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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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157 records · Page 9
All sourcesNASA NTRSDOE OSTI
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 OSTI2022

Transparent conducting oxides: from all-dielectric plasmonics to a new paradigm in integrated photonics

During the past few years, the optics and photonics communities have renewed their attention toward transparent conducting oxides (TCOs), which for over two decades have been broadly employed for the fabrication of transparent electrodes in photovoltaic and communication technologies. This reinvigorated research curiosity is twofold: on the one hand, TCOs, with their metal-like properties, low optical absorption, and fabrication flexibility, represent an appealing alternative to noble metals for designing ultra-compact plasmonic devices. On the other hand, this class of hybrid compounds has been proved to possess exceptionally high optical nonlinearities when operating on a frequency window centered around their crossover point, the wavelength point at which the real part of the dielectric permittivity switches sign. Because TCOs are wide-bandgap materials with the Fermi level located in the conduction band, they are hybrid in nature, thus presenting both interband and intraband nonlinearities. This is the cause of a very rich nonlinear physics that is yet to be fully understood and explored. In addition to this, TCOs are epsilon-near-zero (ENZ) materials within a broad near-infrared spectral range, including the entire telecom bandwidth. In this operational window a myriad of novel electromagnetic phenomena have been demonstrated experimentally such as supercoupling, wavefront freezing, and photon doping. Furthermore, TCOs stand out among all other ENZ systems due to one fundamental characteristic, which is hardly attainable even by using structured materials. In fact, around their ENZ wavelength and for a quite generous operational range, these materials can be engineered to have an extremely small real index. This peculiarity leads to a slow-light effect that is ultimately responsible for a significant enhancement of the material nonlinear properties and is the cornerstone of the emerging field of near-zero-index photonics. In this regard, the recent history of nonlinear optics in conductive oxides is growing extremely fast due to a great number of experiments reporting unprecedentedly remarkable effects, including unitary index change, bandwidth-large frequency shift, efficient ultra-low-power frequency conversion, and many others. This review is meant to guide the reader through the exciting journey of TCOs, starting as an industrial material for transparent electrodes, then becoming a new alternative for low-loss plasmonics, and recently opening up new frontiers in integrated nonlinear optics. The present review is mainly focused on experimental observations.

42 ENGINEERING↗
DOE OSTI2025

Compositionally Complex Spinel Oxides as Conversion Anodes for Lithium-Ion Batteries

Four different compositionally complex multicomponent M 3 O 4 spinels containing 5–8 distinct metals were prepared by a rapid combustion synthesis method or solvothermal synthesis. High resolution synchrotron X-ray diffraction patterns show that the materials consist primarily of spinel phases with small amounts of rock salt impurities, and, in several samples, a minor amount of contracted spinel phase. Materials were investigated as conversion anodes in lithium half-cells and delivered significantly higher capacities than two-component MgFe 2 O 4 made by combustion synthesis. X-ray absorption near-edge structure (XANES) was used to estimate the oxidation states of the metals in the pristine, lithiated (discharged) and delithiated (charged) materials to better understand the redox processes in half cells that led to the improvement. Co, Ni, and Zn are reduced to low oxidation states during lithiation (cell discharge) but are only partially oxidized. The presence of a conductive metallic network that forms after lithiation is thought to account for the improved electrochemical characteristics. Interestingly, in most of the samples, iron is not fully reduced during initial lithiation unlike what happens with a set of related high entropy spinel ferrites studied previously. Finally, the improved electrochemical properties of these materials illustrates both the advantages of complexity and the difficulties in predicting their behavior.

25 ENERGY STORAGE↗
DOE OSTI2020

Mercury Chalcogenide Nanoplatelet–Quantum Dot Heterostructures as a New Class of Continuously Tunable Bright Shortwave Infrared Emitters

