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Results for “Nonlinear optical susceptibility”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2014

Dispersion of the linear and nonlinear optical susceptibilities of the CuAl(S{sub 1–x}Se{sub x})₂ mixed chaclcopyrite compounds

Based on the electronic band structure, we have calculated the dispersion of the linear and nonlinear optical susceptibilities for the mixed CuAl(S{sub 1–x}Se{sub x})₂ chaclcopyrite compounds with x=0.0, 0.25, 0.5, 0.75, and 1.0. Calculations are performed within the Perdew-Becke-Ernzerhof general gradient approximation. The investigated compounds possess a direct band gap of about 2.2 eV (CuAlS₂), 1.9 eV (CuAl(S₀.₇₅Se₀.₂₅)₂), 1.7 eV (CuAl(S₀.₅Se₀.₅)₂), 1.5 eV (CuAl(S₀.₂₅Se₀.₇₅)₂), and 1.4 eV (CuAlSe₂) which tuned to make them optically active for the optoelectronics and photovoltaic applications. These results confirm that substituting S by Se causes significant band gaps' reduction. The optical function's dispersion ε₂{sup xx}(ω) and ε₂{sup zz}(ω)/ε₂{sup xx}(ω), ε₂{sup yy}(ω), and ε₂{sup zz}(ω) was calculated and discussed in detail. To demonstrate the effect of substituting S by Se on the complex second-order nonlinear optical susceptibility tensors, we performed detailed calculations for the complex second-order nonlinear optical susceptibility tensors, which show that the neat parents compounds CuAlS₂ and CuAlSe₂ exhibit | χ₁₂₂²}(-2ω;ω;ω) | as the dominant component, while the mixed alloys exhibit | χ₁₁₁²(-2ω;ω;ω) | as the dominant component. The features of | χ₁₂₃²}(-2ω;ω;ω) | and | χ{sub 111}²}(-2ω;ω;ω) | spectra were analyzed on the basis of the absorptive part of the corresponding dielectric function ε₂(ω) as a function of both ω/2 and ω.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1999

Piezoelectric Field Enhanced Second-Order Nonlinear Optical Susceptibilities in Wurtzite GaN/AlGaN Quantum Wells

Second-order nonlinear optical processes including second-harmonic generation, optical rectification, and difference-frequency generation associated with intersubband transitions in wurtzite GaN/AlGaN quantum well (QW) are investigated theoretically. Taking into account the strain-induced piezoelectric (PZ) effects, we solve the electronic structure of the QW from coupled effective-mass Schrodinger equation and Poisson equation including the exchange-correlation effect under the local-density approximation. We show that the large PZ field in the QW breaks the symmetry of the confinement potential profile and leads to large second-order susceptibilities. We also show that the interband optical pump-induced electron-hole plasma results in an enhancement in the maximum value of the nonlinear coefficients and a redshift of the peak position in the nonlinear optical spectrum. By use of the difference-frequency generation, THz radiation can be generated from a GaN/Al(0.75)Ga(0.25)N with a pump laser of 1.55 micron.

Liu, Ansheng↗
DOE OSTI2019

Effect of Oxygen Flow Rate on Structural, Electrical and Optical Properties of Zinc Aluminum Oxide Thin Films Deposited by DC Magnetron Sputtering

Zinc Aluminum Oxide thin films were deposited on glass substrates by reactive DC magnetron sputtering method by varying oxygen flow rates from 1 to 4 sccm. Glancing angle X-ray diffraction patterns ofzinc aluminum oxide thin films exhibits (0 0 2) peak with c-plane preferentially oriented parallel to the substrate. The surface morphology and elemental analysis of the films was observed by field emission scanning electron microscopy attached with energy dispersive X-ray analysis spectroscopy. An average optical transmittance of 83–90% is obtained for the films deposited at various oxygen flow rates. The optical band gap of the films increases from 3.41 to 3.53 eV with the increase of oxygen flow rate due to Burstein–Moss effect. The optical dispersion parameters such as dispersion energy (E{sub d}), oscillator energy (E{sub o}) and static refractive index (n{sub o}) were determined using the Wemple-DiDomenico (W-D) single oscillator model. The nonlinear optical parameters such as optical susceptibility (χ{sup (1)}), third order nonlinear optical susceptibility (χ{sup (3)}) and nonlinear refractive index (n{sub 2}) were also determined.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Z-scan: A simple technique for determination of third-order optical nonlinearity

