Search NASA⌕ Search

SEARCH · Search NASA

Results for “spontaneous emission”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 55 records · Page 3

Strong Effect of Nonpolar Solvent Molecular Structure on CdSe Nanoplatelet Stacking

We report a drastic difference in stacking behavior of oleic acid-stabilized 4-monolayer (4 ML) CdSe nanoplatelets (NPLs) in toluene and methylcyclohexane (MCH), two nonpolar solvents that differ in the conformational flexibility of their molecules. Using liquid cell transmission electron microscopy (TEM) and small angle scattering (SAXS) techniques, we show that NPLs form microns-long ribbons consisting of 4 ML CdSe NPLs in toluene, the solvent widely used to form stable colloidal solutions of a broad range of quasi-spherical nanoparticles. In contrast, 4 ML CdSe NPLs are well dispersed in MCH. The difference in stacking behavior of NPLs in toluene and MCH suggests that the conformational flexibility of the solvent molecules, such as the ability to adopt multiple chair conformations, modulates nanoplatelet interactions. Molecular dynamics (MD) simulations reveal that solvent molecules subtly alter the structure of the organic ligand shell. These solvent-dependent changes propagate to the inorganic core, modulating the degree of CdSe nanoplatelet (NPL) twisting and, consequently, the properties of the nanoparticles. We show that toluene better solvates oleate ligands while MCH induces a bimodal oleate span distribution, which can lead to increased solubility of CdSe NPLs. In addition, the solvent can also influence the inorganic core, which, in turn, can modify the nanoparticle properties. We demonstrate that destabilization of toluene solution containing ribbons of 4 ML CdSe NPLs without CdS shells results in the formation of NPL assemblies with amplified spontaneous emission (ASE) with a low threshold of 14 µJ cm−2 that is comparable with that of CdSe/CdS core/shell NPLs. Our results emphasize that the solvent plays a major role in mediating interactions between NPLs and hence their processability for fabrication of functional structures.

CdSe↗

Superradiant Neutrino Lasers from Radioactive Condensates

Superradiance emerges from collective spontaneous emission in optically pumped gases, and is characterized by photon emission enhancements of up to $\frac{1}{4}$⁢𝑁 2 in an 𝑁 atom system. The gain mechanism derives from correlations developed within the decay medium rather than from stimulated emission as in lasing, so an analog of this process should be possible for fermionic final states. We introduce here the concept of superradiant neutrino emission from a radioactive Bose Einstein condensate, which can form the basis for a superradiant neutrino laser. A plausible experimental realization based on a condensate of electron-capture isotope 83 Rb could exhibit effective radioactive decay rates accelerated from 86.2 days to minutes in viably sized rubidium condensates of 10 6 atoms.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Metasurfaces with Multipolar Resonances and Enhanced Light–Matter Interaction

Metasurfaces, composed of engineered nanoantennas, enable unprecedented control over electromagnetic waves by leveraging multipolar resonances to tailor light–matter interactions. This review explores key physical mechanisms that govern their optical properties, including the role of multipolar resonances in shaping metasurface responses, the emergence of bound states in the continuum (BICs) that support high-quality factor modes, and the Purcell effect, which enhances spontaneous emission rates at the nanoscale. These effects collectively underpin the design of advanced photonic devices with tailored spectral, angular, and polarization-dependent properties. This review discusses recent advances in metasurfaces and applications based on them, highlighting research that employs full-wave numerical simulations, analytical and semi-analytic techniques, multipolar decomposition, nanofabrication, and experimental characterization to explore the interplay of multipolar resonances, bound and quasi-bound states, and enhanced light–matter interactions. A particular focus is given to metasurface-enhanced photodetectors, where structured nanoantennas improve light absorption, spectral selectivity, and quantum efficiency. By integrating metasurfaces with conventional photodetector architectures, it is possible to enhance responsivity, engineer photocarrier generation rates, and even enable functionalities such as polarization-sensitive detection. The interplay between multipolar resonances, BICs, and emission control mechanisms provides a unified framework for designing next-generation optoelectronic devices. This review consolidates recent progress in these areas, emphasizing the potential of metasurface-based approaches for high-performance sensing, imaging, and energy-harvesting applications.

