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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Giant Enhancement of Four-Wave Mixing by Doubly Zone-Folded Nonlocal Metasurfaces

Resonant optical metasurfaces hold promise for enhancing nonlinear optical signals and manipulating their fundamental properties. However, they rarely excel at amplifying signals from nonlinear processes with two incident pump beams, such as four-wave mixing (FWM) or sum-frequency generation. Frequency-mixing experiments impose challenging requirements for metasurface design due to the need to support multiple optical resonances with compatible field profiles at specified resonant wavelengths, often across a substantial spectral separation. Here, in this work, we introduce nonlocal ‘quadromer’ metasurfaces containing four nanostructures per unit cell as the key to unlocking configurable, multiresonant metasurfaces that enhance frequency-mixing processes. As a proof of concept, we experimentally demonstrate enhanced FWM using quadromer metasurfaces made of silicon and silicon-rich silicon nitride. The results are relevant for applications such as imaging of infrared light upconverted into the visible spectrum and the generation of quantum light via spontaneous FWM.

four-wave mixing↗
DOE OSTI2024

Ultrafast Symmetry Control in Photoexcited Quantum Dots

Symmetry control is essential for realizing unconventional properties, such as ferroelectricity, nonlinear optical responses, and complex topological order, thus it holds promise for the design of emerging quantum and photonic systems. Nevertheless, fast and reversible control of symmetry in materials remains a challenge, especially for nanoscale systems. Here, reversible symmetry changes are unveiled in colloidal lead chalcogenide quantum dots on picosecond timescales. Using a combination of ultrafast electron diffraction and total X-ray scattering, in conjunction with atomic-scale structural modeling and first-principles calculations, it is revealed that symmetry-broken lead sulfide quantum dots restore to a centrosymmetric phase upon photoexcitation. The symmetry restoration is driven by photoexcited electronic carriers, which suppress lead off-centering for about 100 ps. Furthermore, the change in symmetry is closely correlated with the electronic properties, and the bandgap transiently red-shifts in the symmetry-restored quantum dots. Overall, this study elucidates reversible symmetry changes in colloidal quantum dots, and more broadly defines a new methodology to optically control symmetry in nanoscale systems on ultrafast timescales.

36 MATERIALS SCIENCE↗
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 OSTI2026

Time-domain terahertz emission spectroscopy on van der Waals materials

Time-domain terahertz (THz) emission spectroscopy provides a direct method to probe transient photo-currents by recording the emitted terahertz electric field. Although the basic principles of THz surface emission have been understood for more than 30 years, the constant progress in ultrafast laser science to ever shorter pulses, the development of new materials and enhanced sensitivity promote THz emission spectroscopy as a reliable method to gain insights into charge carrier dynamics with unprecedented precision. It provides a versatile tool to study ultrafast processes, such as plasmon-driven hot carriers, dynamics of Dirac fermions, interfacial charge transfer, coherent phonon emission and quantum beating, to name only a few. However, despite the rapidly growing body of research on van der Waals materials, especially in their low-dimensional limit, THz emission spectroscopy has only been applied to a limited extent in these material systems. In this prospective, we review time-domain THz emission spectroscopy as a complementary approach to probe ultrafast charge carrier dynamics and the material’s nonlinear response. After a description of the experimental method, we report on THz emission spectroscopy of bulk and 2D van der Waals materials with special focus on graphene and transition metal dichalcogenide layers.

2D materials↗
DOE OSTI2026

Quantum control of Hubbard excitons

Quantum control of the many-body wavefunction is a central challenge in quantum materials research, as it could yield a precise control knob to manipulate emergent phenomena. Floquet engineering, the coherent dressing of quantum states with periodic non-resonant optical fields, has become an important strategy for quantum control. Most applications to solid-state systems have targeted weakly interacting or single-ion states, leaving the manipulation of many-body wavefunctions largely unexplored. Here, in this work, we use Floquet engineering to achieve quantum control of a strongly correlated Hubbard exciton in the one-dimensional Mott insulator Sr 2 CuO 3 . A nonresonant midinfrared optical field coherently dresses the exciton wavefunction, driving its rotation between bright and dark states. We use resonant third-harmonic generation to quantify ultrafast π/2 rotations on the Bloch sphere spanned by these exciton states. Our work advances the quest towards programmable control of correlated states and exciton-based quantum sensing.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Circularly Polarized Attosecond Pulses Enabled by an Azimuthal Phase and Polarization Grating