Despite broad applications in imaging, energy conversion, and telecommunications, few nanoscale moieties emit light efficiently in the shortwave infrared (SWIR, 1000–2000 nm or 1.24–0.62 eV). We report quantum-confined mercury chalcogenide (HgX, where X = Se or Te) nanoplatelets (NPLs) can be induced to emit bright (QY > 30%) and tunable (900–1500+ nm) infrared emission from attached quantum dot (QD) “defect” states. Here, we demonstrate near unity energy transfer from NPL to these QDs, which completely quench NPL emission and emit with a high QY through the SWIR. This QD defect emission is kinetically tunable, enabling controlled midgap emission from NPLs. Spectrally resolved photoluminescence demonstrates energy-dependent lifetimes, with radiative rates 10–20 times faster than those of their PbX analogues in the same spectral window. Coupled with their high quantum yield, midgap emission HgX dots on HgX NPLs provide a potential platform for novel optoelectronics in the SWIR.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Gradient Field Detection Using Interference of Stimulated Microwave Optical Sidebands

Here, we demonstrate that stimulated microwave optical sideband generation using parametric frequency conversion can be utilized as a powerful technique for coherent state detection in atomic physics experiments. The technique has advantages over traditional absorption or polarization rotation-based measurements and enables the isolation of signal photons from probe photons. We outline a theoretical framework that accurately models sideband generation using a density matrix formalism. Using this technique, we demonstrate a novel intrinsic magnetic gradiometer that detects magnetic gradient fields between two spatially separated vapor cells by measuring the frequency of the beat note between sidebands generated within each cell. The sidebands are produced with high efficiency using parametric frequency conversion of a probe beam interacting with 87 Rb atoms in a coherent superposition of magnetically sensitive hyperfine ground states. Interference between the sidebands generates a low-frequency beat note whose frequency is determined by the magnetic field gradient between the two vapor cells. In contrast to traditional gradiometers the intermediate step of measuring the magnetic field experienced by the two vapor cells is unnecessary. We show that this technique can be readily implemented in a practical device by demonstrating a compact magnetic gradiometer sensor head with a sensitivity of 25 fT/cm/ √ Hz with a 4.4 cm baseline, while operating in a noisy laboratory environment unshielded from Earth’s field.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Highly Conjugated Porphyrin Arrays Enable Optical Resolution of Ferromagnetic and Antiferromagnetic Aligned States of the Triplet Exciton and an Incorporated Stable Radical

Well-defined photogenerated molecular spin systems have potential utility in spintronics and quantum information science (QIS). Because molecular magnetic, optical, and electronic properties can be controlled by design, diverse spin systems can be prepared at modest temperatures. Photogenerated molecular spin systems often involve states prepared from the interaction of excitons and charges. Resolving the nature of electron spin alignment in photogenerated spin states described by the coupling of a triplet exciton and a stable radical commonly relies on EPR spectroscopy. Here, we describe ethyne-bridged (porphinato)metal ( PM n ) oligomers that incorporate a macrocycle-bound Cu(II) radical center. Upon photoexcitation of such PM n arrays, a singdoublet ( 2 S 1 ) state is formed; ultrafast internal conversion (IC) then produces a tripdoublet ( 2 T 1 ) state, which undergoes intersystem crossing (ISC) to produce a tripquartet ( 4 T 1 ) state, before relaxation to the ground state ( 2 S 0 ). These highly conjugated Cu(II) radical-containing PMn arrays enable direct observation of copper porphyrin 2 T 1 → 4 T 1 ISC dynamics from the biexponential decay of the near-infrared (NIR) 2,4 T 1 → 2,4 T n transient absorption manifold. Multireference n-electron valence perturbation theory (NEVPT2) computations illuminate how PM n electronic structure controls the relaxation dynamics of these long-lived (>10 ns) electronically excited multiplet states. These studies show that highly conjugated and polarizable porphyrin arrays incorporating stable spin centers provide rare π-delocalized systems where the ferromagnetic and antiferromagnetic alignment between a triplet exciton and a stable radical are both spectrally resolved and addressable using transient optical spectroscopy at wavelengths exceeding 1 μm, providing new opportunities to QIS.

