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DOE OSTI2022

Semi-empirical quantum optics for mid-infrared molecular nanophotonics

Nanoscale infrared (IR) resonators with sub-diffraction limited mode volumes and open geometries have emerged as new platforms for implementing cavity quantum electrodynamics at room temperature. The use of IR nanoantennas and tip nanoprobes to study strong light–matter coupling of molecular vibrations with the vacuum field can be exploited for IR quantum control with nanometer spatial and femtosecond temporal resolution. In order to advance the development of molecule-based quantum nanophotonics in the mid-IR, we propose a generally applicable semi-empirical methodology based on quantum optics to describe light–matter interaction in systems driven by mid-IR femtosecond laser pulses. The theory is shown to reproduce recent experiments on the acceleration of the vibrational relaxation rate in infrared nanostructures. It also provides physical insights on the implementation of coherent phase rotations of the near-field using broadband nanotips. We then apply the quantum framework to develop general tip-design rules for the experimental manipulation of vibrational strong coupling and Fano interference effects in open infrared resonators. We finally propose the possibility of transferring the natural anharmonicity of molecular vibrational levels to the resonator near-field in the weak coupling regime to implement intensity-dependent phase shifts of the coupled system response with strong pulses and develop a vibrational chirping model to understand the effect. The semi-empirical quantum theory is equivalent to first-principles techniques based on Maxwell’s equations, but its lower computational cost suggests its use as a rapid design tool for the development of strongly coupled infrared nanophotonic hardware for applications ranging from quantum control of materials to quantum information processing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Reconfiguring band-edge states and charge distribution of organic semiconductor–incorporated 2D perovskites via pressure gating

Two-dimensional (2D) semiconductor heterostructures are key building blocks for many electronic and optoelectronic devices. Reconfiguring the band-edge states and modulating their interplay with charge carriers at the interface in a continuous manner have long been sought yet are challenging. Here, using organic semiconductor–incorporated 2D halide perovskites as the model system, we realize the manipulation of band-edge states and charge distribution via mechanical—rather than chemical or thermal—regulation. Compression induces band-alignment switching and charge redistribution due to the different pressure responses of organic and inorganic building blocks, giving controllable emission properties of 2D perovskites. We propose and demonstrate a “pressure gating” strategy that enables the control of multiple emission states within a single material. We also reveal that band-alignment transition at the organic-inorganic interface is intrinsically not well resolved at room temperature owing to the thermally activated transfer and shuffling of band-edge carriers. This work provides important fundamental insights into the energetics and carrier dynamics of hybrid semiconductor heterostructures.

42 ENGINEERING↗

NASA NTRS1977

Magnetic Stirling cycles - A new application for magnetic materials

There is the prospect of a fundamental new application for magnetic materials as the working substance in thermodynamic cycles. Recuperative cycles which use a rare-earth ferromagnetic material near its Curie point in the field of a superconducting magnet appear feasible for applications from below 20 K to above room temperature. The elements of the cycle, advanced in an earlier paper, are summarized. The basic advantages include high entropy density in the magnetic material, completely reversible processes, convenient control of the entropy by the applied field, the feature that heat transfer is possible during all processes, and the ability of the ideal cycle to attain Carnot efficiency. The mean field theory is used to predict the entropy of a ferromagnet in an applied field and also the isothermal entropy change and isentropic temperature change caused by applying a field. Results are presented for J = 7/2 and g = 2. The results for isentropic temperature change are compared with experimental data on Gd. Coarse mixtures of ferromagnetic materials with different Curie points are proposed to modify the path of the cycle in the T-S diagram in order to improve the efficiency or to increase the specific power.

