Evolution of ac conductivity in nonequilibrium warm dense gold.

Using a chirped pulse probe technique, we have obtained single-shot measurements of temporal evolution of ac conductivity at 1.55 eV (800 nm) during electron energy relaxation in nonequilibrium warm dense gold with energy densities up to 4.1 MJ/kg (8×10(10) J/m3). The results uncover important changes that have been masked in an earlier experiment. Equally significant, they provide valuable tests of an ab initio model for the calculation of electron heat capacity, electron-ion coupling, and ac conductivity in a single, first principles framework. While measurements of the real part of ac conductivity corroborate our theoretical temperature-dependent electron heat capacity, they point to an electron-ion coupling factor of ∼2.2×10(16) W/m3 K, significantly below that predicted by theory. In addition, measurements of the imaginary part of ac conductivity reveal the need to improve theoretical treatment of intraband contributions at very low photon energy.

Flux-limited nonequilibrium electron energy transport in warm dense gold.

An abrupt change in energy transport has been observed in femtosecond laser heated gold when the absorbed laser flux exceeds ~7×10(12) W/cm(2). Below this value, the absorbed flux is carried by ballistic motion of nonthermal electrons produced in interband excitation. Above this value energy transport appears to include ballistic transport by nonthermal electrons and heat diffusion by thermalized hot electrons. The ballistic component is limited to a flux of ~7×10(12) W/cm(2). This offers a unique benchmark for comparison with theory on nonequilibrium electron transport.

Pi resonance of chemisorbed alkali atoms on noble metals.

We have performed a joint experimental and theoretical study of the unoccupied electronic structure of alkali adsorbates on the (111) surfaces of Cu and Ag. Combining angle- and time-resolved two-photon photoemission spectroscopy with wave packet propagation calculations we show that, along with the well known sigma resonance oriented along the surface normal, there exist long-lived alkali-localized resonances oriented parallel to the surface (pi symmetry). These new resonances are stabilized by the projected band gap of the substrate and emerge primarily from the mixing of the p and d Rydberg orbitals of the free alkali atom modified by the interaction with the surface.