Search NASA⌕ Search

SEARCH · Search NASA

Results for “two photon absorption”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 145 records · Page 8

Advances in High Resolution Ultrafast Scintillators for Fast timing Applications

Scintillation detectors exhibiting high spatial resolution and fast timing capabilities are of vital importance for synchrotron sources. These detectors may be exposed to a variety of X-ray energies (up to 140 keV) and used in high frame rate applications. Here, we describe the advances in the development of thin-film LuI3:Ce scintillators for higher energy X-ray imaging, with fast timing and high spatial resolution. When grown in a single crystalline form, these scintillators are bright, producing 115 000 photons/MeV. However, to achieve high spatial resolution, these scintillators are grown in thin-film form with a microcolumnar structure, controllable to column diameters of <1-30 mu m. Thus, a much thicker scintillator layer (10 mu m-3 mm or higher) may be grown, providing superior X-ray absorption while achieving high resolutions of 50 mu m or better, at the cost of reduced light yield. To study the timing characteristics of the scintillator, time-resolved X-ray excited optical luminescence (TR-XEOL) was performed on two different sets of three samples of LuI3 at the 1-BM beamline of the Advanced Photon Source at Argonne National Laboratory. Besides, we report timing measurements obtained using a photomultiplier tube (PMT) and oscilloscope at Radiation Monitoring Devices (RMD) Inc. Using the TR-XEOL, we determined the decay constants of LuI3 as a function of Ce doping, recording a fast decay component as low as 3.6 ns (39%), one of the fastest values recorded in inorganic scintillators. This fast decay opens up numerous novel applications, where ultrahigh frame rates are important using synchrotron X-rays. This article will discuss fabrication, characterization, and potential applications for this novel scintillator.

fast timing↗

Hong-Ou-Mandel interference of single-photon-level pulses stored in independent room-temperature quantum memories

Abstract Quantum repeater networks require independent absorptive quantum memories capable of storing and retrieving indistinguishable photons to perform high-repetition entanglement swapping operations. The ability to perform these coherent operations at room temperature is of prime importance for the realization of scalable quantum networks. We perform Hong-Ou-Mandel (HOM) interference between photonic polarization states and single-photon-level pulses stored and retrieved from two sets of independent room-temperature quantum memories. We show that the storage and retrieval of polarization states from quantum memories does not degrade the HOM visibility for few-photon-level polarization states in a dual-rail configuration. For single-photon-level pulses, we measure the HOM visibility with various levels of background in a single polarization, single-rail QM, and investigate its dependence on the signal-to-background ratio. We obtain an HOM visibility of 43%, compared to the 48% no-memory limit of our set-up. These results allow us to estimate a 33% visibility for polarization qubits under the same conditions. These demonstrations lay the groundwork for future applications using large-scale memory-assisted quantum networks.

Physics↗

Bifacial all-perovskite tandem solar cells

The efficiency of all-perovskite tandem devices falls far below theoretical efficiency limits, mainly because a widening bandgap fails to increase open-circuit voltage. We report on a bifacial all-perovskite tandem structures with an equivalent efficiency of 29.3% under back-to-front irradiance ratio of 30. This increases energy yield and reduces the required bandgap of a wide-bandgap cell. Open-circuit voltage deficit is therefore minimized, although its performance under only front irradiance is not ideal. The bifacial device needs a sputtered rear transparent electrode, which could reduce photon path length and deteriorate stability of Pb-Sn perovskites. Embedding a light-scattering micrometer-sized particle layer into perovskite to trap light, effectively increases absorptance by 5 to 15% in the infrared region. Using a nonacidic hole transport layer markedly stabilizes the hole-extraction interface by avoiding proton-accelerated formation of iodine. These two strategies together increase efficiency of semitransparent Pb-Sn cells from 15.6 to 19.4%, enabling fabrication of efficient bifacial all-perovskite tandem devices.

