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DOE OSTI2022

Platinum Graphene Catalytic Condenser for Millisecond Programmable Metal Surfaces

Accelerating catalytic chemistry and tuning surface reactions require precise control of the electron density of metal atoms. In this work, nanoclusters of platinum were supported on a graphene sheet within a catalytic condenser device that facilitated electron or hole accumulation in the platinum active sites with negative or positive applied potential, respectively. The catalytic condenser was fabricated by depositing on top of a p-type Si wafer an amorphous HfO 2 dielectric (70 nm), on which was placed the active layer of 2–4 nm platinum nanoclusters on graphene. A potential of ±6 V applied to the Pt/graphene layer relative to the silicon electrode moved electrons into or out of the active sites of Pt, attaining charge densities more than 1% of an electron or hole per surface Pt atom. At a level of charge condensation of ±10% of an electron per surface atom, the binding energy of carbon monoxide to a Pt(111) surface was computed via density functional theory to change 24 kJ mol –1 (0.25 eV), which was consistent with the range of carbon monoxide binding energies determined from temperature-programmed desorption (ΔBE CO of 20 ± 1 kJ mol –1 or 0.19 eV) and equilibrium surface coverage measurements (ΔBE CO of 14 ± 1 kJ mol –1 or 0.14 eV). Impedance spectroscopy indicated that Pt/graphene condensers with potentials oscillating at 3000 Hz exhibited negligible loss in capacitance and charge accumulation, enabling programmable surface conditions at amplitudes and frequencies necessary to achieve catalytic resonance.

Inorganic carbon compounds↗

DOE OSTI2024

Ultrafast state-selective tunneling in two-dimensional semiconductors with a phase- and amplitude-controlled THz-scanning tunneling microscope

THz-pulse driven scanning tunneling microscopy (THz-STM) enables access to the ultrafast quantum dynamics of low-dimensional material systems at simultaneous ultrafast temporal and atomic spatial resolution. State-selective tunneling requires precise amplitude and phase control of the THz pulses combined with quantitative near-field waveform characterization. Here, we employ our state-of-the-art THz-STM with multi-MHz repetition rates, efficient THz generation, and precisely tunable THz waveforms to investigate a single sulfur vacancy in monolayer MoS2. We demonstrate that 2D transition metal dichalcogenides (TMDs) are an ideal platform for near-field waveform sampling by THz cross-correlation. Furthermore, we determine the THz voltage via QEV scans, which measure the THz rectified charge Q as a function of THz field amplitude E and dc bias Vdc. Mapping the complex energy landscape of localized states with a resolution down to 0.01 electrons per pulse facilitates state-selective tunneling to the HOMO and LUMO orbitals of a charged sulfur vacancy.

Materials Science↗

DOE OSTI2023

Detection and Calibration of Low-Energy Nuclear Recoils for Dark Matter and Neutrino Scattering Experiments

Detection of low-energy nuclear recoil events plays a central role in searches for particle dark matter interactions with atomic matter and studies of coherent neutrino scatters. Precise nuclear recoil calibration data allow the responses of these dark matter and neutrino detectors to be characterized and enable in situ evaluation of an experiment's sensitivity to anticipated signals. This article reviews the common methods for detection of nuclear recoil events and the wide variety of techniques that have been developed to calibrate detector response to nuclear recoils. We summarize the main experimental factors that are critical for accurate nuclear recoil calibrations, investigate mitigation strategies for different backgrounds and biases, and discuss how the presentation of calibration results can facilitate comparison between experiments. Lastly, we discuss the challenges for future nuclear recoil calibration efforts and the physics opportunities they may enable.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2021

TP099-CT-800DR Comparison Between SIRZ-2 and Surface Fit Method ($ρ_{e},Ζ_{e}$) Estimation

The primary objective of this test plan is to acquire dual-energy computed tomography (CT) data of 33 well-known specimens using the Leidos Reveal CT-80DR+ baggage scanner housed at LLNL (hereafter referred to as CT-80DR). These data sets will allow us to compare, for each specimen, the accuracy and precision of electron density ($ρ_{e}$) and effective atomic number ($Z_{e}$) estimates obtained from two different algorithmic methods— from TSL’s surface fits and from LLNL’s SIRZ-2 decomposition. A secondary objective is to determine how often it is necessary to acquire CT-80DR spectral response information.

