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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

Non-destructive testing (NDT) is crucial for ensuring product quality and safety across various industries. Conventional methods such as ultrasonic, terahertz, and X-ray imaging have limitations in terms of probe-contact requirement, depth resolution, or radiation risks. Optical coherence tomography (OCT) is a promising alternative to solve these limitations, but it suffers from strong scattering, limiting its penetration depth. Recently, OCT in the mid-infrared (MIR) spectral region has attracted attention with a significantly lower scattering rate than in the near-infrared region. However, the highest reported A-scan rate of MIR-OCT has been 3 kHz, which requires long data acquisition time to take an image, unsatisfying industrial demands for real-time diagnosis. Here, we present a high-speed MIR-OCT system operating in the 3-4 um region that employs the swept-source OCT technique based on time-stretch infrared spectroscopy. By integrating a broadband femtosecond MIR pulsed laser operating at a repetition rate of 50 MHz, we achieved an A-scan rate of 1 MHz with an axial resolution of 11.6 um and a sensitivity of 55 dB. As a proof-of-concept demonstration, we imaged the surface of substrates covered by highly scattering paint coatings. The demonstrated A-scan rate surpasses previous state-of-the-art by more than two orders of magnitude, paving the way for real-time NDT of industrial products, cultural assets, and structures.

Nonlinear interferometry with entangled photons allows for characterizing a sample without detecting the photons interacting with it. This method enables highly sensitive optical sensing in the wavelength regions where efficient detectors are still under development. Recently, nonlinear interferometry has been applied to interferometric measurement techniques with broadband light sources, such as Fourier-transform infrared spectroscopy and infrared optical coherence tomography. However, they were demonstrated with photon pairs produced through spontaneous parametric down-conversion (SPDC) at a low parametric gain, where the average number of photons per mode is much smaller than one. The regime of high-gain SPDC offers several important advantages, such as the amplification of light after its interaction with the sample and a large number of photons per mode at the interferometer output. In this study, we demonstrate broadband spectroscopy and high-resolution optical coherence tomography with undetected photons generated via high-gain SPDC in an aperiodically poled lithium niobate crystal. To prove the principle, we demonstrate reflective Fourier-transform near-infrared spectroscopy with a spectral bandwidth of 17 THz and optical coherence tomography with an axial resolution of 11 {\mu}m., Comment: 23 pages, 14 figures

Raman scattering spectroscopy is widely used as an analytical technique in various fields, but its measurement process tends to be slow due to the low scattering cross-section. In the last decade, various broadband coherent Raman scattering spectroscopy techniques have been developed to address this limitation, achieving a measurement rate of about 100 kSpectra/s. Here, we present a significantly increased measurement rate of 50 MSpectra/s, which is 500 times higher than the previous state-of-the-art, by developing time-stretch coherent Raman scattering spectroscopy. Our newly-developed system, based on a mode-locked Yb fiber laser, enables highly-efficient broadband excitation of molecular vibrations via impulsive stimulated Raman scattering with an ultrashort femtosecond pulse and sensitive time-stretch detection with a picosecond probe pulse at a high repetition rate of the laser. As a proof-of-concept demonstration, we measure broadband coherent Stokes Raman scattering spectra of organic compounds covering the molecular fingerprint region from 200 to 1,200 cm-1. This high-speed broadband vibrational spectroscopy technique holds promise for unprecedented measurements of sub-microsecond dynamics of irreversible phenomena and extremely high-throughput measurements.

