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NASA NTRS2008

Radiative Susceptibility of Cloudy Atmospheres to Droplet Number Perturbations: 1. Theoretical Analysis and Examples from MODIS

Theoretical and satellite-based assessments of the sensitivity of broadband shortwave radiative fluxes in cloudy atmospheres to small perturbations in the cloud droplet number concentration (N) of liquid water clouds under constant water conditions are performed. Two approaches to study this sensitivity are adopted: absolute increases in N, for which the radiative response is referred to as absolute cloud susceptibility, and relative increases in N or relative cloud susceptibility. Estimating the former is more challenging as it requires an assumed value for either cloud liquid water content or geometrical thickness; both susceptibilities require an assumed relationship between the droplet volume and effective radius. Expanding upon previous susceptibility studies, present radiative calculations include the effect of AN perturbations on droplet asymmetry parameter and single-scattering albedo, in addition to extinction. Absolute cloud susceptibility has a strong nonlinear dependence on the droplet effective radius as expected, while relative cloud susceptibility is primarily dependent on optical thickness. Molecular absorption and reflecting surfaces both reduce the relative contribution of the cloud to the top-of-atmosphere (TOA) flux and therefore also reduce the TOA albedo susceptibility. Transmittance susceptibilities are negative with absolute values similar to albedo susceptibility, while atmospheric absorptance susceptibilities are about an order of magnitude smaller than albedo susceptibilities and can be either positive or negative. Observation-based susceptibility calculations are derived from MODIS pixel-level retrievals of liquid water cloud optical thickness, effective radius, and cloud top temperature; two data granule examples are shown. Susceptibility quantifies the aerosol indirect effect sensitivity in a way that can be easily computed from model fields. As such, susceptibilities derived from MODIS observations provide a higher-order test of model cloud properties used for indirect effect studies. MODIS-derived global distributions of cloud susceptibility and radiative forcing calculations are presented in a companion paper.

Platnick, Steven↗

NASA NTRS1997

Microgravity Processing and Photonic Applications of Organic and Polymeric Materials

In recent years, a great deal of interest has been directed toward the use of organic materials in the development of high-efficiency optoelectronic and photonic devices. There is a myriad of possibilities among organics which allow flexibility in the design of unique structures with a variety of functional groups. The use of nonlinear optical (NLO) organic materials such as thin-film waveguides allows full exploitation of their desirable qualities by permitting long interaction lengths and large susceptibilities allowing modest power input. There are several methods in use to prepare thin films, such as Langmuir-Blodgett (LB) and self-assembly techniques, vapor deposition, growth from sheared solution or melt, and melt growth between glass plates. Organics have many features that make them desirable for use in optical devices such as high second- and third-order nonlinearities, flexibility of molecular design, and damage resistance to optical radiation. However, their use in devices has been hindered by processing difficulties for crystals and thin films. In this chapter, we discuss photonic and optoelectronic applications of a few organic materials and the potential role of microgravity on processing these materials. It is of interest to note how materials with second- and third-order nonlinear optical behavior may be improved in a diffusion-limited environment and ways in which convection may be detrimental to these materials.

Frazier, Donald O.↗

NASA NTRS1998

Microgravity Processing and Photonic Applications of Organic and Polymeric Materials

In recent years, a great deal of interest has been directed toward the use of organic materials in the development of high-efficiency optoelectronic and photonic devices. There is a myriad of possibilities among organic which allow flexibility in the design of unique structures with a variety of functional groups. The use of nonlinear optical (NLO) organic materials such as thin-film waveguides allows full exploitation of their desirable qualities by permitting long interaction lengths and large susceptibilities allowing modest power input. There are several methods in use to prepare thin films, such as Langmuir-Blodgett (LB) and self-assembly techniques, vapor deposition, growth from sheared solution or melt, and melt growth between glass plates. Organics have many features that make Abstract: them desirable for use in optical devices such as high second- and third-order nonlinearities, flexibility of molecular design, and damage resistance to optical radiation. However, their use in devices has been hindered by processing difficulties for crystals and thin films. In this chapter, we discuss photonic and optoelectronic applications of a few organic materials and the potential role of microgravity on processing these materials. It is of interest to note how materials with second- and third-order nonlinear optical behavior may be improved in a diffusion-limited environment and ways in which convection may be detrimental to these materials. We focus our discussion on third-order materials for all-optical switching, and second-order materials for all-optical switching, and second-order materials for frequency conversion and electrooptics.

Frazier, Donald 0↗

NASA NTRS1998

The Effects of Ground and Space Processing on the Properties of Organic, Polymeric, and Colloidal Materials

In recent years, a great deal of interest has been directed toward the use of organic materials in the development of high-efficiency optoelectronic and phototonic devices. There is a myriad of possibilities among organic materials which allow flexibility in the design of unique structures with a variety of functional groups. The use of nonlinear optical (NLO) organic materials as thin film wave-guides allows full exploitation of their desirable qualifies by permitting long interaction lengths and large susceptibilities allowing modest power input. There are several methods in use to prepare thin films such as Langmuir-Blodgett (LB) and self-assembly techniques, vapor deposition, growth from sheared solution or melt, and melt growth between glass plates. Organic-based materials have many features that make them desirable for use in optical devices, such as high second-and third-order nonlinearity, flexibility of molecular design, and damage resistance to optical radiation. However, their use in devices has been hindered by processing difficulties for crystals and thin films. We discuss the potential role of microgravity processing of a few organic and polymeric materials. It is of interest to note how materials with second-and third-order NLO behavior may be improved in a diffusion-limited environment and ways in which convection may be detrimental to these materials. We focus our discussion on third-order materials for all-optical switching, and second-order materials for frequency conversion and electrooptics. The goal of minimizing optical loss obviously depends on processing methods. For solution-based processes, such as solution crystal growth and solution photopolymerization, it is well known that thermal and solutal density gradients can initiate buoyancy-driven convection. Resultant fluid flows can affect transport of material to and from growth interfaces and become manifest in the morphology and homogeneity of the growing film or crystal. Likewise, buoyancy-driven convection can hinder production of defect-free, high-quality crystals or films during crystal and film growth by vapor deposition.

Frazier, Donald O.↗

DOE OSTI2025

Second-order microscopic nonlinear susceptibility in a centrosymmetric material: application to imaging valence electron motion

We report measurements of phase-matched nonlinear x-ray and optical sum-frequency generation from single-crystal silicon using sub-resonant 0.95 eV laser pulses and 9.5 keV hard x-ray pulses from the LCLS free-electron laser. The sum-frequency signal appears as energy and momentum sidebands to the elastic Bragg peak. It is proportional to the magnitude squared of the relevant temporal and spatial Fourier components of the optically induced microscopic charges/currents. We measure the first- and second-order sideband to the 220 Bragg peak and find that the efficiency is maximized when the applied field is along the reciprocal lattice vector. For an optical intensity of $\sim10^{12} \text{W}/\text{cm}^2$, we measure peak efficiencies of $3\times 10^{-7}$ and $3\times 10^{-10}$ for the first and second-order sideband respectively (relative to the elastic Bragg peak). The first-order sideband is consistent with induced microscopic currents along the applied electric field (consistent with an isotropic response). The second-order sideband depends nontrivially on the optical field orientation and is consistent with an anisotropic response originating from induced charges along the bonds with C$_{3v}$ site symmetry. The results agree well with first-principles Bloch-Floquet calculations.

FOS: Physical sciences↗

DOE OSTI2025

Full complex amplitude control of second-harmonic generation via electrically tunable intersubband polaritonic metasurfaces

Nonlinear intersubband polaritonic metasurfaces based on coupling of the intersubband nonlinear optical response of quantum-engineered semiconductor heterostructures and electromagnetic modes of nanoresonators provide efficient frequency mixing with moderate pump intensities. The resonant nonlinear optical response, represented as a complex function, can be modulated via Stark tuning of intersubband transition energies under applied voltages. However, achieving full complex amplitude control (both phase and magnitude) remains challenging. In this work, we present and experimentally validate electrically tunable nonlinear intersubband polaritonic metasurfaces that achieve complete complex amplitude control for second-harmonic generation (SHG). Through a design featuring two in-plane flipped meta-atoms per unit cell, we achieve complete electrical control of both the amplitude and phase of the metasurface second-order nonlinear susceptibility, with a tuning range of 0 to 30 nm V −1 for the magnitude and 0-2π for the phase of the nonlinear optical response. Using these properties, we achieve complete on-off SHG modulation and beam diffraction tuning through electrically controlled amplitude and phase gratings.