High-harmonic generation (HHG) is an extreme nonlinear optical process that can map the properties of an infrared driving laser beam onto short wavelength attosecond pulse trains. However, current techniques for generating circularly polarized high harmonics for probing magnetic materials and chiral systems have limitations: two-color collinear counter-rotating driving lasers result in a low cutoff photon energy, while single-color non-collinear counter-rotating schemes suffer from low conversion efficiency. In this work, we generate circularly polarized attosecond pulse trains by using a structured laser driver which has a rotating polarization and phase grating along the azimuthal coordinate. Furthermore, our experimental and numerical results demonstrate the production of left and right circularly polarized harmonics, which naturally separate upon propagation. Our approach uses a single laser color in a collinear geometry, that can be scaled for high efficiency. Simulations show this scheme can extend into the soft x-ray region when driven by mid-infrared driving lasers, while preserving the same high phase-matching cutoff photon energy as for linearly-polarized high harmonics.

attosecond science↗
DOE OSTI2025

Nonlinear optics in 2D materials: From classical to quantum

Nonlinear optics has long been a cornerstone of modern photonics, enabling a wide array of technologies, from frequency conversion to the generation of ultrafast light pulses. Recent breakthroughs in two-dimensional (2D) materials have opened a frontier in this field, offering new opportunities for both classical and quantum nonlinear optics. These atomically thin materials exhibit strong light–matter interactions and large nonlinear responses, thanks to their tunable lattice symmetries, strong resonance effects, and highly engineerable band structures. In this paper, we explore the potential that 2D materials bring to nonlinear optics, covering topics from classical nonlinear optics to nonlinearities at the few-photon level. We delve into how these materials enable possibilities, such as symmetry control, phase matching, and integration into photonic circuits. The fusion of 2D materials with nonlinear optics provides insights into the fundamental behaviors of elementary excitations—such as electrons, excitons, and photons—in low-dimensional systems and has the potential to transform the landscape of next-generation photonic and quantum technologies.

2D materials↗
DOE OSTI2026

Polarization Control via Artificial Optical Nonlinearity in Dielectric Metasurfaces

Nonlinear optical phenomena are generally governed by geometry in matter systems, as they depend on the spatial arrangement of atoms within materials or molecules. Metasurfaces, through precisely designed geometries on a subwavelength scale, allow the optical response of a material to be tailored far beyond its natural properties. Therefore, metasurfaces are highly appealing for enabling the engineering of nonlinear optical interactions. Current studies of nonlinear metasurfaces predominantly focus on the phase control of the generated light. Nonetheless, investigating the tensorial nature of the nonlinearity of metasurfaces and its effect on the polarization of the generated light is critical to fully unlocking a range of applications, such as nonlinear vector beam generation and nonlinear polarization imaging. Here, we study the artificial optical nonlinearity of a dielectric metasurface originating from its meta-atom symmetry and describe the third-order nonlinear behavior by considering the polarization degree of freedom. We establish an effective nonlinear medium model that serves as a design toolbox for developing amorphous silicon-based geometric metasurfaces with customizable features for third-harmonic generation. We further extract quantitative values of the artificial nonlinear susceptibility tensor elements related to the investigated nonlinear process and geometry. The implemented functional devices demonstrate the versatility of dielectric metasurfaces in shaping the emitted light in terms of amplitude, phase, and polarization for the precise engineering of advanced nonlinear architectures targeting applications in nonlinear imaging and complex light generation.

Diffraction↗
DOE OSTI2025

Magnon-mediated exciton–exciton interaction in a van der Waals antiferromagnet

Excitons are fundamental excitations that govern the optical properties of semiconductors. Interactions between excitons can lead to various emergent phases of matter and large nonlinear optical responses. In most semiconductors, excitons interact via exchange interactions or phase-space filling. Correlated materials that host excitons coupled to other degrees of freedom could offer pathways for controlling these interactions. Here, in this study, we demonstrate magnon-mediated interactions between excitons in CrSBr, an antiferromagnetic semiconductor. These interactions manifest as the dependence of the exciton energy on the exciton density via a magnonic adjustment of the spin canting angle. Our study demonstrates the emergence of quasiparticle-mediated interactions in correlated quantum materials, leading to large nonlinear optical responses and potential device concepts such as magnon-mediated quantum transducers.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Technical Routes to Achieve High Circular Polarized Luminescence in Chiral Perovskites: A Mini‐Review

Chiral hybrid organic-inorganic perovskites (HOIPs) have emerged as promising materials for optoelectronic and spintronic applications, leveraging unique properties such as circularly polarized luminescence (CPL), circularly polarized nonlinear optical (NLO) emission, and chiral-induced spin selectivity (CISS). However, challenges remain in stabilizing these materials under environmental stresses and precisely controlling chirality for scalable use. This review summarizes five main strategies to induce chirality in HOIPs, i.e., direct incorporation of chiral cations, surface modification with chiral ligands, ion doping, template-induced chirality, and chiral metasurfaces. Each approach offers distinct advantages for optimizing CPL efficiency and device stability, paving the way for next-generation applications in CPL detectors, information encryption, spintronic devices, etc.

