comparable, the dimerization occurs only in the presence of light. Intensity dependent measurements at fixed temperatures confirm this finding. KW - enhanced raman-scattering KW - charge-transfer KW - metal KW - nanoparticles KW - catalysis KW - AU KW - 4-nitrobenzenethiol KW - aminothiophenol KW - photocatalysis KW - wavelength Y1 - 2019 U6 - https://doi.org/10.1038/s41598-019-38627-2 SN - 2045-2322 VL - 9 PB - Macmillan Publishers Limited CY - London ER - TY - JOUR A1 - Iurchuk, V. A1 - Schick, D. A1 - Bran, J. A1 - Colson, D. A1 - Forget, A. A1 - Halley, D. A1 - Koc, Azize A1 - Reinhardt, Mathias A1 - Kwamen, C. A1 - Morley, N. A. A1 - Bargheer, Matias A1 - Viret, M. A1 - Gumeniuk, R. A1 - Schmerber, G. A1 - Doudin, B. A1 - Kundys, B. T1 - Optical Writing of Magnetic Properties by Remanent Photostriction JF - Physical review letters N2 - We present an optically induced remanent photostriction in BiFeO3, resulting from the photovoltaic effect, which is used to modify the ferromagnetism of Ni film in a hybrid BiFeO3/Ni structure. The 75% change in coercivity in the Ni film is achieved via optical and nonvolatile control. This photoferromagnetic effect can be reversed by static or ac electric depolarization of BiFeO3. Hence, the strain dependent changes in magnetic properties are written optically, and erased electrically. Light-mediated straintronics is therefore a possible approach for low-power multistate control of magnetic elements relevant for memory and spintronic applications. Y1 - 2016 U6 - https://doi.org/10.1103/PhysRevLett.117.107403 SN - 0031-9007 SN - 1079-7114 VL - 117 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Shayduk, Roman A1 - Herzog, Marc A1 - Bojahr, Andre A1 - Schick, Daniel A1 - Gaal, Peter A1 - Leitenberger, Wolfram A1 - Navirian, Hengameh A1 - Sander, Mathias A1 - Goldshteyn, Jevgenij A1 - Vrejoiu, Ionela A1 - Bargheer, Matias T1 - Direct time-domain sampling of subterahertz coherent acoustic phonon spectra in SrTiO3 using ultrafast x-ray diffraction JF - Physical review : B, Condensed matter and materials physics N2 - We synthesize sub-THz longitudinal quasimonochromatic acoustic phonons in a SrTiO3 single crystal using a SrRuO3/SrTiO3 superlattice as an optical-acoustic transducer. The generated acoustic phonon spectrum is determined using ultrafast x-ray diffraction. The analysis of the generated phonon spectrum in the time domain reveals a k-vector dependent phonon lifetime. It is observed that even at sub-THz frequencies the phonon lifetime agrees with the 1/omega(2) power law known from Akhiezer's model for hyper sound attenuation. The observed shift of the synthesized spectrum to the higher q is discussed in the framework of nonlinear effects appearing due to the high amplitude of the synthesized phonons. Y1 - 2013 U6 - https://doi.org/10.1103/PhysRevB.87.184301 SN - 1098-0121 VL - 87 IS - 18 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Reinhardt, Matthias A1 - Koc, Azize A1 - Leitenberger, Wolfram A1 - Gaal, Peter A1 - Bargheer, Matias T1 - Optimized spatial overlap in optical pump-X-ray probe experiments with high repetition rate using laser-induced surface distortions JF - Journal of synchrotron radiation N2 - Ultrafast X-ray diffraction experiments require careful adjustment of the spatial overlap between the optical excitation and the X-ray probe pulse. This is especially challenging at high laser repetition rates. Sample distortions caused by the large heat load on the sample and the relatively low optical energy per pulse lead to only tiny signal changes. In consequence, this results in small footprints of the optical excitation on the sample, which turns the adjustment of the overlap difficult. Here a method for reliable overlap adjustment based on reciprocal space mapping of a laser excited thin film is presented. KW - ultrafast X-ray diffraction KW - nanostructures KW - surface deformation KW - heat diffusion KW - optical pump Y1 - 2016 U6 - https://doi.org/10.1107/S1600577515024443 SN - 1600-5775 VL - 23 SP - 474 EP - 479 PB - International Union of Crystallography CY - Chester ER - TY - THES A1 - Tchoumba Kwamen, Christelle Larodia T1 - Investigating the dynamics of polarization reversal in ferroelectric thin films by time-resolved X-ray diffraction T1 - Untersuchung der Dynamik der Polarisationsumkehr in ferroelektrischen Dünnschichten durch zeitaufgelöste Röntgenbeugung N2 - Ferroic materials have attracted a lot of attention over the years due to their wide range of applications in sensors, actuators, and memory devices. Their technological applications originate from their unique properties such as ferroelectricity and piezoelectricity. In order to optimize these materials, it is necessary to understand the coupling between their nanoscale structure and transient response, which are related to the atomic structure of the unit cell. In this thesis, synchrotron X-ray diffraction is used to investigate the structure of ferroelectric thin film capacitors during application of a periodic electric field. Combining electrical measurements with time-resolved X-ray diffraction on a working device allows for visualization of the interplay between charge flow and structural motion. This constitutes the core of this work. The first part of this thesis discusses the electrical and structural dynamics of a ferroelectric Pt/Pb(Zr0.2,Ti0.8)O3/SrRuO3 heterostructure during charging, discharging, and polarization reversal. After polarization reversal a non-linear piezoelectric response develops on a much longer time scale than the RC time constant of the device. The reversal process is inhomogeneous and induces a transient disordered domain state. The structural dynamics under sub-coercive field conditions show that this disordered domain state can be remanent and can be erased with an appropriate voltage pulse sequence. The frequency-dependent dynamic characterization of a Pb(Zr0.52,Ti0.48)O3 layer, at the morphotropic phase boundary, shows that at high frequency, the limited domain wall velocity causes a phase lag between the applied field and both the structural and electrical responses. An external modification of the RC time constant of the measurement delays the switching current and widens the electromechanical hysteresis loop while achieving a higher compressive piezoelectric strain within the crystal. In the second part of this thesis, time-resolved reciprocal space maps of multiferroic BiFeO3 thin films were measured to identify the domain structure and investigate the development of an inhomogeneous piezoelectric response during the polarization reversal. The presence of 109° domains is evidenced by the splitting of the Bragg peak. The last part of this work investigates the effect of an optically excited ultrafast strain or heat pulse propagating through a ferroelectric BaTiO3 layer, where we observed an additional current response due to the laser pulse excitation of the metallic bottom electrode of the heterostructure. N2 - Ferroika haben aufgrund vielfältiger Anwendungsmöglichkeiten in Sensoren, Motoren und Speichermedien in den letzten Jahren viel Aufmerksamkeit erhalten. Das Interesse für technologische Anwendungen ist in ihren einzigartigen Eigenschaften wie Ferroelektrizität und Piezoelektrizität begründet. Um die Eigenschaften dieser Materialien zu optimieren ist es notwendig, die Kopplung zwischen ihrer Nanostruktur und der zeitabhängigen Antwort auf die Anregung zu verstehen, welcher von der Atomstruktur der Einheitszelle abhängig ist. In dieser Arbeit wird Röntgenbeugung an einem Synchrotron verwendet, um die Struktur eines ferroelektrischen Dünnschichtkondensators während eines angelegten elektrischen Feld zu beobachten. Den Kern dieser Arbeit bildet die Kombination aus elektrischen zeitaufgelösten Röntgenbeugungsmessungen an einem betriebsfähigen Kondensator, was die Visualisierung des Zusammenspiels zwischen Ladungsbewegung und Strukturdynamik ermöglicht. Der erste Teil der Arbeit befasst sich mit der elektrischen und strukturellen Dynamik einer ferroelektrischen Pt/Pb(Zr0.2,Ti0.8)O3/SrRuO3 Heterostruktur während des Ladens, Entladens und der Polarisationsumkehr. Nach der Umkehr der Polarisation bildet sich auf