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Results for “Coherent spectroscopy”

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At least 541 records · Page 30

All sources NASA NTRS DOE OSTI

DOE OSTI2022

Extremely Slow Diffusion of Gold Nanoparticles under Confinement in Mesoporous Silica

Here, we report an X-ray photon correlation spectroscopy (XPCS) study of the mobility of colloidal gold nanoparticles with a diameter of approximately 4 nm in glycerol under confinement within the channels of SBA-15 mesoporous silica with pore diameters of approximately 6 and 12 nm. The XPCS correlation functions result from an effective heterodyne signal due to the mixing of the coherent scattering from the nanoparticles and the mesoporous silica. Over the range of wave vectors and hence length scales probed, the nanoparticle dynamics are well described by one-dimensional diffusion. The nanoparticle diffusivity varies with temperature in a manner expected based on the temperature-dependent viscosity of glycerol; however, the magnitudes of the diffusion coefficients are several orders of magnitude smaller than those of the nanoparticles in bulk glycerol. We consider mechanisms that might contribute to this reduction in diffusivity including enhancement in hydrodynamic drag under confinement, effects of nanoparticle adsorption to the pore walls, and slowing structural dynamics in glycerol due to the combination of the nanometer-scale confinement and the presence of the nanoparticles.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Atomic-Scale Characterization and Electronic Properties of Gold-Capped Niobium Films for Superconducting Qubits

Niobium thin films are central to superconducting qubits, but their complex native oxides contribute significantly to microwave losses. A promising mitigation strategy is to suppress oxide formation using engineered thin-film encapsulation layers. Recent experiments have shown that ∼10 nm metallic overlayers on Nb capacitor films can improve the energy relaxation time T1 of transmon qubits. Here, we present a comparative study of Au-capped Nb films fabricated in situ by molecular beam epitaxy and ex situ by sequential deposition benchmarked against bare Nb films. Using complementary structural, chemical, and spectroscopic techniques, we correlate the interface quality with superconducting electronic properties of the Au surface. Low-temperature scanning tunneling spectroscopy (STS) provides spatially resolved quasiparticle density-of-states maps. While both Au-capped Nb samples exhibit large areas with uniform, fully gapped density of states, clear differences emerge between the two interfaces. Compared to in situ Nb-Au, ex situ Nb-Au exhibits a reduced induced superconducting gap, broadened coherence peak, and localized in-gap states, consistent with a residual NbxOy layer at the interface. Supported by complementary structural and chemical analyses, these findings demonstrate that STS directly links nanoscale superconducting properties to interface preparation, highlighting the importance of controlled in situ encapsulation for minimizing dissipation and improving quantum coherence.

Makita, Junki [MIT; Temple U.] (ORCID:000000026889↗

NASA NTRS1997

From Top to Bottom - the Multiwavelength Campaign of V824 Ara (HD 155555)

A great deal of progress has been made in recent years in decomposing the 2-D structure in the atmospheres of late-type stars. Doppler images of many photospheres single stars, T Tauri stars, Algols, RS CV(sub n) binaries to name a few - are regularly published (Strassmeier 1996; Richards and Albright 1996; Rice and Strassmeier 1996; Kuerster et al. 1994). Ultraviolet spectral images of chromospheres appear in the literature (e.g., Walter et al. 1987; Neff et al. 1989) but are less common owing to the difficult nature of obtaining complete phase coverage. Zeeman doppler images of magnetic fields are now feasible (e.g., Donati et al. 1992). Performing Doppler imaging of the same targets over many seasons has also been accomplished (e.g, Vogt et al. 1997). Even when a true image reconstruction is not possible due to poor spectral resolution, we can still infer a great deal about spatial structure if enough phases are observed. However, it is increasingly apparent that to make sense of recent results, many different spectral features spanning a range of formation temperature and density must be observed simultaneously for a coherent picture to emerge. Here we report on one such campaign. In 1996, we observed the southern hemisphere RS CV(sub n) binary V824 Ara (P=1(sup d).68, G5IV+K0V-IV-IV) over one complete stellar rotation with the Hubble Space Telescope and EUVE. In conjunction, radio and optical photometry and spectroscopy were obtained from the ground. Unique to this campaign is the complete phase coverage of a number of activity proxy indicators that cover source temperatures ranging from the photosphere to the corona.

