Thermal-Light-Induced Dynamics: Coherence and Revivals in V- and Extended Jaynes-Cummings Systems


  David Avisar  ,  Arlene D. Wilson-Gordon  
Department of Chemistry, Bar-Ilan University

For more than 20 years, the interaction of thermal light with matter has been in the focus of experimental and theoretical research aimed at understanding sunlight-induced photochemistry in photosynthetic systems and, in particular, its coherence properties. In order to achieve a better characterization of thermal light induced material dynamics, we examine the interaction of thermal light with matter with emphasis on two aspects that have not considered before. 1) By employing a fully quantized Jaynes-Cummings-type interaction model on a V-type three-level system, we show that multi-mode thermal light induces coherence in the excited material states. We also show that in some ratios of the detuning and the interaction constant, the thermal light induces dynamics with a 'coherent-like' structure rather than the familiar 'chaotic' one. 2) We extend the Jaynes-Cummings model to a two-state Born-Oppenheimer potential energy surface molecular system, where the internal vibrational degrees of freedom are fully taken into account, and show that single-mode thermal light induces extensive vibrational coherence in the molecular excited state. This coherence is manifested by wavepacket-like dynamics in the coordinate-space representation. These results call for reconsidering some of the previous conclusions reached in the context of thermal light induced material coherence.