Stimulated Raman scattering spectroscopy with quantum-enhanced balanced detection.

Quantum-enhanced stimulated Raman scattering (QE-SRS) is a promising technique for highly sensitive molecular vibrational imaging and spectroscopy surpassing the shot noise limit. However, the previous demonstrations of QE-SRS utilized rather weak optical power which hinders from competing with the sensitivity of state-of-the-art SRS microscopy and spectroscopy using relatively high-power optical pulses. Here, we demonstrate SRS spectroscopy with quantum-enhanced balanced detection (QE-BD) scheme, which works even when using high-power optical pulses. We used 4-ps pulses to generate pulsed squeezed vacuum at a wavelength of 844 nm with a squeezing level of -3.28 ± 0.12 dB generated from a periodically-poled stoichiometric LiTaO waveguide. The squeezed vacuum was introduced to an SRS spectrometer employing a high-speed spectral scanner to acquire QE-SRS spectrum in the wavenumber range of 2000-2280 cm within 50 ms. Using SRS pump pulses with an average power of 11.3 mW, we successfully obtained QE-SRS spectrum whose SNR was better than classical SRS with balanced-detection by 2.27 dB.