Strong Coupling between Surface Plasmon Polaritons and Molecular Vibrations

Memmi, Hala; Benson, Oliver; Sadofev, Sergey; Kalusniak, Sascha

doi:10.1103/physrevlett.118.126802

Cited by 92 publications

(80 citation statements)

References 25 publications

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“…We noted earlier that to couple to such modes with incident light requires some kind of momentum matching. In contrast with the attenuated total reflection technique employed by Memmi et al we made use of grating coupling, a technique previously used with great success by Vasa et al to observe Rabi oscillations associated with excitonic strong coupling . A schematic of the sample structure we used is shown in Figure b.…”

Section: Resultsmentioning

confidence: 99%

“…Strong coupling of vibrational modes was first explored using a planar cavity filled with the polymer polymethyl‐methacrylate (PMMA) where the cavity mode was strongly coupled to the CO vibrational resonance in the polymeric material . Several further investigations have since been reported, involving vibrational resonances in liquids, transition metal complexes, and liquid crystals . Strong coupling of vibrational resonances has also been reported to help catalyze and inhibit chemical reactions and to control the nonlinear optical response in the infrared .…”

Section: Introductionmentioning

confidence: 99%

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Hybridization of Multiple Vibrational Modes via Strong Coupling Using Confined Light Fields

Menghrajani

Fernández

Nash

et al. 2019

Advanced Optical Materials

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to hybridize excitonic resonances associated with two different species. [17,18,15] Hybridization of different vibrational overtones of an excitonic resonance of a single molecular species has also been achieved. [19,20] Meanwhile, in the infrared regime, hybridization of vibrational resonances associated with two distinct molecular species has also been reported recently. [21,22] While hybridization of two different vibrational resonances of a single molecular species to a cavity mode were reported by George et al. [23] Here we present results of experiments that show hybridization of three vibrational resonances of a single mode species to first a cavity mode and second a surface plasmon mode, thereby adding a potentially important component in the strong coupling toolbox, one that may further the degree of control possible over molecular vibrational states in any future polaritonic chemistry.Strong coupling of vibrational modes was first explored using a planar cavity filled with the polymer polymethyl-methacrylate (PMMA) where the cavity mode was strongly coupled to the CO vibrational resonance in the polymeric material. [24,25] Several further investigations have since been reported, [26][27][28][29][30][31][32][33] involving vibrational resonances in liquids, [34] transition metal complexes, [33] and liquid crystals. [35] Strong coupling of vibrational resonances has also been reported to help catalyze and inhibit chemical reactions [36] and to control the nonlinear optical response in the infrared. [37] 2D spectroscopy of molecular vibrations in an optical microcavity has also been explored. [38,39] In the present work, we make use of two different types of confined light field. First we use the well-established planar optical microcavity, second we make use of the surface plasmon mode associated with a single metal surface. Surface plasmons on planar metal films have momenta that cannot be accessed easily by incident light; therefore, we employ grating coupling to overcome this problem, an approach previously explored for strong coupling of excitonic resonances. [40,41] In what follows, we briefly describe the sample structure and material properties. The main probe we use to explore the coupling between vibrational resonances and the optical modes of our confined light fields is to determine the dispersion of the polaritons involved. We describe how these data are acquired and present results from both types of cavity. We then discuss the modeling we have undertaken, both numerical and analytical, before summarizing our findings. Results and DiscussionSchematics of the structures we used are shown in Figure 1. The optical microcavity was based on two gold mirrors 12 nm Strong coupling of molecules placed in an optical microcavity may lead to the formation of hybrid states called polaritons, states that inherit characteristics of both the optical cavity modes and the molecular resonance. This is possible for both excitonic and vibrational molecular resonances. Previous work has shown that strong coupling...

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Hybridization of Multiple Vibrational Modes via Strong Coupling Using Confined Light Fields

Menghrajani

Fernández

Nash

et al. 2019

Advanced Optical Materials

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“…As the evanescent mode is excited on the other surface of the metal layer, any material deposited on the metal will be in close contact with the mode. This geometry was employed for electronic and recently also for vibrational strong coupling …”

Section: Plasmonic–metallic Structures For Scmentioning

confidence: 99%

“…The strong coupling regime generally requires cavities with high‐quality factors

Q_{c} = ω_{c} / γ_{c}

but it is also possible to exploit (SPP) thanks to their strongly localized evanescent electric field, which provides a high DOS in a small volume . This approach has made possible the coupling of excitons with nanoparticle SPP see also the previous section, as well as of molecular vibrations with a metallic film SPP . Although quantum strong coupling has a classical analogue, the purely quantum nature of the polariton states makes them useful for quantum information processing.…”

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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“…As an exact reformulation of the Schrödinger equation, QEDFT can predict exactly correlated electron-photon dynamics in full real-space [14], linking closely with experimental observables. QEDFT has been shown to correctly capture correlated electron-photon systems [15,16], but so far has not been demonstrated for problems in strong vibrationalphoton coupling as observed in recent experiments [1][2][3]. So far, an understanding of vibrational effects in polaritonic chemistry has remained elusive.…”

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confidence: 99%

Cavity-Correlated Electron-Nuclear Dynamics from First Principles

2018

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The rapidly developing and converging fields of polaritonic chemistry and quantum optics necessitate a unified approach to predict strongly correlated light-matter interactions with atomic-scale resolution. Toward this overarching goal, we introduce a general time-dependent density-functional theory to study correlated electron, nuclear, and photon interactions on the same quantized footing. We complement our theoretical formulation with the first ab initio calculation of a correlated electron-nuclear-photon system. For a CO_{2} molecule in an optical cavity, we construct the infrared spectra exhibiting Rabi splitting between the upper and lower polaritonic branches, time-dependent quantum-electrodynamical observables such as the electric displacement field, and observe cavity-modulated molecular motion. Our work opens an important new avenue in introducing ab initio methods to the nascent field of collective strong vibrational light-matter interactions.

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Strong Coupling between Surface Plasmon Polaritons and Molecular Vibrations

Cited by 92 publications

References 25 publications

Hybridization of Multiple Vibrational Modes via Strong Coupling Using Confined Light Fields

Hybridization of Multiple Vibrational Modes via Strong Coupling Using Confined Light Fields

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

Cavity-Correlated Electron-Nuclear Dynamics from First Principles

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