Z-scan is a simple experimental technique to measure intensity dependent nonlinear susceptibilities of third-order nonlinear optical materials. This technique is used to measure the sign and magnitude of both real and imaginary part of the third order nonlinear susceptibility (χ{sup (3)}) of nonlinear optical materials. In this paper, we investigate third-order nonlinear optical properties of Ag-polymer composite film by using single beam z-scan technique with Q-switched, frequency doubled Nd: YAG laser (λ=532 nm) at 5 ns pulse. The values of nonlinear absorption coefficient (β), nonlinear refractive index (n{sub 2}) and third-order nonlinear optical susceptibility (χ{sup (3)}) of permethylazine were found to be 9.64 × 10{sup −7} cm/W, 8.55 × 10{sup −12} cm{sup 2}/W and 5.48 × 10{sup −10} esu, respectively.

36 MATERIALS SCIENCE↗
NASA NTRS1995

Preparation of polymeric diacetylene thin films for nonlinear optical applications

A method for producing polymeric diacetylene thin films having desirable nonlinear optical characteristics has been achieved by producing amorphous diacetylene polymeric films by simultaneous polymerization of diacetylene monomers in solution and deposition of polymerized diacetylenes on to the surface of a transparent substrate through which ultraviolet light has been transmitted. These amorphous polydiacetylene films produced by photo-deposition from solution possess very high optical quality and exhibit large third order nonlinear optical susceptibilities, such properties being suitable for nonlinear optical devices such as waveguides and integrated optics.

Frazier, Donald O.↗
DOE OSTI2018

Linear and nonlinear optical probe of the ferroelectric-like phase transition in a polar metal, LiOsO 3

LiOsO 3 is one of the first materials identified in the current literature as a “polar metal,” a class of materials that are simultaneously noncentrosymmetric and metallic. In this work, the linear and nonlinear optical susceptibility of LiOsO 3 is studied by means of ellipsometry and optical second harmonic generation (SHG). Robust optical birefringence is observed using spectroscopic ellipsometry. The nonlinear optical susceptibility extracted from SHG polarimetry reveals that the tensor components are of the same magnitude as in the isostructural insulator LiNbO 3 , except the component along the polar axis d 33 is suppressed by an order of magnitude. Temperature-dependent SHG measurements in combination with Raman spectroscopy indicate a continuous order-disorder type polar phase transition at 140 K. Linear and nonlinear optical microscopy measurements reveal 109°/71° ferroelastic domain walls, like in other trigonal ferroelectrics. No 180° polar domain walls are observed to emerge across the phase transition.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Plasmonic Nonlinear Energy Transfer Enhanced Second Harmonic Generation Nanoscopy

Nonlinear optical response is a fingerprint of various physicochemical properties of materials related to symmetry, including crystallography, interfacial configuration, and carrier dynamics. However, the intrinsically weak nonlinear optical susceptibility and the diffraction limit of far-field optics restrict probing deep-subwavelength-scale nonlinear optics with measurable signal-to-noise ratio. Here, we propose an alternative approach toward efficient second harmonic generation (SHG) nanoscopy for SHG-active sample (zinc oxide nanowire; ZnO NW) using an SHG-active plasmonic nanotip. Our full-wave simulation suggests that the experimentally observed high near-field SHG contrast is possible when the nonlinear response of ZnO NW is enhanced and/or that of the tip is suppressed. Here, this result suggests possible evidence of quantum mechanical nonlinear energy transfer between the tip and the sample, modifying the nonlinear optical susceptibility. Further, this process probes the nanoscale corrosion of ZnO NW, demonstrating potential use in studying various physicochemical phenomena in nanoscale resolution.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Resonant nonlinear refraction of 4 – 5 - μ m light in CO and C O 2 gas