Dempsey, Robert↗

NASA NTRS2013

Optical Properties of Iron Silicates in the Infrared to Millimeter as a Function of Wavelength and Temperature

The Optical Properties of Astronomical Silicates with Infrared Techniques program utilizes multiple instruments to provide spectral data over a wide range of temperatures and wavelengths. Experimental methods include Vector Network Analyzer and Fourier transform spectroscopy transmission, and reflection/scattering measurements. From this data, we can determine the optical parameters for the index of refraction, n, and the absorption coefficient, k. The analysis of the laboratory transmittance data for each sample type is based upon different mathematical models, which are applied to each data set according to their degree of coherence. Presented here are results from iron silicate dust grain analogs, in several sample preparations and at temperatures ranging from 5 to 300 K, across the infrared and millimeter portion of the spectrum (from 2.5 to 10,000/micron or 4000 to 1/cm).

Dust↗

DOE OSTI2020

Coherent growth and characterization of van der Waals 1T-VSe2 layers on GaAs(111)B using molecular beam epitaxy

We report epitaxial growth of vanadium diselenide (VSe₂) thin films in the octahedrally coordinated (1T) structure on GaAs(111)B substrates by molecular beam epitaxy. Film thickness from a single monolayer (ML) up to 30 ML is demonstrated. Structural and chemical studies using x-ray diffraction, transmission electron microscopy, scanning tunneling microscopy, and x-ray photoelectron spectroscopy indicate high-quality thin films. Further studies show that monolayer VSe₂ films on GaAs are not air stable and are susceptible to oxidation within a matter of hours, which indicates that a protective capping layer should be employed for device applications. This work demonstrates that VSe₂, a candidate van der Waals material for possible spintronic and electronic applications, can be integrated with III-V semiconductors via epitaxial growth for two- and three-dimensional hybrid devices.

2D materials↗

DOE OSTI2025

Possible evidence of excitonic condensation in a topological insulator

The transient excitonic condensate is a nonequilibrium electron-hole Bardeen-Cooper-Schrieffer state in a photoexcited semiconductor and semimetal, where electron-hole pairs undergo a phase transition and condense into a single coherent quantum state. Despite numerous experimental works to realize the predicted excitonic condensation phase, experimental evidence still remains elusive. This is largely due to the absence of direct measurements of a material's transient momentum-dependent electronic structure and the excitonic state in the condensation regime. Here, using time and angle-resolved photoemission spectroscopy, we find direct evidence of a transient excitonic condensate in the spin-polarized spatially indirect excitonic topological states in Bi2Te3. Accompanying the formation of the excitonic topological states by photoexcitation, we reveal a splitting of the hole's and electron's quasi-equilibrium chemical potential followed by the band flattening and backbending of the transient topological surface state. Moreover, within the same momentum range, we report a reshaping of the bulk valence band in the form of a Mexican-hat-like Bogoliubov dispersion-hallmarks of the excitonic condensation, followed by the opening of an energy gap at the Fermi level. The fluence and temperature dependence of these renormalization effects are reminiscent of excitonic condensation within Bardeen-Cooper-Schrieffer (BCS)-like behavior. These results, together with theoretical simulation, point to the possible formation of a transient excitonic condensate and provide opportunities to manipulate topologically protected Bose condensates with light.

ARPES↗

NASA NTRS2013

Optical Properties of Iron Silicates in the Infrared to Millimeter as a Function of Wavelength and Temperature

The Optical Properties of Astronomical Silicates with Infrared Techniques (OPASI-T) program utilizes multiple instruments to provide spectral data over a wide range of temperature and wavelengths. Experimental methods include Vector Network Analyzer (VNA) and Fourier Transform Spectroscopy (FTS) transmission, and reflection/scattering measurements. From this data, we can determine the optical parameters for the index of refraction, n, and the absorption coefficient, k. The analysis of the laboratory transmittance data for each sample type is based upon different mathematical models, which are applied to each data set according to their degree of coherence. Presented here are results from iron silicate dust grain analogs, in several sample preparations and at temperatures ranging from 5-300 K, across the infrared and millimeter portion of the spectrum (from 2.5-10,000 μm or 4,000-1 cm(exp −1).

