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Register a new userVibronic origin of long-lived coherence in an artificial molecular light harvester
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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 ongoing debate, as it is unclear how the loss of coherence due to interaction with the noisy environments in such systems is averted. Here we report experimental and theoretical verification of coherent exciton-vibrational (vibronic) coupling as the origin of long-lasting coherence in an artificial light harvester, a molecular J-aggregate. In this macroscopically aligned tubular system, polarization controlled 2D spectroscopy delivers an uncongested and specific optical response as an ideal foundation for an in-depth theoretical description. We derive analytical expressions that show under which general conditions vibronic coupling leads to prolonged excited-state coherence.
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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 photosynthetic pigment protein complexes and we discuss the contributions of excitonic versus purely vibrational components to these oscillatory features. Considering a dimer model coupled to a structured spectral density we exemplify the fundamental aspects of the electron-phonon dynamics, and by analyzing separately the different contributions to the non linear signal, we show that for realistic parameter regimes purely electronic coherence is of the same order as purely vibrational coherence in the electronic ground state. Moreover, we demonstrate how the latter relies upon the excitonic interaction to manifest. These results link recently proposed microscopic, non-equilibrium mechanisms to support long lived coherence at ambient temperatures with actual experimental observations of oscillatory behaviour using 2D photon echo techniques to corroborate the fundamental importance of the interplay of electronic and vibrational degrees of freedom in the dynamics of light harvesting aggregates.
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.
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 raised two fundamental questions: Firstly, what are the mechanisms supporting long-lived coherences and secondly, how can we assess the possible functional role that the interplay of noise and quantum coherence might play in the seemingly optimal operation of biological systems under natural conditions? Here we review recent results, illuminate them at the hand of two paradigmatic systems, the Fenna-Matthew-Olson (FMO) complex and the light harvesting complex LHII, and present new progress on both questions. In particular we introduce the concept of the phonon antennae and discuss the possible microscopic origin or long-lived electronic coherences.
We observe the coherence of an interacting two-component Bose-Einstein condensate (BEC) surviving for seconds in a trapped Ramsey interferometer. Mean-field driven collective oscillations of two components lead to periodic dephasing and rephasing of condensate wave functions with a slow decay of the interference fringe visibility. We apply spin echo synchronous with the self-rephasing of the condensate to reduce the influence of state-dependent atom losses, significantly enhancing the visibility up to 0.75 at the evolution time of 1.5s. Mean-field theory consistently predicts higher visibility than experimentally observed values. We quantify the effects of classical and quantum noise and infer a coherence time of 2.8 s for a trapped condensate of 5.5e4 interacting atoms.
Confining particles in hollow-core photonic crystal fibers has opened up new prospects to scale up the distance and time over which particles can be made to interact with light. However, maintaining long-lived quantum spin coherence and/or transporting it over macroscopic distances in a waveguide remain challenging. Here, we demonstrate coherent guiding of ground-state superpositions of 85Rb atoms over a centimeter range and hundreds of milliseconds inside a hollow-core photonic crystal fiber. The decoherence is mainly due to dephasing from residual differential light shift (DLS) from the optical trap and the inhomogeneity of ambient magnetic field. Our experiment establishes an important step towards a versatile platform that can lead to applications in quantum information networks and matter wave circuit for quantum sensing.
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