einer längeren Zeitskala als die RC-Zeitkonstante der Probe ein nichtlineares piezoelektrisches Signal aus. Der Umkehrungsprozess ist inhomogen und induziert einen vorübergehenden Zustand ungeordneter Domänen. Die strukturelle Dynamik mit einem angelegten elektrischen Feld unterhalb des Koerzitivfelds zeigt, dass dieser ungeordnete Zustand remanent sein kann und mit einer entsprechenden Abfolge von Spannungspulsen wieder entfernt werden kann. Die frequenzabhängige Charakterisierung der Dynamik einer Pb(Zr0.52,Ti0.48)O3 Schicht mit einer Zusammensetzung, die der morphotropen Phasengrenze entspricht, zeigt, dass bei hohen Frequenzen die begrenzte Domänenwandgeschwindigkeit eine Phasenverzögerung zwischen dem angelegten Feld und dem strukturellen sowie dem elektrischen Signal verursacht. Eine externe Änderung der RC-Zeitkonstante verzögert den Schaltstrom und verbreitert die elektromechanische Hysteresekurve, während im Kristall eine höhere kompressive piezoeletrische Spannung erzeugt wird. In dem zweiten Teil dieser Arbeit wurde der reziproke Raum von multiferroischen dünnen BiFeO3 Filmen vermessen, um die Domänenstruktur zu identifizieren und die Entwicklung eines inhomogenen piezoelektrischen Signals während der Polarisationsumkehr zu untersuchen. Das Aufspalten des Bragg Reflexes ist ein Hinweis auf die Existenz von 109° Domänen. Der letzte Teil der Arbeit beschäftigt sich mit dem Effekt, den ein durch optische Anregung erzeugter ultraschneller Verspannungs- oder Wärmepuls hervorruft, der durch eine ferroelektrische BaTiO3 Schicht propagiert. Dabei wurde durch die Anregung der unteren metallischen Elektrode der Heterostruktur durch den Laserpuls ein zusätzliches Ladungssignal beobachtet. KW - ferroelectrics KW - X-ray diffraction KW - structural dynamics KW - Ferroelektrika KW - Röntgenbeugung KW - Strukturdynamik Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-427815 ER - TY - JOUR A1 - Deb, Marwan A1 - Popova, Elena A1 - Hehn, Michel A1 - Keller, Niels A1 - Petit-Watelot, Sebastien A1 - Bargheer, Matias A1 - Mangin, Stephane A1 - Malinowski, Gregory T1 - Damping of Standing Spin Waves in Bismuth-Substituted Yttrium Iron Garnet as Seen via the Time-Resolved Magneto-Optical Kerr Effect JF - Physical review applied N2 - We investigate spin-wave resonance modes and their damping in insulating thin films of bismuth-substituted yttrium iron garnet by performing femtosecond magneto-optical pump-probe experiments. For large magnetic fields in the range below the magnetization saturation, we find that the damping of high-order standing spin-wave (SSW) modes is about 40 times lower than that for the fundamental one. The observed phenomenon can be explained by considering different features of magnetic anisotropy and exchange fields that, respectively, define the precession frequency for fundamental and high-order SSWs. These results provide further insight into SSWs in iron garnets and may be exploited in many new photomagnonic devices. Y1 - 2019 U6 - https://doi.org/10.1103/PhysRevApplied.12.044006 SN - 2331-7019 VL - 12 IS - 4 PB - American Physical Society CY - College Park ER - TY - THES A1 - Jay, Raphael Martin T1 - Principles of charge distribution and separation BT - the case of iron complexes probed by X-ray spectroscopy N2 - The electronic charge distributions of transition metal complexes fundamentally determine their chemical reactivity. Experimental access to the local valence electronic structure is therefore crucial in order to determine how frontier orbitals are delocalized between different atomic sites and electronic charge is spread throughout the transition metal complex. To that end, X-ray spectroscopies are employed in this thesis to study a series of solution-phase iron complexes with respect to the response of their local electronic charge distributions to different external influences. Using resonant inelastic X-ray scattering (RIXS) and X-ray absorption spectroscopy (XAS) at the iron L-edge, changes in local charge densities are investigated at the iron center depending on different ligand cages as well as solvent