Atoms and molecules in cavities, from weak to strong coupling in quantum-electrodynamics (QED) chemistry

被引：429

作者：

Flick, Johannes ^{[1
,2
]}

Ruggenthaler, Michael ^{[1
,2
]}

Appel, Heiko ^{[1
,2
]}

Rubio, Angel ^{[1
,2
,3
,4
]}

机构：

[1] Max Planck Inst Struct & Dynam Matter, Dept Phys, D-22761 Hamburg, Germany

[2] Ctr Free Electron Laser Sci, D-22761 Hamburg, Germany

[3] Univ Basque Country, Dept Fis Mat, Nanobio Spect Grp, San Sebastian 20018, Spain

[4] Univ Basque Country, Dept Fis Mat, European Theoret Spect Facil, San Sebastian 20018, Spain

来源：

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA | 2017年 / 114卷 / 12期

基金：

欧洲研究理事会; 奥地利科学基金会;

关键词：

QED chemistry; quantum electrodynamical density functional theory; adiabatic polariton surfaces; local control; optimized effective potential; DYNAMICS; FIELD; PHOTONS; DESIGN; MODEL;

D O I：

10.1073/pnas.1615509114

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

In this work, we provide an overview of how well-established concepts in the fields of quantum chemistry and material sciences have to be adapted when the quantum nature of light becomes important in correlated matter-photon problems. We analyze model systems in optical cavities, where the matter-photon interaction is considered from the weak-to the strong-coupling limit and for individual photon modes as well as for the multimode case. We identify fundamental changes in Born-Oppenheimer surfaces, spectroscopic quantities, conical intersections, and efficiency for quantum control. We conclude by applying our recently developed quantum-electrodynamical density-functional theory to spontaneous emission and show how a straightforward approximation accurately describes the correlated electron-photon dynamics. This work paves the way to describe matter-photon interactions from first principles and addresses the emergence of new states of matter in chemistry and material science.

引用

页码：3026 / 3034

页数：9

共 71 条

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