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Register a new userEstablishing non-thermal regimes in pump-probe electron-relaxation dynamics
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Time- and angle-resolved photoemission spectroscopy (TR-ARPES) accesses the electronic structure of solids under optical excitation, and is a powerful technique for studying the coupling between electrons and collective modes. One approach to infer electron-boson coupling is through the relaxation dynamics of optically-excited electrons, and the characteristic timescales of energy redistribution. A common description of electron relaxation dynamics is through the effective electronic temperature. Such a description requires that thermodynamic quantities are well-defined, an assumption that is generally violated at early delays. Additionally, precise estimation of the non-thermal window -- within which effective temperature models may not be applied -- is challenging. We perform TR-ARPES on graphite and show that Boltzmann rate equations can be used to calculate the time-dependent electronic occupation function, and reproduce experimental features given by non-thermal electron occupation. Using this model, we define a quantitative measure of non-thermal electron occupation and use it to define distinct phases of electron relaxation in the fluence-delay phase space. More generally, this approach can be used to inform the non-thermal-to-thermal crossover in pump-probe experiments.
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We explore the influence of the nanoporous structure on the thermal relaxation of electrons and holes excited by ultrashort laser pulses ($sim 7$ fs) in thin gold films. Plasmon decay into hot electron-hole pairs results in the generation of a Fermi-Dirac distribution thermalized at a temperature $T_{mathrm{e}}$ higher than the lattice temperature $T_{mathrm{l}}$. The relaxation times of the energy exchange between electrons and lattice, here measured by pump-probe spectroscopy, is slowed down by the nanoporous structure, resulting in much higher peak $T_{mathrm{e}}$ than for bulk gold films. The electron-phonon coupling constant and the Debye temperature are found to scale with the metal filling factor $f$ and a two-temperature model reproduces the data. The results open the way for electron temperature control in metals by engineering of the nanoporous geometry.
We present a time-resolved infrared (IR) pump and extreme-ultraviolet (XUV) probe diffraction experiment to investigate ultrafast structural dynamics in colloidal crystals with picosecond resolution. The experiment was performed at the FLASH facility at DESY with a fundamental wavelength of 8 nm. In our experiment, the temporal changes of Bragg peaks were analyzed and their frequency components were calculated using Fourier analysis. Periodic modulations in the colloidal crystal were localized at a frequency of about 4-5 GHz. Based on the Lamb theory, theoretical calculations of vibrations of the isotropic elastic polystyrene spheres of 400 nm in size reveal a 5.07 GHz eigenfrequency of the ground (breathing) mode.
We study the role of excited phonon populations in the relaxation rates of nonequilibrium electrons using a nonequilibrium Greens function formalism. The transient modifications in the phononic properties are accounted for by self-consistently solving the Dyson equation for the electron and phonon Greens functions. The pump induced changes manifest in both the electronic and phononic spectral functions. We find that the excited phonon populations suppress the decay rates of nonequilibrium electrons due to enhanced phonon absorption. The increased phonon occupation also sets the nonequilibrium decay rates and the equilibrium scattering rates apart. The decay rates are found to be time-dependent, and this is illustrated in the experimentally observed population decay of photoexcited $mathrm{Bi}_{1.5}mathrm{Sb}_{0.5} mathrm{Te}_{1.7}mathrm{Se}_{1.3}$.
A novel, induction type linear accelerator, the Neutralized Drift Compression eXperiment (NDCX-II), is currently being commissioned at Berkeley Lab. This accelerator is designed to deliver intense (up to 3x1011 ions/pulse), 0.6 to ~600 ns duration pulses of 0.13 to 1.2 MeV lithium ions at a rate of about 2 pulses per minute onto 1 to 10 mm scale target areas. When focused to mm-diameter spots, the beam is predicted to volumetrically heat micrometer thick foils to temperatures of ~30,000 K. At lower beam power densities, the short excitation pulse with tunable intensity and time profile enables pump-probe type studies of defect dynamics in a broad range of materials. We briefly describe the accelerator concept and design, present results from beam pulse shaping experiments and discuss examples of pump-probe type studies of defect dynamics following irradiation of materials with intense, short ion beam pulses from NDCX-II.
We investigated the photoexcited carrier dynamics in Si by using optical pump and terahertz probe spectroscopy in an energy range between 2 meV and 25 meV. The formation dynamics of excitons from unbound e-h pairs was studied through the emergence of the 1s-2p transition of excitons at 12 meV (3 THz). We revealed the thermalization mechanism of the photo-injected hot carriers (electrons and holes) in the low temperature lattice system by taking account of the interband and intraband scattering of carriers with acoustic and optical phonons. The overall cooling rate of electrons and holes was numerically calculated on the basis of a microscopic analysis of the phonon scattering processes, and the results well account for the experimentally observed carrier cooling dynamics. The long formation time of excitons in Si after the above-gap photoexcitation is reasonably accounted for by the thermalization process of photoexcited carriers.
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