14 SOLAR ENERGY↗

Spectroscopy and dynamics of the v = 1 levels derived from the OH(D) stretching modes in the I‾∙HDO complex using CW and time-resolved, resonant two-photon infrared excitation of the cryogenically cooled ions

The vibrational energy levels of the two isotopomers adopted by the I‾∙HDO ion-molecule complex occur such that the OH(D) stretching fundamentals span its dissociation energy, thus enabling a spectroscopic investigation of the dynamics displayed by a system prepared in the vicinity of the dissociation threshold. This regime is explored using infrared photoexcitation of the mass-selected complexes cooled in a cryogenic radiofrequency (Paul) ion trap. Survey spectra are obtained at modest resolution using two-color, IR-IR photodissociation with nanosecond lasers to establish the level structure and unimolecular decay dynamics of the v = 1 and 2 levels of the bound OH(D) oscillator. The v = 1 levels are prepared by fixed frequency excitation in the trap and the absorption spectra arising from this excited state are probed by photofragmentation of the complex with a second pulsed IR laser after a variable delay time (0 to 20 ms). The transitions to levels above the dissociation threshold for I‾ + HDO formation are observed to be sharp (~5 cm -1 FWHM). At low pressure, the bound OD (v = 1) population relaxes very slowly (~3 ms), consistent with resonant fluorescence in the IR. The collisional quenching rate constants of this level by the He buffer gas were estimated to be on the order 3 x 10 -12 cm 3 /s based on a crude Stern-Volmer analysis. Here, the rotational fine structure and linewidths (≲0.01 cm -1 FWHM) arising from transitions of the non-bonded OH stretch fundamental of the OD-bound isotopomer that lies just above the dissociation energy are determined using single photon photodissociation by excitation of the 10 K ions with a single-frequency, CW IR laser in the ion trap.

Cryogenic ion infrared spectroscopy↗

Imaging the magnetic nanowire cross section and magnetic ordering within a suspended 3D artificial spin-ice

Artificial spin-ice systems are patterned arrays of magnetic nanoislands arranged into frustrated geometries and provide insight into the physics of ordering and emergence. The majority of these systems have been realized in two-dimensions, mainly due to the ease of fabrication, but with recent developments in advanced nanolithography, three-dimensional artificial spin ice (ASI) structures have become possible, providing a new paradigm in their study. Such artificially engineered 3D systems provide new opportunities in realizing tunable ground states, new domain wall topologies, monopole propagation, and advanced device concepts, such as magnetic racetrack memory. Direct imaging of 3DASI structures with magnetic force microscopy has thus far been key to probing the physics of these systems but is limited in both the depth of measurement and resolution, ultimately restricting measurement to the uppermost layers of the system. In this work, a method is developed to fabricate 3DASI lattices over an aperture using two-photon lithography, thermal evaporation, and oxygen plasma exposure, allowing the probe of element-specific structural and magnetic information using soft x-ray microscopy with x-ray magnetic circular dichroism (XMCD) as magnetic contrast. The suspended polymer–permalloy lattices are found to be stable under repeated soft x-ray exposure. Analysis of the x-ray absorption signal allows the complex cross section of the magnetic nanowires to be reconstructed and demonstrates a crescent-shaped geometry. Measurement of the XMCD images after the application of an in-plane field suggests a decrease in magnetic moment on the lattice surface due to oxidation, while a measurable signal is retained on sub-lattices below the surface.

36 MATERIALS SCIENCE↗

Cumulative short-lived photofission product yields for nuclear forensic application

