Dynamics of incoherent exciton formation in C u2 O: Time- And angle-resolved photoemission spectroscopy

We study the dynamics of incoherent exciton formation under interband photoexcitation in Cu2O using time-and angle-resolved photoemission spectroscopy at 90 K. Hot electrons injected by allowed optical transitions with 3.40-eV photons show ultrafast relaxation to the conduction-band minimum (CBM), surviving up to 500 fs after excitation. Whereas hot-electron states with high excess energy show a rapid population decay of ∼25 fs, an abrupt increase to 130 fs is observed for states with excess energies of 0.15 eV. This latter is interpreted in terms of phonon bottleneck dynamics characteristic of longitudinal-optical phonon mediated energy relaxation. Excitons, having a small binding energy of 60 meV, are formed below the CBM quasi-instantaneously and subsequently relax to the 1S-exciton state of the yellow series within 1.5 ps. We find that, together with possible plasma screening for electron-hole interaction, the cooling of exciton center-of-mass motion plays an important role in the exciton relaxation dynamics. The characteristic features of exciton photoionization process are critically discussed based on the detailed analysis of angle-resolved photoemission results for the 1S excitons formed 1.5 ps after excitation.