Broadband long-wavelength upconversion in ultra-short nonlinear crystals.

Since the inception of the second-order nonlinear frequency conversion in 1961, enhancing the inherent low conversion efficiency has been a primary objective. This goal has been successfully accomplished through the utilization of cm-long nonlinear crystals characterized by high quality and nonlinearity, coupled with versatile phase-matching strategies and high-power mixing lasers. However, the reliance on lengthy nonlinear crystals and the necessity for precise phase-matching introduce stringent tolerances on acceptance angles and spectral bandwidths for the interacting fields, thereby constraining its widespread applicability in scientific and industrial domains. This challenge is addressed by combining a broadly tunable ∼5 mW quantum cascade laser operating in the 9.5-12.5 µm range with upconversion detection in ∼100 µm long AGS crystals. Using a tightly focused continuous wave Nd:YVO4 laser with 20 mW output power and spatial filtering of the upconverted beam lead to a SNR of 55 for 50 µs averaging time sufficient for many applications.

Tunable infrared upconversion module for the 1.9 to 5.5 µm range.

In this Letter, an efficient tunable upconversion module is demonstrated and characterized. The module combines high conversion efficiency and low noise with broad continuous tuning, covering the spectroscopically important range from 1.9 to 5.5 µm. A fully computer-controlled, compact, portable system is presented and characterized in terms of efficiency, spectral coverage, and bandwidth, using simple globar illumination. The upconverted signal is in the 700-900 nm range, ideal for Si-based detection systems. The output from the upconversion module is fiber coupled, enabling flexible connection to commercial NIR detectors or NIR spectrometers. In order to cover the spectral range of interest using periodically poled LiNbO3 as the nonlinear material, poling periods ranging from 15 to 23.5 µm are needed. The full spectral coverage is reached using a stack of four fanned poled crystals, enabling maximal upconversion efficiency of any spectral signature of interest in the 1.9 to 5.5 µm range.

Synchronous upconversion of quantum cascade lasers in AgGaS2.

We investigate synchronous upconversion of a pulsed, tunable quantum cascade laser (QCL) in the important 5.4-10.2 µm range, with a 30 kHz, Q-switched, 1064 nm laser. The possibility to accurately control the repetition rate and pulse duration of the QCL results in a good temporal overlap with the Q-switched laser, leading to an upconversion quantum efficiency of 16% in a 10 mm-long AgGaS2 crystal. We investigate the noise properties of the upconversion process in terms of pulse-to-pulse energy stability and timing jitter. For QCL pulses in the 30-70 ns range the upconverted pulse-to-pulse stability is approximately 1.75%. The demonstrated combination of broad tunability and high signal to noise in the system is well-suited for mid-IR spectral analysis of highly absorbing samples.

High-resolution mid-infrared optical coherence tomography with kHz line rate.

We report on mid-infrared optical coherence tomography (OCT) at 4 µm based on collinear sum-frequency upconversion and promote the A-scan scan rate to 3 kHz. We demonstrate the increased imaging speed for two spectral realizations, one providing an axial resolution of 8.6 µm, and one providing a record axial resolution of 5.8 µm. Image performance is evaluated by sub-surface micro-mapping of a plastic glove and real-time monitoring of CO2 in parallel with OCT imaging.

Pulse-to-pulse spectral noise in a spontaneous parametric down conversion light source.

The presence of pronounced chemical signatures of several important molecules and gases in the mid-infrared (mid-IR) spectral region has enabled numerous spectroscopic applications in diverse fields such as environmental monitoring and the life sciences. This has motivated the development of new, efficient light sources and detectors in this spectral region. In this work, we report on the development and characterization of a simple, low-cost, tunable mid-IR light source, covering the 1.45 µm to 3.5 µm spectral region, based on spontaneous parametric down conversion (SPDC) in MgO doped periodically poled lithium niobate (MgO:PPLN). The spectral coverage can be easily extended to 5 µm simply by choosing a crystal with an appropriate poling period. A low repetition rate, passively Q-switched laser provides high-energy pump pulses at 1.03 µm for the SPDC source, resulting in the generation of signal and idler fields. The source is characterized in terms of pulse-to-pulse spectral stability of the generated signal field. Interestingly, a high pulse-to-pulse energy stability does not necessarily lead to high spectral stability. Pulse-to-pulse spectral stability is measured at different pump pulse energies, showing improved spectral stability when operated well above the SPDC threshold.

Upconversion dark-field imaging with extended field of view at video frame rate.