environments. A varying degree of charge delocalization from the metal center onto the ligands is observed, which is governed by the capabilities of the ligands to accept charge density into their unoccupied orbitals. Specific solvents are furthermore shown to amplify this process. Solvent molecules of strong Lewis-acids withdraw charge from the ligand allowing in turn for more metal charge to be delocalized onto the ligand. The resulting local charge deficiencies at the metal center are, however, counteracted by competing electron-donation channels from the ligand towards the iron, which are additionally revealed. This is interpreted as a compensating effect which strives to maintain local charge densities at the iron center. This mechanism of charge density preservation is found to be of general nature. Using time-resolved RIXS and XAS at the iron L-edge, an analogous interplay of electron donation and back-donation channels is also revealed for the case of charge-transfer excited states. In such transient configurations, the electronic occupation of iron-centered frontier orbitals has been altered by an optical excitation. Changes in local charge densities that are expected to follow an increased or decreased population of iron-centered orbitals are, however, again counteracted. By scaling the degree of electron donation from the ligand onto the metal, local charge densities at the iron center can be efficiently maintained. Since charge-transfer excitations, however, often constitute the initial step in many electron transfer processes, these findings challenge common notions of charge-separation in transition metal dyes. KW - L-edge spectroscopy KW - charge-transfer excitations KW - transition metal complexes KW - electronic structure KW - photo-chemical pathways Y1 - 2020 ER - TY - JOUR A1 - Bojahr, Andre A1 - Herzog, Marc A1 - Schick, Daniel A1 - Vrejoiu, Ionela A1 - Bargheer, Matias T1 - Calibrated real-time detection of nonlinearly propagating strain waves JF - Physical review : B, Condensed matter and materials physics N2 - Epitaxially grown metallic oxide transducers support the generation of ultrashort strain pulses in SrTiO3 (STO) with high amplitudes up to 0.5%. The strain amplitudes are calibrated by real-time measurements of the lattice deformation using ultrafast x-ray diffraction. We determine the speed at which the strain fronts propagate by broadband picosecond ultrasonics and conclude that, above a strain level of approx. 0.2%, the compressive and tensile strain components travel at considerably different sound velocities, indicating nonlinear wave behavior. Simulations based on an anharmonic linear-chain model are in excellent accord with the experimental findings and show how the spectrum of coherent phonon modes changes with time. Y1 - 2012 U6 - https://doi.org/10.1103/PhysRevB.86.144306 SN - 1098-0121 VL - 86 IS - 14 PB - American Physical Society CY - College Park ER - TY - JOUR A1 - Kiel, Mareike A1 - Möhwald, Helmuth A1 - Bargheer, Matias T1 - Broadband measurements of the transient optical complex dielectric function of a nanoparticle/polymer composite upon ultrafast excitation JF - Physical review : B, Condensed matter and materials physics N2 - We determined experimentally the complex transient optical dielectric function of a well-characterized polyelectrolyte/gold-nanoparticle composite system over a broad spectral range upon short pulse laser excitation by simultaneously measuring the time-dependent reflectance and transmittance of white light pulses with femtosecond pump-probe spectroscopy. We extracted directly the ultrafast changes in the real and imaginary parts of the effective dielectric function, epsilon(eff)(r) (omega,t)and epsilon(eff)(i) (omega,t), from the experiment. This complete experimental set of information on the time-dependent complex dielectric function challenges theories modeling the transient dielectric function of gold particles and the effective medium. Y1 - 2011 U6 - https://doi.org/10.1103/PhysRevB.84.165121 SN - 1098-0121 VL - 84 IS - 16 PB - American Physical Society CY - College Park ER -