Delay-Spectral Focusing Dual-Comb Coherent Raman Spectroscopy for Rapid Detection in the High-Wavenumber Region

Rapid multiplex coherent anti-Stokes Raman scattering (CARS) spectroscopy in the high-wavenumber (HW) region shows great advantages in real-time dynamic process visualizations, clinical diagnosis, abundant microplastic assessment, etc. Fourier transform CARS (FT-CARS) improves the acquisition speed of multiplex CARS to the order of tens of kHz, yet typical approaches to utilize the intrinsic coherence of ultrabroadband pulses notably impede the attainable Raman vibrations in the HW region. Here, a novel delay-spectral focusing dual-comb (DC) CARS scheme is proposed for rapid HW Raman detection based on two fiber combs with 100 MHz repetition rates. By combining the particular advantages of DC asynchronous optical sampling and spectral focusing instantaneous single molecular vibration excitation, the Raman spectrum directly maps to DC relative delay, releasing the coherence constraint of excitation sources. Thus, an Er comb and a Yb comb, as pump and Stokes excitation pulses, respectively, flexibly match the Raman vibration in the HW region. Further, a rapid delay focusing method with intracavity electro-optic modulation is applied to actively control the DC relative delay scanning in the Raman shift region of interest. With these efforts, the spectral acquisition rate is improved more than 1000-fold up to 40 000 spectra/s, while keeping spectral resolution (∼10 cm–1) and the signal-to-noise ratio (∼260) stable along with active acquisition rate tuning. Combined with a microfluidic device, high-speed measurement in the HW region of 15 μm microbeads in flow is demonstrated by the system, reaching a high throughput of around 2150 events/s and more than 99% classification consistency. The prospect of rapid acquiring multiplex CARS spectra without the sacrifice of spectral resolution or the need for the coherence of the pulse sources offers huge potential in rapid monitoring circumstances, such as flow cytometry and microspectroscopic imaging in biomedicine.