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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 127 records · Page 7

Effect of Solvent on Fluorescence Emission from Polyethylene Glycol-Coated Graphene Quantum Dots under Blue Light Illumination

To explore aggregate-induced emission (AIE) properties, this study adopts a one-pot hydrothermal route for synthesizing polyethylene glycol (PEG)-coated graphene quantum dot (GQD) clusters, enabling the emission of highly intense photoluminescence under blue light illumination. The hydrothermal synthesis was performed at 300 °C using o-phenylenediamine as the nitrogen and carbon sources in the presence of PEG. Three different solvents, propylene glycol methyl ether acetate (PGMEA), ethanol, and water, were used for dispersing the PEG-coated GQDs, where extremely high fluorescent emission was achieved at 530–550 nm. It was shown that the quantum yield (QY) of PEG-coated GQD suspensions is strongly dependent on the solvent type. The pristine GQD suspension tends to be quenched (i.e., QY: ~1%) when dispersed in PGMEA (aggregation-caused quenching). However, coating GQD nanoparticles with polyethylene glycol results in substantial enhancement of the quantum yield. When investigating the photoluminescence emission from PEG-coated GQD clusters, the surface tension of the solvents was within the range of from 26.9 to 46.0 mN/m. This critical index can be tuned for assessing the transition point needed to activate the AIE mechanism which ultimately boosts the fluorescence intensity. The one-pot hydrothermal route established in this study can be adopted to engineer PEG-coated GQD clusters with solid-state PL emission capabilities, which are needed for next-generation optical, bio-sensing, and energy storage/conversion devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Quieting a noisy antenna reproduces photosynthetic light-harvesting spectra

Photosynthesis achieves near unity light-harvesting quantum efficiency yet it remains unknown whether there exists a fundamental organizing principle giving rise to robust light harvesting in the presence of dynamic light conditions and noisy physiological environments. Here, we present a noise-canceling network model that relates noisy physiological conditions, power conversion efficiency, and the resulting absorption spectra of photosynthetic organisms. Using light conditions in full solar exposure, light filtered by oxygenic phototrophs, and light filtered under seawater, we derived optimal absorption characteristics for efficient solar power conversion. We show how light-harvesting antennae can be tuned to maximize power conversion efficiency by minimizing excitation noise, thus providing a unified theoretical basis for the observed wavelength dependence of absorption in green plants, purple bacteria, and green sulfur bacteria.

Science & Technology - Other Topics↗

Quenching of the quantum p -strength in light exotic nuclei

One-nucleon spectroscopic overlaps, their strength or spectroscopic factors (SFs), and nucleon removal cross sections for light nuclei in the mass range A≤12 were evaluated using the fully correlated Quantum Monte Carlo (QMC) wave functions (WFs). Harder (AV18+UX) and softer (NV2+3) bare interactions were used providing consistent results. The SFs were also taken from simple Shell Model (SM) calculations. This structure information was incorporated in the standard three-body Faddeev/Alt-Grassberger-Sandhas reaction formalism to evaluate the (p,pN) cross sections. The results further our understanding of the quenching of the quantum p-shell strength obtained from structure and reactions. We have found the ratios of the total QMC sums of SFs to the SM ones to be uniform and ∼ 3/4. The corresponding ratios of the sums Below Particle Threshold (BPT) of SFs, as well as of total cross sections, deviate strikingly from the uniform trend in some special cases. We find these ratios to be close to unit for 9 Li → 8 Li + n and 9 C → 8 B + p. In contrast, they are strongly reduced for 11 C → 10 C + n and 11 B → 10 Be + p mirror transitions, resulting from the quenching of the strength for low-lying 2 + final state transitions. The QMC theoretical cross section BPT for 11 C(p,pn) is about two times smaller than the experimental data.

(p,pN) reactions↗

Octopus, a computational framework for exploring light-driven phenomena and quantum dynamics in extended and finite systems

Over the last few years, extraordinary advances in experimental and theoretical tools have allowed us to monitor and control matter at short time and atomic scales with a high degree of precision. An appealing and challenging route toward engineering materials with tailored properties is to find ways to design or selectively manipulate materials, especially at the quantum level. To this end, having a state-of-the-art ab initio computer simulation tool that enables a reliable and accurate simulation of light-induced changes in the physical and chemical properties of complex systems is of utmost importance. The first principles real-space-based Octopus project was born with that idea in mind, i.e., to provide a unique framework that allows us to describe non-equilibrium phenomena in molecular complexes, low dimensional materials, and extended systems by accounting for electronic, ionic, and photon quantum mechanical effects within a generalized time-dependent density functional theory. This article aims to present the new features that have been implemented over the last few years, including technical developments related to performance and massive parallelism. We also describe the major theoretical developments to address ultrafast light-driven processes, such as the new theoretical framework of quantum electrodynamics density-functional formalism for the description of novel light–matter hybrid states. Those advances, and others being released soon as part of the Octopus package, will allow the scientific community to simulate and characterize spatial and time-resolved spectroscopies, ultrafast phenomena in molecules and materials, and new emergent states of matter (quantum electrodynamical-materials).

