Femtosecond Stimulated Raman Spectroscopy

Dietze, D.; Mathies, Richard A.

doi:10.1002/cphc.201600104

Cited by 167 publications

(202 citation statements)

References 175 publications

(554 reference statements)

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“…Thanks to the different temporal and spectral properties of the pulses, femtosecond SRS represents an ideal tool to study structural changes in ultrafast photophysical and photochemical processes, providing both femtosecond time precision and high spectral resolution. [28,[35][36][37] Here we report the application of stimulated resonance Raman scattering (SRRS) on heme-proteins, tuning the RP at wavelengths matching the two dominant electronic transitions in the visible absorption (Soret and Q bands). In particular, we select a heme-protein model for studying the tertiary protein motions, namely, myoglobin (Mb), [38] which possesses the key elements for understanding the molecular cooperativity exhibited by hemoglobin in the transport of oxygen.…”

Section: Introductionmentioning

confidence: 99%

Resonant broadband stimulated Raman scattering in myoglobin

Ferrante

Batignani

Fumero

et al. 2018

J Raman Spectroscopy

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Spontaneous Raman is a well‐established tool to probe molecular vibrations. Under resonant conditions, it is a largely used method for characterizing the structure of heme‐proteins. In recent years, advances in pulsed laser sources allowed to explore vibrational features with complex techniques based on nonlinear optical interactions, among which is stimulated Raman scattering (SRS). Building on its combined spectral–temporal resolutions and high chemical sensitivities, SRS has been largely applied as a probe for ultrafast, time‐resolved studies, as well as an imaging technique in biological systems. By using a frequency tunable, narrowband pump pulse jointly with a femtosecond white light continuum to initiate the SRS process, here we measure the Raman spectrum of a prototypical heme‐protein, namely deoxy myoglobin, under two different electronic resonances. The SRS results are compared with the spontaneous Raman spectra, and the relative advantages, such as the capability of our experimental approach to provide an accurate mapping of Raman excitation profiles, are discussed.

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Section: Introductionmentioning

confidence: 99%

Resonant broadband stimulated Raman scattering in myoglobin

Ferrante

Batignani

Fumero

et al. 2018

J Raman Spectroscopy

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“…Line shape broadening (blue line) and blue-shifting (green line) again mirror the behavior of −∆T /T , but the ∆I/I line shapes are noticeably broader than ∆R/R. Since TSF is sensitive not only to imaginary component, but also the dispersive real component of χ (3) (Equation 15), the resulting lineshapes are intrinsically broader. In general, for the same dephasing rate, the transient-TSF lineshapes are broader than the transienttransmittance and transient-reflectance lineshapes.…”

Section: B Pump-tsf-probe and Tr Spectroscopymentioning

confidence: 82%

“…Most merits of a pump-probe experiment, such as sensitivity and selectivity, are determined by the choice of a specific probe methodology, of which there are many. [1][2][3][4][5][6][7][8][9][10] The development of Coherent Multidimensional Spectroscopy (CMDS) offers promising possibilities for new probes because CMDS methods can have increased selectivity compared to conventional methods. [11][12][13][14][15][16][17] CMDS uses multiple optical interactions to create a multiple quantum coherence within the material whose optical emission is measured.…”

Section: Introductionmentioning

confidence: 99%

“…By preceding a CMDS pulse sequence by a pump, the selectivity of CMDS can be leveraged as a probe in a "pump-CMDS-probe" measurement. [2,3,6,18,19] In this paper we introduce triple sum-frequency (TSF) spectroscopy as a new probe for material systems by measuring the pump-induced TSF response of model semiconductor systems: transition metal dichalcogenides (TMDCs).…”

Section: Introductionmentioning

confidence: 99%

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Triple sum frequency pump-probe spectroscopy of transition metal dichalcogenides

Morrow¹,

Kohler²,

Zhao³

et al. 2019

Phys. Rev. B

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Triple sum-frequency (TSF) spectroscopy measures multidimensional spectra by resonantly exciting multiple quantum coherences of vibrational and electronic states. In this work we demonstrate pump-TSF-probe spectroscopy in which a pump excites a sample and some time later three additional electric fields generate a probe field which is measured. We demonstrate pump-TSF-probe spectroscopy on polycrystalline, smooth, thin films and spiral nanostructures of both MoS2 and WS2. The pump-TSF-probe spectra are qualitatively similar to the more conventional transient-reflectance spectra. While transient-reflectance sensitivity suffers under low surface coverage, pump-TSF-probe sensitivity is independent of the sample coverage and nanostructure morphologies. Our results demonstrate that pump-TSF-probe is a valuable methodology for studying microscopic material systems.

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“…Raman spectroscopy is a powerful technique for revealing intrinsic local chemical information in different types of systems, and is important in physics, material science, chemistry, biology, and medicine [1][2][3][4][5][6][7][8][9][10][11]. As spontaneous Raman signal is inherently weak, different types of Raman spectroscopy have been proposed and developed, such as surface-enhanced [12][13][14][15], tip-enhanced [16,17], femtosecond-stimulated [18][19][20], femtosecond time-resolved impulsive stimulated [21], polarized [22,23], and shifted excitation [24,25] Raman spectroscopy. Recently, in surface-enhanced Raman spectroscopy (SERS), the so-called 'nanopipette' structures [26,27] and nanoparticles-coated optical fiber-tip probes have garnered significant interest [28][29][30][31].…”

Section: Introductionmentioning

confidence: 99%

Investigation of optical fiber-tip probes for common and ultrafast SERS

et al. 2020

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In this study, we performed a three-dimensional computational experiment on ultrashort pulse propagation in an optical fiber-tip probe that is decorated with gold nanoparticles (NPs) using a constant structure for the probe's dielectric taper and different spatial configurations of the gold nanoparticles. Interestingly, a hot spot with the highest amplitude of the electric field was found not along the same chain of the NPs but between terminal NPs of neighboring chains of NPs at the probe's tip (the amplitude of the electric field in the hot spots between the NPs along the same chain was of the order of 10 1 , while that between terminal NPs of neighboring chains was of the order of 10 3 ). We eventually identified a configuration with only six terminal nanoparticles (Config4) which is characterized by the highest electric field amplitude enhancement and can provide the highest spatial resolution in the SERS interrogation of an object of interest. The ultrashort temporal responses of the hot spots for all configurations exhibited relatively high pulse elongation (relative elongation was greater than 4.3%). At the same time, due to the reflection of the incident pulse and consequent interference, the temporal responses of most hot spots contained several peaks for all configurations except for the optimum Config4. Nonetheless, the ultrashort temporal responses of all hot spots for Config4 were characterized by a single peak but with a relatively large pulse elongation (relative elongation was 234.1%). The results indicate that further examination of this new structure of a nanoparticles-coated optical fiber-tip probe with only six terminal NPs may provide attractive characteristics for its practical applications.

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Femtosecond Stimulated Raman Spectroscopy

Cited by 167 publications

References 175 publications

Resonant broadband stimulated Raman scattering in myoglobin

Resonant broadband stimulated Raman scattering in myoglobin

Triple sum frequency pump-probe spectroscopy of transition metal dichalcogenides

Investigation of optical fiber-tip probes for common and ultrafast SERS

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