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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 OSTI2024

Demonstration of Non-linear Optical Spectroscopy Enhancement utilizing Entangled Photons

Laser-based nonlinear optical spectroscopy approaches have enabled the direct sensing of important chemistry in nearly every fundamental or applied field of science. Yet in many applications, increased detectivity is needed to unravel fundamental mechanisms. One possibility is the use of quantum entanglement to increase detection cross-sections, but it is unproven that enhancement from quantum light extends to practical intensities for chemical sensing. In this report, we investigated the creation and use of entangled photons in nonlinear optical mixing for second harmonic generation and infrared imaging. We observe that the linear scaling of nonlinear mixing from entangled photon sources extends to the mW laser power regime, and enhances direct infrared imaging on Si-based charge coupled device cameras. These results motivate future experimentation on practical uses of entangled photons for nonlinear optical sensing applications.

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

A cavity-enhanced spectroscopist's lens on molecular polaritons

Polariton chemistry has been hailed as a potential new route to direct molecular processes with electromagnetic fields. To make further strides, the community needs to clarify which unusual polaritonic phenomena are true hallmarks of cavity quantum electrodynamics and which can be rationalized with classical optical physics. Here, in this work, we provide a tutorial perspective on the formation, spectroscopy, and behavior of molecular polaritons using classical optics. Where possible, we draw connections to cavity-enhanced spectroscopy and recast open questions in terms that may be more familiar to the broader community of physical chemists.

Cavity quantum electrodynamics↗
DOE OSTI2024

Enhancement of terahertz fields in LiTaO 3 waveguides using a conical pulse front

The development of methods for the generation of strong ultrafast electromagnetic pulses in the terahertz (THz) spectral range has led to a surge of progress in nonlinear THz spectroscopy and THz control of molecular and collective responses. For spectroscopy in the 1-THz range, the submillimeter wavelengths and associated large spot sizes, large optical elements, and short distances between final focusing elements and samples can lead to cumbersome experimental setups that are incompatible with some sample environments. Here, we introduce a novel terahertz ring excitation (TREx) optical pumping geometry to generate superposing, focusing fields in planar THz waveguides made out of the electro-optic material lithium tantalate. High THz fields, >175 kV/cm, are generated and measured optically with no free-space THz propagation. The field level achieved by pumping with a sequence of concentric rings of excitation light exceeds by about 20× the result of a single cylindrically focused line of pump light that has been used routinely in previous work. The technique opens new prospects for compact waveguide-based linear and nonlinear THz spectroscopy and signal processing.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Strong-field Driven Sub-cycle Band Structure Modulation and Dephasing Control

In this work, we present measurements of ultrafast electric-field observables in magnesium oxide using a non-resonant nonlinear optical interaction. Using field observables, we show that strong laser fields modulate the band structure on sub-cycle timescales, thereby altering the material’s nonlinear optical response. We perform time-dependent perturbation theory calculations using a field-dependent dispersion relation and semiconductor Bloch equation calculations, both of which agree with experimental observations. Furthermore, we extract pulse decay times from the real-time signal electric field envelope and show sub-cycle control of dephasing times. Our work offers a new perspective on strong-field-driven electron dynamics in solids through electric-field observables. The demonstrated attosecond modulation of the nonlinear response could have important implications for quantum light generation and quantum spectroscopy using nonlinear optical processes.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Molecular structures of residual solvent in polyacrylonitrile based electrolytes: Implications for conductivity and stability

Lithium-ion batteries increasingly play significant roles in modern technologies; however, increased energy density also raises concerns about electrolyte safety. Traditional electrolytes that use volatile organic solvents face risks of thermal runaways and fires from electrode shorting. In response, polymer-based solid electrolytes have been developed for replacement. Polyacrylonitrile (PAN) is a promising fire-resistant component for electrolyte fabrication, but its limited solubility necessitates using low-volatility solvents, which are notoriously difficult to remove in subsequent drying processes. Here, we use femtosecond two-dimensional infrared spectroscopy to provide an in-depth understanding of how residual solvent from processing affects the molecular structures and dynamics within a polymer electrolyte. To this end, linear and nonlinear infrared spectroscopies are employed to interrogate the molecular interactions in PAN-based electrolytes containing various contents of N,N-dimethylformamide (DMF). We show that the amount of DMF within the PAN electrolyte affects the Li+ structure. Further, the coordination can proceed through the carbonyl group and/or the amide nitrogen to form antiparallel structures with the nitrile groups of PAN through dipole–dipole interactions. The free motion of DMF is drastically inhibited upon interaction with Li+ and PAN, which decreases the ionic conductivity and potentially affects the stability (resistance toward removal and chemical decomposition). These findings have implications for the design and processing of solid polymer electrolytes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Fingerprinting fractons with pump-probe spectroscopy

