The phase-controlled Raman effect

Lanin, A. A.; Федотов, И. В.; Федотов, А. Б.; Sidorov‐Biryukov, D. A.; Желтиков, А. М.

doi:10.1038/srep01842

Cited by 9 publications

(11 citation statements)

References 29 publications

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“…Scanning the time delay between the two chirped pulses can selectively populate different vibrational energy levels. This is known as the spectral focusing approach [29], and there have been great efforts establishing and developing of this phase-controlled technique in the past decade [14,[17][18][30][31][32][33][34][35][36].…”

Section: Resultsmentioning

confidence: 99%

“…However, real-time identifying and mapping for multiple or possibly unknown molecules requires broad spectral breadth, desired resolution and high-speed acquisition, and has been a long-term pursuit in the field [5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23].…”

Section: Introductionmentioning

confidence: 99%

“…Parallel-detection based multiplex SRS technique has also been demonstrated at the speed of microsecond scale [12]. In contrast to the parallel-detection technique, modulation multiplexing CARS and SRS techniques use a point detector, thus enabling high sensitivity and speed [13][14][15][16][17][18]. It generally involves a single femtosecond laser and a mechanical motor for stepping the delay, and the latest techniques enabled by a high-speed resonant-scanner line has achieved tens of microseconds acquisition time [19,20,15,17].…”

Section: Introductionmentioning

confidence: 99%

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Spectral focusing dual-comb coherent anti-Stokes Raman spectroscopic imaging

Chen

et al. 2017

Opt. Lett.

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Coherent Raman microscopy provide label-free imaging by interrogating the intrinsic vibration of biomolecules.Nevertheless, trade-off between high chemical-specificity and high imaging-speed currently exists in transition from spectroscopy to spectroscopic imaging when capturing dynamics in complex living systems. Here, we present a novel concept in dual-comb scheme to substantially beat this trade-off and facilitate high-resolution broadband coherent antiStokes Raman spectroscopic imaging based on down-converted, automatically varying delay-time in spectral focusing excitation. A rapid measurement of vibrational microspectroscopy on sub-microsecond scale over a spectral span ~700 cm -1 with solid signal-to-noise ratio provides access to well-resolved molecular signatures within the fingerprint region. We demonstrate this high-performance spectroscopic imaging of spatially inhomogeneous distributions of chemical substances as well as the carotenoids accumulation in plant cells. This technique offers an unprecedented route for broadband CARS imaging with hundreds of kHz frame rate using available 1-GHz oscillators.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Spectral focusing dual-comb coherent anti-Stokes Raman spectroscopic imaging

Chen

et al. 2017

Opt. Lett.

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“…Ultrashort laser pulses inevitably impose limitations on the spectral resolution in nonlinear‐optical microspectroscopy, making it difficult to resolve closely lying and overlapping lines in Raman spectra and to extract the informative signal in the microscopy of multicomponent biological systems. However, the coherence of laser pulses suggests attractive solutions to this problem, allowing the spectral resolution of nonlinear microspectroscopy to be substantially improved by pulse chirping . A linear chirp defines a one‐to‐one map relating the frequency to the delay time τ between the laser pulses.…”

Section: Introduction and Wolfgang Kiefer's Legacymentioning

confidence: 99%

“…A linear chirp defines a one‐to‐one map relating the frequency to the delay time τ between the laser pulses. With this map defined, the spectrum of a Raman‐active mode can be found by measuring the intensity of the nonlinear Raman signal as a function of τ …”

Section: Introduction and Wolfgang Kiefer's Legacymentioning

confidence: 99%

A compact laser platform for nonlinear Raman microspectroscopy: multimodality through broad chirp tunability