14 SOLAR ENERGY↗
DOE OSTI2025

Influence of substitution pattern on the dynamics of internal conversion and intersystem crossing in thiopyridone isomers

We report a combined experimental and theoretical investigation of the ultrafast internal conversion (IC) and intersystem crossing (ISC) dynamics of two thiopyridone (TP) isomers in solution. Our study used ultrafast transient X-ray absorption spectroscopy (XAS) at the sulfur K-edge, in conjunction with electronic excited state surface hopping molecular dynamics and simulations of the excited state XAS, to investigate the impact of the functional group substitution pattern and solvent on the dynamics of IC and ISC. The combination of the localized X-ray probe and the simulation results enables, in part, the differentiation between ππ* and nπ* character excited states, as well as singlet and triplet states. Access to nπ* character excitations has particular value since they often prove challenging to assess with optical spectroscopy. For 2-TP, the photoexcited S 2 (ππ*) state rapidly undergoes IC to the S 1 (nπ*) state below the instrument response time, followed by ISC to the T 1 (ππ*) state on a timescale of 600 fs in acetonitrile. For 4-TP, the timescale of S 2 to S 1 IC increases to 330 fs and the timescale of ISC increases to more than 10 ps. The differences between isomers are rationalized by considering the key role of the, nπ* intermediates in mediating the intersystem crossing of these systems. Varying the substitution pattern of the molecule can stabilize or destabilize these intermediates leading to the increase in ISC rate in the ortho isomer as compared to the para isomer, while changing the solvent from acetonitrile to water had minimal effect on the electronic excited state relaxation mechanism.

Garratt, Douglas [SLAC National Accelerator Labora↗
DOE OSTI2021

Coherent Acoustic Interferometry during the Photodriven Oxygen Evolution Reaction Associates Strain Fields with the Reactive Oxygen Intermediate (Ti–OH*)

The oxygen evolution reaction (OER) from water requires the formation of metastable, reactive oxygen intermediates to enable oxygen–oxygen bond formation. Conversely, such reactive intermediates could also structurally modify the catalyst. Here, a descriptor for the overall catalytic activity, the first electron and proton transfer OER intermediate from water, (M–OH*), has been associated with significant distortions of the metal–oxygen bonds upon charge-trapping. Time-resolved spectroscopy of in situ, photodriven OER on transition metal oxide surfaces has characterized M–OH* for the charge trapping and the symmetry of the lattice distortions by optical and vibrational transitions, respectively, but had yet to detect an interfacial strain field arising from a surface coverage M–OH*. Here, we utilize picosecond, coherent acoustic interferometry to detect the uniaxial strain normal to the SrTiO 3 /aqueous interface directly caused by Ti–OH*. The spectral analysis applies a fairly general methodology for detecting a combination of the spatial extent, magnitude, and generation time of the interfacial strain through the coherent oscillations’ phase. For lightly n-doped SrTiO 3 , we identify the strain generation time (1.31 ps), which occurs simultaneously with Ti–OH* formation, and a tensile strain of 0.06% (upper limit 0.6%). In addition to fully characterizing this intermediate across visible, mid-infrared, and now GHz-THz probes on SrTiO 3 , we show that strain fields occur with the creation of some M–OH*, which modifies design strategies for tuning catalytic activity and provides insight into photo-induced degradation so prevalent for OER. To that end, the work put forth here provides a unique methodology to characterize intermediate-induced interfacial strain across OER catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Scalable Manufacturing of Efficient Perovskite/Silicon Tandem Modules

