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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
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↗
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 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 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↗
NASA NTRS1995

Photodeposition of amorphous polydiacetylene films from monomer solutions onto transparent substrates

Polydiacetylenes are a very promising class of polymers for both photonic and electronic applications because of their highly conjugated structures. For these applications, high-quality thin polydiacetylene films are required. We have discovered a novel technique for obtaining such films of a polydiacetylene derivative of 2-methyl-4-nitroaniline using photodeposition from monomer solutions onto UV transparent substrates. This heretofore unreported process yields amorphous polydiacetylene films with thicknesses on the order of I micron that have optical quality superior to that of films grown by standard crystal growth techniques. Furthermore, these films exhibit good third-order nonlinear optical susceptibilities; degenerate four-wave mixing experiments give x(3) values on the order of 10(exp -8) - 10(exp -7) esu. We have conducted masking experiments which demonstrate that photodeposition occurs only where the substrate is directly irradiated, clearly indicating that the reaction occurs at the surface. Additionally, we have also been able to carry out photodeposition using lasers to form thin polymer circuits. In this work, we discuss the photodeposition of polydiacetylene thin films from solution, perform chemical characterization of these films, investigate the role of the substrate, speculate on the mechanism of the reaction, and make a preliminary determination of the third-order optical nonlinearity of the films. This simple, straightforward technique may ultimately make feasible the production of polydiacetylene thin films for technological applications.

Paley, M. S.↗
DOE OSTI2023

Topological enhancement of nonlinear transport in unconventional point-node semimetals

The topological singularity of the Bloch states close to the Fermi level significantly enhances nonlinear electric responses in topological semimetals. Here, we systematically characterize this enhancement for a large class of topological nodal-point fermions, including those with linear, linear-quadratic, and quadratic dispersions. Specifically, we determine the leading power-law dependence of the nonlinear response functions on the chemical potential μ defined relative to the nodal point. We identify two characteristics that qualitatively improve nonlinear transports compared to those of conventional Dirac and Weyl fermions. First, the type-II (overtilted) spectrum leads to the log μ enhancement of nonlinear response functions having zero scaling dimension with respect to μ, which is not seen in a type-I (moderately or not tilted) spectrum. Second, the anisotropic linear-quadratic dispersion increases the power of small-μ divergence for the nonlinear response tensors along the linearly dispersing direction. Furthermore, our work reveals new experimental signatures of unconventional nodal points in topological semimetals as well as provides a guiding principle for giant nonlinear electric responses.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1977

Diagrammatic evaluation of the density operator for nonlinear optical calculations

Time-ordered diagrammatic representations are shown to precisely define and to simplify calculations of radiative perturbations to the density matrix. Nonlinear optical susceptibilities, here exemplified by that of CARS, can be obtained by simple propagator rules. An interpretation of transient Raman scattering in terms of time-ordered contributions is also discussed.

Yee, S. Y.↗
NASA NTRS1990

Applications of ultrashort laser pulses in science and technology; Proceedings of the Meeting, The Hague, Netherlands, Mar. 12, 13, 1990

Topics discussed are on the generation of high-intensity femtosecond lasers, the high-repetition and infrared femtosecond pulses, and physics of semiconductors and applications. Papers are presented on the femtosecond pulse generation at 193 nm; the generation of intense subpicosecond and femtosecond pulses; intense tunable subpicosecond and femtosecond pulses in the visible and infrared, generated by optical parametric oscillators; a high-efficiency high-energy optical amplifier for femtosecond pulses; and the generation of solitons, periodic pulsing, and nonlinearities in GaAs. Other papers are on ultrafast relaxation dynamics of photoexcited carriers in GaAs, high-order optical nonlinear susceptibilities of transparent glasses, subnanosecond risetime high-power pulse generation using photoconductive bulk GaAs devices, femtosecond studies of plasma formation in crystalline and amorphous silicon, and subpicosecond dynamics of hot carrier relaxation in InP and GaAs.

Antonetti, Andre↗
DOE OSTI2025

Second harmonic generation in topological insulators under quantizing magnetic fields

We theoretically investigate the second harmonic generation (SHG) of topological insulator surface states in a perpendicular magnetic field. Our theory is based on the microscopic expression of the second-order magneto-optical conductivity developed from the density matrix formalism, taking into account hexagonal warping effects on the surface states' band structure. Using numerically exact Landau-level energies and wave functions including hexagonal warping, we calculate the spectrum of SHG conductivities under normal incidence for different values of magnetic field and chemical potential. The imaginary parts of the SHG conductivities show prominent resonant peaks corresponding to one-photon and two-photon inter-Landau-level transitions. Treating the hexagonal warping term perturbatively, these transitions are clarified analytically within a perturbation theory from which approximate selection rules for the allowable optical transitions for SHG are determined. Furthermore, our results show extremely high SHG susceptibility that is easily tunable by magnetic field and doping level for topological surface states in the far-infrared regime, exceeding that of many conventional nonlinear materials. This work highlights the key role of hexagonal warping effects in generating second-order optical responses and provides insights into the nonlinear magneto-optical properties of the topological insulators.

Landau levels↗
DOE OSTI2023

Extracting spinon self-energies from two-dimensional coherent spectroscopy

Two-dimensional coherent spectroscopy (2DCS) is a nonlinear spectroscopy technique capable of identifying whether apparent continua in linear response are made out of multiplets of sharp deconfined quasiparticles. This makes it a potent tool for experimental identification of fractionalized phases. Previous discussions have focused on limits where the quasiparticles in question are infinitely long lived. In this paper we discuss 2DCS in the regime where the fractionalized quasiparticles can themselves decay. We introduce a powerful path-integral-based approach, whereby the computation of nonlinear susceptibilities reduces to an efficient exercise in diagrammatic perturbation theory. Here, we apply this method to compute the 2DCS response of the one-dimensional transverse field Ising model, in the presence of integrability-breaking perturbations. We discuss aspects of the self-energy of the fractionalized quasiparticles that may be extracted via 2DCS, such as the momentum-dependent decay rate.

