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Recent ultrafast optical experiments show that excitons in large biological light-harvesting complexes are coupled to molecular vibration modes. These high-frequency vibrations will not only affect the optical response, but also drive the…

Quantum Physics · Physics 2015-02-12 Arend G. Dijkstra , Chen Wang , Jianshu Cao , Graham R. Fleming

Until recently it was believed that photosynthesis, a fundamental process for life on earth, could be fully understood with semi-classical models. However, puzzling quantum phenomena have been observed in several photosynthetic…

Experimental and theoretical evidence point out to the crucial role of specific resonant intramolecular vibrational modes in the interpretation of long-lived coherences observed in two-dimensional spectra of some natural and synthetic light…

Chemical Physics · Physics 2020-07-15 Leonardo F. Calderón , Leonardo A. Pachón

Natural and artificial light harvesting processes have recently gained new interest. Signatures of long lasting coherence in spectroscopic signals of biological systems have been repeatedly observed, albeit their origin is a matter of…

Spectroscopic experiments have identified long-lived coherences in several light-harvesting systems, suggesting that coherent effects may be relevant to their performance. However, there is limited experimental evidence of coherence…

Chemical Physics · Physics 2019-10-30 Stefano Tomasi , Sima Baghbanzadeh , Saleh Rahimi-Keshari , Ivan Kassal

We discuss our recent theoretical work on vibronic coupling mechanisms in a model energy transfer system in the context of previous 2DEV experiments on a natural light-harvesting system, light-harvesting complex II (LHCII), where vibronic…

Chemical Physics · Physics 2021-09-22 Eric A. Arsenault , Addison J. Schile , David T. Limmer , Graham R. Fleming

We investigated the exciton transfer dynamics in photosynthetic light-harvesting complex 2 (LH2) coupled to an optical microcavity. Using computational simulations based on Redfield theory, we analyzed how microcavity coupling influences…

Atomic and Molecular Clusters · Physics 2025-12-30 Ilmari Rosenkampff , Tõnu Pullerits

Exciton harvesting is demonstrated in an ensemble of quantum emitters coupled to localized surface plasmons. When the interaction between emitters and the dipole mode of a metallic nanosphere reaches the strong coupling regime, the exciton…

Mesoscale and Nanoscale Physics · Physics 2015-09-16 Carlos Gonzalez-Ballestero , Johannes Feist , Esteban Moreno , Francisco J. Garcia-Vidal

Starting from a microscopic model, we investigate the optical spectra of molecules in strongly-coupled organic microcavities examining how they might self-consistently adapt their coupling to light. We consider both rotational and…

Mesoscale and Nanoscale Physics · Physics 2016-03-25 Justyna A. Cwik , Peter Kirton , Simone De Liberato , Jonathan Keeling

We develop a method to simulate the excitonic dynamics of realistic photosynthetic light harvesting systems including non-Markovian coupling to phonon degrees of freedom, under excitation by N-photon Fock state pulses. This method combines…

Biological Physics · Physics 2023-06-27 Liwen Ko , Robert L. Cook , K. Birgitta Whaley

Light harvesting as the first step in photosynthesis is of prime importance for life on earth. For a theoretical description of photochemical processes during light harvesting, spectral densities are key quantities. They serve as input…

Chemical Physics · Physics 2021-08-25 Sayan Maity , Pooja Sarngadharan , Vangelis Daskalakis , Ulrich Kleinekathöfer

The light-harvesting efficiency of a photoactive molecular complex is largely determined by the properties of its electronic quantum states. Those, in turn, are influenced by molecular vibrational states of the nuclear degrees of freedom.…

Biological Physics · Physics 2019-10-23 Hong-Guang Duan , Michael Thorwart , R. J. Dwayne Miller

We consider bio-inspired ring systems as photovoltaic circuits to explore the advantage of `optical ratcheting', a process whereby the arrangement of coupled optical dipoles enables delocalised excitonic states that are protected against…

Mesoscale and Nanoscale Physics · Physics 2023-02-13 Nicholas Werren , William M. Brown , Erik M. Gauger

Light-harvesting and excitation energy transfer in photosynthesis generally involve chlorophyll-molecules, maintained by their host proteins at short distances from each other, this resulting in excitonic coupling. The transfer of…

Unravelling the nature of energy transport in multi-chromophoric photosynthetic complexes is essential to extract valuable design blueprints for light-harvesting applications. Long-range exciton transport in such systems is facilitated by a…

Usually the study of energy-transfer in the light harvesting complex is limited by a single-exciton motion along the antenna. Starting from the many-body Schr\"odinger equation, we derived Lindblad-type Master equations describing the…

Chemical Physics · Physics 2017-06-13 Shmuel Gurvitz , Gennady P. Berman , Richard T. Sayre

A vibronic exciton model is developed to investigate the origin of long lived coherences in light-harvesting complexes. Using experimentally determined parameters and uncorrelated site energy fluctuations, the model predicts oscillations in…

Biological Physics · Physics 2012-06-07 Niklas Christensson , Harald F. Kauffmann , Tonu Pullerits , Tomas Mancal

Research into the efficiency of photosynthetic light harvesting has focused on two factors: (1) entanglement of chromophores, and (2) environmental noise. While chromophores are conjugated $\pi$-bonding molecules with strongly correlated…

Biological Physics · Physics 2013-03-29 David A. Mazziotti

Photosynthetic organisms use networks of chromophores to absorb sunlight and deliver the energy to reaction centres, where charge separation triggers a cascade of chemical steps to store the energy. We present a detailed model of the…

We present a rigorous theoretical description of excitonic dynamics in molecular light-harvesting aggregates photoexcited by weak-intensity radiation of arbitrary properties. While the interaction with light is included up to the second…

Chemical Physics · Physics 2021-01-01 Veljko Janković , Tomáš Mančal
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