Nonlinear coherent spectroscopy: The contribution due to an excitation induced shift

Frank Schlawin

Daniel Webber, Brian L. Wilmer, Xiao Liu +4 more

Transient four-wave mixing studies of bulk GaAs under conditions of broad bandwidth excitation of primarily interband transitions have enabled four-particle correlations tied to degenerate (exciton-exciton) and nondegenerate (exciton-carrier) interactions to be studied. Real two-dimensional Fourier-transform spectroscopy (2DFTS) spectra reveal a complex response at the heavy-hole exciton emission energy that varies with the absorption energy, ranging from dispersive on the diagonal through absorptive for low-energy interband transitions to dispersive with the opposite sign for interband transitions high above band gap. Simulations using a multilevel model augmented by many-body effects provide excellent agreement with the 2DFTS experiments and indicate that excitation-induced dephasing (EID) and excitation-induced shift (EIS) affect degenerate and nondegenerate interactions equivalently, with stronger exciton-carrier coupling relative to exciton-exciton coupling by approximately an order of magnitude. These simulations also indicate that EID effects are three times stronger than EIS in contributing to the coherent response of the semiconductor.

Wolfgang Demtröder

Tengfei Meng, Zhonghua Ji, Dianqiang Su +3 more

We theoretically present the nonlinear selective reflection spectroscopy of V‐type atomic system at gas‐solid interface in a pump‐probe scheme. The saturation and coherence effects are distinguished by solving Liouville equation in the absence and presence of reduced density matrix element between the two excited levels. When the coherence effect exists, two peaks appear in reflection spectroscopy with asymmetry lineshape. We investigate the dependence of reflection spectroscopy on pump field intensity, frequency detuning and coherent decay rate induced by collision between atoms. The lineshape can be explained based on reflection spectroscopy contributed from atoms with negative (before collision) and positive (after collision) velocities, single‐photon and two‐photon processes. This study is helpful for investigating quantum coherence and dynamic processes of atoms at gas‐solid interface.

Nikolai I Koroteev, M F Ternovskaya

It is shown that in order to obtain a correct interpretation of experiments on four-photon nonlinear spectroscopy within the absorption line, it is necessary to allow not only for a coherent four-photon process due to a resonant electronic nonlinearity but also for a similar process involving generation of optically induced diffraction gratings followed by the diffraction of one of the probe beams from these gratings. It is also necessary to allow for the contribution of highly excited molecular states to the resonant electronic nonlinearity. General expressions are derived and investigated for the cubic susceptibility in an isotropic medium. It is found that all nonzero components of this tensor may be expressed in terms of a single scalar function of the interacting wave frequencies. The explicit form of this function is determined in the lowest order of perturbation theory.