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Results for “single-electron spectroscopy”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Mapping charge excitations in generalized Wigner crystals

Transition metal dichalcogenide-based moiré superlattices exhibit strong electron-electron correlations, thus giving rise to strongly correlated quantum phenomena such as generalized Wigner crystal states. Evidence of Wigner crystals in transition metal dichalcogenide moire superlattices has been widely reported from various optical spectroscopy and electrical conductivity measurements, while their microscopic nature has been limited to the basic lattice structure. Theoretical studies predict that unusual quasiparticle excitations across the correlated gap between upper and lower Hubbard bands can arise due to long-range Coulomb interactions in generalized Wigner crystal states. However, the microscopic proof of such quasiparticle excitations is challenging because of the low excitation energy of the Wigner crystal. Here, in this study, we describe a scanning single-electron charging spectroscopy technique with nanometre spatial resolution and single-electron charge resolution that enables us to directly image electron and hole wavefunctions and to determine the thermodynamic gap of generalized Wigner crystal states in twisted WS 2 moiré heterostructures. High-resolution scanning single-electron charging spectroscopy combines scanning tunnelling microscopy with a monolayer graphene sensing layer, thus enabling the generation of individual electron and hole quasiparticles in generalized Wigner crystals. We show that electron and hole quasiparticles have complementary wavefunction distributions and that thermodynamic gaps of ~50 meV exist for the 1/3 and 2/3 generalized Wigner crystal states in twisted WS 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2022

Sensing ultrashort electronic coherent beating at conical intersections by single-electron pulses

In a theoretical study, we present an ultrafast technique for probing time-dependent molecular charge densities. An ultrafast optical pump first brings the molecule into an electronic nonstationary state. This is followed by coherent inelastic scattering of a broadband single-electron probe pulse with a variable delay T, which is detected spectrally. The technique is applied to reveal phase-sensitive background-free coherent electron beating in the conical intersection passage in uracil and reveals the otherwise elusive coherent beating of strongly coupled electrons and nuclei.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS2004

Progress Towards High-Sensitivity Arrays of Detectors of Sub-mm Radiation Using Superconducting Tunnel Junctions with Integrated Radio Frequency Single-Electron Transistors

For high resolution imaging and spectroscopy in the FIR and submillimeter, space observatories will demand sensitive, fast, compact, low-power detector arrays with 104 pixels and sensitivity less than 10(exp -20) W/Hz(sup 0.5). Antenna-coupled superconducting tunnel junctions with integrated rf single-electron transistor readout amplifiers have the potential for achieving this high level of sensitivity, and can take advantage of an rf multiplexing technique. The device consists of an antenna to couple radiation into a small superconducting volume and cause quasiparticle excitations, and a single-electron transistor to measure current through junctions contacting the absorber. We describe optimization of device parameters, and results on fabrication techniques for producing devices with high yield for detector arrays. We also present modeling of expected saturation power levels, antenna coupling, and rf multiplexing schemes.

Stevenson, T. R.↗
DOE OSTI2026

The Role of Defect Geometry in Localized Emission from Monolayer Tungsten Dichalcogenides

In two-dimensional transition metal dichalcogenides such as tungsten diselenide (WSe 2 ), single photon emission has been broadly attributed to exciton localization from atomic point defects, yet the precise microscopic origins are unclear. This work introduces an empirically grounded computational framework that explains the origins of facile single photon emission in WSe 2 . High-resolution microscopy identifies native defect geometries in monolayer WSe 2 lattices from which the model is built. Here, the qualitative effects of chalcogen type, defect geometry, and mechanical strain on the electronic structure are individually assessed using density functional theory, and a specific divacancy configuration emerges as the candidate for localized single-electron transitions that match observed spectral energies. Spectroscopy and photon correlation measurements further validate this model, establishing a self-consistent link between defect geometry, electronic structure, and quantum emission.

defect emission↗
NASA NTRS2002

Progress Towards High-Sensitivity Arrays of Detectors of Sub-mm Radiation using Superconducting Tunnel Junctions with Radio-Frequency Single-Electron Transistors

The science drivers for the SPIRIT/SPECS missions demand sensitive, fast, compact, low-power, large-format detector arrays for high resolution imaging and spectroscopy in the far infrared and submillimeter. Detector arrays with 10,000 pixels and sensitivity less than 10(exp 20)-20 W/Hz(exp 20)0.5 are needed. Antenna-coupled superconducting tunnel junction detectors with integrated rf single-electron transistor readout amplifiers have the potential for achieving this high level of sensitivity, and can take advantage of an rf multiplexing technique when forming arrays. The device consists of an antenna structure to couple radiation into a small superconducting volume and cause quasiparticle excitations, and a single-electron transistor to measure currents through tunnel junction contacts to the absorber volume. We will describe optimization of device parameters, and recent results on fabrication techniques for producing devices with high yield for detector arrays. We will also present modeling of expected saturation power levels, antenna coupling, and rf multiplexing schemes.

