Two-quantum 2D FT electronic spectroscopy of biexcitons in GaAs quantum wells

The motions of electrons in solids may be highly correlated by strong, long-range Coulomb interactions. Correlated electron-hole pairs (excitons) are accessed spectroscopically through their allowed single-quantum transitions, but higher-order correlations that may strongly influence electronic and optical properties have been far more elusive to study. Here we report direct observation of bound exciton pairs (biexcitons) that provide incisive signatures of four-body correlations among electrons and holes in gallium arsenide (GaAs) quantum wells. Four distinct, mutually coherent, ultrashort optical pulses were used to create coherent exciton states, transform these successively into coherent biexciton states and then new radiative exciton states, and finally to read out the radiated signals, yielding biexciton binding energies through a technique closely analogous to multiple-quantum two-dimensional Fourier transform (2D FT) nuclear magnetic resonance spectroscopy. A measured variation of the biexciton dephasing rate indicated still higher-order correlations.