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The electronic behavior of various solid metals (Al, Ni, Cu, Au, Ti, and W)under ultrashort laser irradiation is investigated by means of densityfunctional theory. Successive stages of extreme nonequilibrium on picosecondtime scale impact the excited material properties in terms of optical couplingand transport characteristics. As these are generally modelled based on thefree-electron classical theory, the free-electron number is a key parameter.However, this parameter remains unclearly defined and dependencies on theelectronic temperature are not considered. Here, from first-principlescalculations, density of states are obtained with respect to electronictemperatures varying from 10^-2 to 10^5 K within a cold lattice. Based on theconcept of localized or delocalized electronic states, temperature dependentfree-electron numbers are evaluated for a series of metals covering a largerange of electronic configurations. With the increase of the electronictemperature we observe strong adjustments of the electronic structures oftransition metals. These are related to variations of electronic occupation inlocalized d bands, via change in electronic screening and electron-ioneffective potential. The electronic temperature dependence of nonequilibriumdensity of states has consequences on electronic chemical potentials,free-electron numbers, electronic heat capacities, and electronic pressures.Thus electronic thermodynamic properties are computed and discussed, serving asa base to derive energetic and transport properties allowing the description ofexcitation and relaxation phenomena caused by rapid laser action.

Free-electron properties of metals under ultrafast laser-induced electron-phonon nonequilibrium: A first-principles study