Dynamics of photosynthetic light harvesting systems interacting with N-photon Fock states
arXiv:2111.06996 · doi:10.1063/5.0082822
Abstract
We develop a method to simulate the excitonic dynamics of realistic photosynthetic light harvesting systems including non-Markovian coupling to phonon degrees of freedom, under excitation by N-photon Fock state pulses. This method combines the input-output formalism and the hierarchical equations of motion (HEOM) formalism into a double hierarchy of coupled linear equations in density matrices. We show analytically that, under weak field excitation relevant to natural photosynthesis conditions, an N-photon Fock state input and a corresponding coherent state input give rise to equal density matrices in the excited manifold. However, an important difference is that an N-photon Fock state input has no off-diagonal coherence between the ground and excited subspaces, in contrast with the coherences created by a coherent state input. We derive expressions for the probability to absorb a single Fock state photon, with or without the influence of phonons. For short pulses (or equivalently, wide bandwidth pulses), we show that the absorption probability has a universal behavior that depends only upon a system-dependent effective energy spread parameter Δ and an exciton-light coupling constant Γ. This holds for a broad range of chromophore systems and for a variety of pulse shapes. We also analyse the absorption probability in the opposite long pulses (narrow bandwidth) regime. We also derive an expression for the long time emission rate in the presence of phonons and use it to study the difference between collective versus independent emission. Finally, we present a numerical simulation for the LHCII monomer (14-mer) system under single photon excitation that illustrates the use of the double hierarchy for calculation of Fock state excitation of a light harvesting system including chromophore coupling to a non-Markovian phonon bath.
arXiv comment54 pages, 17 figures; revised abstract, added acknowledgements
References in corpus (19)
- Heralded Generation of Ultrafast Single Photons in Pure Quantum States
- Perspective: Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM)
- High-performance solution of hierarchical equations of motions for studying energy-transfer in light-harvesting complexes
- N-Photon wave packets interacting with an arbitrary quantum system
- The SLH framework for modeling quantum input-output networks
- Molecular Response in One-Photon Absorption via Natural Thermal Light vs Pulsed Laser Excitation
- Efficient excitation of a two level atom by a single photon in a propagating mode
- Exciton Dynamics in Photosynthetic Complexes: Excitation by Coherent and Incoherent Light
- Dynamics of quantum dissipation systems interacting with Fermion and Boson grand canonical bath ensembles: Hierarchical equations of motion approach
- Reduced density matrix hybrid approach: Application to electronic energy transfer
- Effects of Herzberg--Teller vibronic coupling on coherent excitation energy transfer
- Single-photon absorption by single photosynthetic light-harvesting complexes
- Long-range coherent energy transport in Photosystem II
- Quantum Stratonovich Stochastic Calculus and the Quantum Wong-Zakai Theorem
- Nonequilibrium open quantum systems with multiple bosonic and fermionic environments: A hierarchical equations of motion approach
- Three-dimensional light-matter interface for collective spin squeezing in atomic ensembles
- Open System Perspective on Incoherent Excitation of Light Harvesting Systems
- Note: Vibronic coupling in light-harvesting complex II revisited
- Continuous Measurement and Stochastic Methods in Quantum Optical Systems
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