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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Multidimensional four-wave-mixing spectroscopy with squeezed light

A set of nonlinear spectroscopic measurements with quantum light is presented here. It involves a strong pump with frequency ω pu and a weak probe atω pr interacting with a solid state target to generate a conjugated beam ω c =2ω pu -ω pr via nondegenerate four-wave mixing. The $\chi^{(3)}$ susceptibility can be measured by the noise spectra of the intensity difference of the squeezed beams. We discuss three spectroscopic setups based on squeezed light: first, single four-wave mixing in a single crystal; second, cascading scheme involving two crystals; third, an $\textit{SU}$(1, 1) interferometer based on two separate four-wave mixing processes. We further investigate the microscopic noise and optical losses in all three setups. Simulations are presented for silicon-vacancy color centers in diamond.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Spinon mediation of witness spin dynamics in herbertsmithite

The kagome lattice of spin-1/2 copper atoms in herbertsmithite is conjectured to sustain a quantum spin liquid state with spinon quasiparticles. Ideally, the kagome crystal planes are each separated by a plane of spinless zinc atoms. However, in real crystals, some spin-1/2 copper atoms substitute randomly onto these inter-kagome zinc sites. Here we reconceptualize such ‘impurity’ atoms as quantum witness spins whose dynamics is designed to probe the spin liquid state. We then introduce spin noise spectroscopy to measure the frequency and temperature dependence of witness spin dynamics, demonstrating that their phenomenology is consistent with extensive interactions between witness spins mediated by propagation of spinons through a quantum spin liquid. Ultimately, a sharp transition occurs at around 260 mK, below which the properties of both spin noise and magnetic susceptibility suggest that the witness spins form a spin glass phase. Among the theoretical models considered, we demonstrate that our observations are only consistent with spinon-mediated interactions between witness spins by either a Z 2 or U(1) quantum spin liquid, with the former model more closely matching the data. Our work demonstrates that quantum mechanical witness spins may now conceivably be used as a widely applicable probe of quantum spin liquid physics.

Takahashi, Hiroto [University of Oxford (United Ki↗
DOE OSTI2021

Clock transitions guard against spin decoherence in singlet fission

Short coherence times present a primary obstacle in quantum computing and sensing applications. In atomic systems, clock transitions (CTs), formed from avoided crossings in an applied Zeeman field, can substantially increase coherence times. We show how CTs can dampen intrinsic and extrinsic sources of quantum noise in molecules. Conical intersections between two periodic potentials form CTs in electron paramagnetic resonance experiments of the spin-polarized singlet fission photoproduct. We report on a pair of CTs for a two-chromophore molecule in terms of the Zeeman field strength, molecular orientation relative to the field, and molecular geometry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Squeezing Noise in Microscopy with Quantum Light

Quantum-enhanced microscopes capable of probing classically inaccessible material properties have drawn increasing interest, but most proof-of-principle quantum microscopes have not surpassed classical limits. Here, we discuss the promise and obstacles associated with the use of quantum light with reduced noise (‘squeezed’ light) for quantum-enhanced atomic force microscopy, bioimaging, magneto-optical measurements, and Raman spectroscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Quantum-enhanced Imaging and Spectroscopy and their Relevance to International Safeguards

As a follow-up to our previous report on quantum sensing for safeguards, here we delve deeper into quantum-enhanced imaging & spectroscopy and address their relevance to international safeguards. Much of the approaches rely on entangled photons, a quantum phenomenon not possible with classical physics, although just correlated photons will work for some applications, such as ghost imaging. We provide a comprehensive survey of quantum approaches, including multiple entangled photon ghost imaging and spectroscopy techniques. Entangled photons for noise reduction are also described, as well as Non-Line-Of-Sight imaging, compressive techniques, and squeezed light. Of particular interest is the generation of entangled photons with large wavelength separation, such as infrared/visible entangled photon pairs. Such entangled pairs would allow interaction with objects in the IR, such as in the molecular “fingerprint” wavelength region, while the recording device captures the visible photons, thus leveraging the high efficiency and lower cost of visible detectors. Unfortunately, entangled x-ray photons are not practical, which would have been useful for safeguards to interrogate shielded materials. Entangled gamma rays are even further beyond reason. We provide our assessment for application of quantum-enhanced imaging & spectroscopy for international safeguards, including suggested improvements to existing IAEA instruments and destructive assay measurements that are done at IAEA lab facilities.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1986

EUV astronomical spectroscopy with CCD detectors

The applicability of CCD detectors to astronomical extreme ultraviolet (EUV) spectroscopy (100-1250 A) is discussed. The advantages of CCDs in this spectral region include internal electron yield, the potential for very high quantum efficiency (about 50-90 percent), and broad wavelength response. Visible light suppression is achieved by a combination of low grating scattering, greater than unity electron yield in the EUV, and various filter techniques. For the current generation of CCDs, detection of only a few EUV photons will rapidly overwhelm the read noise; thus, for all practical S/N ratios used in astronomical spectroscopy, read noise will be negligible compared to the poisson statistics of the detected photons. A model based on experimental data for the quantum efficiency and electron yield of CCDs in the EUV is discussed.

