Search: onr:"swepub:oai:research.chalmers.se:516245fd-dc11-4738-9c6a-38c74ef15d1a" >
A perspective on ab...
A perspective on ab initio modeling of polaritonic chemistry: The role of non-equilibrium effects and quantum collectivity
-
- Sidler, Dominik (author)
- Center for Free-Electron Laser Science (CFEL),Max Planck Gesellschaft zur Förderung der Wissenschaften e.V. (MPG),Max Planck Society for the Advancement of Science (MPG),Universität Hamburg,University of Hamburg
-
- Ruggenthaler, Michael (author)
- Max Planck Gesellschaft zur Förderung der Wissenschaften e.V. (MPG),Max Planck Society for the Advancement of Science (MPG),Universität Hamburg,University of Hamburg,Center for Free-Electron Laser Science (CFEL)
-
- Schäfer, Christian, 1989 (author)
- Chalmers tekniska högskola,Chalmers University of Technology
-
show more...
-
- Ronca, Enrico (author)
- CNR-IPCF
-
- Rubio, Angel (author)
- Center for Free-Electron Laser Science (CFEL),Universität Hamburg,University of Hamburg,Universidad del Pais Vasco / Euskal Herriko Unibertsitatea,University of the Basque Country (UPV/EHU),Max Planck Gesellschaft zur Förderung der Wissenschaften e.V. (MPG),Max Planck Society for the Advancement of Science (MPG),Flatiron Institute
-
show less...
-
Center for Free-Electron Laser Science (CFEL) Max Planck Gesellschaft zur Förderung der Wissenschaften eV. (MPG) (creator_code:org_t)
- AIP Publishing, 2022
- 2022
- English.
-
In: Journal of Chemical Physics. - : AIP Publishing. - 1089-7690 .- 0021-9606. ; 156:23
- Related links:
-
https://research.cha... (primary) (free)
-
show more...
-
https://research.cha...
-
https://doi.org/10.1...
-
show less...
Abstract
Subject headings
Close
- This Perspective provides a brief introduction into the theoretical complexity of polaritonic chemistry, which emerges from the hybrid nature of strongly coupled light-matter states. To tackle this complexity, the importance of ab initio methods is highlighted. Based on those, novel ideas and research avenues are developed with respect to quantum collectivity, as well as for resonance phenomena immanent in reaction rates under vibrational strong coupling. Indeed, fundamental theoretical questions arise about the mesoscopic scale of quantum-collectively coupled molecules when considering the depolarization shift in the interpretation of experimental data. Furthermore, to rationalize recent findings based on quantum electrodynamical density-functional theory (QEDFT), a simple, but computationally efficient, Langevin framework is proposed based on well-established methods from molecular dynamics. It suggests the emergence of cavity-induced non-equilibrium nuclear dynamics, where thermal (stochastic) resonance phenomena could emerge in the absence of external periodic driving. Overall, we believe that the latest ab initio results indeed suggest a paradigmatic shift for ground-state chemical reactions under vibrational strong coupling from the collective quantum interpretation toward a more local, (semi)-classically and non-equilibrium dominated perspective. Finally, various extensions toward a refined description of cavity-modified chemistry are introduced in the context of QEDFT, and future directions of the field are sketched.
Subject headings
- NATURVETENSKAP -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)
- NATURVETENSKAP -- Kemi -- Teoretisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Theoretical Chemistry (hsv//eng)
Publication and Content Type
- art (subject category)
- ref (subject category)
Find in a library
To the university's database