Interband second-order nonlinear optical susceptibility of asymmetric coupled quantum wells

Asymmetric molecular bonds possess a microscopic second-order nonlinear optical polarizability p((2)). Crystals built from them possess a macroscopic second-order nonlinear optical susceptibility, chi((2)), if their structure lacks centrosymmetry. chi((2)) can be enhanced by introducing additional asymmetry at the meta-structural level. Here, we use a dipole matrix formalism to calculate chi((2)) of asymmetric GaAs/AlGaAs coupled quantum well structures at telecommunication frequencies, for which interband (rather than previously considered intersubband) optical transitions govern optical nonlinearities. Using unit cell and envelope wavefunctions and considering all possible transitions between two bound electron and two bound hole states, we predict tenfold enhancement in chi((2)) in previously underexplored ranges of quantum well asymmetry and coupling barrier thickness. This work paves the way toward enhanced, tailorable second-order optical nonlinearities for semiconductor digital alloy and superlattice structures.