Phase-sensitive stimulated Raman adiabatic passage in dipolar extended lambda systems.
The authors investigate the possible phase-sensitive behavior of (multiphoton) stimulated Raman adiabatic passage population transfer in extended lambda systems, if more than one state of an anharmonic progression of target levels is accessible in transitions of different photonicities. They use a minimal model four-level system (4LS) with one initial state separated from two target states by an apex state. The parameters of the 4LS are adapted from the bend states of the HCN-HNC system. Using a dressed-state analysis within the rotating wave approximation (RWA), the authors identify phase-dependent diabatic transitions between the two dressed states contributing to the state vector as the mechanism leading to phase-sensitive target populations. The essential features giving rise to the phase dependence are found to be different (non-zero-) diagonal elements of the dipole matrix, i.e., permanent dipole moments, and the presence of a direct two-photon overtone coupling between the apex state and the lower target state which formally enters the RWA Hamiltonian upon inclusion of permanent dipole moments. Among the parameters controlling the extent of the effect are the anharmonic properties of the target progression and the absolute values of the field frequencies, so that in view of the requirement to tune the driving fields into the vicinity of resonance, details of the level structure are of importance. A comparative numerical study executed without invoking RWA shows that qualitatively there are similar trends in the appearance of phase sensitivity, although the effects are considerably more pronounced in the full treatment. In the full treatment the authors also explore off-resonance conditions and discuss the signatures of phase sensitivity in the target populations.
Marx
Christoph A
CA
Institut für Theoretische Chemie, Universität Wien, Währingerstrasse 17, 1090 Wien, Austria. cmarx@uci.edu
Jakubetz
Werner
W