Kerker effect↗

Gain roll-off in cadmium selenide colloidal quantum wells under intense optical excitation

Colloidal quantum wells, or nanoplatelets, show among the lowest thresholds for amplified spontaneous emission and lasing among solution-cast materials and among the highest modal gains of any known materials. Using solution measurements of colloidal quantum wells, this work shows that under photoexcitation, optical gain increases with pump fluence before rolling off due to broad photoinduced absorption at energies lower than the band gap. Despite the common occurrence of gain induced by an electron–hole plasma found in bulk materials and epitaxial quantum wells, under no measurement conditions was the excitonic absorption of the colloidal quantum wells extinguished and gain arising from a plasma observed. Instead, like gain, excitonic absorption reaches a minimum intensity near a photoinduced carrier sheet density of 2 × 10 13 cm –2 above which the absorption peak begins to recover. To understand the origins of these saturation and reversal effects, measurements were performed with different excitation energies, which deposit differing amounts of excess energy above the band gap. Across many samples, it was consistently observed that less energetic excitation results in stronger excitonic bleaching and gain for a given carrier density. Transient and static optical measurements at elevated temperatures, as well as transient X-ray diffraction of the samples, suggest that the origin of gain saturation and reversal is a heating and disordering of the colloidal quantum wells which produces sub-gap photoinduced absorption.

36 MATERIALS SCIENCE↗

Quantum Fluctuations and Lineshape Anomaly in a High‐ β Silver‐Coated InP‐Based Metallic Nanolaser

Abstract Metallic nanocavity lasers provide important technological advancement toward even smaller integrable light sources. They give access to widely unexplored lasing physics in which the distinction between different operational regimes, like those of thermal or coherent light emission, becomes increasingly challenging upon approaching a device with a near‐perfect spontaneous‐emission coupling factor . In fact, quantum‐optical studies have to be employed to reveal a transition to coherent emission in the intensity fluctuation behavior of nanolasers when the input–output characteristic appears thresholdless for nanolasers. Here, a new indicator for lasing operation in high‐ lasers is identified by showing that stimulated emission can give rise to a lineshape anomaly manifested as a transition from a Lorentzian to a Gaussian component in the emission linewidth that dominates the spectrum above the lasing threshold.

Koulas‐Simos, Aris↗

Design of AlGaN-Zn(Si,Ge)N2 quantum wells for high-efficiency ultraviolet light emitters

The effect of inserting a nm-scale layer of Zn(Si,Ge)N2 into an AlGaN quantum well structure designed for light emission in the wavelength range from 255 to 305 nm is investigated here. The enhanced confinement of the hole within the quantum well results in an enhancement of the overlap of the hole and electron wave functions, resulting in an enhancement of the radiative recombination rate. In this theoretical calculation, for emission at a 270 nm wavelength, the enhancement in the wavefunction overlap can reach a factor of 7 when compared to an AlGaN quantum well device specifically engineered for optimal emission at the identical wavelength. Increases of almost an order of magnitude in both the peak spontaneous emission intensity and the radiative recombination rate are predicted. The peak emission wavelength can be tuned from 255 to 305 nm by adjusting the width and/or the composition of the inserted layer. The proposed structures provide a route to higher efficiency ultraviolet practical light emitting diodes and lasers.

Physics↗

Quantum entanglement distribution coexisting with high-rate, broadband classical optical communications over a real-world fiber connecting remote, synchronized nodes

Compatibility with existing classical network infrastructure offers a scalable path towards deploying large-scale quantum networks. Here, we demonstrate O-band polarization-encoded quantum entanglement distribution over an installed 24.4-km fiber while coexisting with a state-of-the-art fully loaded C-band classical communications line system and a picosecond-level precision L-band synchronization signal. The classical system carries two 800-Gbps channels while the remainder of the C-band is filled with amplified spontaneous emission, as is standard for such state-of-the-art communications systems. We examine the spontaneous Raman scattering spectrum generated from this broadband C-band light and offer insights into wavelength allocation for O-band quantum channels. Optimal wavelength selection and narrow filtering enable well-preserved Bell state fidelity when coexisting with 21.4-dBm aggregate launch power across the C-band suitable for 36-Tbps transmission. To the best of our knowledge, this is the first implementation of entanglement-based quantum communications between two remote nodes coexisting with independent classical communications traffic. We demonstrate coexistence of quantum entanglement with ultra-high power levels and record classical bandwidth, offering promise for real-world entanglement-based networking integrated within high-capacity communications infrastructure.

