Analytic model reveals local molecular polarizability changes induced by collective strong coupling in optical cavities DOI

Jacob Horak,

Dominik Sidler, Thomas Schnappinger

и другие.

Physical Review Research, Год журнала: 2025, Номер 7(1)

Опубликована: Март 5, 2025

Despite recent numerical evidence, one of the fundamental theoretical mysteries polaritonic chemistry is how and if collective strong coupling can induce local changes electronic structure to modify chemical properties. Here we present nonperturbative analytic results for a model system consisting an ensemble N harmonic molecules under vibrational (VSC) that alters our understanding this question. By applying cavity Born-Oppenheimer partitioning on Pauli-Fierz Hamiltonian in dipole approximation, dressed many-molecule problem be solved nonperturbatively analytically dilute limit, i.e., self-consistent solution with mean-field Hartree-product wave function becomes exact. We discover molecular polarizabilities are modified even case vanishingly small single-molecule couplings. Consequently, polarization mechanism persists large-N limit. In contrast, perturbative calculation based uncoupled leads qualitatively erroneous scaling behavior vanishing effects large-N Nevertheless, exact (self-consistent) determined from simulations instead. Our observations demonstrate hitherto existing collective-scaling arguments insufficient they pave way refined single- (or few-)molecule strong-coupling systems coupling. Published by American Physical Society 2025

Язык: Английский

Ultrastrong coupling between light and matter DOI
Anton Frisk Kockum, Adam Miranowicz, Simone De Liberato

и другие.

Nature Reviews Physics, Год журнала: 2019, Номер 1(1), С. 19 - 40

Опубликована: Янв. 3, 2019

Язык: Английский

Процитировано

550

Moiré heterostructures as a condensed-matter quantum simulator DOI
Dante M. Kennes, Martin Claassen, Lede Xian

и другие.

Nature Physics, Год журнала: 2021, Номер 17(2), С. 155 - 163

Опубликована: Фев. 1, 2021

Язык: Английский

Процитировано

503

Strong light–matter interactions: a new direction within chemistry DOI Creative Commons
Manuel Hertzog, Mao Wang, Jürgen Mony

и другие.

Chemical Society Reviews, Год журнала: 2019, Номер 48(3), С. 937 - 961

Опубликована: Янв. 1, 2019

It is possible to modify the chemical and physical properties of molecules, not only through modifications but also by coupling molecules strongly light. More intriguingly, strong between light even without presence a photon. The phenomenon that makes this called vacuum fluctuations, which finite zero point energy quantized electromagnetic field inside an optical cavity. light-matter coupling, can be as large 1 eV (100 kJ mol-1), leads formation new hybrid states, polaritons. formed states viewed linear combination (vacuum field) matter (molecules), thus completely changing landscape system. Using interactions have for instance been used change reactivity, charge conductivity, excited state relaxation pathways rates reactions organic molecules. In review brief history given, followed theoretical framework, methods analysis, accomplishments. Finally, personal reflection on future perspectives applications within given.

Язык: Английский

Процитировано

364

Cavity Catalysis by Cooperative Vibrational Strong Coupling of Reactant and Solvent Molecules DOI Creative Commons

Jyoti Lather,

Pooja Bhatt,

Anoop Thomas

и другие.

Angewandte Chemie International Edition, Год журнала: 2019, Номер 58(31), С. 10635 - 10638

Опубликована: Июнь 12, 2019

Here, we report the catalytic effect of vibrational strong coupling (VSC) on solvolysis para-nitrophenyl acetate (PNPA), which increases reaction rate by an order magnitude. This is observed when microfluidic Fabry-Perot cavity in VSC generated tuned to C=O stretching mode both reactant and solvent molecules. Thermodynamic experiments confirm nature system. The change follows exponential relation with respect strength solvent, indicating a cooperative between molecules reactant. Furthermore, study kinetic isotope clearly shows that overlap bands strongly coupled critical for catalysis this reaction. combination effects confirms potential as new frontier chemistry.

Язык: Английский

Процитировано

269

Strong light-matter coupling in quantum chemistry and quantum photonics DOI Creative Commons
Johannes Flick, Nicholas Rivera, Prineha Narang

и другие.