Science & Technology - Other Topics↗

DOE OSTI2025

Simulating quantum-classical interfaces via the Lindblad master equation

In hybrid quantum systems, the interface between quantum and classical domains is essential for the generation, control, and measurement of quantum states. Quantum-classical interfaces (QCIs) are ubiquitous in devices such as optical modulators, quantum sensors, and signal processors, where classical signals influence quantum dynamics. In this paper, we employ the Lindblad master equation to simulate the evolution of a quantum system interacting with a classical control system. Our model captures both linear and nonlinear interactions by incorporating first- and second-order susceptibilities, and it quantifies the influence of externally applied control parameters on decoherence and state evolution. As an illustrative example, we analyze an optical modulator and demonstrate how variations in material response and drive conditions affect photon statistics, coherence, and phase-space distributions. In conclusion, the findings offer a path to an all-encompassing model for understanding and optimizing QCIs, with wide-ranging implications for the performance, design, and robustness of next-generation quantum devices.

Quantum engineering↗

NASA NTRS1997

Validity Using Pump-Probe Pulses to Determine the Optical Response of Niobate Crystals

A variety of niobate crystals have found their places in nonlinear optical applications as well as in laser devices. In recent years much attention has been paid to study the ultrafast optical response in a variety of photorefractive crystals such as KTa(1-x)Nb(x)O3 and KNbO3 crystals, glasses, semiconductors and polymers for applications in optical switching, information processing, optical computing, and all-optical device systems. Third-order optical nonlinearity is the most important property for realization of all-optical switching. Therefore experiments have been performed on the third order susceptibility using a variety of techniques such as the third-order harmonic generation, EFISH and degenerate four-wave mixing(DFWM). The latter has been conducted with a variety of pump wavelengths and with nanosecond, picosecond and femtosecond pulses. Niobate crystals, such as potassium niobate KNbO3, potassium tantalate niobate KTN family (KTa(1-x)Nb(x)O3), strontium barium niobate SBN (Sr(x)Ba(1-x)Nb2O6) and potassium-sodium niobate SBN (KNSBN) are attractive due to their photorefractive properties for application in optical storage and processing. The pulsed probe experiments performed on theses materials have suggested two types of time responses. These responses have been associated with an coherent response due to Chi(sup 3), and a long lived component due to excited state population. Recent study of DFWM on KNbO3 and KTN family reveals that the long lived component of those crystals depends on the crystal orientation. A slowly decaying signal is observable when the grating vector K(sub g) is not perpendicular to the C-axis of those photorefractive crystals', otherwise the optical response signal would be only a narrow coherent peak with FWHM equal to the cross-correlation width of the write beam pulses. Based on this understanding, we study the photodynamical process of a variety of niobate crystals using DFWM in a Kg perpindicular to C geometry with a ps-YAG: Nd laser operating at 532nm. However, the discrepancies in numerical estimations of Chi(sup 3) in these materials and other nonlinear optical media have resulted in a number of discussions. In order to better understand the photodynamical process of niobate crystals after an short pulse excitation we analyze the factors governing the coherent signal and present the DFWM spectra of niobate crystals.