Optical↗

NASA NTRS2013

Optical Properties of Iron Silicates in the Infrared to Millimeter as a Function of Wavelength and Temperature

Methods: laboratory↗

DOE OSTI2024

Overview of Quantum Sensing Materials and Techniques for Energy Sector Applications

The energy sector has become increasingly dependent upon highly sensitive sensing devices for a wide range of applications. Variables such as temperature, pH, electromagnetic fields, ions, and pressure must be measured with high precision, often in harsh conditions (e.g. highly corrosive environments due to high temperature, pressure and humidity). These sensors are deployed in infrastructure such as transformers, pipelines, mines, nuclear power plants, and other areas to ensure safe operating conditions and uninterrupted, optimized service. Moreover, new opportunities for sensors have emerged due to the expansion of smart grids/meters, driverless vehicles, and the discovery of new oil, gas, and critical mineral deposits. The continued maturation of quantum sensing technologies offers exciting opportunities for quantum-enhanced measurements within the energy sector that may provide significant improvements in sensitivity beyond the classical limit. Here, an overview of established and emerging quantum materials for sensing applications will be provided, from trapped ions to color centers in diamond and silicon carbide. Associated quantum sensing methods for these materials will be discussed, with an emphasis on platforms that are nearing commercial viability. Specific application opportunities within the energy sector for quantum sensors will then be analyzed, including oil/gas discovery, greenhouse gas emission monitoring, pH and ion sensing, current measurement in electric vehicle batteries, and quantum-enhanced spectroscopy. Remaining barriers, such as quantum sensor platform miniaturization and ruggedization, will also be analyzed. A specific project at the National Energy Technology Laboratory involving the functionalization of qubits using metal-organic frameworks for enhanced quantum sensing will also be highlighted. Here, nitrogen vacancy centers (NV) in nanodiamonds, a commercially available qubit with long coherence times and utilizable quantum properties at room temperature, are encapsulated in a controlled way using the metal-organic framework ZIF-8. The ZIF-8 provides a well-defined, porous scaffold that can be controlled to promote the selective uptake of specific target analytes, such as gas molecules or ions. The quantum sensing performance of this composite material is either preserved or enhanced following ZIF-8 encapsulation; the optically detected magnetic resonance response of the NV nanodiamonds with and without the ZIF-8 coating are identical, while the ZIF-8 coating increases the longitudinal spin relaxation lifetime (T1) of the NV centers, an important parameter for spin relaxometry-based quantum sensing experiments. Taken together, these results demonstrate the importance of qubit functionalization as a crucial step for rationally designing high performance quantum sensors.

Crawford, Scott↗

DOE OSTI2025

Femtosecond x-ray photon correlation spectroscopy enables direct observations of atomic-scale relaxations of glass forming liquids

Glass-forming liquids exhibit structural relaxation behaviors, reflecting underlying atomic rearrangements on a wide range of timescales and playing a crucial role in determining material properties. However, the relaxation processes on the atomic scale are not well-understood due to the experimental difficulties in directly characterizing the evolving correlations of atomic-scale order in disordered systems. Here, in this study, we harness the coherence and ultrashort pulse characteristics of an x-ray free electron laser to directly probe atomic-scale ultrafast relaxation dynamics in the model system Ge 15 Te 85 . We demonstrate an analysis strategy for determining the intermediate scattering function by extracting the contrast decay of summed scattering patterns from two rapidly successive, nearly identical femtosecond x-ray pulses generated by a split-delay system. The result indicates a full decorrelation of atomic-scale order on the sub-picosecond timescale, supporting the argument for a high-fluidity fragile state of liquid Ge 15 Te 85 above its dynamic crossover temperature. The demonstrated strategy opens an avenue for experimental studies of relaxation dynamics in liquids, glasses, and other highly disordered systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Vortex-Controlled Quasiparticle Multiplication and Self-Growth Dynamics in Superconducting Resonators

