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NASA NTRS1988

Mid-infrared solid-state lasers and laser materials

An account is given of NASA-Langley's objectives for the development of advanced lasers and laser materials systems applicable to remote sensing in the mid-IR range. Prominent among current concerns are fiber-optic spectroscopy, eye-safe solid-state lasers for both Doppler sensing and mid-IR wavelength-generation laser pumping, and nonlinear optics generating tunable mid-IR radiation. Ho:YAG lasers are noted to exhibit intrinsic advantages for the desired applications, and are pumpable by GaAlAs laser diodes with a quantum efficiency approaching 2.

Barnes, Norman P.↗

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 NTRS1986

Optical image subtraction techniques, 1975-1985

Real- and nonreal-time optical image subtraction (OIS) techniques are reviewed. Real-time OIS techniques include source encoding, polarization modulation, pseudocolor image difference detection, the holographic shear lens technique, and nonlinear optics. Included in the nonreal-time category are speckle diffuser encoding, speckle-pattern encoding, halftone screen encoding, and polarization-shifted encoding. It is concluded that the most useful techniques are the real-time operations. It is noted that some nonreal-time optical techniques can be applied directly while others may be converted into real-time ones through the use of advance real-time spatial light modulators or electrooptic devices.

Liu, Hua-Kuang↗

NASA NTRS1991

Line narrowing of AgGaSe2 optical parametric oscillator by injection seeding

Solid-state lasers are developed for atmospheric applications. Optical parametric oscillators (OPO) are being investigated as sources of tunable radiation in the 2.5-12 micron range where development of conventional lasers is subject to numerous difficulties. Parametric oscillation is a nonlinear optical technique for converting laser output to longer wavelengths. Incident photons, typically from a pulsed pump laser, are converted into two photons of longer wavelength, while satisfying energy conservation. The particular split of energy is determined by momentum conservation; the wavelength of interest is usually selected by angle orientation of the nonlinear material with respect to the direction of propagation of the pump beam. An OPO based on AgGaSe2 was considered.

Watson, George H.↗

DOE OSTI2025

Chemical Control of Symmetry and Bandgap in Tungsten Oxyhalide van der Waals Semiconductors

Tunability in solid-state materials is essential for testing theory, discovering quantum phases, and enabling functionality. Layered van der Waals (vdW) semiconductors offer a unique platform, providing new degrees of freedom at the two-dimensional (2D) limit through exfoliation and external controls. Here, in this study, we demonstrate tunability of symmetry and electronic structure via halogen substitution in a family of layered vdW tungsten oxyhalides. Substituting the halogens in WO 2 X 2 (X = I, Br, Cl) tunes the bandgap across a broad energy range and modifies the structural symmetry from centrosymmetric to noncentrosymmetric. By alloying WO 2 I 2– y Br y , we continuously tune the polar distortion and optical gap across the visible range. These insights into halogen substitution effects on symmetry and electronic structure lay the foundation for new tunable vdW semiconductors for optoelectronics and nonlinear optics.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Quantum control of exciton wave functions in 2D semiconductors

Excitons—bound electron-hole pairs—play a central role in light-matter interaction phenomena and are crucial for wide-ranging applications from light harvesting and generation to quantum information processing. A long-standing challenge in solid-state optics has been to achieve precise and scalable control over excitonic motion. We present a technique using nanostructured gate electrodes to create tailored potential landscapes for excitons in 2D semiconductors, enabling in situ wave function shaping at the nanoscale. Our approach forms electrostatic traps for excitons in various geometries, such as quantum dots, rings, and arrays thereof. We show independent spectral tuning of spatially separated quantum dots, achieving degeneracy despite material disorder. Owing to the strong light-matter coupling of excitons in 2D semiconductors, we observe unambiguous signatures of confined exciton wave functions in optical reflection and photoluminescence measurements. This work unlocks possibilities for engineering exciton dynamics and interactions at the nanometer scale, with implications for optoelectronic devices, topological photonics, and quantum nonlinear optics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1999

Near-Infrared Laser Pumped Intersubband THz Laser Gain in InGaAs-AlAsSb-InP Quantum Wells

We investigate the possibility of using InGaAs-AlAsSb-InP coupled quantum wells to generate THz radiation by means of intersubband optical pumping. We show that large conduction band offsets of these quantum wells make it possible to use conventional near-infrared diode lasers around 1.55 micron as pump sources. Taking into account the pump-probe coherent interaction and the optical nonlinearity for the pump field, we calculate the THz gain of the quantum well structure. We show that resonant Raman scattering enhances the THz gain at low and moderate optical pumping levels. When the pump intensity is strong, the THz gain is reduced by pump-induced population redistribution and pump-probe coherent interactions.

