Frequency combs present a unique tool for high-precision and rapid molecular spectroscopy. Difference frequency generation (DFG) of near-infrared sources is a common approach to generate passively stabilized mid-infrared combs. However, only little attention has been paid so far to precisely measure the coherence properties of such sources. Here, we investigate these using a Raman-soliton based DFG source driven by an Yb:fiber frequency comb. A heterodyne beat between the second harmonic of the phase-locked DFG comb near 4 µm and a 2 µm Tm:fiber frequency comb locked to the same optical reference is performed. Using this method, we measure the relative phase noise power spectral density of both combs. This results in a sub-Hz relative linewidth between the DFG comb and the Tm:fiber comb. We also introduce a new pump/seed delay locking mechanism based on interferometry for long-term stable intensity noise suppression.
Optical rectification of near-infrared laser pulses generates broadband terahertz radiation in chalcopyrite crystals CdGeP2, ZnGeP2 and CdSiP2. The emission is characterized using linear-polarized excitation from 0.8 eV to 1.55 eV (1550 nm - 800 nm). All three crystals are (110)-cut and polished to 0.5 mm, thinner than the coherence length across most of the excitation photon energy range, such that they all produce a bandwidth ~2.5 THz when excited with ~100 fs pulses. It is found that CdGeP2 produced the strongest emission at telecoms wavelengths, while CdSiP2 is generally the strongest source. Pump-intensity dependence provides the nonlinear coefficients for each crystal.
Spectroscopy in the wavelength range from 2 to 11 µm (900 to 5000 cm-1) implies a multitude of applications in fundamental physics, chemistry, as well as environmental and life sciences. The related vibrational transitions, which all infrared-active small molecules, the most common functional groups, as well as biomolecules like proteins, lipids, nucleic acids, and carbohydrates exhibit, reveal information about molecular structure and composition. However, light sources and detectors in the mid-infrared have been inferior to those in the visible or near-infrared, in terms of power, bandwidth, and sensitivity, severely limiting the performance of infrared experimental techniques. This article demonstrates the generation of femtosecond radiation with up to 5 W at 4.1 µm and 1.3 W at 8.5 µm, corresponding to an order-of-magnitude average power increase for ultrafast light sources operating at wavelengths longer than 5 µm. The presented concept is based on power-scalable near-infrared lasers emitting at a wavelength near 1 µm, which pump optical parametric amplifiers. In addition, both wavelength tunability and supercontinuum generation are reported, resulting in spectral coverage from 1.6 to 10.2 µm with power densities exceeding state-of-the-art synchrotron sources over the entire range. The flexible frequency conversion scheme is highly attractive for both up-conversion and frequency comb spectroscopy, as well as for a variety of time-domain applications.
Continuous-wave (cw) optical parametric oscillators (OPOs) are ideally suited for applications, for example high-resolution spectroscopy, that need coherent sources combining narrow-linewidth emission with good wavelength tunability. Here, we demonstrate for the first time cw OPOs based on a millimeter-sized whispering gallery resonator (WGR) made of cadmium silicon phosphide (CdSiP2). By employing a compact laser diode at 1.57-µm wavelength for pumping, a cw OPO with wavelength tunability from 2.3 µm to 5.1 µm is realized based on such a resonator. The oscillation thresholds are in the milliwatt range. The maximum total power conversion efficiency reaches more than 15%. The intrinsic quality factor at 1.57 µm is determined to be 3.5 × 106. This work suggests that CdSiP2 is a very promising alternative for constructing mid-infrared parametric devices.
We describe a compact and efficient mid-infrared (mid-IR) source based on zinc germanium phosphide (ZGP) and cadmium silicon phosphide (CSP) optical parametric oscillators (OPOs), operating in near degenerate condition, directly pumped by a 1.94 µm thulium (Tm)-doped yttrium-aluminum-perovskite (YAP) laser. The Tm:YAP laser is passively Q-switched by a chromium-doped zinc sulfide saturable absorber, and is operated to 4 W average power with a peak power of 29 kW. The laser emission was used to pump CSP and ZGP doubly resonant linear OPO cavities, generating a maximum 3.5-4.2 µm mid-IR emission of 2.5 W for CSP and 2.3 W for ZGP, with maximum optical conversion efficiencies of 65% and 58%, respectively, achieved for the two OPO crystals.
