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Register a new userDynamics of colloidal crystals studied by pump-probe experiments at FLASH
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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.
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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.
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.
The ultrafast thermal and mechanical dynamics of a two-dimensional lattice of metallic nano-disks has been studied by near infrared pump-probe diffraction measurements, over a temporal range spanning from 100 fs to several nanoseconds. The experiments demonstrate that, in these systems, a two-dimensional surface acoustic wave (2DSAW), with a wavevector given by the reciprocal periodicity of the array, can be excited by ~120 fs Ti:sapphire laser pulses. In order to clarify the interaction between the nanodisks and the substrate, numerical calculations of the elastic eigenmodes and simulations of the thermodynamics of the system are developed through finite-element analysis. At this light, we unambiguously show that the observed 2DSAW velocity shift originates from the mechanical interaction between the 2DSAWs and the nano-disks, while the correlated 2DSAW damping is due to the energy radiation into the substrate.
Linear and non-linear spectroscopies are powerful tools used to investigate the energetics and dynamics of electronic excited states of both molecules and crystals. While highly accurate emph{ab initio} calculations of molecular spectra can be performed relatively routinely, extending these calculations to periodic systems is challenging. Here, we present calculations of the linear absorption spectrum and pump-probe two-photon photoemission spectra of the naphthalene crystal using equation-of-motion coupled-cluster theory with single and double excitations (EOM-CCSD). Molecular acene crystals are of interest due to the low-energy multi-exciton singlet states they exhibit, which have been studied extensively as intermediates involved in singlet fission. Our linear absorption spectrum is in good agreement with experiment, predicting a first exciton absorption peak at 4.4 eV, and our two-photon photoemission spectra capture the behavior of multi-exciton states, whose double-excitation character cannot be captured by current methods. The simulated pump-probe spectra provide support for existing interpretations of two-photon photoemission in closely-related acene crystals such as tetracene and pentacene.
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.
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