Lanin

Stepanov

Tikhonov

et al. 2016

J Raman Spectroscopy

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We demonstrate a compact laser platform that integrates stimulated and coherent Raman microscopy with high-resolution nonlinear Raman spectroscopy. Ultrashort laser pulses with a carefully managed, broadly tunable chirp are shown to enable a comfortable switching between the high-contrast microscopy and high-resolution spectroscopy modalities in both stimulated and coherent versions of nonlinear Raman scattering. Sub-10-cm À1 spectral resolution in stimulated Raman spectroscopy is demonstrated through a careful compensation of nonlinear phase distortions of ultrashort laser pulses. This offers a powerful tool for a reliable identification of molecular vibrations with close frequencies, enhancing the chemical selectivity of spectroscopic analysis of complex multicomponent systems. Introduction and Wolfgang Kiefer's legacyHigh-resolution spectroscopic analysis and ultrafast, short-pulse interrogation are the two main modalities of optical technologies based on nonlinear Raman scattering. [1,2] While high-resolution Raman spectroscopy [3,4] requires narrowband probes, capable of resolving individual molecular or atomic features in often crowded Raman spectra of complex chemical systems, broadband, shortpulse drivers offer a vast arsenal of tools [5,6] for time-resolved studies of ultrafast dynamics in physical, chemical, and biological systems [1,2,7] and open a whole new world of chemically specific, high-speed nonlinear microscopy. [8][9][10] The requirements on laser fields needed to implement these modalities are seemingly incompatible.Wolfgang Kiefer, one of the pioneers of the field of Raman spectroscopy, whose work had a profound impact on the field and who prominently contributed to the development of high-spectralresolution Raman methods, [11,12] was also among the first visionary scientists who recognized the tremendous potential of emerging short-pulse laser sources for Raman technologies. [13][14][15] This vision has in many ways shaped the future of the field. Within the past two decades, nonlinear Raman processes driven by ultrashort pulses have played a central role in ultrafast science, providing methods that help to probe [16,17] and control [18][19][20][21] ultrafast processes on the picosecond, femtosecond, and attosecond time scale, [22] as well as open new horizons in standoff detection [23,24] and ultrashort waveform synthesis. [25,26] With a powerful impetus gained from the invention of nonlinear Raman microscopy, [8,27] short-pulse Raman techniques find growing applications in bioimaging, enabling a chemically selective, high-frame-rate detection of intracellular dynamics, [28] diagnostics of lipid membranes, [29] and neurophysiological studies. [30][31][32][33][34] Ultrashort laser pulses inevitably impose limitations on the spectral resolution in nonlinear-optical microspectroscopy, making it difficult to resolve closely lying and overlapping lines in Raman spectra and to extract the informative signal in the microscopy of multicomponent biological systems. However, the coherence of laser p...

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Single‐beam dual‐color alternate‐pathway two‐photon spectroscopy: Toward an optical toolbox for redox biology

Chebotarev

Lanin

Raevskii

et al. 2021

J Raman Spectroscopy

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We demonstrate a versatile single-laser platform for single-beam dual-color two-photon spectroscopy that combines a short-pulse laser source with a tunable broadband wavelength converter based on a highly nonlinear photoniccrystal fiber (PCF). We show that the short-pulse PCF output can be tailored, via dispersion and nonlinearity management, to deliver a broadband optical driver whose spectral structure is ideally suited for a single-beam two-photon absorption (2PA) spectroscopy of the next-generation genetically encodable fluorescent-protein (FP) sensors of pH and redox-responsive contrast agents. As a promising spectroscopic resource for redox biology, the short-pulse PCF output can be finely sculpted to alternately drive an FP system via a one of its two 2PA-allowed quantum pathways, yielding a high-contrast fluorescence readout for a highly sensitive detection of redox reactions and signaling, pH sensing, and oxidative-stress diagnosis.

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The phase-controlled Raman effect

Cited by 9 publications

References 29 publications

Spectral focusing dual-comb coherent anti-Stokes Raman spectroscopic imaging

Spectral focusing dual-comb coherent anti-Stokes Raman spectroscopic imaging

A compact laser platform for nonlinear Raman microspectroscopy: multimodality through broad chirp tunability

Single‐beam dual‐color alternate‐pathway two‐photon spectroscopy: Toward an optical toolbox for redox biology

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