Time- and angle-resolved photoelectron spectroscopy is employed to study the thermalization of a nonequilibrium carrier distribution in the Dirac cone of graphite generated upon absorption of linearly polarized near-infrared laser pulses. The data reveal a characteristic time constant of $(20\ifmmode\pm\else\textpm\fi{}3)\phantom{\rule{0.16em}{0ex}}\mathrm{fs}$ for the decay of a photoinduced momentum anisotropy in the nascent carrier population. Additionally, the nascent carrier spectral peak shows a downshift in energy by $\ensuremath{\sim}100\phantom{\rule{0.16em}{0ex}}\mathrm{m}\mathrm{eV}$ within the first $30\phantom{\rule{0.16em}{0ex}}\mathrm{f}\mathrm{s}$ after excitation, which is associated with the emission of strongly coupled ${A}_{1}^{\ensuremath{'}}$ optical phonons at $K$. In agreement with previous findings for graphene, a pronounced momentum anisotropy is also observed for an intermediate quasithermalized state of the carrier population. A fully thermalized distribution (with respect to energy and momentum) is finally established on a characteristic timescale of $(40\ifmmode\pm\else\textpm\fi{}10)\phantom{\rule{0.16em}{0ex}}\mathrm{fs}$. The results underscore the complexity of carrier thermalization on ultrafast timescales resulting from the interplay of carrier-carrier and carrier-phonon interaction.
Read full abstract