Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “nonlinear optical response”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
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↗
DOE OSTI2022

Multifunctional Cu 2 TSiS 4 (T = Mn and Fe): Polar Semiconducting Antiferromagnets with Nonlinear Optical Properties

In this work, Cu 2 TSiS 4 (T = Mn and Fe) polycrystalline and single-crystal materials were prepared with high-temperature solid-state and chemical vapor transport methods, respectively. The polar crystal structure (space group Pmn2 1 ) consists of chains of corner-sharing and distorted CuS 4 , Mn/FeS 4 , and SiS 4 tetrahedra, which is confirmed by Rietveld refinement using neutron powder diffraction data, X-ray single-crystal refinement, electron diffraction, energy-dispersive X-ray spectroscopy, and second harmonic generation (SHG) techniques. Magnetic measurements indicate that both compounds order antiferromagnetically at 8 and 14 K, respectively, which is supported by the temperature-dependent (100–2 K) neutron powder diffraction data. Additional magnetic reflections observed at 2 K can be modeled by magnetic propagation vectors k = (1/2,0,1/2) and k = (1/2,1/2,1/2) for Cu 2 MnSiS 4 and Cu 2 FeSiS 4 , respectively. The refined antiferromagnetic structure reveals that the Mn/Fe spins are canted away from the ac plane by about 14°, with the total magnetic moments of Mn and Fe being 4.1(1) and 2.9(1) μ B , respectively. Both compounds exhibit an SHG response with relatively modest second-order nonlinear susceptibilities. Density functional theory calculations are used to describe the electronic band structures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

TRUST Contact Thermal Conductance (TRUST-CTC) Report: FY24

The objective of the Delivery Environments (DE) Testbeds to Reduce Uncertainties in Simulations and Tests (TRUST) project is to quantify and help increase confidence in specific areas of computational and experimental capabilities that are applicable to current and future delivery environments. More complete quantification of confidence in experimental and computational capabilities and the sufficient increase of confidence in those capabilities is critical to improving weapons engineering design, qualification, and assessment efforts that are critical to the current and future stockpile. Staff development will include cross-discipline collaboration to provide engineers with experience in both numerical simulations and experimental methods. This work uses and provides feedback on analysis tools and experimental results databases for efficient and responsive engineering which are currently under development. TRUST currently includes five testbeds and their associated engineering analysis baseline models (EABMs): 1. contact thermal conductivity, (CTC) 2. nonlinear dynamics, (ND) 3. sensors in environments for accelerometers, (SEA) 4. sensors in environments for fiber optic displacement gages, and (SEFOD) 5. sensors in environments for thermocouples (SETC). The TRUST project uses single-feature testbeds to quantify uncertainties in specific models and experiments and to identify capability development needs that can help to reduce these uncertainties. Each testbed is designed, configured, and tested in collaboration with groups with design and experimental capability: E-14 and MPA-CINT. The complementary simulations are conducted using W-13 analysis tools and stored in model repositories with plans for incremental progress toward EABM requirements. W-13 extends and exercises the testbed simulations in collaboration with experimentalists for uncertainty quantification of current and future materials, geometries, and environments. Additionally, TRUST is intended to provide engineers in W-13 and E-14 with experience in both numerical simulations and experimental methods through cross-discipline collaborations. Following the introduction to the TRUST project, the remainder of this report focuses on experimental and analytical efforts conducted in Fiscal Year (FY) 2024 relevant to the TRUST Contact Thermal Conductance (CTC) testbed.

42 ENGINEERING↗
DOE OSTI2020

Highly Tunable Thiol-Ene Photoresins for Volumetric Additive Manufacturing

Volumetric additive manufacturing (VAM) forms complete 3D objects in a single photocuring operation without layering defects, enabling 3D printed polymer parts with mechanical properties similar to their bulk material counterparts. This study presents the first report of VAM-printed thiol-ene resins. With well-ordered molecular networks, thiol-ene chemistry accesses polymer materials with a wide range of mechanical properties, moving VAM beyond the limitations of commonly used acrylate formulations. Since free-radical thiol-ene polymerization is not inhibited by oxygen, the nonlinear threshold response required in VAM is introduced by incorporating 2,2,6,6-tetramethyl-1-piperidinyloxy (TEMPO) as a radical scavenger. Tuning of the reaction kinetics is accomplished by balancing inhibitor and initiator content. Coupling this with quantitative measurements of the absorbed volumetric optical dose allows control of polymer conversion and gelation during printing. Importantly, this work thereby establishes the first comprehensive framework for spatial–temporal control over volumetric energy distribution, demonstrating structures 3D printed in thiol-ene resin by means of tomographic volumetric VAM. Mechanical characterization of this thiol-ene system, with varied ratios of isocyanurate and triethylene glycol monomers, reveals highly tunable mechanical response far more versatile than identical acrylate-based resins. This broadens the range of materials and properties available for VAM, taking another step toward high-performance printed polymers.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Quantum sensing of paramagnetic analytes by nanodiamonds in levitated microdroplets and aqueous solutions

