Dual-comb coherent Raman spectroscopy with lasers of 1-GHz pulse repetition frequency

Mohler, Kathrin J.; Bohn, Bernhard J.; Yan, Ming; Mélen, Gwenaëlle; Hänsch, Theodor W.; Picqué, N.

doi:10.1364/ol.42.000318

Cited by 61 publications

(35 citation statements)

References 34 publications

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“…In fact, if f max is the highest vibrational frequency to be sampled (approximately corresponding to the inverse of the laser pulsewidth), then according to the Nyquist criterion one should have

Δ t = \frac{Δ f_{rep}}{f_{rep}^{2}} \leq \frac{1}{2 f_{\max}}

, so that

Δ f_{rep} \leq \frac{f_{rep}^{2}}{2 f_{\max}}

; this shows that the maximum pixel dwell rate should in principle scale quadratically with the repetition rate of the laser. Recently, Mohler et al . demonstrated dual‐comb CARS using two mode‐locked Ti:sapphire lasers at 1 GHz repetition rate.…”

Section: Broadband Cars Techniquesmentioning

confidence: 99%

Broadband Coherent Raman Scattering Microscopy

Polli

Kumar

Valensise

et al. 2018

Laser & Photonics Reviews

100

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Spontaneous Raman (SR) microscopy allows label-free chemically specific imaging based on the vibrational response of molecules; however, due to the low Raman scattering cross section, it is intrinsically slow. Coherent Raman scattering (CRS) techniques, by coherently exciting all the vibrational oscillators in the focal volume, increase signal levels by several orders of magnitude. In its single-frequency version, CRS microscopy has reached very high imaging speeds, up to the video rate; however, it provides an information which is not sufficient to distinguish spectrally overlapped chemical species within complex heterogeneous systems, such as cells and tissues. Broadband CRS combines the acquisition speed of CRS with the information content of SR, but it is technically very demanding. This paper reviews the current state of the art in broadband CRS microscopy, both in the coherent anti-Stokes Raman scattering (CARS) and the stimulated Raman scattering (SRS) versions. Different technical solutions for broadband CARS and SRS, working both in the frequency and in the time domains, are compared and their merits and drawbacks assessed.2

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Δ t = \frac{Δ f_{rep}}{f_{rep}^{2}} \leq \frac{1}{2 f_{\max}}

, so that

Δ f_{rep} \leq \frac{f_{rep}^{2}}{2 f_{\max}}

Section: Broadband Cars Techniquesmentioning

confidence: 99%

Broadband Coherent Raman Scattering Microscopy

Polli

Kumar

Valensise

et al. 2018

Laser & Photonics Reviews

100

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“…Dual‐comb coherent anti‐Stokes Raman spectroscopy (CARS) circumvents these difficulties by providing a motionless multi‐photon pump–probe scheme, combing high resolution reaching the intrinsic linewidth of Raman transitions, short measurement times down to a few microseconds, high contrast against spectral background due to time and frequency filtering, and simultaneous detection, with a single detector, of a broadband spectrum. This multiheterodyne technique has been refined by further developments respecting rapidness and broad bandwidth possibly covering the entire molecular fingerprint region (400–3300 cm −1 ) . However, detecting molecules in a sensitive manner remains challenging for this rapid dual‐comb method due to its inefficient utilization of comb modes (or teeth) for broadband Raman excitation and the nonlinear nature of coherent Raman spectroscopy (CRS).…”

Section: Introductionmentioning

confidence: 99%

Surface‐Enhanced Dual‐Comb Coherent Raman Spectroscopy with Nanoporous Gold Films

Yan

Zhang

Hao

et al. 2018

Laser & Photonics Reviews

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With two asynchronous frequency combs beating on a single detector, dual‐comb spectroscopy (DCS) enables rapid, broadband, and precise molecular fingerprinting on a comb tooth‐by‐tooth basis and thus holds much promise in molecular sensing. Sensitivity, however, has been an Achilles’ heel of this technique. Here, an approach for ultrasensitive nonlinear DCS based on plasmon‐enhanced coherent Raman spectroscopy (CRS) with ultrathin (100 nm) nanoporous gold films is presented. A high‐resolution (<8 cm−1) Raman spectrum is obtained within 32.8 µs for characterizing low‐density chemicals. The achieved sensitivity enhancement reaches ≈106–8 relative to nonenhanced dual‐comb CRS of liquid samples. The demonstrated approach may open up a new avenue for fast identification of trace amounts of chemicals.

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“…In the recent dual-comb scheme by using 1-GHz frequency oscillators, Mohler and his co-workers reported a refresh rate of 2 kHz, and they also believe that several tens of kHz refresh rate will be within reach with 10-GHz combs in the future [23]. Repetition frequencies above 1-GHz provides a straightforward way to speed up the imaging process, but makes the nonlinear excitation more challenging and necessitates a high-speed and high-sensitivity detector, since the CARS signal scales with the cube of the peak power of the laser pulses.…”

Section: Discussionmentioning

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%

“…Larger repetition frequency difference can lead to increase in refresh rate, but dramatically decrease signal-to-noise ratio (SNR). One solution would be to use combs with larger spacing lines which has been demonstrated very recently with 1-GHz oscillators [23]. The refresh rate is improved in proportion to the repletion rate of laser and the measurement time may get down to 5 μs, while the spectrum has a SNR about one order of magnitude worse than that measured with the 100-MHz system.…”

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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Dual-comb coherent Raman spectroscopy with lasers of 1-GHz pulse repetition frequency

Cited by 61 publications

References 34 publications

Broadband Coherent Raman Scattering Microscopy

Broadband Coherent Raman Scattering Microscopy

Surface‐Enhanced Dual‐Comb Coherent Raman Spectroscopy with Nanoporous Gold Films

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

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