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arXiv 2002.10461quant-phphysics.chem-phphysics.comp-phphysics.optics
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从第一性原理研究弱到强光-物质耦合及耗散动力学

Weak-to-Strong Light-Matter Coupling and Dissipative Dynamics from First Principles

Derek S. Wang, Tomáš Neuman, Johannes Flick, Prineha Narang

AI总结:

本文推广量子电动力学密度泛函理论以纳入耗散动力学,从头算描述苯和甲苯在弱到强耦合区间的腔-分子动力学,并实现腔介导的电子激发态能量转移。

摘要:

腔介导的光-物质耦合能够显著改变分子的光电和物理化学性质。对这些体系进行从头算理论预测,需要将基于非微扰、多体电子结构理论的方法与腔量子电动力学以及开放量子系统理论相结合。在此,我们推广了量子电动力学密度泛函理论,以计入耗散动力学,并描述弱耦合到强耦合区间中的腔-分子相互作用。具体而言,为建立这一广义技术,我们研究了苯和甲苯在弱到强光-物质耦合下的激发态动力学和光谱响应。通过调节耦合,我们实现了电子激发态之间由腔介导的能量转移。这种广义的从头算量子电动力学密度泛函理论处理可以自然扩展,用于描述任意电磁环境中的腔介导相互作用,获取关联的光-物质可观测量,从而弥合电子结构理论与量子光学之间的差距。

英文摘要:

Cavity-mediated light-matter coupling can dramatically alter opto-electronic and physico-chemical properties of a molecule. Ab initio theoretical predictions of these systems need to combine non-perturbative, many-body electronic structure theory-based methods with cavity quantum electrodynamics and theories of open quantum systems. Here we generalize quantum-electrodynamical density functional theory to account for dissipative dynamics and describe coupled cavity-molecule interactions in the weak-to-strong-coupling regimes. Specifically, to establish this generalized technique, we study excited-state dynamics and spectral responses of benzene and toluene under weak-to-strong light-matter coupling. By tuning the coupling we achieve cavity-mediated energy transfer between electronic excited states. This generalized ab initio quantum-electrodynamical density functional theory treatment can be naturally extended to describe cavity-mediated interactions in arbitrary electromagnetic environments, accessing correlated light-matter observables and thereby closing the gap between electronic structure theory and quantum optics.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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