Coherent transient in photoluminescence of excitonic molecules in GaAs quantum wells

Time-resolved photoluminescence (PL) of excitonic molecules in GaAs quantum wells (QW’s) reveals an initial transient characterized by a finite rise and an extremely fast nonexponential decay [H. Wang, J. Shah, and T. C. Damen et al., Solid State Commun. 98, 807 (1996)]. The transient is attributed to coherent quantum evolution towards the molecule ground state of two optically correlated excitons, ${\sigma }^{+}$ and ${\sigma }^{-},$ which undergo the Coulombic attraction. In the present paper, we develop a theory of the transient PL and fit the experimental data. The radiative decay of a quasi-two-dimensional (2D) excitonic molecule is analyzed with the giant oscillator strength model adapted to QW’s and with the bipolariton model. Within the 2D bipolariton model, the main “hidden” channel of the radiative decay of an excitonic molecule is the resonant dissociation into two outgoing interface (surface) polaritons rather than the observable decay into the bulk radiative modes. We conclude that quasi-2D molecules dissociate already within the initial transient of PL, while the following exponential decay of the molecule-mediated PL is due to the escape of secondary interface polaritons into the bulk modes. According to the 2D bipolariton model, the sequence “two incoming $\mathrm{photons}\to \mathrm{two}$ virtual $\mathrm{excitons}\to 2\mathrm{D}$ $\mathrm{molecule}\to \mathrm{two}$ outgoing interface polaritons” is a completely coherent process. The fit of the time-resolved molecule-mediated PL provides us with numerical estimates of the exciton-photon coupling in GaAs QW’s.