Dark-field imaging is a well-known optical method for obtaining edge-enhanced images of objects containing steep gradients in either amplitude or phase. Edge enhancement is commonly achieved by using a small physical obstruction in the center of the Fourier plane of a 4f imaging setup. By blocking the low spatial frequencies in the center of the Fourier plane, only the higher spatial frequencies from the object reach the image plane. In this work, simultaneous optical image processing (i.e., dark-field imaging) and sum-frequency generation are performed by placing a periodically poled lithium niobate crystal in the Fourier plane of a 4f setup and using a 1575 nm upconversion pump beam with a dark core. We demonstrate upconversion dark-field (UDF) imaging in which edge-enhanced images are obtained at the upconverted wavelength ($\sim{630}\;{\rm nm}$∼630nm) as a result of infrared object illumination ($\sim 1\;\unicode{x00B5}{\rm m}$∼1µm). Furthermore, we experimentally confirm that UDF imaging can be extended from collinear to noncollinear interactions between the signal and pump. The presented system allows for adjustment of the spatial cutoff frequency while maximizing the power conversion efficiency. Simultaneous collinear and noncollinear upconversion imaging of phase objects is demonstrated using broadband 1 µm illumination with a spectral bandwidth of 6 nm-resulting in a UDF imaging system with an enhanced field of view at video frame rates.

Real-time high-resolution mid-infrared optical coherence tomography.

The potential for improving the penetration depth of optical coherence tomography systems by using light sources with longer wavelengths has been known since the inception of the technique in the early 1990s. Nevertheless, the development of mid-infrared optical coherence tomography has long been challenged by the maturity and fidelity of optical components in this spectral region, resulting in slow acquisition, low sensitivity, and poor axial resolution. In this work, a mid-infrared spectral-domain optical coherence tomography system operating at a central wavelength of 4 µm and an axial resolution of 8.6 µm is demonstrated. The system produces two-dimensional cross-sectional images in real time enabled by a high-brightness 0.9- to 4.7-µm mid-infrared supercontinuum source with a pulse repetition rate of 1 MHz for illumination and broadband upconversion of more than 1-µm bandwidth from 3.58-4.63 µm to 820-865 nm, where a standard 800-nm spectrometer can be used for fast detection. The images produced by the mid-infrared system are compared with those delivered by a state-of-the-art ultra-high-resolution near-infrared optical coherence tomography system operating at 1.3 µm, and the potential applications and samples suited for this technology are discussed. In doing so, the first practical mid-infrared optical coherence tomography system is demonstrated, with immediate applications in real-time non-destructive testing for the inspection of defects and thickness measurements in samples that exhibit strong scattering at shorter wavelengths.

Pulsed upconversion imaging of mid-infrared supercontinuum light using an electronically synchronized pump laser.

In this paper, a versatile method for synchronized imaging upconversion in the mid-IR wavelength range is presented. A 1064 nm master oscillator power amplifier source pump laser is electronically adjusted in pulse duration and repetition rate to match the output from a 40 kHz, 1.6 ns pulse mid-IR supercontinuum light source followed by upconversion to the near-infrared captured by a sensitive CCD camera. The systems noise is characterized, and we present a simple algorithm for correcting for the image distortion caused by the use of off-axis parabolic mirrors.

Enhancing the detectivity of an upconversion single-photon detector by spatial filtering of upconverted parametric fluorescence.

Due to advantages of low dark-count rate, reduced dead-time, and room-temperature operation, single-photon upconversion detectors for the telecom band are gaining strong interest as an alternative to other single-photon counters. In this work, we investigate the spatial and spectral distribution of upconverted spontaneous parametric downconversion (USPDC) noise, which is the typical dominant noise source in short-wavelength-pumped single-photon upconversion detectors for 1.5 µm - 1.6 µm. Our upconversion detector relies on a bulk periodically poled lithium niobate (PPLN) crystal and a 1064 nm intracavity pump system that spectrally translates the signal to the visible (~630 nm) where efficient, uncooled, and low dark-count Si based single-photon detectors operate. Experimental results show that the spectral and spatial distribution of the USPDC noise has a relatively broadband and radially modulated pattern that depends on the PPLN temperature, which is in good agreement with our numerical simulations. We also demonstrate that for narrow-linewidth 1575 nm signal photons, the dark-count rate can be significantly reduced by (1) using a phase-matched signal angle that corresponds to an upconverted output angle where the USPDC noise is at a "local minimum" and (2) applying a spatial filter (instead of an ultra-narrow bandpass filter) at the output. This simple spatial filtering technique resulted in a 14 dB dark-count rate reduction. Due to a corresponding decrease in the interaction length of the signal with the pump, the upconversion efficiency also decreased, but only with a 2.2 dB penalty.

Upconversion raster scanning microscope for long-wavelength infrared imaging of breast cancer microcalcifications.

Long-wavelength identification of microcalcifications in breast cancer tissue is demonstrated using a novel upconversion raster scanning microscope. The system consists of quantum cascade lasers (QCL) for illumination and an upconversion system for efficient, high-speed detection using a silicon detector. Absorbance spectra and images of regions of ductal carcinoma in situ (DCIS) from the breast have been acquired using both upconversion and Fourier-transform infrared (FTIR) systems. The spectral images are compared and good agreement is found between the upconversion and the FTIR systems.

