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DOE OSTI2025

Measurements of attenuation and scattering properties of water-based liquid scintillator

Water-based liquid scintillator (WbLS) is a hybrid detector medium which has been proposed as a fill material for future large-volume rare event searches, including ν − detectors. This family of scintillating suspensions promises waterlike attenuation and scattering behavior, while offering scintillation light yield for sub-Cherenkov-threshold events. These features may allow for improved vertex and energy resolution, and concomitant improvements in background rejection and particle identification. While subscale measurements of light yield, timing and pulse-shape have been performed in several WbLS formulations, detailed measurements of the attenuation and scattering properties of WbLS remain a critical, unresolved step along the pathway to deployment. In pursuit of a better understanding of these parameters, a “long-arm” attenuation and scattering instrument has been developed at Lawrence Livermore National Laboratory, dubbed LASE (Livermore Attenuation and Scattering Experiment). Optical property measurements have been performed using LASE in DI water, Gd-water, WbLS and Gd-WbLS. Measurements of the optical properties of WbLS (1% LAB-PPO scintillator) provided by Brookhaven National Laboratory demonstrate an attenuation minimum of 4.87 × 10 − 4 ± 1.42 × 10 − 4 cm − 1 at 450 nm, while Gd-loaded WbLS (1% LAB-PPO scintillator, 0.1% Gd) demonstrated a minimum attenuation coefficient of 4.77 × 10 − 4 ± 1.27 × 10 − 4 cm − 1 at the same wavelength. Measurements of scattering in WbLS show a scattering coefficient of 3.39 × 10 − 4 ± 1.98 × 10 − 5 cm − 1 at the 450 nm attenuation minimum, while Gd-WbLS has a scattering coefficient of 2.8 × 10 − 4 ± 1.63 × 10 − 5 cm − 1 at that wavelength. These scattering and attenuation coefficients are significantly larger than measured for DI water at similar wavelengths ( 8.8 × 10 − 5 cm − 1 ± 3.8 × 10 − 5 attenuation at 430 nm, 2.2 × 10 − 5 ± 1.28 × 10 − 6 cm − 1 scattering). Though the WbLS attenuation and scattering coefficients measured are lower than the corresponding values published for ultrapure oils and LAB-PPO liquid scintillator, the material tested attenuates significantly more than water across the blue and green portions of the visible spectrum. This attenuation is markedly stronger at wavelengths under 430 nm. Published by the American Physical Society 2025

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Multi-mode THz quantum-cascade VECSELs based on disordered metasurfaces

Quantum-cascade vertical-external-cavity surface-emitting-lasers (VECSELs) based on disordered amplifying metasurfaces are demonstrated and explored as potential broadband, multi-mode THz sources. The disorder is introduced along one spatial axis of the metasurface by pseudo-randomly varying the width of its resonant ridge antennas. Compared to a quantum-cascade (QC) VECSEL based on a uniform metasurface, the disordered structure supports much more localized transverse modes with reduced spatial overlap within the QC gain material. This localization is hypothesized to facilitate the spatial hole burning of the gain material and, therefore, enable multi-mode lasing, particularly for short cavities on the order of a few wavelengths. Several devices have been fabricated and shown to differ from uniform QC-VECSELs in a few key ways, possessing highly nonlinear light-current characteristics, angle-dependent emission spectra and broadband multi-mode lasing. At most, 17 modes are simultaneously observed, spanning 680 GHz. The number of VECSEL modes is shown to have an inverse relationship with the cavity length, which is attributed to increased diffractive losses in the open plano-plano cavity. As the cavity length is tuned, the device emits over a quasi-continuous band from 3.15 to 3.97 THz or up to 4.24 THz with a longitudinal mode hop.

