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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 919 records · Page 51
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Energy Shifts and Broadening of Excitonic Resonances in Electrostatically Doped Semiconductors

Tuning the density of resident electrons or holes in semiconductors through electrostatic doping provides crucial insight into the composition of the many excitonic complexes that are routinely observed as absorption or photoluminescence resonances in optical studies. Moreover, we can change the way these resonances shift and broaden in energy by controlling the quantum numbers (e.g., spin and valley) of the resident carriers with applied magnetic fields and doping levels, as well as by selecting the quantum numbers of the photoexcited or recombining electron-hole (𝑒−ℎ) pair through optical polarization. Here, we discuss the roles of distinguishability and optimality of excitonic complexes, showing them to be key ingredients that determine the energy shifts and broadening of optical resonances in charge-tunable semiconductors. A distinguishable 𝑒−ℎ pair means that the electron and hole undergoing photoexcitation or recombination have quantum numbers that are not shared by any of the resident carriers. An optimal excitonic complex refers to a complex whose particles come with all available quantum numbers of the resident carriers. Based on the carrier density, magnetic field, and light polarization, all optical resonances may be classified as either distinct or indistinct depending on the distinguishability of the 𝑒−ℎ pair, and the underlying excitonic complex can be classified as either optimal or suboptimal. The universality of these classifications, inherited from the fundamental Pauli exclusion principle, allows us to understand how optical resonances shift in energy and whether they should broaden as doping is increased. This understanding is supported by conclusive evidence that the broadening and decay of optical resonances cannot be simply attributed to enhanced screening when resident carriers are added to a semiconductor. Finally, applying the classification scheme in either monolayer or moiré heterobilayer semiconductor systems, we relate the energy shift and amplitude of the neutral-exciton resonance to the compressibility of the resident carrier gas.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Optical imprinting of superlattices in two-dimensional materials

We propose a novel optical method to imprint superlattice structures in two-dimensional electronic systems. By changing the shape of the optical field, we synthesize various lattice structures with different spatial symmetry, periodicity, and strength. We find that the wide optical tunability allows one to tune different properties of the effective band structure, including Chern number, energy bandwidths, and band gaps. We consider the high-frequency regime where the electronic system can remain in the quasi-equilibrium phase for an extended amount of time. The spatiotemporal reconfigurablity of our approach opens up new possibilities to control light-matter interaction to generate novel electronic states and optoelectronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Manipulating efficient light emission in two-dimensional perovskite crystals by pressure-induced anisotropic deformation

The hybrid nature and soft lattice of organolead halide perovskites render their structural changes and optical properties susceptible to external driving forces such as temperature and pressure, remarkably different from conventional semiconductors. Here, we investigate the pressure-induced optical response of a typical two-dimensional perovskite crystal, phenylethylamine lead iodide. At a moderate pressure within 3.5 GPa, its photoluminescence red-shifts continuously, exhibiting an ultrabroad energy tunability range up to 320 meV in the visible spectrum, with quantum yield remaining nearly constant. First-principles calculations suggest that an out-of-plane quasi-uniaxial compression occurs under a hydrostatic pressure, while the energy is absorbed by the reversible and elastic tilting of the benzene rings within the long-chain ligands. This anisotropic structural deformation effectively modulates the quantum confinement effect by 250 meV via barrier height lowering. The broad tunability within a relatively low pressure range will expand optoelectronic applications to a new paradigm with pressure as a tuning knob.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Linewidth-tunable laser diode array for rubidium laser pumping

To optimise the pump source for a high-power diodepumped rubidium vapour laser, we have designed a laser diode array (LDA) with a narrowed and tunable linewidth and an external cavity formed by two volume Bragg gratings (VBGs). Through controlling the temperature differences between the two VBGs, the LDA linewidth, which was 1.8 nm before mounting the two VBGs, was tunable from 100 pm to 0.2 nm, while the output power changed by no more than 4 %. By changing simultaneously the temperature in both VBGs, the centre wavelength in air of the linewidth-tunable LDA was tunable from 779.40 nm to 780.05 nm. (control of laser radiation parameters)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Dynamic Implications of Noncovalent Interactions in Amphiphilic Single-Chain Polymer Nanoparticles

