Non-perturbative System-bath Interactions Research Articles

Optimizing co-operative multi-environment dynamics in a dark-state-enhanced photosynthetic heat engine.

We analyze the role of coherent, non-perturbative system-bath interactions in a photosynthetic heat engine. Using the reaction-coordinate formalism to describe the vibrational phonon-environment in the engine, we analyze the efficiency around an optimal parameter regime predicted in earlier studies. We show that, in the limit of high-temperature photon irradiation, the phonon-assisted population transfer between bright and dark states is suppressed due to dephasing from the photon environment, even in the Markov limit where we expect the influence of each bath to have an independent and additive effect on the dynamics. Manipulating the phonon bath properties via its spectral density enables us to identify both optimal low- and high-frequency regimes where the suppression can be removed. This suppression of transfer and its removal suggests that it is important to consider carefully the non-perturbative and cooperative effects of system-bath environments in designing artificial photosynthetic systems and also that manipulating inter-environmental interactions could provide a new multidimensional "lever" by which photocells and other types of quantum devices can be optimized.

Quantum heat transport of a two-qubit system: Interplay between system-bath coherence and qubit-qubit coherence.

We consider a system consisting of two interacting qubits that are individually coupled to separate heat baths at different temperatures. The quantum effects in heat transport are investigated in a numerically rigorous manner with a hierarchial equations of motion (HEOM) approach for non-perturbative and non-Markovian system-bath coupling cases under non-equilibrium steady-state conditions. For a weak interqubit interaction, the total system is regarded as two individually thermostatted systems, whereas for a strong interqubit interaction, the two-qubit system is regarded as a single system coupled to two baths. The roles of quantum coherence (or entanglement) between the two qubits (q-q coherence) and between the qubit and bath (q-b coherence) are studied through the heat current calculated for various strengths of the system-bath coupling and interqubit coupling for high and low temperatures. The same current is also studied using the time convolutionless (TCL) Redfield equation and using an expression derived from the Fermi golden rule (FGR). We find that the HEOM results exhibit turnover behavior of the heat current as a function of the system-bath coupling strength for all values of the interqubit coupling strength, while the results obtained with the TCL and FGR approaches do not exhibit such behavior, because they do not possess the capability of treating the q-b and q-q coherences. The maximum current is obtained in the case that the q-q coherence and q-b coherence are balanced in such a manner that coherence of the entire heat transport process is realized. We also find that the heat current does not follow Fourier's law when the temperature difference is very large, due to the non-perturbative system-bath interactions.

Real-time and imaginary-time quantum hierarchal Fokker-Planck equations.

We consider a quantum mechanical system represented in phase space (referred to hereafter as "Wigner space"), coupled to a harmonic oscillator bath. We derive quantum hierarchal Fokker-Planck (QHFP) equations not only in real time but also in imaginary time, which represents an inverse temperature. This is an extension of a previous work, in which we studied a spin-boson system, to a Brownian system. It is shown that the QHFP in real time obtained from a correlated thermal equilibrium state of the total system possesses the same form as those obtained from a factorized initial state. A modified terminator for the hierarchal equations of motion is introduced to treat the non-Markovian case more efficiently. Using the imaginary-time QHFP, numerous thermodynamic quantities, including the free energy, entropy, internal energy, heat capacity, and susceptibility, can be evaluated for any potential. These equations allow us to treat non-Markovian, non-perturbative system-bath interactions at finite temperature. Through numerical integration of the real-time QHFP for a harmonic system, we obtain the equilibrium distributions, the auto-correlation function, and the first- and second-order response functions. These results are compared with analytically exact results for the same quantities. This provides a critical test of the formalism for a non-factorized thermal state and elucidates the roles of fluctuation, dissipation, non-Markovian effects, and system-bath coherence. Employing numerical solutions of the imaginary-time QHFP, we demonstrate the capability of this method to obtain thermodynamic quantities for any potential surface. It is shown that both types of QHFP equations can produce numerical results of any desired accuracy. The FORTRAN source codes that we developed, which allow for the treatment of Wigner space dynamics with any potential form (TanimuranFP15 and ImTanimuranFP15), are provided as the supplementary material.

Diagram Technique for Nonlinear Optical Spectroscopy in the Fast Electronic Dephasing Limit

AbstractWe show that applying the double‐sided Feynman diagrams to systems with fast electronic dephasing opens up new possibilities for using this technique in resonance nonlinear optical spectroscopy. The novel potentials are including non‐perturbative system‐bath interactions (non‐Markovian relaxation) and the summation of diagrams. The last procedure enables us to obtain new equations for a nonperturbative description of the light‐matter interaction.