Brown, G. V.↗

NASA NTRS1993

SAMPEX payload operation control center implementation

The Solar Anomolous and Magnetospheric Explorer (SAMPEX) satellite was launched in July 1992. It was the first in the NASA Small Explorer (SMEX) series. In building the real-time control center facility, several new mission support challenges had to be met: CCSDS telemetry and command format, 900 Kbps telemetry data, and shorter turn-around time for control center development than previous missions. The SAMPEX Payload Operations Control Ccnter (POCC) was also the first control center for a new satellite to be based on the Transportable Payload Operations Control Center (TPOCC) system architecture and methodology. This approach has both guided the implementation of the SAMPEX control center and provided some of the building blocks. By using the TPOCC architecture to build the SAMPEX POCC, the real-time operations area was miniaturized into one room, whereas previous missions needed multiple large rooms. The development cost of the SAMPEX POCC was reduced from previous missions and will provide for further cost savings in the future SMEX satellites. This paper describes the system as built and some of the enhancements in progress to create this teleoperations environment.

Mandl, Daniel↗

NASA NTRS1992

Inelastic deformation mechanisms in a transverse MMC lamina under compression

An investigation was undertaken to study the inelastic deformation mechanisms in (90)(sub 8) Ti 15-3/SCS-6 lamina subjected to pure compression. Both mechanical behavior and microstructural evaluation were undertaken at room temperature, 538 and 650 C. Results indicate that mechanical response and deformation characteristics are significantly different in monotonic tension and compression. The inelastic deformation mechanisms in compression are controlled by radial fiber fracture, matrix plasticity and fiber-matrix debonding. The radial fiber fracture is a new damage mode observed for metal-matrix composites (MMC).

Newaz, Golam M.↗

NASA NTRS1994

Preparation and characterization of poly (arylene ether isoxazole)s by fluoride ion-mediated aromatic nucleophilic displacement reactions

As part of a continuing effort to prepare novel thermally stable high-performance polymers, poly(arylene ether isoxazole)s have been prepared by fluoride ion-catalyzed aromatic nucleophilic substitution reactions with bis(trimethylsiloxyphenyl) isoxazoles and activated bisarylhalides in diphenyl sulfone. Initial investigation involving the preparation of these materials with isoxazole bisphenols and activated bisarylhalides in the presence of potassium carbonate indicated that, under reaction conditions necessary to prepare high-molecular-weight materials, the isoxazole monomer was converted to an enamino ketone. This side reaction was avoided by using fluoride as a base. However, trimethylsilyl ether derivatives of the isoxazole bisphenols were required in these polymerizations for the preparation of high-molecular-weight materials. Moderate to high inherent viscosity eta(sub inh): 0.43-0.87 dl/g) materials with good thermal stability (air: 409-477 C, helium: 435-512 C) can be prepared by the silyl ether method. Glass transition temperatures ranged from 182 to 225 C for polymers with phenyl pendants and from 170 to 214 C for those without. Molecular weight control by 2% endcapping and the incorporation of a phenyl pendant at the 4 position of the isoxazole is necessary to yield polymers soluble in polar aprotic solvents at room temperature. There is evidence, however, indicating the existence of crosslinks between the polymer chains when the silyl ether approach is utilized.

Herbert, C. G.↗

NASA NTRS2011

The Traverse Planning Process for the Drats 2010 Analog Field Simulations

Traverse planning concentrates on optimizing the science return within the overall objectives of planetary surface missions or their analog field simulations. Such simulations were conducted in the San Francisco Volcanic Field, northern Arizona, from Aug. 26 to Sept 17, 2010 and involved some 200 individuals in the field, with some 40 geoscientists composing the science team. The purpose of these Desert Research and Technology Studies (DRATS) is to exercise and evaluate developmental hardware, software and operational concepts in a mission-like, fully-integrated, setting under the direction of an onsite Mobile Mission Control Center(MMCC). DRATS 2010 focused on the simultaneous operation of 2 rovers, a historic first. Each vehicle was manned by an astronaut-commander and an experienced field geologist. Having 2 rovers and crews in the field mandated substantially more complex science and mission control operations compared to the single rover DRATS tests of 2008 and 2009, or the Apollo lunar missions. For instance, the science support function was distributed over 2 "back rooms", one for each rover, with both "tactical" teams operating independently and simultaneously during the actual traverses. Synthesis and integration of the daily findings and forward planning for the next day(s) was accomplished overnight by yet another "strategic" science team.

