Perspective: Quantum Hamiltonians for optical interactions

Andrews, Davıd L.; Jones, G.; Salam, A.; Woolley, Richard

doi:10.1063/1.5018399

Cited by 97 publications

(117 citation statements)

References 123 publications

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“…We start from a inhomogeneous ensemble first and then discuss the conditions under which the commonly used homogeneous results emerge. We describe light-matter coupling in the point-dipole approximation within a multipolar framework [121], to give the Hamiltonian…”

Section: Microscopic Cavity Qed Approachmentioning

confidence: 99%

“…The first term describes an empty cavity (no molecules). This term is in general defined by the electromagnetic energy density over the optical structure, and takes into account the dispersive and absorptive character of the cavity materials [121]. The termĤ m (x i ) describes the electronic, vibrational, and rotational degrees of freedom of the i-th molecule in the ensemble, located at position x i .…”

Section: Microscopic Cavity Qed Approachmentioning

confidence: 99%

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Molecular polaritons for controlling chemistry with quantum optics

Herrera

Owrutsky

2020

The Journal of Chemical Physics

260

248

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This is a tutorial-style introduction to the field of molecular polaritons. We describe the basic physical principles and consequences of strong light-matter coupling common to molecular ensembles embedded in UV-visible or infrared cavities. Using a microscopic quantum electrodynamics formulation, we discuss the competition between the collective cooperative dipolar response of a molecular ensemble and local dynamical processes that molecules typically undergo, including chemical reactions. We highlight some of the observable consequences of this competition between local and collective effects in linear transmission spectroscopy, including the formal equivalence between quantum mechanical theory and the classical transfer matrix method, under specific conditions of molecular density and indistinguishability. We also overview recent experimental and theoretical developments on strong and ultrastrong coupling with electronic and vibrational transitions, with a special focus on cavity-modified chemistry and infrared spectroscopy under vibrational strong coupling. We finally suggest several opportunities for further studies that may lead to novel applications in chemical and electromagnetic sensing, energy conversion, optoelectronics, quantum control and quantum technology.

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Section: Microscopic Cavity Qed Approachmentioning

confidence: 99%

Section: Microscopic Cavity Qed Approachmentioning

confidence: 99%

Molecular polaritons for controlling chemistry with quantum optics

Herrera

Owrutsky

2020

The Journal of Chemical Physics

260

248

View full text Add to dashboard Cite

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“…C. The quadratic coupling (13) in contrast is an energetic shift between eigenstates. The equivalence between the presented Born-Huang expansion and the Power-Zienau-Woolley transformation [64,65] is elaborated in section III A. In combination, (14) and (18) constitute the polaritonic subsystem which is interacting with the nuclei.…”

Section: Born-oppenheimer Hamiltonianmentioning

confidence: 99%

Ab initiononrelativistic quantum electrodynamics: Bridging quantum chemistry and quantum optics from weak to strong coupling

2018

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By applying the Born-Huang expansion, originally developed for coupled nucleus-electron systems, to the full nucleus-electron-photon Hamiltonian of non-relativistic quantum electrodynamics (QED) in the long-wavelength approximation, we deduce an exact set of coupled equations for electrons on photonic energy surfaces and the nuclei on the resulting polaritonic energy surfaces. This theory describes seamlessly many-body interactions between nuclei, electrons and photons including the quantum fluctuation of the electromagnetic field and provides a proper first-principle framework to describe QED-chemistry phenomena, namely polaritonic and cavity chemistry effects. Since the photonic surfaces and the corresponding non-adiabatic coupling elements can be solved analytically, the resulting expansion can be brought into a compact form which allows us to analyze aspects of coupled nucleus-electron-photon systems in a simple and intuitive manner. Furthermore, we discuss structural differences between the exact quantum treatment and Floquet theory, show how existing implementations of Floquet theory can be adjusted to adhere to QED and highlight how standard drawbacks of Floquet theory can be overcome. We then highlight, by assuming that the relevant photonic frequencies of a prototypical cavity QED experiment are in the energy range of the electrons, how from this generalized Born-Huang expansion an adapted Born-Oppenheimer approximation for nuclei on polaritonic surfaces can be deduced. This form allows a direct application of first-principle methods of quantum chemistry such as coupled-cluster or configuration interaction approaches to QED chemistry. By restricting the basis set of this generalized Born-Oppenheimer approximation we furthermore bridge quantum chemistry and quantum optics by recovering simple models of coupled matter-photon systems employed in quantum optics and polaritonic chemistry. We finally highlight numerically that simple few-level models can lead to physically wrong predictions, even in weak-coupling regimes, and show how the presented derivations from first principles help to check and derive physically reliable simplified models. * Electronic address: christian.schaefer@mpsd.mpg.de †

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“…In the Power-Zienau-Woolley formulation of quantum electrodynamics, matter-light coupling comprises just three terms [84,85]: …”

Section: Light-matter Interactionsmentioning

confidence: 99%

Quantum formulation for nanoscale optical and material chirality: symmetry issues, space and time parity, and observables

Andrews

2018

J. Opt.

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To properly represent the interplay and coupling of optical and material chirality at the photonmolecule or photon-nanoparticle level invites a recognition of quantum facets in the fundamental aspects and mechanisms of light-matter interaction. It is therefore appropriate to cast theory in a general quantum form, one that is applicable to both linear and nonlinear optics as well as various forms of chiroptical interaction including chiral optomechanics. Such a framework, fully accounting for both radiation and matter in quantum terms, facilitates the scrutiny and identification of key issues concerning spatial and temporal parity, scale, dissipation and measurement. Furthermore it fully provides for describing the interactions of structured or twisted light beams with a vortex character, and it leads to the complete identification of symmetry conditions for materials to provide for chiral discrimination. Quantum considerations also lend a distinctive perspective to the very different senses in which other aspects of chirality are recognized in metamaterials. Duly attending to the symmetry principles governing allowed or disallowed forms of chiral discrimination supports an objective appraisal of the experimental possibilities and developing applications.

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Perspective: Quantum Hamiltonians for optical interactions

Cited by 97 publications

References 123 publications

Molecular polaritons for controlling chemistry with quantum optics

Molecular polaritons for controlling chemistry with quantum optics

Ab initiononrelativistic quantum electrodynamics: Bridging quantum chemistry and quantum optics from weak to strong coupling

Quantum formulation for nanoscale optical and material chirality: symmetry issues, space and time parity, and observables

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