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

TL;DR

This study investigates the ultrafast formation and relaxation dynamics of incoherent excitons in Cu$_2$O using time- and angle-resolved photoemission spectroscopy, revealing phonon bottleneck effects and exciton relaxation pathways.

Contribution

It provides the first detailed time-resolved analysis of exciton formation and relaxation in Cu$_2$O, highlighting the roles of phonon bottleneck and plasma screening in exciton dynamics.

Findings

Hot electrons relax to CBM within 25 fs

Excitons form quasi-instantaneously below CBM

Excitons relax to 1S state within 1.5 ps

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.