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Springer series in optical sciences/SPringer series in optical sciences

Phase-Sensitive Quantum Spectroscopy

Daniel F. Walls, M. D. Reid, P. Zoller, Matthew J. Collett

Published Jan 1, 1985• 0 citations
Publisher
DOI
10.1007/978-3-540-39664-2_78

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Abstract The sensitivity of classical Raman spectroscopy methods, such as coherent anti-stokes Raman spectroscopy (CARS) or stimulated Raman spectroscopy (SRS), is ultimately limited by shot-noise from the stimulating fields. We present the complete theoretical analysis of a squeezing-enhanced version of Raman spectroscopy that overcomes the shot-noise limit of sensitivity with enhancement of the Raman signal and inherent background suppression, while remaining fully compatible with standard Raman spectroscopy methods. By incorporating the Raman sample between two phase-sensitive parametric amplifiers that squeeze the light along orthogonal quadrature axes, the typical intensity measurement of the Raman response is converted into a quantum-limited, super-sensitive estimation of phase. The resonant Raman response in the sample induces a phase shift to signal-idler frequency-pairs within the fingerprint spectrum of the molecule, resulting in amplification of the resonant Raman signal by the squeezing factor of the parametric amplifiers, whereas the non-resonant background is annihilated by destructive interference. Seeding the interferometer with classical coherent light stimulates the Raman signal further without increasing the background, effectively forming squeezing-enhanced versions of CARS and SRS, where the quantum enhancement is achieved on top of the classical stimulation.
Phase-sensitive optical parametric amplification of squeezed states helps to overcome detection loss and noise and thus increases the robustness of sub-shot-noise sensing. Because such techniques, e.g., imaging and spectroscopy, operate with multimode light, multimode amplification is required. Here we find the optimal methods for multimode phase-sensitive amplification and verify them in an experiment where a pumped second-order nonlinear crystal is seeded with a Gaussian coherent beam. Phase-sensitive amplification is obtained by tightly focusing the seed into the crystal, rather than seeding with close-to-plane waves. This suggests that phase-sensitive amplification of sub-shot-noise images should be performed in the near field. A similar recipe can be formulated for the time and frequency, which makes this work relevant for quantum-enhanced spectroscopy.