The even exciton series in Cu$_2$O

Abstract

In $\mathrm{Cu_{2}O}$ parity is a good quantum number and thus the exciton spectrum falls into two parts: The dipole-active exciton states of negative parity and odd angular momentum, which can be observed in one-photon absorption ($Γ_4^-$ symmetry) and the exciton states of positive parity and even angular momentum, which can be observed in two-photon absorption ($Γ_5^+$ symmetry). The unexpected observation of $D$ excitons in two-photon absorption and of $F$ excitons in one-photon absorption has given evidence that the dispersion properties of the $Γ_5^+$ orbital valence band is giving rise to a coupling of the yellow and green exciton series. In this paper we show that the even and odd parity exciton system can be consistently described within the same theoretical approach. However, the Hamiltonian of the even parity system needs, in comparison to the odd exciton case, modifications to account for the very small radius of the $1S$ exciton. In the presented treatment we take special care of the central-cell corrections, which comprise a reduced screening of the Coulomb potential at distances comparable to the polaron radius, the exchange interaction being responsible for the exciton splitting into ortho and para states, and the inclusion of terms in the fourth power of $p$ in the kinetic energy. Since the yellow $1S$ exciton state is coupled to all other states of positive parity, we show how the central-cell corrections affect the whole even exciton series. The close resonance of the $1S$ green exciton with states of the yellow exciton series has a strong impact on the energies and oscillator strengths of all implied states. The consistency between theory and experiment with respect to energies and oscillator strengths for the even and odd exciton system in $\mathrm{Cu_{2}O}$ is a convincing proof for the validity of the applied theory.