Morag, Eilam [Univ. of California, Los Angeles, CA↗

DOE OSTI2024

ORBITAL ANGULAR MOMENTUM BEAMS RESEARCH USING A FREE-ELECTRON LASER OSCILLATOR

Orbital angular momentum (OAM) photon beams are excellent tools for non-contact optical manipulation of mat- ter in a broad photon energy range. A free-electron laser (FEL) oscillator is well-suited for studying OAM beams with various features including a wide spectral coverage, wavelength tunability, two-color lasing, polarization control, etc. Here, we report the first experimental demonstration of superposed OAM beams from an oscillator FEL. Lasing at around 458 nm, we have generated superposed OAM beams up to the fourth order as a superposition of two pure OAM modes with opposite helicities. These generated beams have a good beam quality, a high degree of circular polarization, and high power. Using external rf modulation with frequen- cies from 1 to 30 Hz, we also developed a pulsed mode operation of the OAM beams with a highly reproducible temporal structure. FEL operation showcased in this work can be extended to higher photon energies, e.g. using a future x-ray FEL oscillator. The operation of such an OAM FEL also paves the way for the generation of OAM gamma-ray beams via Compton scattering.

Liu, P.↗

DOE OSTI2024

Lateral Confinement in 2D Nanoplatelets: A Strategy to Expand the Colloidal Quantum Engineering Toolbox

Among colloidal nanocrystals, 2D nanoplatelets offer a unique set of properties with exceptionally narrow luminescence and low lasing thresholds. Furthermore, their anisotropic shape expands the playground for the complex design of heterostructures where spectra but also scattering rates can be engineered. A challenge that still remains is to combine shell growth which makes NPLs stable, with spectral tunability. Indeed, most reported shelled nanoplatelets end up being red emitters due to a loss of quantum confinement. Here, the combination of both lateral and in-plane confinements within a single heterostructure is explored. A CdS/CdSe/CdS/CdZnS core–crown–crown shell structure that enables yellow emission is grown and that is responsive to a large range of excitation including visible photons, X-ray photons, electron beams, and electrical excitations. k.p simulations predict that emission tunability of up to several 100 s of meV can be obtained in ideal structures. This material also displays stimulated emission resulting from bi-exciton emission with a low threshold. Once integrated into an LED stack, this material is compatible with sub-bandgap excitation and exhibits high luminance. Scaling of the electroluminescence properties by downsizing the pixel size is also investigated.

2D materials↗

DOE OSTI2025

Ligand‐Induced Crystallization Control in MAPbBr 3 Hybrid Perovskites for High Quality Nanostructured Films

AbstractControlling the formation of hybrid perovskite thin films is crucial in obtaining high‐performance optoelectronic devices, since factors like morphology and film thickness have a profound impact on a film's functionality. For light‐emitting applications grain sizes in the sub‐micrometer‐range have previously shown enhanced brightness. It is therefore crucial to develop simple, yet reliable methods to produce such films. Here, a solution‐based synthesis protocol for the on‐substrate formation of MAPbBr3 (MA = methylammonium) nanostructures by adding the bifunctional rac‐3‐aminobutyric acid to the precursor solution is reported. This synthesis route improves key optical properties such as photoluminescence quantum yields and life times of excited states by inducing a controlled slow‐down of the film formation and suppressing agglomeration effects. In situ spectroscopy reveals a delayed and slowed down crystallization process, which achieves synthesis of perovskite structures with much reduced defect densities. Further, aggregation can be controlled by the amount of amino acid added and adjusting the synthesis protocol allows to produce cubic crystallites with targeted size from nanometer to micrometer scales. The nanocrystalline MAPbBr3 samples show enhanced amplified spontaneous emission (ASE) intensities, reduced ASE thresholds and purer ASE signals, compared to pristine films, even under intense optical driving, making them promising structures for lasing applications.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Lines of Bound States in the Continuum in Monodisperse Microsphere Structures

