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DOE OSTI2024

Tunable-fidelity wave functions for the ab initio description of scattering and reactions

Here, the no-core shell model (NCSM) is an ab initio method that solves the nuclear many-body problem by expanding the many-particle wave function into a (typically) harmonic oscillator basis and minimizing the energy to obtain the expansion coefficients. Extensions of the NCSM, such as its coupling with microscopic-cluster basis states, further allow for an ab initio treatment of light-ion nuclear reactions of interest for both astrophysics and nuclear technology applications. A downside of the method is the exponential scaling of the basis size with increasing number of nucleons and excitation quanta, which limits its applicability to mass A ≲ 16 nuclei, except for variants where the basis is further down-selected via some truncation scheme. We consider a basis selection method for the NCSM that was first introduced in the context of the large-scale shell model and captures the essential degrees of freedom of the nuclear wave function leading to a favorable complexity scaling for calculations and enabling ab initio reaction calculations in sd-shell nuclei. The particle configurations within the NCSM basis are ordered based on their contribution to the first moment of the Hamiltonian matrix that results from the projection onto the many-body basis. The truncation scheme then consists in retaining only the lowest-first-moment configurations, which typically contain only few many-body basis states (Slater determinants). As the energy threshold above which configurations are disregarded is increased, the size of the basis becomes an almost-continuous variable, allowing for tunable fidelity in the obtained wave functions. The resulting wave functions can then be used directly in ab initio reaction calculations. We present calculations for 7 Li and n + 12 C scattering using nucleon-nucleon interactions derived from chiral effective field theory and softened using the similarity renormalization group method. The obtained energy levels invariably demonstrate exponential convergence with the size of the basis, and we find improved convergence in scattering calculations. To demonstrate the possibilities enabled by the approach, we also present a first calculation for the scattering of neutrons from 24 Mg. The method presented in this work appears promising for future studies of nuclei with mass A > 16, opening multiple future research directions impacting both nuclear astrophysics and nuclear technology applications.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Chemically Controllable Porous Polymer–Nanocrystal Composites with Hierarchical Arrangement Show Substrate Transport Selectivity

Functional organic–inorganic hybrid materials with tunable properties are useful across many application areas, ranging from gas storage to electronics, flame retardants, separations, and catalysis. Combining polymers, with a suite of functional groups and conformational flexibility, and inorganic nanoparticles, with tunable surface chemistry and composition, yields hybrids with novel functional properties. Specifically, in catalysis, control of the electronic environment at a metal interface is paramount in determining the catalytic properties. In this contribution, we describe a modular process to prepare porous polymer–nanocrystal (NC) composites in a hierarchical, multilayered synthesis, in which multiple parameters can be accurately tuned: polymer functional groups and the corresponding pore structure, the polymer layer thickness, and the NC size, shape, and composition. This process provides for a variety of controlled materials with high surface area, tunable chemistry, and thermal and chemical stabilities. Furthermore, we demonstrate their utility for shape- and size-selective catalytic conversions both in oxidation and hydrogenation reactions, where they show increased selectivity by orders of magnitude compared to conventional polymer-supported metal catalysts. In light of the high degree of control in the composite structure, this method allows for the design and realization of catalysts for several reactions and reaction environments and for nanomaterials with other applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Ultranarrow electroluminescence from magnetic excitons in the van der Waals antiferromagnetic semiconductor NiPS 3

Electrically driven light emission from two-dimensional (2D) semiconducting materials has enabled numerous optoelectronic technologies, including light-emitting diodes, solid-state lasers, and single-photon sources for quantum communication. Here we report ultranarrow electroluminescence from the magnetic excitonic state of the van der Waals antiferromagnetic semiconductor NiPS 3 . This electroluminescence is enabled by the fabrication of gate-tunable NiPS 3 devices that remain electrically conductive below the antiferromagnetic ordering temperature of 155 K, ultimately allowing field-effect mobilities of 1.3 cm 2 V –1 s –1 and 4.5 cm 2 V –1 s –1 to be directly measured at room temperature and 7 K, respectively. By applying a high-frequency square wave voltage to the gate electrode of the resulting field-effect transistors, electroluminescence is capacitively induced from the magnetic excitons of NiPS 3 . Due to the coupling of these excitons with the underlying NiPS 3 antiferromagnetic order, the electroluminescence has an ultranarrow linewidth of 1 meV and a high degree of linear polarization (ρ = 0.78). In addition to facilitating fundamental studies of the coupling between spin states and excitons in van der Waals magnetic semiconductors, this work will accelerate the development of emerging 2D opto-spintronic applications.