Liu, Huimin↗

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.↗

DOE OSTI2024

Quantum limits of superconducting-photonic links and their extension to millimeter waves

Photonic addressing of superconducting circuits has been proposed to overcome wiring complexity and heat-load challenges. However, such superconducting-photonic links suffer from an efficiency-noise trade-off that limits scalability. This trade-off arises because increasing power conversion efficiency entails reducing optical power, which makes the converted signal susceptible to shot noise. We analyze this trade-off and find that the laser-driven qubit gate infidelity scales inversely with the number of photons used. While methods such as nonlinear detection or squeezed light could mitigate this effect, we consider generating higher-frequency electrical signals, such as millimeter waves (100 GHz), using laser light. At these higher frequencies, circuits have higher operating temperatures and cooling power budgets and alleviate constraints posed by the trade-off. Therefore, we demonstrate an optically driven cryogenic millimeter-wave source with a maximum power efficiency of 8 ×10 −5 that can generate a maximum of 0.7 μ⁢W of 80 GHz power, with a 1200-thermal-photon equivalent of added noise at 4K. Using this source, we perform frequency-domain spectroscopy of superconducting NbTiN resonators at 80–90 GHz. Our results show a promising approach to lessen the efficiency-noise constraints on superconducting-photonic links, while leveraging the benefits of photonic signal delivery. Further optimization of power efficiency and noise at high frequencies could make scalable photonic control of superconducting qubits viable at temperatures exceeding 1K.

Optoelectronics↗

DOE OSTI2024

Second-harmonic generation tensors from high-throughput density-functional perturbation theory

Optical materials play a key role in enabling modern optoelectronic technologies in a wide variety of domains such as the medical or the energy sector. Among them, nonlinear optical crystals are of primary importance to achieve a broader range of electromagnetic waves in the devices. However, numerous and contradicting requirements significantly limit the discovery of new potential candidates, which, in turn, hinders the technological development. In the present work, the static nonlinear susceptibility and dielectric tensor are computed via density-functional perturbation theory for a set of 579 inorganic semiconductors. The computational methodology is discussed and the provided database is described with respect to both its data distribution and its format. Several comparisons with both experimental and ab initio results from literature allow to confirm the reliability of our data. The aim of this work is to provide a relevant dataset to foster the identification of promising nonlinear optical crystals in order to motivate their subsequent experimental investigation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Tunable Semiconducting Behavior and Linear-Nonlinear Optical Properties of Ag–Sn Dual-Doped Nanocrystalline CdO Thin Films for Optoelectronics

Semiconductor-based thin films have a great impact on determining the anticipated optoelectronic device construction and the advancement of cutting-edge applications. Herein, Ag and Sn dual-doped nanocrystalline transparent conducting CdO thin films were prepared on glass substrates using a cost-effective spray coating method, and their structural, morphological, optical, and semiconducting behaviors were investigated. The successful incorporation of Ag and Sn resulted in the polycrystalline nature of the deposited films without the additional peaks, as verified by X-ray diffraction (XRD) analysis. The XRD report also revealed the enhanced crystallinity (65%) at the higher doping level (3 wt % Ag and Sn-doped CdO film). All the deposited CdO films exhibited homogeneous, spherical, or round-shaped grains, with agglomeration revealed by scanning electron microscopy analysis. UV–visible spectroscopy was utilized to determine the linear and nonlinear optical properties of the deposited CdO thin films, and a reduction in the band gap from 3.891 to 3.772 eV was observed. A significant enhancement in the first- and third-order nonlinear susceptibility and nonlinear refractive index of the doped CdO films was also observed with increasing doping concentration. Hall effect data were collected at room temperature to investigate the electrical properties of all of the CdO films. The charge carrier concentration of CdO thin films was increased from 142.08 × 10 18 to 169.10 × 10 18 cm –3 , and the highest conductivity was found to be 192 s/cm on doping 3 wt % Ag–Sn. All the CdO thin films exhibited n-type conductivity, while an incredible n-type to p-type charge carrier transition was noticed at a higher doping level (3 wt % Ag–Sn). The findings of the current work are expected to advance the synthesis of semiconductor thin films through cost-effective spray coating methods for optoelectronic device applications.

