Leonardo A. Pachon

Bringing Entanglement to the High Temperature Limit

Decoherence due to contact with a hot environment typically restricts quantum phenomena to the low temperature limit, k_{B}T/ℏω≪1 (ℏω is the typical energy of the system). Here we report the existence of a nonequilibrium state for two coupled, parametrically driven, dissipative harmonic oscillators which, contrary to generalized intuition, has stationary entanglement at high temperatures. This clarifies the role of temperature and could lighten the burden on quantum experiments requiring delicate precooling setups.

Physical Basis for Long-Lived Electronic Coherence in Photosynthetic Light-Harvesting Systems

The physical basis for observed long-lived electronic coherence in photosynthetic light-harvesting systems is identified using an analytically soluble model. Three physical features are found to be responsible for their long coherence lifetimes, (i) the small energy gap between excitonic states, (ii) the small ratio of the energy gap to the coupling between excitonic states, and (iii) the fact that the molecular characteristics place the system in an effective low-temperature regime, even at ambient conditions. Using this approach, we obtain decoherence times for a dimer model with FMO parameters of ∼160 fs at 77 K and ∼80 fs at 277 K. As such, significant oscillations are found to persist for 600 and 300 fs, respectively, in accord with the experiment and with previous computations. Similar good agreement is found for PC645 at room temperature, with oscillations persisting for 400 fs. The analytic expressions obtained provide direct insight into the parameter dependence of the decoherence time scales.

Semiclassical propagation of Wigner functions

We present a comprehensive study of semiclassical phase-space propagation in the Wigner representation, emphasizing numerical applications, in particular as an initial-value representation. Two semiclassical approximation schemes are discussed. The propagator of the Wigner function based on van Vlecks approximation replaces the Liouville propagator by a quantum spot with an oscillatory pattern reflecting the interference between pairs of classical trajectories. Employing phase-space path integration instead, caustics in the quantum spot are resolved in terms of Airy functions. We apply both to two benchmark models of nonlinear molecular potentials, the Morse oscillator and the quartic double well, to test them in standard tasks such as computing autocorrelation functions and propagating coherent states. The performance of semiclassical Wigner propagation is very good even in the presence of marked quantum effects, e.g., in coherent tunneling and in propagating Schrodinger cat states, and of classical chaos in four-dimensional phase space. We suggest options for an effective numerical implementation of our method and for integrating it in Monte-Carlo-Metropolis algorithms suitable for high-dimensional systems.

Mechanisms in environmentally assisted one-photon phase control

The ability of an environment to assist in one-photon phase control relies upon entanglement between the system and bath and on the breaking of the time reversal symmetry. Here, one-photon phase control is examined analytically and numerically in a model system, allowing an analysis of the relative strength of these contributions. Further, the significant role of non-Markovian dynamics and of moderate system-bath coupling in enhancing one-photon phase control is demonstrated, and an explicit role for quantum mechanics is noted in the existence of initial non-zero stationary coherences. Finally, desirable conditions are shown to be required to observe such environmentally assisted control, since the system will naturally equilibrate with its environment at longer times, ultimately resulting in the loss of phase control.

Synchronization in a semiclassical Kuramoto model

Synchronization is a ubiquitous phenomenon occurring in social, biological, and technological systems when the internal rythms of their constituents are adapted to be in unison as a result of their coupling. This natural tendency towards dynamical consensus has spurred a large body of theoretical and experimental research in recent decades. The Kuramoto model constitutes the most studied and paradigmatic framework in which to study synchronization. In particular, it shows how synchronization appears as a phase transition from a dynamically disordered state at some critical value for the coupling strength between the interacting units. The critical properties of the synchronization transition of this model have been widely studied and many variants of its formulations have been considered to address different physical realizations. However, the Kuramoto model has been studied only within the domain of classical dynamics, thus neglecting its applications for the study of quantum synchronization phenomena. Based on a system-bath approach and within the Feynman path-integral formalism, we derive equations for the Kuramoto model by taking into account the first quantum fluctuations. We also analyze its critical properties, the main result being the derivation of the value for the synchronization onset. This critical coupling increases its value as quantumness increases, as a consequence of the possibility of tunneling that quantum fluctuations provide.

