Dissipative quantum coherent dynamics probed in phase-space: Electronically resonant 5-color 4-wave mixing on I2(B) in solid Kr

摘要

Spectrally resolved, 4-wave mixing measurements in five resonant colors are used to interrogate vibronic quantum coherences in phase-space. We highlight the principles through measurements on the B-state of I2 in solid Kr – a prototype of a system strongly coupled to its environment. The measurements consist of preparing a superposition of wavepackets on the B-state and interrogating their cross-coherence as they get entangled with the environment. The study provides direct realizations of fundamental quantum principles in the mechanics of molecular matter, among them: the distinction between quantum and classical coherent dynamics of a system entangled with the environment, coherent dissipation, event-driven decoherence, environment selected coherent states, and non-local mechanics. © 2011 American Institute of Physics Article Outline INTRODUCTION EXPERIMENTAL RESULTS AND ANALYSIS Coherence in the spectral coordinate Differential scattering between k-vetor tagged packets Coherent dissipation in a driven common bath Decoherence in energy representation Synchronization between packets Heterodyned four-wave signal Selection by the environment: Arrested dissipation in a quiescent cage Two-time correlation Dependence on spectral overlap CONCLUSIONS