deposition↗

DOE OSTI2024

Giant optical second- and third-order nonlinearities at a telecom wavelength

A material platform that excels in both optical second- and third-order nonlinearities at a telecom wavelength is theoretically and experimentally demonstrated. In this TiN-based coupled metallic quantum well structure, electronic subbands are engineered to support doubly resonant inter-subband transitions for an exceptionally high second-order nonlinearity and provide single-photon transitions for a remarkable third-order nonlinearity within the 1400–1600 nm bandwidth. The second-order susceptibility χ (2) reaches 2840 pm/V at 1440 nm, while the Kerr coefficient n 2 arrives at 2.8 × 10 −10 cm 2 /W at 1460 nm. The achievement of simultaneous strong second- and third-order nonlinearities in one material at a telecom wavelength creates opportunities for multi-functional advanced applications in the field of nonlinear optics.

Chen, Ching-Fu (ORCID:0000000262510722)↗

NASA NTRS1993

Nonlinear optical parameters of 7-prime,7-prime-dicyano-7-prime-apo-beta-carotene in hexane by self-action techniques

Quantitative measurements of the nonlinear refractive index coefficient n(2) and the third-order nonlinear susceptibility chi(3) for a solution of 7-prime,7-prime-dicyano-7-prime-apo-beta-carotene (DCAC) in hexane have been measured at different concentrations. The measurements have been performed by both the self-trapping and self-phase modulation techniques using a CW Ar(+) laser. The results show that DCAC has a relatively large nonlinearity, attributed to a thermal mechanism, with n(2) of the order of 10 exp 9 times that of CS2.

Abdeldayem, Hossin A.↗

DOE OSTI2024

Harnessing complexity: Nonlinear optical phenomena in L-shapes, nanocrescents, and split-ring resonators

Here, we conduct systematic studies of the optical characteristics of plasmonic nanoparticles that exhibit C 2v symmetry. In particular, we analyze three distinct geometric configurations: an L-type shape, a crescent, and a split-ring resonator shaped like the Greek letter π. Optical properties are examined using the finite-difference time-domain method. It is demonstrated that all three shapes exhibit two prominent plasmon modes associated with the two axes of symmetry. This is in addition to a wide range of resonances observed at high frequencies corresponding to quadrupole modes and peaks due to sharp corners. Next, to facilitate nonlinear analysis, we employ a semiclassical hydrodynamic model, where the electron pressure term is explicitly accounted for. This model goes beyond the standard Drude description and enables capturing nonlocal and nonlinear effects. Employing this model enables us to rigorously examine the second-order angular resolved nonlinear optical response of these nanoparticles in each of the three configurations. Two pumping regimes are considered, namely, continuous wave (CW) and pulsed excitations. For CW pumping, we explore the properties of the second harmonic generation (SHG). Polarization and angle-resolved SHG spectra are obtained, revealing strong dependence on the nanoparticle geometry and incident wave polarization. The C 2v symmetry is shown to play a key role in determining the polarization states and selection rules of the SHG signal. For pulsed excitations, we discuss the phenomenon of broadband terahertz (THz) generation induced by the difference-frequency generation . It is shown that the THz emission spectra exhibit unique features attributed to the plasmonic resonances and symmetry of the nanoparticles. The polarization of the generated THz waves is also examined, revealing interesting patterns tied to the nanoparticle geometry. To gain deeper insight, we propose an analytical theory that agrees very well with the numerical experiments. The theory shows that the physical origin of the THz radiation is the mixing of various frequency components of the fundamental pulse by the second-order nonlinear susceptibility. An expression for the far-field THz intensity is derived in terms of the incident pulse parameters and the nonlinear response tensor of the nanoparticle. The results presented in this work offer new insights into the linear and nonlinear optical properties of nanoparticles with C 2v symmetry. The demonstrated strong SHG response and efficient broadband THz generation hold great promise for applications in nonlinear spectroscopy, nanophotonics, and optoelectronics. The proposed theoretical framework also provides a valuable tool for understanding and predicting the nonlinear behavior of other related nanostructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Reverse Polarizability of Rare Earth Ions (La 3+ , Gd 3+ , Lu 3+ , Y 3+ ) in Tellurite Glasses and Glass Ceramics for Optical Limiting

