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Quantum Jump Approach for Photosynthetic Energy Transfer with Chemical Reaction and Fluorescence Loss

Rui Li, Yi Li, Kai-Ya Zhang, Qing Ai

TL;DR

The paper addresses the computational challenge of simulating excitation-energy transfer in large photosynthetic complexes by integrating a quantum-jump approach with coherent modified Redfield theory (QJA-CMRT) to include chemical reactions and fluorescence loss. It maps the CMRT master equation onto stochastic trajectories, preserving accuracy while dramatically reducing resource requirements, with CR/FL treated via Lindblad-like terms and positive/negative channel dynamics capturing memory effects. Demonstrations on a dimer show exact agreement with CMRT-based simulations and reveal physical trends where the EET efficiency increases with electronic coupling $J$ and decreases with fluorescence loss rate; the method also exhibits significantly improved scaling with system size, approximately $N^{2.0}$ versus higher powers for conventional approaches. Overall, QJA-CMRT enables accurate, scalable modeling of energy transfer in large-scale photosynthetic systems (PSI/PSII) and supports the design of artificial photosynthetic devices by providing a practical, efficient computational framework.

Abstract

Recently, the coherent modified Redfield theory (CMRT) has been widely used to simulate the excitation-energy-transfer (EET) processes in photosynthetic systems. However, the numerical simulation of the CMRT is computationally expensive when dealing with large-scale systems, e.g. photosystem I (PSI) and II (PSII). On the other hand, the chemical reaction and fluorescence loss traditionally treated by the non-Hermitian Hamiltonian approach may result in significantly error in a wide range of parameters. To address these issues, we introduce a quantum jump approach (QJA) based on the CMRT to simulate the evolution of photosynthetic complexes including both the chemical reaction and fluorescence loss. The QJA shows higher accuracy and efficiency in simulating the EET processes. The QJA-CMRT approach may provide a powerful tool to design and optimize artificial photosynthetic systems, which benefits future innovation in the field of energy.

Quantum Jump Approach for Photosynthetic Energy Transfer with Chemical Reaction and Fluorescence Loss

TL;DR

The paper addresses the computational challenge of simulating excitation-energy transfer in large photosynthetic complexes by integrating a quantum-jump approach with coherent modified Redfield theory (QJA-CMRT) to include chemical reactions and fluorescence loss. It maps the CMRT master equation onto stochastic trajectories, preserving accuracy while dramatically reducing resource requirements, with CR/FL treated via Lindblad-like terms and positive/negative channel dynamics capturing memory effects. Demonstrations on a dimer show exact agreement with CMRT-based simulations and reveal physical trends where the EET efficiency increases with electronic coupling and decreases with fluorescence loss rate; the method also exhibits significantly improved scaling with system size, approximately versus higher powers for conventional approaches. Overall, QJA-CMRT enables accurate, scalable modeling of energy transfer in large-scale photosynthetic systems (PSI/PSII) and supports the design of artificial photosynthetic devices by providing a practical, efficient computational framework.

Abstract

Recently, the coherent modified Redfield theory (CMRT) has been widely used to simulate the excitation-energy-transfer (EET) processes in photosynthetic systems. However, the numerical simulation of the CMRT is computationally expensive when dealing with large-scale systems, e.g. photosystem I (PSI) and II (PSII). On the other hand, the chemical reaction and fluorescence loss traditionally treated by the non-Hermitian Hamiltonian approach may result in significantly error in a wide range of parameters. To address these issues, we introduce a quantum jump approach (QJA) based on the CMRT to simulate the evolution of photosynthetic complexes including both the chemical reaction and fluorescence loss. The QJA shows higher accuracy and efficiency in simulating the EET processes. The QJA-CMRT approach may provide a powerful tool to design and optimize artificial photosynthetic systems, which benefits future innovation in the field of energy.

Paper Structure

This paper contains 8 sections, 17 equations, 1 figure.

Table of Contents

  1. Introduction
  2. Model
  3. Master Equation Including Chemical Reaction and Fluorescence Loss
  4. Quantum Jump Approach
  5. Numerical Simulation and Discussion
  6. The Dimer Model
  7. The $N$-dependency of the computational time of QJA and QUTIP
  8. Conclusion

Figures (1)

  • Figure 1: (a) An energy diagram of the dimer system. The two single-excitation states are $\vert1\rangle$ and $\vert2\rangle$. The ground state and the product state of the CR are $\vert g\rangle$ and $\vert g^\prime\rangle$, respectively. (b) The population dynamics of the dimer system are respectively simulated by the QJA (solid line) and the QUTIP (dashed line). (c) The dependence of efficiency $\eta$ on the electronic coupling $J$ and the FL rate $\gamma$. The energy gap $\Delta$ and the CR rate are fixed at $763$ cm$^{-1}$ and $1.33$ cm$^{-1}$. (d) The scaling of the computational time $t$ against the number of sites $N$ by the two approaches.