Nanodiamonds (ND) hosting negatively charged nitrogen-vacancy (NV-) color centers have received attention for applications in magnetic field, electric field, chemical, and bio-sensing. The versatility of these probes is their excellent room-temperature optical and spin properties, along with their small size, functionalized surfaces and resistance to bleaching, making them ideal as nanoscopic sensors in picoliter volumes (e.g. single cells, but also microcompartments and aerosols). For quantitative ND-NV- sensing of paramagnetic analytes in such contexts, however, there remains an incomplete understanding of how factors related to the aqueous phase environment control detection efficiency. To address this, optically detected magnetic resonance (ODMR) is measured in bulk macroscale solutions and single levitated microdroplets as a function of Gd+3 concentration (340 nM to 1.5 mM), nanodiamond size, pH, competitor ions, and ligands. The ODMR response to [Gd+3] is found to be nonlinear, and pH, ND and sample volume dependent; indicating the detection of Gd+3 requires efficient adsorption of the analyte to the diamond surface. Langmuir adsorption isotherms embedded in a quantitative photophysical model links the ODMR response to adsorption thermodynamics of Gd+3. The equilibrium constant for Gd+3 adsorption to a carboxylated ND surface is determined to be (1 ± 0.5) x 105 M-1 corresponding to a free energy of adsorption of (-28 ± 1) kJ mol-1. These results provide general insight into how complex aqueous and microscale environments impact nanodiamond based quantum sensing modalities, and portend their application as quantitative chemical sensors in microenvironments.

Brown, Emily K↗
DOE OSTI2024

Electrochemical Control of the Ultrafast Lattice Response of a Layered Semimetal

The unique layer-stacking in two-dimensional (2D) van der Waals materials facilitates the formation of nearly degenerate phases of matter and opens novel routes for the design of low-power, reconfigurable functional materials. Electrochemical ion intercalation between stacked layers offers a promising approach to stabilize bulk metastable phases and to explore the effects of extreme carrier doping and strain. However, in situ characterization methods to study the structural evolution and dynamical functional properties of these intercalated materials remains limited. Here a novel experimental platform is presented capable of simultaneously performing electrochemical lithium-ion intercalation and multimodal ultrafast characterization of the lattice using both electron diffraction and nonlinear optical techniques. Using the layered semimetal WTe 2 as a model system, the interlayer shear phonon mode that modulates stacking between 2Dlayers is probed, showing that small amounts of lithiation enhance the amplitude and lifetime of the phonon, contrary to expectations. This results from the dynamically fluctuating and anharmonic structure between nearly degenerate phases at room temperature, which can be stabilized by electronic carriers accompanying the inserted lithium ions. At high lithiation, the T d ’ structure emerges and quenches the phonon response. This work defines new approaches for using electrochemistry to engineer the dynamic structure of 2D materials.

36 MATERIALS SCIENCE↗
NASA NTRS2001

Synthesis of Two-Photon Materials and Two-Photon Liquid Crystals

The duration of the grant was interrupted by two major accidents that the PI met with-- an auto accident in Pasadena, CA during her second summer at JPL which took almost eight months for recovery and a second accident during Fall 2000 that left her in crutches for the entire semester. Further, the time released agreed by the University was not given in a timely fashion. The candidate has been given post-grant expire time off. In spite of all these problems, the PI synthesized a number of new two-photon materials and studied the structure-activity correlation to arrive at the best-optimized structure. The PI's design proved to be one of the best in the sense that these materials has a hitherto unreported two-photon absorption cross section. Many materials based on PI's design was later made by the NASA colleague. This is Phase 1. Phase II of this grant is to orate liquid crystalline nature into this potentially useful materials and is currently in progress. Recent observations of nano- and pico-second response time of homeotropically aligned liquid crystals suggest their inherent potentials to act as laser hardening materials, i.e., as protective devices against short laser pulses. The objective of the current project is to exploit this potential by the synthesis of liquid crystals with high optical nonlinearity and optimizing their performance. The PI is trying structural variations to bring in liquid crystalline nature without losing the high two-photon cross section. Both Phase I and Phase II led to many invited presentations and publications in reputed journals like 'Science' and 'Molecular Crystals'. The list of presentations and reprints are enclosed. Another important and satisfying outcome of this grant is the opportunity that this grant offered to the budding undergraduate scientists to get involved in a visible research of international importance. All the students had a chance to learn a lot during research, had the opportunity to present their work at the National level conferences. They continue to retain their interest in their research and went on to accomplish further laurels.