Incorporating epitaxially grown active semiconductor media into self-assembled microsphere crystals has remained a major challenge as the curved geometry of the spheres is incompatible with conventional planar growth and patterning techniques. As a result, active photonic devices based on such self-assembled structures, which have other desirable properties such as enabling the rapid assembly of large area systems, have been elusive. Here, we numerically demonstrate an alternative route to creating high-Q resonances in microsphere-based nanophotonic assemblies compatible with standard optical gain materials. We show that close-packed layers of monodisperse microspheres can exhibit symmetry bandgaps, regardless of their layer stacking order. Thus, this microsphere environment can be used to create lines of bound states in the continuum (BICs) of an embedded slab made of active material. Using a realistic ZnS@SiO 2 (core-shell) architecture and sphere diameters compatible with scalable colloidal assembly, we predict sharp spectral features in angle-resolved transmission that trace these lines of BICs and persist in the presence of some fabrication disorder. Altogether, in enabling the integration of unpatterned epitaxial gain slabs with large-area colloidal microsphere assemblies, this approach opens a practical path toward active, dynamically reconfigurable photonic devices that leverage BIC physics for narrow-linewidth lasing and enhanced light–matter interactions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Elucidating the Role of InGaAs and InAlAs Buffers on Carrier Dynamics of Tensile-Strained Ge Double Heterostructures

Extensive research efforts of strained germanium (Ge) are currently underway due to its unique properties, namely, (i) possibility of band gap and strain engineering to achieve a direct band gap, thus exhibiting superior radiative properties, and (ii) higher electron and hole mobilities than Si for upcoming technology nodes. Realizing lasing structures is vital to leveraging the benefits of tensile-strained Ge (ε-Ge). Here, we use a combination of different analytical tools to elucidate the effect of the underlying InGaAs/InAlAs and InGaAs overlaying heterostructures on the material quality and strain state of ε-Ge grown by molecular beam epitaxy. Using X-ray analysis, we show the constancy of tensile strain in sub-50 nm ε-Ge in a quantum-well (QW) heterostructure. Further, effective carrier lifetime using photoconductive decay as a function of buffer type exhibited a high (low) defect-limited carrier lifetime of ~68 ns (~13 ns) in 0.61% (0.66%) ε-Ge grown on an InGaAs (InAlAs) buffer. These results correspond well with the measured surface roughness of 1.289 nm (6.303 nm), consistent with the surface effect of the ε-Ge/III–V heterointerface. Furthermore, a reasonably high effective lifetime of ~78 ns is demonstrated in a QW of ~30 nm 1.6% ε-Ge, a moderate reduction from ~99 ns in uncapped ε-Ge, alluding to the surface effect of the overlying heterointerface. Thus, the above results highlight the prime quality of ε-Ge that can be achieved via III–V heteroepitaxy and paves a path for integrated Ge photonics.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Harmonic and Subharmonic RF Injection Locking of THz Metasurface Quantum-Cascade VECSEL

Harmonic and subharmonic RF injection locking is demonstrated in a terahertz (THz) quantum-cascade vertical-external-cavity surface-emitting laser (QC-VECSEL). By tuning the RF injection frequency around integer multiples and submultiples of the cavity round-trip frequency, different harmonic and subharmonic orders can be excited in the same device. Modulation-dependent behavior of the device has been studied with recorded lasing spectral broadening and locking bandwidths in each case. In particular, harmonic injection locking results in the observation of harmonic spectra with bandwidths over 200 GHz. A semiclassical Maxwell-density matrix formalism has been applied to interpret QC-VECSEL dynamics, which aligns well with experimental observations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Towards higher frequencies in a compact prebunched waveguide THz-FEL

Free-electron-lasers fill a critical gap in the space of THz-sources as they can reach high average and peak powers with spectral tunability. Using a waveguide in a THz FEL significantly increases the coupling between the relativistic electrons and electromagnetic field enabling large amounts of radiation to be generated in a single passage of electrons through the undulator. In addition to transversely confining the radiation, the dispersive properties of the waveguide critically affect the velocity and slippage of the radiation pulse which determine the central frequency and bandwidth of the generated radiation. In this paper, we characterize the spectral properties of a compact waveguide THz FEL including simultaneous lasing at two different frequencies and demonstrating tuning of the radiation wavelength in the high frequency branch by varying the beam energy and ensuring that the electrons injected into the undulator are prebunched on the scale of the resonant radiation wavelength.