Talcott, Gina M. [Northwestern U.] (ORCID:00000002↗

Seeded stimulated X-ray emission at 5.9 keV

X-ray free-electron lasers (XFELs) provide intense pulses that can generate stimulated X-ray emission, a phenomenon that has been observed and studied in materials ranging from neon to copper. Two schemes have been employed: amplified spontaneous emission (ASE) and seeded stimulated emission (SSE), where a second color XFEL pulse provides the seed. Both phenomena are currently explored for coherent X-ray laser sources and spectroscopy. Here, we report measurements of ASE and SSE of the 5.9 keV Mn K α 1 fluorescence line from a 3.9 molar NaMnO 4 solution, pumped with 7 femtosecond FWHM XFEL pulses at 6.6 keV. We observed ASE at a pump pulse intensity of 1.7×10 19 W/cm 2 , consistent with earlier findings. We observed SSE at dramatically reduced pump pulse intensities down to 1.1×10 17 W/cm 2 . These intensities are well within the range of many existing XFEL instruments, which supports the experimental feasibility of SSE as a tool to generate coherent X-ray pulses, spectroscopic studies of transition metal complexes, and other applications.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Resonant X-ray emission spectroscopy from broadband stochastic pulses at an X-ray free electron laser

Abstract Hard X-ray spectroscopy is an element specific probe of electronic state, but signals are weak and require intense light to study low concentration samples. Free electron laser facilities offer the highest intensity X-rays of any available light source. The light produced at such facilities is stochastic, with spikey, broadband spectra that change drastically from shot to shot. Here, using aqueous ferrocyanide, we show that the resonant X-ray emission (RXES) spectrum can be inferred by correlating for each shot the fluorescence intensity from the sample with spectra of the fluctuating, self-amplified spontaneous emission (SASE) source. We obtain resolved narrow and chemically rich information in core-to-valence transitions of the pre-edge region at the Fe K-edge. Our approach avoids monochromatization, provides higher photon flux to the sample, and allows non-resonant signals like elastic scattering to be simultaneously recorded. The spectra obtained match well with spectra measured using a monochromator. We also show that inaccurate measurements of the stochastic light spectra reduce the measurement efficiency of our approach.

Fuller, Franklin D. (ORCID:0000000237737087)↗

Theory of molecular emission power spectra. I. Macroscopic quantum electrodynamics formalism

In this work, we study the emission power spectrum of a molecular emitter with multiple vibrational modes in the framework of macroscopic quantum electrodynamics. The theory we present is general for a molecular spontaneous emission spectrum in the presence of arbitrary inhomogeneous, dispersive, and absorbing media. Moreover, the theory shows that the molecular emission power spectra can be decomposed into the electromagnetic environment factor and lineshape function. In order to demonstrate the validity of the theory, we investigate the lineshape function in two limits. In the incoherent limit (single molecules in a vacuum), the lineshape function exactly corresponds to the Franck–Condon principle. In the coherent limit (single molecules strongly coupled with single polaritons or photons) together with the condition of high vibrational frequency, the lineshape function exhibits a Rabi splitting, the spacing of which is exactly the same as the magnitude of exciton–photon coupling estimated by our previous theory [S. Wang et al., J. Chem. Phys. 151, 014105 (2019)]. Finally, we explore the influence of exciton–photon and electron–phonon interactions on the lineshape function of a single molecule in a cavity. The theory shows that the vibronic structure of the lineshape function does not always disappear as the exciton–photon coupling increases, and it is related to the loss of a dielectric environment.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Controlling electric and magnetic Purcell effects in phosphorene via strain engineering

Here, we investigate the spontaneous emission lifetime of a quantum emitter near a substrate coated with phosphorene under the influence of uniaxial strain. We consider both electric dipole and magnetic dipole-mediated spontaneous transitions from the excited to the ground state. The modeling of phosphorene is performed by employing a tight-binding model that goes beyond the usual low energy description. We demonstrate that both electric and magnetic decay rates can be strongly tuned by the application of uniform strain, ranging from a near-total suppression of the Purcell effect to a remarkable enhancement of more than 1300% due to the high flexibility associated with the puckered lattice structure of phosphorene. We also unveil the use of strain as a mechanism to tailor the most probable decay pathways of the emitted quanta. Our results show that uniaxially strained phosphorene is an efficient and versatile material platform for the active control of light-matter interactions thanks to its extraordinary optomechanical properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Manipulation of quantum dot emission with semiconductor metasurfaces exhibiting magnetic quadrupole resonances