74 ATOMIC AND MOLECULAR PHYSICS↗

Geometrically Tunable Beamed Light Emission from a Quantum‐Dot Ensemble Near a Gradient Metasurface

Abstract Optical metasurfaces have been widely investigated in recent years as a means to tailor the wavefronts of externally incident light for passive device applications. At the same time, their use in active optoelectronic devices such as light emitters is far less established. This work explores their ability to control the radiation properties of a nearby continuous ensemble of randomly oriented incoherent dipole sources via near‐field interactions. Specifically, a film of colloidal quantum dots is deposited on a plasmonic metasurface consisting of a 1D array of metallic nanoantennas on a metal film. The array is designed to introduce a linear phase profile upon reflection, and a bi‐periodic nanoparticle arrangement is introduced to ensure adequate sampling of the desired phase gradient. Highly directional radiation patterns are correspondingly obtained from the quantum dots at an enhanced emission rate. The underlying radiation mechanism involves the near‐field excitation of surface plasmon polaritons at the metal film, and their selective diffractive scattering by the metasurface into well‐collimated beams along predetermined geometrically tunable directions. These results underscore the distinctive ability of metasurfaces to control radiation properties directly at the source level, which is technologically significant for the continued miniaturization and large‐scale integration of optoelectronic devices.

Wang, Xiaowei↗

Light-Front Field Theory on Current Quantum Computers

We present a quantum algorithm for simulation of quantum field theory in the light-front formulation and demonstrate how existing quantum devices can be used to study the structure of bound states in relativistic nuclear physics. Specifically, we apply the Variational Quantum Eigensolver algorithm to find the ground state of the light-front Hamiltonian obtained within the Basis Light-Front Quantization (BLFQ) framework. The BLFQ formulation of quantum field theory allows one to readily import techniques developed for digital quantum simulation of quantum chemistry. This provides a method that can be scaled up to simulation of full, relativistic quantum field theories in the quantum advantage regime. As an illustration, we calculate the mass, mass radius, decay constant, electromagnetic form factor, and charge radius of the pion on the IBM Vigo chip. This is the first time that the light-front approach to quantum field theory has been used to enable simulation of a real physical system on a quantum computer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

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)↗

Efficient Source of Shaped Single Photons Based on an Integrated Diamond Nanophotonic System

An efficient, scalable source of shaped single photons that can be directly integrated with optical fiber networks and quantum memories is at the heart of many protocols in quantum information science. We demonstrate a deterministic source of arbitrarily temporally shaped single-photon pulses with high efficiency [detection efficiency = 14.9 %] and purity [g (2) (0) = 0.0168] and streams of up to 11 consecutively detected single photons using a silicon-vacancy center in a highly directional fiber-integrated diamond nanophotonic cavity. Finally, combined with previously demonstrated spin-photon entangling gates, this system enables on-demand generation of streams of correlated photons such as cluster states and could be used as a resource for robust transmission and processing of quantum information.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Light-driven transitions in quantum paraelectrics

Motivated by recent experiments on pump-induced polar ordering in the quantum paraelectric SrTiO 3 , we study a driven phonon system close to a second-order phase transition. Analyzing its classical dynamics, we find that sufficiently strong driving leads to transitions into polar phases whose structures, determined by the light polarization, are not all accessible in equilibrium. In addition, for certain intensity profiles, we demonstrate the possibility of two-step transitions as a function of fluence. For even stronger field intensities, the possibility of period-doubling and chaotic behavior is demonstrated. Finally we develop a generalized formalism that allows us to consider quantum corrections to the classical dynamics in a systematic fashion. Furthermore, we predict a shift in the critical pump fluence due to quantum fluctuations with a characteristic dependence on the fluence increase rate that should be observable in experiment.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Light-wave control of correlated materials using quantum magnetism during time-periodic modulation of coherent transport

Light–wave quantum electronics utilizes the oscillating carrier wave to control electronic properties with intense laser pulses. Without direct light–spin interactions, however, magnetic properties can only be indirectly affected by the light electric field, mostly at later times. A grand challenge is how to establish a universal principle for quantum control of charge and spin fluctuations, which can allow for faster-than-THz clock rates. Using quantum kinetic equations for the density matrix describing non–equilibrium states of Hubbard quasiparticles, here we show that time–periodic modulation of electronic hopping during few cycles of carrier–wave oscillations can dynamically steer an antiferromagnetic insulating state into a metalic state with transient magnetization. While nonlinearities associated with quasi-stationary Floquet states have been achieved before, magneto–electronics based on quasiparticle acceleration by time–periodic multi–cycle fields and quantum femtosecond/attosecond magnetism via strongly–coupled charge–spin quantum excitations represents an alternative way of controlling magnetic moments in sync with quantum transport.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Parallel Quantum-Enhanced Sensing