Low repetition rate 343 nm passively Q-switched solid-state laser for time-resolved fluorescence spectroscopy.

We demonstrate a low-cost 343 nm solid-state laser delivering up to 20 µJ per pulse, with a pulse width of 2.3 ns at a repetition rate of 100 Hz. The 343 nm is obtained through a third harmonic generation of a passively Q-switched 1030 nm Yb:YAG laser with pulse energy of 190 µJ at 100 Hz and a pulse width of 5.4 ns. The IR-UV conversion efficiency is 10.4%, comparable to that achieved with mode-locked IR lasers. The light source is electronically controlled for easy synchronization with a detection circuit. The low repetition rate specifically targets applications exploiting the millisecond scale lifetime of lanthanides employed in fluoroimmunoassay measurements for time-resolved fluorescence spectroscopy. Low repetition rate and even pulse-on-demand operation is demonstrated.

Electronically delay-tuned upconversion cross-correlator for characterization of mid-infrared pulses.

In this Letter, a novel method for the characterization of mid-infrared pulses is presented. A cross-correlator system, with no moving parts, combining ultra-broadband pulsed upconversion detection with fast active electronic delay tuning was built to perform time-resolved spectral characterization of 1.6 ns mid-infrared supercontinuum pulses. Full wavelength/time spectrograms were acquired in steps of 20 ps over a range that can, in theory, extend to microseconds in a matter of seconds, with 48 ps temporal resolution and 22 cm-1 spectral resolution in the 2700-4300 nm range. This work proves the potential for the use of electronic delay tuning instead of mechanical delay tuning for applications such as cross-correlators and laser spectroscopy, where their fast precise tunability and long delay ranges are a strong asset.

Time-resolved infrared photoluminescence spectroscopy using parametric three-wave mixing with angle-tuned phase matching.

A setup for time-resolved photoluminescence spectroscopy, based on parametric three-wave mixing in a periodically poled lithium niobate crystal, is characterized. Special attention is given to adjusting the phase matching condition by angle tuning of the luminescent light relative to a strong, continuous-wave laser beam within the crystal. The detection system is capable of operating at room temperature and in a wavelength range from 1.55 to 2.20 µm. Its sensitivity is compared to a commercial photomultiplier, and its capability of nanosecond time resolution is demonstrated.

Upconversion detector for range-resolved DIAL measurement of atmospheric CH4.

We demonstrate a robust, compact, portable and efficient upconversion detector (UCD) for a differential absorption lidar (DIAL) system designed for range-resolved methane (CH4) atmospheric sensing. The UCD is built on an intracavity pump system that mixes a 1064 nm pump laser with the lidar backscatter signal at 1646 nm in a 25-mm long periodically poled lithium niobate crystal. The upconverted signal at 646 nm is detected by a photomultiplier tube (PMT). The UCD with a noise equivalent power around 127 fW/Hz1/2 outperforms a conventional InGaAs based avalanche photodetector when both are used for DIAL measurements. Using the UCD, CH4 DIAL measurements have been performed yielding differential absorption optical depths with relative errors of less than 11% at ranges between 3 km and 9 km.

Mid-infrared upconversion based hyperspectral imaging.

Mid-infrared hyperspectral imaging has in the past decade emerged as a promising tool for medical diagnostics. In this work, nonlinear frequency upconversion based hyperspectral imaging in the 6 to 8 µm spectral range is presented for the first time, using both broadband globar and narrowband quantum cascade laser illumination. AgGaS2 is used as the nonlinear medium for sum frequency generation using a 1064 nm mixing laser. Angular scanning of the nonlinear crystal provides broad spectral coverage at every spatial position in the image. This study demonstrates the retrieval of series of monochromatic images acquired by a silicon based CCD camera, using both broadband and narrowband illumination and a comparison is made between the two illumination sources for hyperspectral imaging.

Thermal noise in mid-infrared broadband upconversion detectors.

Low noise detection with state-of-the-art mid-infrared (MIR) detectors (e.g., PbS, PbSe, InSb, HgCdTe) is a primary challenge owing to the intrinsic thermal background radiation of the low bandgap detector material itself. However, researchers have employed frequency upconversion based detectors (UCD), operable at room temperature, as a promising alternative to traditional direct detection schemes. UCD allows for the use of a low noise silicon-CCD/camera to improve the SNR. Using UCD, the noise contributions from the nonlinear material itself should be evaluated in order to estimate the limits of the noise-equivalent power of an UCD system. In this article, we rigorously analyze the optical power generated by frequency upconversion of the intrinsic black-body radiation in the nonlinear material itself due to the crystals residual emissivity, i.e. absorption. The thermal radiation is particularly prominent at the optical absorption edge of the nonlinear material even at room temperature. We consider a conventional periodically poled lithium niobate (PPLN) based MIR-UCD for the investigation. The UCD is designed to cover a broad spectral range, overlapping with the entire absorption edge of the PPLN (3.5 - 5 µm). Finally, an upconverted thermal radiation power of ~30 pW at room temperature (~30°C) and a maximum of ~70 pW at 120°C of the PPLN crystal are measured for a CW mixing beam of power ~60 W, supporting a good quantitative agreement with the theory. The analysis can easily be extended to other popular nonlinear conversion processes including OPO, DFG, and SHG.

