Ab initio linear-response approach to vibro-polaritons in the cavity
Born-Oppenheimer approximation
- URL: http://arxiv.org/abs/2108.11564v1
- Date: Thu, 26 Aug 2021 03:12:21 GMT
- Title: Ab initio linear-response approach to vibro-polaritons in the cavity
Born-Oppenheimer approximation
- Authors: John Bonini and Johannes Flick
- Abstract summary: We study mixed vibration-photon (vibro-polariton) states of molecules based on the cavity Born-Oppenheimer approximation and quantum-electrodynamical density-functional theory.
We develop an accurate model that highlights the consistent treatment of cavity coupled electrons in the vibrational strong coupling regime.
- Score: 0.0
- License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
- Abstract: Recent years have seen significant developments in the study of strong
light-matter coupling including the control of chemical reactions by altering
the vibrational normal modes of molecules. In the vibrational strong coupling
regime the normal modes of the system become hybrid modes which mix nuclear,
electronic, and photonic degrees of freedom. First principles methods capable
of treating light and matter degrees of freedom on the same level of theory are
an important tool in understanding such systems. In this work, we develop and
apply a generalized force constant matrix approach to the study of mixed
vibration-photon (vibro-polariton) states of molecules based on the cavity
Born-Oppenheimer approximation and quantum-electrodynamical density-functional
theory. With this method vibro-polariton modes and infrared spectra can be
computed via linear response techniques analogous to those widely used for
conventional vibrations and phonons. We also develop an accurate model that
highlights the consistent treatment of cavity coupled electrons in the
vibrational strong coupling regime. These electronic effects appear as new
terms previously disregarded by simpler models. This effective model also
allows for an accurate extrapolation of single and two molecule calculations to
the collective strong coupling limit of hundreds of molecules. We benchmark
these approaches for single and many CO$_2$ molecules coupled to a single
photon mode and the iron-pentacarbonyl Fe(CO)$_5$ molecule coupled to a few
photon modes. Our results are the first ab-initio results for collective
vibrational strong coupling effects. This framework for efficient computations
of vibro-polaritons paves the way to a systematic description and improved
understanding of the behavior of chemical systems in vibrational strong
coupling.
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