Quantum metrology takes advantage of quantum correlations to enhance the sensitivity of sensors and measurement techniques beyond their fundamental classical limit, given by the shot-noise limit. The use of both temporal and spatial correlations present in quantum states of light can extend quantum-enhanced sensing to a parallel configuration that can simultaneously probe an array of sensors or independently measure multiple parameters. To this end, we use multispatial-mode bright twin beams of light, which are characterized by independent quantum-correlated spatial subregions in addition to quantum temporal correlations, to probe a four-sensor quadrant plasmonic array. We show that it is possible to independently and simultaneously measure local changes in refractive index for all four sensors with a quantum enhancement in sensitivity in the range of 22% to 24% over the corresponding classical configuration. Finally, these results provide a first step toward highly parallel spatially resolved quantum-enhanced sensing techniques and pave the way toward more complex quantum sensing and quantum imaging platforms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Colloidal Germanium Quantum Dots with Broadly Tunable Size and Light Emission

Germanium (Ge) colloidal quantum dots (CQDs) were synthesized by thermal decomposition of GeI 2 using capping ligand mixtures of oleylamine (OAm), octadecene (ODE), and trioctylphosphine (TOP). Average diameters could be tuned across a wide range, from 3 to 18 nm, by adjusting reactant concentrations, heating rates, and reaction temperatures. OAm promotes decomposition of GeI 2 to Ge and serves as a weakly bound capping ligand. ODE displaces OAm during the reaction to terminate particle growth and prevent surface oxidation. TOP is necessary for obtaining nanocrystals larger than 11 nm. In conclusion, the Ge CQDs have relatively narrow size distributions and exhibit size-dependent, band-edge photoluminescence (PL), with peak energies from 0.8 to 1.34 eV, across a wide spectral range in the infrared (IR).

Noh, Jungchul [Univ. of Texas, Austin, TX (United ↗

Interplay of negative electronic compressibility and capacitance enhancement in lightly-doped metal oxide Bi 0.95 La 0.05 FeO 3 by quantum capacitance model

Light-sensitive capacitance variation of Bi 0.95 La 0.05 FeO 3 (BLFO) ceramics has been studied under violet to UV irradiation. The reversible capacitance enhancement up to 21% under 405 nm violet laser irradiation has been observed, suggesting a possible degree of freedom to dynamically control this in high dielectric materials for light-sensitive capacitance applications. By using ultraviolet photoemission spectroscopy (UPS), we show here that exposure of BLFO surfaces to UV light induces a counterintuitive shift of the O 2p valence state to lower binding energy of up to 243 meV which is a direct signature of negative electronic compressibility (NEC). A decrease of BLFO electrical resistance agrees strongly with the UPS data suggesting the creation of a thin conductive layer on its insulating bulk under light irradiation. By exploiting the quantum capacitance model, we find that the negative quantum capacitance due to this NEC effect plays an important role in this capacitance enhancement.

36 MATERIALS SCIENCE↗

One Pot Synthesis of Cyan Emitting CdZnSSe Quantum Dots for Human Centric Lighting

A one pot synthesis of blue and green emissive CdZnSSe quantum dots (QDs) from thio- and selenoureas and Cd and Zn carboxylates is optimized using high throughput robotic optimization. A large set of spectral data (N = 192) is used to train machine learning models that accurately predict the photoluminescence emission wavelength (λmax) and full-width half-maximum, and the relative photoluminescence quantum yield (PLQY) from the S:Se and Zn:Cd stoichiometries and reaction time. ZnS shells are deposited on the crude QD heterostructures using 4-tert-butylbenzyl mercaptan, a more reactive source of sulfide that enables shell growth below the temperature where ion diffusion in the QD can broaden its optical spectrum (≤275 °C). These optimized procedures provide gram quantities of blue-green emitting QDs (PLQY = 85–99%) in a single reaction vessel. A solid state lighting device (4260 K) that incorporates cyan emissive QDs achieved a higher luminous efficacy of 179 lm/W and melanopic daylight efficiency ratio (0.71) than existing commercial human centric lighting devices.

Jordan, Abraham J↗

Reduction of efficiency droop in c -plane InGaN/GaN light-emitting diodes using a thick single quantum well with doped barriers

We report on c-plane InGaN/GaN single quantum well (QW) light-emitting diodes (LEDs) of different well widths (3 or 9 nm) with and without doped barriers. QW barriers were doped with the aim of reducing the internal electric field (F QW ) in the QW to increase the electron-hole overlap, therefore increasing the recombination rates and resulting in the reduction of the efficiency droop. We, indeed, observed, through biased photocurrent spectroscopy, a reduction in F QW with doped barriers, with F QW being in the same direction of the p-n junction field at zero bias as opposed to the junction field for LEDs without doped barriers. Even with the improvement in the ground state wavefunction overlap, the ground state transition rate remains low for thick QWs. Transitions through excited states were observed for both thick QW LEDs with and without doped barriers. Here, the thick QW LED without doped barriers displayed low external quantum efficiency (EQE), likely as a result of the carrier overflow due to the poor confinement of carriers in the excited states. On the other hand, for LEDs with doped barriers, the flatter band in the QW resulting from the lower F QW reduces the energy separation between the eigenstates, leading to better confinement of carriers in the excited states. With doped barriers, we demonstrated a low efficiency droop 9-nm-thick single QW LED with a peak EQE of 42% at 40 A/cm 2 and an EQE of 36% at 400 A/cm 2 .

42 ENGINEERING↗