Stern, R. A.↗
NASA NTRS1978

Infrared heterodyne spectroscopy for astronomical purposes

Heterodyne infrared astronomy was carried out using CO2 lasers and some solid state tunable lasers. The best available detectors are mercury cadmium telluride photodiodes. Their quantum efficiencies reach values near 0.5 and in an overall system an effective quantum efficiency, taking into account optical losses and amplifier noise, of about 0.25 was demonstrated. Initial uses of 10 micron heterodyne spectroscopy were for the study of planetary molecular spectra.

Townes, C. H.↗
DOE OSTI2020

Synchrotron infrared nano-spectroscopy and -imaging

Infrared (IR) spectroscopy has evolved into a powerful analytical technique to probe molecular and lattice vibrations, low-energy electronic excitations and correlations, and related collective surface plasmon, phonon, or other polaritonic resonances. In combination with scanning probe microscopy, near-field infrared nano-spectroscopy and -imaging techniques have recently emerged as a frontier in imaging science, enabling the study of complex heterogeneous materials with simultaneous nanoscale spatial resolution and chemical and quantum state spectroscopic specificity. Here, we describe synchrotron infrared nano-spectroscopy (SINS), which takes advantage of the low-noise, broadband, high spectral irradiance, and coherence of synchrotron infrared radiation for near-field infrared measurements across the mid- to far-infrared with nanometer spatial resolution. This powerful combination provides a qualitatively new form of broadband spatio-spectral analysis of nanoscale, mesoscale, and surface phenomena that were previously difficult to study with IR techniques, or even any form of micro-spectroscopy in general. We review the development of SINS, describe its technical implementations, and highlight selected examples representative of the rapidly growing range of applications in physics, chemistry, biology, materials science, geology, and atmospheric and space sciences.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

High signal-to-noise ratio differential conductance spectroscopy

The scanning tunneling microscope (STM) has enabled manipulation and interrogation of surfaces with atomic-scale resolution. Electronic information about a surface is obtained by combining the imaging capability of the STM with scanning tunneling spectroscopy, i.e., measurement of current-voltage (I/V) characteristics of the surface. We propose a change in the STM feedback loop that enables capturing a higher quality dI/dV image. A high frequency dither voltage is added to the bias voltage of the sample, and the fundamental frequency component of the resulting current is demodulated. The in-phase component of this signal is then plotted along with the X and Y position data, constructing the dI/dV image. Here, we show that by incorporating notch filters in the STM feedback loop, we may utilize a high-amplitude dither voltage to significantly improve the quality of the obtained dI/dV image.

42 ENGINEERING↗
NASA NTRS1986

Ultrasensitive detection of atmospheric trace gases using frequency modulation spectroscopy

Frequency modulation (FM) spectroscopy is a new technique that promises to significantly extend the state-of-the-art in point detection of atmospheric trace gases. FM spectroscopy is essentially a balanced bridge optical heterodyne approach in which a small optical absorption or dispersion from an atomic or molecular species of interest generates an easily detected radio frequency (RF) signal. This signal can be monitored using standard RF signal processing techniques and is, in principle, limited only by the shot noise generated in the photodetector by the laser source employed. The use of very high modulation frequencies which exceed the spectral width of the probed absorption line distinguishes this technique from the well-known derivative spectroscopy which makes use of low (kHz) modulation frequencies. FM spectroscopy was recently extended to the 10 micron infrared (IR) spectral region where numerous polyatomic molecules exhibit characteristic vibrational-rotational bands. In conjunction with tunable semiconductor diode lasers, the quantum-noise-limited sensitivity of the technique should allow for the detection of absorptions as small as .00000001 in the IR spectral region. This sensitivity would allow for the detection of H2O2 at concentrations as low as 1 pptv with an integration time of 10 seconds.

Cooper, David E.↗
NASA NTRS1980

Comparative performance of HgCdTe photodiodes for heterodyne application

The use of photodiodes as optical photomixers in laser heterodyne spectroscopy systems is discussed. The quantum efficiency of the photodiodes is reported with the emphasis on its effect on the system's signal to noise ratio. The measurement techniques used to determine photodiode dc and heterodyne quantum efficiencies are described. The theory behind the measurements as well as actual measurements data for two HgCdTe photodiodes are presented.

