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.
Time-resolved coherent anti-Stokes Raman scattering is applied to prepare and interrogate vibrational coherences on the ground electronic surface of molecular iodine isolated in Ar matrices. The coherence decay time shows a linear dependence on vibrational quantum numbers for vϭ3-15. The temperature dependence of decoherence rates is negligible for vϽ7 in the experimental range Tϭ18-32 K. For a vϭ13, 14 superposition, the temperature dependence indicates dephasing by a 66 cm Ϫ1 pseudo-local phonon, just outside the Debye edge of the solid. The accuracy of the data is limited due to two-photon induced dissociation of the molecule, a process which is characterized using polarized fields. The T→0 limit of dephasing is discussed.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.