Time-Domain Observation of Surface-Enhanced Coherent Raman Scattering with 10<sup>5</sup>–10<sup>6</sup> Enhancement

Kumar, Pardeep; Kuramochi, Hikaru; Takeuchi, Satoshi; Tahara, Tahei

doi:10.1021/acs.jpclett.0c01411

Cited by 13 publications

(16 citation statements)

References 57 publications

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“…TR-SE-ISRS will also be a powerful tool to study plasmon-induced photochemical reactions, which have been attracting extensive attention although their mechanisms have been controversial . In this direction, we recently reported time-domain measurements of surface-enhanced Raman signals and demonstrated that surface-enhanced ISRS (SE-ISRS) can achieve an enhancement factor as high as 10 6 …”

Section: Discussionmentioning

confidence: 99%

“…138 In this direction, we recently reported time-domain measurements of surfaceenhanced Raman signals and demonstrated that surfaceenhanced ISRS (SE-ISRS) can achieve an enhancement factor as high as 10 6 . 139 Extending TR-ISRS to multi-dimensional spectroscopy is another exciting direction. In TR-ISRS, the actinic pump pulse is used primarily to populate the excited state.…”

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confidence: 99%

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Tracking Ultrafast Structural Dynamics by Time-Domain Raman Spectroscopy

Kuramochi

Tahara

2021

J. Am. Chem. Soc.

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In traditional Raman spectroscopy, narrow-band light is irradiated on a sample, and its inelastic scattering, i.e., Raman scattering, is detected. The energy difference between the Raman scattering and the incident light corresponds to the vibrational energy of the molecule, providing the Raman spectrum that contains rich information about the molecular-level properties of the materials. On the other hand, by using ultrashort optical pulses, it is possible to induce Raman-active coherent nuclear motion of the molecule and to observe the molecular vibration in real time. Moreover, this time-domain Raman measurement can be combined with femtosecond photoexcitation, triggering chemical changes, which enables tracking ultrafast structural dynamics in a form of "time-resolved" time-domain Raman spectroscopy, also known as time-resolved impulsive stimulated Raman spectroscopy. With the advent of stable, ultrashort laser pulse sources, time-resolved impulsive stimulated Raman spectroscopy now realizes high sensitivity and a wide detection frequency window from THz to 3000 cm −1 , and has seen success in unveiling the molecular mechanisms underlying the efficient functions of complex molecular systems. In this Perspective, we overview the present status of time-domain Raman spectroscopy, particularly focusing on its application to the study of femtosecond structural dynamics. We first explain the principle and a brief history of time-domain Raman spectroscopy and then describe the apparatus and recent applications to the femtosecond dynamics of complex molecular systems, including proteins, molecular assemblies, and functional materials. We also discuss future directions for time-domain Raman spectroscopy, which has reached a status allowing a wide range of applications.

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Section: Discussionmentioning

confidence: 99%

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confidence: 99%

Tracking Ultrafast Structural Dynamics by Time-Domain Raman Spectroscopy

Kuramochi

Tahara

2021

J. Am. Chem. Soc.

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Section: Sers Substrate In 4d Space and Time Domainsmentioning

confidence: 99%

“…213 In fact, the work combining SERS and coherent nonlinear time-resolved Raman spectroscopy has been reported. Kumar et al 214 combined surfaceenhanced Raman scattering with the coherent nonlinear Raman technique and made it a promising route for achieving higher sensitivity and time-resolved SERS measurements. They also reported time domain Raman measurements of trans-1,2bis(4-pyridyl)ethylene (BPE) adsorbed on Au nanoparticle assemblies, which are carried out with impulsive stimulated Raman spectroscopy using sub-8 fs pulses (Figure 12a).…”