High-speed measurement confronts the extreme speed limit when the signal becomes comparable to the noise level. In the context of broadband mid-infrared spectroscopy, state-of-the-art ultrafast Fourier-transform infrared spectrometers, in particular dual-comb spectrometers, have improved the measurement rate up to a few Mspectra/s, which is limited by the signal-to-noise ratio. Time-stretch infrared spectroscopy, an emerging ultrafast frequency-swept mid-infrared spectroscopy technique, has shown a record-high rate of 80 Mspectra/s with an intrinsically higher signal-to-noise ratio than Fourier-transform spectroscopy by more than the square-root of the number of spectral elements. However, it can measure no more than ~30 spectral elements with a low resolution of several cm-1. Here, we significantly increase the measurable number of spectral elements to more than 1,000 by incorporating a nonlinear upconversion process. The one-to-one mapping of a broadband spectrum from the mid-infrared to the near-infrared telecommunication region enables low-loss time-stretching with a single-mode optical fiber and low-noise signal detection with a high-bandwidth photoreceiver. We demonstrate high-resolution mid-infrared spectroscopy of gas-phase methane molecules with a high resolution of 0.017 cm-1. This unprecedentedly high-speed vibrational spectroscopy technique would satisfy various unmet needs in experimental molecular science, e.g., measuring ultrafast dynamics of irreversible phenomena, statistically analyzing a large amount of heterogeneous spectral data, or taking broadband hyperspectral images at a high frame rate.

Broadband mid-infrared (MIR) molecular spectroscopy demands a bright and broadband light source in the molecular fingerprint region. To this end, intra-pulse difference frequency generation (IDFG) has shown excellent properties among various techniques. However, previous IDFG systems have mainly used unconventional long-wavelength 2-${\mu}$m ultrashort pulsed lasers. A few systems have been demonstrated with 1-${\mu}$m lasers, but they use bulky 100-W-class high-power Yb thin-disk lasers. In this work, we demonstrate a simple and robust approach of 1-${\mu}$m-pumped broadband IDFG with a conventional mode-locked Yb-doped fiber laser. We first generate 3.3-W, 12.1-fs ultrashort pulses at 50 MHz by a simple combination of spectral broadening with a short single-mode fiber and pulse compression with chirped mirrors. Then, we use them for pumping a thin orientation-patterned gallium phosphide (OP-GaP) crystal, generating 1.2-mW broadband MIR pulses with the -20-dB bandwidth of 480 cm$^{-1}$ in the fingerprint region (760-1240 cm$^{-1}$, 8.1-13.1 ${\mu}$m). The 1-${\mu}$m-based IDFG system allows for simultaneous generation of ultrashort pulses in the ultraviolet and visible regions, enabling, for example, 100-MHz-level high-repetition-rate vibrational sum-frequency generation spectroscopy or pump-probe spectroscopy.

Epitaxial thin films of REBa2Cu3O7-d (RE123, RE: rare earth) having a high entropy (HE) RE site were successfully fabricated on a SrTiO3 substrate by the pulsed laser deposition method. One to five RE elements are solved at the RE site, which results in an increase in configurational entropy of mixing (dSmix). Through the measurements of critical current density (Jc) by a magnetization and the Bean's model analysis, we found that the Jc of the HE films exceeds an order of 1.0 MA/cm2 under conditions of T < 20 K and H < 7 T. Since the HE effects have a potential to an improvement of irradiation tolerance, the present results encourage further development of HE RE123 superconducting materials for a practical use in the environment with high magnetic fields and irradiation, for example in fusion reactors., Comment: 7 pages, 4 figures

One of the essential goals of molecular spectroscopy is to measure all fundamental molecular vibrations simultaneously. To this end, one needs to measure broadband infrared (IR) absorption and Raman scattering spectra, which provide complementary vibrational information. A recently demonstrated technique called complementary vibrational spectroscopy (CVS) enables simultaneous measurements of IR and Raman spectra with a single device based on a single laser source. However, the spectral coverage was limited to ~1000 cm-1, which partially covers the spectral regions of the fundamental vibrations. In this work, we demonstrate a simple method to expand the spectral bandwidth of the CVS with a cascaded intra-pulse difference-frequency generation (IDFG). Using the system, we measure broadband CVS spectra of organic liquids spanning over 2000 cm-1, more than double the previous study.