The resonant nonlinear refraction of 4–5-μm light in CO and CO 2 gas at a peak intensity of 15MW/cm 2 was demonstrated using time- and frequency-resolved measurements of self-focusing and self-defocusing. The nonlinearity of these molecular gases exhibits intensity-dependent sign reversals and a <4-ns response time. A change from self-focusing to self-defocusing or vice versa was observed to occur for Rabi frequencies that are comparable to the collisional linewidth. A density matrix model for the nonlinear susceptibility of a strongly driven two-level system provides a qualitative explanation for these results.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2015

Growth and characterization of a third order nonlinear optical single crystal: Ethylenediamine-4-nitrophenolate monohydrate

Highlights: • EDA4NPH crystal possesses negative nonlinear refractive index. • The crystal exhibits high third-order NLO susceptibility. • Wide transparency of the crystal makes it suitable for NLO applications. • Dielectric studies substantiate the suitability for electro-optic applications. • The crystal possesses suitable mechanical strength for device fabrication. - Abstract: Bulk crystals of the charge-transfer complex, ethylenediamine-4-nitrophenolate monohydrate, were grown by slow solvent evaporation method from aqueous solution at room temperature. The X-ray diffraction measurements showed that the crystal belongs to centrosymmetric space group C2/c of monoclinic system. The functional groups in the complex were identified using FTIR, FTRaman and FTNMR analyses. The Z-scan measurements revealed the negative nonlinear refractive index of the crystal. The nonlinear absorption coefficient and third order nonlinear optical susceptibility calculated from the measurements were −3.5823 × 10{sup −3} cm/W and 2.3762 × 10{sup −6} esu respectively. The crystal was shown to be highly transparent above 366 nm by UV–vis spectroscopy and a yellow fluorescence was observed from PL spectrum. The TG–DTA and DSC analyses showed that the crystal is thermally stable up to 117.4 °C. The crystals were characterized by dielectric, etching and microhardness studies.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Sub-wavelength modulation of χ (2) optical nonlinearity in organic thin films

Modulating the second-order nonlinear optical susceptibility (χ (2) ) of materials at the nanoscale represents an ongoing technological challenge for a variety of integrated frequency conversion and nonlinear nanophotonic applications. Here we exploit the large hyperpolarizability of intermolecular charge transfer states, naturally aligned at an organic semiconductor donor–acceptor (DA) interface, as a means to control the magnitude and sign of χ (2) at the nanoscale. Focusing initially on a single pentacene-C 60 DA interface, we confirm that the charge transfer transition is strongly aligned orthogonal to the heterojunction and find that it is responsible for a large interfacial nonlinearity probed via second harmonic generation that is sufficient to achieve d 33 > 10pm V –1 , when incorporated in a non-centrosymmetric DA multilayer stack. Lastly, using grating-shadowed oblique-angle deposition to laterally structure the DA interface distribution in such multilayers subsequently enables the demonstration of a χ (2) grating with 280 nm periodicity, which is the shortest reported to date.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Growth and characterization studies on L-threoninium p-toluenesulfonate monohydrate crystal

