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.Comment: 7 pages, 3 figure

Influence of Non-Markovian Dynamics in Thermal-Equilibrium Uncertainty-Relations

Contrary to the conventional wisdom that deviations from standard thermodynamics originate from the strong coupling to the bath, it is shown that in quantum mechanics, these deviations originate from the uncertainty principle and are supported by the non-Markovian character of the dynamics. Specifically, it is shown that the lower bound of the dispersion of the total energy of the system, imposed by the uncertainty principle, is dominated by the bath power spectrum and therefore, quantum mechanics inhibits the system thermal-equilibrium-state from being described by the canonical Boltzmann's distribution. We show that for a wide class of systems, systems interacting via central forces with pairwise-self-interacting environments, this general observation is in sharp contrast to the classical case, for which the thermal equilibrium distribution, irrespective of the interaction strength, is \emph{exactly} characterized by the canonical Boltzmann distribution and therefore, no dependence on the bath power spectrum is present. We define an \emph{effective coupling} to the environment that depends on all energy scales in the system and reservoir interaction. Sample computations in regimes predicted by this effective coupling are demonstrated. For example, for the case of strong effective coupling, deviations from standard thermodynamics are present and, for the case of weak effective coupling, quantum features such as stationary entanglement are possible at high temperatures.Comment: 9 pages, 3 figure

Engineering an all-optical route to ultracold molecules in their vibronic ground state

We propose an improved photoassociation scheme to produce ultracold molecules in their vibronic ground state for the generic case where non-adiabatic effects facilitating transfer to deeply bound levels are absent. Formation of molecules is achieved by short laser pulses in a Raman-like pump-dump process where an additional near-infrared laser field couples the excited state to an auxiliary state. The coupling due to the additional field effectively changes the shape of the excited state potential and allows for efficient population transfer to low-lying vibrational levels of the electronic ground state. Repetition of many pump-dump sequences together with collisional relaxation allows for accumulation of molecules in v=0.Comment: Phys. Rev. A, in pres

Statistical mechanics of Floquet systems with regular and chaotic states

We investigate the asymptotic state of time-periodic quantum systems with regular and chaotic Floquet states weakly coupled to a heat bath. The asymptotic occupation probabilities of these two types of states follow fundamentally different distributions. Among regular states the probability decreases from the state in the center of a regular island to the outermost state by orders of magnitude, while chaotic states have almost equal probabilities. We derive an analytical expression for the occupations of regular states of kicked systems, which depends on the winding numbers of the regular tori and the parameters temperature and driving frequency. For a constant winding number within a regular island it simplifies to Boltzmann-like weights \exp(-\betaeff \Ereg_m), similar to time-independent systems. For this we introduce the regular energies \Ereg_m of the quantizing tori and an effective winding-number-dependent temperature 1/\betaeff, different from the actual bath temperature. Furthermore, the occupations of other typical Floquet states in a mixed phase space are studied, i.e. regular states on nonlinear resonances, beach states, and hierarchical states, giving rise to distinct features in the occupation distribution. Avoided crossings involving a regular state lead to drastic consequences for the entire set of occupations. We introduce a simplified rate model whose analytical solutions describe the occupations quite accurately.Comment: 18 pages, 11 figure

Decoherence Effects in Reactive Scattering

Decoherence effects on quantum and classical dynamics in reactive scattering are examined using a Caldeira-Leggett type model. Through a study of dynamics of the collinear H+H2 reaction and the transmission over simple one-dimensional barrier potentials, we show that decoherence leads to improved agreement between quantum and classical reaction and transmission probabilities, primarily by increasing the energy dispersion in a well defined way. Increased potential nonlinearity is seen to require larger decoherence in order to attain comparable quantum-classical agreement.Comment: 25 pages, 6 figures, to be published in J. Chem. Phy

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.Comment: 10 pages, 7 figure