Stevenson, T. R.↗
DOE OSTI2024

The insufficiency of the charge transfer model for resonant $\text{XES}$ in $\text{UF}$ 4

Recently, it was suggested that the single-electron charge transfer model (ligand 2p to Uranium 5f transition) could be used to explain the U M 4,5 Resonant X-ray Emission Spectroscopy (XES) of uranium dioxide (UO 2 ) and uranium tetrafluoride (UF 4 ). Here in this report, it is shown that this model produces results inconsistent with a joint consideration of both of the bandgaps of UO 2 and UF 4 and is thus insufficient to explain the observed behavior. An alternative Raman-based model is proposed.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Single-electron charge transfer into putative Majorana and trivial modes in individual vortices

Majorana bound states are putative collective excitations in solids that exhibit the self-conjugate property of Majorana fermions—they are their own antiparticles. In iron-based superconductors, zero-energy states in vortices have been reported as potential Majorana bound states, but the evidence remains controversial. Here, we use scanning tunneling noise spectroscopy to study the tunneling process into vortex bound states in the conventional superconductor NbSe 2 , and in the putative Majorana platform FeTe 0.55 Se 0.45 . We find that tunneling into vortex bound states in both cases exhibits charge transfer of a single electron charge. Our data for the zero-energy bound states in FeTe 0.55 Se 0.45 exclude the possibility of Yu–Shiba–Rusinov states and are consistent with both Majorana bound states and trivial vortex bound states. Our results open an avenue for investigating the exotic states in vortex cores and for future Majorana devices, although further theoretical investigations involving charge dynamics and superconducting tips are necessary.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Characterization of the Cherenkov Photon Background for Low-noise Silicon Detectors in Space

Future space observatories that seek to perform imaging and spectroscopy of faint astronomical sources will require ultra-low-noise detectors that are sensitive over a broad wavelength range. Silicon charge-coupled devices (CCDs), such as EMCCDs, skipper CCDs, multi-amplifier sensing CCDs, and single-electron sensitive read out CCDs have demonstrated the ability to detect and measure single photons from X-ray energies to near the silicon band gap (∼1.1 μm), making them candidate technologies for this application. Here, in this context, we study a relatively unexplored source of low-energy background coming from Cherenkov radiation produced by energetic cosmic rays traversing a silicon detector. We present a model for Cherenkov photon production and absorption that is calibrated to laboratory data, and we use this model to characterize the residual background rate for ultra-low-noise silicon detectors in space. We study how the Cherenkov background rate depends on detector thickness, variations in solar activity, and the contribution of heavy cosmic ray species (Z > 2). We find that for thick silicon detectors, such as those required to achieve high quantum efficiency at long wavelengths, the rate of cosmic-ray-induced Cherenkov photon production is comparable to other detector and astrophysical backgrounds. We apply our Cherenkov background model to simulated spectroscopic observations of extra-solar planets, and we find that thick detectors continue to outperform their thinner counterparts at longer wavelengths despite a larger Cherenkov background rate. Furthermore, we find that minimal masking of cosmic-ray tracks continues to maximize the signal-to-noise ratio of very faint sources despite the existence of extended halos of Cherenkov photons.

Astronomical detectors↗
DOE OSTI2021

Defying Thermodynamics: Stabilization of Alane Within Covalent Triazine Frameworks for Reversible Hydrogen Storage