We demonstrate how pump-probe techniques enable specific spectroscopic diagnostics of fracton phases of matter by studying lineon-planon braiding in the paradigmatic X-cube model. Our discussion builds on previous works probing anyonic exchange statistics in conventional spin liquids, but the extension to fracton phases reveals qualitatively different phenomena due to the restricted mobility of fractionalized excitations. A key feature is that nearby planons can form an emergent bound state by accessing different planes via alternative pairing configurations. We show that this bound state qualitatively modifies the long-time linear and nonlinear responses, leading to an asymptotic linear-in-𝑡 behavior for the pump-probe signal 𝜒 𝑍𝑍𝑋 . By contrast, swapping the pump and probe polarizations produces a nonlinear response 𝜒 𝑋𝑋𝑍 that is asymptotically 𝑡 independent. This asymmetry reflects the fact that the two species of fractionalized excitations live in different spatial dimensions. Thus the pump-probe signals studied here are sensitive to (i) nontrivial braiding statistics in three dimensions, (ii) the existence of bound states among fractionalized excitations, and (iii) the one-dimensional mobility of lineons. Furthermore, our results therefore provide spectroscopic signatures that distinguish fracton phases from conventional topologically ordered spin liquids.

braiding↗
DOE OSTI2024

Excitation and detection of coherent nanoscale spin waves via extreme ultraviolet transient gratings

The advent of free electron lasers has opened the opportunity to explore interactions between extreme ultraviolet (EUV) photons and collective excitations in solids. While EUV transient grating spectroscopy, a noncollinear four-wave mixing technique, has already been applied to probe coherent phonons, the potential of EUV radiation for studying nanoscale spin waves has not been harnessed. Here we report EUV transient grating experiments with coherent magnons in Fe/Gd ferrimagnetic multilayers. Magnons with tens of nanometers wavelengths are excited by a pair of femtosecond EUV pulses and detected via diffraction of a probe pulse tuned to an absorption edge of Gd. The results unlock the potential of nonlinear EUV spectroscopy for studying magnons and provide a tool for exploring spin waves in a wave vector range not accessible by established inelastic scattering techniques.

Science & Technology - Other Topics↗
DOE OSTI2025

Strong adsorption of guanidinium cations to the air–water interface

Combining Deep-UV second harmonic generation spectroscopy with molecular simulations, we confirm and quantify the specific adsorption of guanidinium cations to the air–water interface. Using a Langmuir analysis of measurements at multiple concentrations, we extract the Gibbs free energy of adsorption, finding it larger than typical thermal energies. Molecular simulations clarify the role of polarizability in tuning the thermodynamics of adsorption, and establish the preferential parallel alignment of guanidinium at the air–water interface. As a polyatomic cation, guanidinium represents one of the few examples of a positively charged species to exhibit a propensity for the air-water interface. As such, these results expand on the growing body of work on specific ion adsorption.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Quantum Theory of Surface Lattice Resonances

The collective interactions of nanoparticles arranged in periodic structures give rise to high‐ in‐plane diffractive modes known as surface lattice resonances. Although these resonances and their broader implications have been extensively studied within the framework of classical electrodynamics and linear response theory, a quantum optical theory capable of describing the dynamics of these structures, especially in the presence of material nonlinearities beyond ad hoc few‐mode approximations, is largely missing. To this end, we consider a lattice of metallic nanoparticles coupled to the electromagnetic field and derive the quantum input–output relations within the electric dipole approximation. As applications, we analyze coupling between the nanoparticle array and external quantum emitters, and show how the formalism extends to molecular optomechanics, where the high ‐factors of SLRs enable coupling to collective vibrational modes. We further consider arrays composed of saturable excitonic emitters, demonstrating how emitter nonlinearities can be used to switch the SLR condition between electronic transitions. Using a perturbative approach that accounts for population dynamics, we show how these effects can be probed in pump–probe experiments and give rise to nonlinear phase‐matching phenomena. Our work provides a microscopic framework for modeling SLRs interacting with quantum emitters without phenomenological descriptions of the electromagnetic environment.