Nanophotonics, Год журнала: 2018, Номер 7(9), С. 1479 - 1501

Опубликована: Сен. 1, 2018

Abstract In this article, we review strong light-matter coupling at the interface of materials science, quantum chemistry, and photonics. The control light heat thermodynamic limits enables exciting new opportunities for rapidly converging fields polaritonic chemistry optics atomic scale from a theoretical computational perspective. Our follows remarkable experimental demonstrations that now routinely achieve limit matter. many molecules couple collectively to single-photon mode, whereas, in field nanoplasmonics, can be achieved single-molecule limit. Theoretical approaches address these experiments, however, are more recent come spectrum merging developments electrodynamics alike. We latest highlight common features between two different limits, maintaining focus on tools used analyze classes systems. Finally, present perspective need steps toward merging, formally computationally, most prominent Nobel Prize-winning theories physics chemistry: electronic structure (density functional) theory. case how fully description matter treats electrons, photons, phonons same quantized footing will unravel effects cavity-controlled chemical dynamics, optomechanics, nanophotonics, other use phonons.

Язык: Английский

Процитировано

244

Polariton panorama DOI Creative Commons
D. N. Basov, Ana Asenjo-Garcı́a, P. James Schuck

и другие.

Nanophotonics, Год журнала: 2020, Номер 10(1), С. 549 - 577

Опубликована: Ноя. 11, 2020

Abstract In this brief review, we summarize and elaborate on some of the nomenclature polaritonic phenomena systems as they appear in literature quantum materials optics. Our summary includes at least 70 different types light–matter dressing effects. This also unravels a broad panorama physics applications polaritons. A constantly updated version review is available https://infrared.cni.columbia.edu .

Язык: Английский

Процитировано

234

Selective manipulation of electronically excited states through strong light–matter interactions DOI Creative Commons
Kati Stranius, Manuel Hertzog, Karl Börjesson

и другие.

Nature Communications, Год журнала: 2018, Номер 9(1)

Опубликована: Июнь 5, 2018

Abstract Strong coupling between light and matter leads to the spontaneous formation of hybrid light–matter states, having different energies than uncoupled states. This opens up for new ways modifying energy landscape molecules without changing their atoms or structure. Heavy metal-free organic emitting diodes (OLED) use reversed intersystem crossing (RISC) harvest from excited triplet is a slow process, thus increasing rate RISC could potentially enhance OLED performance. Here we demonstrate selective singlet state Erythrosine B perturbing level nearby state. The reduces triplet–singlet gap, leading four-time enhancement decay rate, most likely due an enhanced RISC. Furthermore, anticipate that strong can be used create energy-inverted molecular systems ground lowest

Язык: Английский

Процитировано

219

Cavity quantum-electrodynamical polaritonically enhanced electron-phonon coupling and its influence on superconductivity DOI Creative Commons
Michael A. Sentef, Michael Ruggenthaler, Ángel Rubio

и другие.

Science Advances, Год журнала: 2018, Номер 4(11)

Опубликована: Ноя. 2, 2018

Cavity photons can enhance the coupling between electrons and lattice vibrations affect important properties of 2D materials.

Язык: Английский

Процитировано

213

Resonance Energy Transfer: From Fundamental Theory to Recent Applications DOI Creative Commons
Garth A. Jones, David S. Bradshaw

Frontiers in Physics, Год журнала: 2019, Номер 7

Опубликована: Июль 12, 2019

Resonance energy transfer (RET), the transport of electronic from one atom or molecule to another, has significant importance a number diverse areas science. Since pioneering experiments on RET by Cario and Franck in 1922, theoretical understanding process been continually refined. This review presents historical account post-Förster outlook RET, based quantum electrodynamics, up present-day viewpoint. It is through this framework that short-range, R–6 distance dependence Förster theory was unified with long range, radiative governed inverse-square law. Crucial knowledge electric dipole-electric dipole coupling tensor; we outline its mathematical derivation view explaining some key physical concepts RET. The higher order interactions involve magnetic dipoles quadrupoles are also discussed. To conclude, survey provided latest research, which includes between nanomaterials, enhancement due surface plasmons, possibilities outside usual ultraviolet visible range within cavity.

Язык: Английский

Процитировано

213

Modification of excitation and charge transfer in cavity quantum-electrodynamical chemistry DOI Creative Commons
C. Schäfer, Michael Ruggenthaler,

Heiko Appel

и другие.

Proceedings of the National Academy of Sciences, Год журнала: 2019, Номер 116(11), С. 4883 - 4892

Опубликована: Фев. 7, 2019

Significance Excitation and charge transfer are fundamental processes in nature, controlling these is a major goal of quantum chemistry. While well understood for the usual free-space case, when electromagnetic vacuum changed due to, e.g., cavity, can be dramatically different. We consider changes with real-space donor–acceptor models, where we put an emphasis on impact electron–electron correlations. find results line recent experiments, strong light–matter interaction leads to enhanced reactions, even corresponding situation no should possible. highlight that depend crucially Coulomb self-polarization interactions.

Язык: Английский

Процитировано

194