Single-chain polymer nanoparticles (SCNPs) combine the chemical diversity of synthetic polymers with the intricate structure of biopolymers, generating versatile biomimetic materials. The mobility of polymer chain segments at length scales similar to secondary structural elements in proteins is critical to SCNP structure and thus function. However, the influence of noncovalent interactions used to form SCNPs (e.g., hydrogen-bonding and biomimetic secondary-like structure) on these conformational dynamics is challenging to quantitatively assess. To isolate the effects of noncovalent interactions on SCNP structure and conformational dynamics, we synthesized a series of amphiphilic copolymers containing dimethylacrylamide and monomers capable of forming these different interactions: (1) di(phenylalanine) acrylamide that forms intramolecular β-sheet-like cross-links, (2) phenylalanine acrylamide that forms hydrogen-bonds but lacks a defined local structure, and (3) benzyl acrylamide that has the lowest propensity for hydrogen-bonding. Each SCNP formed folded structures comparable to those of intrinsically disordered proteins, as observed by size exclusion chromatography and small angle neutron scattering. The dynamics of these polymers, as characterized by a combination of dynamic light scattering and neutron spin echo spectroscopy, was well described using the Zimm with internal friction (ZIF) model, highlighting the role of each noncovalent interaction to additively restrict the internal relaxations of SCNPs. These results demonstrate the utility of local scale interactions to control SCNP polymer dynamics, guiding the design of functional biomimetic materials with refined binding sites and tunable kinetics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Non-spectroscopic surface plasmon sensor with a tunable sensitivity

We demonstrate a non-spectroscopic surface plasmon sensor with a tunable sensitivity which is based on the relationship between the wave number of surface plasmon polaritons (SPPs) on metal film and the refractive index of the specimen in contact with the metal film. A change in the wave number of the SPPs results in a variation in the propagation angle of the leakage radiation of the SPPs. A reference light is used to interfere with the leakage radiation, and the refractive index of the specimen can be obtained by measuring the period of the interference fringes. The sensitivity of the sensor can be tuned by changing the incident direction of the reference light and this cannot be realized by conventional surface plasmon sensors. For a reference angle of 1.007°, the sensitivity and resolution of the sensor are 4629 μm/RIU (RIU stands for refractive index unit) and 3.6 × 10{sup −4} RIU, respectively. In addition, the sensor only needs a monochromatic light source, which simplifies the measurement setup and reduces the cost.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1993

Measured optical performance of three Fabry-Perot interferometers for use in a tunable ultraviolet filter

A narrowband ultraviolet (UV) filter would allow the first monochromatic two-dimensional images of astrophysical plasmas to be obtained in UV emission lines. The high etendue and spectral resolving power of the Fabry-Perot (FP) interferometer make it an excellent candidate for use in a tunable UV filter, provided that adequate optical performance can be obtained. Laboratory measurements of three UV FP interferometers with progressively greater dielectric mirror reflectances are described. The measurements demonstrate the adequate reflectivity, absorption, and small-scale smoothness of currently available coatings and substrates for UV interferometry. The measurements are conducted at 228.8 nm utilizing a cadmium hollow cathode light source. The best performing interferometer has a finesse of 41 and maximum transmittance of 0.38 over a coating-performance-dominated 3-mm-diam subaperture and a finesse of 26 and maximum transmittance of 0.32 over a parabolic-defect-dominated 30-mm-diam aperture. This interferometer is well suited for use in a UV filter system.

Korendyke, Clarence M.↗
DOE OSTI2015

High Photoluminescence Quantum Yield in Band Gap Tunable Bromide Containing Mixed Halide Perovskites