L-threoninium p-toluenesulfonate monohydrate (LTPTM) (IUPAC name: 1-carboxy-2-hydroxypropan-1-aminium 4-methylbenzenesulfonate monohydrate), a new organic nonlinear optical (NLO) crystal, is grown by solution growth method at room temperature. It crystallizes in monoclinic crystal system with noncentrosymmetric space group P2{sub 1}. Presence of NH{sub 3}{sup +} and SO{sub 3}{sup −} vibrations in IR and Raman spectra confirms the formation of LTPTM molecule. The {sup 1}H and {sup 13}C nuclear magnetic resonance (NMR) spectra establish the molecular structure. In the {sup 1}H–NMR spectrum of LTPTM, the chemical shift corresponding to H-SO{sub 3} (6.57 ppm) of p-toluenesulfonic acid monohydrate is absent. This is due to the fact that the hydrogen in H–SO{sub 3} is released and combines with the amine group of L-threonine. This ensures the formation of LTPTM molecule. The O5-H5A…O3 intermolecular interaction is also established by the observed upfield shift of COOH group in LTPTM molecule. The crystal is thermally stable up to 73 °C. LTPTM is transparent from 235 to 1100 nm. The second harmonic generation (SHG) conversion efficiency of LTPTM is 0.77 times that of KDP. Third order nonlinear optical susceptibility (χ{sup (3)}) of the title crystal is 1.3035 × 10{sup −7} esu which is higher than some reported NLO crystals.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Many-body effects in nonlinear optical responses of 2D layered semiconductors

We performed ultrafast degenerate pump-probe spectroscopy on monolayer WSe2 near its exciton resonance. The observed differential reflectance signals exhibit signatures of strong many-body interactions including the exciton-exciton interaction and free carrier induced band gap renormalization. The exciton-exciton interaction results in a resonance blue shift which lasts for the exciton lifetime (several ps), while the band gap renormalization manifests as a resonance red shift with several tens ps lifetime. Our model based on the many-body interactions for the nonlinear optical susceptibility ts well the experimental observations. The power dependence of the spectra shows that with the increase of pump power, the exciton population increases linearly and then saturates, while the free carrier density increases superlinearly, implying that exciton Auger recombination could be the origin of these free carriers. Our model demonstrates a simple but efficient method for quantitatively analyzing the spectra, and indicates the important role of Coulomb interactions in nonlinear optical responses of such 2D materials.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Glass formation and the third harmonic generation of Cu{sub 2}Se–GeSe{sub 2}–As{sub 2}Se{sub 3} glasses

We have performed the investigation of the nonlinear optical properties namely the third harmonic generation (THG) of the glass-formation region in the Cu{sub 2}Se–GeSe{sub 2}–As{sub 2}Se{sub 3} system. The samples were synthesized by direct single-temperature method from high-purity elementary substances. We have found that the value of disorder parameter Δ depends on the composition of the glassy alloys. The measurements show that increasing the Cu{sub 2}Se concentration leads to increased slope of the absorption edge, which may be explained by the decrease of the height of random potential relief for the electrons in the tails of the state density which border the band edges. A very sharp increase in the THG at low temperature was observed. Significant enhancement in THG was obtained with decreasing the energy gap, which agreed well with the nonlinear optical susceptibilities obtained from other glasses.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Time-Resolved Ultrafast Transient Polarization Spectroscopy to Investigate Nonlinear Processes and Dynamics in Electronically Excited Molecules on the Femtosecond Time Scale

Here, we report a novel experimental technique to investigate ultrafast dynamics in photoexcited molecules by probing the third-order nonlinear optical susceptibility. A non-colinear 3-pulse scheme is developed to probe the ultrafast dynamics of excited electronic states using the optical Kerr effect by time-resolved polarization spectroscopy. Optical heterodyne and optical homodyne detection are demonstrated to measure the third-order nonlinear optical response for the S 1 excited state of liquid nitrobenzene, which is populated by 2-photon absorption of a 780 nm 35 fs excitation pulse.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Enhanced second-harmonic generation from WS 2 /ReSe 2 heterostructure

Van der Waals stacking presents new opportunities for nonlinear optics with its remarkable tunability and scalability. However, the fundamental role of interlayer interactions in modifying the overall nonlinear optical susceptibilities remains elusive. In this work, we report anisotropic enhancement of second-harmonic generation (SHG) from a WS 2 /ReSe 2 heterobilayer, where the individual composite layers possess distinctive crystal phases. We investigate polarization-resolved response and twist-angle dependence in SHG and reveal that band alignment alone is insufficient to explain the observed anisotropy in the modified SHG response. Spectral shifts in excitonic features highlight band renormalization, supporting the role of hybridization between the two layers. Furthermore, SHG enhancement is highly anisotropic and can even be suppressed in some orientations, suggesting possible intensity-borrowing mechanisms within the heterostructure. Our work demonstrates the ability to tune both the intensity and polarization dependence of nonlinear optical responses with van der Waals stacking of distinctive crystal phases.

