Ultrafast lattice dynamics and electron-phonon coupling in platinum extracted with a global fitting approach for time-resolved polycrystalline diffraction data
Daniela Zahn, Hélène Seiler, Yoav William Windsor, Ralph Ernstorfer
Quantitative knowledge of electron-phonon coupling is important for many applications as well as for the fundamental understanding of nonequilibrium relaxation processes. Time-resolved diffraction provides direct access to this knowledge through its sensitivity to laser-induced lattice dynamics. Here, we present an approach for analyzing time-resolved polycrystalline diffraction data. A two-step routine is used to minimize the number of time-dependent fit parameters. The lattice dynamics are extracted by finding the best fit to the full transient diffraction pattern rather than by analyzing transient changes of individual Debye-Scherrer rings. We apply this approach to platinum, an important component of novel photocatalytic and spintronic applications, for which a large variation of literature values exists for the electron-phonon coupling parameter $G_\mathrm{ep}$. Based on the extracted evolution of the atomic mean squared displacement (MSD) and using a two-temperature model (TTM), we obtain $G_\mathrm{ep}=(3.9\pm0.2)\cdot10^{17}\frac{\mathrm{W}}{\mathrm{m}^3\hspace{1pt}\mathrm{K}}$ (statistical error). We find that at least up to an absorbed energy density of $124\hspace{2pt}\frac{\mathrm{J}}{\mathrm{cm}^3}$, $G_\mathrm{ep}$ is not fluence-dependent. Our results for the lattice dynamics of platinum provide insights into electron-phonon coupling and phonon thermalization and constitute a basis for quantitative descriptions of platinum-based heterostructures in nonequilibrium conditions.
Phase formation and transitions in platinum silicide films on polycrystalline Si in the process of Pt magnetron sputtering and heat treatments at different temperatures are studied using X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy and X-ray diffractometry. Phases of amorphous and polycrystalline Pt$_3$Si and Pt$_2$Si are shown to form during the room-temperature Pt deposition on poly-Si beneath the Pt layer. The relaxation of the interfacial film and partial transformation of Pt$_3$Si into Pt$_2$Si occurs as a result of the thermal treatment for 30 minute…
Understanding melting in metals is a hot topic of present research. This may be accomplished by pumping the system with infrared (IR) laser radiation, and probing it with hard X-rays produced by an X-ray Free-Electron Laser (XFEL). In this work we studied nanostructured polycrystalline thin films of platinum that were illuminated by IR radiation of increasing fluences. We characterized the structural response as well as the nucleation and propagation of the liquid phase as a function of time delay between the IR pump and X-ray probe. We observed partial melting of the samples for IR fluences h…
We investigate the ultrafast electron dynamics triggered by terahertz and optical pulses in thin platinum and gold films by probing their transient optical reflectivity. The response of the platinum film to an intense terahertz pulse is similar to the optically-induced dynamics of both films and can be described by a two-temperature model. Surprisingly, gold can exhibit a much smaller terahertz pulse-induced reflectivity change and with opposite sign. For platinum, we estimate a 20% larger electron-phonon coupling for the terahertz-driven dynamics compared to the optically-induced one, which w…
The dynamics of thermal and non-thermal lattice deformation of nanometer thick polycrystalline aluminum film has been studied by means of femtosecond (fs) time-resolved electron diffraction. We utilized two different pump wavelengths: 800 nm, the fundamental of Ti: sapphire laser and 1250 nm generated by a home-made optical parametric amplifier(OPA). Our data show that, although coherent phonons were generated under both conditions, the diffraction intensity decayed with the characteristic time of 0.9+/-0.3 ps and 1.7+/-0.3 ps under 800 nm and 1250 nm excitation, respectively. Because the 800 …
