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At least 433 records · Page 24
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Making and breaking terahertz waves with fluid plasmas

Vigorous research efforts during the past several decades have successfully closed the “terahertz gap” between microwaves and infrared light, offering new and increasingly efficient ways to produce, detect, and manipulate radiation fields in the terahertz (THz) frequency range. In our laboratory, THz time-domain spectroscopy (THz-TDS) and optical-pump THz-probe (OPTP) experiments have been routinely utilized as ultrafast spectroscopy tools to investigate a variety of emerging quantum materials and metamaterials. The ultrafast THz pulses are produced by femtosecond laser excitation of photoconductive antennas, semiconductor surfaces (InAs), and nonlinear crystals (ZnTe, GaSe, and LiNbO 3 ). Photoconductive antennas and nonlinear crystals also allow for the coherent detection of these pulses in the time domain, with amplitude and phase spectra obtained in the frequency domain via fast Fourier transform. Although such solid-state schemes are highly desirable in many aspects and thus also commonly utilized in many research laboratories and industrial applications, they typically suffer from limited bandwidths due to the absorption and frequency dispersion induced primarily by phonon resonances, limiting THz applications such as spectroscopy of emerging materials, imaging and detection, and biomedical characterization.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Role of weak interlayer coupling in ultrafast exciton-exciton annihilation in two-dimensional rhenium dichalcogenides

Strong interactions between excitons are a characteristic feature of two-dimensional (2D) semiconductors, determining important excitonic properties, such as exciton lifetime, coherence, and photon-emission efficiency. Rhenium disulfide (ReS 2 ), a member of the 2D transition-metal dichalcogenide (TMD) family, has recently attracted great attention due to its unique excitons that exhibit excellent polarization selectivity and coherence features. However, an in-depth understanding of exciton-exciton interactions in ReS 2 is still lacking. In this work, we used ultrafast pump-probe spectroscopy to study exciton-exciton interactions in monolayer (1L), bilayer (2L), and triple layer ReS 2 . Additionally, we directly measure the rate of exciton-exciton annihilation, a representative Auger-type interaction between excitons. It decreases with increasing layer number, as observed in other 2D TMDs. However, while other TMDs exhibit a sharp weakening of exciton-exciton annihilation between 1L and 2L, such behavior was not observed in ReS 2 . We attribute this distinct feature in ReS 2 to the relatively weak interlayer coupling, which prohibits a substantial change in the electronic structure when the thickness varies. This work not only highlights the unique excitonic properties of ReS 2 but also provides novel insight into the thickness dependence of exciton-exciton interactions in 2D systems.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Dielectronic satellite emission from a solid-density Mg plasma: Relationship to models of ionization potential depression

Here, we report on experiments where solid-density Mg plasmas are created by heating with the focused output of the Linac Coherent Light Source x-ray free-electron laser. We study the K-shell emission from the helium- and lithium-like ions using Bragg crystal spectroscopy. Observation of the dielectronic satellites in lithium-like ions confirms that the M-shell electrons appear bound for these high charge states. An analysis of the intensity of these satellites indicates that when modeled with an atomic-kinetics code, the ionization potential depression model employed needs to produce depressions for these ions which lie between those predicted by the well known Stewart-Pyatt and Ecker-Kroll models. These results are largely consistent with recent density functional theory calculations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Coherent Acoustic Interferometry during the Photodriven Oxygen Evolution Reaction Associates Strain Fields with the Reactive Oxygen Intermediate (Ti–OH*)

The oxygen evolution reaction (OER) from water requires the formation of metastable, reactive oxygen intermediates to enable oxygen–oxygen bond formation. Conversely, such reactive intermediates could also structurally modify the catalyst. Here, a descriptor for the overall catalytic activity, the first electron and proton transfer OER intermediate from water, (M–OH*), has been associated with significant distortions of the metal–oxygen bonds upon charge-trapping. Time-resolved spectroscopy of in situ, photodriven OER on transition metal oxide surfaces has characterized M–OH* for the charge trapping and the symmetry of the lattice distortions by optical and vibrational transitions, respectively, but had yet to detect an interfacial strain field arising from a surface coverage M–OH*. Here, we utilize picosecond, coherent acoustic interferometry to detect the uniaxial strain normal to the SrTiO 3 /aqueous interface directly caused by Ti–OH*. The spectral analysis applies a fairly general methodology for detecting a combination of the spatial extent, magnitude, and generation time of the interfacial strain through the coherent oscillations’ phase. For lightly n-doped SrTiO 3 , we identify the strain generation time (1.31 ps), which occurs simultaneously with Ti–OH* formation, and a tensile strain of 0.06% (upper limit 0.6%). In addition to fully characterizing this intermediate across visible, mid-infrared, and now GHz-THz probes on SrTiO 3 , we show that strain fields occur with the creation of some M–OH*, which modifies design strategies for tuning catalytic activity and provides insight into photo-induced degradation so prevalent for OER. To that end, the work put forth here provides a unique methodology to characterize intermediate-induced interfacial strain across OER catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Rotational coherence dominates early-time dynamics and produces long-time revivals in the S 2 state of azulene

