相关论文: The Physical Basis for Long-lived Electronic Coher…
The observed prevalence of oscillatory signals in the spectroscopy of biological light-harvesting complexes at ambient temperatures has led to a search for mechanisms supporting coherent transport through larger molecules in noisy…
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…
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…
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…
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…
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.…
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…
Photosynthetic antenna complexes are responsible for absorbing energy from sunlight and transmitting it to remote locations where it can be stored. Recent experiments have found that this process involves long-lived quantum coherence…
In the primary step of light-harvesting, the energy of a photon is captured in antenna chlorophyll as an exciton. Its efficient conversion to stored chemical potential occurs in the special pair reaction center, which has to be reached by…
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…
The nature of excited states of open quantum systems produced by incoherent natural thermal light is analyzed based on a description of the generator of the dynamics. Natural thermal light is shown to generate long-lasting coherent dynamics…
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.…
Compositional engineering of the optical properties of hybrid organic-inorganic lead halide perovskites is one of the cornerstones for the realization of efficient solar cells and tailored light-emitting devices. We study the effect 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…
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…
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…
Photosynthetic light harvesting provides a natural blueprint for bioengineered and biomimetic solar energy and light detection technologies. Recent evidence suggests some individual light harvesting protein complexes (LHCs) and LHC subunits…
Electronic coherence is of utmost importance for the access and control of quantum-mechanical solid-state properties. Using a purely electronic observable, the photocurrent, we measure an electronic coherence time of 22 +/- 4 fs in…
Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the…
The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond…