Quantum coherent vibrational relaxation of an impurity strongly coupled to its solid host is demonstrated through four-wave mixing measurements to infer sustained coherence in the bath, which is recognized as a superposition of macroscopically distinct states.
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 I(2) 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.
We focus on a dissipative three-level system as a case study to analytically demonstrate that strong system-bath coupling separates the relaxation dynamics of this dissipative quantum system into two distinct regimes: a short-time dynamics that, as expected, accelerates with increasing coupling to the environment, and a slow dynamics that, counterintuitively, becomes prolonged at sufficiently strong coupling. Using the reaction-coordinate polaron-transform mapping, we uncover the general mechanism behind this effect and derive accurate expressions for both relaxation timescales. Numerical simulations confirm our analytical predictions. From a practical perspective, our results suggest that strong coupling to a dissipative bath can autonomously generate and sustain long-lived quantum coherences, offering a promising strategy for bath-engineered quantum state preparation.
The technique of COIN (coherence observation by interference noise) relies on the measurement of correlated fluorescence fluctuations subsequent to two-pulse excitation with randomized relative phase [Kinrot et al., Phys. Rev. Lett. 75, 3822 (1995)]. In this paper, a comprehensive theoretical study on the use of random-phase fluorescence interferometry in the measurement of solid-state, molecular coherence is given. Optical response functions in terms of populations expanded to second order in a perturbational approach are presented for a guest/host system that are based on a generalized Bloch–Liouville formalism including inhomogeneous site broadening and harmonic vibrational modes. The theoretical treatment is intended to explain the coherence and coherence loss mechanisms measured, very recently, in the pentacene/p-terphenyl mixed crystal at low phonon temperatures. The expressions derived within the limits of the usual approximations are quite general and valid for both δ- and finite-width pulses. The perturbative solutions reproduce the temperature variation of the experimental COIN interferograms and reveal the effects of inhomogeneous dephasing and impurity–bath coupling, quite satisfactorily.