two-dimensional materials↗

DOE OSTI2019

Coherent soft X-ray pulses from an echo-enabled harmonic generation free-electron laser

It is known that X-ray free-electron lasers (FELs), which amplify light emitted by a relativistic electron beam, are extending nonlinear optical techniques to shorter wavelengths, adding element specificity by exciting and probing electronic transitions from core levels. These techniques would benefit tremendously from having a stable FEL source, generating spectrally pure and wavelength-tunable pulses. Here, we show that such requirements can be met by operating the FEL in the so-called echo-enabled harmonic generation (EEHG) configuration. Here, two external conventional lasers are used to precisely tailor the longitudinal phase space of the electron beam before emission of X-rays. We demonstrate high-gain EEHG lasing producing stable, intense, nearly fully coherent pulses at wavelengths as short as 5.9 nm (~211 eV) at the FERMI FEL user facility. Low sensitivity to electron-beam imperfections and observation of stable, narrow-band, coherent emission down to 2.6 nm (~474 eV) make the technique a prime candidate for generating laser-like pulses in the X-ray spectral region, opening the door to multidimensional coherent spectroscopies at short wavelengths.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2014

An analytical study on the diffraction quality factor of open cavities

Open cavities are often employed as interaction structures in a new generation of coherent millimeter, sub-millimeter, and terahertz (THz) radiation sources called the gyrotron. One of the open ends of the cavity is intended for rapid extraction of the radiation generated by a powerful electron beam. Up to the sub-THz regime, the diffraction loss from this open end dominates over the Ohmic losses on the walls, which results in a much lower diffraction quality factor (Q{sub d}) than the Ohmic quality factor (Q{sub ohm}). Early analytical studies have led to various expressions for Q{sub d} and shed much light on its properties. In this study, we begin with a review of these studies, and then proceed with the derivation of an analytical expression for Q{sub d} accurate to high order. Its validity is verified with numerical solutions for a step-tunable cavity commonly employed for the development of sub-THz and THz gyrotrons. On the basis of the results, a simplified equation is obtained which explicitly expresses the scaling laws of Q{sub d} with respect to mode indices and cavity dimensions.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2018

A metasurface optical modulator using voltage-controlled population of quantum well states

We present that the ability to control the light-matter interaction with an external stimulus is a very active area of research since it creates exciting new opportunities for designing optoelectronic devices. Recently, plasmonic metasurfaces have proven to be suitable candidates for achieving a strong light-matter interaction with various types of optical transitions, including intersubband transitions (ISTs) in semiconductor quantum wells (QWs). For voltage modulation of the light-matter interaction, plasmonic metasurfaces coupled to ISTs offer unique advantages since the parameters determining the strength of the interaction can be independently engineered. In this work, we report a proof-of-concept demonstration of a new approach to voltage-tune the coupling between ISTs in QWs and a plasmonic metasurface. In contrast to previous approaches, the IST strength is here modified via control of the electron populations in QWs located in the near field of the metasurface. By turning on and off the ISTs in the semiconductor QWs, we observe a modulation of the optical response of the IST coupled metasurface due to modulation of the coupled light-matter states. Because of the electrostatic design, our device exhibits an extremely low leakage current of ~6 pA at a maximum operating bias of +1 V and therefore very low power dissipation. Finally, our approach provides a new direction for designing voltage-tunable metasurface-based optical modulators.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

Mid-infrared spectroscopy with a broadly tunable thin-film lithium niobate optical parametric oscillator

Mid-infrared spectroscopy, an important technique for sensing molecules, has encountered barriers from sources either limited in tuning range or excessively bulky for widespread use. We present a compact, efficient, and broadly tunable optical parametric oscillator surmounting these challenges. Leveraging dispersion-engineered thin-film lithium niobate-on-sapphire photonics and a singly resonant cavity allows broad, controlled tuning over an octave from 1.5–3.3 µm. The device generates >25mW of mid-infrared light at 3.2 µm with 15% conversion efficiency. The ability to precisely control the device’s mid-infrared emission enables spectroscopy of methane and ammonia, demonstrating our approach’s relevance for sensing. Our work signifies an important advance in nonlinear photonics miniaturization, bringing practical field applications of high-speed, broadband mid-infrared spectroscopy closer to reality.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Hybrid Metal Halides: Advancing Optoelectronic Materials (Final Technical Report)