42 ENGINEERING↗

DOE OSTI2025

Understanding the optoelectronic properties of doped 2D organic-inorganic halide perovskite quantum wells: towards efficient ultrafast quantum well IR photodetectors

This project, titled “Understanding the optoelectronic properties of doped 2D organic-inorganic halide perovskite quantum wells: towards efficient quantum well IR photodetectors”, was funded by the U.S. Department of Energy to explore a new class of materials that could make future light-sensing technologies, such as infrared (IR) cameras and detectors more efficient, affordable, and widely available. The research focused on special layered materials called 2D halide perovskites, which are made up of alternating organic and inorganic layers only a few atoms thick. These materials can be tuned at the atomic level to absorb and emit light in precise ways, making them very attractive for use in optoelectronic devices. The main goal of the project was to understand how these perovskite materials absorb light and move electrical charges at very small scales. However, this is not an easy task. These materials often contain a mixture of different structures in the same film, and traditional tools like regular absorption or photoluminescence spectroscopy are not good at telling those structures apart. To solve this, the research team, led by Professor Luisa Whittaker-Brooks at the University of Utah developed a powerful method called electroabsorption spectroscopy. This technique uses electric fields to highlight the unique “fingerprints” of different excitons, which are tiny packets of energy formed when light hits the material. By using this method, the team could separate overlapping signals and learn exactly how the materials respond to light under different conditions, including changes in temperature, thickness, and chemical makeup.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Field-gradient measurement using a Stern-Gerlach atomic interferometer with butterfly geometry

Atomic interferometers have been studied as a promising device for precise sensing of external fields. Among various configurations, a particular configuration with a butterfly-shaped geometry has been designed to sensitively probe field gradients. Here, we introduce a Stern-Gerlach (SG) butterfly interferometer by incorporating magnetic field in the conventional butterfly-shaped configuration. Atomic trajectories of the interferometer can be flexibly adjusted by controlling magnetic fields to increase the sensitivity of the interferometer, while the conventional butterfly interferometer using Raman transitions can be understood as a special case. We also show that the SG interferometer can keep high contrast against a misalignment in position and momentum caused by the field gradient.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2020

Jefferson Lab High Precision Proton Radius Measurement Experiment: PRad

Proton is not a point-like particle; it has a finite size and an internal structure. The proton charge radius is usually measured through two different methods: using spectroscopy of hydrogen atoms, or through electron-proton (e - p) elastic scattering at low momentum transfer. In 2010, Phol et al [1] published a new measurement for proton charge radius obtained using the spectroscopy method from muonic hydrogen atoms. An ordinary hydrogen (H) atom is a bound state of an electron orbiting a proton. Likewise, a muonic hydrogen atom has a muon orbiting a proton. Since a muon has 200 times more mass than an electron, resulting in a much smaller orbiting radius, its orbit is much more sensitive to the proton charge distribution in space than the electron’s of an ordinary H-atom. Thus, the measurement from muonic hydrogen provides a 10 times more precise result than the previous methods. The radius from the muonic hydrogen measurement reported in [1] was significantly smaller than all the p

Bai, Xinzhan↗

DOE OSTI2022

Probing nuclear quadrupole deformation from correlation of elliptic flow and transverse momentum in heavy ion collisions

In heavy ion collisions, elliptic flow v2 and radial flow, characterized by eventwise average transverse momentum [p T ], are related to the shape and size of the overlap region, which are sensitive to the shape of colliding atomic nuclei. The Pearson correlation coefficient between v 2 and [p T ], ρ 2 , was found to be particularly sensitive to the quadrupole deformation parameter β that is traditionally measured in low energy experiments. Built on earlier insight that the prolate deformation β>0 reduces the ρ 2 in ultracentral collisions (UCC), we show that the prolate deformation β<0 enhances the value of ρ 2 . As β>0 and β<0 are the two extremes of triaxiality, the strength and sign of v 2 2 -[pT] correlation can be used to provide valuable information on the triaxiality of the nucleus. Our study provide further arguments for using the hydrodynamic flow as a precision tool to directly image the deformation of the atomic nuclei at extremely short timescale (<10 -24 s).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2020

