TY - JOUR A1 - Sarhan, Radwan Mohamed A1 - Koopman, Wouter-Willem Adriaan A1 - Pudell, Jan-Etienne A1 - Stete, Felix A1 - Rössle, Matthias A1 - Herzog, Marc A1 - Schmitt, Clemens Nikolaus Zeno A1 - Liebig, Ferenc A1 - Koetz, Joachim A1 - Bargheer, Matias T1 - Scaling up nanoplasmon catalysis BT - the role of heat dissipation JF - The journal of physical chemistry : C, Nanomaterials and interfaces N2 - 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. KW - Gold KW - Raman spectroscopy KW - Silicon KW - Irradiation KW - Lasers Y1 - 2019 U6 - https://doi.org/10.1021/acs.jpcc.8b12574 SN - 1932-7447 VL - 123 IS - 14 SP - 9352 EP - 9357 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Zeuschner, Steffen A1 - Parpiiev, Tymur A1 - Pezeril, Thomas A1 - Hillion, Arnaud A1 - Dumesnil, Karine A1 - Anane, Abdelmadjid A1 - Pudell, Jan-Etienne A1 - Willig, Lisa A1 - Rössle, Matthias A1 - Herzog, Marc A1 - von Reppert, Alexander A1 - Bargheer, Matias T1 - Tracking picosecond strain pulses in heterostructures that exhibit giant magnetostriction JF - Structural Dynamics N2 - We combine ultrafast X-ray diffraction (UXRD) and time-resolved Magneto-Optical Kerr Effect (MOKE) measurements to monitor the strain pulses in laser-excited TbFe2/Nb heterostructures. Spatial separation of the Nb detection layer from the laser excitation region allows for a background-free characterization of the laser-generated strain pulses. We clearly observe symmetric bipolar strain pulses if the excited TbFe2 surface terminates the sample and a decomposition of the strain wavepacket into an asymmetric bipolar and a unipolar pulse, if a SiO2 glass capping layer covers the excited TbFe2 layer. The inverse magnetostriction of the temporally separated unipolar strain pulses in this sample leads to a MOKE signal that linearly depends on the strain pulse amplitude measured through UXRD. Linear chain model simulations accurately predict the timing and shape of UXRD and MOKE signals that are caused by the strain reflections from multiple interfaces in the heterostructure. KW - Heterostructures KW - Magnetooptical effects KW - Metal oxides KW - Crystal lattices KW - Transition metals KW - Magnetism KW - Ultrafast X-ray diffraction KW - Lasers KW - Bragg peak KW - Phonons Y1 - 2019 U6 - https://doi.org/10.1063/1.5084140 SN - 2329-7778 VL - 6 IS - 2 PB - AIP Publishing LLC CY - Melville, NY ER - TY - GEN A1 - Zeuschner, Steffen A1 - Parpiiev, Tymur A1 - Pezeril, Thomas A1 - Hillion, Arnaud A1 - Dumesnil, Karine A1 - Anane, Abdelmadjid A1 - Pudell, Jan-Etienne A1 - Willig, Lisa A1 - Rössle, Matthias A1 - Herzog, Marc A1 - von Reppert, Alexander A1 - Bargheer, Matias T1 - Tracking picosecond strain pulses in heterostructures that exhibit giant magnetostriction T2 - Postprints der Universität Potsdam : Mathematisch-naturwissenschaftliche Reihe N2 - We combine ultrafast X-ray diffraction (UXRD) and time-resolved Magneto-Optical Kerr Effect (MOKE) measurements to monitor the strain pulses in laser-excited TbFe2/Nb heterostructures. Spatial separation of the Nb detection layer from the laser excitation region allows for a background-free characterization of the laser-generated strain pulses. We clearly observe symmetric bipolar strain pulses if the excited TbFe2 surface terminates the sample and a decomposition of the strain wavepacket into an asymmetric bipolar and a unipolar pulse, if a SiO2 glass capping layer covers the excited TbFe2 layer. The inverse magnetostriction of the temporally separated unipolar strain pulses in this sample leads to a MOKE signal that linearly depends on the strain pulse amplitude measured through UXRD. Linear chain model simulations accurately predict the timing and shape of UXRD and MOKE signals that are caused by the strain reflections from multiple interfaces in the heterostructure. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 706 KW - Heterostructures KW - Magnetooptical effects KW - Metal oxides KW - Crystal lattices KW - Transition metals KW - Magnetism KW - Ultrafast X-ray diffraction KW - Lasers KW - Bragg peak KW - Phonons Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-428457 SN - 1866-8372 IS - 706 ER - TY - GEN A1 - Mattern, M. A1 - Pudell, Jan-Etienne A1 - Laskin, G. A1 - von Reppert, A. A1 - Bargheer, Matias T1 - Analysis of the temperature- and fluence-dependent magnetic stress in laser-excited SrRuO3 T2 - Postprints der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe N2 - We use ultrafast x-ray diffraction to investigate the effect of expansive phononic and contractive magnetic stress driving the picosecond strain response of a metallic perovskite SrRuO3 thin film upon femtosecond laser excitation. We exemplify how the anisotropic bulk equilibrium thermal expansion can be used to predict the response of the thin film to ultrafast deposition of energy. It is key to consider that the laterally homogeneous laser excitation changes the strain response compared to the near-equilibrium thermal expansion because the balanced in-plane stresses suppress the Poisson stress on the picosecond timescale. We find a very large negative Grüneisen constant describing the large contractive stress imposed by a small amount of energy in the spin system. The temperature and fluence dependence of the strain response for a double-pulse excitation scheme demonstrates the saturation of the magnetic stress in the high-fluence regime. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 1144 KW - Thin films KW - Thermodynamic properties KW - Bragg peak KW - Ultrafast X-ray diffraction KW - Thermal effects KW - Phonons KW - Magnetism KW - Lattice dynamics KW - Lasers KW - Perovskites Y1 - 2021 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-515718 SN - 1866-8372 ER - TY - JOUR A1 - Witzorky, Christoph A1 - Paramonov, Guennaddi A1 - Bouakline, Foudhil A1 - Jaquet, Ralph A1 - Saalfrank, Peter A1 - Klamroth, Tillmann T1 - Gaussian-type orbital calculations for high harmonic generation in vibrating molecules BT - Benchmarks for H-2(+) JF - Journal of chemical theory and computation N2 - The response of the hydrogen molecular ion, H-2(+), to few-cycle laser pulses of different intensities is simulated. To treat the coupled electron-nuclear motion, we use adiabatic potentials computed with Gaussian-type basis sets together with a heuristic ionization model for the electron and a grid representation for the nuclei. Using this mixed-basis approach, the time-dependent Schrodinger equation is solved, either within the Born-Oppenheimer approximation or with nonadiabatic couplings included. The dipole response spectra are compared to all-grid-based solutions for the three-body problem, which we take as a reference to benchmark the Gaussian-type basis set approaches. Also, calculations employing the fixed-nuclei approximation are performed, to quantify effects due to nuclear motion. For low intensities and small ionization probabilities, we get excellent agreement of the dynamics using Gaussian-type basis sets with the all-grid solutions. Our investigations suggest that high harmonic generation (HHG) and high-frequency response, in general, can be reliably modeled using Gaussian-type basis sets for the electrons for not too high harmonics. Further, nuclear motion destroys electronic coherences in the response spectra even on the time scale of about 30 fs and affects HHG intensities, which reflect the electron dynamics occurring on the attosecond time scale. For the present system, non-Born-Oppenheimer effects are small. The Gaussian-based, nonadiabatically coupled, time-dependent multisurface approach to treat quantum electron-nuclear motion beyond the non-Born-Oppenheimer approximation can be easily extended to approximate wavefunction methods, such as time-dependent configuration interaction singles (TD-CIS), for systems where no benchmarks are available. KW - Basis sets KW - Chemical calculations KW - Ionization KW - Lasers KW - Quantum mechanics Y1 - 2021 U6 - https://doi.org/10.1021/acs.jctc.1c00837 SN - 1549-9618 SN - 1549-9626 VL - 17 IS - 12 SP - 7353 EP - 7365 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Mattern, Maximilian A1 - Pudell, Jan-Etienne A1 - Laskin, Gennadii A1 - Reppert, Alexander von A1 - Bargheer, Matias T1 - Analysis of the temperature- and fluence-dependent magnetic stress in laser-excited SrRuO3 JF - Structural dynamics N2 - We use ultrafast x-ray diffraction to investigate the effect of expansive phononic and contractive magnetic stress driving the picosecond strain response of a metallic perovskite SrRuO3 thin film upon femtosecond laser excitation. We exemplify how the anisotropic bulk equilibrium thermal expansion can be used to predict the response of the thin film to ultrafast deposition of energy. It is key to consider that the laterally homogeneous laser excitation changes the strain response compared to the near-equilibrium thermal expansion because the balanced in-plane stresses suppress the Poisson stress on the picosecond timescale. We find a very large negative Grüneisen constant describing the large contractive stress imposed by a small amount of energy in the spin system. The temperature and fluence dependence of the strain response for a double-pulse excitation scheme demonstrates the saturation of the magnetic stress in the high-fluence regime. KW - Thin films KW - Thermodynamic properties KW - Bragg peak KW - Ultrafast X-ray diffraction KW - Thermal effects KW - Phonons KW - Magnetism KW - Lattice dynamics KW - Lasers KW - Perovskites Y1 - 2020 U6 - https://doi.org/10.1063/4.0000072 SN - 2329-7778 VL - 8 IS - 2 PB - AIP Publishing LLC CY - Melville, NY ER -