14 SOLAR ENERGY↗
DOE OSTI2026

A tutorial on high-order harmonic generation in atoms, molecules, and condensed matter

This tutorial introduces strong-field-driven high-order harmonics, their experimental generation and characterization techniques, and their main applications including attosecond pulse generation and ultrafast spectroscopy of the target material. We begin from the use of atomic targets, where the first high-order harmonic generation (HHG) experiments were realized in the late 1980s. Then, we briefly discuss the basics of the microscopic generation mechanism and how various steps of the mechanism were exploited in applications such as generating isolated attosecond pulses and probing molecular orbitals. We introduce and describe the standard experimental approaches for condensed phase HHG, where we discuss unique technical challenges of the use of solid-state materials, such as the mitigation of plasma formation and laser damage. We cover the fundamentals of high-harmonic spectroscopy in condensed matter systems, such as wide bandgap dielectrics, semiconductors, liquid media, and 2D-crystals. We provide some examples of rapidly emerging spectroscopic capabilities, such as for probing crystal symmetries, Berry phases, and associated non-trivial topological properties of the source material. Finally, we provide an overview of the research field, including some of the challenges, opportunities, and open questions.

Attosecond pulses↗
DOE OSTI2025

Local charge-screening and polarization switching in a ferroelectric ionic-superconductor

For ferroelectric ionic-conductors, polarization switching is complicated by the interplay between ion mobility and charge screening effects. When the ionic charge carriers also play a key role in the domain reversal, such as in Rb-doped KTiOPO 4 (RKTP), a higher level of complexity is introduced. RKTP provides an ideal platform for investigating the relationship between ionic conductivity and polarization reversal because its highly anisotropic crystal properties allow selective modification of material characteristics through diffusive cation doping. Here, we use indiffused Ba/K doping to create a significant increase in the ionic conductivity. Time-of-flight secondary ion mass spectrometry is employed to map Ba/K doping within the RKTP crystal and correlate it to changes in ionic mobility and polarization switching characteristics under an external field applied to the nonpolar face. Using band-excitation piezoresponse force microscopy, we demonstrate a selective switching-inhibition mechanism driven by the enhanced charge screening.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Unconventional nonlinear Hall effects in twisted multilayer 2D materials

We present the first investigation of unusual nonlinear Hall effects in twisted multilayer 2D materials. Contrary to expectations, our study shows that these nonlinear effects are not merely extensions of their monolayer counterparts. Instead, we find that stacking order and pairwise interactions between neighboring layers, mediated by Berry curvatures, play a pivotal role in shaping their collective nonlinear optical response. By combining large-scale Real-Time Time-Dependent Density Functional Theory (RT-TDDFT) simulations with model Hamiltonian analyses, we demonstrate a remarkable second-harmonic transverse response in hexagonal boron nitride four-layers, even in cases where the total Berry curvature cancels out. Furthermore, our symmetry analysis of the layered structures provides a simplified framework for predicting nonlinear responses in multilayer materials in general. Our investigation challenges the prevailing understanding of nonlinear optical responses in layered materials and opens new avenues for the design and development of advanced materials with tailored optical properties.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Applying deep learning methods to develop new models of molecular charge transfer, nonadiabatic dynamics, and nonlinear spectroscopy in the condensed phase

Photon- and field-induced charge transfer has central importance in the generation and storage of electricity, the novel properties of materials, photo-induced catalysis, and electro-optic activity (e.g., photovoltaic cells, fuel cells, and organic chromophores for use in optical fibers and light-emission diodes). These non-equilibrium electronic and chemical transformations are probed by ultrafast, nonlinear spectroscopies. Accurate simulations play a crucial role in our ability to understand, optimize, and control these transformations. This project applies modern deep learning and machine learning (ML) methods to dramatically improve models of electronic dynamics, electronic-nuclear dynamics, and spectroscopic measurements for improved simulations of chemistry in complex environments, far from equilibrium phenomena, and processes in extreme environments, such as materials exposed to strong or resonant fields. This project develops accurate neural net models that go beyond predictive capability to also provide new insight into the fundamental physics underlying electron and nuclear dynamics. To achieve its objectives, this project explores and develops customized versions of high-capacity deep learning algorithms/models. These techniques are developed with an emphasis on fundamental chemical insight, not just predictive accuracy, to assist the development of the next generation of quantum simulation methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Tailoring spectral properties for entangled photon generation