Hybrid metal halides, particularly main group halide perovskites, are a unique class of materials that oﬀer exceptional optoelectronic properties along with a remarkable materials design space. Initial research on this class of materials was driven by the ability of the prototype hybrid 3D perovskite-structured compound methylammonium lead iodide to function as the active layer in thin film solar cells. It is now known that this class of materials comprise a large family with tunable band gaps, relatively high charge carrier mobilities in both single crystal and polycrystalline forms, and relatively low concentrations of (deleterious) electrically active states within the band gap. Beyond applications in solar cells, the potential of these materials has been extended to emitters in light emitting diodes, and active components of radiation detectors. Complementing new functionality, the design space for hybrid metal halides continues to increase with discovery of new structural motifs. In this project, the combination of organic and inorganic functionalities has been employed to open pathways to the design and synthesis new, functional hybrid metal halides. Beyond the simple perovskites, Ruddlesden-Popper and Dion-Jacobsen compounds, and other variants, such as the newly advanced “hollow” perovskites have been studied. The materials have provided routes to understanding the unique electronic properties of hybrid metal halides because of their natural quantum well structures as well as other means of controlling band gaps and band dispersions. Understanding these materials, including the design rules for their formation, their structures and compositions in bulk and in thin films form, and the role of local (non-crystallographic) structure has an important aspect of this endeavor. The goal of advancing new materials and new fundamental understanding within this deceptively simple, yet fascinating class of compounds, so richly endowed with interesting and useful functionality, has been fulfilled.

36 MATERIALS SCIENCE↗

NASA NTRS1993

Solid state laser

A wavelength-tunable, injection-seeded, dispersion-compensated, dispersively-pumped solid state laser includes a lasing medium; a highly reflective mirror; an output coupler; at least one isosceles Brewster prism oriented to the minimum deviation angle between the medium and the mirror for directing light of different wavelengths along different paths; means for varying the angle of the highly reflective mirror relative to the light from at least one Brewster angle for selecting a predetermined laser operating wavelength; a dispersion compensation apparatus associated with the lasing medium; a laser injection seeding port disposed between the dispersion compensation apparatus and one of the mirror and coupler and including a reflective surface at an acute non-Brewster angle to the laser beam for introducing a seed input; a dispersion compensation apparatus associated with the laser medium including opposite chirality optical elements; the lasing medium including a pump surface disposed at an acute angle to the laser beam to define a discrete path for the pumping laser beam separate from the pumped laser beam.

Rines, Glen A.↗

NASA NTRS2011

Pulsed Lidar for Measurement of C02 Concentrations for the ASCENDS Mission - Update

We have been developing a laser-based sounding technique for the remote measurement of the tropospheric CO2 concentrations from orbit for NASA is ASCENDS mission. The mission's goals are to provide measurements of tropospheric CO2 abundance with global-coverage, a few hundred km spatial and monthly temporal resolution. These are needed to better understand CO2 fluxes and the processes that regulate CO2 storage by the land and oceans. For the lIP, we are developing and demonstrating the lidar techniques and key lidar technology that will permit measurements of the CO2 column abundance in the lower troposphere from aircraft. Our final goal is to demonstrate the key capabilities needed for a space lidar and mission approach for the ASCENDS mission. We use a pulsed lidar technique, which is much less sensitive to errors from cloud and atmospheric scattering and to noise from solar background. It allows continuous measurements of CO2 mixing ratio in the lower troposphere during day and night. Our approach uses the 1570nm CO2 band and a two-wavelength laser absorption spectrometer, which continuously measures at nadir from a circular polar orbit. It directs the narrow co-aligned laser beams from the instrument's lasers toward nadir, and measures the energy of the laser echoes reflected from land and water surfaces. It uses a pair of tunable laser transmitters, which allowing measurement of the extinction from a single selected CO2 absorption line in the 1570 nm band and from a line pair in the Oxygen A-band near 765 nm. These regions have temperature insensitive absorption lines are free from interference from other gases. The lasers pulse at 10KHz, use tunable diode seed lasers followed by laser amplifiers, and have MHz spectral widths. During the measurement the lasers are stepped across the selected lines at a kHz rate. The receiver uses a 1-m class telescope and photon sensitive detectors and measures the background light and energies of the laser echoes from the surface. The extinction and column densities for the CO2 and O2 gases are estimated from the ratio of the on and off line echo pulse energies via the integrated path differential absorption (IPDA) technique. Our technique exploits the atmospheric pressure broadening of the lines to weight the measurement sensitivity to the atmospheric column below 5 km. Pulsed laser signals, time gated receiver are used to isolate the surface laser echo signals and to exclude photons scattered from clouds and aerosols. We have successfully demonstrated many key aspects of the approach and lidar technology in the laboratory. We have demonstrated CO2 column measurements in airborne flights during the summers of 2009 and 2010. These included measurements from 3-l3 km altitudes made over a variety of surfaces and through thin and broken clouds. We demonstrated initial airborne measurements of O2 column density to 10 km altitudes during the summer 2010 flights. More details approach, key technologies, and demonstration measurements will be given in the presentation.

