Recently, we have theoretically proposed and experimentally demonstrated an exact and efficient quantum simulation of photosynthetic light harvesting in nuclear magnetic resonance (NMR), cf. B. X. Wang, textit{et al.} npj Quantum Inf.~textbf{4}, 52 (
2018). In this paper, we apply this approach to simulate the open quantum dynamics in various photosynthetic systems with different Hamiltonians. By numerical simulations, we show that for Drude-Lorentz spectral density the dimerized geometries with strong couplings within the donor and acceptor clusters respectively exhibit significantly-improved efficiency. Based on the optimal geometry, we also demonstrate that the overall energy transfer can be further optimized when the energy gap between the donor and acceptor clusters matches the peak of the spectral density. Moreover, by exploring the quantum dynamics for different types of spectral densities, e.g. Ohmic, sub-Ohmic, and super-Ohmic spectral densities, we show that our approach can be generalized to effectively simulate open quantum dynamics for various Hamiltonians and spectral densities. Because $log_{2}N$ qubits are required for quantum simulation of an $N$-dimensional quantum system, this quantum simulation approach can greatly reduce the computational complexity compared with popular numerically-exact methods.
There is a remarkable characteristic of photosynthesis in nature, that is, the energy transfer efficiency is close to 100%. Recently, due to the rapid progress made in the experimental techniques, quantum coherent effects have been experimentally dem
onstrated. Traditionally, the incoherent theories are capable of calculating the energy transfer efficiency, e.g., (generalized) Forster theory and modified Redfield theory. However, in order to describe the quantum coherent effects in photosynthesis, the coherent theories have been developed, such as hierarchical equation of motion, quantum path integral, coherent modified Redfield theory, small-polaron quantum master equation, and general Bloch-Redfield theory in addition to the Redfield theory. Here, we summarize the main points of the above approaches, which might be beneficial to the quantum simulation of quantum dynamics of exciton energy transfer in natural photosynthesis, and shed light on the design of artificial light-harvesting devices.
We propose a scheme to simulate the exciton energy transfer (EET) of photosynthetic complexes in a quantum superconducting circuit system. Our system is composed of two pairs of superconducting charge qubits coupled to two separated high-Q supercondu
cting transmission line resonators (TLRs) connected by a capacitance. When the frequencies of the qubits are largely detuned with those of the TLRs, we simulate the process of the EET from the first qubit to the fourth qubit. By tuning the couplings between the qubits and the TLRs, and the coupling between the two TLRs, we can modify the effective coupling strengths between the qubits and thus demonstrate the geometric effects on the EET. It is shown that a moderate clustered geometry supports optimal EET by using exciton delocalization and energy matching condition. And the population loss during the EET has been trapped in the two TLRs.
We theoretically study the longitudinal relaxation of a nitrogen-vacancy (NV) center surrounded by a 13C nuclear spin bath in diamond. By incorporating electron spin in the cluster, we generalize the cluster-correlation expansion (CCE) to theoretical
ly simulate the population dynamics of electron spin of NV center. By means of the generalized CCE, we numerically demonstrate the decay process of electronic state induced by cross relaxation at the ambient temperature. It is shown that the CCE method is not only capable of describing pure-dephasing effect at large-detuning regime, but it can also simulate the quantum dynamics of populations in the nearly-resonant regime.
Near-unity energy transfer efficiency has been widely observed in natural photosynthetic complexes. This phenomenon has attracted broad interest from different fields, such as physics, biology, chemistry and material science, as it may offer valuable
insights into efficient solar-energy harvesting. Recently, quantum coherent effects have been discovered in photosynthetic light harvesting, and their potential role on energy transfer has seen heated debate. Here, we perform an experimental quantum simulation of photosynthetic energy transfer using nuclear magnetic resonance (NMR). We show that an N- chromophore photosynthetic complex, with arbitrary structure and bath spectral density, can be effectively simulated by a system with log2 N qubits. The computational cost of simulating such a system with a theoretical tool, like the hierarchical equation of motion, which is exponential in N, can be potentially reduced to requiring a just polynomial number of qubits N using NMR quantum simulation. The benefits of performing such quantum simulation in NMR are even greater when the spectral density is complex, as in natural photosynthetic complexes. These findings may shed light on quantum coherence in energy transfer and help to provide design principles for efficient artificial light harvesting.
We theoretically study artificial light harvesting by a dimerized Mobius ring. When the donors in the ring are dimerized, the energies of the donor ring are splitted into two sub-bands. Because of the nontrivial Mobius boundary condition, both the ph
oton and acceptor are coupled to all collectiveexcitation modes in the donor ring. Therefore, the quantum dynamics in the light harvesting are subtly influenced by the dimerization in the Mobius ring. It is discovered that energy transfer is more efficient in a dimerized ring than that in an equally-spaced ring. This discovery is also confirmed by the calculation with the perturbation theory, which is equivalent to the Wigner-Weisskopf approximation. Our findings may be benificial to the optimal design of artificial light harvesting.
The structure of Fenna-Matthews-Olson (FMO) light-harvesting complex has long been recognized as containing seven bacteriochlorophyll (BChl) molecules. Recently, an additional BChl molecule was discovered in the crystal structure of the FMO complex,
which may serve as a link between baseplate and the remaining seven molecules. Here, we investigate excitation energy transfer (EET) process by simulating single-molecule pump-dump experiment in the eight-molecules complex. We adopt the coherent modified Redfield theory and non-Markovian quantum jump method to simulate EET dynamics. This scheme provides a practical approach of detecting the realistic EET pathway in BChl complexes with currently available experimental technology. And it may assist optimizing design of artificial light-harvesting devices.
