@article{ShaydukHallmannRodriguezFernandezetal.2022, author = {Shayduk, Roman and Hallmann, J{\"o}rg and Rodriguez-Fernandez, Angel and Scholz, Markus and Lu, Wei and B{\"o}senberg, Ulrike and M{\"o}ller, Johannes and Zozulya, Alexey and Jiang, Man and Wegner, Ulrike and Secareanu, Radu-Costin and Palmer, Guido and Emons, Moritz and Lederer, Max and Volkov, Sergey and Lindfors-Vrejoiu, Ionela and Schick, Daniel and Herzog, Marc and Bargheer, Matias and Madsen, Anders}, title = {Femtosecond x-ray diffraction study of multi-THz coherent phonons in SrTiO3}, series = {Applied physics letters}, volume = {120}, journal = {Applied physics letters}, number = {20}, publisher = {AIP Publishing}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/5.0083256}, pages = {5}, year = {2022}, abstract = {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.}, language = {en} } @article{MatternvonReppertZeuschneretal.2022, author = {Mattern, Maximilian and von Reppert, Alexander and Zeuschner, Steffen Peer and Pudell, Jan-Etienne and K{\"u}hne, F. and Diesing, Detlef and Herzog, Marc and Bargheer, Matias}, title = {Electronic energy transport in nanoscale Au/Fe hetero-structures in the perspective of ultrafast lattice dynamics}, series = {Applied physics letters}, volume = {120}, journal = {Applied physics letters}, number = {9}, publisher = {AIP Publishing}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/5.0080378}, pages = {5}, year = {2022}, abstract = {We study the ultrafast electronic transport of energy in a photoexcited nanoscale Au/Fe hetero-structure by modeling the spatiotemporal profile of energy densities that drives transient strain, which we quantify by femtosecond x-ray diffraction. This flow of energy is relevant for intrinsic demagnetization and ultrafast spin transport. We measured lattice strain for different Fe layer thicknesses ranging from few atomic layers to several nanometers and modeled the spatiotemporal flow of energy densities. The combination of a high electron-phonon coupling coefficient and a large Sommerfeld constant in Fe is found to yield electronic transfer of nearly all energy from Au to Fe within the first hundreds of femtoseconds.}, language = {en} } @article{MorHerzogNoacketal.2018, author = {Mor, Selene and Herzog, Marc and Noack, Johannes and Katayama, Naoyuki and Nohara, Minoru and Takagi, Hide and Trunschke, Annette and Mizokawa, Takashi and Monney, Claude and St{\"a}hler, Julia}, title = {Inhibition of the photoinduced structural phase transition in the excitonic insulator Ta2NiSe5}, series = {Physical review : B, Condensed matter and materials physics}, volume = {97}, journal = {Physical review : B, Condensed matter and materials physics}, number = {11}, publisher = {American Physical Society}, address = {College Park}, issn = {2469-9950}, doi = {10.1103/PhysRevB.97.115154}, pages = {5}, year = {2018}, abstract = {Femtosecond time-resolved midinfrared reflectivity is used to investigate the electron and phonon dynamics occurring at the direct band gap of the excitonic insulator Ta2NiSe5 below the critical temperature of its structural phase transition. We find that the phonon dynamics show a strong coupling to the excitation of free carriers at the Gamma point of the Brillouin zone. The optical response saturates at a critical excitation fluence F-C = 0.30 +/- 0.08 mJ/cm(2) due to optical absorption saturation. This limits the optical excitation density in Ta2NiSe5 so that the system cannot be pumped sufficiently strongly to undergo the structural change to the high-temperature phase. We thereby demonstrate that Ta2NiSe5 exhibits a blocking mechanism when pumped in the near-infrared regime, preventing a nonthermal structural phase transition.}, language = {en} } @article{PudellMaznevHerzogetal.2018, author = {Pudell, Jan-Etienne and Maznev, A. A. and Herzog, Marc and Kronseder, M. and Back, Christian H. and Malinowski, Gregory and von Reppert, Alexander and Bargheer, Matias}, title = {Layer specific observation of slow thermal equilibration in ultrathin metallic nanostructures by femtosecond X-ray diffraction}, series = {Nature Communications}, volume = {9}, journal = {Nature Communications}, publisher = {Nature Publ. Group}, address = {London}, issn = {2041-1723}, doi = {10.1038/s41467-018-05693-5}, pages = {7}, year = {2018}, abstract = {Ultrafast heat transport in nanoscale metal multilayers is of great interest in the context of optically induced demagnetization, remagnetization and switching. If the penetration depth of light exceeds the bilayer thickness, layer-specific information is