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We demonstrate that the coupling of excitonic and vibrational motion in biological complexes can provide mechanisms to explain the long-lived oscillations that have been obtained in non linear spectroscopic signals of different…

化学物理 · 物理学 2015-06-17 M. B. Plenio , J. Almeida , S. F. Huelga

Recent observations of beating signals in the excitation energy transfer dynamics of photosynthetic complexes have been interpreted as evidence for sustained coherences that are sufficiently long-lived for energy transport and coherence to…

量子物理 · 物理学 2013-03-05 A. W. Chin , J. Prior , R. Rosenbach , F. Caycedo-Soler , S. F. Huelga , M. B. Plenio

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…

生物物理 · 物理学 2012-06-07 Niklas Christensson , Harald F. Kauffmann , Tonu Pullerits , Tomas Mancal

We theoretically investigate exciton relaxation dynamics in molecular aggregates based on model photosynthetic complexes under various conditions of incoherent excitation. We show that noise-induced quantum coherence is generated between…

生物物理 · 物理学 2014-08-14 Dmitri V. Voronine , Konstantin E. Dorfman , Bin Cao , Amitabh Joshi

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…

Luminescence properties of colloidal quantum dots have found applications in imaging, light-sources, and displays. Despite wide interest, several experimental observations from these quantum dots, such as the short lifetime on the scale of…

介观与纳米尺度物理 · 物理学 2018-06-05 Meenakshi Khosla , Sravya Rao , Shilpi Gupta

A remarkable amount of theoretical research has been carried out to elucidate the physical origins of the recently observed long-lived quantum coherence in the electronic energy transfer process in biological photosynthetic systems.…

量子物理 · 物理学 2015-03-19 Sangwoo Shim , Patrick Rebentrost , Stéphanie Valleau , Alan Aspuru-Guzik

The quantum dynamics of transport networks in the presence of noisy environments have recently received renewed attention with the discovery of long-lived coherences in different photosynthetic complexes. This experimental evidence has…

生物物理 · 物理学 2015-06-04 A. W. Chin , S. F. Huelga , M. B. Plenio

A general theory of electronic excitations in aggregates of molecules coupled to intramolecular vibrations and the harmonic environment is developed for simulation of the third-order nonlinear spectroscopy signals. The model is applied in…

化学物理 · 物理学 2014-01-17 Vytautas Butkus , Leonas Valkunas , Darius Abramavicius

Quantum coherence is highly involved in photochemical functioning of complex molecular systems. Co-existence and intermixing of electronic and/or vibrational coherences, while never unambiguously identified experimentally, has been proposed…

We investigate the exciton dynamics in an exactly solvable two-band model for semiconductors. The model incorporates light-matter, electron-electron and electron-phonon interactions, and captures exciton formation as well as the transition…

材料科学 · 物理学 2025-02-13 Zhenlin Zhang , Wei Hu , Enrico Perfetto , Gianluca Stefanucci

We identify an intriguing feature of the electron-vibrational dynamics of molecular systems via a computational examination of \emph{trans}-polyacetylene oligomers. Here, via the vibronic interactions, the decay of an electron in the…

量子物理 · 物理学 2013-04-09 Ignacio Franco , Angel Rubio , Paul Brumer

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…

量子物理 · 物理学 2015-02-12 Arend G. Dijkstra , Chen Wang , Jianshu Cao , Graham R. Fleming

We present a theoretical study of noise-induced quantum coherences in a model three-level V-type system interacting with incoherent radiation, an important prototype for a wide range of physical systems ranging from trapped ions to…

化学物理 · 物理学 2015-06-19 Timur V. Tscherbul , Paul Brumer

Photosynthetic proteins have evolved over billions of years so as to undergo optimal energy transfer to the sites of charge separation. Based on spectroscopically detected quantum coherences, it has been suggested that this energy transfer…

化学物理 · 物理学 2016-07-13 David Paleček , Petra Edlund , Sebastian Westenhoff , Donatas Zigmantas

A vibronic-exciton model is applied to investigate the mechanism of enhancement of coherent oscillations due to mixing of electronic and nuclear degrees of freedom recently proposed as the origin of the long-lived oscillations in 2D spectra…

化学物理 · 物理学 2016-05-26 Aurélia Chenu , Niklas Christensson , Harald F. Kauffmann , Tomáš Mančal

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…

化学物理 · 物理学 2020-07-15 Leonardo F. Calderón , Leonardo A. Pachón

During the long course of evolution, nature has learnt how to exploit quantum effects. In fact, recent experiments reveal the existence of quantum processes whose coherence extends over unexpectedly long time and space ranges. In…

量子物理 · 物理学 2015-07-14 G. L. Giorgi , M. Roncaglia , F. A. Raffa , M. Genovese

Strong light-matter coupling to form exciton- and vibropolaritons is increasingly touted as a powerful tool to alter the fundamental properties of organic materials. It is proposed that these states and their facile tunability can be used…

The idea that excitonic state (electronic) coherences are of fundamental importance to natural photosynthesis gained popularity when, a decade ago, slowly dephasing quantum beats were observed in the two-dimensional electronic spectra of…

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