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.
54 pages, 17 figures; revised abstract, added acknowledgements
References in corpus (6)
- 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
- Dynamics of quantum dissipation systems interacting with Fermion and Boson grand canonical bath ensembles: Hierarchical equations of motion approach
- Effects of Herzberg--Teller vibronic coupling on coherent excitation energy transfer
- Continuous Measurement and Stochastic Methods in Quantum Optical Systems
Cited by in corpus (9)
- Fundamental limits of pulsed quantum light spectroscopy: Dipole moment estimation
- Coupled charge and energy transfer dynamics in light harvesting complexes from a hybrid hierarchical equations of motion approach
- Does entanglement enhance single-molecule pulsed biphoton spectroscopy?
- Performing quantum entangled biphoton spectroscopy using classical light pulses
- On the role of chirping in pulsed single photon spectroscopy
- Quantum simulation of weak-field light-matter interactions
- Energetics of self-organization in a dissipative two-site quantum system driven by single-photon pulses
- Non-Gaussian Phase Transition and Cascade of Instabilities in the Dissipative Quantum Rabi Model
- Optimal quantum spectroscopy using single-photon pulses