unavailable from optical probes. Femtosecond diffraction experiments provide unique experimental access to heat transport over single digit nanometer distances. Here, we investigate the structural response and the energy flow in the ultrathin double-layer system: gold on ferromagnetic nickel. Even though the excitation pulse is incident from the Au side, we observe a very rapid heating of the Ni lattice, whereas the Au lattice initially remains cold. The subsequent heat transfer from Ni to the Au lattice is found to be two orders of magnitude slower than predicted by the conventional heat equation and much slower than electron-phonon coupling times in Au. We present a simplified model calculation highlighting the relevant thermophysical quantities.}, language = {en} } @article{vonReppertWilligPudelletal.2018, author = {von Reppert, Alexander and Willig, Lisa and Pudell, Jan-Etienne and Roessle, M. and Leitenberger, Wolfram and Herzog, Marc and Ganss, F. and Hellwig, O. and Bargheer, Matias}, title = {Ultrafast laser generated strain in granular and continuous FePt thin films}, series = {Applied physics letters}, volume = {113}, journal = {Applied physics letters}, number = {12}, publisher = {American Institute of Physics}, address = {Melville}, issn = {0003-6951}, doi = {10.1063/1.5050234}, pages = {5}, year = {2018}, abstract = {We employ ultrafast X-ray diffraction to compare the lattice dynamics of laser-excited continuous and granular FePt films on MgO (100) substrates. Contrary to recent results on free-standing granular films, we observe in both cases a pronounced and long-lasting out-of-plane expansion. We attribute this discrepancy to the in-plane expansion, which is suppressed by symmetry in continuous films. Granular films on substrates are less constrained and already show a reduced out-of-plane contraction. Via the Poisson effect, out-of-plane contractions drive in-plane expansion and vice versa. Consistently, the granular film exhibits a short-lived out-of-plane contraction driven by ultrafast demagnetization which is followed by a reduced and delayed expansion. From the acoustic reflections of the observed strain waves at the film-substrate interface, we extract a 13\% reduction of the elastic constants in thin 10 nm FePt films compared to bulk-like samples. (C) 2018 Author(s).}, language = {en} } @article{ZeuschnerMatternPudelletal.2021, author = {Zeuschner, S. P. and Mattern, M. and Pudell, Jan-Etienne and von Reppert, A. and R{\"o}ssle, M. and Leitenberger, Wolfram and Schwarzkopf, J. and Boschker, J. E. and Herzog, Marc and Bargheer, Matias}, title = {Reciprocal space slicing}, series = {Structural Dynamics}, volume = {8}, journal = {Structural Dynamics}, publisher = {AIP Publishing LLC}, address = {Melville, NY}, issn = {2329-7778}, doi = {10.1063/4.0000040}, pages = {11}, year = {2021}, abstract = {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.}, language = {en} } @article{PudellvonReppertSchicketal.2019, author = {Pudell, Jan-Etienne and von Reppert, Alexander and Schick, D. and Zamponi, F. and R{\"o}ssle, Matthias and Herzog, Marc and Zabel, Hartmut and Bargheer, Matias}, title = {Ultrafast negative thermal expansion driven by spin disorder}, series = {Physical review : B, Condensed matter and materials physics}, volume = {99}, journal = {Physical review : B, Condensed matter and materials physics}, number = {9}, publisher = {American Physical Society}, address = {College Park}, issn = {2469-9950}, doi = {10.1103/PhysRevB.99.094304}, pages = {7}, year = {2019}, abstract = {We measure the transient strain profile in a nanoscale multilayer system composed of yttrium, holmium, and niobium after laser excitation using ultrafast x-ray diffraction. The strain propagation through each layer is determined by transient changes in the material-specific Bragg angles. We experimentally derive the exponentially decreasing stress profile driving the strain wave and show that it closely matches the optical penetration depth. Below the Neel temperature of Ho, the optical excitation triggers negative thermal expansion, which is induced by a quasi-instantaneous contractive stress and a second contractive stress contribution increasing on a 12-ps timescale. These two timescales were recently measured for the spin disordering in Ho [Rettig et al., Phys. Rev. Lett. 116, 257202 (2016)]. As a consequence, we observe an unconventional bipolar strain pulse with an inverted sign traveling through the heterostructure.