Optical metasurfaces were suggested as a route for engineering advanced light sources with tailored emission properties. In particular, they provide a control over the emission directionality, which is essential for single-photon sources and LED applications. Here, we experimentally study light emission from a metasurface composed of III-V semiconductor Mie-resonant nanocylinders with integrated quantum dots (QDs). Specifically, we focus on the manipulation of the directionality of spontaneous emission from the QDs due to excitation of different magnetic quadrupole resonances in the nanocylinders. To this end, we perform both back focal plane imaging and momentum-resolved spectroscopy measurements of the emission. This allows for a comprehensive analysis of the effect of the different resonant nanocylinder modes on the emission characteristics of the metasurface. Our results show that the emission directionality can be manipulated by an interplay of the excited quadrupolar nanocylinder modes with the metasurface lattice modes and provide important insights for the design of novel smart light sources and new display concepts.

Vaskin, Aleksandr↗

Discovery of tunable and soluble organic emitters for solid-state lasers with a self-driving laboratory

We have recently demonstrated the ability of using self-driving laboratories for AI-driven searches of organic emitters for solid-state lasing devices. Our past workflow featured solubility challenges for such large molecular moieties. In this next-generation study, we return to the drawing board to explore a family of com-pounds that are much solution processable and composed of a set of electronic cores that provide a broader color response. Out of 252 potential candidates,and with guidance from DFT calculations, we selectively perform a compre-hensive study exploring 51 fluorene-based A-B-A type organic laser oligomers, armed with our self-driving lab. The candidates range from simple hydrocarbon molecules to complex hetero atom-mixed molecules. As a result of this study, we highlight diketopyrrolopyrrole and benzodiazole derivatives for their largely red-shifted emissions. Furthermore, we investigate the effect of color change aris-ing from hetero atom permutation, fluorine addition, thiophene coupling, and a combination of fluorine addition and thiophene coupling. Amplified spontaneous emission (ASE) measurements in the solid state further corroborate the lasing potential of selected candidates, reinforcing their suitability for future device applications. The computational study with density functional theory confirms the experimental results.

fluorescence↗

Long-range cooperative resonances in rare-earth ion arrays inside photonic resonators

Engineering arrays of active optical centers to control the interaction Hamiltonian between light and matter has been the subject of intense research recently. Collective interaction of atomic arrays with optical photons can give rise to directionally enhanced absorption or emission, which enables engineering of broadband and strong atom-photon interfaces. Here, we report on the observation of long-range cooperative resonances in an array of rare-earth ions controllably implanted into a solid-state lithium niobate micro-ring resonator. We show that cooperative effects can be observed in an ordered ion array extended far beyond the light’s wavelength. We observe enhanced emission from both cavity-induced Purcell enhancement and array-induced collective resonances at cryogenic temperatures. Engineering collective resonances as a paradigm for enhanced light-matter interactions can enable suppression of free-space spontaneous emission. The multi-functionality of lithium niobate hosting rare-earth ions can open possibilities of quantum photonic device engineering for scalable and multiplexed quantum networks.

42 ENGINEERING↗

Quantum nanophotonic interface for tin-vacancy centers in thin-film diamond

The negatively charged tin-vacancy center in diamond (SnV − ) is an excellent solid state qubit with optically-addressable transitions and a long electron spin coherence time at elevated (∼1.7 K). However, implementing scalable quantum nodes with high-fidelity optical readout of the electron spin state requires efficient photon emission and collection from the system. Here, in this manuscript, we report a quantum photonic interface for SnV−centers based on one-dimensional photonic crystal cavities fabricated in diamond thin films. Furthermore, we provide a rigorous description of the spontaneous emission dynamics of our system, taking into account individual contributions from both the C and D transitions of the emitter. This allows for determination of Purcell factors per transition and, by extension, the C/D branching ratio SnV− zero phonon line. We observe quality factors up to ~6000 across this sample, and measure up to a 12-fold lifetime reduction, which translates into a Purcell factor of 𝐹 𝐶 =26.2±1.5 for a targeted C transition. By considering the cavity mode polarization alignment with the C and D transition dipole moments, we validate the C/D branching ratio to be 𝜂 BR =0.75±0.01, in line with previous theoretical and experimental findings.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Design of InGaN-ZnSnGa 2 N 4 quantum wells for high-efficiency amber light emitting diodes