Experimental particle physics↗

DOE OSTI2024

Two-dimensional-lattice-confined single-molecule-like aggregates

Intermolecular distance largely determines the optoelectronic properties of organic matter. Conventional organic luminescent molecules are commonly used either as aggregates or as single molecules that are diluted in a foreigner matrix. They have garnered great research interest in recent decades for a variety of applications, including light-emitting diodes, lasers and quantum technologies, among others. However, there is still a knowledge gap on how these molecules behave between the aggregation and dilution states. Here we report an unprecedented phase of molecular aggregate that forms in a two-dimensional hybrid perovskite superlattice with a near-equilibrium distance, which we refer to as a single-molecule-like aggregate (SMA). By implementing two-dimensional superlattices, the organic emitters are held in proximity, but, surprisingly, remain electronically isolated, thereby resulting in a near-unity photoluminescence quantum yield, akin to that of single molecules. Moreover, the emitters within the perovskite superlattices demonstrate strong alignment and dense packing resembling aggregates, allowing for the observation of robust directional emission, substantially enhanced radiative recombination and efficient lasing. Molecular dynamics simulations together with single-crystal structure analysis emphasize the critical role of the internal rotational and vibrational degrees of freedom of the molecules in the two-dimensional lattice for creating the exclusive SMA phase. Furthermore, this two-dimensional superlattice unifies the paradoxical properties of single molecules and aggregates, thus offering exciting possibilities for advanced spectroscopic and photonic applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Solving tricky quantum optics problems with assistance from large language models

The capabilities of modern artificial intelligence (AI) as a “scientific collaborator” are explored by engaging it with three nuanced problems in quantum optics: state populations in optical pumping, resonant transitions between decaying states (the Burshtein effect), and degenerate mirrorless lasing. Through iterative dialogue, the authors observe that AI models–when prompted and corrected–can reason through complex scenarios, refine their answers, and provide expert-level guidance, closely resembling the interaction with an adept colleague. The findings highlight that AI can democratize access to sophisticated modeling and analysis, shifting the focus in scientific practice from technical mastery to the generation and testing of ideas, and reducing the time for completing research tasks from days to minutes.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2025

Delay-resolved spectroscopy in terahertz photonic circuits

Photonic integrated circuits incorporating intersubband transitions are ideal for mid-infrared and terahertz nanophotonics. However, the design of epitaxies has long been inhibited by two factors: the modest predictivity of ab initio theory and the absence of absolute intersubband gain and loss measurements under operating conditions. Existing measurements either yield inaccurate gain profiles or do not accurately assess dependence on frequency, bias, and temperature. Here, we present a delay-resolved absolute-referencing method for accurate gain evaluation without these limitations, addressing a long-standing challenge. By creating a photonic circuit that allows broadband pulses to traverse different lengths of a gain medium, we measure the absolute transmission of intersubband structures. Gain profiles match theoretical predictions at lower temperatures, with gain and dispersion clamping after lasing, and faster-than-expected degradation occurs at higher temperatures. Our approach provides a precise experimental evaluation of temperature-dependent gain performance and gives insight into optimizing temperature performance and frequency comb designs.