All-optical modulation using inherent third-order optical nonlinearity of a medium has garnered considerable interest in photonics and optoelectronics. Herein, nonlinear optical (NLO) properties of tellurite glasses and glass ceramics (GCs) containing four different rare earths (RE = La, Gd, Lu, and Y) have been deliberated in near-infrared regions under an ultrafast regime. The La-based glass exhibits ~10 times higher nonlinear refraction (n 2 ) and absorption (α 2 ) than reported NLO materials. The NLO susceptibility [χ (3) ] trend in the studied glasses is La > Gd > Lu > Y, matching with RE 3+ polarizability. Furthermore, Ln 2 Te 6 O 15 nanocrystallite-embedded transparent GCs exhibit a larger NLO coefficient due to the enhanced local field from oxygen vacancies in crystallites. Interestingly, the trend of χ (3) in GCs follows the sequence of Y > Lu > Gd > La, precisely opposite to the glasses. This observation challenges the general polarizability approach of RE 3+ ions, emphasizing that quadratic hyperpolarizability of RE 3+ is pivotal for NLO properties of GCs. Among the studied matrices, Y-containing GCs showed the lowest optical limiting (OL) threshold (5.4 mJ/cm 2 at 800 nm), much lower than those of the reported NLO materials, suggesting its potential as a femtosecond NIR-laser safety material. A combination of large α 2 and n 2 from the studied matrices indicates their advantage for harmonic generation, potentially aiding in the design of ultrafast signal processing devices.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Exciton Enhanced Nonlinear Optical Responses in Monolayer h-BN and MoS 2 : Insight from First-Principles Exciton-State Coupling Formalism and Calculations

Excitons are vital in the photophysics of materials, especially in low-dimensional systems. The conceptual and quantitative understanding of excitonic effects in nonlinear optical (NLO) processes is more challenging compared to linear ones. Here, we present an ab initio approach to second-order NLO responses, incorporating excitonic effects, that employs an exciton-state coupling formalism and allows for a detailed analysis of the role of individual excitonic states. Taking monolayer h-BN and MoS 2 as two prototype 2D materials, we calculate their second harmonic generation (SHG) susceptibility and shift current conductivity tensor. We find strong excitonic enhancement in the NLO responses requires that the resonant excitons are not only optically bright themselves but also able to couple strongly to other bright excitons. Our results explain the occurrence of two strong peaks in the SHG of monolayer h-BN and why the A and B excitons of MoS 2 unexpectedly exhibit minimal excitonic enhancement in both SHG and shift current generation.

36 MATERIALS SCIENCE↗

NASA NTRS2001

Mechanisms for the Crystallization of Zblan

The heavy metal fluoride glasses represent a class of reasonably good glass forming compositions with very unique infrared optical properties that have been of interest to researchers for 20 years. The most extensively studied glass with the most potential for practical applications is ZBLAN which contains the fluorides of zirconium, barium, lanthanum, aluminum, and sodium. It has a broad transmission range (0.3-6 um), low index of refraction (about 1.43), low dispersion, low Raleigh scattering, ultra-low thermal 2 dispersion, and potential ultra-low signal attenuation. Potential applications include fiber amplifiers, fiber optic gyroscopes, delivery systems for laser cutting, drilling and surgery, radiation resistant data links, nonlinear optical systems, and ultra-low-loss repeater-less transcontinental and transoceanic optical fiber. Potential markets for these materials are in the tens of billions of dollars per year. Optical fiber from this system possess excellent transmission characteristics in the IR, but the glass is somewhat susceptible to nucleation and crystallization. The theoretical intrinsic loss coefficient for ZBLAN at 2 microns is 0.00 1 dB/Km. Extrinsic losses, however, cause significant attenuation. The lowest loss coefficient measured is 0.7 dB/Km. This compares with the loss coefficient for fiber optic grade fused silica glass of 0.2 dB/Km. The extrinsic losses in ZBLAN have been attributed to 1) impurities which might be lowered by containerless processing and 2) to scattering from micro-crystallites that form during glass preform production or during fiber drawing.

Ethridge, Edwin C.↗