Abshire, James↗

DOE OSTI2016

Correlated Perovskites as a New Platform for Super-Broadband-Tunable Photonics

The electron-doping-induced phase transition of a prototypical perovskite SmNiO 3 induces a large and non-volatile optical refractive-index change and has great potential for active-photonic-device applications. Strong optical modulation from the visible to the mid-infrared is demonstrated using thin-film SmNiO 3 . Finally, modulation of a narrow band of light is demonstrated in this paper using plasmonic metasurfaces integrated with SmNiO 3 .

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2021

Electrochromic Properties of Perovskite NdNiO 3 Thin Films for Smart Windows

Semiconductors with electrically tunable band gaps are of great interest in controlling transparency to electromagnetic radiation. Thin films of perovskite nickelate NdNiO 3 (NNO), a class of correlated oxides, were deposited on single-crystal (LaAlO 3 (LAO)) and polycrystalline (fluorine-doped tin oxide-coated glass (FTO)) substrates by magnetron sputtering, chemical solution deposition (CSD), and atomic layer deposition (ALD). Their electrochromic behaviors were investigated using a three-electrode setup in basic (KOH solution, pH = 12) electrolyte. During bleaching/coloration process, the proton intercalation/deintercalation and simultaneous electron compensation in the NNO lattice under electrical bias led to crossover of the material between the pristine-conducting phase (Ni 3+ ) and the strongly correlated insulating phase (Ni 2+ ), which serves as the working principle for electrochromic (tunable opacity in the visible range) behavior. Cyclic voltammetry (CV) scans demonstrate that NNO films are electrochemically stable in basic solutions for all three film deposition methods explored here. CV scans at varying rates enabled the extraction of diffusion coefficient of protons in thin film NNO, which is similar to 10 –7 cm 2 s –1 among all films studied. Large light transmittance modulation by bleaching and coloration was observed on films grown on both LAO and FTO substrates, suggesting its potential as an electrochromic material candidate for smart windows and optical shutter applications. Here, porous NNO films obtained by chemical solution deposition tend to demonstrate stronger electrochromic activity than dense films grown by sputtering or ALD.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Thermally Activated Delayed Photoluminescence: Deterministic Control of Excited-State Decay

Thermally activated photophysical processes are ubiquitous in numerous organic and metal-organic molecules, leading to chromophores with excited state properties that can be considered an equilibrium mixture of the available low-lying states. Relative populations of the equilibrated states are governed by temperature. Such molecules have been devised as high quantum yield emitters in modern organic light-emitting diode technology and for deterministic excited state lifetime control to enhance chemical reactivity in solar energy conversion and photocatalytic schemes. This recent discovery of thermally activated photophysics at CdSe nanocrystal-molecule interfaces enables a new paradigm wherein molecule-quantum dot constructs are used to systematically generate material with predetermined photophysical response and excited state properties. Semiconductor nanomaterials feature size-tunable energy level engineering, which considerably expands the purview of thermally activated photophysics beyond what is possible using only molecules. This Perspective is intended to provide a non-exhaustive overview of the advances that led to the integration of semiconductor quantum dots in thermally activated delayed photoluminescence (TADPL) schemes and to identify important challenges moving into the future. The initial establishment of excited state lifetime extension utilizing triplet-triplet excited-state equilibria is detailed. Next, advances involving the rational design of molecules composed of both metal-containing and organic-based chromophores that produce the desired TADPL are described. Lastly, the recent introduction of semiconductor nanomaterials into hybrid TADPL constructs is discussed, paving the way towards the realization of fine-tuned deterministic control of excited state decay. It is envisioned that libraries of synthetically facile composites will be broadly deployed as photosensitizers and light emitters for numerous synthetic and optoelectronic applications in the near future.

