Two-dimensional infrared spectroscopy of vibrational polaritons of molecules in an optical cavity

Saurabh, Prasoon; Mukamel, Shaul

doi:10.1063/1.4944492

Cited by 61 publications

(62 citation statements)

References 47 publications

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“…Another nonrephasing pathway that is usually difficult to measure is the so-called double-quantum version of 2D IR spectroscopy that is emitted in the k 1 + k 2 − k 3 direction. There has been past 44 and recent 45 interest in this particular implementation of 2D IR due to the ease of measuring vibrational couplings and anharmonicities. This pathway is not usually measured because it further complicates the most common experimental geometries.…”

Section: The 2d Ir Experimentsmentioning

confidence: 99%

Watching Proteins Wiggle: Mapping Structures with Two-Dimensional Infrared Spectroscopy

2017

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Proteins exhibit structural fluctuations over decades of time scales. From the picosecond side chain motions to aggregates that form over the course of minutes, characterizing protein structure over these vast lengths of time is important to understanding their function. In the past 15 years, two-dimensional infrared spectroscopy (2D IR) has been established as a versatile tool that can uniquely probe proteins structures on many time scales. In this review, we present some of the basic principles behind 2D IR and show how they have, and can, impact the field of protein biophysics. We highlight experiments in which 2D IR spectroscopy has provided structural and dynamical data that would be difficult to obtain with more standard structural biology techniques. We also highlight technological developments in 2D IR that continue to expand the scope of scientific problems that can be accessed in the biomedical sciences.

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Section: The 2d Ir Experimentsmentioning

confidence: 99%

Watching Proteins Wiggle: Mapping Structures with Two-Dimensional Infrared Spectroscopy

2017

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“…In parallel, groups pursue the investigation of the influence of the coupling between the different degrees of freedom in polaritonic systems. It is important to consider the vibronic structure to model fluorescence, while the effects of anharmonicity of the vibrational modes are also investigated under the strong coupling regime. The study of the interaction between photons, excitons, and vibrations is useful for understanding luminescence and light‐harvesting complexes .…”

Section: Quantum Mechanical Aspects Of Strong Couplingmentioning

confidence: 99%

“…The quantum coherence of polaritons gives opportunities to control transport properties of materials. For instance, the study of the energy transfers inside matter under the strong coupling regime by 2D infrared spectroscopy for the amide‐I (CO) and amide‐II (CN) vibrations demonstrated that the coupling influences directly the vibrational excitation lifetimes. The vibration lifetimes are also strongly modified in this pump–probe infrared absorption study of the CO group stretching vibration, with additional evidence of coherent energy transfers between the two polaritons provided by the prediction of quantum beats.…”

Section: Strong Coupling Applicationsmentioning

confidence: 99%

Strong Light–Matter Coupling as a New Tool for Molecular and Material Engineering: Quantum Approach

et al. 2018

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When atoms come together and bond, these new states are called molecules and their properties determine many aspects of our daily life. Strangely enough, it is conceivable for light and molecules to bond, creating new hybrid light–matter states with far‐reaching consequences for these strongly coupled materials. Even stranger, there is no “real” light needed to obtain the effects; it simply appears from the vacuum, creating “something from nothing.” Surprisingly, the setup required to create these materials has become moderately straightforward. In its simplest form, one only needs to put a strongly absorbing material at the appropriate place between two mirrors, and quantum magic can appear. Only recently has it been discovered that strong coupling can affect a host of significant effects at a material and molecular level, which were thought to be independent of the “light” environment: phase transitions, conductivity, chemical reactions, etc. This review addresses the fundamentals of this opportunity: the quantum mechanical foundations, the relevant plasmonic and photonic structures, and a description of the various applications, connecting material chemistry with quantum information, entanglement, nonlinear optics, and chemical reactivity. Ultimately, revealing the interplay between light and matter in this new regime opens attractive avenues for various new technologies.

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“…12 Its potential application to molecular cooling, 13,14 as a tool to probe larger molecules, 15,16 to enhance vibrational spectra, [17][18][19][20] for use with electromagnetically induced transparency, 21 and to expedite cavity-modified photo chemistry 22,23 have been objects of intensive studies. Strong cavity coupling in molecular systems has been demonstrated recently for electronic transitions 24 and for vibrational transitions.…”

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confidence: 99%

Cavity Femtochemistry: Manipulating Nonadiabatic Dynamics at Avoided Crossings

Kowalewski

Bennett

Mukamel

2016

J. Phys. Chem. Lett.

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209

331

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Molecular potential energy surfaces can be actively manipulated by light. This is usually done by strong classical laser light but was recently demonstrated for the quantum field in an optical cavity. The photonic vacuum state of a localized cavity mode can be strongly mixed with the molecular degrees of freedom to create hybrid field-matter states known as polaritons. We simulate the avoided crossing of sodium iodide in a cavity by incorporating the quantized cavity field into the nuclear wave packet dynamics calculation. The quantized field is represented on a numerical grid in quadrature space, thus avoiding the limitations set by the rotating wave approximation (RWA) when the field is expanded in Fock space. This approach allows the investigation of cavity couplings in the vicinity of naturally occurring avoided crossings and conical intersections, which is too expensive in the fock space expansion when the RWA does not apply. Numerical results show how the branching ratio between the covalent and ionic dissociation channels can be strongly manipulated by the optical cavity.

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Two-dimensional infrared spectroscopy of vibrational polaritons of molecules in an optical cavity

Cited by 61 publications

References 47 publications

Watching Proteins Wiggle: Mapping Structures with Two-Dimensional Infrared Spectroscopy

Watching Proteins Wiggle: Mapping Structures with Two-Dimensional Infrared Spectroscopy

Strong Light–Matter Coupling as a New Tool for Molecular and Material Engineering: Quantum Approach

Cavity Femtochemistry: Manipulating Nonadiabatic Dynamics at Avoided Crossings

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