Multimode Vibrational Strong Coupling of Methyl Salicylate to a Fabry–Pérot Microcavity

Takele, Wassie Mersha; Wackenhut, Frank; Piątkowski, Łukasz; Meixner, Alfred J.; Waluk, Jacek

doi:10.1021/acs.jpcb.0c03815

Cited by 20 publications

(17 citation statements)

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“…2c. When the cavity mode was tuned towards the carbonyl stretch resonance, new transitions at 1650 cm À1 and 1710 cm À1 could be observed in the transmission spectrum of the coupled system (red line), which has been described in detail by Takele et al 54 These are the signatures of the vibrational hybrid light-matter states (VP À and VP + ) in MS. The presence of VSC in MS is verified by the polariton anticrossing behaviour as a function of cavity tuning (see Fig.…”

Section: Resultsmentioning

confidence: 61%

“…[32][33][34] In ref. 54, we have used a piezo-based tunable Fabry-Pérot type open microcavity to investigate infrared VSC of organic molecules and Fig. 1b shows the structure of the microcavity used in our experiments.…”

Section: Resultsmentioning

confidence: 99%

“…Open microcavity preparation 54,55 The Ag films, typically 10 nm thick (unless otherwise explicitly stated), were deposited on a CaF 2 substrate by a high vacuum sputter coater (Leica EM MED 020 coating system). The thickness of the metal film was controlled using a quartz microbalance film thickness monitoring system (EM QSG100) as a reference during sputtering.…”

Section: Methodsmentioning

confidence: 99%

“…For the liquid phase samples, benzonitrile (BN) and methyl salicylate (MS), the experiments were realized by coupling the CQO and CRN Raman vibrational mode with the vacuum cavity field of an open IR-microcavity. 54 Additionally, we study the Raman scattering characteristics of a solid PVAc film under VSC. In order to obtain a complete picture of Raman VSC, we utilize different cavity geometries, which were prepared by varying the thickness and sequence of the cavity layers.…”

Section: Introductionmentioning

confidence: 99%

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Scouting for strong light–matter coupling signatures in Raman spectra

Takele

Piątkowski

Wackenhut

et al. 2021

Phys. Chem. Chem. Phys.

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Section: Resultsmentioning

confidence: 61%

Section: Resultsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Scouting for strong light–matter coupling signatures in Raman spectra

Takele

Piątkowski

Wackenhut

et al. 2021

Phys. Chem. Chem. Phys.

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“…Third, it would be interesting to try and measure the Raman signal in an angle-resolved way, so as to better compare the Raman signal with the measured dispersion. Finally, during submission of this paper, Takele et al [52] showed that even in the vibrational strong coupling regime, changes in Raman spectra may result from surface enhancement (SERS) effects and do not necessarily result from strong coupling.…”

Section: Summary and Discussionmentioning

confidence: 94%

Probing Vibrational Strong Coupling of Molecules with Wavelength‐Modulated Raman Spectroscopy

Menghrajani

Chen

Dholakia

et al. 2021

Advanced Optical Materials

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that are shifted from that of the incident laser light. In particular, peaks appear in the spectrum of the scattered light that correspond to vibrational resonances of the molecules/materials of which the sample is composed. These spectral peaks form the characteristic fingerprints of the molecules/materials under investigation; the study of such spectra is known as Raman spectroscopy and has become a well-established and powerful analytic technique. [5] Unfortunately, Raman signals are very weak with cross-sections of order 10 −30 cm 2 for non-resonant Raman and 10 −24 cm 2 for resonant Raman. [6] In many situations, these very weak signals are swamped by light produced by other processes, notably fluorescence, which can be many orders of magnitude stronger than the Raman signal. Background fluorescence is particularly problematic when the samples to be investigated are dyes/pigments, [3] for example, resonant Raman, [6] and also when they involve metals. [7] In both cases, fluorescence can be so significant as to mask the desired Raman signals.Various approaches have been adopted to try and deal with the background problem, [8,9] and they fall into three broad categories. First, post-processing can be used to try and subtract the background. [10,11] Although appealing and commonly used, this approach has its drawbacks, especially in that it does not overcome the problem of noise in the background signal. Second, one can move to the time-domain. Raman scattering is an instantaneous process, whereas fluorescence occurs over a protracted time-scale; however, this approach comes at a very significant increase in complexity. [12] Third, a differential approach can be adopted. Here, the idea is to modify the way the data are acquired so as to directly filter out the background and its associated noise. A number of such approaches have been successfully deployed. One technique is based on acquiring spectra for slightly different grating settings in the spectrometer. [7] Another approach is to subtract two Raman spectra obtained with different polarization configurations. [13] Then, there are techniques that make use of the fact that if the pump wavelength is shifted the Raman peaks will also move in wavelength, but the fluorescence will not. Spectra acquired at two or more closely spaced pump wavelengths can thus be processed to provide a differential signal that largely eliminates the background; [14] this technique is known as shifted excitation Raman difference spectroscopy (SERDS). We make use of one variant of this approach here, that of wavelength-modulated Raman spectroscopy (WMRS). WMRS [15] is a significant improvement on Raman spectroscopy is a powerful technique that enables fingerprinting of materials, molecules, and chemical environments by probing vibrational resonances. In many applications, the desired Raman signals are masked by fluorescence, either from the molecular system being studied, or from adjacent metallic nanostructures. Here, it is shown that wavelength-modulated Raman spectroscopy provides...

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The Rise and Current Status of Polaritonic Photochemistry and Photophysics

Bhuyan,

Mony,

Kotov

et al. 2023

Chem. Rev.

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The interaction between molecular electronic transitions and electromagnetic fields can be enlarged to the point where distinct hybrid light–matter states, polaritons, emerge. The photonic contribution to these states results in increased complexity as well as an opening to modify the photophysics and photochemistry beyond what normally can be seen in organic molecules. It is today evident that polaritons offer opportunities for molecular photochemistry and photophysics, which has caused an ever-rising interest in the field. Focusing on the experimental landmarks, this review takes its reader from the advent of the field of polaritonic chemistry, over the split into polariton chemistry and photochemistry, to present day status within polaritonic photochemistry and photophysics. To introduce the field, the review starts with a general description of light–matter interactions, how to enhance these, and what characterizes the coupling strength. Then the photochemistry and photophysics of strongly coupled systems using Fabry–Perot and plasmonic cavities are described. This is followed by a description of room-temperature Bose–Einstein condensation/polariton lasing in polaritonic systems. The review ends with a discussion on the benefits, limitations, and future developments of strong exciton–photon coupling using organic molecules.

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Multimode Vibrational Strong Coupling of Methyl Salicylate to a Fabry–Pérot Microcavity

Cited by 20 publications

References 56 publications

Scouting for strong light–matter coupling signatures in Raman spectra

Scouting for strong light–matter coupling signatures in Raman spectra

Probing Vibrational Strong Coupling of Molecules with Wavelength‐Modulated Raman Spectroscopy

The Rise and Current Status of Polaritonic Photochemistry and Photophysics

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