Influence of band occupation on electron-phonon coupling in gold

Electron-phonon coupling is a fundamental process that governs the energy relaxation dynamics of solids excited by ultrafast laser pulses. It has been found to strongly depend on electron temperature as well as on nonequilibrium effects. Recently, the effect of occupational nonequilibrium in noble metals, which outlasts the fully kinetic stage, has come into increased focus. In this work, we investigate the influence of nonequilibrium density distributions in gold on the electron-phonon coupling. We find a large effect on the coupling parameter which describes the energy exchange between the two subsystems. Our results challenge the conventional view that electron temperature alone is a sufficient predictor of electron-phonon coupling

Interplay of electron-magnon scattering and spin-orbit induced electronic spin-flip fcattering in a two-band Stoner model

Magnons are one of the carriers of angular momentum that are involved in the ultrafast magnetization dynamics in ferromagnets, but their contribution to the electronic dynamics and their interplay with other scattering process that occur during ultrafast demagnetization has not yet been studied in the framework of a microscopic dynamical model. The present paper presents such an investigation of electronic scattering dynamics in itinerant ferromagnets at the level of Boltzmann scattering integrals for the magnon distributions and spin-dependent electron distributions. In addition to electron-magnon scattering, we include spin-conserving and effective Elliott-Yafet like spin-flip electron-electron scattering processes and the influence of phonons. In our model system, the creation or annihilation of magnons leads to transitions between two spin-split electronic bands with energy and momentum conservation. Due to the presence of spin-orbit coupling, Coulomb scattering transitions between these bands are also possible, and we describe them on an equal footing in terms of Boltzmann scattering integrals. For an instantaneous carrier excitation process we analyze the influence of both interaction processes on the magnon and spin-dependent electron dynamics, and show that their interplay gives rise to an efficient creation of magnons at higher energies and wave vectors accompanied by only a small increase of the electronic spin polarization. These results present a microscopic dynamical scenario that shows how non-equilibrium magnons may dominate the magnetic response of a ferromagnet on ultrafast timescales

Time-resolved spectral densities of non-thermal electrons in gold

Noble-metal nanoparticles for photocatalysis have become a major research object in recent years due to their plasmon-enhanced strong light-matter interaction. The dynamics of the hot electrons in the noble metal are crucial for the efficiency of the photocatalysis and for the selective control of reactions. In this work, we present a kinetic description of the non-equilibrium electron distribution created by photoexcitation, based on full energy-resolved Boltzmann collision integrals for the laser excitation as well as for the electron-electron thermalization. The laser-induced electronic non-equilibrium and the inherently included secondary electron generation govern the dynamics of non-thermal electrons. Applying our method to gold, we show a significant dependence of hot electron dynamics on kinetic energy. Specifically, the timescales of the relaxation as well as the qualitative behavior are depending on the evaluated energy window. During the thermalization processes there are cases of increasing electron density as well as of decreasing electron density. Studying the influence of excitation parameters, we find that the photon energy and the fluence of the exciting laser can be tuned to influence not only the initial excitation but also the subsequent characteristics of the time-resolved electronic spectral density dynamics. The electronic thermalization including secondary electron generation leads to time-dependent spectral densities which differ from their specific final equilibrium values for picoseconds after irradiation ended

Nonequilibrium band occupation and optical response of gold after ultrafast XUV excitation

Free electron lasers offer unique properties to study matter in states far from equilibrium as they combine short pulses with a large range of photon energies. In particular, the possibility to excite core states drives new relaxation pathways that, in turn, also change the properties of the optically and chemically active electrons. Here, we present a theoretical model for the dynamics of the nonequilibrium occupation of the different energy bands in solid gold driven by exciting deep core states. The resulting optical response is in excellent agreement with recent measurements and, combined with our model, provides a quantitative benchmark for the description of electron–phonon coupling in strongly driven gold. Focusing on sub-picosecond time scales, we find essential differences between the dynamics induced by XUV and visible light

