激子-极化子输运的量子动力学模拟

IF 15.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Niclas Krupp, Gerrit Groenhof, Oriol Vendrell
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引用次数: 0

摘要

激子和受限光模式之间的强耦合为有机材料中可调和增强的能量传输提供了一条有希望的途径。通过形成混合光物质准粒子,激子-极化子,电子激发可以通过弹道流以高速穿越长距离。然而,激子-极化子的输运行为在不同的实验中变化很大,包括扩散输运和弹道输运。材料和光模式的哪些性质决定了极化子的输运行为仍然是一个悬而未决的问题。通过全量子动力学模拟,我们揭示了理想腔和有耗腔中极化子输运对分子内振动相互作用和静态失序的强烈依赖。具体来说,我们表明分子内振动介导弛豫过程,在超快时间尺度上改变极化子组成、寿命和速度。对位置和动量空间中传播波包的分析,为在低温条件下实验发现的激子-极化子的弹道流的鲁棒性提供了机制上的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Quantum dynamics simulation of exciton-polariton transport

Quantum dynamics simulation of exciton-polariton transport

Strong coupling between excitons and confined modes of light presents a promising pathway to tunable and enhanced energy transport in organic materials. By forming hybrid light-matter quasiparticles, exciton-polaritons, electronic excitations can traverse long distances at high velocities through ballistic flow. However, transport behavior of exciton-polaritons varies strongly across experiments, spanning both diffusive and ballistic transport regimes. Which properties of the material and light-modes govern the transport behavior of polaritons remains an open question. Through full-quantum dynamical simulations we reveal a strong dependence of polariton transport on vibronic interactions and static disorder within molecules in both ideal and lossy cavities. Specifically, we show that intramolecular vibrations mediate relaxation processes that alter polariton composition, lifetime and velocity on ultrafast timescales. Analysis of the propagating wavepacket in position and momentum space provides mechanistic insight into the robustness of ballistic flow of exciton-polaritons found experimentally under cryogenic conditions.

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来源期刊
Nature Communications
Nature Communications Biological Science Disciplines-
CiteScore
24.90
自引率
2.40%
发文量
6928
审稿时长
3.7 months
期刊介绍: Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.
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