Liu, An-Sheng↗

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.↗

DOE OSTI2024

Broadband Frequency Conversion of Spectrally Incoherent Pulses and Initial Laser-Plasma Instabilities Mitigation Experiments

There is a need for efficient broadband frequency conversion schemes from the infrared, where optical pulses are efficiently amplified by solid-state laser materials, to the ultraviolet, a wavelength range more suitable for inertial confinement fusion (ICF). The current schemes are inadequate for broadband, spectrally incoherent optical pulses composed of a large number of frequency components distributed over a large frequency range. Implementing novel technologies that generate optical pulses with a large number of spectral components improves the laser-target interaction. In particular, it has long been believed that broad bandwidth mitigates the electron-plasma-wave instabilities that generate suprathermal electrons, which degrade ICF performance by increasing the fuel adiabat and reducing the shell areal density. It is important to develop a platform to demonstrate hot electron suppression caused by the larger available bandwidth, which has not previously been feasible in the laboratory. Experimentally measuring and theoretically assessing these effects with adequately benchmarked simulation codes are paramount to the design and development of novel laser facilities aiming at producing energy via laser fusion. The Laboratory for Laser Energetics is building a new laser facility, the Fourth-generation Laser for Ultrabroadband eXperiments (FLUX), to generate high-energy nanosecond laser pulses with fractional bandwidth larger than 1% in the ultraviolet and perform combined experiments with the 60-beam Omega facility. This large increase in bandwidth from the ~ 0.1% currently available on high-energy laser systems, is achieved by combining amplification in nonlinear optical parametric amplifiers (OPAs) around 1053 nm (1w) with nonlinear frequency conversion to the ultraviolet (around 351 nm, 3w). The novel scheme for frequency conversion is based on the noncollinear sum-frequency generation (SFG) of the angularly dispersed amplified 1w output with a narrowband 2w pulse, which is also used to pump the OPA system. The proposal funded scientific and engineering studies necessary to implement this novel laser facility, accelerated the SFG deployment by funding additional project team resources (shop time, engineers, and technicians), and funded preliminary experiments on the Omega Laser.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS2002

Slow Light in Coupled Resonator Optical Waveguides

Recently, we discovered that a splitting of the whispering gallery modes (WGMs) occurs in coupled resonator optical waveguides (CROWs), and that these split modes are of a higher Q than the single-resonator modes, leading to enormous circulating intensity magnification factors that dramatically reduce thresholds for nonlinear optical (NLO) processes. As a result of the enhancements in Q, pulses propagating at a split resonance can propagate much slower (faster) for over (under)-coupled structures, due to the modified dispersion near the split resonance. Moreover, when loss is considered, the mode-splitting may be thought of as analogous to the Autler-Townes splitting that occurs in atomic three-level lambda systems, i.e., it gives rise to induced transparency as a result of destructive interference. In under- or over-coupled CROWs, this coupled resonator induced transparency (CRIT) allows slow light to be achieved at the single-ring resonance with no absorption, while maintaining intensities such that NLO effects are maximized. The intensity magnification of the circulating fields and phase transfer characteristics are examined in detail.

Chang, Hongrok↗

NASA NTRS2007

Recent Progress Made in the Development of High-Energy UV Transmitter

In this paper, the status of an all-solid-state UV converter development for ozone sensing applications is discussed. A high energy Nd:YAG laser for pumping the UV converter arrangement was recently reported. The pump is an all-solid-state, single longitudinal mode, and conductively cooled Nd:YAG laser operating at 1064 nm wavelength. Currently, this pump laser provides an output pulse energy of greater than 1J/pulse at 50 Hz PRF and a pulsewidth of 22 ns with an electrical-to-optical system efficiency of greater than 7% and a M(sup 2) value of approx. 2. The spatial profile of the output beam is a rectangular super Gaussian. This Nd:YAG pump laser has been developed to pump the nonlinear optics based UV converter arrangement to generate 320 nm and 308 nm wavelengths by means of 532 nm wavelength. Previously, this UV converter arrangement has demonstrated IR-to-UV conversion efficiency of 24% using a flash lamp pumped laser providing a round, flat top spatial profile. Recently, the UV converter was assembled and tested at NASA LaRC for pumping with the diode pumped Nd:YAG laser. With current spatial profile, the UV converter was made operational. Current efforts to maximize the nonlinear conversion efficiency by refining its spatial profile to match RISTRA OPO requirements are progressing.

