We calculate the two-photon absorption for squeezed light pumped by a continuous-wave source, near or far from resonance, beyond the low intensity limit. For typical two-photon absorption parameters, we find no squeezed light enhancement.
We present a theoretical analysis of two-photon absorption of classical and squeezed light valid when one-photon absorption to an intermediate state is either resonant or far-detuned from resonance, and in both the low and high intensity regimes. In this paper we concentrate on continuous-wave excitation, although the approach we develop is more general. We calculate the energy removed from an incident field for typical experimental parameters and consider the limiting cases when the photon pairs are narrowband or broadband compared to the molecular linewidths. We find an enhancement of the two-photon absorption due to resonant contributions from the large squeezed light bandwidth and due to photon bunching in the low intensity regime. However, in both cases, for the parameters we choose, the one-photon absorption is the dominant process in the region of parameter space where a large enhancement of the two-photon absorption is possible.
We apply our quantum theory of multiwave mixing for the two-photon two-level model to the generation of squeezed states of light. Because of the two-photon transition, a larger number of interaction potentials are present compared to one-photon models, leading to effects absent in the one-photon case. The two most significant of these are the appearance of dynamic Stark shifts and conjugate scattering off the pump induced two-photon coherence. We show that this can lead to almost perfect squeezing, even for low pump intensities and low detunings from the two-photon resonance.
Label-free optical microscopy through absorption or scattering spectroscopy provides fundamental insights across biology and materials science, yet its sensitivity remains fundamentally limited by photon shot noise. While recent demonstrations of quantum nonlinear microscopy show sub-shot-limited sensitivity, they are intrinsically limited by availability of high peak-power squeezed light sources. Here, we introduce squeezing-enhanced photothermal (SEPT) microscopy, a quantum imaging technique that leverages twin-beam quantum correlations to detect absorption induced signals with unprecedented sensitivity. SEPT achieves 3.5 dB noise suppression beyond the standard quantum limit, enabling a 2.5-fold increase in imaging throughput or 31% reduction in pump power, while providing an unmatched versatility through the intrinsic compatibility between continuous-wave squeezing and photothermal modulation. We showcase SEPT applications by providing high-precision characterization of nanoparticles and revealing subcellular structures, such as cytochrome c, that remain undetectable under shot-noise-limited imaging. By combining label-free contrast, quantum-enhanced sensitivity, and compatibility with existing microscopy platforms, SEPT establishes a new paradigm for molecular absorption imaging with far-reaching implications in cellular biology, nanoscience, and materials characterization.