Femtosecond deep-infrared optical parametric oscillator pumped directly by a Ti:sapphire laser

We report a high-repetition-rate femtosecond optical parametric oscillator (OPO) for the deep-infrared (deep-IR) based on the nonlinear optical crystal, CdSiP2 (CSP), pumped directly by a Ti:sapphire laser, for the first time. By pumping CSP at <1 μm, we have achieved practical output powers at the longest wavelengths generated by any Ti:sapphire-pumped OPO. Using a combination of pump wavelength tuning, type-I critical phase-matching, and cavity delay tuning, we have generated continuously tunable radiation across 6654−8373 nm (1194−1503 cm-1) at 80.5 MHz repetition rate, providing up to 20 mW of average power at 7314 nm and <7 mW beyond 8000 nm, with idler spectra exhibiting bandwidths of 140−180 nm across the tuning range. Moreover, the near-IR signal is tunable across 1127−1192 nm, providing up to 37 mW of average power at 1150 nm. Signal pulses, characterised using intensity autocorrelation, have durations of ∼260–320 fs, with corresponding time-bandwidth product of ∆υ∆τ∼1. The idler and signal output exhibit a TEM00 spatial profile with single-peak Gaussian distribution. With an equivalent spectral brightness of ∼6.68×1020 photons s-1 mm-2 sr-1 0.1% BW-1, this OPO represents a viable table-top alternative to synchrotron and supercontinuum sources for deep-IR applications in spectroscopy, metrology and medical diagnostics.Peer ReviewedPostprint (author's final draft

Narrowband, mid-infrared, seeded optical parametric generator based on non-critical CdSiP2 pumped by 120-ps, single longitudinal mode 1,064 nm pulses

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Intrinsic Point Defects (Vacancies and Antisites) in CdGeP\u3csub\u3e2\u3c/sub\u3e Crystals

Cadmium germanium diphosphide (CdGeP2) crystals, with versatile terahertz-generating properties, belong to the chalcopyrite family of nonlinear optical materials. Other widely investigated members of this family are ZnGeP2 and CdSiP2. The room-temperature absorption edge of CdGeP2 is near 1.72 eV (720 nm). Cadmium vacancies, phosphorous vacancies, and germanium-on-cadmium antisites are present in as-grown CdGeP2 crystals. These unintentional intrinsic point defects are best studied below room temperature with electron paramagnetic resonance (EPR) and optical absorption. Prior to exposure to light, the defects are in charge states that have no unpaired spins. Illuminating a CdGeP2 crystal with 700 or 850 nm light while being held below 120 K produces singly ionized acceptors (VCd−) and singly ionized donors (GeCd+), as electrons move from VCd2− vacancies to GeCd2+ antisites. These defects become thermally unstable and return to their doubly ionized charge states in the 150–190 K range. In contrast, neutral phosphorous vacancies (VP0) are only produced with near-band-edge light when the crystal is held near or below 18 K. The VP0 donors are unstable at these lower temperatures and return to the singly ionized VP+ charge state when the light is removed. Spin-Hamiltonian parameters for the VCd− acceptors and VP0 donors are extracted from the angular dependence of their EPR spectra. Exposure at low-temperature to near-band-edge light also introduces broad optical absorption bands peaking near 756 and 1050 nm. A consistent picture of intrinsic defects in II-IV-P2 chalcopyrites emerges when the present CdGeP2 results are combined with earlier results from ZnGeP2, ZnSiP2, and CdSiP2

Identification of Native Defects (Vacancies and Antisites) in CdSiP2 Crystals

Electron paramagnetic resonance (EPR) is used to identify four native defects in single crystals of CdSiP2. This nonlinear optical material is used in optical parametric oscillators to generate tunable output in the mid-infrared. The performance of these frequency-conversion devices is limited when infrared absorption bands associated with native defects overlap a pump wavelength. Cadmium, silicon, and phosphorus vacancies and also silicon-on-cadmium antisites are present in the as-grown undoped CdSiP2 crystals. Using near-band-edge 632.8 nm light from a He-Ne laser, a paramagnetic charge state, and thus an EPR spectrum, is formed at liquid-helium temperatures for three of the four defects. The EPR spectrum from the singly ionized silicon vacancy (V-Si) is present without light and has five hyperfine lines due to equal interactions with the four neighboring 31P nuclei. In contrast, the photoinduced EPR spectrum from the singly ionized cadmium vacancy (V-Cd) has a three-line hyperfine pattern due to equal interactions with only two of its four neighboring 31P nuclei. The light-induced spectrum from the singly ionized silicon-on-cadmium antisite (Si+Cd) also has a three-line hyperfine pattern, thus indicating that the unpaired spin interacts primarily with only two 31P neighbors. For the neutral phosphorus vacancy (V0P), the unpaired spin is primarily localized on the nearest-neighbor silicon ions and the photoinduced EPR spectrum has no resolved 31P hyperfine interactions. The silicon and cadmium vacancies are acceptors, and the silicon-on-cadmium antisite and the phosphorus vacancy are donors