Crystalline-Si (c-Si) technology produces excellent solar cells with conversion efficiencies of up to 26.7%—nearly their practical limit of 27%—and has been commercialized extensively to produce panels below $\$0.40$/W. Techno-economic analysis shows that module efficiency will continue to be a primary cost driver because of high balance-ofsystems costs, and there is no path to higher efficiencies with single-junction silicon cells. In this project, three research teams from University of North Carolina, Arizona State University and National Renewable National Laboratory worked together to develop perovskite-silicon tandem cells with a high throughput process which can handle 5000 wafers per hour, enabled by very low added CAPEX of ~$20k for a doctor-blade coater. This can potentially increase the module efficiency to 30% (with grid) with small increase of cost, which will drive down the cost of silicon modules to be at least 16% cheaper than present silicon PERC modules. We also explored the alternative narrow bandgap perovskites as silicon replacement for all perovskite tandem cells. This project has substantially advanced the progress of solution-process perovskitessilicon tandem solar cells and perovskite-perovskite tandem solar cells with many inventions and discoveries, evidenced by 18 publications and 6 invention disclosures. Several notable examples include 1) we developed the new idea of small pyramid in combination with solution grown perovskites and demonstrated record-efficiency of 28.5% for 1 cm2 on textured silicon bottom cells and 25.2% for 24 cm2 on chemically etched silicon bottom cells for perovskite-silicon tandem cells. 2) We developed perovskite ink that can coat perovskites onto texture silicon without voids;, and new device structure to enhance the yield of fabrication by reducing shunting 3) We identified the origin of open circuit voltage on mixed halide wide bandgap perovskites, and came with a solution for this problem, reducing the voltage loss to a record small value, which can potentially push the perovskite-silicon tandem cell efficiency to over 31%; 4) We have developed efficient alternative low bandgap semiconductors, i.e. gradient-doped Sn based perovskites by Ba ions, new oxide hole transport layers which increase the efficiency of perovskite/perovskite tandem cells reached record efficiency of 26.3%; 5) We developed bifacial perovskite/perovskite tandem cells by overcoming contacts issues and regaining light absorption, further boosting the equivalent efficiency to 29.3% under 1 sun illumination with 30% albedo light; 6) We developed the first all perovskite tandem module fabricated in air by discovery a combination of oxidization and reduction couples, yield an aperture efficiency of 21.6% for all perovskite mininodules, exceeding that of single junction perovskite minimodules. These discoveries not only accelerate the commercialization of perovskite-silicon tandem solar cells, but also provide guidance in designing other type of perovskite solar cell technologies.

14 SOLAR ENERGY↗
DOE OSTI2025

Semiconducting Zn x Mo 3 S 13 -GO Chalcocarbogel: A High-Capacity and Stable Sulfur-Equivalent Conversion-Based Electrode for Lithium-Ion Batteries

Lithium–sulfur batteries with a sulfur electrode offer a theoretical capacity of ∼1672 mAh g –1 , but rapid capacity loss mainly constrains their practical application. This work introduces a semiconducting and amorphous Zn x Mo 3 S 13 -GO (x = 0.5) chalcocarbogel sulfur-equivalent electrode with superior capacity and stability for lithium-ion batteries (LIBs). The Zn x Mo 3 S 13 -GO is synthesized in solution under ambient conditions, and its local structure contains S–S, M-Q (M = Mo, Zn; Q = S, O), C–S, and Mo–Mo bonding motifs with Mo coordination environment closely related to Mo 3 S 13 anions, as determined by X-ray photoelectron spectroscopy, synchrotron X-ray scattering, X-ray absorption spectroscopy, and ab initio molecular dynamics simulations. The Li/Zn x Mo 3 S 13 -GO cell offers an initial discharge capacity of 1019 mAh g –1 at a rate of C/3. After the activation cycles, the Li/Zn x Mo 3 S 13 -GO cell demonstrates good cycling stability, retaining a discharge capacity of 519.4 mAh g –1 after 250 cycles with ∼99.98% Coulombic efficiency and excellent rate capabilities. Moreover, it provides an initial discharge capacity of ∼574 mAh g –1 and maintains a retention capacity of 279 mAh g –1 at 1C after 625 cycles. The Lewis acidic Zn 2+ ion enhances the Lewis basic polysulfide anchoring ability and reduces the dissolution of polysulfides produced during the redox process through Zn–S covalent interaction, while the semiconducting and amorphous structure of the chalcocarbogel increases the electrical and ionic conductivity. Furthermore, this work highlights chalcocarbogels’ potential for developing high-capacity and stable electrodes for LIBs.

25 ENERGY STORAGE↗
DOE OSTI2026

Chemical and morphological evolution of hybrid conversion coatings in low-Earth orbit space environment