Nonclassical phase-space trajectories for the damped harmonic quantum oscillator

The phase-space path-integral approach to the damped harmonic oscillator is analyzed beyond the Markovian approximation. It is found that pairs of nonclassical trajectories contribute to the path-integral representation of the Wigner propagating function. Due to the linearity of the problem, the sum coordinate of a pair still satisfies the classical equation of motion. Furthermore, it is shown that the broadening of the Wigner propagating function of the damped oscillator arises due to the time-nonlocal interaction mediated by the heat bath.

Time-Domain Scars: Resolving the Spectral Form Factor in Phase Space

We study the relationship of the spectral form factor with quantum as well as classical probabilities to return. Defining a quantum return probability in phase space as a trace over the propagator of the Wigner function allows us to identify and resolve manifolds in phase space that contribute to the form factor. They can be associated with classical invariant manifolds such as periodic orbits, but also to nonclassical structures such as sets of midpoints between periodic points. In contrast to scars in wave functions, these features are not subject to the uncertainty relation and therefore need not show any smearing. They constitute important exceptions from a continuous convergence in the classical limit of the Wigner towards the Liouville propagator. We support our theory with numerical results for the quantum cat map and the harmonically driven quartic oscillator.

Classical approach to multichromophoric resonance energy transfer.

A classical formulation of the quantum multichromophoric theory of resonance energy transfer is developed on the basis of classical electrodynamics. The theory allows for the identification of a variety of processes of different order in the interactions that contribute to the energy transfer in molecular aggregates with intracoupling in donors and acceptor chromophores. Enhanced rates in multichromophoric resonance energy transfer are shown to be well described by this theory. Specifically, in a coupling configuration between N_{A} acceptors and N_{D} donors, the theory correctly predicts an enhancement of the energy transfer rate dependent on the total number of donor-acceptor pairs. As an example, the theory, applied to the transfer rate in light harvesting II, gives results in excellent agreement with experiment. Finally, it is explicitly shown that as long as linear response theory holds, the classical multichromophoric theory formally coincides with the quantum formulation.

Quantum driven dissipative parametric oscillator in a blackbody radiation field

We consider the general open system problem of a charged quantum oscillator confined in a harmonic trap, whose frequency can be arbitrarily modulated in time, that interacts with both an incoherent quantized (blackbody) radiation field and with an arbitrary coherent laser field. We assume that the oscillator is initially in thermodynamic equilibrium with its environment, a non-factorized initial density matrix of the system and the environment, and that at t = 0 the modulation of the frequency, the coupling to the incoherent and the coherent radiation are switched on. The subsequent dynamics, induced by the presence of the blackbody radiation, the laser field, and the frequency modulation, is studied in the framework of the influence functional approach. This approach allows incorporating, in analytic closed formulae, the non-Markovian character of the oscillator-environment interaction at any temperature as well the non-Markovian character of the blackbody radiation and its zero-point fluctuations. Expressions for the time evolution of the covariance matrix elements of the quantum fluctuations and the reduced density-operator are obtained.

Open system perspective on incoherent excitation of light-harvesting systems

The nature of excited states of open quantum systems produced by incoherent natural thermal light is analyzed based on a description of the quantum dynamical map. Natural thermal light is shown to generate long-lasting coherent dynamics because of (i) the super-Ohmic character of the radiation, and (ii) the absence of pure dephasing dynamics. In the presence of an environment, the long-lasting coherences induced by suddenly turned-on incoherent light dissipate and stationary coherences are established. As a particular application, dynamics in a subunit of the PC645 light-harvesting complex is considered where it is further shown that aspects of the energy pathways landscape depend on the nature of the exciting light and number of chromophores excited. Specifically, pulsed laser and natural broadband incoherent excitation induce significantly different energy transfer pathways. In addition, we discuss differences in perspective associated with the eigenstate versus site basis, and note an important difference in the phase of system coherences when coupled to blackbody radiation or when coupled to a phonon background. Finally, an appendix contains an open systems example of the loss of coherence as the turn-on time of the light assumes natural time scales.