Prasad, Narasimha S.↗

NASA NTRS1974

Mathematical operations by optical processing

Some recent developments in coherent optical processing are described in this paper. Specifically, the use of one or more elementary gratings to perform useful processing operations and computer-generated spatial filters to obtain generalized transforms are discussed. Applications incorporating nonlinear optical elements and optical feedback into the processing system are also presented.

Lee, S. H.↗

NASA NTRS2008

Tailored Asymmetry for Enhanced Coupling to WGM Resonators

Coupling of light into and out of whispering- gallery-mode (WGM) optical resonators can be enhanced by designing and fabricating the resonators to have certain non-axisymmetric shapes (see figure). Such WGM resonators also exhibit the same ultrahigh values of the resonance quality factor (Q) as do prior WGM resonators. These WGM resonators are potentially useful as tunable narrow-band optical filters having throughput levels near unity, high-speed optical switches, and low-threshold laser resonators. These WGM resonators could also be used in experiments to investigate coupling between high-Q and chaotic modes within the resonators. For a WGM resonator made of an optically nonlinear material (e.g., lithium niobate) or another material having a high index of refraction, a prism made of a material having a higher index of refraction (e.g., diamond) must be used as part of the coupling optics. For coupling of a beam of light into (or out of) the high-Q resonator modes, the beam must be made to approach (or recede from) the resonator at a critical angle determined by the indices of refraction of the resonator and prism materials. In the case of a lithium niobate/diamond interface, this angle is approximately 22 .

Mohageg, Makan↗

DOE OSTI2024

Optimizing spectral phase transfer in four-wave mixing with gas-filled capillaries

Four-wave mixing (FWM) in gas-filled hollow-core capillaries, a nonlinear optical process that mixes signal and pump photon frequencies to generate idler frequency photons, offers a method for precise spectral phase transfer from signal to idler at ultrashort timescales and extreme powers. However, this regime is challenged by competing linear and nonlinear dynamics, leading to significant trade-offs between spectral phase transfer and conversion efficiency. Our computational investigation focuses on the upconversion of femtosecond pulses from the infrared (IR) to the ultraviolet (UV), a range notoriously difficult to manipulate. We explore an intermediate energy regime that strikes an optimal balance between FWM-mediated phase-transfer fidelity and nonlinear conversion efficiency. By adjusting the energy ratios and spectral phase profiles of the input signal, we achieve conversion efficiencies of approximately 5-15% while maintaining an effective quasi-linear spectral phase transfer. These findings will contribute to establishing first-principles and scaling laws essential for applications such as high-precision imaging, spectroscopy, quantum transduction, and distributed entangled interconnects, facilitating advanced control of ultrafast photonic and electronic wavepackets in quantum materials with unprecedented spatial and temporal precision.

Zhang, Hao↗

NASA NTRS1998

Fabrication and Atomic Force Microscopy Characterization of Molecular Composites of Fullerenes in Aerogel Matrix for Optical Limiting

An optical limiter is a device which exhibits a decrease in the transmittance in a material with an increase in intensity of light. Sol-gel techniques offer many advantages in the fabrication of materials. These materials possess many desirable properties for nonlinear optical (NLO) device applications which include transparency, high thermal and chemical stabilities, very low refractive index and dielectric constants. C60 shows a higher excited state absorption cross section than the ground state absorption cross section over the complete visible spectrum, and the spectrum of the excited state absorption of C60 has the same general shape as the ground state absorption. This fact suggests that fullerenes are ideal optical limiting materials. Aerogels are fabricated by sol-gel processing. One of the key issues is the dispersion of fullerenes into small and uniform pores of silica aerogel host matrices. The aerogel network was characterized by Raman spectroscopy. Atomic force microscopy is a technique with many advantages to characterize the aerogel materials. The morphology of the cleaved surface for a C60/aerogel sample shows that there are long paralleled shaped stripes with 20-30 nm in width and about 500 nm in length on the cleaved surface. The cleaved surface also was etched by 5% HF solution for one minutes, and it became smoother after HF etching. The main feature in on the surface is the spherical particles with the size of few nanometers, and no aggregated fullerenes appear. The fullerenes are well dispersed in the aerogel matrices.