1-dimensional spin chains↗
NASA NTRS2021

On Parametric Generation of Deep UV Light in Monolithic Cavities With Cubic Nonlinearity

Coherent ultra violet (UV) light has broad applications in optical atomic clocks and quantum computers. Since availability of semiconductor tunable monochromatic lasers is limited at short wavelengths, optical nonlinear processes are frequently used to produce the desirable radiation wavelength. Optical crystals with quadratic nonlinearity are promising for this purpose because of their transparency and high optical damage threshold. In this paper we discuss a possibility of generation of coherent deep UV light utilizing high quality factor (-Q) monolithic optical microcavities made of crystalline optical materials characterized with cubic nonlinearities. We show that the generation is feasible in spite of the relatively small cubic nonlinearities, due to the ultra-broad-band high optical transparency of the crystals and associated high-Q achievable in the cavities created out of the materials. We found that the birefringence as well as the tensor nature of the nonlinear susceptibility of the crystalline optical materials can simplify the phase matching of the nonlinear processes.

Matsko, A.B.↗
NASA NTRS1973

Phase matching in second-harmonic generation using artificial periodic structures.

The use of artificial periodic structures, consisting of spatial modulations of the linear and nonlinear susceptibilities of a nonlinear optical medium, to achieve phase matching in second-harmonic generation is analyzed. Dispersion relations and approximate formulas for the second-harmonic fields generated under various conditions are obtained and used to evaluate the experimental situation.

Tang, C. L.↗
NASA NTRS1999

Transmission Measurement of the Third-Order Susceptibility of Gold

Gold nanoparticle composites are known to display large optical nonlinearities. In order to assess the validity of generalized effective medium theories (EMT's) for describing the linear and nonlinear optical properties of metal nanoparticle composites, knowledge of the linear and nonlinear susceptibilities of the constituent materials is a prerequisite. In this study the inherent nonlinearity of the metal is measured directly (rather than deduced from a suitable EMT) using a very thin gold film. Specifically, we have used the z-scan technique at a wavelength near the transmission window of bulk gold to measure the third-order susceptibility of a continuous thin gold film deposited on a quartz substrate surface-modified with a self-assembled monolayer to promote adhesion and uniformity without affecting the optical properties. We compare our results with predictions which ascribe the nonlinear response to a Fermi-smearing mechanism. Further, we note that the sign of the nonlinear susceptibility is reversed from that of gold nanoparticle composites.

Smith, David D.↗
DOE OSTI2025

Quantum critical electro-optic and piezo-electric nonlinearities

Although electro-optic (EO) nonlinearities are essential for many quantum and classical photonics applications, a major challenge is inefficient modulation in cryogenic environments. Guided by the connection between phase transitions and nonlinearity, we identify the quantum paraelectric perovskite SrTiO 3 as a strong cryogenic EO [>500 picometers per volt (pm/V)] and piezo-electric material (>90 picocoulombs per newton) at T = 5 K, at frequencies to at least 1 megahertz. Furthermore, by tuning SrTiO 3 toward quantum criticality, we more than double the EO and piezo-electric effects, demonstrating a linear Pockels coefficient above 1000 pm/V. Furthermore, our results probe the link between quantum phase transitions, dielectric susceptibility, and nonlinearity, unlocking opportunities in cryogenic optical and mechanical systems and providing a framework for discovering new nonlinear materials.

Anderson, Christopher P. [Stanford University, CA ↗
NASA NTRS1990

Compounds Generate Optical Second Harmonics

Newly synthesized organic salts found to generate relatively large second-harmonic signals when illuminated by fundamental signals in near-infrared spectrum. Made by crystallizing, with appropriate counterions, organic ions having large molecular hyperpolarizibilities. Large second-order nonlinear susceptibilities observed. These and other compounds having large nonlinear optical properties used in electro-optical modulators, switches, and signal-processing equipment.

Marder, Seth R.↗
NASA NTRS1989

Diphenylpolyynes For Nonlinear Optical Devices

Several diphenylpolyyne compounds found to exhibit second-order nonlinear electric susceptibilities and chemical structures conducive to orientation in appropriate chemical environments. These features make new materials suitable for use in optical devices. Diphenylacetylene links give molecules rodlike characteristics making them amenable to orientation by suspension in liquid crystals. New molecules also have inherent liquid-crystalline properties enabling them to be oriented directly.

Stiegman, Albert E.↗
DOE OSTI2025

Nonlinear van der Waals Metasurfaces with Resonantly Enhanced Light Generation

Efficient nonlinear wave mixing is of paramount importance for a wide range of applications. However, weak optical nonlinearities pose significant challenges for accessing nonlinear light–matter interaction in compact systems. Here, we experimentally study second harmonic generation in deeply subwavelength 3R-MoS 2 metasurfaces (<λ/13 thick). Our measurements, supported by theoretical analysis, reveal a complex interplay and coupling between geometric resonances, optical extinction, and exciton-driven strong nonlinear susceptibility dispersion. We further demonstrate >150-fold enhancement in second harmonic signal at 740 nm mediated by the A exciton resonance. Additionally, our theoretical studies predict an enhancement of more than 10 6 in second harmonic generation in <100 nm thick structures exhibiting bound states in the continuum resonance. These findings provide insight into accessing and harnessing the unprecedented 3R-MoS 2 nonlinearities at a subwavelength scale, paving the way to ultracompact nonlinear photonic devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