Section: Femtosecond Temporal Resolutionmentioning

confidence: 99%

Dimensional Design for Surface-Enhanced Raman Spectroscopy

Yang

et al. 2022

ACS Mater. Au

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Surface-enhanced Raman spectroscopy (SERS) is a vibrational spectroscopy technique that enables specific identification of target analytes with sensitivity down to the single-molecule level by harnessing metal nanoparticles and nanostructures. Excitation of localized surface plasmon resonance of a nanostructured surface and the associated huge local electric field enhancement lie at the heart of SERS, and things will become better if strong chemical enhancement is also available simultaneously. Thus, the precise control of surface characteristics of enhancing substrates plays a key role in broadening the scope of SERS for scientific purposes and developing SERS into a routine analytical tool. In this review, the development of SERS substrates is outlined with some milestones in the nearly half-century history of SERS. In particular, these substrates are classified into zero-dimensional, one-dimensional, two-dimensional, and three-dimensional substrates according to their geometric dimension. We show that, in each category of SERS substrates, design upon the geometric and composite configuration can be made to achieve an optimized enhancement factor for the Raman signal. We also show that the temporal dimension can be incorporated into SERS by applying femtosecond pulse laser technology, so that the SERS technique can be used not only to identify the chemical structure of molecules but also to uncover the ultrafast dynamics of molecular structural changes. By adopting SERS substrates with the power of four-dimensional spatiotemporal control and design, the ultimate goal of probing the single-molecule chemical structural changes in the femtosecond time scale, watching the chemical reactions in four dimensions, and visualizing the elementary reaction steps in chemistry might be realized in the near future.

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“…Surfaceenhanced CRS was first demonstrated in 1979 where the coherent anti-Stokes Raman scattering (CARS) signal from liquid benzene was amplified with the help of surface plasmon polaritons supported on a flat Ag film antenna [12]. Subsequent progress on surface-enhanced CRS has focused largely on engineering metallic nanoantennas based on Au and Ag to increase and/or optimize the sensitivity of detection [13][14][15][16][17][18][19][20][21][22][23][24][25][26][27]. The quest has seen considerable success and single-molecule sensitivity has been demonstrated by multiple groups [28][29][30][31].…”

Section: Introductionmentioning

confidence: 99%

Enhancement of molecular coherent anti-Stokes Raman scattering with silicon nano-antennas

Abedin,

Li,

Sifat

et al. 2022

Preprint

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Surface-enhanced coherent anti-Stokes Raman scattering (SE-CARS) takes advantage of surface plasmon resonances supported on metallic nanostructures to amplify the coherent Raman response of target molecules. While these metallic antennas have found significant success in SE-CARS studies, photo-induced morphological changes to the nanoantenna under ultrafast excitation introduce significant hurdles in terms of stability and reproducilibty. These hurdles need to be overcome in order to establish SE-CARS as a reliable tool for rapid biomolecular sensing. Here we address this challenge by performing molecular CARS measurements enhanced by nanoantennas made from high-index dielectric particles with more favorable thermal properties. We present the first experimental demonstration of enhanced molecular CARS signals observed at Si nano-antennas, which offer much improved thermal stability compared to their metallic counterparts.

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Time-Domain Observation of Surface-Enhanced Coherent Raman Scattering with 10⁵–10⁶ Enhancement

Cited by 13 publications

References 57 publications

Tracking Ultrafast Structural Dynamics by Time-Domain Raman Spectroscopy

Tracking Ultrafast Structural Dynamics by Time-Domain Raman Spectroscopy

Dimensional Design for Surface-Enhanced Raman Spectroscopy

Enhancement of molecular coherent anti-Stokes Raman scattering with silicon nano-antennas

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Time-Domain Observation of Surface-Enhanced Coherent Raman Scattering with 105–106 Enhancement

Cited by 13 publications

References 57 publications

Tracking Ultrafast Structural Dynamics by Time-Domain Raman Spectroscopy

Tracking Ultrafast Structural Dynamics by Time-Domain Raman Spectroscopy

Dimensional Design for Surface-Enhanced Raman Spectroscopy

Enhancement of molecular coherent anti-Stokes Raman scattering with silicon nano-antennas

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Product

Resources

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Time-Domain Observation of Surface-Enhanced Coherent Raman Scattering with 10⁵–10⁶ Enhancement