Electron Kinetics Induced by Ultrafast Photoexcitation of Warm Dense Matter in a 30-nm-Thick Foil.

We report on the study of electron kinetics induced by intense femtosecond (fs) laser excitation of electrons in the 5d band of Au. Changes in the electron system are observed from the temporal evolution of ac conductivity and conduction electron density. The results reveal an increase of electron thermalization time with excitation energy density, contrary to the Fermi-liquid behavior of the decrease of thermalization time associated with the heating of conduction electrons. This is attributed to the severe mitigation of photoexcitation by Auger decay. The study also uncovers the shortening of 5d hole lifetime with the increase of photoexcitation rates. These unique findings provide valuable insights for understanding electron kinetics under extreme nonequilibrium conditions.

Ultrafast multi-cycle terahertz measurements of the electrical conductivity in strongly excited solids.

Key insights in materials at extreme temperatures and pressures can be gained by accurate measurements that determine the electrical conductivity. Free-electron laser pulses can ionize and excite matter out of equilibrium on femtosecond time scales, modifying the electronic and ionic structures and enhancing electronic scattering properties. The transient evolution of the conductivity manifests the energy coupling from high temperature electrons to low temperature ions. Here we combine accelerator-based, high-brightness multi-cycle terahertz radiation with a single-shot electro-optic sampling technique to probe the evolution of DC electrical conductivity using terahertz transmission measurements on sub-picosecond time scales with a multi-undulator free electron laser. Our results allow the direct determination of the electron-electron and electron-ion scattering frequencies that are the major contributors of the electrical resistivity.

Determination of the electron-lattice coupling strength of copper with ultrafast MeV electron diffraction.

Electron-lattice coupling strength governs the energy transfer between electrons and the lattice and is important for understanding the material behavior under highly non-equilibrium conditions. Here we report the results of employing time-resolved electron diffraction at MeV energies to directly study the electron-lattice coupling strength in 40-nm-thick polycrystalline copper excited by femtosecond optical lasers. The temporal evolution of lattice temperature at various pump fluence conditions were obtained from the measurements of the Debye-Waller decay of multiple diffraction peaks. We observed the temperature dependence of the electron-lattice relaxation time which is a result of the temperature dependence of electron heat capacity. Comparison with two-temperature model simulations reveals an electron-lattice coupling strength of (0.9 ± 0.1) × 1017 W/m3/K for copper.

Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction.

The ultrafast laser excitation of matters leads to nonequilibrium states with complex solid-liquid phase-transition dynamics. We used electron diffraction at mega-electron volt energies to visualize the ultrafast melting of gold on the atomic scale length. For energy densities approaching the irreversible melting regime, we first observed heterogeneous melting on time scales of 100 to 1000 picoseconds, transitioning to homogeneous melting that occurs catastrophically within 10 to 20 picoseconds at higher energy densities. We showed evidence for the heterogeneous coexistence of solid and liquid. We determined the ion and electron temperature evolution and found superheated conditions. Our results constrain the electron-ion coupling rate, determine the Debye temperature, and reveal the melting sensitivity to nucleation seeds.

Measurements of ionization states in warm dense aluminum with betatron radiation.

Time-resolved measurements of the ionization states of warm dense aluminum via K-shell absorption spectroscopy are demonstrated using betatron radiation generated from laser wakefield acceleration as a probe. The warm dense aluminum is generated by irradiating a free-standing nanofoil with a femtosecond optical laser pulse and was heated to an electron temperature of ∼20-25 eV at a close-to-solid mass density. Absorption dips in the transmitted x-ray spectrum due to the Al^{4+} and Al^{5+} ions are clearly seen during the experiments. The measured absorption spectra are compared to simulations with various ionization potential depression models, including the commonly used Stewart-Pyatt model and an alternative modified Ecker-Kröll model. The observed absorption spectra are in approximate agreement with these models, though indicating a slightly higher state of ionization and closer agreement for simulations with the modified Ecker-Kröll model.

Single-shot mega-electronvolt ultrafast electron diffraction for structure dynamic studies of warm dense matter.

We have developed a single-shot mega-electronvolt ultrafast-electron-diffraction system to measure the structural dynamics of warm dense matter. The electron probe in this system is featured by a kinetic energy of 3.2 MeV and a total charge of 20 fC, with the FWHM pulse duration and spot size at sample of 350 fs and 120 µm respectively. We demonstrate its unique capability by visualizing the atomic structural changes of warm dense gold formed from a laser-excited 35-nm freestanding single-crystal gold foil. The temporal evolution of the Bragg peak intensity and of the liquid signal during solid-liquid phase transition are quantitatively determined. This experimental capability opens up an exciting opportunity to unravel the atomic dynamics of structural phase transitions in warm dense matter regime.

Kirkpatrick-Baez microscope for hard X-ray imaging of fast ignition experiments.

A Kirkpatrick-Baez X-ray microscope has been developed for use on the Titan laser facility at the Lawrence Livermore National Laboratory in Fast Ignition experiments. It was developed as a broadband alternative to narrow band Bragg crystal imagers for imaging Kα emission from tracer layers. A re-entrant design is employed which allows for alignment from outside the chamber. The mirrors are coated with Pt and operate at a grazing incident angle of 0.5° providing higher resolution than an equal brightness pinhole and sufficient bandwidth to image thermally shifted characteristic Kα emission from heated Cu tracer layers in Fast Ignition experiments. The superpolished substrates (<1 Å rms roughness) had a final visible wavelength roughness of 1.7 Å after coating, and exhibited a reflectivity corresponding to an X-ray wavelength roughness of 7 ± 1 Å. A unique feature of this design is that during experiments, the unfiltered direct signal along with the one-dimensional reflections are retained on the detector in order to enable a live indication of alignment and incident angle. The broad spectral window from 4 to 9 keV enables simultaneous observation of emission from several spectral regions of interest, which has been demonstrated to be particularly useful for cone-wire targets. An experimentally measured resolution of 15 µm has been obtained at the center of the field of view.

Laser wakefield generated X-ray probe for femtosecond time-resolved measurements of ionization states of warm dense aluminum.

We have developed a laser wakefield generated X-ray probe to directly measure the temporal evolution of the ionization states in warm dense aluminum by means of absorption spectroscopy. As a promising alternative to the free electron excited X-ray sources, Betatron X-ray radiation, with femtosecond pulse duration, provides a new technique to diagnose femtosecond to picosecond transitions in the atomic structure. The X-ray probe system consists of an adjustable Kirkpatrick-Baez (KB) microscope for focusing the Betatron emission to a small probe spot on the sample being measured, and a flat Potassium Acid Phthalate Bragg crystal spectrometer to measure the transmitted X-ray spectrum in the region of the aluminum K-edge absorption lines. An X-ray focal spot size of around 50 µm was achieved after reflection from the platinum-coated 10-cm-long KB microscope mirrors. Shot to shot positioning stability of the Betatron radiation was measured resulting in an rms shot to shot variation in spatial pointing on the sample of 16 µm. The entire probe setup had a spectral resolution of ~1.5 eV, a detection bandwidth of ~24 eV, and an overall photon throughput efficiency of the order of 10(-5). Approximately 10 photons were detected by the X-ray CCD per laser shot within the spectrally resolved detection band. Thus, it is expected that hundreds of shots will be required per absorption spectrum to clearly observe the K-shell absorption features expected from the ionization states of the warm dense aluminum.