Defect-related Optical Absorption Bands in CdSiP\u3csub\u3e2\u3c/sub\u3e Crystals

When used as optical parametric oscillators, CdSiP2 crystals generate tunable output in the mid-infrared. Their performance, however, is often limited by unwanted optical absorption bands that overlap the pump wavelengths. A broad defect-related optical absorption band peaking near 800 nm, with a shoulder near 1 µm, can be photoinduced at room temperature in many CdSiP2 crystals. This absorption band is efficiently produced with 633 nm laser light and decays with a lifetime of ∼0.5 s after removal of the excitation light. The 800 nm band is accompanied by a less intense absorption band peaking near 1.90 µm. Data from eight CdSiP2crystals grown at different times show that the singly ionized silicon vacancy (V-Si) is responsible for the photoinduced absorption bands. Electron paramagnetic resonance (EPR) is used to identify and directly monitor these silicon vacancies. © 2017 Optical Society of Americ

Deep Selenium Donors in ZnGeP\u3csub\u3e2\u3c/sub\u3e Crystals: An Electron Paramagnetic Resonance Study of a Nonlinear Optical Material

Zinc germanium diphosphide (ZnGeP2) is a ternary semiconductor best known for its nonlinear optical properties. A primary application is optical parametric oscillators operating in the mid-infrared region. Controlled donor doping provides a method to minimize the acceptor-related absorption bands that limit the output power of these devices. In the present study, a ZnGeP2 crystal is doped with selenium during growth. Selenium substitutes for phosphorus and serves as a deep donor. Significant concentrations of native defects (zinc vacancies, germanium-on-zinc antisites, and phosphorous vacancies) are also present in the crystal. Electron paramagnetic resonance (EPR) is used to establish the atomic-level model for the neutral charge state of the selenium donor. The S = 1/2 signal from the neutral donors is produced at 6 K by illuminating with 633 nm light (electrons excited from doubly ionized Zn vacancies convert Se+p donors to Se0p donors). A g matrix, with principal values of 2.088, 2.203, and 1.904, is extracted from the angular dependence of the EPR spectrum. The principal-axis direction associated with the 1.904 principal value is close to a Se–Ge bond. This indicates an asymmetric distribution of unpaired spin density around the selenium ion and thus predicts the deep donor behavior

Optically Active Selenium Vacancies in BaGa\u3csub\u3e4\u3c/sub\u3eSe\u3csub\u3e7\u3c/sub\u3e Crystals

Barium gallium selenide (BaGa4Se7) is a recently developed nonlinear optical material with a transmission window extending from 470 nm to 17 μm. A primary application of these crystals is the production of tunable mid-infrared laser beams via optical parametric oscillation. Unintentional point defects, such as selenium vacancies, cation vacancies (barium and/or gallium), and trace amounts of transition-metal ions, are present in BaGa4Se7 crystals and may adversely affect device performance. Electron paramagnetic resonance (EPR) and optical absorption are used to identify and characterize these defects. Five distinct EPR spectra, each representing an electron trapped at a selenium vacancy, are observed at low temperature (there are seven crystallographically inequivalent selenium sites in the crystal). One spectrum is stable at room temperature and is present before illumination. The other four are produced at lower temperatures with 532 nm laser light and are thermally unstable at room temperature. Each S = 1/2 singly ionized selenium vacancy has a large, nearly isotropic, hyperfine interaction with 69Ga and 71Ga nuclei at one neighboring Ga site. A significant portion of the unpaired spin resides in a 4s orbital on this adjacent Ga ion and gives principal values of the hyperfine matrices in the 3350–6400 MHz range. Broad photoinduced optical absorption bands in the visible and near-infrared are assigned to the selenium vacancies