The highly unfavorable thermodynamics of direct aluminum hydrogenation can be overcome by stabilizing alane within a nanoporous bipyridine-functionalized covalent triazine framework (AlH 3 @CTF-bipyridine). This material and the counterpart AlH 3 @CTF-biphenyl rapidly desorb H 2 between 95 and 154°C, with desorption complete at 250°C. Sieverts measurements, 27 Al MAS NMR and 27 Al{ 1 H} REDOR experiments, and computational spectroscopy reveal that AlH 3 @CTF-bipyridine dehydrogenation is reversible at 60°C under 700 bar hydrogen, >10 times lower pressure than that required to hydrogenate bulk aluminum. DFT calculations and EPR measurements support an unconventional mechanism whereby strong AlH 3 binding to bipyridine results in single-electron transfer to form AlH 2 (AlH 3 ) n clusters. Here the resulting size-dependent charge redistribution alters the dehydrogenation/rehydrogenation thermochemistry, suggesting a novel strategy to enable reversibility in high-capacity metal hydrides.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Defying Thermodynamics: Stabilization of Alane Within Covalent Triazine Frameworks for Reversible Hydrogen Storage

Metastable metal hydrides such as AlH 3 have many attractive features as hydrogen storage media, but generally require complex reaction schemes for regeneration following H 2 release. Here in this paper, we demonstrate that the highly unfavorable thermodynamics of direct aluminum hydrogenation can be overcome by stabilizing alane within a nanoporous bipyridine-functionalized Covalent Triazine Framework (AlH 3 @CTF-bipyridine). This material and the counterpart AlH 3 @CTF-biphenyl rapidly desorb H 2 between 95 and 154 °C, with desorption complete at 250 °C. Sieverts measurements, 27 Al MAS NMR and 27 Al{ 1 H} REDOR experiments, and computational spectroscopy reveal that AlH 3 @CTF-bipyridine dehydrogenation is reversible at 60 °C under 700 bar hydrogen, >10 times lower pressure than that required to hydrogenate bulk aluminum. DFT calculations and EPR measurements support an unconventional mechanism whereby strong AlH 3 binding to bipyridine results in single-electron transfer to form AlH 2 (AlH 3 ) n clusters. The resulting size-dependent charge redistribution alters the dehydrogenation/rehydrogenation thermochemistry, suggesting a novel strategy to enable reversibility in high-capacity metal hydrides.

Coordination Chemistry↗
DOE OSTI2020

Time-resolved resonant inelastic x-ray scattering in a pumped Mott insulator

Collective excitations contain rich information about photoinduced transient states in correlated systems. In a Mott insulator, charge degrees of freedom are frozen, but can be activated by photodoping. The energy-momentum distribution of the charge excitation spectrum reflects the propagation of charge degrees of freedom and provides information about the interplay among various intertwined instabilities on the timescale set by the pump. To reveal charge excitations out of equilibrium, here we simulate time-resolved x-ray absorption and resonant inelastic x-ray scattering using a Hubbard model. After pumping, the former resolves photodoping, while the latter characterizes the formation, dispersion, weight, and nonlinear effects of collective excitations. Intermediate-state information from time-resolved resonant inelastic x-ray scattering (trRIXS) can be used to decipher the origin of these excitations, including bimagnons, Mott-gap excitations, doublon and single-electron in-gap states, and anti-Stokes relaxation during an ultrafast pump. This paper provides a theoretical foundation for existing and future trRIXS experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Toward Å-fs-meV Resolution in Electron Microscopy: Systematic Simulation of the Temporal Spread of Single-Electron Packets

Though efforts to improve the temporal resolution of transmission electron microscopes (TEMs) have waxed and waned for decades, with relatively recent advances routinely reaching sub-picosecond scales, fundamental and practical challenges have hindered the advance of combined Å-fs-meV resolutions, particularly for core-loss spectroscopy and real-space imaging. This is due in no small part to the complexity of the approach required to access timescales upon which electrons, atoms, molecules, and materials first begin to respond and transform – attoseconds to picoseconds. Here we present part of a larger effort devoted to systematically mapping the instrument parameter space of a TEM modified to reach ultrafast timescales. With General Particle Tracer, we studied the statistical temporal distributions of single-electron packets as a function of various fs pulsed-laser parameters and electron-gun configurations and fields for the exact architecture and dimensions of a Thermo Fisher Tecnai Femto ultrafast electron microscope. We focused on easily-adjustable parameters, such as laser pulse duration, laser spot size, photon energy, Wehnelt aperture diameter, and photocathode size. In addition to establishing trends and dispersion behaviors, we identify regimes within which packet duration can be 100s of fs and approach the 300-fs laser limit employed here. Overall, the results provide a detailed picture of the temporal behavior of single-electron packets in the Tecnai Femto gun region, forming the initial contribution of a larger effort.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Ni/Photoredox-Catalyzed C(sp 3 )–C(sp 3 ) Coupling between Aziridines and Acetals as Alcohol-Derived Alkyl Radical Precursors