Horz, Friedrich↗

NASA NTRS2018

Autonomous Path-Following for a Tilt-Wing, Distributed Electric Propulsion, Vertical Take-Off and Landing Unmanned Aerial System in Hover Mode

This paper presents an autonomous path-following control architecture for a tilt-wing, distributed electric propulsion, vertical take-off and landing unmanned aerial system in hover mode and presents indoor flight test results. The test-bed vehicle is a subscale model with the same configuration as the NASA GL-10 aircraft. The control architecture consists of an inner-loop attitude controller, outer-loop trajectory controller, and a trajectory generation scheme. The flight test results show that the vehicle can satisfactorily follow a path prescribed by a list of waypoints around the indoor flight room.

Cooper, John R.↗

DOE OSTI2017

Position and orientation determination system and method

A position determination system and method is provided that may be used for obtaining position and orientation information of a detector in a contaminated room. The system includes a detector, a sensor operably coupled to the detector, and a motor coupled to the sensor to move the sensor around the detector. A CPU controls the operation of the motor to move the sensor around the detector and determines distance and angle data from the sensor to an object. The method includes moving a sensor around the detector and measuring distance and angle data from the sensor to an object at incremental positions around the detector.

47 OTHER INSTRUMENTATION↗

DOE OSTI2015

Broadband control of emission wavelength of InAs/GaAs quantum dots by GaAs capping temperature

We investigated the effects of the GaAs capping temperature on the morphological and photoluminescence (PL) properties of InAs quantum dots (QDs) on GaAs(001). The broadband tuning of the emission wavelength from 1.1 to 1.3 μm was achieved at room temperature by only adjusting the GaAs capping temperature. As the capping temperature was decreased, the QD shrinkage due to In desorption and In-Ga intermixing during the capping process was suppressed. This led to QDs with a high aspect ratio, and resultantly, the emission wavelength shifted toward the longer-wavelength side. In addition, the linearly polarized PL intensity elucidated anisotropic characteristics reflecting the shape anisotropy of the embedded QDs, in which a marked change in polarization anisotropy occurred at capping temperatures lower than 460 °C.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1999

Acute effect of ephedrine on 24-h energy balance

Ephedrine is used to help achieve weight control. Data on its true efficacy and mechanisms in altering energy balance in human subjects are limited. We aimed to determine the acute effect of ephedrine on 24-h energy expenditure, mechanical work and urinary catecholamines in a double-blind, randomized, placebo-controlled, two-period crossover study. Ten healthy volunteers were given ephedrine (50 mg) or placebo thrice daily during each of two 24-h periods (ephedrine and placebo) in a whole-room indirect calorimeter, which accurately measures minute-by-minute energy expenditure and mechanical work. Measurements were taken of 24-h energy expenditure, mechanical work, urinary catecholamines and binding of (+/-)ephedrine in vitro to human beta1-, beta2- and beta3-adrenoreceptors. Twenty-four-hour energy expenditure was 3.6% greater (8965+/-1301 versus 8648+/-1347 kJ, P<0.05) with ephedrine than with placebo, but mechanical work was not different between the ephedrine and placebo periods. Noradrenaline excretion was lower with ephedrine (0.032+/-0.011 microg/mg creatinine) compared with placebo (0.044+/-0.012 microg/mg creatinine) (P<0.05). (+/-)Ephedrine is a relatively weak partial agonist of human beta1- and beta2-adrenoreceptors, and had no detectable activity at human beta3-adrenoreceptors. Ephedrine (50 mg thrice daily) modestly increases energy expenditure in normal human subjects. A lack of binding of ephedrine to beta3-adrenoreceptors and the observed decrease in urinary noradrenaline during ephedrine treatment suggest that the thermogenic effect of ephedrine results from direct beta1-/beta2-adrenoreceptor agonism. An indirect beta3-adrenergic effect through the release of noradrenaline seems unlikely as urinary noradrenaline decreased significantly with ephedrine.

