A. Yelisseyev

LiInSe2: A biaxial ternary chalcogenide crystal for nonlinear optical applications in the midinfrared

Single crystals of lithium selenoindate (LiInSe2) are grown by the Bridgman–Stockbarger technique up to sizes of 10 mm in diameter and 20 mm in length. The different phases have color from yellow (as grown) to dark red (after annealing) but all have the same wurtzite type structure mm2 with slightly differing cell parameters. The band gap for the yellow phase at 300 K is at 2.86–2.87 eV. The red color is attributed to point defects and can be removed by proper illumination. Sellmeier equations are constructed for the 0.5–11 μm range and their validity is checked with second harmonic generation which provides first estimations of the nonlinear coefficients of LiInSe2. The potential of LiInSe2 is compared to that of the widely spread and technologically mature AgGaS2.

Optical, vibrational, thermal, electrical, damage, and phase-matching properties of lithium thioindate

Lithium thioindate (LiInS2) is a new nonlinear chalcogenide biaxial material transparent from 0.4 to 12 μm that has been successfully grown in large sizes and with good optical quality. We report on new physical properties that are relevant for laser and nonlinear optics applications. With respect to AgGaS(e)2 ternary chalcopyrite materials, LiInS2 displays a nearly isotropic thermal expansion behavior, a 5-times-larger thermal conductivity associated with high optical damage thresholds, and an extremely low-intensity-dependent absorption, allowing direct high-power downconversion from the near-IR to the deep mid-IR. Continuous-wave difference-frequency generation (5–11 μm) of Ti:sapphire laser sources is reported for the first time to our knowledge.

Optical properties of Nd 3+ - and Tb 3+ -doped KPb 2 Br 5 and RbPb 2 Br 5 with low nonradiative decay

We report on the optical properties of Nd3+- and Tb3+-doped low-phonon-energy moisture-resistant host crystals, potassium lead bromide (KPb2Br5), and rubidium lead bromide (RbPb2Br5), including absorption, emission, and emission lifetime measurements as well as calculations of the multiphonon decay rate, Judd–Ofelt parameters, and radiative transition probabilities for relevant (laser) transitions in these crystals. The RE3+:MPb2Br5 (M=Rb, K) crystal is a promising candidate for long-wavelength infrared applications because of the low phonon frequencies and other favorable features.

Optical, thermal, electrical, damage, and phase-matching properties of lithium selenoindate

Lithium selenoindate (LiInSe2) is a new nonlinear chalcogenide biaxial crystal, related to LiInS2 and transparent from 0.54 to 10 μm at the 50% level (10 mm thickness), which has been successfully grown in large sizes and with good optical quality. We report on what we believe to be new physical properties that are relevant for laser and nonlinear optical applications and summarize all relevant characteristics, both from the literature and as measured in the present work. With respect to AgGaS(e)2 ternary chalcopyrite materials, LiInSe2 displays a nearly isotropic thermal expansion behavior with three- to five-times-larger thermal conductivities associated with high optical damage thresholds, and low intensity-dependent absorption, allowing direct high-power downconversion from the near-infrared, especially 1064 nm, to the deep mid-infrared. Continuous-wave difference-frequency generation (5.9–8.1 μm) of Ti:sapphire laser sources is reported for the first time as well as nanosecond optical parametric oscillation with a Nd:YAG laser as the pump source at 100 Hz and idler tuning between 4.7 and 8.7 μm.

Growth and characterization of LiInS2 single crystals

Bulk LiInS 2 single crystals were grown using the Bridgman}Stockbarger technique. The crystals were characterized in composition, structure and defects. The composition was determined both in average and local versions, the latter was carried out using the unique di!erential dissolution technique. For all crystals a departure from ideal LiInS 2 stoichiometry, especially for cations, was detected. In the optical absorption spectra a strong band at 360 nm which disappears after annealing in S 2 vapor was, with a high probability, related to sulfur vacancies V S : their oscillator strength is f*1.3 * 10~4. The blue photoluminescence in all crystals is likely to be due to In L* antisite defect with an energy level 0.62 eV below the conduction band. The universal values of forbidden band gap, E ’ are 3.72 and 3.57 eV at 80 and 300 K, respectively, for all crystals studied indicating the similar character of dominant bonds. ( 2000 Elsevier Science B.V. All rights reserved.

