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Ultrafast X-ray diffraction is used to quantify the transport of energy in laser-excited nanoscale gold-nickel (Au-Ni) bilayers.
Electron transport and efficient electron-phonon coupling in Ni convert the laser-deposited energy in the conduction electrons within a few picoseconds into a strong non-equilibrium between hot Ni and cold Au phonons at the bilayer interface.
Modeling of the subsequent equilibration dynamics within various two-temperature models confirms that for ultrathin Au films, the thermal transport is dominated by phonons instead of conduction electrons because of the weak electron-phonon coupling in Au.
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.
Phonons are often regarded as delocalized quasiparticles with certain energy and momentum. The anharmonic interaction of phonons determines macroscopic properties of the solid, such as thermal expansion or thermal conductivity, and a detailed understanding becomes increasingly important for functional nanostructures. Although phonon-phonon scattering processes depicted in simple wave-vector diagrams are the basis of theories describing these macroscopic phenomena, experiments directly accessing these coupling channels are scarce. We synthesize monochromatic acoustic phonon wave packets with only a few cycles to introduce nonlinear phononics as the acoustic counterpart to nonlinear optics. Control of the wave vector, bandwidth, and consequently spatial extent of the phonon wave packets allows us to observe nonlinear phonon interaction, in particular, second harmonic generation, in real time by wave-vector-sensitive Brillouin scattering with x-rays and optical photons.
Optical excitation of spin-ordered rare earth metals triggers a complex response of the crystal lattice since expansive stresses from electron and phonon excitations compete with a contractive stress induced by spin disorder. Using ultrafast x-ray diffraction experiments, we study the layer specific strain response of a dysprosium film within a metallic heterostructure upon femtosecond laser-excitation. The elastic and diffusive transport of energy to an adjacent, non-excited detection layer clearly separates the contributions of strain pulses and thermal excitations in the time domain. We find that energy transfer processes to magnetic excitations significantly modify the observed conventional bipolar strain wave into a unipolar pulse. By modeling the spin system as a saturable energy reservoir that generates substantial contractive stress on ultrafast timescales, we can reproduce the observed strain response and estimate the time- and space dependent magnetic stress. The saturation of the magnetic stress contribution yields a non-monotonous total stress within the nanolayer, which leads to unconventional picosecond strain pulses.
We investigate the ultrafast magnetization dynamics of FePt in the L1(0) phase after an optical heating pulse, as used in heat-assisted magnetic recording. We compare continuous and nano-granular thin films and emphasize the impact of the finite size on the remagnetization dynamics. The remagnetization speeds up significantly with increasing external magnetic field only for the continuous film, where domain-wall motion governs the dynamics. The ultrafast remagnetization dynamics in the continuous film are only dominated by heat transport in the regime of high magnetic fields, whereas the timescale required for cooling is prevalent in the granular film for all magnetic field strengths. These findings highlight the necessary conditions for studying the intrinsic heat transport properties in magnetic materials.
We study gadolinium thin films as a model system for ferromagnets with negative thermal expansion. Ultrashort laser pulses heat up the electronic subsystem and we follow the transient strain via ultrafast x-ray diffraction. In terms of a simple Grueneisen approach, the strain is decomposed into two contributions proportional to the thermal energy of spin and phonon subsystems. Our analysis reveals that upon femtosecond laser excitation, phonons and spins can be driven out of thermal equilibrium for several nanoseconds.