Aziridines are readily available C(sp 3 ) precursors that afford valuable β-functionalized amines upon ring opening. In this article, we report a Ni/photoredox methodology for C(sp 3 )–C(sp 3 ) cross-coupling between aziridines and methyl/1°/2° aliphatic alcohols activated as benzaldehyde dialkyl acetals. Orthogonal activation modes of each alkyl coupling partner facilitate cross-selectivity in the C(sp 3 )–C(sp 3 ) bond-forming reaction: the benzaldehyde dialkyl acetal is activated via hydrogen atom abstraction and β-scission via a bromine radical (generated in situ from single-electron oxidation of bromide), whereas the aziridine is activated at the Ni center via reduction. Here, we demonstrate that an Ni(II) azametallacycle, conventionally proposed in aziridine cross-coupling, is not an intermediate in the productive cross-coupling. Rather, stoichiometric organometallic and linear free energy relationship studies indicate that aziridine activation proceeds via Ni(I) oxidative addition, a previously unexplored elementary step.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Structural and spectroscopic characterization of an einsteinium complex

The transplutonium elements (atomic numbers 95–103) are a group of metals that lie at the edge of the periodic table. As a result, the patterns and trends used to predict and control the physics and chemistry for transition metals, main-group elements and lanthanides are less applicable to transplutonium elements. Furthermore, understanding the properties of these heavy elements has been restricted by their scarcity and radioactivity. This is especially true for einsteinium (Es), the heaviest element on the periodic table that can currently be generated in quantities sufficient to enable classical macroscale studies. Here we characterize a coordination complex of einsteinium, using less than 200 nanograms of 254 Es (with half-life of 275.7(5) days), with an organic hydroxypyridinone-based chelating ligand. X-ray absorption spectroscopic and structural studies are used to determine the energy of the L 3 -edge and a bond distance of einsteinium. Photophysical measurements show antenna sensitization of EsIII luminescence; they also reveal a hypsochromic shift on metal complexation, which had not previously been observed in lower-atomic-number actinide elements. Here, these findings are indicative of an intermediate spin–orbit coupling scheme in which j–j coupling (whereby single-electron orbital angular momentum and spin are first coupled to form a total angular momentum, j) prevails over Russell–Saunders coupling. Together with previous actinide complexation studies, our results highlight the need to continue studying the unusual behaviour of the actinide elements, especially those that are scarce and short-lived.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Valley splittings in Si/SiGe quantum dots with a germanium spike in the silicon well

Silicon-germanium heterostructures have successfully hosted quantum dot qubits, but the intrinsic near-degeneracy of the two lowest valley states poses an obstacle to high-fidelity quantum computing. Here we present a modification to the Si/SiGe heterostructure by the inclusion of a spike in germanium concentration within the quantum well in order to increase the valley splitting. The heterostructure is grown by chemical vapor deposition and magnetospectroscopy is performed on gate-defined quantum dots to measure the excited state spectrum. We demonstrate a large and widely tunable valley splitting as a function of applied vertical electric field and lateral dot confinement. We further investigate the role of the germanium spike by means of tight-binding simulations in single-electron dots and show a robust doubling of the valley splitting when the spike is present, as compared to a standard (spike-free) heterostructure. This doubling effect is nearly independent of the electric field, germanium content of the spike, and spike location. This experimental evidence of a stable, tunable quantum dot, despite a drastic change to the heterostructure, provides a foundation for future heterostructure modifications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Impact of Arsenic- and Indium-Terminated InGaAs Stressors on Carrier Confinement, Strain, Defects, and Transport Properties of Tensile-Strained Ge

