We present a new method to study extreme nonlinearities with quantum spectroscopy. Our spectroscopy approach increases the sensitivity to detect nonlinearities by an order of magnitude while remaining robust against experimental noise.
We attract attention to the fact that the ultimate (shot-noise-limited) polarimetric sensitivity can be enhanced by orders of magnitude leaving the photon flux incident onto the photodetector on the same low level. This opportunity is of crucial importance for present-day spin noise spectroscopy, where a direct increase of sensitivity by increasing the probe beam power is strongly restricted by the admissible input power of the broadband photodetectors. The gain in sensitivity is achieved by replacing the 45${}^{\ensuremath{\circ}}$ polarization geometry commonly used in conventional schemes with balanced detectors by geometries with stronger polarization extinction. The efficiency of these high-extinction polarization geometries with enhancement of the detected signal by more than an order of magnitude is demonstrated by measurements of the spin noise spectra of bulk n:GaAs in the spectral range 835--918 nm. It is shown that the inevitable growth of the probe beam power with the sensitivity gain makes spin noise spectroscopy much more perturbative, but, at the same time, opens up fresh opportunities for studying nonlinear interactions of strong light fields with spin ensembles.
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.