Quantum-enhanced continuous-wave stimulated Raman scattering spectroscopy
Rayssa B. de Andrade, Hugo Kerdoncuff, Kirstine Berg-Sørensen, Tobias Gehring, Mikael Lassen, Ulrik L. Andersen
Abstract
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 <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mn>2950</mml:mn> <mml:mspace width="thickmathspace"/> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:msup> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">c</mml:mi> <mml:mi mathvariant="normal">m</mml:mi> </mml:mrow> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mo>−</mml:mo> <mml:mn>1</mml:mn> </mml:mrow> </mml:msup> </mml:mrow> </mml:math> 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.