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P. Brumer

Publications and source records attributed to P. Brumer.

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Steady-State Coherences under Partial Collective non-Markovian Decoherence

Steady-state coherence in open quantum systems is crucial for quantum technologies, yet its behavior is not fully understood due to the interplay between collective and individual decoherence. While collective decoherence is thought to induce steady-state coherence, experiments often fail to observe this because of individual decoherence. We study a system of two harmonic oscillators coupled to both individual and collective environments, introducing a tunable parameter to adjust the decoherence proportions. By analytically solving the exact dynamical equations, we find that steady-state coherence depends on the initial state under collective decoherence, but not under partial decoherence. Interestingly, non-Markovianity induces rich and complex steady-state coherence behaviors. Our results offer new insights into the role of non-Markovian decoherence in quantum systems and serve as a benchmark for evaluating approximate methods in modelling quantum processes.

quant-ph

Quantum Yields from Stationary States: Cis-Trans Isomerization of Model Retinal

Cis-trans isomerization in retinal, the first step in vision, is often computationally studied from a time dependent viewpoint. Motivation for such studies lies in coherent pulsed laser experiments that explore the isomerization dynamics. However, such biological processes take place naturally in the presence of incoherent light, which excites a non-evolving mixture of stationary states. Here the isomerization problem is considered from the latter viewpoint and applied to a standard two-state, two-mode linear vibronic coupling model of retinal that explicitly includes a conical intersection between the ground and first excited electronic states. The calculated quantum yield at 500 nm agrees well with both the previous time-dependent calculations of Hahn and Stock (0.63) and with experiment ($0.65\pm0.01$), as does its wavelength dependence. Significantly, the effects of environmental relaxation on the quantum yield in this well-established model are found to be negligible. The results make clear the connection of the photoisomerization quantum yield to properties of stationary eigenstates, providing alternate insights into conditions for yield optimization.

physics.chem-ph

Temperature crossover of decoherence rates in chaotic and regular bath dynamics

The effect of chaotic bath dynamics on the decoherence of a quantum system is examined for the vibrational degrees of freedom of a diatomic molecule in a realistic, constant temperature collisional bath. As an example, the specific case of I$_2$ in liquid xenon is examined as a function of temperature, and the results compared with an integrable xenon bath. A crossover in behavior is found: the integrable bath induces more decoherence at low bath temperatures than does the chaotic bath, whereas the opposite is the case at the higher bath temperatures. These results, verifying a conjecture due to Wilkie, shed light on the differing views of the effect of chaotic dynamics on system decoherence.

quant-ph

Overlapping resonances in the control of intramolecular vibrational redistribution

Coherent control of bound state processes via the interfering overlapping resonances scenario [Christopher et al., J. Chem. Phys. 123, 064313 (2006)] is developed to control intramolecular vibrational redistribution (IVR). The approach is applied to the flow of population between bonds in a model of chaotic OCS vibrational dynamics, showing the ability to significantly alter the extent and rate of IVR by varying quantum interference contributions.

quant-ph

Aspects of quantum coherence in the optical Bloch equations

Aspects of coherence and decoherence are analyzed within the optical Bloch equations. By rewriting the analytic solution in an alternate form, we are able to emphasize a number of unusual features: (a) despite the Markovian nature of the bath, coherence at long times can be retained; (b) the long-time asymptotic degree of coherence in the system is intertwined with the asymptotic difference in level populations; (c) the traditional population-relaxation and decoherence times, $T_1$ and $T_2$, lose their meaning when the system is in the presence of an external field, and are replaced by more general overall timescales; (d) increasing the field strength, quantified by the Rabi frequency, $Ω$, increases the rate of decoherence rather than reducing it, as one might expect; and (e) maximum asymptotic coherence is reached when the system parameters satisfy $Ω^2 = 1/(T_1 T_2)$.

quant-ph