A novel type-II InGaN-ZnSnGa 2 N 4 quantum well (QW) structure is proposed based on recent experimental achievements for the successful epitaxy of ZnSnN 2 -GaN alloys and the determination of their band offsets with GaN. The simulation results indicate that this structure is promising as the active region for high-efficiency InGaN-based amber (λ ~ 590 nm) light-emitting diodes (LEDs). The hole wavefunction in the valence band is better confined with the insertion of a monolayer scale of ZnSnGa 2 N 4 into the InGaN QW while the electron wavefunction in the conduction band is better confined with the incorporation of an AlGaN layer in the GaN quantum barrier. The band structure of the InGaN-ZnSnGa 2 N 4 QW is numerically simulated based on the experimentally measured band offsets between ZnSnGa 2 N 4 and GaN. With the InGaN-ZnSnGa 2 N 4 QW design, a low In content (20%) is required in the InGaN layer to reach a peak emission wavelength of ~590 nm, yet an In composition of 25% is needed to reach the same emission wavelength for a conventional InGaN QW with the same layer thicknesses. Moreover, the electron-hole wavefunction overlap (Гe1-hh1) for the InGaN-ZnSnGa 2 N 4 QW design reaches 18% for an emission wavelength at ~590 nm. This result is much improved over the conventional InGaN QW overlap of 5% emitting at the same wavelength. The increase in electron-hole wavefunction overlap results in an approximately 14 times enhancement in the predicted spontaneous emission radiative recombination rate of the InGaN-ZnSnGa 2 N 4 QW as compared to that of the conventional InGaN QW. This InGaN-ZnSnGa 2 N 4 QW structure design can be promising to pave a new way to achieve high efficiency amber LEDs.

42 ENGINEERING↗

Quantum Shell in a Shell: Engineering Colloidal Nanocrystals for a High-Intensity Excitation Regime

Many optoelectronic processes in colloidal semiconductor nanocrystals (NCs) suffer an efficiency decline under high-intensity excitation. This issue is caused by Auger recombination of multiple excitons, which converts the NC energy into excess heat, reducing the efficiency and life span of NC-based devices, including photodetectors, X-ray scintillators, lasers, and high-brightness light-emitting diodes (LEDs). Recently, semiconductor quantum shells (QSs) have emerged as a promising NC geometry for the suppression of Auger decay; however, their optoelectronic performance has been hindered by surface-related carrier losses. Here, we address this issue by introducing quantum shells with a CdS–CdSe–CdS–ZnS core–shell–shell–shell multilayer structure. Further, the ZnS barrier inhibits the surface carrier decay, which increases the photoluminescence (PL) quantum yield (QY) to 90% while retaining a high biexciton emission QY of 79%. The improved QS morphology allows demonstrating one of the longest Auger lifetimes reported for colloidal NCs to date. The reduction of nonradiative losses in QSs also leads to suppressed blinking in single nanoparticles and low-threshold amplified spontaneous emission. We expect that ZnS-encapsulated quantum shells will benefit many applications exploiting high-power optical or electrical excitation regimes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Plasmonic Diamond Membranes for Ultrafast Silicon Vacancy Emission

Silicon vacancy centers (SiVs) in diamond have emerged as a promising platform for quantum sciences due to their excellent photostability, minimal spectral diffusion, and substantial zero-phonon line emission. However, enhancing their slow nanosecond excited-state lifetime by coupling to optical cavities remains an outstanding challenge, as current demonstrations are limited to ~10-fold. Here, we couple negatively charged SiVs to sub-diffraction-limited plasmonic cavities and achieve an instrument-limited ≤8 ps lifetime, corresponding to a 135-fold spontaneous emission rate enhancement and a 19-fold photoluminescence enhancement. Nanoparticles are printed on ultrathin diamond membranes on gold films which create arrays of plasmonic nanogap cavities with ultrasmall volumes. SiVs implanted at 5 and 10 nm depths are examined to elucidate surface effects on their lifetime and brightness. The interplay between cavity, implantation depth, and ultrathin diamond membranes provides insights into generating ultrafast, bright SiV emission for next-generation diamond devices.

Purcell enhancement↗