In this thesis we study the coherent energy transfer in photosynthetic systems. This resonant energy transfer has proven to be a coherent transfer in some light harvest complexes. The model which we suggest to describe this mechanism is an exciton hopping on an N-site ring coupled to a spin bath. Analytic results are found for both the dynamics of the influence functional and of the reduced density matrix of the excitons.We also give results for the dynamics of the current as a function of time. By setting states splitting initially into 2 separate wave-packets moving at different velocities, we reproduce the coherent beating phenomenon in experiments.
In this thesis we study the coherent energy transfer in photosynthetic systems. This resonant energy transfer has proven to be a coherent transfer in some light harvest complexes. The model which we suggest to describe this mechanism is an exciton hopping on an N-site ring coupled to a spin bath. Analytic results are found for both the dynamics of the influence functional and of the reduced density matrix of the excitons.We also give results for the dynamics of the current as a function of time. By setting states splitting initially into 2 separate wave-packets moving at different velocities, we reproduce the coherent beating phenomenon in experiments.
Ultrafast spectroscopy experiments show that photosynthetic systems can preserve quantum beats in the process of electronic energy transfer between pigments, even at room temperature. But what does this discovery imply for biology - and for quantum mechanics? This dissertation examines photosynthesis through the tools of quantum information science. We evaluate to what extent photosynthesis can be thought of as a type of quantum technology, and consider how we can apply experimental tools widely used for quantum technologies (state tomography and coherent control) to photosynthesis. Throughout, we use the Fenna-Matthews-Olson (FMO) complex of greens sulfur bacteria as a model photosynthetic pigment-protein complex.In Part I, we evaluate two mechanisms for the possible biological relevance of quantum coherent motion. First, we consider the extent to which dynamics in light-harvesting systems exhibit the quantum speedups characteristic of quantum algorithms and quantum walks. Second, we demonstrate a ratchet effect in electronic energy transfer enabled by partially coherent dynamics. To do so, we build a new model of energy transfer between weakly coupled light-harvesting complexes to understand how electronic coherence arises under natural conditions.In Part II, we present proposals for experimental probes of light harvesting dynamics with ultrafast spectroscopy. We show how the signal from pump-probe spectroscopy can be formally inverted to determine the excited state electronic density matrix. Finally, we examine the feasiblity of coherent control experiments on light-harvesting systems, and provide two realistic targets feasible with present-day technology.
In natural photosynthesis systems, pigment-protein complexes harvest the photon from sunlight with near-unity quantum efficiency. These complexes show incredible properties that cannot be merely extrapolated from knowledge of their composition. Additionally, the environment perturbing the light-harvesting process significantly affects the mechanism of photosynthesis. This research investigates the photosystem II reaction center (PSII RC) from a new perspective which considers the restricted path of the exciton transfer, in the photosynthesis system, as a quantum trajectory picture with the quantum continuous measurement. In this work, the corridor path of exciton transfer dynamics satisfies the equation of motion, as the spin dynamics, which consists of precession, relaxation, and random force rapidly fluctuating spin splitting arising from the bath. Moreover, the width of the corridor is an important factor for restricting path dynamics resulting in the localization and decoherence phenomenon. Our method is to analyze exciton transfer dynamics through paths on the Bloch sphere, in order to investigate the propagating states in accordance with the weight functional which depends on the coupling parameter between the system and environment as the phonon bath. Our results show that the paths outside the width of the corridor have a considerably lower weight functional and decoherence functional than those inside the width. Therefore, the degrees of localization, the weight functional, and the decoherence functional are related. Furthermore, the simulation reveals three characteristics of exciton transfer: gradual transfer, no transfer, and rapid transfer, relying significantly on the coupling between the system and phonons.
Abstract 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 the 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 log2N 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.
A variety of open quantum networks are currently under intense examination to model energy transport in photosynthetic systems. Here, we study the coherent transfer of a quantum excitation over a network incoherently coupled with a structured and small environment that effectively models the photosynthetic reaction center. Our goal is to distill a few basic, possibly universal, mechanisms or effects that are featured in simple energy-transfer models. In particular, we identify three different phenomena: the congestion effect, the asymptotic unitarity, and the staircase effects. We begin with few-site models, in which these effects can be fully understood, and then proceed to study more complex networks similar to those employed to model energy transfer in light-harvesting complexes.
Many biological phenomena including avian navigation and photosynthesis manifest quantum coherent effects. In avian navigation, the weak geomagnetic field and spin-dependent chemical reactions are utilized for navigation. As one of the most important energy sources on earth, photosynthesis has always been a point of discussion for scientists. The study of energy transmission in photosynthetic systems can support the design or performance optimization of artificial light-harvesting devices. Currently, the quantum coherent effect has been observed in photosynthetic complexes, and the quantum efficiency of energy transmission in photosynthetic complexes is close to 100%. These important findings prompted many experts in different disciplines to use quantum physical methods to explore the physical mechanism behind the energy transmission in photosynthetic systems and the role of the quantum coherent effect in the exciton energy transmission in photosynthetic complexes. It has been proven that energy transfer in pigment-protein complexes is mainly in the form of coherent energy transfer. Moreover, the importance of the quantum coherent effect in energy transmission has been proven. Furthermore, several researchers have used the quantum coherent effect to improve energy transmission in photosynthetic systems and achieved some progress. For open quantum systems, such as photosynthetic systems, many theoretical methods have been proposed to analyze their quantum dynamics. These theoretical methods can be divided into two categories according to whether they can describe the diagonal term of the system density matrix, namely, coherent and incoherent theories. Moreover, the application conditions of these theoretical methods differ according to their established processes. Recently, with the progress in research, several groups have proposed several quantum simulation methods based on different quantum computing systems, including quantum simulation methods based on nuclear magnetic resonance systems, superconducting quantum circuit systems, and ion trap systems, to analyze the phenomena in photosynthetic systems. Compared with the traditional theoretical calculation methods, these quantum simulation methods have higher computational efficiency and lower computational complexity. This paper mainly reviews the progress in research on quantum coherent effects in photosynthesis and the related theoretical calculation and quantum simulation methods.
Assessing the role of interference in natural and artificial quantum dynamical processes is a crucial task in quantum information theory. To this aim, an appropriate formalism is provided by the decoherent histories framework. While this approach has been deeply explored from different theoretical perspectives, it still lacks of a comprehensive set of tools able to concisely quantify the amount of coherence developed by a given dynamics. In this paper, we introduce and test different measures of the (average) coherence present in dissipative (Markovian) quantum evolutions, at various time scales and for different levels of environmentally induced decoherence. In order to show the effectiveness of the introduced tools, we apply them to a paradigmatic quantum process where the role of coherence is being hotly debated: exciton transport in photosynthetic complexes. To spot out the essential features that may determine the performance of the transport, we focus on a relevant trimeric subunit of the Fenna-Matthews-Olson complex and we use a simplified (Haken-Strobl) model for the system-bath interaction. Our analysis illustrates how the high efficiency of environmentally assisted transport can be traced back to a quantum recoil avoiding effect on the exciton dynamics, that preserves and sustains the benefits of the initial fast quantum delocalization of the exciton over the network. Indeed, for intermediate levels of decoherence, the bath is seen to selectively kill the negative interference between different exciton pathways, while retaining the initial positive one. The concepts and tools here developed show how the decoherent histories approach can be used to quantify the relation between coherence and efficiency in quantum dynamical processes.