Optical Properties of KTP Crystals and Their Potential for Terahertz Generation
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crystals Article Optical Properties of KTP Crystals and Their Potential for Terahertz Generation Alexander Mamrashev 1,* ID , Nazar Nikolaev 1 ID , Valery Antsygin 1, Yury Andreev 2,3, Grigory Lanskii 2,3 and Arkady Meshalkin 4 1 Institute of Automation & Electrometry, SB RAS, 1, Ac. Koptyug Ave., Novosibirsk 630090, Russia; [email protected] (N.N.); [email protected] (V.A.) 2 Institute of Monitoring of Climatic and Ecological Systems, SB RAS, 10/3, Akademicheskii Ave., Tomsk 634055, Russia; [email protected] (Y.A.); [email protected] (G.L.) 3 Siberian Physical Technical Institute of Tomsk State University, 1 Novosobornaya Sq., Tomsk 634050, Russia 4 Institute of Thermophysics, SB RAS, 1, Ac. Lavrent’ev Ave., Novosibirsk 630090, Russia; [email protected] * Correspondence: [email protected]; Tel.: +7-383-330-8378 Received: 30 June 2018; Accepted: 28 July 2018; Published: 31 July 2018 Abstract: High nonlinearity, wide transparency range and optical quality allowed potassium titanyl phosphate (KTiOPO4, KTP) crystals to be used in a wide range of nonlinear applications. The success of KTP usage in the visible and infrared (IR) ranges drives interest in applying it at longer wavelengths, that is, in the terahertz (THz) range. We use THz optical properties of KTP crystals measured by terahertz time-domain spectrometer (THz-TDS) and refractive index approximated in the form of Sellmeier equations to investigate KTP application possibilities for IR-to-THz and THz-to-THz wave conversion. As a result, phase matching for s − f ! f and s − f ! s types of difference frequency generation (DFG) of Ti:Sapphire laser (at the wavelengths of 0.65, 0.8 and 1.1 µm) is found possible, as well as second harmonic generation (SHG) of THz waves by f + s ! f type of interaction in the XZ principle plane of the crystal. Terahertz wave generation by phase-matched parametric processes in KTP demonstrates evident advantages in comparison with that of widely used MgO-doped LiNbO3 crystals. Keywords: KTP; nonlinear crystal; frequency conversion; SHG; DFG; THz radiation; THz wave 1. Introduction Potassium titanyl phosphate (KTiOPO4, KTP) is one of the most widely used nonlinear optical crystals [1]. KTP belongs to the mm2 point group symmetry and its dielectric and crystallographic axes are assigned as X, Y, Z ! a, b, c. Its structure consists of chains of connected rigid PO4 tetrahedra and TiO6 octahedra with alternating long and short Ti–O bonds that are responsible for its nonlinear properties [2]. KTP advantages are high nonlinear coefficients: d15 = 1.9 pm/V, d24 = 4.2 pm/V, d31 = 2.2 pm/V, d32 = 2.7 pm/V and d33 = 17.4 pm/V, wide ranges of angles and temperatures for the phase matching, low absorption in the range of 0.35 µm to 4.5 µm, excellent mechanical stability and optical quality. One of the few KTP disadvantages is its susceptibility to photochromic damage, that is, grey-tracking, that causes slow deterioration of light conversion efficiency. The abovementioned properties of KTP determine its wide range of nonlinear applications such as sum [3] and difference [4,5] frequency generation (SFG and DFG), second harmonic generation (SHG) [6], optical parametric oscillation/generation (OPO/OPG) and amplification (OPA) [7–9]. Parametric generation based on stimulated polariton scattering in KTP shows superior performance in terms of gain and laser damage resistance in comparison to lithium niobate and lithium tantalate [10,11]. Other KTP applications include modulators for the near- and the mid-IR ranges [12–14]. Crystals 2018, 8, 310; doi:10.3390/cryst8080310 www.mdpi.com/journal/crystals Crystals 2018, 8, 310 2 of 8 Crystals 2018, 8, x FOR PEER REVIEW 2 of 8 The successsuccess ofof KTP KTP nonlinear nonlinear applications applications in the in visiblethe visible and IR and ranges IR drivesranges interestdrives ininterest studying in itsstudying terahertz its dielectricterahertz anddielectric optical and (THz) optical properties (THz) topr substituteoperties to the substitute widely usedthe widely pure and used MgO-doped pure and lithiumMgO-doped niobate lithium crystals niobate (LiNbO crystals3, LN) (LiNbO in this3, LN) range in [this15]. range Previously, [15]. Previously, infrared reflectivity infrared reflectivity spectrum ofspectrum KTP was of studiedKTP was up studied to the wavenumberup to the wavenumber of 4000 cm of− 40001 (120 cm THz)−1 (120 at THz) the temperatures at the temperatures of 7 K, 80 of K7 andK, 80 293 K and K [16 293]. Later,K [16]. the Later, results the wereresults supplemented were supplemented by Raman by Raman spectroscopy spectroscopy measurements measurements at the wavenumbersat the wavenumbers below below 4000 cm 4000−1 [cm17].