Subramaniam, Girija↗
NASA NTRS1991

Nonlinear optical properties of organic materials: A theoretical study

Replacement of electronic switching circuits in computing and telecommunication systems with purely optical devices offers the potential for extremely high throughput and compact information processing systems. The potential application of organic materials containing molecules with large nonresonant nonlinear effects in this area have triggered intensive research during the last decade. Interest on this area was due to two facts: (1) that many organic materials show nonlinearities that are orders of magnitude larger than those of conventional inorganic materials such as lithium niobate and potassium dihydrogen phosphate; and (2) that organic materials show much flexibility in terms of molecular designs. Some of the desirable characteristics that these materials should have are that they be transparent to the frequency of the incident laser and its second or third harmonic, that they have a high damage threshold, and, in the case of second-order effects, that their crystal structure or molecular orientation be accentric. Since polymeric assemblages can enhance the nonlinear response of organic molecules severalfold, efforts have been directed toward the synthesis of thin films with interpenetrating lattices of electroactive molecules. The goal of this theoretical investigation is to predict the magnitude of the molecular polarizabilities of organic molecules that could be incorporated into films. These calculations are intended to become a powerful tool to assist material scientists in screening for the best candidates for optical applications. The procedure that was developed for the present calculations is based on the static-field approach, and is a modification to the method developed by Dewar and Stewart, 1984 for calculating molecular linear polarizabilities.

Cardelino, Beatriz H.↗
DOE OSTI2025

High harmonic generation in Haldane model quantum dots

We study theoretically the nonlinear electron dynamics of Haldane model quantum dots placed in the field of an ultrashort optical pulse. One of the tuning parameters of the Haldane model is the phase accumulated by an electron during its transfer between the next nearest neighbor sites. We study how this parameter affect the nonlinear electron dynamics and the generation of high optical harmonics. With increasing the phase from its zero value to 90°, the low-energy electron states in the conduction and valence bands become more localized near the edges of the quantum dot resulting in suppression of the band gap, enhancement of the dipole inter-band coupling, and strong suppression of the average low-energy electron density of the states. As a result, the nonlinear response of the electron system of a Haldane model quantum dot is the strongest at intermediate values of the phase, ≈ 30− 40°. At these values of the phase, the electron dynamics is irreversible and a few first high-order harmonics have the largest intensities. Here, when the phase approaches 90° value the generation of high harmonics is strongly suppressed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Linear response of molecular polaritons

In this article, we show that the collective light–matter strong coupling regime where N molecular emitters couple to the photon mode of an optical cavity can be mapped to a quantum impurity model where the photon is the impurity that is coupled to a bath of anharmonic transitions. In the thermodynamic limit where N ≫ 1, we argue that the bath can be replaced with an effective harmonic bath, leading to a dramatic simplification of the problem into one of the coupled harmonic oscillators. We derive simple analytical expressions for linear optical spectra (transmission, reflection, and absorption) where the only molecular input required is the molecular linear susceptibility. This formalism is applied to a series of illustrative examples, showing the role of temperature, disorder, vibronic coupling, and optical saturation of the molecular ensemble, explaining that it is useful even when describing an important class of nonlinear optical experiments. For completeness, we provide Appendixes A–C that include a self-contained derivation of the relevant spectroscopic observables for arbitrary anharmonic systems (for both large and small N) within the rotating-wave approximation. While some of the presented results herein have already been reported in the literature, we provide a unified presentation of the results as well as new interpretations that connect powerful concepts in open quantum systems and linear response theory with molecular polaritonics.