Fermi Gases in Bichromatic Superlattices

The purpose of the program is the broad study of designer materials made of ultra-cold atoms and light, which provides new paradigms for emulating exotic layered systems. Bichromatic superlattices enable control and study of both dimensionality and dispersion in layered, strongly correlated Fermi gases, to model high-temperature superfluidity/superconductivity. Most layered materials are quasi-two-dimensional, neither two-dimensional, like a sheet, nor three-dimensional, like a gas, but somewhere in between. In quasi-2D layers with an unequal number of spin-up and spin-down electrons, particularly strong attraction between pairs of electrons with opposite spins is predicted to achieve the highest possible superconducting transition temperatures. To understand these materials, we emulate them with a layered, ultra-cold Fermi gas of 6Li atoms, magnetically tuned near a collisional (Feshbach) resonance, where precise control of the attraction, spin-composition, dimensionality and dispersion provides new tests of theory. The primary goals are of the program are: (1) Elucidation of the effects of dimensionality and confining potential shape on the enhancement of high-temperature superfluidity in a layered, strongly correlated Fermi gases; (2) Control of dispersion and the study of tunable Dirac points in one dimension.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Facile Size-Selective Defect Sealing in Large-Area Atomically Thin Graphene Membranes for Sub-Nanometer Scale Separations

Atomically thin graphene with a high-density of precise subnanometer pores represents the ideal membrane for ionic and molecular separations. However, a single large-nanopore can severely compromise membrane performance and differential etching between pre-existing defects/grain boundaries in graphene and pristine regions presents fundamental limitations. Here, we show for the first time that size-selective interfacial polymerization after high-density nanopore formation in graphene not only seals larger defects (>0.5 nm) and macroscopic tears but also successfully preserves the smaller subnanometer pores. Low-temperature growth followed by mild UV/ozone oxidation allows for facile and scalable formation of high-density (4–5.5 $\times$ 10 12 cm –2 ) useful subnanometer pores in the graphene lattice. We demonstrate scalable synthesis of fully functional centimeter-scale nanoporous atomically thin membranes (NATMs) with water (~0.28 nm) permeance ~23$\times$ higher than commercially available membranes and excellent rejection to salt ions (~0.66 nm, >97% rejection) as well as small organic molecules (~0.7–1.5 nm, ~100% rejection) under forward osmosis. $\times$

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Sculpting the Plasmonic Responses of Nanoparticles by Directed Electron Beam Irradiation

Spatial confinement of matter in functional nanostructures has propelled these systems to the forefront of nanoscience, both as a playground for exotic physics and quantum phenomena and in multiple applications including plasmonics, optoelectronics, and sensing. In parallel, the emergence of monochromated electron energy loss spectroscopy (EELS) has enabled exploration of local nanoplasmonic functionalities within single nanoparticles and the collective response of nanoparticle assemblies, providing deep insight into associated mechanisms. However, modern synthesis processes for plasmonic nanostructures are often limited in the types of accessible geometry, and materials and are limited to spatial precisions on the order of tens of nm, precluding the direct exploration of critical aspects of the structure-property relationships. Here, the atomic-sized probe of the scanning transmission electron microscope is used to perform precise sculpting and design nanoparticle configurations. Using low-loss EELS, dynamic analyses of the evolution of the plasmonic response are provided. It is shown that within self-assembled systems of nanoparticles, individual nanoparticles can be selectively removed, reshaped, or patterned with nanometer-level resolution, effectively modifying the plasmonic response in both space and energy. This process significantly increases the scope for design possibilities and presents opportunities for unique structure development, which are ultimately the key for nanophotonic design.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