The linear intensity scaling of entangled two-photon absorption (ETPA) offers a fundamental mechanism to enable nonlinear optical spectroscopy and microscopy under a substantially lower excitation power than is currently feasible. However, the long data acquisition time and low signal-to-noise ratio in reported ETPA-based spectroscopic and microscopic studies prevent its widespread application. To gain the full potential of this novel quantum light approach, it is essential to optimize entangled photon generation for significantly enhanced ETPA responses. Here, we report a new quantum light source by combining entangled photon generation with free-space femtosecond pump-pulse shaping. Here, through measurements of singles and coincidence counts by varying the patterns applied to a spatial light modulator to control the spectral widths of the pump pulses, we reveal strong dependence of the singles and coincidence count rates as well as their ratios on the spectral widths of pump pulses. An optimal spectral width for the highest ratios between the coincidence photon and the signal or idler photon count rates is also determined. Identification of such optimal spectral widths for entangled photon generation in the presence of postgeneration spectral selection makes this quantum light source a promising choice for ETPA-based spectroscopy and imaging.

Photon pairs & parametric down-conversion↗
DOE OSTI2025

Hydrogen from low-density polyethylene via nonthermal plasma: Effects of energy density and process parameters

Nonthermal plasma processes are promising for the modular valorization of plastic waste, especially into hydrogen and carbon materials, due to their high intensity, lack of reliance on catalysts or consumables, and suitability to be directly powered by electricity. We investigate the production of hydrogen from low-density polyethylene (LDPE) as a plastic waste model using streamer Dielectric Barrier Discharge (sDBD) plasma in nitrogen at atmospheric pressure. Here, we examine the effects of process energy density (energy input per unit of feedstock mass), feedstock mass, and plasma intensity (electric voltage) on plasma properties, hydrogen yield and energy efficiency via gas chromatography, optical emission spectroscopy, and electrical diagnostics, together with reactor-scale and nonlinear electric circuit modeling. The characteristic temperature of free electrons in the sDBD plasma is approximately 15000 K (1.3 eV), and that of gas species 10 times lower, demonstrating strong thermal non-equilibrium that can lead to molecular bond scission via charged species impact rather than direct heating. Experimental results show that higher energy density leads to greater hydrogen production and diminishing energy efficiency, and that higher plasma intensity and larger feedstock mass lead to greater hydrogen yield due to higher plasma temperatures and enhanced energy fluxes to the feedstock.

08 HYDROGEN↗
DOE OSTI2026

Shock compression of diamond single crystals to 120 GPa: Refractive index and nonlinear photoelasticity

The optical response of transparent solids at extreme conditions is important for both fundamental science and many applications. Strong transparent solids are of particular interest for use as optical windows in dynamic compression experiments. Due to diamond’s exceptional strength and optical properties, laser-driven shock experiments and plate impact experiments were carried out to examine the diamond optical response for shock wave compression along two different crystal orientations. Using laser interferometry at 532 nm and 1550 nm wavelengths, optical transparency was observed and refractive indices were determined for [100] diamond at stresses up to 119 GPa and for [111] diamond at stresses up to 87 GPa. From these results, the nonlinear photoelastic response for [100] and [111] diamond was determined, revealing significant dependence on both crystal orientation and laser wavelength. To enable [100] diamond as an interferometry window in dynamic compression experiments, the requisite window corrections were determined for 532 nm and 1550 nm wavelengths. Because of diamond’s excellent x-ray transparency, the present findings will be particularly useful for incorporating [100] diamonds as windows in dynamic compression experiments involving x-ray diffraction or other x-ray diagnostics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Topology-imprinting in nonlinear metasurfaces

Flat optical components, or metasurfaces, have transformed optical imaging, data storage, information processing, and biomedical applications by providing unprecedented control over light-matter interactions. These nano-engineered structures enable compact, multidimensional manipulation of light’s amplitude, phase, polarization, and wavefront, producing scalar and vector beams with unique properties such as orbital angular momentum and knotted topologies. This flexibility has potential applications in optical communication and imaging, particularly in complex environments such as atmospheric turbulence and undersea scattering. However, designing metasurfaces for shorter wavelengths, such as visible and ultraviolet light, remains challenging due to fabrication limitations and material absorption. Here, we introduce an innovative concept called topology imprinting using judiciously designed all-dielectric nonlinear optical metasurfaces to replicate desired waveforms at fundamental and harmonic frequencies, opening promising avenues for advanced photonic applications.

42 ENGINEERING↗