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arXiv:2610.10294

Sub-shot-noise mid-infrared photothermal measurements using twin beams

Kazuki Hashimoto, Takuro Ideguchi

physics.opticsquant-phSubmitted Oct 7, 2026• Announced Oct 8, 2026
arXivHTMLPDF

Abstract

Mid-infrared photothermal (MIP) measurement probes refractive-index changes induced by mid-infrared (MIR) absorption using visible or near-infrared light and has recently emerged as a powerful modality for MIR spectro-imaging in the life sciences. Reducing measurement noise allows the probe power to be lowered without compromising the signal-to-noise ratio (SNR), thereby mitigating the risk of sample damage. However, even in the absence of classical noise, the SNR of conventional MIP measurements using a classical coherent probe is fundamentally limited by shot noise. Here, we demonstrate sub-shot-noise MIP measurement using twin beams generated through seeded optical parametric amplification. Balanced detection of the twin beams suppresses the noise by more than 5 dB below the shot-noise level established using a coherent beam. As a proof-of-principle demonstration, we measure the MIP signal from liquid water using balanced twin-beam detection and achieve an SNR enhancement of more than 2 dB over the balanced coherent-beam detection.

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Mid-infrared photothermal (MIP) measurement probes refractive-index changes induced by mid-infrared (MIR) absorption using visible or near-infrared light and has recently emerged as a powerful modality for MIR spectro-imaging in the life sciences. Reducing measurement noise allows the probe power to be lowered without compromising the signal-to-noise ratio (SNR), thereby mitigating the risk of sample damage. However, even in the absence of classical noise, the SNR of conventional MIP measurements using a classical coherent probe is fundamentally limited by shot noise. Here, we demonstrate sub-shot-noise MIP measurement using twin beams generated through seeded optical parametric amplification. Balanced detection of the twin beams suppresses the noise by more than 5 dB below the shot-noise level established using a coherent beam. As a proof-of-principle demonstration, we measure the MIP signal from liquid water using balanced twin-beam detection and achieve an SNR enhancement of more than 2 dB over the balanced coherent-beam detection.
The optical shot-noise limit of a laser beam represents the classical limit in precision and signal to noise ratio achievable in optical sensors and imaging systems. It is known that quantum states of light, such as squeezed light and quantum correlated twin beams can be used to enhance precision and signal to noise ratio to beyond this limit. This promises optical sensors with fundamentally superior performance to the state of the art. While quantum-enhanced signal to noise ratio has been demonstrated with macroscopic powers of squeezed probe beam, demonstrations of quantum enhanced precision have remained at extremely low powers of light (femto-Watts). Here we will give examples where increasing SNR with quantum light is not sufficient to increase precision and we will review proof of principle experiments that have demonstrated sub shot noise precision, including for absorption spectroscopy and imaging. We will also report our efforts to achieve this sub-shot-noise precision performance for transmission measurement with ~0.1mW of average probe power, equating to ~10W peak power in a pulsed experiment. Time permitting, we will discuss how integrated optics and integrated electronics enables 10s GHz bandwidth in the detection of squeezed light, for integrated quantum sensor technology.
Recently, we have observed as much as 7 dB of quantum-noise reduction in the direct difference detection of twin-beam signal and idler outputs from a traveling-wave optical parametric amplifier (OPA).1 The OPA, which consists of a type-II phase-matched KTiOPO4 crystal, is pumped by the second harmonic of a mode-locked and Q-switched Nd:YAG laser. Here we describe an experiment in which we used these twin-beam pulses to improve on the optimal (shot-noise-limited) direct-detection signal-to-noise ratio (SNR) that can be achieved with coherent-state pulses of light of the same peak power.
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.
By exploiting the quantised nature of light, we demonstrate a sub-shot-noise scanning optical transmittance microscope. Our microscope demonstrates, with micron scale resolution, a factor of improvement in precision of 1.76(9) in transmittance estimation gained per probe photon relative to an optimal classical version at the same optical power. This would allow us to observe photosensitive samples with nearly twice the precision,without sacrificing image resolution or increasing optical power to improve signal-to-noise ratio. Our setup uses correlated twin-beams produced by parametric down-conversion, and a hybrid detection scheme comprising photon-counting-based feed-forward and a highly efficient CCD camera.
Quantum-intensity-correlated twin beams of light can be used to measure absorption with precision beyond the classical shot-noise limit. The degree to which this can be achieved with a given estimator is defined by the quality of the twin-beam intensity correlations, which is quantified by the noise reduction factor. We derive an analytical model of twin-beam experiments, incorporating experimental parameters such as the relative detection efficiency of the beams, uncorrelated optical noise, and uncorrelated detector noise. We show that for twin beams without excessive noise, measured correlations can be improved by increasing the detection efficiency of each beam; notwithstanding, this may unbalance detection efficiency. However, for beams with excess intensity or other experimental noise, one should balance detection efficiency, even at the cost of reducing detection efficiency—we specifically define these noise conditions and verify our results with statistical simulation. This has application in design and optimization of absorption spectroscopy and imaging experiments.
Nondegenerate optical parametric oscillators generate above-threshold signal and idler beams that have intensity fluctuations correlated at the quantum level (twin beams). We describe what is to our knowledge the first high-sensitivity spectroscopy experiment using twin beams emitted by a cw optical parametric oscillator: a very weak two-photon absorption signal, in the 10(-7) range, is recorded on the 4S(1/2)-5S(1/2) transition of atomic potassium with a noise background that is reduced by 1.9 dB with respect to the shot-noise limit of the light used in the experiment.