Hybrid organic-inorganic halide perovskite based semiconductor materials are attractive for use in a wide range of optoelectronic devices because they combine the advantages of suitable optoelectronic attributes and simultaneously low-cost solution processability. Here, we present a two-step low-pressure vapor-assisted solution process to grow high quality homogeneous CH 3 NH 3 PbI 3-x Br x perovskite films over the full band gap range of 1.6-2.3 eV. Photoluminescence light-in versus light-out characterization techniques are used to provide new insights into the optoelectronic properties of Br-containing hybrid organic-inorganic perovskites as a function of optical carrier injection by employing pump-powers over a 6 orders of magnitude dynamic range. The internal luminescence quantum yield of wide band gap perovskites reaches impressive values up to 30%. This high quantum yield translates into substantial quasi-Fermi level splitting and high "luminescence or optically implied" open-circuit voltage. Most importantly, both attributes, high internal quantum yield and high optically implied open-circuit voltage, are demonstrated over the entire band gap range (1.6 eV ≤ E g ≤ 2.3 eV). These results establish the versatility of Br-containing perovskite semiconductors for a variety of applications and especially for the use as high-quality top cell in tandem photovoltaic devices in combination with industry dominant Si bottom cells. (Figure Presented).

36 MATERIALS SCIENCE↗
DOE OSTI2018

Highly sensitive up-conversion optical thermometry based on Yb3+-Er3+ co-doped NaLa(MoO4)2 green phosphors

Highlights: • Phosphors NaLa(MoO{sub 4}){sub 2}:Er{sup 3+}/Yb{sup 3+} UC with intense green emission were synthesized. • The thermometric property based on FIR {sup 2}H{sub 11/2}/{sup 4}S{sub 3/2} → {sup 4}I{sub 15/2} was evaluated. - Abstract: Pursuing highly sensitive thermometry is a permanent goal in recent scientific research, which can be achieved through Fluorescence intensity ratio (FIR) technique due to its fast response, excellent accuracy, high spatial resolution and tunable size. Herein, highly sensitive micro-thermometers based on FIR of the thermal coupled levels (TCLs) {sup 2}H{sub 11/2}/{sup 4}S{sub 3/2} → {sup 4}I{sub 15/2} from Er{sup 3+} in phosphors NaLa(MoO{sub 4}){sub 2}: Yb{sup 3+}/Er{sup 3+} up-conversion (UC) were developed, which emits dazzling green light with the excitation of 980 nm laser and its UC spectra consisted of intense green bands peaked at 530 and 552 nm and a negligible 658 nm red emission ({sup 4}F{sub 9/2} → {sup 4}I{sub 15/2}), respectively. The maximum absolute sensitivity approached to 0.023 K{sup -1} at 490 K through assessing FIR based on thermo-responsive green emissions. Results suggest the present green-emitting phosphors have great potential to serve as UC thermometers with high and stable sensitivity, which greatly meet the growing demand for sensing applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Electro-optic modulation of a laser at microwave frequencies for interferometric purposes

A multi-point microwave interferometer (MPMI) concept was previously proposed by the authors for spatially-resolved, non-invasive tracking of a shock, reaction, or detonation front in energetic media [P. Specht et al., AIP Conf. Proc. 1793, 160010 (2017).]. The advantage of the MPMI concept over current microwave interferometry techniques is its detection of Doppler shifted microwave signals through electro-optic (EO) modulation of a laser. Since EO modulation preserves spatial variations in the Doppler shift, collecting the EO modulated laser light into a fiber array for recording with an optical heterodyne interferometer yields spatially-resolved velocity information. This work demonstrates the underlying physical principle of the MPMI diagnostic: the monitoring of a microwave signal with nanosecond temporal resolution using an optical heterodyne interferometer. For this purpose, the MPMI concept was simplified to a single-point construction using two tunable 1550 nm lasers and a 35.2 GHz microwave source. A (110) ZnTe crystal imparted the microwave frequency onto a laser, which was combined with a reference laser for determination of the microwave frequency in an optical heterodyne interferometer. A single, characteristic frequency associated with the microwave source was identified in all experiments, providing a means to monitor a microwave signal on nanosecond time scales. Lastly, areas for improving the frequency resolution of this technique are discussed, focusing on increasing the phase-modulated signal strength.