Energy and momentum distribution of surface plasmon-induced hot carriers isolated via spatiotemporal separation

Understanding the differences between photon-induced and plasmon-induced hot electrons is essential for the construction of devices for plasmonic energy conversion. The mechanism of the plasmonic enhancement in photochemistry, photocatalysis, and light-harvesting and especially the role of hot carriers is still heavily discussed. The question remains, if plasmon-induced and photon-induced hot carriers are fundamentally different or if plasmonic enhancement is only an effect of field concentration producing these carriers in greater numbers. For the bulk plasmon resonance, a fundamental difference is known, yet for the technologically important surface plasmons, this is far from being settled. The direct imaging of surface plasmon-induced hot carriers could provide essential insight, but the separation of the influence of driving laser, field-enhancement, and fundamental plasmon decay has proven to be difficult. Here, we present an approach using a two-color femtosecond pump–probe scheme in time-resolved 2-photon-photoemission (tr-2PPE), supported by a theoretical analysis of the light and plasmon energy flow. We separate the energy and momentum distribution of the plasmon-induced hot electrons from that of photoexcited electrons by following the spatial evolution of photoemitted electrons with energy-resolved photoemission electron microscopy (PEEM) and momentum microscopy during the propagation of a surface plasmon polariton (SPP) pulse along a gold surface. With this scheme, we realize a direct experimental access to plasmon-induced hot electrons. We find a plasmonic enhancement toward high excitation energies and small in-plane momenta, which suggests a fundamentally different mechanism of hot electron generation, as previously unknown for surface plasmons

Key role of surface plasmon polaritons in generation of periodic surface structures following single-pulse laser irradiation of a gold step edge

Understanding the mechanisms and controlling the possibilities of surface nanostructuring is of crucial interest for both fundamental science and application perspectives. Here, we report a direct experimental observation of laser-induced periodic surface structures (LIPSS) formed near a predesigned gold step edge following single-pulse femtosecond laser irradiation. Simulation results based on a hybrid atomistic-continuum model fully support the experimental observations. We experimentally detect nanosized surface features with a periodicity of ∼300 nm and heights of a few tens of nanometers.We identify two key components of single-pulse LIPSS formation: excitation of surface plasmon polaritons and material reorganization. Our results lay a solid foundation toward simple and efficient usage of light for innovative material processing technologies

Laser-induced creation of antiferromagnetic 180-degree domains in NiO/Pt bilayers

The antiferromagnetic order in heterostructures of NiO/Pt thin films can be modified by optical pulses. After the irradiation with laser light, the optically induced creation of antiferromagnetic domains can be observed by imaging the created domain structure utilizing the X-ray magnetic linear dichroism effect. The effect of different laser polarizations on the domain formation can be studied and used to identify a polarization-independent creation of 180° domain walls and domains with 180° different Néel vector orientation. By varying the irradiation parameters, the switching mechanism can be determined to be thermally induced. This study demonstrates experimentally the possibility to optically create antiferromagnetic domains, an important step towards future functionalization of all optical switching mechanisms in antiferromagnets

Femtosecond formation dynamics of the spin Seebeck effect revealed by terahertz spectroscopy.

Understanding the transfer of spin angular momentum is essential in modern magnetism research. A model case is the generation of magnons in magnetic insulators by heating an adjacent metal film. Here, we reveal the initial steps of this spin Seebeck effect with <27 fs time resolution using terahertz spectroscopy on bilayers of ferrimagnetic yttrium iron garnet and platinum. Upon exciting the metal with an infrared laser pulse, a spin Seebeck current js arises on the same ~100 fs time scale on which the metal electrons thermalize. This observation highlights that efficient spin transfer critically relies on carrier multiplication and is driven by conduction electrons scattering off the metal-insulator interface. Analytical modeling shows that the electrons' dynamics are almost instantaneously imprinted onto js because their spins have a correlation time of only ~4 fs and deflect the ferrimagnetic moments without inertia. Applications in material characterization, interface probing, spin-noise spectroscopy and terahertz spin pumping emerge