Brillouin microscopy, which maps the elastic modulus from the frequency shift of scattered light, has evolved to a faster speed for the investigation of rapid biomechanical changes. Impulsive stimulated Brillouin scattering (ISBS) spectroscopy has the potential to speed up measurement through the resonant amplification interaction from pulsed excitation and time-domain continuous detection. However, significant progress has not been achieved due to the limitation in signal-to-noise ratio (SNR) and the corresponding need for excessive averaging to maintain high spectral precision. Moreover, the limited spatial resolution also hinders its application in mechanical imaging. Here, by scrutinizing the SNR model, we design a high-speed ISBS microscope through multi-parameter optimization including phase, reference power, and acquisition time. Leveraging this, with the further assistance of the Matrix Pencil method for data processing, three-dimensional mechanical images are mapped under multiple contrast mechanisms for a millimeter-scale polydimethylsiloxane pattern immersed in methanol, enabling the identification of these two transparent materials without any contact or labeling. Our experimental results demonstrate the capability to maintain high spectral precision and resolution at a sub-millisecond integration time for one pixel. With a two-order improvement in the speed and a tenfold improvement in the spatial resolution over the state-of-the-art systems, this method makes it possible for ISBS microscopes to sensitively investigate rapid mechanical changes in time and space.

This publisher’s note corrects the funding order in Photon. Res.11, 357 (2023)10.1364/PRJ.473841.

Exploiting the time-resolving ability of ultrafast pulses, Fourier-transform coherent anti-Stokes Raman scattering (FT-CARS) stands out among the coherent Raman spectroscopic techniques for providing high-speed vibrational spectra with high spectral resolution, high Raman intensity, and immunity to nonresonant background. However, the impulsive stimulation nature of FT-CARS imposes heavy demands on the laser source and makes it inherently difficult to monitor high-frequency vibrations. Here, a novel FT-CARS strategy to our knowledge based on interpulse stimulation is proposed to provide more flexible measuring wavenumber region and lighten the requirement on ultrafast pulses. The mechanism of this technique is analyzed theoretically, and simulation is performed to show an orders-of-magnitude improvement of Raman intensity in the high-wavenumber region by the method. Experimentally, an ytterbium-doped fiber laser and photonic crystal fiber-based solitons are employed to provide two ∼100-fs pulses as the pump and Stokes, respectively, and to perform interpulse stimulation FT-CARS without sophisticated dispersion control devices. The high-wavenumber region and upper-part fingerprint region measurements are demonstrated as examples of flexible measurement. Combined with other rapid scanning techniques, such as resonant scanners or a dual-comb scheme, this interpulse stimulation FT-CARS promises to make the fascinating FT-CARS available for any desired wavenumber region, covering many more realistic scenarios for biomedical, pathological, and environmental research.

Resolution and bandwidth are critical for cavity-enhanced dual-comb spectroscopy (CE-DCS). Here, we pioneer an adaptive approach in CE-DCS to improve the broadband as well as the resolution. Postcorrections to dual-comb interferograms adaptively compensate the relative phase jitters of the optical frequency combs and result in both a mode-resolved spectral resolution and a signal-to-noise ratio of 440:1 in 1 s. Meanwhile, an adaptive comb-cavity locking scheme exploits more than 90% of the comb modes, covering 340cm 1 (10 THz) at 6450cm 1. For a single dual-comb interferogram, more than 40,000 comb teeth spaced by 250 MHz are measured in less than 7.5 ms, contributing to a noise equivalent absorption per spectral element of 2×10 10cm 1·Hz 1/2. This adaptive cavity-enhanced dual-comb spectroscopy technique provides an attractive spectroscopic tool that may be utilized in trace-gas sensing, breath and cancer analysis, and engine combustion diagnosis.