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Register a new userAn Efficient Quantum Jump Method for Coherent Energy Transfer Dynamics in Photosynthetic Systems under the Influence of Laser Fields
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We present a non-Markovian quantum jump approach for simulating coherent energy transfer dynamics in molecular systems in the presence of laser fields. By combining a coherent modified Redfield theory (CMRT) and a non-Markovian quantum jump (NMQJ) method, this new approach inherits the broad-range validity from the CMRT and highly efficient propagation from the NMQJ. To implement NMQJ propagation of CMRT, we show that the CMRT master equation can be casted into a generalized Lindblad form. Moreover, we extend the NMQJ approach to treat time-dependent Hamiltonian, enabling the description of excitonic systems under coherent laser fields. As a benchmark of the validity of this new method, we show that the CMRT-NMQJ method accurately describes the energy transfer dynamics in a prototypical photosynthetic complex. Finally, we apply this new approach to simulate the quantum dynamics of a dimer system coherently excited to coupled single-excitation states under the influence of laser fields, which allows us to investigate the interplay between the photoexcitation process and ultrafast energy transfer dynamics in the system. We demonstrate that laser-field parameters significantly affect coherence dynamics of photoexcitations in excitonic systems, which indicates that the photoexcitation process must be explicitly considered in order to properly describe photon-induced dynamics in photosynthetic systems. This work should provide a valuable tool for efficient simulations of coherent control of energy flow in photosynthetic systems and artificial optoelectronic materials.
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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 demonstrated. 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.
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 characterize the coherent dynamics of a two-level quantum emitter driven by a pair of symmetrically-detuned phase-locked pulses. The promise of dichromatic excitation is to spectrally isolate the excitation laser from the quantum emission, enabling background-free photon extraction from the emitter. Paradoxically, we find that excitation is not possible without spectral overlap between the exciting pulse and the quantum emitter transition for ideal two-level systems due to cancellation of the accumulated pulse area. However, any additional interactions that interfere with cancellation of the accumulated pulse area may lead to a finite stationary population inversion. Our spectroscopic results of a solid-state two-level system show that while coupling to lattice vibrations helps to improve the inversion efficiency up to 50% under symmetric driving, coherent population control and a larger amount of inversion are possible using asymmetric dichromatic excitation, which we achieve by adjusting the ratio of the intensities between the red and blue-detuned pulses. Our measured results, supported by simulations using a real-time path-integral method, offer a new perspective towards realising efficient, background-free photon generation and extraction.
Energy transfer within photosynthetic systems can display quantum effects such as delocalized excitonic transport. Recently, direct evidence of long-lived coherence has been experimentally demonstrated for the dynamics of the Fenna-Matthews-Olson (FMO) protein complex [Engel et al., Nature 446, 782 (2007)]. However, the relevance of quantum dynamical processes to the exciton transfer efficiency is to a large extent unknown. Here, we develop a theoretical framework for studying the role of quantum interference effects in energy transfer dynamics of molecular arrays interacting with a thermal bath within the Lindblad formalism. To this end, we generalize continuous-time quantum walks to non-unitary and temperature-dependent dynamics in Liouville space derived from a microscopic Hamiltonian. Different physical effects of coherence and decoherence processes are explored via a universal measure for the energy transfer efficiency and its susceptibility. In particular, we demonstrate that for the FMO complex an effective interplay between free Hamiltonian and thermal fluctuations in the environment leads to a substantial increase in energy transfer efficiency from about 70% to 99%.
Models based on non-Hermitian Hamiltonians can exhibit a range of surprising and potentially useful phenomena. Physical realizations typically involve couplings to sources of incoherent gain and loss; this is problematic in quantum settings, because of the unavoidable fluctuations associated with this dissipation. Here, we present several routes for obtaining unconditional non-Hermitian dynamics in non-dissipative quantum systems. We exploit the fact that quadratic bosonic Hamiltonians that do not conserve particle number give rise to non-Hermitian dynamical matrices. We discuss the nature of these mappings from non-Hermitian to Hermitian Hamiltonians, and explore applications to quantum sensing, entanglement dynamics and topological band theory. The systems we discuss could be realized in a variety of photonic and phononic platforms using the ubiquitous resource of parametric driving.
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