Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userEnhanced light-harvesting of protein-pigment complexes assisted by a quantum dot antenna
116
0
0.0
(
0
)
Added by
Gabriel Jos\\'e Gil P\\'erez
Publication date
2020
fields
Physics
and research's language is
English
Ask ChatGPT about the research
No Arabic abstract
We predict the enhanced light harvesting of a protein-pigment complex when assembled to a quantum dot (QD) antenna. Our prototypical nanoassembly setup is composed of a Fenna-Mattews-Olson system hosting 8 Bacteriochlorophyll (BChl) a dyes, and a near-infrared emitting CdSe$_x$Te$_{(1-x)}$/ZnS alloy-core/shell nanocrystal. BChl a has two wide windows of poor absorption in the green and orange-red bands, precisely where most of the sunlight energy lies. The selected QD is able to collect sunlight efficiently in a broader band and funnel its energy by a (non-radiative) Forster resonance energy transfer mechanism to the dyes embedded in the protein. By virtue of the coupling between the QD and the dyes, the nanoassembly absorption is dramatically improved in the poor absorption window of the BChl a.
rate research
Read More
We provide a unified theoretical approach to the quantum dynamics of absorption of single photons and subsequent excitonic energy transfer in photosynthetic light-harvesting complexes. Our analysis combines a continuous mode <n>-photon quantum optical master equation for the chromophoric system with the hierarchy of equations of motion describing excitonic dynamics in presence of non-Markovian coupling to vibrations of the chromophores and surrounding protein. We apply the approach to simulation of absorption of single-photon coherent states by pigment-protein complexes containing between one and seven chromophores, and compare with results obtained by excitation using a thermal radiation field. We show that the values of excitation probability obtained under single-photon absorption conditions can be consistently related to bulk absorption cross-sections. Analysis of the timescale and efficiency of single-photon absorption by light-harvesting systems within this full quantum description of pigment-protein dynamics coupled to a quantum radiation field reveals a non-trivial dependence of the excitation probability and the excited state dynamics induced by exciton-phonon coupling during and subsequent to the pulse, on the bandwidth of the incident photon pulse. For bandwidths equal to the spectral bandwidth of Chlorophyll a, our results yield an estimation of an average time of ~0.09 s for a single chlorophyll chromophore to absorb the energy equivalent of one (single-polarization) photon under irradiation by single-photon states at the intensity of sunlight.
The primary steps of photosynthesis generate, transport and trap delocalised electronic excitations (excitons) in pigment-protein complexes (PPCs). Generically, PPCs possess highly structured vibrational spectra with a large number of discrete intra- and quasi-continuous inter-pigment modes while exhibiting electron-vibrational (vibronic) couplings that are comparable to electronic inter-pigment coupling. Consequently, establishing a quantitative connection between spectroscopic data and underlying microscopic models of PPC dynamics remains an outstanding challenge. We address this challenge with two numerically exact simulation methods that support an analytical theory of multimode vibronic effects. Vibronic coupling across the entire vibrational spectrum, including high-frequency modes, needs to be accounted for to ensure quantitatively correct description of optical spectra, where dynamic localization effects modulate the intensity of vibrational sidebands and multimode mixing shifts the absorption peaks. Furthermore, we show that high-frequency modes can support long-lived oscillations in multidimensional nonlinear spectra, which are not obtained in a coarse-grained description of the electron-vibrational coupling.
Light harvesting components of photosynthetic organisms are complex, coupled, many-body quantum systems, in which electronic coherence has recently been shown to survive for relatively long time scales despite the decohering effects of their environments. Within this context, we analyze entanglement in multi-chromophoric light harvesting complexes, and establish methods for quantification of entanglement by presenting necessary and sufficient conditions for entanglement and by deriving a measure of global entanglement. These methods are then applied to the Fenna-Matthews-Olson (FMO) protein to extract the initial state and temperature dependencies of entanglement. We show that while FMO in natural conditions largely contains bipartite entanglement between dimerized chromophores, a small amount of long-range and multipartite entanglement exists even at physiological temperatures. This constitutes the first rigorous quantification of entanglement in a biological system. Finally, we discuss the practical utilization of entanglement in densely packed molecular aggregates such as light harvesting complexes.
Disordered quantum networks, as those describing light-harvesting complexes, are often characterized by the presence of antenna structures where the light is captured and inner structures (reaction centers) where the excitation is transferred. Antennae often display distinguished coherent features: their eigenstates can be separated, with respect to the transfer of excitation, in the two classes of superradiant and subradiant states. Both are important to optimize transfer efficiency. In absence of disorder superradiant states have an enhanced coupling strength to the RC, while subradiant ones are basically decoupled from it. Disorder induces a coupling between subradiant and superradiant states, thus creating an indirect coupling to the RC. We consider the problem of finding the maximal excitation transfer efficiency as a function of the RC energy and the disorder strength, first in a paradigmatic three-level system and then in a realistic model for the light-harvesting complex of purple bacteria. Specifically, we focus on the case in which the excitation is initially on a subradiant state, showing that the optimal disorder is of the order of the superradiant coupling. We also determine the optimal detuning between the initial state and the RC energy. We show that the efficiency remains high around the optimal detuning in a large energy window, proportional to the superradiant coupling. This allows for the simultaneous optimization of excitation transfer from several initial states with different optimal detuning.
The electronic excitation population and coherence dynamics in the chromophores of the photosynthetic light harvesting complex 2 (LH2) B850 ring from purple bacteria (Rhodopseudomonas acidophila) have been studied theoretically at both physiological and cryogenic temperatures. Similar to the well-studied Fenna-Matthews-Olson (FMO) protein, oscillations of the excitation population and coherence in the site basis are observed in LH2 by using a scaled hierarchical equation of motion (HEOM) approach. However, this oscillation time (300 fs) is much shorter compared to the FMO protein (650 fs) at cryogenic temperature. Both environment and high temperature are found to enhance the propagation speed of the exciton wave packet yet they shorten the coherence time and suppress the oscillation amplitude of coherence and the population. Our calculations show that a long-lived coherence between chromophore electronic excited states can exist in such a noisy biological environment.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
