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Huelga, S. F.

Publications and source records attributed to Huelga, S. F..

Enhancing light-harvesting power with coherent vibrational interactions: A quantum heat engine picture

Recent evidence suggests that quantum effects may have functional importance in biological light-harvesting systems. Along with delocalized electronic excitations, it is now suspected that quantum coherent interactions with certain near-resonant vibrations may contribute to light-harvesting performance. However, the actual quantum advantage offered by such coherent vibrational interactions has not yet been established. We investigate a quantum design principle, whereby coherent exchange of single energy quanta between electronic and vibrational degrees of freedom can enhance a light-harvesting system’s power above what is possible by thermal mechanisms alone. We present a prototype quantum heat engine which cleanly illustrates this quantum design principle and quantifies its quantum advantage using thermodynamic measures of performance. We also demonstrate the principle’s relevance in parameter regimes connected to natural light-harvesting structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mappings of open quantum systems onto chain representations and Markovian embeddings

We study systems coupled linearly to a bath of oscillators. In an iterative process, the bath is transformed into a chain of oscillators with nearest neighbour interactions. A systematic procedure is provided to obtain the spectral density of the residual bath in each step, and it is shown that under general conditions these data converge. That is, the asymptotic part of the chain is universal, translation invariant with semicircular spectral density. The methods are based on orthogonal polynomials, in which we also solve the outstanding so-called “sequence of secondary measures problem” and give them a physical interpretation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Origin of long-lived oscillations in 2D-spectra of a quantum vibronic model: Electronic versus vibrational coherence

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 nonlinear 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 nonlinear 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.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