Light-Matter Response Functions in Quantum-Electrodynamical Density-Functional Theory: Modifications of Spectra and of the Maxwell Equations
Light-Matter Response Functions in Quantum-Electrodynamical Density-Functional Theory: Modifications of Spectra and of the Maxwell Equations
复制标题
量子电动密度泛函理论中的光物质响应函数：光谱和麦克斯韦方程的修改
DOI：
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发表时间：
2018
期刊：
影响因子：
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通讯作者：
Á. Rubio
中科院分区：
文献类型：
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作者：
Johannes Flick;Davis M. Welakuh;M. Ruggenthaler;H. Appel;Á. Rubio
我们介绍了线性响应理论的非相对论量子电动力学在长波长的限制，这使我们能够处理相关的激发态现象的物质-光子系统的第一性原理。利用量子电动力学密度泛函理论，我们可以将得到的完全耦合的光子-物质响应方程转化为一个伪本征值问题。这提供了传统的物质响应理论的直接扩展。我们的方法可以非常有效地解决数值和现有的从头算密度泛函响应的实现可以很容易地扩展到考虑到完整的光子-物质响应。我们强调光和物质之间的耦合如何改变通常的响应函数，并引入了新类型的响应函数，测量物质光子子系统的响应。我们展示了光和物质的相关性如何改变麦克斯韦方程，并强调了真实的系统的光谱是如何在强耦合到光子场时发生变化的。处理组合的物质-光子响应的一个关键特征是，激发的自然寿命变得可以从第一原理直接获得，并且不再需要人为加宽光谱。通过引入一个简单的扩展的随机相位近似的耦合物质-光子问题，我们能够提出的第一个从头算光谱的真实的分子系统，耦合到量子化的电磁场。
We introduce linear-response theory for non-relativistic quantum-electrodynamics in the long wavelength limit, which allows us to treat correlated excited-state phenomena of matter-photon systems from first principles. By using quantum-electrodynamical density-functional theory we can reformulate the resulting fully coupled photon-matter response equations as a pseudo-eigenvalue problem. This provides a direct extension of the conventional matter-only response theory. Our approach can be solved numerically very efficiently and existing ab-initio density-functional response implementations can be easily extended to take the full photon-matter response into account. We highlight how the coupling between light and matter changes the usual response functions and introduces new types of response functions that measure the matter-photon subsystem responses. We show how correlating light and matter changes the Maxwell equations and highlight how the spectra of real systems are changed upon strongly coupling to the photon field. A key feature of treating the combined matter-photon response is that natural lifetimes of excitations become directly accessible from first principles and no artificial broadening of spectra is required anymore. By introducing a straightforward extension of the random-phase approximation for the coupled matter-photon problem, we are able to present the first ab-initio spectra for a real molecular system that is coupled to the quantized electromagnetic field.
影响因子：
8.6
作者：
Cirio, Mauro;De Liberato, Simone;Nori, Franco
通讯作者：
Nori, Franco
影响因子：
56.9
作者：
Riek, C.;Seletskiy, D. V.;Leitenstorfer, A.
通讯作者：
Leitenstorfer, A.