}, language = {en} } @article{SarhanKoopmanPudelletal.2019, author = {Sarhan, Radwan Mohamed and Koopman, Wouter-Willem Adriaan and Pudell, Jan-Etienne and Stete, Felix and R{\"o}ssle, Matthias and Herzog, Marc and Schmitt, Clemens Nikolaus Zeno and Liebig, Ferenc and Koetz, Joachim and Bargheer, Matias}, title = {Scaling up nanoplasmon catalysis}, series = {The journal of physical chemistry : C, Nanomaterials and interfaces}, volume = {123}, journal = {The journal of physical chemistry : C, Nanomaterials and interfaces}, number = {14}, publisher = {American Chemical Society}, address = {Washington}, issn = {1932-7447}, doi = {10.1021/acs.jpcc.8b12574}, pages = {9352 -- 9357}, year = {2019}, abstract = {Nanoscale heating by optical excitation of plasmonic nanoparticles offers a new perspective of controlling chemical reactions, where heat is not spatially uniform as in conventional macroscopic heating but strong temperature gradients exist around microscopic hot spots. In nanoplasmonics, metal particles act as a nanosource of light, heat, and energetic electrons driven by resonant excitation of their localized surface plasmon resonance. As an example of the coupling reaction of 4-nitrothiophenol into 4,4′-dimercaptoazobenzene, we show that besides the nanoscopic heat distribution at hot spots, the microscopic distribution of heat dictated by the spot size of the light focus also plays a crucial role in the design of plasmonic nanoreactors. Small sizes of laser spots enable high intensities to drive plasmon-assisted catalysis. This facilitates the observation of such reactions by surface-enhanced Raman scattering, but it challenges attempts to scale nanoplasmonic chemistry up to large areas, where the excess heat must be dissipated by one-dimensional heat transport.}, language = {en} } @article{PudellSanderBaueretal.2019, author = {Pudell, Jan-Etienne and Sander, M. and Bauer, R. and Bargheer, Matias and Herzog, Marc and Ga{\´a}l, Peter}, title = {Full Spatiotemporal Control of Laser-Excited Periodic Surface Deformations}, series = {Physical review applied}, volume = {12}, journal = {Physical review applied}, number = {2}, publisher = {American Physical Society}, address = {College Park}, issn = {2331-7019}, doi = {10.1103/PhysRevApplied.12.024036}, pages = {11}, year = {2019}, abstract = {We demonstrate full control of acoustic and thermal periodic deformations at solid surfaces down to subnanosecond time scales and few-micrometer length scales via independent variation of the temporal and spatial phase of two optical transient grating (TG) excitations. For this purpose, we introduce an experimental setup that exerts control of the spatial phase of subsequent time-delayed TG excitations depending on their polarization state. Specific exemplary coherent control cases are discussed theoretically and corresponding experimental data are presented in which time-resolved x-ray reflectivity measures the spatiotemporal surface distortion of nanolayered heterostructures. Finally, we discuss examples where the application of our method may enable the control of functional material properties via tailored spatiotemporal strain fields.}, language = {en} } @article{SanderHerzogPudelletal.2017, author = {Sander, Mathias and Herzog, Marc and Pudell, Jan-Etienne and Bargheer, Matias and Weinkauf, N. and Pedersen, M. and Newby, G. and Sellmann, J. and Schwarzkopf, J. and Besse, V. and Temnov, V. V. and Gaal, P.}, title = {Spatiotemporal Coherent Control of Thermal Excitations in Solids}, series = {Physical review letters}, volume = {119}, journal = {Physical review letters}, publisher = {American Physical Society}, address = {College Park}, issn = {0031-9007}, doi = {10.1103/PhysRevLett.119.075901}, pages = {102 -- 110}, year = {2017}, abstract = {X-ray reflectivity measurements of femtosecond laser-induced transient gratings (TG) are applied to demonstrate the spatiotemporal coherent control of thermally induced surface deformations on ultrafast time scales. Using grazing incidence x-ray diffraction we unambiguously measure the amplitude of transient surface deformations with sub-angstrom resolution. Understanding the dynamics of femtosecond TG excitations in terms of superposition of acoustic and thermal gratings makes it possible to develop new ways of coherent control in x-ray diffraction experiments. Being the dominant source of TG signal, the long-living thermal grating with spatial period. can be canceled by a second, time-delayed TG excitation shifted by Lambda/2. The ultimate speed limits of such an ultrafast x-ray shutter are inferred from the detailed analysis of thermal and acoustic dynamics in TG experiments.}, language = {en} }