Here, the ultrafast dynamics of azulene have been debated for decades, with reported picosecond decay constants variously attributed to intramolecular vibrational redistribution (IVR), internal conversion, or rotational dephasing. Using polarization- and femtosecond time-resolved resonance-enhanced multiphoton ionization spectroscopy with a nanosecond delay window, we disentangle this long-standing inconsistency and show that the early 2–5 ps decay component arises entirely from the rotational dephasing of an excited-state wavepacket. Identical time constants extracted from the decay of the parallel signal and the rise of the perpendicular signal across multiple vibronic origins provide an unambiguous rotational anisotropy signature, eliminating the need for IVR-based interpretations. Extending the measurement window to 1.3 ns reveals well-structured J-type and C-type rotational coherence revivals in S 2 azulene on top of the well-documented fluorescence decay, demonstrating that both the short- and long-time dynamics contain information about the coherent rotational dynamics. These results show that azulene, and by extension polycyclic aromatic hydrocarbons, can sustain structured rotational coherence deep into the nanosecond regime, positioning PAHs as model systems for quantum-coherent wavepacket dynamics and providing a framework for probing coherence, decoherence, and rotational control in electronically rich molecular systems.

Zhan, Jie [University of Georgia, Athens, GA (Unit↗
DOE OSTI2024

A Bottom-Up Approach to Rational Design of Crystalline Materials: Investigation of Vibronic Coherences Underlying Exciton Dynamics in Semiconductors

In this project we uncovered structure-function relationships of donor-acceptor co-crystals used to develop next-generation optoelectronic devices. Unraveling the photodynamics of molecular crystalline materials poses many challenges for spectroscopy due to broad, overlapping features representing numerous underlying dynamical processes. This leads researchers to make many assumptions about the dynamics of a system in choosing an appropriate kinetic fitting model. Computationally, electronic structure methods are either prohibitively expensive or underdeveloped for computing the excited state structure of molecular materials, especially states that exhibit charge transfer. Researchers must therefore perform calculations of excited electronic states using truncated models of molecular materials. Here we present a joint experimental-theoretical approach to bridging the gap between the photodynamics of a molecular material and its constituent molecules. We focus our efforts on quantifying the timescales and mechanisms of photoexcitation in donor-acceptor co-crystals and donor-acceptor dimers where the lowest-lying excited state is characterized by charge transfer from the donor to the acceptor. We employ ultrafast UV pump, UV-Vis probe transient absorption spectroscopy to unravel the time-resolved spectroscopic signatures of the photodynamics in both the crystalline material and donor-acceptor dimers in solution. We perform electronic structure and excited state dynamics calculations of the dimers to inform kinetic fitting models and assign the spectral features. The photodynamics of the crystal vs. dimer systems have many similarities, enabling unprecedented insights into the formation and evolution of charge transfer excitons in the crystalline systems.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Stochastic modeling of x-ray superfluorescence

An approach to modeling the dynamics of x-ray amplified spontaneous emission and superfluorescence, the phenomenon of collective x-ray emission initiated by intense pulses of x-ray free-electron lasers, is developed based on stochastic partial differential equations. The equations are derived from first principles, and the relevant approximations, derivation steps, and extensions specific to stimulated x-ray emission are presented. The resulting equations take the form of three-dimensional generalized Maxwell-Bloch equations augmented with noise terms for both field and atomic variables. The derived noise terms possess specific correlation properties that enable the correct reconstruction of spontaneous emission. Consequently, the developed theoretical formalism is universally suitable for describing all stages of stimulated x-ray emission: spontaneous emission, amplified spontaneous emission, and superfluorescence. Here, we present numerical examples that illustrate various properties of the emitted field, including spatiotemporal coherence and spectral-angular and polarization characteristics. We anticipate that the proposed theoretical framework will establish a robust foundation for interpreting measurements in stimulated x-ray emission spectroscopy, modeling x-ray laser oscillators, and describing other experiments leveraging x-ray superfluorescence.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Ancilla-free continuous-variable SWAP test

