Contributions of Bound and Unbound Two-Exciton States to the Nonlinear Optical Response of GaAs Quantum Wells

The strong influence of exciton/exciton interaction on the nonlinear optical response of the 2D exciton in GaAs quantum wells has been demonstrated in several recent experimental studies. The theoretical model for the microscopic coupling mechanism is still the subject of controversy, however. In ref. [1], we have presented a model including a density dependent coupling between opposite spin excitons which assumes that the interaction results in a renormalization of the matrix elements, dephasing rates and energies of the transition from the single-exciton state to the two-exciton state with respect to the corresponding quantities for the single exciton transitions. In contrast, Wang et al. claim that all experimental observations are explained by a density induced dephasing rate and that biexciton states play no role [2]. Here we present a new 3-pulse degenerate-four-wave-mixing (DFWM) configuration which is able to differentiate between pure local field effects and biexcitonic contributions to the time-integrated signal. Experiments were performed on an almost homogeneously broadened GaAs/Al0.3Ga0.7As single QW (well width 20 nm, photoluminescence line 0.3 meV, homogenous linewidth 0.15 meV) in the backward reflection geometry. The sample was cooled to 10 K and excited by a sequence of three pulses (1.1 ps duration) with equal intensity, wave vectors 𝑘→1,𝑘→2,𝑘→3 and delays τ12 and τ13 between the second and first and the third and first pulse, respectively. The signal was monitored in the direction 𝑘→𝑠=𝑘→1+𝑘→2−𝑘→3 which provides no signal for the chosen pulse length if local field and renormalization effects are negligible. The peak intensity of the time-integrated DFWM signal has been calculated by solving the optical Bloch for a system of two non-interacting two-level systems (2LS) with opposite circular polarization selection rules (local field effect) and for the renormalized four-level system (4LS) depicted in Fig. 1 which assumes the formation of biexcitons between excitons with opposite spins. The signal strength is proportional to the strength of the local field in the case of the 2LS and to the renormalization for the 4LS. The peak signal intensities expected for pure local field and pure biexction contributions are summarized in the second and third column of Table 1 for eight experimental configurations applying different linear and circularly polarized pulses. The values are normalized to the signal strength predicted for three parallel linearly polarized pulses. Close inspection of the data reveals remarkable differences of the peak amplitude with polarization geometry for the two coupling models.