Chemistry↗
DOE OSTI2023

In situ high-harmonic microscopy of a nanostructured solid

Nanostructured optical surfaces allow exquisite control over linear and nonlinear light interactions, where the surface actively creates new frequencies up to high-order harmonics of an intense infrared driving laser field. The function and performance of these surfaces depend sensitively on the distribution of the high-harmonic fields in and between the nanostructured elements, as the high-harmonic wavelength becomes comparable to the nanoscale features of the surface. Imaging the nonlinear response at the active surface with nanometer resolution would greatly benefit the optimization of the metasurface's function. Here we demonstrate an approach to lensless imaging of extreme ultraviolet high harmonics that resolves the amplitude and phase of nonlinear polarization at the active nanostructured surface of an MgO crystal. Imaging the near-field distribution of high harmonics is the gateway to optimized functional high-harmonic metasurfaces and the integration of high harmonics on a chip.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Synthesis, structure, linear and nonlinear optical properties of noncentrosymmetric quaternary diamond-like semiconductors, Cu 2 ZnGeSe 4 (CZGSe) and the novel Cu 4 ZnGe 2 Se 7

In this work, two quaternary diamond-like semiconductors (DLSs) in the Cu-Zn-Ge-Se system, the known Cu 2 ZnGeSe 4 (also referred to as CZGSe) and the new Cu 4 ZnGe 2 Se 7 , are compared in terms of their crystal structures, electronic structures and physicochemical properties. Both compounds were prepared by high-temperature, solid-state synthesis at 800 degrees C. Single crystal X-ray diffraction was used to determine the structure of Cu 4 ZnGe 2 Se 7 . The structures of both Cu 2 ZnGeSe 4 and Cu 4 ZnGe 2 Se 7 can be considered as derivatives of cubic diamond. Cu 4 ZnGe 2 Se 7 , with a reduced symmetry due to the cation ordering pattern, adopts the Cu 4 NiSi 2 S 7 structure type, with space group C2. The corner-sharing tetrahedra in Cu 4 ZnGe 2 Se 7 are slightly distorted because the charge for some of the S 2 - anions is not compensated by the first-nearest-neighbor cations. Rietveld refinements using synchrotron X-ray powder diffraction data were used to assess the phase purity of the samples and confirm the bulk structural behavior. Diffuse reflectance UV/Vis/NIR spectroscopy shows that Cu 2 ZnGeSe 4 and Cu 4 ZnGe 2 Se 7 have direct optical bandgaps of 1.38 and 0.91 eV, respectively. Electronic structure calculations implementing density functional theory confirm the direct bandgap for Cu 4 ZnGe 2 Se 7 , with a calculated value of 0.62 eV. Both compounds are air stable, thermally stable up to relatively high temperatures, undergo phase transitions and have wide windows of optical clarity. The Kurtz-Perry powder technique was used to determine the second harmonic generation (SHG) responses using a commercial AgGaSe 2 standard. While Cu 4 ZnGe 2 Se 7 displays a weak SHG response, Cu 2 ZnGeSe 4 exhibits a response that is greater than several benchmark materials, with a large SHG coefficient, χ (2) , of 43 ± 6 pm/V at λ = 2900 nm.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Multi-Functional Applications of H-Glass Embedded with Stable Plasmonic Gold Nanoislands

Metal nanoparticles (MNPs) are synthesized using various techniques on diverse substrates that significantly impact their properties. However, among the substrate materials investigated, the major challenge is the stability of MNPs due to their poor adhesion to the substrate. Herein, it is demonstrated how a newly developed H-glass can concurrently stabilize plasmonic gold nanoislands (GNIs) and offer multifunctional applications. The GNIs on the H-glass are synthesized using a simple yet, robust thermal dewetting process. The H-glass embedded with GNIs demonstrates versatility in its applications, such as i) acting as a room temperature chemiresistive gas sensor (70% response for NO 2 gas); ii) serving as substrates for surface-enhanced Raman spectroscopy for the identifications of Nile blue (dye) and picric acid (explosive) analytes down to nanomolar concentrations with enhancement factors of 4.8 × 10 6 and 6.1 × 10 5 , respectively; and iii) functioning as a nonlinear optical saturable absorber with a saturation intensity of 18.36 × 10 15 W m -2 at 600 nm, and the performance characteristics are on par with those of materials reported in the existing literature. In conclusion, this work establishes a facile strategy to develop advanced materials by depositing metal nanoislands on glass for various functional applications.