Kowitz, H. R.↗
DOE OSTI2021

DR-RINS: Digital real-time relative intensity noise suppressor for pump–probe spectroscopy and microscopy

Relative intensity noise (RIN) inherent in fiber lasers poses a serious obstacle to their use in pump–probe spectroscopy and imaging. RIN can be removed through an analog balanced detector, or, as we have previously shown, software adaptive noise cancellation (ANC) on digitized signals. One major drawback to software ANC is the added time required for digitizing and post-processing. In this article, we describe a design for ANC on a field-programmable gate array (FPGA), making use of high-level synthesis tools and fixed-point arithmetic to achieve real-time laser RIN suppression at 25 MHz sample rates. Unlike the software-ANC approach, the FPGA-ANC device can serve as a dedicated drop-in denoiser, placed between the detectors and a commercial lock-in amplifier. We demonstrate its application to transient absorption spectroscopy and microscopy, lowering the noise floor to ~17 dB above the shot noise limit. Furthermore, we demonstrate a dramatic improvement in data acquisition time from ~6 h to ~5 min in a real-time imaging scenario.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Time-Resolved Line Shapes of Single Quantum Emitters via Machine Learned Photon Correlations

Solid-state single-photon emitters (SPEs) are quantum light sources that combine atomlike optical properties with solid-state integration and fabrication capabilities. SPEs are hindered by spectral diffusion, where the emitter’s surrounding environment induces random energy fluctuations. Timescales of spectral diffusion span nanoseconds to minutes and require probing single emitters to remove ensemble averaging. Photon correlation Fourier spectroscopy (PCFS) can be used to measure time-resolved single emitter line shapes, but is hindered by poor signal-to-noise ratio in the measured correlation functions at early times due to low photon counts. Here, we develop a framework to simulate PCFS correlation functions directly from diffusing spectra that match well with experimental data for single colloidal quantum dots. We use these simulated datasets to train a deep ensemble autoencoder machine learning model that outputs accurate, noiseless, and probabilistic reconstructions of the noisy correlations. Using this model, we obtain reconstructed time-resolved single dot emission line shapes at timescales as low as 10 ns, which are otherwise completely obscured by noise. This enables PCFS to extract optical coherence times on the same timescales as Hong-Ou-Mandel two-photon interference, but with the advantage of providing spectral information in addition to estimates of photon indistinguishability. Further, our machine learning approach is broadly applicable to different photon correlation spectroscopy techniques and SPE systems, offering an enhanced tool for probing single emitter line shapes on previously inaccessible timescales.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Enhancing spectroscopy and microscopy with emerging methods in photon correlation and quantum illumination

Quantum optics has led to important advancements in our ability to prepare and detect correlations between individual photons. Its principles are increasingly translated into nanoscale characterization tools, furthering methods in spectroscopy, microscopy and metrology. Here, in this Review, we discuss the rapid progress in this field driven by advanced technologies of single-photon detectors and quantum-light sources, including time-resolved single-photon counting cameras, superconducting nanowire single-photon detectors and entangled photon sources of increasing brightness. We emphasize emerging applications in super-resolution microscopy, measurements below classical noise limits and photon-number-resolved spectroscopy—a powerful paradigm for the characterization of nanoscale electronic materials. We conclude by discussing key technological challenges and future opportunities in materials science and bionanophotonics alike.

Tsao, Chieh [University of California, Berkeley, C↗
DOE OSTI2023

Single-photon detection using high-temperature cuprate superconductors

The detection of individual quanta of light is important for quantum computation, fluorescence lifetime imaging, single-molecule detection, remote sensing, correlation spectroscopy, and more. Thanks to their broadband operation, high detection efficiency, exceptional signal-to-noise ratio, and fast recovery times, superconducting nanowire single-photon detectors (SNSPDs) have become a critical component in these applications. The operation of SNSPDs based on conventional superconductors, which have a low critical temperature (T c ), requires costly and bulky cryocoolers. This motivated exploration of other superconducting materials with higher T c that would enable single-photon detection at elevated temperatures, yet this task has proven exceedingly difficult. Here we show that with proper processing, high-T c cuprate superconductors can meet this challenge. We fabricated superconducting nanowires (SNWs) out of thin flakes of Bi 2 Sr 2 CaCu2O 8+δ and La 1.55 Sr 0.45 CuO 4 /La 2 CuO 4 (LSCO-LCO) bilayer films and demonstrated their single-photon response up to 25 and 8 K, respectively. The single-photon operation is revealed through the linear scaling of the photon count rate (PCR) on the radiation power. Both of our cuprate-based SNSPDs exhibited single-photon sensitivity at the technologically-important 1.5 μm telecommunications wavelength. Our work expands the family of superconducting materials for SNSPD technology, opens the prospects of raising the temperature ceiling, and raises important questions about the underlying mechanisms of single-photon detection by unconventional superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Response of CR-39 nuclear track detectors to protons with non-normal incidence