Specht, Paul E. (ORCID:000000027007000X)↗
DOE OSTI2011

Anomalous dimers in quantum mixtures near broad resonances: Pauli blocking, Fermi surface dynamics, and implications

We study the energetics and dispersion of anomalous dimers that are induced by the Pauli blocking effect in a quantum Fermi gas of majority atoms near interspecies resonances. Unlike in vacuum, we find that both the sign and magnitude of the dimer masses are tunable via Feshbach resonances. We also investigate the effects of particle-hole fluctuations on the dispersion of dimers and demonstrate that the particle-hole fluctuations near a Fermi surface (with Fermi momentum ({Dirac_h}/2{pi})k{sub F}) generally reduce the effective two-body interactions and the binding energy of dimers. Furthermore, in the limit of light minority atoms the particle-hole fluctuations disfavor the formation of dimers with a total momentum ({Dirac_h}/2{pi})k{sub F}, because near ({Dirac_h}/2{pi})k{sub F} the modes where the dominating particle-hole fluctuations appear are the softest. Our calculation suggests that near broad interspecies resonances when the minority-majority mass ratio m{sub B}/m{sub F} is smaller than a critical value (estimated to be 0.136), dimers in a finite-momentum channel are energetically favored over dimers in the zero-momentum channel. We apply our theory to quantum gases of {sup 6}Li{sup 40}K, {sup 6}Li{sup 87}Rb, {sup 40}K{sup 87}Rb, and {sup 6}Li{sup 23}Na near broad interspecies resonances, and discuss the limitations of our calculations and implications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Bound Exciton Complexes in Near-Infrared Emitting Quantum Shells

Near-infrared (NIR) light sources based on colloidal semiconductor nanocrystals (NCs) represent a scalable, low-cost alternative to epitaxial semiconductor platforms. However, their performance remains hindered by rapid Auger recombination, a problem that is particularly pronounced in narrow-bandgap materials. Here, we report on CdS/HgS/CdS and CdS/HgCdSe/ ZnS quantum shells (QSs), a class of spherical quantum wells specifically engineered for a suppression of nonradiative Auger processes. Fabricated QSs exhibit tunable NIR emission with photoluminescence quantum yields reaching ∼60% below 1000 nm and up to 30% near 1300 nm. Optical gain and stimulated emission were observed in CdS/HgS/CdS QSs. In contrast, CdS/HgCdSe/ZnS QSs displayed a photoinduced absorption in lieu of optical gain despite demonstrating a comparatively stronger Auger suppression. Transient absorption spectroscopy revealed that this phenomenon arises from the formation of bound multiexciton complexes that induce long-lived sub-bandgap multiexciton states. The observation of such bound excitonic clusters at room temperature offers a pathway toward nonlinear NIR photonic phenomena, including biexciton−exciton cascade emission, optical modulation, and singleexciton gain.

Auger recombination↗
DOE OSTI2015

Rigidity of poly-L-glutamic acid scaffolds: Influence of secondary and supramolecular structure

Poly-L-glutamic acid (PGA) is a widely used biomaterial, with applications ranging from drug delivery and biological glues to food products and as a tissue engineering scaffold. A biodegradable material with flexible conjugation functional groups, tunable secondary structure, and mechanical properties, PGA has potential as a tunable matrix material in mechanobiology. Some recent studies in proteins connecting dynamics, nanometer length scale rigidity, and secondary structure suggest a new point of view from which to analyze and develop this promising material. Our paper characterizes the structure, topology, and rigidity properties of PGA prepared with different molecular weights and secondary structures through various techniques including scanning electron microscopy, FTIR, light, and neutron scattering spectroscopy. On the length scale of a few nanometers, rigidity is determined by hydrogen bonding interactions in the presence of neutral species and by electrostatic interactions when the polypeptide is negatively charged. Finally, when probed over hundreds of nanometers, the rigidity of these materials is modified by long range intermolecular interactions that are introduced by the supramolecular structure.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Photophysics and Carrier Dynamics of Lasing in Quasi-2D Lead Halide Perovskites

