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Fourier-transform infrared spectroscopy (FTIR) is an indispensable analytical method that allows label-free identification of substances via fundamental molecular vibrations. However, the sensitivity of FTIR is often limited by the low efficiency of mid-infrared (MIR) photodetectors. SU(1,1) interferometry has previously enabled FTIR with undetected MIR photons via spontaneous parametric down-conversion in the low-parametric-gain regime, where the number of photons per mode is much less than one and sensitive photodetectors are needed. In this work, we develop a high-parametric-gain SU(1,1) interferometer for MIR-range FTIR with undetected photons. Using our new method, we demonstrate three major advantages: a high photon number at the interferometer output, a considerably lower photon number at the sample, and improved interference contrast. In addition, we analyze different methods to broaden the spectral range of the interferometer by aperiodic poling and temperature gradient in the gain medium. Exploiting the broadband SU(1,1) interferometer, we measure and evaluate the MIR absorption spectra of polymers in the 3-{\mu}m region., Comment: 17 pages, 14 figures

We analyze theoretically and experimentally cases of asymmetric detection, stimulation, and loss within a quantum nonlinear interferometer of entangled pairs. We show that the visibility of the SU(1,1) interference directly discerns between loss on the measured mode (signal) and the conjugated mode (idler). This asymmetry also affects the phase sensitivity of the interferometer, where coherent seeding is shown to mitigate losses that are suffered by the conjugated mode; therefore increasing the maximum threshold of loss that permits sub-shot-noise phase detection. Our findings can improve the performance of setups that rely on direct detection of entangled pairs, such as quantum interferometry and imaging with undetected photons.

In their seminal paper, Caves and Schumaker presented a new formalism for quantum optics, intended to serve as a building block for describing two-photon processes, in terms of new, generalized qudratures. The important, revolutionary concept in their formalism was that it was fundamentally two-mode, i.e. the related observables could not be attributed to any single one of the comprising modes, but rather to a generalized complex quadrature that could only be attributed to both of them. Here, we propose a subtle, but fundamentally meaningful modification to their important work. Unlike the above proposal, we deliberately choose a frequency-agnostic definition of the two-mode quadrature, that we motivate on physical grounds. This simple modification has far-reaching implications to the formalism -- the real and imaginary parts of the quadratures now coincide with the famous EPR variables, and our two-mode operators transform trivially under two-mode and single-mode squeezing operations. Their quadratic forms, which we call the "quadrature power" are shown to succinctly generate the $SU(1,1)$ algebra of squeezing Hamiltonians, and correspond directly to important, broadband physical observables, that have been directly measured in experiment and are explicitly related to properties like squeezing and entanglement. This new point of view gives a fresh perspective on two-mode processes that is completely agnostic to the bandwidth, and reveals intriguing new ways for understanding and measuring broadband two-mode squeezing.

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.

Homodyne measurement is a corner-stone of quantum optics. It measures the fundamental variables of quantum electrodynamics - the quadratures of light, which represent the cosine-wave and sine-wave components of an optical field and constitute the quantum optical analog of position and momentum. Yet, standard homodyne, which is used to measure the quadrature information, suffers from a severe bandwidth limitation: While the bandwidth of optical states can easily span many THz, standard homodyne detection is inherently limited to the electrically accessible, MHz to GHz range, leaving a dramatic gap between the relevant optical phenomena and the measurement capability. We demonstrate a fully parallel optical homodyne measurement across an arbitrary optical bandwidth, effectively lifting this bandwidth limitation completely. Using optical parametric amplification, which amplifies one quadrature while attenuating the other, we measure two-mode quadrature squeezing of 1.7dB below the vacuum level simultaneously across a bandwidth of 55THz, using just one local-oscillator - the pump. As opposed to standard homodyne, our measurement is highly robust to detection inefficiency, and was obtained with $>50\%$ loss in the detection channel. This broadband parametric homodyne measurement opens a wide window for parallel processing of quantum information.