An efficient approach to the quantum dynamics and rates of processes induced by natural incoherent light

Abstract

In many important cases, the rate of excitation of a system embedded in an environment is significantly smaller than the internal system relaxation rates. An important example is that of light-induced processes under natural conditions, in which the system is excited by weak, incoherent (e.g., solar) radiation. Simulating the dynamics on the time scale of the excitation source can thus be computationally intractable. Here we describe a method for obtaining the dynamics of quantum systems without directly solving the master equation. We present an algorithm for the numerical implementation of this method, and, as an example, use it to reconstruct the internal conversion dynamics of pyrazine excited by sunlight. Significantly, this approach also allows us to assess the role of quantum coherence on biological time scales, which is a topic of ongoing interest.

References in corpus (15)

• Long-lived quantum coherence in photosynthetic complexes at physiological temperature
• Noise-induced dynamics in bistable systems with delay
• Multiple steady-states in nonequilibrium quantum systems with electron-phonon interactions
• Nonequilibrium quantum systems with electron-phonon interactions: Transient dynamics and approach to steady state
• Long-lived quasi-stationary coherences in V-type system driven by incoherent light
• Generalized Gibbs state with modified Redfield solution: Exact agreement up to second order
• Reduced density matrix for nonequilibrium steady states: A modified Redfield solution approach
• Modified Bloch-Redfield Master Equation for Incoherent Excitation of Multilevel Quantum Systems
• Secular vs. Non-secular Redfield Dynamics and Fano Coherences in Incoherent Excitation: An Experimental Proposal
• Quantum dynamics of incoherently driven V-type system: Analytic solutions beyond the secular approximation
• Excitation energy transfer efficiency: equivalence of transient and stationary setting and the absence of non-Markovian effects
• Coherent dynamics of V-type systems driven by time-dependent incoherent radiation
• Iterative solutions to the steady state density matrix for optomechanical systems
• A perturbative method for nonequilibrium steady state of open quantum systems
• Steady-state solution methods for open quantum optical systems

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• Generalized Adiabatic Theorems: Quantum Systems Driven by Modulated Time-Varying Fields
• Nonequilibrium steady-state picture of incoherent light-induced excitation harvesting
• Photochemical dynamics under incoherent illumination: light harvesting in self-assembled molecular J-aggregates
• From Goldilocks to Twin Peaks: multiple optimal regimes for quantum transport in disordered networks
• Localisation determines the optimal noise rate for quantum transport
• An efficient spectral method for numerical time-dependent perturbation theory
• Fully differentiable optimization protocols for non-equilibrium steady states