Understanding how protective coatings respond to the harsh low-Earth orbit (LEO) environment is essential for ensuring the safety, longevity, and cost-effectiveness of spacecraft. In particular, identifying environmentally friendly, non-chromate alternatives that can maintain performance under such conditions has both technological and regulatory significance. This study investigates the environmental stability of zirconium-based hybrid conversion coatings with Cu additives (Cu10 and Cu20) applied to cold-rolled steel, tested in the Materials International Space Station Experiment (MISSE) outside the International Space Station (ISS). Chemical and morphological analyses were carried out using a combination of electron microscopy and X-ray spectroscopy techniques, including scanning electron microscopy (SEM), scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy (STEM-EDS), X-ray photoelectron spectroscopy (XPS), and X-ray absorption near-edge structure (XANES) spectroscopy. After exposure outside the ISS, all coatings remained structurally intact, with all exhibiting a uniform Zr-rich matrix and embedded Cu-rich clusters, while a thin Si-rich surface layer developed from interaction with space environments. Depth-resolved XPS showed a layered structure with CuO on the surface, Cu 2 O, and partial Zr(IV) reduction near Cu-rich sites, evidence of Atomic Oxygen (AO)-driven surface oxidation. These results demonstrate that Cu–Zr coatings maintain their chemical integrity and microstructure in harsh space environments, offering a non-chromate alternative for long-term aerospace protection. These insights provide valuable guidance for developing next-generation protective coatings that combine environmental sustainability with the reliability required for future aerospace and orbital applications.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Dynamics of disordered intermediates during the two-electron alkaline MnO 2 conversion reaction for grid-scale batteries

Battery technologies beyond Li-ion are likely needed for extensive integration of grid-scale storage. The rechargeable Zn-MnO 2 chemistry has the potential for high sustainability, high safety, and low cost, using Earth-abundant basis materials. In an alkaline electrolyte, the MnO 2 cathode can cycle reversibly if modified by including a Bi-containing additive, although the cycling mechanism remains mostly unknown. This work presents an account of the intermediate species involved in the electrochemical transformation from layered δ-MnO 2 to Mn(OH) 2 and back. During charge, a disordered intermediate with a structure resembling layered β-MnOOH exists stably for an extended period, corresponding to a regime known to have unexpected electrochemical activity of Bi. During discharge, β-MnOOH exists only briefly and is never the majority material, revealing that the cycling mechanism is asymmetric. In conclusion, these findings represent a significant advance in mechanistic knowledge and can enable engineering to develop the system for commercial use.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Porous and Amorphous Mn x Mo 3 S 13 Chalcogel Electrode for High-Capacity Conversion-Based Lithium-Ion Batteries

While Li-ion batteries (LIBs) are a leading energy storage technology, their energy densities are limited by the low capacity of conventional intercalation cathodes, driving interest in high energy-density Li–S batteries that make use of conversion chemistry. Achieving high capacity, reversibility, and cycle stability, and controlling volume changes in conversion batteries during the charge–discharge process, however, remains challenging. Here, in this study, we present a porous, amorphous, sulfide-based Mn x Mo 3 S 13 chalcogel, which concurrently offers high capacity and cycle stability. The solution-processable room temperature synthesized Mn x Mo 3 S 13 (x = 0.25) chalcogel exhibits a local structure that resembles the Mo 3 S 13 cluster with Mn 2+ distributed across the Mo 3 S 13 matrix, as determined by synchrotron X-ray pair distribution function (PDF) and extended X-ray absorption fine structure (EXAFS). Ab initio molecular dynamics (AIMD) simulations reveal that Mn 2+ incorporation shortens the polysulfide chain in the gel matrix compared to the Mo 3 S 13 chalcogel, while forming a coordination environment with disulfide groups, analogous to the experimental findings. A Li/Mn 0.25 Mo 3 S 13 half-cell delivers 897 mAh g –1 capacity during the first discharge and retains 571 mAh g –1 capacity after 100 cycles at a C/3 rate. Distribution of relaxation time (DRT) unveils a stable solid–electrolyte interphase (SEI) formation upon cycling that enables charge–discharge reversibility. Here, the enhanced capacity retention and cycle stability compared to those of the Li/Mo 3 S 13 cell are attributed to the reduced dissolution of active mass into the electrolyte, facilitated by the formation of shorter polysulfide chains within the Mn 0.25 Mo 3 S 13 structure and the strong affinity of Lewis-acidic Mn 2+ for polysulfide anions generated during the charge–discharge process of the Li/Mn 0.25 Mo 3 S 13 cell. Thus, this work illustrates a design principle of material for high-capacity and cycle-stable Li-metal sulfide batteries.

25 ENERGY STORAGE↗