We propose a continuous-variable (CV) SWAP test that requires no ancilla register, thereby generalizing the ancilla-free SWAP test for qubits. In this ancilla-free CV SWAP test, the computational basis measurement is replaced by photon number-resolving measurement, and we calculate an upper bound on the error of the overlap estimate obtained from a finite Fock cutoff in the detector. As an example, we show that estimation of the overlap of pure, centered, single-mode Gaussian states of energy E and squeezed in opposite quadratures can be obtained to error ϵ using photon statistics below a Fock basis cutoff O(Elnϵ –1 ). This cutoff is greatly reduced to E + O(√ Elnϵ –1 ) when the states have rapidly decaying Fock tails, such as coherent states. We show how the ancilla-free CV SWAP test can be extended to many modes and applied to quantum algorithms such as variational compiling and entanglement spectroscopy in the CV setting. For the latter we also provide a new algorithm which does not have an analog in qubit systems. The ancilla-free CV SWAP test is implemented on Xanadu's 8-mode photonic processor in order to estimate the vacuum probability of a two-mode squeezed state.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1980

New experimental possibilities and the future at far IR wavelengths

The observation of molecular phenomena in interstellar clouds through spectroscopy in the longer wavelength region of the infrared is discussed. This is a region where sensitivity is almost universally influenced by background continua; appropriate methods may be either coherent or incoherent, and work above most of the atmosphere is required for much of the spectral range. Thus far, only a very limited amount of molecular work has been done in the far-infrared, but rapid growth and important results are to be expected.

Townes, C. H.↗
DOE OSTI2025

Stretched exponential magnetic relaxation dynamics in artificial square ice revealed through x-ray photon correlation spectroscopy

X-ray photon correlation scattering measurements are undertaken on a thermally active artificial spin ice based on the square lattice, referred to as artificial square ice, to probe the fluctuation timescales as a function of temperature as the system passes through the paramagnetic-antiferromagnetic phase transition, which belongs to the two-dimensional Ising universality class. In the paramagnetic regime, a single exponential timescale is seen, whereas at and below the critical temperature, a stretched exponential decorrelation is observed, with the stretching exponent decreasing from unity down to below one-half as the temperature reduces. This trend is confirmed by kinetic Monte Carlo simulations of a simplified point-dipolar square ice system, and is in agreement with past theoretical work on the kinetic Ising model where stretched exponential relaxation due to equilibrium domain wall dynamics below the critical temperature was found.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Nearly degenerate two-color impulsive coherent Raman hyperspectral imaging

Impulsive stimulated Raman scattering (ISRS) is a robust technique for studying low frequency (<300 cm –1 ) Raman vibrational modes, but ISRS has faced difficulty in translation to an imaging modality. A primary challenge is the separation of the pump and probe pulses. Here we introduce and demonstrate a simple strategy for ISRS spectroscopy and hyperspectral imaging that uses complementary steep edge spectral filters to separate the probe beam detection from the pump and enables simple ISRS microscopy with a single-color ultrafast laser source. ISRS spectra are obtained that span from the fingerprint region down to <50 cm –1 vibrational modes. Furthermore, hyperspectral imaging and polarization-dependent Raman spectra are also demonstrated.

47 OTHER INSTRUMENTATION↗
DOE OSTI2025

Coupling of electronic transition to ferroelectric order in a 2D semiconductor

A ferroelectric material often exhibits a soft transverse optical (TO) phonon mode which governs its phase transition. Charge coupling to this ferroelectric soft mode may further mediate emergent physical properties, including superconductivity and defect tolerance in semiconductors. However, direct experimental evidence for such coupling is scarce. Here we show that a photogenerated coherent phonon couples strongly to the electronic transition above the bandgap in the van der Waals (vdW) two-dimensional (2D) ferroelectric semiconductor NbOI 2 . Using terahertz time-domain spectroscopy and first-principles calculations, we identify this mode as the TO phonon responsible for ferroelectric order. This exclusive coupling occurs only with the above-gap electronic transition and is absent in the valence band as revealed by resonant inelastic X-ray scattering. Our findings suggest a new role of the soft TO phonon mode in electronic and optical properties of ferroelectric semiconductors.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Single-hole physics in GaAs/AlGaAs double quantum dot system with strong spin–orbit interaction

There is rapidly expanding interest in exploiting the spin of valence-band holes rather than conduction-band electrons for spin qubit semiconductor circuits composed of coupled quantum dots. The hole platform offers stronger spin–orbit interaction (SOI), large difference between in-dot-plane and out-of-dot-plane g-factors, i.e. g-factor anisotropy, and a significantly reduced hyperfine coupling to nuclei in the host material. These attributes collectively can deliver fast all-electric coherent spin manipulation, efficient spin-flip inter-dot tunneling channels, a voltage tunable effective g-factor, a g-factor adjustable to nearly zero in an appropriately oriented external magnetic field, and long spin relaxation and coherence times. In this work, we review our recent work on the physics of heavy holes confined in a planar GaAs/AlGaAs double quantum dot system with strong SOI. For a single-hole, we have performed resonant tunneling magneto-spectroscopy to extract spin-flip and spin-conserving tunneling strengths, implemented spin-flip Landau–Zener–Stückelberg–Majorana (LZSM) interferometry, determined the spin relaxation time T 1 as a function of magnetic field using a fast single-shot latched charge technique, electrically tuned the effective g-factor revealed by electric dipole spin resonance, and found signatures of the hyperfine interaction and dynamic nuclear polarization with holes. For two-holes, we have measured the energy spectrum in the presence of strong SOI (and so not limited by Pauli spin blockade), quantified the heavy-hole (HH) g-factor anisotropy on tilting the magnetic field, described a scheme to employ HHs whose g-factor is tunable to nearly zero for an in-plane magnetic field for a coherent photon-to-spin interface, and observed a well-defined LZSM interference pattern at small magnetic fields on pulsing through the singlet-triplet anti-crossing.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Nonlinear time-domain spectroscopy near a band inversion