Non-NASA Center↗

DOE OSTI2016

Room temperature strong light-matter coupling in three dimensional terahertz meta-atoms

We demonstrate strong light-matter coupling in three dimensional terahertz meta-atoms at room temperature. The intersubband transition of semiconductor quantum wells with a parabolic energy potential is strongly coupled to the confined circuital mode of three-dimensional split-ring metal-semiconductor-metal resonators that have an extreme sub-wavelength volume (λ/10). The frequency of these lumped-element resonators is controlled by the size and shape of the external antenna, while the interaction volume remains constant. This allows the resonance frequency to be swept across the intersubband transition and the anti-crossing characteristic of the strong light-matter coupling regime to be observed. The Rabi splitting, which is twice the Rabi frequency (2Ω{sub Rabi}), amounts to 20% of the bare transition at room temperature, and it increases to 28% at low-temperature.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS2006

Highly Efficient Multilayer Thermoelectric Devices

Multilayer thermoelectric devices now at the prototype stage of development exhibit a combination of desirable characteristics, including high figures of merit and high performance/cost ratios. These devices are capable of producing temperature differences of the order of 50 K in operation at or near room temperature. A solvent-free batch process for mass production of these state-of-the-art thermoelectric devices has also been developed. Like prior thermoelectric devices, the present ones have commercial potential mainly by virtue of their utility as means of controlled cooling (and/or, in some cases, heating) of sensors, integrated circuits, and temperature-critical components of scientific instruments. The advantages of thermoelectric devices for such uses include no need for circulating working fluids through or within the devices, generation of little if any noise, and high reliability. The disadvantages of prior thermoelectric devices include high power consumption and relatively low coefficients of performance. The present development program was undertaken in the hope of reducing the magnitudes of the aforementioned disadvantages and, especially, obtaining higher figures of merit for operation at and near room temperature. Accomplishments of the program thus far include development of an algorithm to estimate the heat extracted by, and the maximum temperature drop produced by, a thermoelectric device; solution of the problem of exchange of heat between a thermoelectric cooler and a water-cooled copper block; retrofitting of a vacuum chamber for depositing materials by sputtering; design of masks; and fabrication of multilayer thermoelectric devices of two different designs, denoted I and II. For both the I and II designs, the thicknesses of layers are of the order of nanometers. In devices of design I, nonconsecutive semiconductor layers are electrically connected in series. Devices of design II contain superlattices comprising alternating electron-acceptor (p)-doped and electron-donor (n)-doped, nanometer- thick semiconductor layers.

Boufelfel, Ali↗

DOE OSTI2016

Minimize the Voltage Degradation in Li-rich Layered Oxide Cathode Materials by Morphology Control

Li-rich layered oxides, either as a solid solution or as a nano-composite of layered Li 2 MnO 3 and Li(TM)O 2 (TM=Ni, Co, Mn), draw significant attention as the next-generation cathode materials for high-energy-density lithium ion batteries in electric vehicles. Over the past twenty years, the discharge capacity at room temperature of these cathode materials has been improved from 200 mAh g -1 to over 320 mAh g -1 today, even higher at elevated temperatures. While the research has continued to push the limit of the available capacity of the materials throughout the years, there are many issues still unclear. And numerous scientific challenges, especially voltage degradation during cycling of these materials, that must be overcome to realize their utilization in commercial lithium ion batteries. Here, we report a design of modified co-precipitation method without ammonia addition to synthesize morphology controlled Li-rich material Li 1.2 Ni 0.2 Mn 0.6 O 2 as high energy density cathode for lithium ion batteries. The obtained material has spherical secondary particles with uniform dispersion. The secondary particles are dense, and have an average diameter of approximately 3 μm. These secondary spherical particles consist of primary particles with particle size approximately 150 nm. The morphology controlled sample can minimize voltage decay as well as improve capacity retention during cycling. And furthermore, the influence of morphology control on the cycling performance has been investigated through Transmission X-ray Microscope.

