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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

Oscillations in time-dependent 2D electronic spectra appear as evidence of quantum coherence in light-harvesting systems related to electronic-vibrational resonant interactions. Nature, however, takes place in a non-equilibrium…

量子物理 · 物理学 2022-12-29 Leonardo F. Calderón , Chern Chuang , Paul Brumer

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…

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

Identifying signatures of quantum coherent behaviour in photoactive systems that are maintained in stationary states away from thermal equilibrium is an open problem of wide interest in a variety of physical scenarios, including single…

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…

化学物理 · 物理学 2019-10-30 Stefano Tomasi , Sima Baghbanzadeh , Saleh Rahimi-Keshari , Ivan Kassal

Coherence-enhanced light harvesting has not been directly observed experimentally, despite theoretical evidence that coherence can significantly enhance light-harvesting performance. The main experimental obstacle has been the difficulty in…

化学物理 · 物理学 2021-06-30 Stefano Tomasi , Dominic M. Rouse , Erik M. Gauger , Brendon W. Lovett , Ivan Kassal

Energy transfer between chromophores in photosynthesis proceeds with near unity quantum efficiency. Understanding the precise mechanisms of these processes is made difficult by the complexity of the electronic structure and interactions…

化学物理 · 物理学 2015-03-03 Gethin H. Richards , Krystyna E. Wilk , Paul M. G. Curmi , Jeffrey A. Davis

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…

The physical basis for observed long-lived electronic coherence in photosynthetic light-harvesting systems is identified using an analytically soluble model. Three physical features are found to be responsible for their long coherence…

量子物理 · 物理学 2011-10-18 Leonardo A. Pachon , Paul Brumer

Coherent dynamics of coupled molecules are effectively characterized by the two-dimensional (2D) electronic coherent spectroscopy. Depending on the coupling between electronic and vibrational states, oscillating signals of purely…

化学物理 · 物理学 2013-10-17 Vytautas Butkus , Donatas Zigmantas , Darius Abramavicius , Leonas Valkunas

We present a perturbation approach rooted in time-dependent density-functional theory to calculate electron hole (eh)-pair excitation spectra during the non-adiabatic vibrational damping of adsorbates on metal surfaces. Our analysis for the…

化学物理 · 物理学 2017-11-22 Simon P. Rittmeyer , Jörg Meyer , Karsten Reuter

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 present various types of reduced models including five vibrational modes and three electronic states for the pyrazine molecule in order to investigate the lifetime of electronic coherence in a rigid and neutral system. Using an ultrafast…

化学物理 · 物理学 2020-08-26 A. Csehi , P. Badankó , G. J. Halász , Á. Vibók , B. Lasorne

The prevalence of long-lasting oscillatory signals in the 2d echo-spectroscopy of light-harvesting complexes has led to a search for possible mechanisms. We investigate how two causes of oscillatory signals are intertwined: (i) electronic…

生物物理 · 物理学 2013-08-20 Christoph Kreisbeck , Tobias Kramer , Alan Aspuru-Guzik

We analyze electronically excited nuclear wave functions and their coherence when subjecting a molecule to the action of natural, pulsed incoherent solar-like light, and to that of ultrashort coherent light assumed to have the same center…

量子物理 · 物理学 2015-06-12 Alex C. Han , Moshe Shapiro , Paul Brumer

We characterize both entanglement and quantum coherence in a molecular system by connecting the linear entropy of electronic-nuclear entanglement with Wigner-Yanase skew information measuring vibronic coherence and local quantum uncertainty…

量子物理 · 物理学 2018-11-21 Mihaela Vatasescu

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…

生物物理 · 物理学 2013-03-29 David A. Mazziotti

The coherence of light has been proposed as a quantum-mechanical control for enhancing light-harvesting efficiency. In particular, optical coherence can be manipulated by changing either the polarization state or spectral phase of the…

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
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