Quasi-2D perovskites have recently been extensively studied due to their narrow-bandwidth-tunable emission, solution processability, and applicability as optical gain media. Quasi-2D perovskites are composed of inorganic perovskite crystal layers encapsulated with a bulky organic ligand such as phenylethylammonium, endowing the perovskite with a quantum-well structure and improved stability. In this article, we explore the photophysics of a quasi-2D metal halide perovskite as a promising light-harvesting and emitting medium. We find it exhibits high optical absorption (~10 5 cm -1 ) and an optically pumped amplified spontaneous emission threshold at 623 μJ/cm 2 . We study charge transfer processes in the complex mixed quantum wells of these perovskites through transient absorption and time-resolved photoluminescence measurements and develop a phenomenological model that incorporates optical gain for lasing. Further, while both free carriers and excitons are observed, we show surprisingly that photoluminescence is dominated by excitons despite the relatively small binding energy (~16 meV) of the low-energy band edge. Additionally, we extract the rates of exciton relaxation pathways, revealing a relatively large radiative term of 4.6 x 10 8 s -1 as well as an exciton-exciton annihilation term of 3.6 x 10 -13 cm 3 s -1 that is 3 orders of magnitude smaller than in similar quasi-2D perovskites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Controlling the Properties of Matter with Quantum Dots

Solar cells and photodetectors could soon be made from new types of materials based on semiconductor quantum dots, thanks to new insights based on ultrafast measurements capturing real-time photoconversion processes. Photoconversion is a process wherein the energy of a photon, or quantum of light, is converted into other forms of energy, for example, chemical or electrical. Semiconductor quantum dots are chemically synthesized crystalline nanoparticles that have been studied for more than three decades in the context of various photoconversion schemes including photovoltaics (generation of photo-electricity) and photo-catalysis (generation of “solar fuels”). The appeal of quantum dots comes from the unmatched tunability of their physical properties, which can be adjusted by controlling the size, shape and composition of the dots. At Los Alamos, the research connects to the institutional mission of solving national security challenges through scientific excellence, in this case focusing on novel physical principles for highly efficient photoconversion, charge manipulation in exploratory device structures and novel nanomaterials.

14 SOLAR ENERGY↗
DOE OSTI2016

Optically Thin Metallic Films for High-Radiative-Efficiency Plasmonics

Plasmonics enables deep-subwavelength concentration of light and has become important for fundamental studies as well as real-life applications. Two major existing platforms of plasmonics are metallic nanoparticles and metallic films. Metallic nanoparticles allow efficient coupling to far field radiation, yet their synthesis typically leads to poor material quality. Metallic films offer substantially higher quality materials, but their coupling to radiation is typically jeopardized due to the large momentum mismatch with free space. We propose and theoretically investigate optically thin metallic films as an ideal platform for high-radiative-efficiency plasmonics. For far-field scattering, adding a thin high-quality metallic substrate enables a higher quality factor while maintaining the localization and tunability that the nanoparticle provides. For near-field spontaneous emission, a thin metallic substrate, of high quality or not, greatly improves the field overlap between the emitter environment and propagating surface plasmons, enabling high-Purcell (total enhancement >10 4 ), high-quantum-yield (>50%) spontaneous emission, even as the gap size vanishes (3–5 nm). The enhancement has almost spatially independent efficiency and does not suffer from quenching effects that commonly exist in previous structures.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2017

Enhanced Light Absorption in Fluorinated Ternary Small-Molecule Photovoltaics

Using small-molecule donor (SMD) semiconductors in organic photovoltaics (OPVs) has historically afforded lower power conversion efficiencies (PCEs) than their polymeric counterparts. The PCE difference is attributed to shorter conjugated backbones, resulting in reduced intermolecular interactions. Here, a new pair of SMDs is synthesized based on the diketopyrrolopyrrole-benzodithiophene-diketopyrrolopyrrole (BDT-DPP2) skeleton but having fluorinated and fluorinefree aromatic side-chain substituents. Ternary OPVs having varied ratios of the two SMDs with PC61BM as the acceptor exhibit tunable open-circuit voltages (Vocs) between 0.833 and 0.944 V due to a fluorination-induced shift in energy levels and the electronic “alloy” formed from the miscibility of the two SMDs. A 15% increase in PCE is observed at the optimal ternary SMD ratio, with the short-circuit current density (Jsc) significantly increased to 9.18 mA/cm2. The origin of Jsc enhancement is analyzed via charge generation, transport, and diffuse reflectance measurements, and is attributed to increased optical absorption arising from a maximum in film crystallinity at this SMD ratio, observed by grazing incidence wide-angle X-ray scattering.

14 SOLAR ENERGY↗