This paper presents a fast method for global search of atomic structures at ab initio level. The structures global optimization (SGO) engine consists of a high-efficiency differential evolution algorithm, accelerated local relaxation methods and an ultrafast plane-wave density functional theory code run on GPU machines. It can search the global-minimum configurations of crystals, two-dimensional materials and quantum clusters without symmetry restriction in a very short time (half or several hours). The engine is also able to search the energy landscape of a given system, which is useful for e…
Ultrafast lattice deformation of tens to hundreds of nanometer thick metallic crystals, after femtosecond laser excitation, was measured directly using 8.04 keV subpicosecond x-ray and 59 keV femtosecond electron pulses. Coherent phonons were generated in both single crystal and polycrystalline films. Lattice compression was observed within the first few picoseconds after laser irradiation in single crystal aluminum, which was attributed to the generation of a blast force and the propagation of elastic waves. The different time scale of lattice heating for tens and hundreds nanometer thick fil…
Digital image correlation of laser-ablated platinum nanoparticles on the surface of a polycrystalline metal (nickel-based superalloy Rene 88DT) was used to obtain the local strain behavior from an in situ scanning electron microscope tensile experiment at room temperature. By fusing this information with crystallographic orientations from EBSD, a subsequent analysis shows that the average maximum shear strain tends to increase with increasing Schmid factor. Additionally, the range of the extreme values for the maximum shear strain also increases closer to the grain boundary, signifying that gr…
Electronic Signature of Melting Onset in Polycrystalline Copper at Extreme Conditions
Stanford University（斯坦福大学）；RPTU University Kaiserslautern-Landau（凯泽斯劳滕-兰道理工大学）；SLAC National Accelerator Laboratory（SLAC国家加速器实验室）；Bundeswehr University Munich（德国联邦国防军慕尼黑大学）；University of Warwick（华威大学）
Ultrafast lattice dynamics of few quintuple layers of topological insulator (TI) Bi$_2$Te$_3$ is studied with time-resolved optical pump-probe spectroscopy. Both optical and acoustic phonons are photogenerated and detected. Here, in order to get new insights on the out-of-equilibrium electron-phonon coupling and phonons dynamics in confined TI, different nanostructures have been investigated (single or polycrystalline QLs assemblies and nano-crystallized islands). Contrary to previous literature claims, we show that even for nanostructures containing only 10 quintuple layers (QLs), the symmetr…
In this work, we report on modelling results obtained with our recently developed simulation tool enabling nanoscopic description of electronic processes in X-ray irradiated ferromagnetic materials. With this tool, we have studied the response of Co/Pt multilayer system irradiated by an ultrafast extreme ultraviolet pulse at the M-edge of Co (photon energy $\sim$ 60 eV). It was previously investigated experimentally at the FERMI free-electron-laser facility, using the magnetic small-angle X-ray scattering technique. Our simulations show that the magnetic scattering signal from cobalt decreases…
One of the frontiers in electron scattering is to couple ultrafast temporal resolution with highly localized probes to investigate the role of microstructure on material properties. Here, taking advantage of the unprecedented average brightness of the APEX electron gun providing relativistic electron pulses at high repetition rates, we demonstrate for the first time the generation of ultrafast relativistic electron beams with picometer-scale emittance and their ability to probe nanoscale features on materials with complex microstructures. At the sample plane, the APEX beam is tightly focused b…
Impacts of Hot Electron Diffusion, Electron-Phonon Coupling, and Surface Atoms on Metal Surface Dynamics Revealed by Reflection Ultrafast Electron Diffraction
With its direct correspondence to electronic structure, angle-resolved photoemission spectroscopy (ARPES) is a ubiquitous tool for the study of solids. When extended to the temporal domain, time-resolved (TR)-ARPES offers the potential to move beyond equilibrium properties, exploring both the unoccupied electronic structure as well as its dynamical response under ultrafast perturbation. Historically, ultrafast extreme ultraviolet (XUV) sources employing high-order harmonic generation (HHG) have required compromises that make it challenging to achieve a high energy resolution - which is highly …
