Journal Article

PUBDB-2021-00408

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Polaritonic Chemistry: Collective Strong Coupling Implies Strong Local Modification of Chemical Properties

Sidler, D.CFEL*MPG* ; Schäfer, C. ; Ruggenthaler, M.CFEL*MPG* ; Rubio, A. (Corresponding author)CFEL*MPG*

2021
ACS Washington, DC

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Please use a persistent id in citations: doi:10.1021/acs.jpclett.0c03436  doi:10.3204/PUBDB-2021-00408

Abstract: A fundamental question in the field of polaritonic chemistry is whether collective coupling implies local modifications of chemical properties scaling with the ensemble size. Here we demonstrate from first-principles that an impurity present in a collectively coupled chemical ensemble features such locally scaling modifications. In particular, we find the formation of a novel dark state for a nitrogen dimer chain of variable size, whose local chemical properties are altered considerably at the impurity due to its embedding in the collectively coupled environment. Our simulations unify theoretical predictions from quantum optical models (e.g., collective dark states and bright polaritonic branches) with the single molecule quantum chemical perspective, which relies on the (quantized) redistribution of charges leading to a local hybridization of light and matter. Moreover, our findings suggest that recently developed ab initio methods for strong light-matter coupling are suitable to access these local polaritonic effects and provide a detailed understanding of photon-modified chemistry.

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Contributing Institute(s):

1. Forschungsgruppe für strukturelle Dynamik (MPSD)
2. MPSD (CFEL-MPT)

Research Program(s):

1. 899 - ohne Topic (POF4-899) (POF4-899)

Experiment(s):

1. No specific instrument

Appears in the scientific report 2021

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Database coverage:
; ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; Essential Science Indicators ; IF >= 5 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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