Device-quality tensile-strained Ge (ε-Ge) grown on a large bandgap semiconductor with superior electrical and optical carrier confinement is essential for group-IV-based optoelectronics. Properties of ε-Ge active layers synthesized on In 0.24 Ga 0.76 As buffers with two different surface terminations─arsenic-rich and indium-rich─were experimentally demonstrated, highlighting the factors not considered in theoretical calculations. High-resolution X-ray diffraction and Raman spectroscopy analyses of these ε-Ge/In 0.24 Ga 0.76 As heterostructures confirmed the fully strained (1.6%) and partially relaxed (0.82%) nature of the ε-Ge bonded with arsenic-terminated (Ge As-terminated ) and indium-terminated (Ge In-terminated ) In 0.24 Ga 0.76 As stressors, respectively. High-resolution cross-sectional transmission electron microscopy showed a coherent, sharp, and fully strained ε-Ge/In 0.24 Ga 0.76 As heterointerface in the Ge As-terminated heterostructure, whereas microtwin defects were present in the Ge In-terminated heterostructure. These heterostructures were further characterized by evaluating the minority carrier lifetimes, high for Ge As-terminated (525 ns) and low for Ge In-terminated (69 ns), using the photoconductive decay technique. Moreover, band alignment was constructed using X-ray photoelectron spectroscopy, where the Ge As-terminated heterostructure revealed that both holes and electrons were confined within the ε-Ge active layer as a type-I band alignment with ΔE V, As-terminated = 0.22 eV and ΔE C,As-terminated = 0.38 eV. On the other hand, the Ge In-terminated heterostructure exhibited a type-II band alignment with ΔE V,In-terminated = – 0.02 eV and ΔE C,In-terminated = 0.53 eV. Furthermore, the magnetotransport properties revealed high mobility (321 cm 2 /(V s)) with single-electron transport in Ge As-terminated heterostructure and low mobility (3.34 cm 2 /(V s)) with multihole transport in the Ge In-terminated heterostructure. Therefore, preferring the ε-Ge on the arsenic-rich surface of In 0.24 Ga 0.76 As stressor over the indium-rich surface during material synthesis offers device-quality materials with high carrier lifetime and superior carrier confinement, which can provide an opportunity to fabricate efficient group-IV-based optoelectronic devices.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Strengths of plasmon satellites in XPS: Real-time cumulant approach

Plasmon satellites observed in x-ray photoemission spectra (XPS) reflect many-body effects beyond the single-electron approximation. However, theoretical calculations are challenging and simplified theories based on electron gas models are not always satisfactory. Here, a cumulant Green’s function approach with a real-time time-dependent density functional theory calculation of the cumulant is described for calculations of these effects, without the need for adjustable parameters. Here, the approach yields good agreement with experimental XPS results, as illustrated for Ge and Al. Corrections due to extrinsic losses and interference are also briefly discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS2006

Using Quasiparticle Poisoning To Detect Photons

According to a proposal, a phenomenon associated with excitation of quasiparticles in certain superconducting quantum devices would be exploited as a means of detecting photons with exquisite sensitivity. The phenomenon could also be exploited to perform medium-resolution spectroscopy. The proposal was inspired by the observation that Coulomb blockade devices upon which some quantum logic gates are based are extremely sensitive to quasiparticles excited above the superconducting gaps in their leads. The presence of quasiparticles in the leads can be easily detected via the charge states. If quasiparticles could be generated in the leads by absorption of photons, then the devices could be used as very sensitive detectors of electromagnetic radiation over the spectral range from x-rays to submillimeter waves. The devices in question are single-Cooper-pair boxes (SCBs), which are mesoscopic superconducting devices developed for quantum computing. An SCB consists of a small superconducting island connected to a reservoir via a small tunnel junction and connected to a voltage source through a gate capacitor. An SCB is an artificial two-level quantum system, the Hamiltonian of which can be controlled by the gate voltage. One measures the expected value of the charge of the eigenvectors of this quantum system by use of a radio-frequency single-electron transistor. A plot of this expected value of charge as a function of gate voltage resembles a staircase that, in the ideal case, consists of steps of height 2 e (where e is the charge of one electron). Experiments have shown that depending on the parameters of the device, quasiparticles in the form of "broken" Cooper pairs present in the reservoir can tunnel to the island, giving rise to steps of 1 e. This effect is sometimes called "poisoning." Simulations have shown that an extremely small average number of quasiparticles can generate a 1-e periodic signal. In a device according to the proposal, this poisoning would be turned to advantage. Depending on the wavelength, an antenna or other component would be used to couple radiation into the reservoir, wherein the absorption of photons would break Cooper pairs, thereby creating quasiparticles that, in turn, would tunnel to the island, creating a 1-e signal. On the basis of conservative estimates of device parameters derived from experimental data and computational simulations that fit the data, it has been estimated that the noise equivalent power of a device according to the proposal could be as low as 6 10(exp -22) W/Hz(exp 1/2). It has also been estimated that the spectroscopic resolution (photon energy divided by increment of photon energy) of such a device in visible light would exceed 100.

Echternach, Pierre↗