Pressure-Stimulated Synthesis and Luminescence Properties of Microcrystalline (Lu,Y)3Al5O12:Ce3+ Garnet Phosphors

The Lu2.98Ce0.01Y0.01Al5O12 and Y2.99Ce0.01Al5O12 phosphors were synthesized by solid state reaction at temperature 1623 K and pressure 1.5 × 10(7) Pa in (95% N2 + 5% H2) atmosphere. Under the conditions, the compounds crystallize in the form of isolated euhedral partly faceted microcrystals ∼19 μm in size. The crystal structures of the Lu2.98Ce0.01Y0.01Al5O12 and Y2.99Ce0.01Al5O12 garnets have been obtained by Rietveld analysis. The photoluminescence (PL) and X-ray excited luminescence (XL) spectra obtained at room temperature indicate broad asymmetric bands with maxima near 519 and 540 nm for Y2.99Ce0.01Al5O12 and Lu2.98Ce0.01Y0.01Al5O12, respectively. The light source was fabricated using the powder Lu2.98Ce0.01Y0.01Al5O12 phosphor and commercial blue-emitting n-UV LED chips (λ(ex) = 450 nm). It is found that the CIE chromaticity coordinates are (x = 0.388, y = 0.563) with the warm white light emission correlated color temperature (CCT) of 6400 K and good luminous efficiency of 110 lm/W.

New paramagnetic centres containing nickel ions in diamond

Abstract Electron spin resonance (ESR) and optical spectroscopy were used to investigate synthetic diamonds, obtained by a temperature gradient method. Three new ESR spectra were discovered due to Ni + defects in a divacancy position in the diamond lattice. Their optical analogues are S2 and S3 vibronic systems and the system with a zero phonon line at 523.2 nm, well known for natural diamond. The variety of defects is due to the presence of two or three nitrogen atoms in the nearest coordination sphere of the Ni + ion.

Effect of HPHT annealing on the photoluminescence of synthetic diamonds grown in the Fe-Ni-C system

Abstract The photoluminescence (PL) spectra of synthetic diamonds (SD) containing high concentrations of nitrogen and nickel impurities have been examined in both as-grown samples and the ones annealed at 1950 or 2200 K. A large number of zero-phonon lines (ZPLs), including two tens of vibronic PL systems, have been identified and their behaviour on annealing has been studied, one-third of documented lines have also been observed in natural diamonds. An analysis of their behaviour on annealing allows their division into three main groups, namely: (I) The systems present in as-grown SD, but which disappear after annealing at 1950 K; (II) The systems, which appear after annealing at approximately 1950 K, but their intensity is lower or they disappear completely after annealing at 2200 K; (III) The system, whose intensity increases after annealing at 1950 K and does not decrease after further annealing at 2200 K. A combined optical and ESR study allowed one to identify the systems of group I with individual impurities, whereas the items within group III were associated with nickel–nitrogen complexes containing a single nickel ion in the divacancy position surrounded by a few (n≥2) nitrogen atoms. The systems within group II are related to a relaxed single nickel defect (nickel ion in divacancy position) and simple nickel–nitrogen complexes, containing a single nitrogen atom. The PL excitation spectra were measured for 15 most intense PL systems. A broad absorption band in the annealed SD, with a peak approximately 450 nm and a superimposed fine structure, was decomposed into individual components, related to the NE1, NE2 and NE3 paramagnetic centres. The lower excited states of these three centres are split with ΔE=125 meV, 62 meV and 221 meV, respectively, while the spin-allowed electronic transitions take place only to the upper sublevel.

LiInSe 2 nanosecond optical parametric oscillator

Optical parametric oscillation using the new lithium selenoindate nonlinear crystal is reported for what is to our knowledge the first time. A 17 mm long, type II phase-matched sample is pumped by a 10 ns Nd:YAG laser. The minimum pump energy threshold is 3 mJ for a signal-resonant configuration. The signal and idler waves are tunable between 1.47 and 1.57 microm, and 3.3 and 3.78 microm, with a total output energy of 170 microJ corresponding to a 2.4% energy conversion at 8 mJ pump, only limited by the AR coatings damage. With optimized crystal quality and coatings, lithium selenoindate should show superior performance as compared with AgGaS(e)2 crystals, owing to its 4x larger thermal conductivity.

Nd:YAG pumped nanosecond optical parametric oscillator based on LiInSe2 with tunability extending from 4.7 to 8.7 µm

LiInSe(2) is one of the few (only 5) non-oxide nonlinear optical crystals whose band-gap (2.86 eV) and transparency allowed in the past nanosecond optical parametric oscillation in the mid-IR without two-photon absorption for a pump wavelength of 1064 nm. However, the first such demonstration was limited to the 3.3-3.78 microm range for the idler and the average idler power did not exceed 2.5 mW. Here we report broadly tunable operation, from 4.7 to 8.7 microm, of an OPO based on LiInSe(2), achieving maximum idler pulse energy of 282 microJ at approximately 6.5 microm, at a repetition rate of 100 Hz (approximately 28 mW of average power).