Even in the quantum limit, non-equilibrium quasiparticle (QP) populations induce QP poisoning that irreversibly relaxes the quantum state and significantly degrades the coherence of transmon qubits. A particularly detrimental yet previously unexplored mechanism arises from QP multiplication facilitated by vortex trapping in superconducting quantum circuits, where a high-energy QP relaxes by breaking additional Cooper pairs and amplifying the QP population due to the locally reduced excitation gap and enhanced quantum confinement within the vortex core. Here we directly resolve this elusive QP multiplication process by revealing vortex-controlled QP self-generation in a highly nonequilibrium regime preceding the phonon bottleneck of QP relaxation. At sufficiently low fluence, femtosecond-resolved magneto-reflection spectroscopy directly reveals a continuously increasing QP population that is strongly dependent on magnetic-field-tuned vortex density and absent at higher excitation fluences. Quantitative analysis of the emergent QP pre-bottleneck dynamics further reveals that, although the phonon population saturates within $\simeq$10~ps, both free and trapped QPs continue to grow in a self-sustained manner--hallmarks of the long-anticipated QP-vortex interactions in nonequilibrium superconductivity. We estimate a substantial increase of $\sim$34% in QP density at vortex densities of $\sim$ 100 magnetic flux quanta per $\mathrm{Î¼m^{2}}$. Our findings establish a powerful spectroscopic tool for uncovering QP multiplication and reveal vortex-assisted QP relaxation as a critical materials bottleneck whose mitigation will be essential for resolving QP poisoning and enhancing coherence in superconducting qubits.

Park, Joong M. [Ames Lab]↗

DOE OSTI2021

Direct observation of kink evolution due to Hund’s coupling on approach to metal-insulator transition in NiS 2- x Se x

Understanding characteristic energy scales is a fundamentally important issue in the study of strongly correlated systems. In multiband systems, an energy scale is affected not only by the effective Coulomb interaction but also by the Hund’s coupling. Direct observation of such energy scale has been elusive so far in spite of extensive studies. Here, we report the observation of a kink structure in the low energy dispersion of NiS 2- x Se x and its characteristic evolution with x , by using angle resolved photoemission spectroscopy. Dynamical mean field theory calculation combined with density functional theory confirms that this kink originates from Hund’s coupling. We find that the abrupt deviation from the Fermi liquid behavior in the electron self-energy results in the kink feature at low energy scale and that the kink is directly related to the coherence-incoherence crossover temperature scale. Our results mark the direct observation of the evolution of the characteristic temperature scale via kink features in the spectral function, which is the hallmark of Hund’s physics in the multiorbital system.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Symmetry-protected electronic metastability in an optically driven cuprate ladder

Optically excited quantum materials exhibit non-equilibrium states with remarkable emergent properties, but these phenomena are usually transient, decaying on picosecond timescales and limiting practical applications. Advancing the design and control of non-equilibrium phases requires the development of targeted strategies to achieve long-lived, metastable phases. Here, in this study, we report the discovery of symmetry-protected electronic metastability in the model cuprate ladder Sr 14 Cu 24 O 41 . Using femtosecond resonant X-ray scattering and spectroscopy, we show that this metastability is driven by a transfer of holes from chain-like charge reservoirs into the ladders. This ultrafast charge redistribution arises from the optical dressing and activation of a hopping pathway that is forbidden by symmetry at equilibrium. Relaxation back to the ground state is, hence, suppressed after the pump coherence dissipates. Our findings highlight how dressing materials with electromagnetic fields can dynamically activate terms in the electronic Hamiltonian, and provide a rational design strategy for non-equilibrium phases of matter.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Excitons: Energetics and spatiotemporal dynamics

The concept of an exciton as a quasiparticle that represents collective excited states was originally adapted from solid-state physics and has been successfully applied to molecular aggregates by relying on the well-established limits of the Wannier exciton and the Frenkel exciton. However, the study of excitons in more complex chemical systems and solid materials over the past two decades has made it clear that simple concepts based on Wannier or Frenkel excitons are not sufficient to describe detailed excitonic behavior, especially in nano-structured solid materials, multichromophoric macromolecules, and complex molecular aggregates. In addition, important effects such as vibronic coupling, the influence of charge-transfer (CT) components, spin-state interconversion, and electronic correlation, which had long been studied but not fully understood, have turned out to play a central role in many systems. This has motivated new experimental approaches and theoretical studies of increasing sophistication. This article provides an overview of works addressing these issues that were published for A Special Topic of the Journal of Chemical Physics on ``Excitons: Energetics and spatio-temporal dynamics" and discusses their implications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Solar Contamination in Extreme-precision Radial-velocity Measurements: Deleterious Effects and Prospects for Mitigation