Optical spectroscopy↗

DOE OSTI2024

Imaging of dark line defect growth in high-power diode laser cavities using broadband near infrared light emission from the laser cavity

An in situ and nondestructive technique is developed to image the formation and evolution of dark line defects in the cavity of a high-power diode laser. Here, the technique uses broadband near infrared emission that originates in the laser's core layers and enables defects to be imaged with high spatial resolution through the substrate. In particular, it enables defect imaging through the substrate of shorter wavelength lasers, even when the substrate is opaque near the lasing wavelength. The evolution of dark line defects during aging is studied in several devices, with correlations established between the observed characteristics of defect growth and changes in device parameters such as optical power, operating wavelength, threshold current, and slope efficiency. Gradual degradation is found to be associated with dark line defects that slowly propagate from dark spots that are present in the device interior in its fresh (unaged) condition, rather than propagating from spots that are formed during aging, suggesting a strategy to screen fresh devices for expected reliability. This defect growth phenomenon is found to be particularly evident in the dark spots near the output facet.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

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↗

DOE OSTI2025

Long-Lived Population Inversion in Resonantly Driven Excitonic Antiferromagnet

Van der Waals magnets are an emerging material family for investigating light-matter interactions and spin-correlated excitations. Here, we report the discovery of a photo-induced state with a lifetime of 17 ps in the van der Waals antiferromagnet NiPS 3 , which appears exclusively with resonant pumping at 1.476 eV in the antiferromagnetic state. Furthermore, the long-lived state comes with a negative photoconductivity, a characteristic optical response of population inversion. Our findings demonstrate a promising pathway to potentially achieve long-lived lasing at terahertz frequencies in reduced dimensions.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Floquet engineering of polaritonic amplification in dispersive photonic time crystals

In this study, we investigate the dynamics of dispersive photonic time crystals (PTCs) and their potential applications for controlling light-matter interaction. Using the Lorentz-Drude as dispersive material model, we analyze the effects of periodic modulation of dispersion parameters through both theoretical and numerical analysis, revealing the emergence of hybrid bandgaps from the interaction of polaritonic branches with distinctive characteristics. Our study demonstrates that dispersive PTCs offer novel excitation channels and amplification possibilities, that require lower modulation frequencies compared to nondispersive systems thus alleviating experimental challenges for the realization of PTCs in the optical regime. These findings pave the way for advancements in polaritonic lasing and resonant Raman scattering.

Classical optics↗

DOE OSTI2026

Startup regime of high-efficiency tapering-enhanced FEL oscillator

In this paper, we present a design of a high-efficiency high-gain free-electron laser oscillator based on the use of a strongly tapered undulator for extracting energy from high-brightness electron beams. We provide an analytical model of the setup followed by numerical simulations for lasing at the wavelength of 13.5 nm. We discuss the optimization of the system in steady state and the conditions necessary for the pass-per-pass buildup of the power from shot noise level. We propose the use of fast phase shifters as a way to accelerate the buildup. Finally, we present time-dependent simulations of the oscillator and discuss the role of spectral filtering. The optimized working point yields a total energy conversion efficiency from the electron beam to output radiation above 1% at the wavelength of 13.5 nm.

Beam dynamics↗

DOE OSTI2024

Aging Mechanisms of Broad Area ~800 nm Laser Diodes

Here, this work presents a comprehensive study of early aging behavior (<500 hr) in ~800 nm, phosphide-based laser diodes grown by solid-source MBE with different oxygen concentration levels incorporated into the diode epitaxial layers during growth. The data indicate that lasing characteristics prior to aging are degraded by oxygen introduction, but the gradual power degradation rate after the onset of aging is not a strong function of oxygen at these concentration levels. Devices with oxygen concentrations of ~2.5 × 10 15 cm -3 showed significantly longer delay before the onset of aging (incubation time) than devices with less than 1 × 10 15 cm -3 oxygen. Generation-Recombination current and Laser Beam Induced Current measurements indicate that defect densities and aggregation are suppressed at the facets by oxygen, which can explain longer incubation times. Diagnostic data and parametric fits to diode simulation models show that increased cavity optical loss and defect density are primarily responsible for gradual power degradation during aging, rather than changes in nonradiative recombination. Mechanisms are proposed that explain this behavior, based on density functional theory (DFT) simulations and known recombination-enhanced defect generation phenomena.

47 OTHER INSTRUMENTATION↗