−1 Recently,[17]. Recently, THz refractiveTHz refractive index index and absorption and absorption coefficient coefficient were directlywere directly measured measured using using growingly growingly accessible accessible THz THz time-domain time-domain spectrometers spectrometers (THz-TDS) (THz-TDS) [18 –[18–21]. The21]. The most most comprehensive comprehensive study study of its of THz its THz optical optical properties properties for thefor the waves waves polarized polarized parallel parallel to allto threeall three optical optical axes axes of the of KTPthe KTP crystals crystals was was carried carrie outd inout [20 in]. [20]. The refractiveThe refractive index index components components at room at temperatureroom temperature were approximatedwere approximated in the in form the of form Sellmeier of Sellmeier equations equations [21]. [21]. In this paper, wewe reportreport terahertzterahertz optical propertiesproperties of KTP crystals at the room temperature of 293 K (RT)(RT) andand atat thethe liquid liquid nitrogen nitrogen temperature temperature of of 81 81 K andK and calculate calculate phase-matching phase-matching conditions conditions for nonlinearfor nonlinear frequency frequency conversion conversion into into and and within within the the THz THz range. range. 2. Materials and Methods KTP single-crystalsingle-crystal ingotsingots were were grown grown using using the the Czochralski Czochralski method method from from a Pt a crucible Pt crucible of 100 of mm100 inmm diameter. in diameter. The crucible The crucible closed closed with Pt with cover Pt with cover about with 1 about kg of charge1 kg of was charge disposed was indisposed the resistivity in the oven.resistivity After oven. heating, After the heating, melt was the homogenized melt was homogenized and cooled downand cooled to liquidus downtemperature. to liquidus temperature. The crystals wereThe crystals grown were using grown single-domain using single-domain seed in the directionseed in the of directionX-axis. Duringof X-axis. the During growth the period growth of ◦ ◦ 45–55period days, of 45–55 the meltdays, was the cooled melt was down cooled by 70–120 down C.by The70–120 cooling °С. rateThe ofcooling the crystal rate of was the 0.1–4 crystalC/day was while0.1–4 ° itsС/day rotation while speed its rotation varied from speed 30 tovaried 40 rpm. from In 30 parallel, to 40 therpm. pulling In parallel, speed changedthe pulling from speed 0 to 1.2changed mm/day. from By 0 selectingto 1.2 mm/day. optimal By growth selecting conditions optima high-qualityl growth conditions single-crystal high-quality ingots having single-crystal a weight 3 ofingots 260 ghaving and dimensions a weight of of 260X ×g andY × dimensionsZ = 40 × 60 of× X70 × mm Y × Zwere = 40 grown.× 60 × 70 mm3 were grown. 3 At first,first, a large plateplate withwith dimensionsdimensions ofof XX × YY ×× ZZ == 11 11 × ×2828 × ×58 58mm mm3 waswas manufactured manufactured to toevaluate evaluate the the quality quality of ofthe the grown grown crystal crystal and and me measureasure its its transmission transmission spectrum spectrum in in the main transparency window. window. Then Then three three pairs pairs samples samples with with different different thickness thickness with dimensions with dimensions of 10 × 10 of 3 10× (0.28,× 10 0.35× (0.28 and, 0.351.08) and mm 1.08)3 were mm cut orthogonalwere cut orthogonal to the optical to the axes optical X (KTP axesx) andX (KTP Z (KTPx) andz) (FigureZ (KTP 1).z) (FigureSides of1 ).the Sides KTP ofx thesample KTP werex sample parallel were to parallel the Y toand the ZY axesand andZ axes sides and of sides the ofKTP thez KTPsamplez sample were wereparallel parallel to the to X the andX andY axes.Y axes. So, every So, every pair pair of samples of samples allowed allowed us usto tomeasure measure all all three three (x (x, ,yy andand zz)) components of the absorption coefficientcoefficient and refractiverefractive index for waves polarized parallel to the X, Y and Z axes, respectively and select the best-thickness crystalscrystals forfor thethe study.study. Figure 1. A pair of prepared KTP crystal samples cut orthogonal to the X and Z axes. Figure 1. A pair of prepared KTP crystal samples cut orthogonal to the X and Z axes. Transmission spectra in the transparency window were measured by UV-2101/3101 Transmission spectra in the transparency window were measured by UV-2101/3101 spectrophotometer (Shimadzu, Kyoto, Japan). Terahertz optical properties were studied using a spectrophotometer (Shimadzu, Kyoto, Japan). Terahertz optical properties were studied using THz-TDS (IA&E SB RAS, Novosibirsk, Russia) with a cryostat described elsewhere [20] at the temperatures of 293 K and 81 K. Crystals 2018, 8, 310 3 of 8 a THz-TDS (IA&E SB RAS, Novosibirsk, Russia) with a cryostat described elsewhere [20] at the temperaturesCrystals 2018, 8, x of FOR 293 PEER K and REVIEW 81 K. 3 of 8 3.3. Results TheThe resistivityresistivity ofof aa growngrown KTPKTP crystalcrystal isis oneone ofof indicatorsindicators ofof itsits quality.quality. HigherHigher valuesvalues ofof resistivityresistivity makemake the the crystals crystals applicable applicable for manufacturingfor manufacturing electro-optic electro-optic devices: devices: amplitude amplitude and phase and modulatorsphase modulators [12].