We report the first, to the best of our knowledge, femtosecond-laser-pumped optical parametric oscillator (OPO) based on the newly developed nonlinear crystal, CdSiP2. The OPO was synchronously pumped by a mode-locked Yb:KYW/Yb:fiber master-oscillator power amplifier, providing 1.053 µm pump pulses with durations of 130 fs at a repetition rate of 100 MHz. The 0.5-mm-thick CdSiP2 crystal was cut for a type-I noncritical interaction, providing a broad phase-matching bandwidth and ensuring excellent temporal overlap among the pump, signal, and idler pulses. The OPO generated signal pulses with a spectral coverage over 1260-1310 nm and mid-infrared idler pulses with a broad spectral coverage at 5.8-6.6 µm (6.2 THz). With a 2% output coupler (OC), the threshold pump power was 600 mW. At the maximum pump power of 1.6 W, 0.55 W was absorbed due to two-photon absorption and residual linear absorption in the CdSiP2 crystal, 0.75 W was transmitted, and 53 mW signal power was extracted through the OC. We estimate that the generated idler power was 24 mW.
Low-threshold, efficient optical parametric generation at ~4.64 µm is demonstrated using CdSiP2 nonlinear crystal pumped by 150 ps Raman shifted pump pulses at 1198 nm in noncritical configuration at 1 kHz repetition rate. Maximum single pulse idler energy of 6 µJ and total conversion efficiency of 30% are achieved. Seeding at the signal wavelength with a distributed feedback laser diode enables ~25 fold narrowing of the bandwidths down to ~10 GHz, resulting in a Fourier product of ~1 for the ~100 ps long signal (1615 nm) and idler (4.64 µm) pulses.
Low-threshold, efficient optical parametric generation at ~6100 nm is demonstrated using CdSiP2 nonlinear crystal at 1 to 10 kHz repetition rates with relatively long 500 ps pump pulses at 1064 nm. Maximum single pulse energy of 8.7 µJ and average power of 79 mW are achieved for the idler. Seeding at the signal wavelength is employed using a distributed feedback laser diode, which enables approximately tenfold narrowing of the idler bandwidth down to less than 1 nm.
A 21.4 mm long noncritically cut CdSiP2 crystal, pumped by 8 ns pulses at 1064 nm in a double-pass configuration for pump, signal, and idler, generated 523 µJ, 5.8 ns idler pulses at 6.125 µm. The average power of 52.3 mW at the repetition rate of 100 Hz is the highest ever achieved at such wavelengths with direct down conversion from the 1 µm spectral range.
We directly measured the second harmonic generation and difference frequency generation phase-matching directions of the nonlinear crystal CdSiP(2) until 9.5 µm using the sphere method. The simultaneous fit of the experimental angular data allowed the Sellmeier equations of the ordinary and extraordinary principal refractive indices to be refined over the entire transparency range of the crystal.
Operation of an optical parametric oscillator based on CdSiP(2) and pumped at 1064 nm is demonstrated at a repetition rate of 1 kHz. The maximum output idler energy of 24 microJ at 6.125 microm corresponds to an average power of 24 mW. Increasing the crystal temperature up to 150 degrees in the noncritical (90 degrees) configuration leads to idler wavelength tuning from 6.117 to 6.554 microm. Subnanosecond pulse durations are obtained for the signal and idler as a result of the 1 ns pulse duration of the pump, made possible by the rather short crystal and cavity lengths (approximately 1 cm).
The recently developed chalcopyrite CdSiP(2) is employed in a picosecond, 90 degrees -phase-matched, synchronously pumped, optical parametric oscillator pumped at 1064 nm to produce steady-state idler pulses near 6.4 microm with an energy as high as 2.8 microJ at 100 MHz, in a train of 2-micros-long macropulses following at a repetition rate of 25 Hz. Without an intracavity etalon, the 12.6-ps-long micropulses have a spectral width of 240 GHz.
CdSiP(2) is employed in a nanosecond, 90 degrees -phase-matched, singly resonant optical parametric oscillator pumped at 1064 nm to produce idler pulses near 6.2 microm with an energy as high as 470 microJ at 10 Hz.
Optical properties and valence band density of states near the Fermi level of high-quality VO(2) thin films have been investigated by mid-infrared reflectometry and hard-UV (hν = 150 eV) photoemission spectroscopy. An exceptionally large change in reflectance from 2 to 94% is found upon the thermally driven metal-insulator transition (MIT). The infrared dispersion spectra of the reflectance across the MIT are presented and evidence for the percolative nature of the MIT is pointed out. The discrepancy between the MIT temperatures defined from the electrical and optical properties is found and its origin is discussed. The manifestation of the MIT is observed in the photoemission spectra of the V 3d levels. The analysis of the changes of the V 3d density of states is done and the top valence band shift upon the MIT is measured to be 0.6 eV.