36 MATERIALS SCIENCE↗
NASA NTRS1996

Analysis of Measurements for Solid State Lidar Development

A Detector Characterization Facility (DCF), capable of measuring 2-micron detection devices and evaluating heterodyne receivers, was developed at the Marshall Space Flight Center. The DCF is capable of providing all the necessary detection parameters for design, development, and calibration of coherent and incoherent solid state laser radar (lidar) systems. The coherent lidars in particular require an accurate knowledge of detector heterodyne quantum efficient, nonlinearity properties, and voltage-current relationship as a function of applied optical power. At present, no detector manufacturer provides these qualities or adequately characterizes their detectors for heterodyne detection operation. In addition, the detector characterization facility measures the detectors DC and AC quantum efficiencies noise equivalent power and frequency response up to several GHz. The DCF is also capable of evaluating various heterodyne detection schemes such as balanced detectors and fiber optic interferometers. The design and analyses of measurements for the DCF were preformed over the previous year and a detailed description of its design and capabilities was provided in the NASA report NAS8-38609/DO77. It should also be noted that the DCF design was further improved to allow for the characterization of diffractive andholographical optical elements and other critical components of coherent lidar systems.

Amzajerdian, Farzin↗
DOE OSTI2021

Structure Tuning, Strong Second Harmonic Generation Response, and High Optical Stability of the Polar Semiconductors Na 1- x K x AsQ 2

We report the mixed cation compounds Na 1-x K x AsSe 2 (x = 0.8, 0.65, 0.5) and Na 0.1 K 0.9 AsS 2 crystallize in the polar noncentrosymmetric space group Cc. The AAsQ(2) (A = alkali metals, Q = S, Se) family features one-dimensional (1D) 1 / ∞ [AQ 2 - ] chains comprising corner-sharing pyramidal AQ 3 units in which the packing of these chains is dependent on the alkali metals. The parallel 1 / ∞ [AQ(2) - ] chains interact via short As ∙∙∙Se contacts, which increase in length when the fraction of K atoms is increased. The increase in the As ∙∙∙Se interchain distance increases the band gap from 1.75 eV in γ-NaAsSe 2 to 2.01 eV in Na 0.35 K 0.65 AsSe 2 , 2.07 eV in Na 0.2 K 0.8 AsSe 2 , and 2.18 eV in Na 0.1 K 0.9 AsS 2 . The Na 1-x K x AsSe 2 (x = 0.8, 0.65) compounds melt congruently at approximately 316 °C. Wavelength-dependent second harmonic generation (SHG) measurements on powder samples of Na 1-x K x AsSe 2 (x = 0.8, 0.65, 0.5) and Na 0.1 K 0.9 AsS 2 suggest that Na 0.2 K 0.8 AsSe 2 and Na 0.1 K 0.9 AsS 2 have the highest SHG response and exhibit significantly higher laser-induced damage thresholds (LIDTs). Theoretical SHG calculations on Na 0.5 K 0.5 AsSe 2 confirm its SHG response with the highest value of d 33 = 22.5 pm/V χ 333 (2) = 45.0 pm/V). The effective nonlinearity for a randomly oriented powder is calculated to be d eff = 18.9 pm/V χ eff (2) = 37.8 pm/V), which is consistent with the experimentally obtained value of d eff = 16.5 pm/V χ eff (2) = 33.0 pm/V). Three-photon absorption is the dominant mechanism for the optical breakdown of the compounds under intense excitation at 1580 nm, with Na 0.2 K 0.8 AsSe 2 exhibiting the highest stability.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe 2 .

Strong optical nonlinearities play a central role in realizing quantum photonic technologies. Exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such interactions is generally not sufficient to reach the regime of quantum nonlinear optics. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities. Here we demonstrate the formation of exciton-polaritons using excited excitonic states in monolayer tungsten diselenide (WSe 2 ) embedded in a microcavity. The realized excited-state polaritons exhibit an enhanced nonlinear response ~[Formula: see text] which is ~4.6 times that for the ground-state exciton. The demonstration of enhanced nonlinear response from excited exciton-polaritons presents the potential of generating strong exciton-polariton interactions, a necessary building block for solid-state quantum photonic technologies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1994

Nonlinear Optical Image Processing with Bacteriorhodopsin Films

The transmission properties of some bacteriorhodopsin film spatial light modulators are uniquely suited to allow nonlinear optical image processing operations to be applied to images with multiplicative noise characteristics. A logarithmic amplitude transmission feature of the film permits the conversion of multiplicative noise to additive noise, which may then be linearly filtered out in the Fourier plane of the transformed image. The bacteriorhodopsin film displays the logarithmic amplitude response for write beam intensities spanning a dynamic range greater than 2.0 orders of magnitude. We present experimental results demonstrating the principle and capability for several different image and noise situations, including deterministic noise and speckle. Using the bacteriorhodopsin film, we successfully filter out image noise from the transformed image that cannot be removed from the original image.

Downie, John D.↗