We develop a theory for the nonlinear time-domain response of a semimetal driven by an ultrafast optical pulse. At quadratic order in the driving field we find that the response near a band inversion transition contains a coherent oscillating component proportional to field intensity with a frequency that can be tuned over a wide range (from terahertz to the near IR) selected by the chemical potential. Finally, we illustrate the effect by calculating the induced current as a function of time for a two-band system with time-reversal symmetry but broken parity symmetry to study semimetals where large Berry curvature near a band inversion transition promotes this nonlinear response.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1976

Hyperfine spectroscopy using transverse modulated optical pumping

Population inversion is observed between the field-independent ground hyperfine states of Rb-87 when using an optical pumping technique which is applicable to a large number of species of atoms and ions. Inversion occurs upon a coherent transfer of angular momentum to the Rb-87 spin system from circularly polarized light propagating in a transverse direction to a magnetic field. Coherence is established by modulating, at certain frequencies, the light intensity or magnetic-field strength.

Hughes, W. M.↗
DOE OSTI2024

Ultrathin Magnesium-Based Coating as an Efficient Oxygen Barrier for Superconducting Circuit Materials

Scaling up superconducting quantum circuits based on transmon qubits necessitates substantial enhancements in qubit coherence time. Over recent years, tantalum (Ta) has emerged as a promising candidate for transmon qubits, surpassing conventional counterparts in terms of coherence time. However, amorphous surface Ta oxide layer may introduce dielectric loss, ultimately placing a limit on the coherence time. In this study, a novel approach for suppressing the formation of tantalum oxide using an ultrathin magnesium (Mg) capping layer is presented. Synchrotron-based X-ray photoelectron spectroscopy studies demonstrate that oxide is confined to an extremely thin region directly beneath the Mg/Ta interface. Additionally, it is demonstrated that the superconducting properties of thin Ta films are improved following the Mg capping, exhibiting sharper and higher-temperature transitions to superconductive and magnetically ordered states. Moreover, an atomic-scale mechanistic understanding of the role of the capping layer in protecting Ta from oxidation is established based on computational modeling. Further, this work provides valuable insights into the formation mechanism and functionality of surface tantalum oxide, as well as a new materials design principle with the potential to reduce dielectric loss in superconducting quantum materials. Ultimately, the findings pave the way for the realization of large-scale, high-performance quantum computing systems.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Hierarchical Phased-Array Antennas Coupled to Al KIDs: A Scalable Architecture for Multi-band Millimeter/Submillimeter Focal Planes

We present the optical characterization of two-scale hierarchical phased-array antenna kinetic inductance detectors (KIDs) for millimeter/submillimeter wavelengths. Our KIDs have a lumped-element architecture with parallel plate capacitors and aluminum inductors. The incoming light is received with a hierarchical phased array of slot dipole antennas, split into 4 frequency bands (between 125 GHz and 365 GHz) with on-chip lumped-element band-pass filters, and routed to different KIDs using microstriplines. Individual pixels detect light for the 3 higher-frequency bands (190–365 GHz), and the signals from four individual pixels are coherently summed to create a larger pixel detecting light for the lowest frequency band (125–175 GHz). The spectral response of the band-pass filters was measured using Fourier transform spectroscopy (FTS), the far-field beam pattern of the phased-array antennas was obtained using an infrared source mounted on a 2-axis translating stage, and the optical efficiency of the KIDs was characterized by observing loads at 294 K and 77 K. We report on the results of these three measurements.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Signatures of possible surface states in TaAs

In this work, we study Shubnikov-de Haas oscillations in single crystals of TaAs and find a previously undetected two-dimensional quantum oscillation that does not belong to the bulk Fermi surface. We cannot find an impurity phase consistent with our observations, and extensive diffraction measurements have not shown the presence of known impurity phases. We conjecture that the frequency originates from surface states that are sensitive to surface disorder. One candidate is the interference of coherent quasiparticles traversing two distinct Fermi arcs on the [001] crystallographic surface. The frequency and effective mass quantitatively agree with predictions of density functional theory and previous angle-resolved photoemission spectroscopy measurements of the Fermi arcs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