Solar contamination, due to moonlight and atmospheric scattering of sunlight, can cause systematic errors in stellar radial velocity (RV) measurements that significantly detract from the ∼10 cm s{sup −1} sensitivity required for the detection and characterization of terrestrial exoplanets in or near habitable zones of Sun-like stars. The addition of low-level spectral contamination at variable effective velocity offsets introduces systematic noise when measuring velocities using classical mask-based or template-based cross-correlation techniques. Here we present simulations estimating the range of RV measurement error induced by uncorrected scattered sunlight contamination. We explore potential correction techniques, using both simultaneous spectrometer sky fibers and broadband imaging via coherent fiber imaging bundles, that could reliably reduce this source of error to below the photon-noise limit of typical stellar observations. We discuss the limitations of these simulations, the underlying assumptions, and mitigation mechanisms. We also present and discuss the components designed and built into the NEID (NN-EXPLORE Exoplanet Investigations with Doppler spectroscopy) precision RV instrument for the WIYN 3.5 m telescope, to serve as an ongoing resource for the community to explore and evaluate correction techniques. We emphasize that while “bright time” has been traditionally adequate for RV science, the goal of 10 cm s{sup −1} precision on the most interesting exoplanetary systems may necessitate access to darker skies for these next-generation instruments.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1981

Time-resolved spectroscopy of the Mercury 6 3P1 state

The time-resolved fluorescence was observed from the Hg 6 3P1 state under the influence of the earth's magnetic field and with applied fields of up to 14 G. Modulation of the fluorescence decay signal was observed as a function of both time and space and can be interpreted in terms of a classical precession of the excited atom about the magnetic field or as quantum beats resulting from interference between coherently populated Zeeman sublevels. This modulation was studied for each of the five resolvable components of the hyperfine structure separately. The fluorescence from the even isotopes was determined to be almost completely modulated while the fluorescence from the odd isotopes was only partially modulated. The frequency of modulation of the fluorescence from the mercury-202 isotope was observed as a function of the applied magnetic field and a value for the Lande factor of 1.46 + or - 0.03 was obtained. This is within experimental error of the accepted value of 1.486. In addition, the frequency of modulation as a function of applied magnetic field was determined for each of the three resolvable components with more than one contributing isotopic hyperfine line. An investigation of the effect of radiation trapping on the degree modulation was also made.

Halstead, J. A.↗

NASA NTRS2005

The Visible Nulling Coronagraph--Architecture Definition and Technology Development

This paper describes the advantages of visible direct detection and spectroscopy of Earth-like extrasolar planets using a nulling coronagraph instrument behind a moderately sized single aperture space telescope. Our concept synthesizes a nulling interferometer by shearing the telescope pupil, with the resultant producing a deep null. We describe nulling configurations that also include methods to mitigate stellar leakage, such as spatial filtering by a coherent array of single mode fibers, and post-starlight suppression wavefront sensing and control. With diffraction limited telescope optics and similar quality components in the optical train (lambda/20), suppression of the starlight to 1e-10 is readily achievable. We describe key features of the architecture and analysis, present latest results of laboratory measurements demonstrating achievable null depth and component development, and discuss future key technical milestones.

nulling interferometer↗

NASA NTRS2020

Solar Contamination in Extreme-precision Radial-velocity Measurements: Deleterious Effects and Prospects for Mitigation

Solar contamination, due to moonlight and atmospheric scattering of sunlight, can cause systematic errors in stellar radial velocity (RV) measurements that signiﬁcantly detract from the ~10 cm/s sensitivity required for the detection and characterization of terrestrial exoplanets in or near habitable zones of Sun-like stars. The addition of low-level spectral contamination at variable effective velocity offsets introduces systematic noise when measuring velocities using classical mask-based or template-based cross-correlation techniques. Here we present simulations estimating the range of RV measurement error induced by uncorrected scattered sunlight contamination. We explore potential correction techniques, using both simultaneous spectrometer sky ﬁbers and broadband imaging via coherent ﬁber imaging bundles, that could reliably reduce this source of error to below the photon-noise limit of typical stellar observations. We discuss the limitations of these simulations, the underlying assumptions, and mitigation mechanisms. We also present and discuss the components designed and built into the NEID (NN-EXPLORE Exoplanet Investigations with Doppler spectroscopy) precision RV instrument for the WIYN 3.5m telescope, to serve as an ongoing resource for the community to explore and evaluate correction techniques. We emphasize that while “bright time” has been traditionally adequate for RV science, the goal of 10 cm/s precision on the most interesting exoplanetary systems may necessitate access to darker skies for these next generation instruments.

Arpita Roy↗