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Matthias Rössle

Publications and source records attributed to Matthias Rössle.

7 recordsLinked to original sources

Boltzmann-Bloch Equation Approach to the Theory of the Optical Inter- and Intraband Response in Noble Metals

In this paper we introduce momentum-resolved metal Boltzmann-Bloch equations (MBBE) for the combined description of electronic intra- and interband processes in noble metals. This microscopic framework incorporates a full treatment of many-body electron-electron and electron-phonon interactions, relevant for relaxation and dephasing processes after optical excitation. For the example of gold, we calculate the linear optical response for near-infrared and visible energies. This provides insight into the interplay of microscopic processes hidden in phenomenological Drude-Lorentz models. The complex geometry of the Fermi surface is treated by an anisotropic electronic dispersion model, which is necessary to explain the temperature dependent spectrum over the whole frequency range of intra- and interband transitions.

cond-mat.mes-hall↗

Non-thermal electrons open the non-equilibrium pathway of the phase transition in FeRh

We use ultrafast x-ray diffraction to study non-equilibrium pathways of the phase transition in FeRh parametrized by the structural response. By increasing the pump-pulse duration beyond the electron-phonon coupling time, we suppress the electron-phonon non-equilibrium present upon femtosecond laser excitation but still photoexcite electrons to non-thermal states. Irrespective of the pump pulse duration, we find an optically induced nucleation of ferromagnetic domains on an $8\,\text{ps}$ timescale that starts as soon as the successively deposited energy surpasses the site-specific threshold energy. If in contrast, FeRh is only indirectly excited by diffusion of thermalized electrons from an opaque Pt cap layer, the ferromagnetic phase rises on a $50\,\text{ps}$ timescale. These findings unambiguously identify the photo-excitation of non-thermal electrons and not electron-phonon non-equilibria to enable the non-equilibrium pathway of the phase transition in FeRh.

cond-mat.mtrl-sci↗

Unveiling the nanomorphology of HfN thin films by ultrafast reciprocal space mapping

Hafnium Nitride (HfN) is a promising and very robust alternative to gold for applications of nanoscale metals. Details of the nanomorphology related to variations in strain states and optical properties can be crucial for applications in nanophotonics and plasmon-assisted chemistry. We use ultrafast reciprocal space mapping (URSM) with hard x-rays to unveil the nanomorphology of thin HfN films. Static high-resolution x-ray diffraction reveals a twofold composition of the thin films being separated into regions with identical lattice constant and similar out-of-plane but hugely different in-plane coherence lengths. URSM upon femtosecond laser excitation reveals different transient strain dynamics for the two respective Bragg peak components. This unambiguously locates the longer in-plane coherence length in the first 15\,nm of the thin film adjacent to the substrate. The transient shift of the broad diffraction peak displays the strain dynamics of the entire film, implying that the near-substrate region hosts nanocrystallites with small and large coherence length, whereas the upper part of the film grows in small columnar grains. Our results illustrate that URSM is a suitable technique for non-destructive investigations of the depth-resolved nanomorphology of nanostructures.

cond-mat.mtrl-sci↗

Accelerating the laser-induced phase transition in nanostructured FeRh via plasmonic absorption

By ultrafast x-ray diffraction we show that the laser-induced magnetostructural phase transition in FeRh nanoislands proceeds faster and more complete than in continuous films. We observe an intrinsic 8 ps timescale for nucleation of ferromagnetic (FM) domains in both types of samples. For the continuous film, the substrate-near regions, which are not directly exposed to light, are only slowly transformed to the FM state by domain wall motion following heat transport. In contrast, numerical modeling of the plasmonic absorption in the investigated nanostructure reveals a strong contribution near the FeRh/MgO interface. On average, the absorption is larger and more homogeneous in the nanoislands, enabling the phase transition throughout the entire volume at the intrinsic nucleation timescale.

cond-mat.mtrl-sci↗

Speed limits of the laser-induced phase transition in FeRh

We use ultrafast x-ray diffraction (UXRD) and the polar time-resolved magneto-optical Kerr effect (tr-MOKE) to study the laser-induced metamagnetic phase transition in two FeRh films with thicknesses below and above the optical penetration depth. In the thin film, we identify an intrinsic timescale for the light-induced nucleation of ferromagnetic (FM) domains in the antiferromagnetic material of $8\,\text{ps}$ that is substantially slower than the speed of sound. For the inhomogeneously excited thicker film, only the optically excited near-surface part transforms within $8\,\text{ps}$. For strong excitations we observe an additional slow rise of the FM phase, which we experimentally relate to a growth of the FM phase into the depth of the layer by comparing the transient magnetization in front- and backside excitation geometry. In the lower lying parts of the film, which are only excited via near-equilibrium heat transport, the FM phase emerges significantly slower than $8\,\text{ps}$ after heating above the transition temperature.

cond-mat.mtrl-sci↗

Critical behavior of the damping rate of GHz acoustic phonons in SrTiO3 at the antiferrodistortive phase transition measured by time- and frequency-resolved Brillouin scattering

We determine the temperature dependent damping rate of longitudinal acoustic phonons in SrTiO3 using frequency domain Brillouin scattering and time domain Brillouin scattering. We investigate samples with (La,Sr)MnO3 and SrRuO3 capping layers, which result in compressive or tensile strain at the layer - substrate interface, respectively. The different strain states lead to dif- ferent domain structures in SrTiO3 that extend into the bulk of the SrTiO3 substrates and strongly affect the phonon propagation. Our experiments show that the damping rate of acoustic phonons in the interfacial STO layer depends strongly on the sample temperature and strain induced do- main structure. We also show that the damping rate as function of temperature exhibits a critical behavior close to the cubic-to-tetragonal phase transition of SrTiO3.

cond-mat.mtrl-sci↗

Influence of La and Mn vacancies on the electronic and magnetic properties of LaMnO$_{3}$ thin films grown by pulsed laser deposition

With pulsed laser deposition we have grown c-axis oriented thin films of the nominal composition LaMnO$_{3}$ (LMO) on LSAT(001) substrates. We find that, depending on the oxygen background pressure during growth, the LMO films contain sizeable amounts of La and/or Mn vacancies that strongly influence their electronic and magnetic properties. Specifically, we show that the Mn/La ratio can be systematically varied from 0.92 at 0.11 mbar to 1.09 at 0.30 mbar of oxygen. These cationic vacancies lead to markedly different disorder effects that become most pronounced once the samples are fully oxygenated and thus strongly hole doped. All as-grown and thus slightly oxygen deficient LMO films are ferromagnetic insulators with saturation moments in excess of 2.5 μ$_{B}$ per Mn ion, their transport and optical properties that can be understood in terms of trapped ferromagnetic polarons. Upon oxygen annealing, the most La-deficient films develop a metallic response with an even larger ferromagnetic saturation moment of 3.8 μ$_{B}$ per Mn ion. In contrast, in the oxygenated Mn-deficient films the ferromagnetic order is almost completely suppressed to less than 0.5 μ$_{B}$ per Mn ion and the transport remains insulator-like. We compare our results with the ones that were previously obtained on bulk samples and present an interpretation in terms of the much stronger disorder potential of the Mn vacancies as compared to the La vacancies. We also discuss the implications for the growth of LMO thin films with well-defined physical properties that, for example, are a prerequisite for the study of interface effects in multilayers.

cond-mat.str-el↗