This paper presents data from experiments with protons at non-normal incidence to CR-39 nuclear track detectors, analyzing the properties of detection efficiency, proton track diameter, track contrast, and track eccentricity. Understanding the CR-39 response to protons incident at an angle is important for designing charged particle detectors for inertial confinement fusion (ICF) applications. This study considers protons with incident energies less than 3 MeV. In this regime, an incident angle of 10° has no effect on CR-39 detection efficiency, and >85% detection efficiency is preserved up through 25° in the range of 1.0 MeV–2.1 MeV. For ICF applications, incident angles above 30° are deemed impractical for detector design due to significant drops in proton detection at all energies. We observe significant reductions in detection efficiency compared to theoretical predictions, particularly at low energies where proton tracks are etched away. The proton track diameter measured by the scan system is observed to decrease with higher incident angles. The track diameters are analyzed with two fitting models, and it is shown that the diameter–energy relation can be fit with the existing models at angles up to 30° . The optical contrast of the tracks tends to increase with the angle, meaning that the tracks are fainter, and a larger increase is observed for higher energies. Eccentricity, a measure of how elongated proton tracks are, increases with the incident angle and drops after the critical angle. The lowest energy tracks remain nearly circular even at higher angles.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Excited-state uncertainties in lattice-QCD calculations of multi-hadron systems

Excited-state effects lead to hard-to-quantify systematic uncertainties in lattice quantum chromodynamics (LQCD) spectroscopy calculations when computationally accessible imaginary times are smaller than inverse excitation gaps, as often arises for multi-hadron systems with signal-to-noise problems. Lanczos residual bounds address this by providing two-sided constraints on energies that do not require assumptions beyond Hermiticity, but often give very conservative systematic uncertainty estimates. Here, a more-constraining set of gap bounds is introduced for hadron spectroscopy. These bounds provide tighter constraints whose validity requires an explicit assumption about an energy gap. Exactly solvable lattice field theory correlators are used to test the utility of residual and gap bounds at finite and infinite statistics. Two-sided bounds and other analysis methods are then applied to a high-statistics LQCD calculation of nucleon-nucleon scattering at $m_π\sim 800$ MeV. Generalized eigenvalue problem (GEVP) and Lanczos energy estimators are compatible when applied to the same correlator data, but analyses including different interpolating operators show statistically significant inconsistencies. However, two-sided bounds from all operators are consistent. Under the assumption that the number of energy levels below $NΔ$ and $ΔΔ$ thresholds is the same as for non-interacting nucleons, gap bounds are sufficient to constrain nucleon-nucleon scattering amplitudes at phenomenologically relevant precision. Lanczos methods further reveal that energy-eigenstate estimates from previously studied asymmetric correlators have not converged over accessible imaginary times. Nevertheless, data-driven examples demonstrate why assumptions are required to draw conclusions about the natures of two-nucleon ground states at these masses.

Detmold, William [MIT, Cambridge, CTP]↗
NASA NTRS2006

InGaAsSb/AlGaAsSb Heterojunction Phototransistors for Infrared Applications

High quality infrared (IR) quantum detectors are important for several applications, such as atmospheric remote sensing, chemical detection and absorption spectroscopy. Although several IR detectors are commercially available, with different materials and structures, they provide limited performance regarding the signal-to-noise ratio and the corresponding minimum detectable signal. InGaAsSb/AlGaAsSb heterojunction based phototransistors show strong potential for developing IR sensors with improved performance. In this paper, the performance of a novel npn InGaAsSb/AlGaAsSb heterojunction phototransistor is presented. This performance study is based on experimental characterization of the device dark current, noise and spectral response. Detectivity of 1.7x10(exp 9) cmHz(exp 1/2)/W at 2 microns was obtained at 100 C temperature and 2 V bias voltage. This corresponds to a responsivity of 94.7 A/W and an internal gain of 156 with about 37.7% quantum efficiency. Reducing the temperature to -30 C allows to increase the bias to 3V and enhance the detectivity to 8.7x10(exp 10) cmHz(exp 1/2)/W at the same wavelength, which corresponds to a responsivity of 386.5 A/W and an internal gain of 288.2 with about 83.3% quantum efficiency. The device impulse response and linearity, including the corresponding dynamic range, also are presented. Impulse response analysis indicated a settling time of about 1.1 s at 2V and 100 C, while linearity measurements indicated a constant responsivity in the radiation intensity range of 1.6x10(exp -7) W/sq cm and 31.6 mW/sq cm.

Refaat, Tamer F.↗