2D materials↗
DOE OSTI2016

Synthesis, growth, structure, mechanical and optical properties of a new semi-organic 2-methyl imidazolium dihydrogen phosphate single crystal

Highlights: • 2MIDP crystals were grown by slow evaporation solution growth technique. • Single crystal XRD revealed self-assembled supramolecular framework. • Z scan technique is employed for third order nonlinear optical susceptibility. • Structure-property correlation is established. - Abstract: A new semi-organic compound, 2-methyl imidazolium dihydrogen phosphate (2MIDP), was prepared and good quality single crystals of 2MIDP were grown by slow evaporation solution growth technique. Crystal structure elucidated using Single crystal XRD showed that 2MIDP crystallizes in monoclinic system with P2{sub 1}/c space group. FT-IR, UV-Vis-NIR, Fluorescence and FT-NMR spectra confirm the molecular structure of 2MIDP. The UV-Vis-NIR spectra established the suitability of the compound for NLO applications. TG-DSC showed that 2MIDP is thermally stable up to 200 °C. Mechanical characteristics like hardness number (H{sub v}), stiffness constant (C{sub 11}), yield strength (σ{sub v}), fracture toughness (K{sub c}) and brittleness index (B{sub i}) were assessed using Vicker’s microhardness tester. Third order nonlinear optical properties determined from Z-scan measurement using femto and picosecond lasers showed two photon reverse saturable absorption. The enhancement of nonlinear optical properties in femto second laser, revealed the suitability of 2MIDP for optical limiting applications.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Optical nonlinearities of excitons in monolayer MoS 2

We calculate linear and nonlinear optical susceptibilities arising from the excitonic states of monolayer MoS 2 for in-plane light polarizations, using second-quantized bound and unbound exciton operators. Optical selection rules are critical for obtaining the susceptibilities. We derive the valley-chirality rule for the second-order harmonic generation in monolayer MoS 2 and find that the third-order harmonic process is efficient only for linearly polarized input light while the third-order two-photon process (optical Kerr effect) is efficient for circularly polarized light using a higher order exciton state. The absence of linear absorption due to the band gap and the unusually strong two-photon third-order nonlinearity make the monolayer MoS 2 excitonic structure a promising resource for coherent nonlinear photonics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Sol–gel synthesis of silver nanocrystals embedded in sodium borosilicate monolithic transparent glass with giant third-order optical nonlinearities

Highlights: • We prepared Ag-doped sodium borosilicate monolithic glass. • The influence of temperature on the SPR absorption peak intensity was studied. • Nonlinear optical properties of the glass were investigated. • A mechanism for the formation of Ag quantum dots glass was proposed. - Abstract: We report the preparation of uniform spherical shape silver nanocrystals doped sodium borosilicate monolithic transparent glass by sol–gel method. The characterization of the resulting Ag nanocrystals was accomplished by using X-ray powder diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, and energy dispersive X-ray spectrum. Surface plasma resonance absorption peaks of the silver nanocrystals glass at about 406 nm have been obtained from ultraviolet–visible absorption spectrometer and their intensity is changed with different heat treatment temperatures. We have investigated the nonlinear optical properties of silver quantum dots doped glass using Z-scan technique. Third-order nonlinear optical susceptibility χ{sup (3)} of the glass was estimated to be 1.01 × 10{sup −11} esu. In particular, a mechanism for the formation of Ag quantum dots glass is proposed. This work will significantly promote the obtained material applications in optical devices.

36 MATERIALS SCIENCE↗