High-precision mass measurement of Si 24 and a refined determination of the r p process at the A = 22 waiting point

We report a high-precision mass measurement of 24 Si, performed with the Low Energy Beam and Ion Trap (LEBIT) facility at the National Superconducting Cyclotron Laboratory. The atomic mass excess, 10 753.8 (37) keV, is a factor of 5 more precise than previous results. This substantially reduces the uncertainty of the 23 Al(p ,γ) 24 Si reaction rate, which is a key part of the rapid proton capture (rp) process powering type I x-ray bursts. Furthermore, the updated rate constrains the onset temperature of the (α,p) process at the 22 Mg waiting point to a precision of 9%.

20 ≤ A ≤ 38↗

DOE OSTI2023

Spin Squeezing by Rydberg Dressing in an Array of Atomic Ensembles

Here, we report on the creation of an array of spin-squeezed ensembles of cesium atoms via Rydberg dressing, a technique that offers optical control over local interactions between neutral atoms. We optimize the coherence of the interactions by a stroboscopic dressing sequence that suppresses super-Poissonian loss. We thereby prepare squeezed states of N = 200 atoms with a metrological squeezing parameter ξ 2 = 0.77⁢(9) quantifying the reduction in phase variance below the standard quantum limit. We realize metrological gain across three spatially separated ensembles in parallel, with the strength of squeezing controlled by the local intensity of the dressing light. Our method can be applied to enhance the precision of tests of fundamental physics based on arrays of atomic clocks and to enable quantum-enhanced imaging of electromagnetic fields.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Non-Linear Optics at Twist Interfaces in h-BN/SiC Heterostructures

Understanding the emergent electronic structure in twisted atomically thin layers has led to the exciting field of twistronics. However, practical applications of such systems are challenging since the specific angular correlations between the layers must be precisely controlled and the layers have to be single crystalline with uniform atomic ordering. Here, in this work, an alternative, simple, and scalable approach is suggested, where nanocrystalline two-dimensional (2D) film on 3D substrates yields twisted-interface-dependent properties. Ultrawide-bandgap hexagonal boron nitride (h-BN) thin films are directly grown on high in-plane lattice mismatched wide-bandgap silicon carbide (4H-SiC) substrates to explore the twist-dependent structure-property correlations. Concurrently, nanocrystalline h-BN thin film shows strong non-linear second-harmonic generation and ultra-low cross-plane thermal conductivity at room temperature, which are attributed to the twisted domain edges between van der Waals stacked nanocrystals with random in-plane orientations. First-principles calculations based on time-dependent density functional theory manifest strong even-order optical nonlinearity in twisted h-BN layers. This work unveils that directly deposited 2D nanocrystalline thin film on 3D substrates could provide easily accessible twist-interfaces, therefore enabling a simple and scalable approach to utilize the 2D-twistronics integrated in 3D material devices for next-generation nanotechnology.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Characterization of Fuel Cladding Chemical Interaction on a High Burnup U-10Zr Metallic Fuel via Electron Energy Loss Spectroscopy Enhanced by Machine Learning

Fuel cladding chemical interaction (FCCI) is one of the main performance limiting factors for metallic nuclear fuels. The interaction destabilizes the martensitic microstructure and deteriorates mechanical properties of HT-9 cladding. The detection of low atomic number elements (Z<10) and overlapping of elemental peaks can be problematic in interpreting energy dispersive X-ray spectroscopy (EDS) data. Electron energy loss spectroscopy (EELS) provides precise elemental edge energy values and can detect elements with a low atomic number. This work utilizes EELS to study the distribution of lanthanides and light elements at the interaction region. The sample was prepared from the FCCI region of a U-10Zr (wt.%) solid fuel with HT-9 cladding, irradiated to a burnup of 13.2 at.%. Processing the EELS data included three major steps: 1) enhance the signal to noise ratio by denoising the spectrum with principal component analysis (PCA) method, removing background and performing deconvolution; 2) identify chemical elements with core energy loss edges; 3) confirm different phases using a popular machine learning method, K-means. This work presents qualitative assessment of lanthanides and light elements like carbon (C) and oxygen (O) enhanced by the application of machine learning algorithms. By comparing with EDS elemental maps, EELS provides higher resolution chemical maps, reveals the distribution of carbon at the interaction region supporting the formation of zirconium carbide, a rind-like microstructure feature that was proposed to mitigate the chemical interaction. Furthermore, the plasmon peak map was also found to indicate an energy shift associated with the formation of phases/compounds. K-means clustering method was used on the processed electron energy loss (EEL) spectrum to automatically reveal different phases. The resulting clustered maps from K-means clustering align well with elemental maps confirming certain phases, especially Fe-Ce and Zr-C, in the FCCI region.