14 SOLAR ENERGY↗

DOE OSTI2022

Light-induced ferromagnetism in moiré superlattices

Many-body interactions between carriers lie at the heart of correlated physics. The ability to tune such interactions would allow the possibility to access and control complex electronic phase diagrams. Recently, two-dimensional moiré superlattices have emerged as a promising platform for quantum engineering such phenomena. The power of the moiré system lies in the high tunability of its physical parameters by adjusting the layer twist angle, electrical field, moiré carrier filling and interlayer coupling. In this work, we report that optical excitation can highly tune the spin–spin interactions between moiré-trapped carriers, resulting in ferromagnetic order in WS 2 /WSe 2 moiré superlattices. Near the filling factor of v = 1/3 (that is, one hole per three moiré unit cells), as the excitation power at the exciton resonance increases, a well-developed hysteresis loop emerges in the reflective magnetic circular dichroism signal as a function of magnetic field, a hallmark of ferromagnetism. The hysteresis loop persists down to charge neutrality, and its shape evolves as the moiré superlattice is gradually filled, indicating changes of magnetic ground state properties. The observed phenomenon points to a mechanism in which itinerant photoexcited excitons mediate exchange coupling between moiré-trapped holes. This exciton-mediated interaction can be of longer range than direct coupling between moiré-trapped holes, and thus magnetic order arises even in the dilute hole regime. This discovery adds a dynamic tuning knob to the rich many-body Hamiltonian of moiré quantum matter.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Low-Loss Charge Transfer Plasmons in Graphene/α-RuCl 3 Heterostructures Below 40 K

Charge transfer at material interfaces governs a wide range of physical properties, from electronic band structures to emergent collective excitations. In two-dimensional (2D) material heterostructures, charge transfer phenomena play important roles in enabling novel quantum phases, proximity effects, and tunable plasmonic responses. One representative charge transfer interface is formed between α-RuCl 3 , a van der Waals material with high electron affinity, and graphene. Significant charge transfer across this interface induces the formation of charge-transfer plasmon polaritons (CPPs), hybrid excitations between light and charge oscillations. However, previous studies found that as the charge transfer process takes place, α-RuCl 3 becomes lossy, which limits the quality factor of CPPs. Here, we investigate CPPs down to 10 K using a home-built scattering-type scanning near-field optical microscope (s-SNOM) optimized for low-temperature measurements. Our study reveals a dramatic suppression of plasmon loss channels below 40 K, contributing to a significant enhancement in the plasmonic quality factor. This reduction in loss is likely attributed to the blue shift of the correlation-induced Mott gap in α-RuCl 3 with decreasing temperature, along with the reduction of phonon scattering at low temperature. In conclusion, our results highlight the potential of using s-SNOM and CPPs to study complex 2D interfaces and reveal correlated electron dynamics in the underlying material.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Enhanced Sampling Aided Design of Molecular Photoswitches

Advances in the evolving field of atomistic simulations promise important insights for the design and fundamental understanding of novel molecular photoswitches. Here, in this study, we use state-of-the-art enhanced simulation techniques to unravel the complex, multistep chemistry of donor–acceptor Stenhouse adducts (DASAs). Our reaction discovery workflow consists of enhanced sampling for efficient chemical space exploration, refinement of newly observed pathways with more accurate ab initio electronic structure calculations, and structural modifications to introduce design principles within future generations of DASAs. We showcase our discovery workflow by not only recovering the full photoswitching mechanism of DASA but also predicting a plethora of new plausible thermal pathways and suggesting a way for their experimental validation. Furthermore, we illustrate the tunability of these newly discovered reactions, leading to a potential avenue for controlling DASA dynamics through multiple external stimuli. Overall, these insights could offer alternative routes to increase the efficiency and control of DASA’s photoswitching mechanism, providing new elements to design more complex light-responsive materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2015

Active control of chirality in nonlinear metamaterials

An all-optical tunabe chirality is realized in a photonic metamaterial, the metamolecule of which consists of a nonlinear nano-Au:polycrystalline indium-tin oxide layer sandwiched between two L-shaped gold nano-antennas twisted 90° with each other. The maximum circular dichroism reached 30%. Under excitation of a 40 kW/cm{sup 2} weak pump light, the peak in the circular dichroism shifts 45 nm in the short-wavelength direction. An ultrafast response time of 35 ps is maintained. This work not only opens up the possibility for the realization of ultralow-power and ultrafast all-optical tunable chirality but also offers a way to construct ultrahigh-speed on-chip biochemical sensors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Photon upconversion with hot carriers in plasmonic systems

In this paper, we propose a scheme of photon upconversion based on harnessing the energy of plasmonic hot carriers. Low-energy photons excite hot electrons and hot holes in a plasmonic nanoparticle, which are then injected into an adjacent semiconductor quantum well where they radiatively recombine to emit a photon of higher energy. We theoretically study the proposed upconversion scheme using Fermi-liquid theory and determine the internal quantum efficiency of upconversion to be as high as 25% in 5 nm silver nanocubes. This upconversion scheme is linear in its operation, does not require coherent illumination, offers spectral tunability, and is more efficient than conventional upconverters.

36 MATERIALS SCIENCE↗