Toward Molecular Chiral Polaritons

Baranov, Denis G.; Schäfer, Christian; Gorkunov, M. V.

doi:10.1021/acsphotonics.2c02011

Cited by 22 publications

(17 citation statements)

References 182 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…It is worth mentioning that while in this review we focus on the linear polarization of radiation, exotic effects may be achieved when coupling matter to circularly polarized radiation modes in chiral cavities which allows to break fundamental materials symmetries . This recent direction in polaritonic chemistry in chiral cavities may enable enantioselective photochemistry, enhancing the circular dichroism signal and inducing valley polariton depolarization according to recent theoretical works. This preferential treatment of molecules may give rise to additional tunability afforded by the cavity to control outcomes of reactions that exhibit one or more chiral centers.…”

Section: Fundamental Theory Of Light–matter Interactionsmentioning

confidence: 99%

“…This preferential treatment of molecules may give rise to additional tunability afforded by the cavity to control outcomes of reactions that exhibit one or more chiral centers. Although it is beyond the scope of this review, there have been many recent studies exploring this phenomenon from both theoretical and ab initio perspectives. ,,, …”

Section: Fundamental Theory Of Light–matter Interactionsmentioning

confidence: 99%

“…Although it is beyond the scope of this review, there have been many recent studies exploring this phenomenon from both theoretical and ab initio perspectives. 172,173,175,176 With the motivation of this model in mind, in the next section, we first present a generalized dipole-gauge Hamiltonian and then a generalized Tavis-Cummings Hamiltonian.…”

Section: Many Molecules Coupled To Many Cavity Modesmentioning

confidence: 99%

See 2 more Smart Citations

Theoretical Advances in Polariton Chemistry and Molecular Cavity Quantum Electrodynamics

et al. 2023

View full text Add to dashboard Cite

When molecules are coupled to an optical cavity, new light–matter hybrid states, so-called polaritons, are formed due to quantum light–matter interactions. With the experimental demonstrations of modifying chemical reactivities by forming polaritons under strong light–matter interactions, theorists have been encouraged to develop new methods to simulate these systems and discover new strategies to tune and control reactions. This review summarizes some of these exciting theoretical advances in polariton chemistry, in methods ranging from the fundamental framework to computational techniques and applications spanning from photochemistry to vibrational strong coupling. Even though the theory of quantum light–matter interactions goes back to the midtwentieth century, the gaps in the knowledge of molecular quantum electrodynamics (QED) have only recently been filled. We review recent advances made in resolving gauge ambiguities, the correct form of different QED Hamiltonians under different gauges, and their connections to various quantum optics models. Then, we review recently developed ab initio QED approaches which can accurately describe polariton states in a realistic molecule–cavity hybrid system. We then discuss applications using these method advancements. We review advancements in polariton photochemistry where the cavity is made resonant to electronic transitions to control molecular nonadiabatic excited state dynamics and enable new photochemical reactivities. When the cavity resonance is tuned to the molecular vibrations instead, ground-state chemical reaction modifications have been demonstrated experimentally, though its mechanistic principle remains unclear. We present some recent theoretical progress in resolving this mystery. Finally, we review the recent advances in understanding the collective coupling regime between light and matter, where many molecules can collectively couple to a single cavity mode or many cavity modes. We also lay out the current challenges in theory to explain the observed experimental results. We hope that this review will serve as a useful document for anyone who wants to become familiar with the context of polariton chemistry and molecular cavity QED and thus significantly benefit the entire community.

show abstract

Section: Fundamental Theory Of Light–matter Interactionsmentioning

confidence: 99%

Section: Fundamental Theory Of Light–matter Interactionsmentioning

confidence: 99%

Section: Many Molecules Coupled To Many Cavity Modesmentioning

confidence: 99%

See 1 more Smart Citation

Theoretical Advances in Polariton Chemistry and Molecular Cavity Quantum Electrodynamics

et al. 2023

View full text Add to dashboard Cite

show abstract

“…One of the very latest discoveries in chiral metaphotonics is the field of chiral polaritonics, describing formation of polaritons exhibiting chiral features via interaction between chiral quantum emitters and modes of chiral cavities. 101 This field is in its infancy, and the very first models have been developed to describe the behavior of chiral polaritons in the formalism of cavity quantum electrodynamics. 102 We believe that a variety of novel effects will be discovered soon in nonlinear chiral polaritonics that could be enabled by strong coupling between chiral light and nonlinear matter.…”

Section: Discussionmentioning

confidence: 99%

Nonlinear chiral metaphotonics: a perspective

Koshelev,

Tonkaev,

Kivshar

2023

Adv. Photon.

View full text Add to dashboard Cite

“…Nevertheless, some progress has been made for a sinusoidal field in the semiclassical and QED frameworks. 196,199,202,[204][205][206] Riso et al 196 developed a QED coupled cluster method for the minimal coupling (MC) Hamiltonian, called MC-QED-CC, to investigate chiral polaritonics from an ab initio perspective. The complete shape of the field is retained and therefore there are no origin-dependence issues, and a chiral field is obtained by a proper superposition of two modes traveling in opposite directions.…”

Section: Beyond the Dipole Approximationmentioning

confidence: 99%

Polaritonic response theory for exact and approximate wave functions

Castagnola,

Riso,

Barlini

et al. 2023

WIREs Comput Mol Sci

View full text Add to dashboard Cite

Polaritonic chemistry is an interdisciplinary emerging field that presents several challenges and opportunities in chemistry, physics, and engineering. A systematic review of polaritonic response theory is presented, following a chemical perspective based on molecular response theory. We provide the reader with a general strategy for developing response theory for ab initio cavity quantum electrodynamics (QED) methods and critically emphasize details that still need clarification and require cooperation between the physical and chemistry communities. We show that several well‐established results can be applied to strong coupling light‐matter systems, leading to novel perspectives on the computation of matter and photonic properties. The application of the Pauli–Fierz Hamiltonian to polaritons is discussed, focusing on the effects of describing operators in different mathematical representations. We thoroughly examine the most common approximations employed in ab initio QED, such as the dipole approximation. We introduce the polaritonic response equations for the recently developed ab initio QED Hartree–Fock and QED coupled cluster methods. The discussion focuses on the similarities and differences from standard quantum chemistry methods, providing practical equations for computing the polaritonic properties.This article is categorized under: Electronic Structure Theory > Ab Initio Electronic Structure Methods Theoretical and Physical Chemistry > Spectroscopy Software > Quantum Chemistry

show abstract

Toward Molecular Chiral Polaritons

Cited by 22 publications

References 182 publications

Theoretical Advances in Polariton Chemistry and Molecular Cavity Quantum Electrodynamics

Theoretical Advances in Polariton Chemistry and Molecular Cavity Quantum Electrodynamics

Nonlinear chiral metaphotonics: a perspective

Polaritonic response theory for exact and approximate wave functions

Contact Info

Product

Resources

About