molecular optomechanics↗
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 OSTI2026

Long-term stabilization of intensity-difference squeezing from four-wave mixing in rubidium vapor

Generation of quantum states of light through off-resonance four-wave mixing in rubidium vapor is a straightforward and well-established technique. However, achieving a sufficiently high and consistent level of intensity difference squeezing (IDS) and intrinsic quantum correlations between photon pairs over an extended timescale, necessary for quantum-light-based nonlinear optical spectroscopy and microscopy, remains challenging and largely unexplored. Here, we report a simple stabilization method combining an active periodic laser frequency retuning with an automatic control algorithm based on quantitatively assessing the factors affecting the IDS level and squeezed light intensity. Validation of our method was performed by acquiring data over a 5-hour period, and the results demonstrate a remarkably stable squeezing level of -7.8 dB in combination with a > 4× reduction of the standard deviation of IDS level from 0.46 dB to 0.10 dB. The achieved stabilization further enables us to quantitatively assess the IDS reduction due to the scattering in a polystyrene bead suspension as a function of sample transmission. Our approach should enable a variety of applications requiring an extended squeezing stability over multiple hours, especially for those following biological processes and chemical reactions in real time.

Allen, Christian Harry [Oak Ridge National Laborat↗
DOE OSTI2025

Solvated Ionic Liquid-based Electrolytes: Experimental Characterization, Atomistic Modeling and Applications in Energy Storage

This study aimed on understanding the molecular structure and transport mechanisms of high-concentration lithium electrolytes, with a particular focus on solvate ionic liquids (SILs) based on glyme solvents, for use in next-generation, high-voltage energy storage systems. The hypothesis is that the composition of the solvents in these electrolytes can be designed and adjusted to control cation solvation, enabling charge transport via an ion-hopping mechanism. This mechanism resembles Grotthuss conduction of protons in water and is independent of electrolyte viscosity. The experimental studies employed linear and nonlinear infrared spectroscopy (FTIR and 2D IR), electrochemical measurements, and vibrational probes.

25 ENERGY STORAGE↗
DOE OSTI2025

Super-resolution stimulated X-ray Raman spectroscopy

Propagation of intense X-ray pulses through dense media has led to the observation of phenomena such as atomic X-ray lasing, self-induced transparency and stimulated X-ray Raman scattering (SXRS)4. SXRS has been long predicted as a means to launch and probe valence-electron wavepackets and as a building block for nonlinear X-ray spectroscopies. However, experimental observations of SXRS to date have not provided spectroscopic information, and theoretical modelling has largely implemented hard-to-realize phase-coherent attosecond pulses. Here we demonstrate SXRS with spectroscopic precision, that is, detection of valence-excited states in neon with a near Fourier-limited joint energy–time resolution of 0.1 eV–40 fs. We used a new covariance analysis between statistically spiky broadband incident X-ray and scattered X-ray Raman pulses. Using 18,000 single shots, we beat not only the incident (about 8 eV) bandwidth but also the approximately 0.2 eV instrumental energy resolution, thus creating super-resolution conditions, in analogy to super-resolved fluorescence microscopy. Our experimental results, supported by ab initio propagation simulations, reveal the competition between lasing in the ion and stimulated Raman scattering in the neutral. We demonstrate enhanced signal collection efficiency and a broad excitation window, surpassing spontaneous Raman efficiencies by orders of magnitude. This stochastic SXRS approach represents a first step towards tracking elementary events that determine chemical outcomes.

nonlinear x-ray spectroscopy↗
DOE OSTI2025

Observation of cupratelike nonlinear terahertz responses in superconducting infinite-layer nickelates via two-dimensional coherent spectroscopy