Fourier-transform infrared spectroscopy (FTIR) is the golden standard of mid-infrared (MIR) molecular spectroscopic analysis through optically-encoded vibrational signatures. Michelson-type FTIR and MIR dual-comb spectrometers allow us to simultaneously investigate multiple molecular species via the broadband and high-resolution spectroscopic capabilities. However, these are not applicable to high-speed measurements due to the low temporal resolution which is fundamentally limited by the signal-to-noise ratio (SNR). In this study, we develop a high-speed FTIR spectroscopy technique called phase-controlled Fourier-transform infrared spectroscopy (PC-FTIR) that has the capability to measure MIR absorption spectra at a rate of above 10 kHz. PC-FTIR demonstrates the high scan rate with a high SNR for various spectral bandwidths by arbitrarily adjusting the instrumental spectral resolution. As a proof of principle demonstration, we measure high-speed mixing dynamics of two liquids at a rate of 24 kHz. We also measure MIR spectra of gas-phase molecules with higher spectral resolution at a rate of 12 kHz. This high-speed MIR spectrometer could be especially useful for measuring non-repetitive fast phenomena and acquiring a large amount spectral data within a short time.

Nonlinear optical microscopy allows rapid high-resolution microscopy with image contrast generated from intrinsic properties of the sample. Established modalities such as multiphoton excited fluorescence and second/third-harmonic generation can be combined with other nonlinear techniques, such as coherent Raman spectroscopy which typically allow chemical imaging of a single resonant vibrational mode of a sample. Here, we utilize a single ultrafast laser source to obtain broadband coherent Raman spectra on a microscope, together with other nonlinear microscopy approaches on the same instrument. We demonstrate that the coherent Raman modality allows broadband measurement (>1000 cm-1), with high spectral resolution (<5 cm-1), with a rapid spectral acquisition rate (3-12 kHz). This enables Raman hyperspectral imaging of > kilo-pixel images at >11 frames per second.

The spectral resolution of broadband Fourier-transform coherent anti-Stokes Raman spectroscopy is limited by the maximum optical path length difference that can be scanned within a short time in an interferometer. However, alternatives to the Fourier-transform exist which can bypass this limitation with certain assumptions. We apply one such approach to broadband coherent Raman spectroscopy using interferometers with short delay line (low Fourier spectral resolution) and large delay line (high Fourier spectral resolution). With this method, we demonstrate broadband coherent Raman spectroscopy of closely spaced vibrational bands is possible using a short delay line interferometer, with superior spectral resolution to the longer delay line instrument. We discuss how this approach may be particularly useful for more complex Raman spectra, such as those measured from biological samples.

Vibrational spectroscopy, comprised of infrared absorption and Raman scattering spectroscopy, is widely used for label-free optical sensing and imaging in various scientific and industrial fields. The group theory states that the two molecular spectroscopy methods are sensitive to vibrations categorized in different point groups and provide complementary vibrational spectra. Therefore, complete vibrational information cannot be acquired by a single spectroscopic device, which has impeded the full potential of vibrational spectroscopy. Here, we demonstrate simultaneous infrared absorption and Raman scattering spectroscopy that allows us to measure the complete broadband vibrational spectra in the molecular fingerprint region with a single instrument based on an ultrashort pulsed laser. The system is based on dual-modal Fourier-transform spectroscopy enabled by efficient use of nonlinear optical effects. Our proof-of-concept experiment demonstrates rapid, broadband and high spectral resolution measurements of complementary spectra of organic liquids for precise and accurate molecular analysis.

Fourier-transform spectroscopy (FTS) has been widely used as a standard analytical technique over the past half-century. FTS is a simple and robust autocorrelation-based technique that is compatible with both temporally coherent and incoherent light sources, which functions as an active or passive spectrometer. However, this technique has been mostly used for static measurements due to the low scan rate imposed by technological restrictions. This has impeded its application to continuous rapid measurements, which would be of significant interest for a variety of fields, especially when monitoring of non-repeating/transient complex dynamics is desirable. Here, we demonstrate highly efficient FTS operating at a high spectral acquisition rate with a simple delay line based on a dynamic phase-control technique. The independent adjustability of phase and group delays allows us to achieve the Nyquist-limited spectral acquisition rate over 10,000 spectra per second, while maintaining a large spectral bandwidth and high resolution. In addition, we demonstrate the ability of this passive spectrometer working with an incoherent light source.