Quantum-enhanced stimulated Raman scattering (QESRS) microscopy is expected to realize molecular vibrational imaging with sub-shot-noise sensitivity, so that weak signals buried in the laser shot noise can be uncovered. Nevertheless, the sensitivity of previous QESRS did not exceed that of state-of-the-art stimulated Raman scattering (SOA-SRS) microscopes mainly because of the low optical power (3 mW) of amplitude squeezed light [Nature 594, 201 (2021)10.1038/s41586-021-03528-w]. Here, we present QESRS based on quantum-enhanced balanced detection (QE-BD). This method allows us to operate QESRS in a high-power regime (>30 mW) that is comparable to SOA-SRS microscopes, at the expense of 3 dB sensitivity drawback due to balanced detection. We demonstrate QESRS imaging with 2.89 dB noise reduction compared with classical balanced detection scheme. The present demonstration confirms that QESRS with QE-BD can work in the high-power regime, and paves the way for breaking the sensitivity of SOA-SRS microscopes.
Compared with visible light, near-infrared (NIR) light has deeper penetration in biological tissues. Three-photon fluorescence microscopy (3PFM) can effectively utilize the NIR excitation to obtain high-contrast images in the deep tissue. However, the weak three-photon fluorescence signals may be not well presented in the traditional fluorescence intensity imaging mode. Fluorescence lifetime of certain probes is insensitive to the intensity of the excitation laser. Moreover, fluorescence lifetime imaging microscopy (FLIM) can detect weak signals by utilizing time-correlated single photon counting (TCSPC) technique. Thus, it would be an improved strategy to combine the 3PFM imaging with the FLIM together. Herein, DCDPP-2TPA, a novel aggregation-induced emission luminogen (AIEgen), was adopted as the fluorescent probes. The three-photon absorption cross-section of the AIEgen, which has a deep-red fluorescence emission, was proved to be large. DCDPP-2TPA nanoparticles were synthesized, and the three-photon fluorescence lifetime of which was measured in water. Moreover, in vivo three-photon fluorescence lifetime microscopic imaging of a craniotomy mouse was conducted via a home-made optical system. High contrast cerebrovascular images of different vertical depths were obtained and the maximum depth was about 600 [Formula: see text]m. Even reaching the depth of 600 [Formula: see text]m, tiny capillary vessels as small as 1.9 [Formula: see text]m could still be distinguished. The three-photon fluorescence lifetimes of the capillaries in some representative images were in accord with that of DCDPP-2TPA nanoparticles in water. A vivid 3D reconstruction was further organized to present a wealth of lifetime information. In the future, the combination strategy of 3PFM and FLIM could be further applied in the brain functional imaging.
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 LiTaO3 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-1 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.
In high-precision optical measurements, squeezed vacuum states are a promising resource for reducing the shot noise. To utilize a squeezed vacuum, it is important to lock the phase of the local oscillator (LO) to the squeezed light. The coherent control sideband (CCSB) scheme has been established for the precise phase locking, while the previous CCSB scheme was designed for the squeezed vacuum generated with an optical parametric oscillator (OPO). Thus the previous CCSB scheme is not applicable to squeezing by a single-pass optical parametric amplifier (OPA), which is attractive for generating broadband squeezed vacuum states. In this study, we propose a variant of CCSB scheme, which is applicable to the squeezing by single-pass OPA. In this scheme, we inject pump light and frequency-shifted signal light into an OPA crystal in the same way as the previous CCSB scheme. The parametric process in the OPA crystal generates a squeezed vacuum, amplifies the signal light, generates an idler light, and causes the pump depletion reflecting the interference of the amplified signal light and the idler light. Through the lock-in detection of the pump depletion, we can phase-lock the injected signal light to the pump light. Then, after the heterodyne detection of the signal and the idler light, we get the error signal of LO and realize the precise phase locking of LO to the squeezed quadrature. We show the feasibility of the proposed scheme by deriving the signal-to-noise ratio (SNR) of the modulated pump signal. We experimentally demonstrate the proposed scheme on pulsed squeezing by a single-pass OPA.
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