Lu, W. J .↗

DOE OSTI2024

Strain-concentration for fast, compact photonic modulation and non-volatile memory

A critical figure of merit (FoM) for electro-optic (EO) modulators is the transmission change per voltage, d T / d V . Conventional approaches in wave-guided modulators maximize d T / d V via a high EO coefficient or longer light-material interaction lengths but are ultimately limited by material losses and nonlinearities. Optical and RF resonances improve d T / d V at the cost of spectral non-uniformity, especially for high- Q optical cavity resonances. Here, we introduce an EO modulator based on piezo-strain-concentration of a photonic crystal cavity to address both trade-offs: (i) it eliminates the trade-off between d T / d V and waveguide loss—i.e., enhancement of the resonance tuning efficiency d v c / d V for the fixed EO coefficient, waveguide length, and cavity Q —and (ii) at high DC strains it exhibits a non-volatile (NV) cavity tuning Δ v c ,NV for passive memory and programming of multiple devices into resonance despite fabrication variations. The device is fabricated on a scalable silicon nitride-on-aluminum nitride platform. We measure d v c / d V =177±1MHz/V, corresponding to Δ v c =40±0.32GHz for a voltage spanning ±120V with an energy consumption of δ U /Δ v c =0.17nW/GHz. The modulation bandwidth is flat up to ω BW,3dB /2 π =3.2±0.07MHz for broadband DC-AC and 142±17MHz for resonant operation near a 2.8 GHz mechanical resonance. Optical extinction up to 25 dB is obtained via Fano-type interference. Strain-induced beam-buckling modes are programmable under a “read-write” protocol with a continuous, repeatable tuning range of 5±0.25GHz, allowing for storage and retrieval, which we quantify with mutual information of 2.4 bits and a maximum non-volatile excursion of 8 GHz. Using a full piezo-optical finite-element-model (FEM) we identify key design principles for optimizing strain-based modulators and chart a path towards achieving performance comparable to lithium niobate-based modulators and the study of high strain physics on-chip.

Wen, Y. Henry (ORCID:0009000685423628)↗

NASA NTRS1998

Nonlinear Optothermal Properties of Metal-Free Phthalocyanine

The nonlinear optical properties of metal-free phthalocyanine (MFPC) thin films were examined using the second harmonic at 532 nm from a pulsed Nd:YAG laser, and the cw He-Ne , and Ar+ lasers. The He-Ne laser transmission at fixed input intensity was found to increase temporally within a time scale of twelve hours. The origin of this temporal change of transmission is discussed. The third order nonlinear susceptibilities (chi (exp(3))) by four-wave mixing were measured for films of different thickness. The saturation intensity of MFPC, and its absorption cross section, at 633 nm from a He-Ne laser, are reported. An optical bistability was recorded using a He-Ne laser. An AND logic gate was also demonstrated in the system. These phenomena in the system are attributed to refractive index modulation by thermal excitations.

Abdeldayem, Hossin A.↗

NASA NTRS1992

Solid-state lasers for coherent communication and remote sensing

Semiconductor-diode laser-pumped solid-state lasers have properties that are superior to other lasers for the applications of coherent communication and remote sensing. These properties include efficiency, reliability, stability, and capability to be scaled to higher powers. We have demonstrated that an optical phase-locked loop can be used to lock the frequency of two diode-pumped 1.06 micron Nd:YAG lasers to levels required for coherent communication. Monolithic nonplanar ring oscillators constructed from solid pieces of the laser material provide better than 10 kHz frequency stability over 0.1 sec intervals. We have used active feedback stabilization of the cavity length of these lasers to demonstrate 0.3 Hz frequency stabilization relative to a reference cavity. We have performed experiments and analysis to show that optical parametric oscillators (OPO's) reproduce the frequency stability of the pump laser in outputs that can be tuned to arbitrary wavelengths. Another measurement performed in this program has demonstrated the sub-shot-noise character of correlations of the fluctuations in the twin output of OPO's. Measurements of nonlinear optical coefficients by phase-matched second harmonic generation are helping to resolve inconsistency in these important parameters.

Byer, Robert L.↗