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arXiv:1504.05848

Thermal-Light-Induced Coherent Dynamics in Atoms and Molecules -- an Exact Quantum Mechanical Treatment

David Avisar, A. Eilam, A. D. Wilson‐Gordon

Published Apr 22, 2015• 0 citations
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Abstract

The question of whether sunlight induces coherent dynamics in biological systems is under debate. Here we show, on the basis of an exact fully quantum mechanical treatment, that thermal light induces excited-state coherences in matter similar to those induced by a coherent state. We demonstrate the phenomenon on a V-type model system and a two-state Born-Oppenheimer molecular system. Remarkably, wavepacket-like dynamics is induced in the excited molecular potential-energy surface.

DOI
10.48550/arxiv.1504.05848

Related papers

Thermal-light-induced dynamics: Coherence and revivals in V -type and molecular Jaynes-Cummings systems

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We examine the interaction of thermal light with matter with emphasis on two aspects that have not been considered before. By employing a fully quantized Jaynes-Cummings--type interaction model on a $V$-type three-level system, we show that multimode thermal light induces coherence in the excited material states. This is in contrast to previous studies that suggest thermal light cannot induce coherence in material systems. We also show that the ratio between the field detuning and the interaction constant has a significant influence on the characteristic time-dependent dynamics. In particular, for some ratio regimes, the thermal light induces dynamics with a ``coherentlike'' collapse and revivals pattern rather than the familiar pattern. We then extend the Jaynes-Cummings model to a two-state Born-Oppenheimer potential energy surface molecular system where the internal vibrational degrees of freedom are fully taken into account. The matter-field bipartite system is represented, and propagated, in the full electronic bond-coordinate Fock product space. We show that single-mode thermal light induces extensive excited-state vibrational coherence in the molecule that, when observed in coordinate space, exhibits wave-packet-like dynamics. The molecular Jaynes-Cummings model we propose is useful for cavity molecular dynamics simulations.

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Comment on “Thermal-light-induced dynamics: Coherence and revivals in V -type and molecular Jaynes-Cummings systems”

Amro Dodin, Paul W. Brumer

Recent numerical and analytical results have been obtained for the dynamics of a $V$-type system, and of a model molecular system, interacting with the thermal states of a cavity with a single mode or with a few discrete modes [D. Avisar and A. D. Wilson-Gordon, Phys. Rev. A 93, 033843 (2016)]. The authors speculate that these results may be relevant to excitation with natural incoherent radiation, such as sunlight, which has a continuous spectrum. We claim that this is incorrect, as are their comments about prior work on natural incoherent radiation that does properly deal with a continuous spectrum. Specifically, while their results obtained for the Jaynes-Cummings systems may be of interest for excitation by thermal states of cavities with a few modes, the discrete nature of their field modes produces dynamics that are fundamentally different from those induced by natural sunlight. Hence, we show here that the criticisms leveled in their paper regarding prior treatments that dealt with the continuous spectrum of natural incoherent radiation, as well as their speculation that excitation with continuous-mode thermal radiation can induce long-lived molecular coherences, are incorrect.

Physical Review A•Jun 28, 2017•1 citation

Reply to “Comment on ‘Thermal-light-induced dynamics: Coherence and revivals in V -type and molecular Jaynes-Cummings systems’ ”

David Avisar, A. D. Wilson‐Gordon

We recently presented an extended Jaynes-Cummings model for the interaction of a realistic molecular system of two Born-Oppenheimer potential energy surfaces and a quantized electromagnetic field [Avisar and Wilson-Gordon, Phys. Rev. A 93, 033843 (2016)]. We studied the interaction of this molecular model, and also a prototype $V$-type system, with single-mode and multimode thermal states of the field, characterized by low and high average photon number $\overline{n}$. Among our results, we showed that the three-mode thermal state of the field induces excited-state material coherence and that a thermal state of high $\overline{n}$ can induce ``coherentlike'' collapse and revival patterns. The preceding Comment by Dodin and Brumer [Phys. Rev. A 95, 067801 (2017)] criticizes our work for allegedly drawing conclusions regarding sunlight-induced dynamics from our results, and for unjustified citation of previous work. However, we think the Comment fails to represent the contents of our paper, and we therefore reply to it. We show it is based on misinterpretation of our paper.

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Abstract Excitation of molecules by incident incoherent electromagnetic radiation, such as sunlight, is described in detail and contrasted with the effect of coherent (e.g. laser) light. The nature of the quantum coherences induced by the former, relevant to transport processes in nature and in technology, is emphasized. Both equilibrium and steady state scenarios are discussed, three examples: simple models, calcium excitation in polarized light, and the isomerization of retinal in rhodopsin are used to expose the underlying qualitative nature of the established coherences.

arXiv:2109.06803•Journal of Physics B Atomic Molecular and Optical Physics•Nov 17, 2021•18 citations
The question of whether sunlight induces coherent dynamics in biological systems is under debate. Here we show, on the basis of an exact fully quantum mechanical treatment, that thermal light induces excited-state coherences in matter similar to those induced by a coherent state. We demonstrate the phenomenon on a V-type model system and a two-state Born-Oppenheimer molecular system. Remarkably, wavepacket-like dynamics is induced in the excited molecular potential-energy surface.
We examine the interaction of thermal light with matter with emphasis on two aspects that have not been considered before. By employing a fully quantized Jaynes-Cummings--type interaction model on a VVV-type three-level system, we show that multimode thermal light induces coherence in the excited material states. This is in contrast to previous studies that suggest thermal light cannot induce coherence in material systems. We also show that the ratio between the field detuning and the interaction constant has a significant influence on the characteristic time-dependent dynamics. In particular, for some ratio regimes, the thermal light induces dynamics with a ``coherentlike'' collapse and revivals pattern rather than the familiar pattern. We then extend the Jaynes-Cummings model to a two-state Born-Oppenheimer potential energy surface molecular system where the internal vibrational degrees of freedom are fully taken into account. The matter-field bipartite system is represented, and propagated, in the full electronic bond-coordinate Fock product space. We show that single-mode thermal light induces extensive excited-state vibrational coherence in the molecule that, when observed in coordinate space, exhibits wave-packet-like dynamics. The molecular Jaynes-Cummings model we propose is useful for cavity molecular dynamics simulations.
Recent numerical and analytical results have been obtained for the dynamics of a VVV-type system, and of a model molecular system, interacting with the thermal states of a cavity with a single mode or with a few discrete modes [D. Avisar and A. D. Wilson-Gordon, Phys. Rev. A 93, 033843 (2016)]. The authors speculate that these results may be relevant to excitation with natural incoherent radiation, such as sunlight, which has a continuous spectrum. We claim that this is incorrect, as are their comments about prior work on natural incoherent radiation that does properly deal with a continuous spectrum. Specifically, while their results obtained for the Jaynes-Cummings systems may be of interest for excitation by thermal states of cavities with a few modes, the discrete nature of their field modes produces dynamics that are fundamentally different from those induced by natural sunlight. Hence, we show here that the criticisms leveled in their paper regarding prior treatments that dealt with the continuous spectrum of natural incoherent radiation, as well as their speculation that excitation with continuous-mode thermal radiation can induce long-lived molecular coherences, are incorrect.
We recently presented an extended Jaynes-Cummings model for the interaction of a realistic molecular system of two Born-Oppenheimer potential energy surfaces and a quantized electromagnetic field [Avisar and Wilson-Gordon, Phys. Rev. A 93, 033843 (2016)]. We studied the interaction of this molecular model, and also a prototype VVV-type system, with single-mode and multimode thermal states of the field, characterized by low and high average photon number n‾\overline{n}n. Among our results, we showed that the three-mode thermal state of the field induces excited-state material coherence and that a thermal state of high n‾\overline{n}n can induce ``coherentlike'' collapse and revival patterns. The preceding Comment by Dodin and Brumer [Phys. Rev. A 95, 067801 (2017)] criticizes our work for allegedly drawing conclusions regarding sunlight-induced dynamics from our results, and for unjustified citation of previous work. However, we think the Comment fails to represent the contents of our paper, and we therefore reply to it. We show it is based on misinterpretation of our paper.
Under natural conditions, excitation of biological molecules, which display nonunitary open system dynamics, occurs via incoherent processes such as temperature changes or irradiation by sunlight or moonlight. The dynamics of such processes is explored analytically in a non-Markovian generic model. Specifically, a system S in equilibrium with a thermal bath TB is subjected to an external incoherent perturbation BB (such as sunlight) or another thermal bath TB${}^{\ensuremath{'}}$, which induces time evolution in (S+TB\text{S}+\text{TB}S+TB). Particular focus is on (i) the extent to which the resultant dynamics is coherent, and (ii) the role of ``stationary coherences'' established in the (S+TB\text{S}+\text{TB}S+TB) equilibration in response to the second incoherent perturbation. Results for systems with parameters analogous to those in light-harvesting molecules in photosynthesis show that the resultant dynamical behavior is incoherent beyond a very short response to the turn on of the perturbation.
One of the most pertinent problems in the debate on non-trivial quantum effects in biology concerns natural photosynthesis. Since sunlight is composed of thermal photons, it was argued to be unable to induce quantum coherence in matter, and that quantum mechanics is therefore irrelevant for the dynamical processes following photoabsorption. Our present analysis of a toy 'molecular aggregate'—composed of two dipole–dipole interacting two-level atoms treated as an open quantum system—however shows that incoherent excitations indeed can trigger persistent, coherent dynamics in both the site and the exciton bases: we demonstrate that collective decay processes induced by the dipole–dipole interactions create coherent intermolecular transport—regardless of the coherence properties of the incoming radiation. Our analysis shows that the steady state coherence is mediated by the population imbalance between the molecules and, therefore, increases with the energy difference between the two-level atoms. Our results establish the importance of collective decay processes in the study of ultrafast photophysics, and especially their potential role to generate stationary coherence in incoherently driven quantum transport.
Abstract Excitation of molecules by incident incoherent electromagnetic radiation, such as sunlight, is described in detail and contrasted with the effect of coherent (e.g. laser) light. The nature of the quantum coherences induced by the former, relevant to transport processes in nature and in technology, is emphasized. Both equilibrium and steady state scenarios are discussed, three examples: simple models, calcium excitation in polarized light, and the isomerization of retinal in rhodopsin are used to expose the underlying qualitative nature of the established coherences.