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Quantum 2.0 Conference and Exhibition

Using Kerr Squeezing to Enhance Stimulated Raman Scattering

Nikolay A. Kalinin, Kilian Scheffter, Seungwon Moon, Hanieh Fattahi, Hannah Gallop, Mehdi Alizadeh, Adrian F. Pegoraro, Peter Rose, Mitchel Morrison, Lora Ramunno, Albert Stolow, Luis Lorenzo Sánchez-Soto, Alexey V. Andrianov, Gerd Leuchs

Published Jan 1, 2025• 1 citation
Publisher

Abstract

We report the first quantum enhancement of stimulated Raman scattering using Kerr squeezed light generated by a standard telecom fiber. Applications in biology will benefit from this stable and robust squeezing of intense laser pulses.
DOI
10.1364/quantum.2025.qth2c.3

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Stimulated Raman scattering (SRS) microscopes are a standard technique to image cells, tissues or track the uptake of drugs [1] . The sensitivity in these devices is directly linked to the laser power. While an increase of sensitivity is desired, increasing the laser power is challenging and squeezed light offers a solution to this challenge. Recently squeezed light has been used to enhance the sensitivity of continuous-wave and pulsed SRS [2] , [3] setups and stimulated emission spectroscopy [4] .
In many state-of-the-art stimulated Raman spectroscopy (SRS) experiments, shot noise is the dominating noise source. We apply polarization-squeezed light generated in a silica fiber via the Kerr effect for SRS. The non-classical state of light allows for lowering the noise power below the shot noise limit, which enhances the signal-to-noise ratio (SNR). In our experiment, we achieved 3.0 dB SNR improvement when compared to coherent state SRS. We additionally investigate spectral focusing of squeezed pulses to improve SRS resolution without loss in SNR.
Stimulated Raman spectroscopy has become a powerful tool to study the spatio-dynamics of molecular bonds with high sensitivity, resolution, and speed. However, the sensitivity and speed of stimulated Raman spectroscopy are ultimately limited by the shot-noise of the light beam probing the Raman process. Here, we demonstrate an enhancement of the sensitivity of stimulated Raman spectroscopy by reducing the noise below the shot-noise limit by means of squeezed states of light. Our demonstration constitutes the first step towards a new generation of quantum-enhanced Raman microscopes.
Stimulated Raman spectroscopy has become a powerful tool to study the spatiodynamics of molecular bonds with high sensitivity, resolution, and speed. However, the sensitivity and speed of state-of-the-art stimulated Raman scattering spectroscopy are currently limited by the shot-noise of the light beam probing the Raman process. Here, we demonstrate in a proof-of-principle experiment an enhancement of the sensitivity of continuous-wave stimulated Raman spectroscopy by reducing the quantum noise of the probing light below the shot-noise limit by means of amplitude squeezed states of light. Probing polymer samples with Raman shifts around 2950 c m − 1 with squeezed states, we demonstrate a quantum enhancement of the stimulated Raman signal-to-noise ratio (SNR) of 3.60 dB relative to the shot-noise limited SNR. Our proof-of-concept demonstration of quantum-enhanced continuous-wave Raman spectroscopy paves the way for more elaborate demonstrations using state-of-the-art stimulated Raman scattering microscopes, and thus constitutes the very first step towards a new generation of Raman microscopes, where weak Raman transitions can be imaged without the use of markers or an increase in the total optical power.
Abstract Stimulated Raman scattering (SRS) is a powerful technique for imaging and spectroscopy, in particular in chemistry and biology. By introducing a full quantum description, we determine the ultimate quantum limits of precision and optimal strategies to approach them within the rigorous framework offered by quantum metrology. This approach reveals optimal uses of squeezed states, and the possibility of enhancing the resolution beyond recent experiments. Our work establishes a basis for approaching quantum precision limits in SRS and integrating nonlinear spectroscopy and imaging with emerging quantum technologies.
Stimulated Raman scattering (SRS) microscopy has emerged as a powerful technique for probing the spatiotemporal dynamics of molecular bonds with exceptional sensitivity, resolution, and speed. However, classically, its performance remains fundamentally constrained by optical shot noise, which imposes a strict limit on detection sensitivity and speed. Here, we demonstrate a quantum-enhanced SRS microscopy platform that circumvents this barrier by harnessing amplitude-squeezed light. Specifically, we generate a Stokes beam with 5.2 dB5.2~\mathrm{dB}5.2 dB of amplitude squeezing using traveling-wave optical parametric amplification in second-order nonlinear waveguides, and combine it with a tunable coherent pump to access vibrational modes spanning from 100010001000 to 3100 cm−13100~\mathrm{cm}^{-1}3100 cm−1. Applied to quantum imaging of metabolites in biological tissue (pork muscle), our quantum-enhanced Raman microscope achieves an average noise suppression of 3.6 dB3.6~\mathrm{dB}3.6 dB and a 51%51\%51% enhancement in signal-to-noise ratio (SNR) -- to the best of our knowledge, the largest improvement reported to date in quantum-enhanced SRS microscopy of biological samples.