Zhang, Minghao↗

DOE OSTI2022

Redox-controlled reorganization and flavin strain within the ribonucleotide reductase R2b–NrdI complex monitored by serial femtosecond crystallography

Redox reactions are central to biochemistry and are both controlled by and induce protein structural changes. Here, we describe structural rearrangements and crosstalk within the Bacillus cereus ribonucleotide reductase R2b–NrdI complex, a di-metal carboxylate-flavoprotein system, as part of the mechanism generating the essential catalytic free radical of the enzyme. Femtosecond crystallography at an X-ray free electron laser was utilized to obtain structures at room temperature in defined redox states without suffering photoreduction. Together with density functional theory calculations, we show that the flavin is under steric strain in the R2b–NrdI protein complex, likely tuning its redox properties to promote superoxide generation. Moreover, a binding site in close vicinity to the expected flavin O 2 interaction site is observed to be controlled by the redox state of the flavin and linked to the channel proposed to funnel the produced superoxide species from NrdI to the di-manganese site in protein R2b. These specific features are coupled to further structural changes around the R2b–NrdI interaction surface. The mechanistic implications for the control of reactive oxygen species and radical generation in protein R2b are discussed

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2014

Implementation of Statistical Process Control: Evaluating the Mechanical Performance of a Candidate Silicone Elastomer Docking Seal

The National Aeronautics and Space Administration has been developing a novel docking system to meet the requirements of future exploration missions to low-Earth orbit and beyond. A dynamic gas pressure seal is located at the main interface between the active and passive mating components of the new docking system. This seal is designed to operate in the harsh space environment, but is also to perform within strict loading requirements while maintaining an acceptable level of leak rate. In this study, a candidate silicone elastomer seal was designed, and multiple subscale test articles were manufactured for evaluation purposes. The force required to fully compress each test article at room temperature was quantified and found to be below the maximum allowable load for the docking system. However, a significant amount of scatter was observed in the test results. Due to the stochastic nature of the mechanical performance of this candidate docking seal, a statistical process control technique was implemented to isolate unusual compression behavior from typical mechanical performance. The results of this statistical analysis indicated a lack of process control, suggesting a variation in the manufacturing phase of the process. Further investigation revealed that changes in the manufacturing molding process had occurred which may have influenced the mechanical performance of the seal. This knowledge improves the chance of this and future space seals to satisfy or exceed design specifications.

docking seal↗

DOE OSTI2018

Lateral Standing of the Pentacene Derivative 5,6,7-Trithiapentacene-13-one on Gold: A Combined STM, DFT, and NC-AFM Study

In this paper, high resolution scanning tunneling microscopy investigation of the pentacene derivative, 5,6,7-trithiapentacene-13-one (TTPO), on close-packed gold surfaces reveals nanoscale structures ranging from molecular chains at low coverage to highly ordered self-assembled molecular monolayers. Robust, thermally stable, and highly inert to photo-oxidation, TTPO is a promising organic semiconductor with potential applications in high-temperature photovoltaic devices. When adsorbed on a gold electrode, experiment and first-principle computation reveal a novel 3-D angular assembly of the TTPO molecules, with the long axis of the molecule parallel to the gold surface, distinctive from previously observed pentacene and pentacene derivative assemblies. Structures assembled are angularly dependent on TTPO molecular interactions while commensurate with the underlying gold substrate, allowing for potential tailoring of π-molecular orbital overlap through tilt-angle control. Finally, rigorous noncontact atomic force microscopy analysis was used to experimentally determine the molecular tilt of the molecule at 5 K, consistent with the calculated and observed structures at room temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Mid-Infrared Photoluminescence from Tellurium Thin Films

Tellurium is an elemental semiconductor with a 0.34 eV optical band gap, showing promise for mid-infrared (MIR) optoelectronics including light-emitting diodes. However, quantitative measurement of the tellurium luminescence efficiency has not yet been investigated, and growing optically active films remain challenging. Here, we demonstrate the low-temperature growth of bright tellurium thin films by using physical vapor transport. The sample morphology is controlled by varying the growth temperature, yielding continuous thin films, microparticles, or nanowires. Additionally, we demonstrated patterned growth by using a seed layer for selective nucleation. Quantitative photoluminescence measurements at room temperature reveal an internal quantum yield of 2.0% at 0.34 eV for the as-grown tellurium films, comparable to the best-reported efficiencies of III-V and II-VI compound semiconductors with similar band gaps. Furthermore, we demonstrate band-gap tunability with Te-Se alloys, where up to 20% selenium incorporation gradually blue-shifts the band gap to 0.55 eV. The work demonstrates the potential use of tellurium for efficient MIR devices.

Wang, Shu↗