Dynamics of incoherent exciton formation in Cu${}_2$O: Time- and angle-resolved photoemission spectroscopy

Abstract

We study dynamics of incoherent exciton formation under interband photoexcitation in Cu${}_2$O 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. While 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 LO-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.

35 pages, 14 figures

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• Coherence and de-coherence in the Time-Resolved ARPES of realistic materials: an ab-initio perspective
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