High-sensitivity detection of cardiac troponin I with UV LED excitation for use in point-of-care immunoassay.

High-sensitivity cardiac troponin assay development enables determination of biological variation in healthy populations, more accurate interpretation of clinical results and points towards earlier diagnosis and rule-out of acute myocardial infarction. In this paper, we report on preliminary tests of an immunoassay analyzer employing an optimized LED excitation to measure on a standard troponin I and a novel research high-sensitivity troponin I assay. The limit of detection is improved by factor of 5 for standard troponin I and by factor of 3 for a research high-sensitivity troponin I assay, compared to the flash lamp excitation. The obtained limit of detection was 0.22 ng/L measured on plasma with the research high-sensitivity troponin I assay and 1.9 ng/L measured on tris-saline-azide buffer containing bovine serum albumin with the standard troponin I assay. We discuss the optimization of time-resolved detection of lanthanide fluorescence based on the time constants of the system and analyze the background and noise sources in a heterogeneous fluoroimmunoassay. We determine the limiting factors and their impact on the measurement performance. The suggested model can be generally applied to fluoroimmunoassays employing the dry-cup concept.

GHz-bandwidth upconversion detector using a unidirectional ring cavity to reduce multilongitudinal mode pump effects.

We demonstrate efficient upconversion of modulated infrared (IR) signals over a wide bandwidth (up to frequencies in excess of 1 GHz) via cavity-enhanced sum-frequency generation (SFG) in a periodically poled LiNbO3. Intensity modulated IR signal is produced by combining beams from two 1547 nm narrow-linewidth lasers in a fiber coupler while tuning their wavelength difference down to 10 pm or less. The SFG crystal is placed inside an Nd:YVO4 ring cavity that provides 1064 nm circulating pump powers of up to 150 W in unidirectional operation. Measured Fabry-Pérot spectrum at 1064 nm confirms the enhanced spectral stability from multiple to single longitudinal mode pumping condition. We describe analytically and demonstrate experimentally the deleterious effects of using a multimode pump to the high-bandwidth RF spectrum of the 630 nm SFG output. Offering enhanced sensitivity without the need for cooling, the GHz-bandwidth upconverter can readily be extended to the mid-IR (2 - 5 µm) as an alternative to cooled low-bandgap semiconductor detectors for applications such as high-speed free-space optical communications.

Ultra-broadband mid-wave-IR upconversion detection.

In this Letter, we demonstrate efficient room temperature detection of ultra-broadband mid-wave-infrared (MWIR) light with an almost flat response over more than 1200 nm, exploiting an efficient nonlinear upconversion technique. Black-body radiation from a hot soldering iron rod is used as the IR test source. Placing a 20 mm long periodically poled lithium niobate crystal in a compact intra-cavity setup (>20 W CW pump at 1064 nm), MWIR wavelengths ranging from 3.6 to 4.85 µm are upconverted to near-infrared (NIR) wavelengths (820-870 nm). The NIR light is detected using a standard low-noise silicon-based camera/grating spectrometer. The proposed technique allows high conversion efficiency over a wider bandwidth without any need for a shorter crystal length. Different analytical predictions and numerical simulations are performed a priori to support the experimental demonstrations.

Upconversion imaging using short-wave infrared picosecond pulses.

To the best of our knowledge, we present the first demonstration of short-wavelength infrared image upconversion that employs intense picosecond signal and pump beams. We use a fiber laser that emits a signal beam at 1877 nm and a pump beam at 1550 nm-both with a pulse width of 1 ps and a pulse repetition rate of 21.7 MHz. Due to synchronization of high peak-power pulses, efficient upconversion is achieved in a single-pass setup that employs a bulk lithium niobate crystal. Optimizing the temporal overlap of the pulses for high upconversion efficiency enables us to exploit a relatively large pump beam diameter to upconvert a wider range of signal spatial frequencies in the crystal. The 1877 nm signal is converted into 849 nm-enabling an image to be acquired by a silicon CCD camera. The measured size of the smallest resolvable element of this imaging system is consistent with the value predicted by an improved model that considers the combined image blurring effect due to finite pump beam size, thick nonlinear crystal, and polychromatic infrared illumination.