The 𝑑-wave pairing symmetry in newly discovered infinite-layer nickelates remains highly debated compared to the widely accepted 𝑑-wave superconductivity in cuprates, despite recent intense efforts using equilibrium optical and electrical transport measurements. A complementary approach involves characterizing THz coherent nonlinear responses, which is currently lacking but needed, as it would offer new insights into the superconducting gap structure by characterizing Higgs modes and quasiparticle excitations. Here, in this study, we report THz 2D coherent spectroscopy (THz-2DCS) responses from the superconducting state in an infinite-layer nickelate. The 2D spectra clearly demonstrate the absence of hallmark signatures of 𝑠-wave pairing symmetry, such as resonant 2⁢Δ peaks at superconducting gaps. Instead, we observe gapless 2D spectra in the nickelate, centered around the THz driving frequency, with no noticeable shift as the temperature increases. These findings closely resemble the nodal superconductivity behavior expected in cuprates. Together with our simulations, these findings suggest that 2⁢Δ signatures in the 2D spectra of 𝑑-wave gap structures can be obscured by significant nodal quasiparticle excitations at arbitrarily low energies. This contrasts with the long-lived Higgs modes, observed as distinct 2⁢Δ peaks in a controlled THz-2DCS experiment on niobium, a representative example of dirty-limit s-wave superconductors. Our results have implications for understanding the unconventional superconductivity in nickelates and highlight the need to explore their coherent nonlinear dynamics.

Pairing mechanisms↗
DOE OSTI2026

Instantaneous difference frequency locking observed during toroidicity-induced Alfvén eigenmode coupling in the DIII-D tokamak

In magnetic confinement fusion, toroidicity-induced Alfvén eigenmodes (TAEs) are well-studied, weakly stable solutions of the linearized ideal magnetohydrodynamic equations. Driven unstable by suprathermal populations of energetic particles, TAE pose a key vulnerability to the confinement of high-energy alpha particles generated by fusion reactions. Hence, it is paramount to understand TAE dynamics if a working reactor is to be realized. In this work, we detect and characterize signatures of nonstationary nonlinear coupling between TAE using a novel, time-resolved bispectral analysis; results are supported by analytic signal of band-passed data. Crucially, a stationary phase relationship between two TAE and a nascent low frequency fluctuation is observed precisely when the triple product of magnetic fluctuation amplitudes is enhanced. Local mode number and frequency spectrum, gleaned from beam-emission spectroscopy, corroborates simultaneous satisfaction of nonlinear matching conditions, and provides a tool to identify theorized pathways of energy transfer, e.g. TAE parametric instability.

bispectral analysis↗
DOE OSTI2024

Hole‐Carrier‐Dominant Transport in 2D Single‐Crystal Copper

Abstract In 2D noble metals like copper, the carrier scattering at grain boundaries has obscured the intrinsic nature of electronic transport. However, it is demonstrated that the intrinsic nature of transport by hole carriers in 2D copper can be revealed by growing thin films without grain boundaries. As even a slight deviation from the twin boundary is perceived as grain boundaries by electrons, it is only through the thorough elimination of grain boundaries that the hidden hole‐like attribute of 2D single‐crystal copper can be unmasked. Two types of Fermi surfaces, a large hexagonal Fermi surface centered at the zone center and the triangular Fermi surface around the zone corner, tightly matching to the calculated Fermi surface topology, confirmed by angle‐resolved photoemission spectroscopy (ARPES) measurements and vivid nonlinear Hall effects of the 2D single‐crystal copper account for the presence of hole carriers experimentally. This breakthrough suggests the potential to manipulate the majority carrier polarity in metals by means of grain boundary engineering in a 2D geometry.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Enabling robust, stable, and accurate nonlinear optical measurements from squeezed light generated in hot rubidium vapor

The feasibility of nonlinear optical (NLO) imaging and spectroscopy using low intensity quantum states of light including entangled photon and squeezed light sources, such as those driven by two-photon absorption (TPA), has been a topic of ongoing debate. An unambiguous identification of the appreciable quantum advantage in such quantum light applications could enable NLO imaging of biological samples without photodegradation and phototoxicity. Recently, we have constructed a two-mode squeezed light source based on four-wave mixing in 85Rb vapor, which is capable of 7.9 dB of intensity-difference squeezing (IDS), corresponding to 8.7 dB upon electronic noise correction. In this talk, we discuss the stability of our system, including implementation details on achieving and maintaining 8.7 dB of IDS for several hours, and ensuring the two spatially multimode beams are properly overlapped in a sample with minimal optical loss.

Allen, Harry [ORNL] (ORCID:0000000190253914)↗