EELS↗

DOE OSTI2024

High-angular-momentum Rydberg states in a room-temperature vapor cell for dc electric-field sensing

We prepare and analyze Rydberg states with orbital quantum numbers ℓ ≤ 6 using three-optical-photon electromagnetically induced transparency (EIT) and radio frequency (rf) dressing, and employ the high- ℓ states in electric-field sensing. Rubidium-85 atoms in a room-temperature vapor cell are first promoted into the 25 F 5 / 2 state via Rydberg-EIT with three infrared laser beams. Two rf dressing fields then (near-)resonantly couple the 25 F , 25 H ( ℓ = 5 ) , and 25 I ( ℓ = 6 ) Rydberg states. The dependence of the rf-dressed Rydberg-state level structure on rf powers, rf and laser frequencies is characterized using EIT. Furthermore, we discuss the principles of dc-electric-field sensing using high- ℓ Rydberg states and experimentally demonstrate the method using test electric fields of ≲ 50 V/m induced via photo-illumination of the vapor-cell wall. We measure the highly nonlinear dependence of the dc-electric-field strength on the power of the photo-illumination laser. Numerical calculations, which reproduce our experimental observations well, elucidate the underlying physics. Our paper is relevant to high-precision spectroscopy of high- ℓ Rydberg states, Rydberg-atom-based electric-field sensing, and plasma electric-field diagnostics. Published by the American Physical Society 2024

Duspayev, Alisher (ORCID:0000000153225762)↗

DOE OSTI2024

Optimizing the quality factor of InP nanobeam cavities using atomic layer deposition

Photonic crystal nanobeam cavities are valued for their small mode volume, CMOS compatibility, and high coupling efficiency-crucial features for various low-power photonic applications and quantum information processing. However, despite their potential, nanobeam cavities often suffer from low quality factors due to fabrication imperfections that create surface states and optical absorption. In this work, we demonstrate InP nanobeam cavities with up to 140% higher quality factors by applying a coating of Al 2 O 3 via atomic layer deposition to terminate dangling bonds and reduce surface absorption. Additionally, changing the deposition thickness allows precise tuning of the cavity mode wavelength without compromising the quality factor. This Al 2 O 3 atomic layer deposition approach holds great promise for optimizing nanobeam cavities that are well-suited for integration with a wide range of photonic applications.

42 ENGINEERING↗

DOE OSTI2024

Final state interactions for high energy scattering off atomic electrons

We consider the scattering of high energy leptons off bound atomic electrons focusing primarily on final state interactions between the outgoing energetic electron, and the heavy residual charged “debris” in the final state. These effects are inherently absent from calculations for a free electron at rest. Coulomb exchanges are enhanced by the large number of electrons in the atomic debris, and are unsuppressed by nonrelativistic velocities in the debris. We find that these exchanges can be resummed using operator methods, and cancel at the level of the cross section until at least 𝑂⁡(𝛼 3 ). Furthermore, we argue that both final and initial state Coulomb exchanges (enhanced by the number of electrons in the atom) do not affect the cross section until at least 𝑂⁡(𝛼 3 ). Transverse photon couplings to nonrelativistic electrons are proportional to their small velocities, and rotational invariance suppresses their contribution to 𝑂⁡(𝛼 3 ). Our results are relevant for precision experiments involving neutrinos, electrons, positrons, and muons scattering off of atomic electrons in a fixed target.

Atoms↗