Experiments have long been carried out with linear accelerator (linac) produced bremsstrahlung X-rays to study high-energy photon-induced fission, known as “photofission”. One benefit of photofission, when compared with neutron-induced fission, is the ability to investigate fundamental physics of fission at excitation energies lower than what is possible with neutrons [1]. Absorption of an incident neutron results in a compound nucleus with an excitation energy at least equal to the neutron binding energy; thus, the lowest energy region of the fission barrier cannot be studied. Fission product yield distributions are dependent on the incident particle energy and the target nucleus mass. They are generally represented by a double-humped curve, with low and high mass “peaks” and an intermediate mass “valley”. As incident particle energy increases, the excitation energy of the nucleus increases, thereby increasing the overall yield of isotopes in the valley with respect to the two maxima or peaks of the fission product curve [3]. Photofission is most probable for incident photons around 14 MeV due to the giant dipole resonance. Induced photofission around this energy results in a fission product yield distribution that resembles 14 MeV DT neutron fission more than thermal or fast (500 keV) neutron fission. In post-detonation nuclear forensics, the peak-to-valley ratio of the fission product yield curve could be used for characterizing device type by providing an indication of the neutron energy spectrum that had induced fission (e.g., 500 keV vs. 14 MeV). The goal of this work is to improve nuclear data for isotopes of interest in nuclear forensics and special nuclear material (SNM) detection, specifically the fission product yield data via photofission experiments for the isotopes of 238U and 232Th. Photofission has been proposed as a less costly and more flexible production method for the valley isotopes that are representative of DT neutron fission product yield distributions, which would benefit nuclear forensics exercises in testing for analysis techniques. Natural uranium and thorium targets were irradiated with bremsstrahlung photons (nominal endpoint energies of 8, 14, and 20 MeV), generated via impingement of high-energy electrons on a tungsten electron-to-photon radiator. Gamma-ray spectroscopy was used to observe and identify the decay of the resulting fission products. The photofission yields of 102 fission products were measured for the set of the 238U and 232Th targets at the three bremsstrahlung X-ray endpoint energies 8, 14, and 20 MeV. These fragments included masses ranging from A=84 to A=144, with half-lives as short as 1.07 seconds.

07 ISOTOPE AND RADIATION SOURCES↗

Bragg-Primakoff axion photoconversion in crystal detectors

Abstract Axions and axion-like pseudoscalar particles with dimension-5 couplings to photons exhibit coherent Primakoff scattering with ordered crystals at keV energy scales, making for a natural detection technique in searches for solar axions. We find that there are large suppressive corrections, potentially greater than a factor of$$ \mathcal{O} $$ O (10 3 ), to the coherent enhancement when taking into account absorption of the final state photon. This effect has already been accounted for in light-shining-through-wall experiments through the language of Darwin classical diffraction, but is missing from the literature in the context of solar axion searches that use a matrix element approach. We extend the treatment of the event rate with a heuristic description of absorption effects to bridge the gap between these two languages. Furthermore, we explore the Borrmann effect of anomalous absorption in lifting some of the event rate suppression by increasing the coherence length of the conversion. We study this phenomenon in Ge, NaI, and CsI crystal experiments and its impact on the projected sensitivities of SuperCDMS, LEGEND, and SABRE to the solar axion parameter space. Lastly, we comment on the reach of multi-tonne scale crystal detectors and strategies to maximize the discovery potential of experimental efforts in this vein.

Physics↗

Pathways to excitation of atoms with bicircular laser pulses

We study the excitation of the hydrogen atom by bichromatic circularly polarized laser pulses using numerical solutions of the time-dependent Schrödinger equation. The results are in agreement with the selection rules for multiphoton processes in such fields, namely, excited states are populated in which orbital angular momentum and magnetic quantum numbers are either both odd or both even, independent of the relative helicity, peak intensity, and pulse duration of the pulses. For co-rotating pulses the results show that excitation predominantly proceeds to states with magnetic quantum number of the same helicity as the laser pulses. Besides pathways via direct photon absorption from the ground state our results indicate that a transfer of population among the Rydberg states occurs via Λ-type transitions. In the case of counter-rotating pulses the largest excitation probability is found for Rydberg states that differ in magnetic quantum number by Δm=±3. This pattern allows us to estimate how many photons from each of the two bichromatic fields have been absorbed. Finally, we confirm that a population in Rydberg states beyond a maximum orbital angular quantum number is unlikely.

74 ATOMIC AND MOLECULAR PHYSICS↗

Plasmonic Terahertz Devices and Sensors Based on Carbon Electronics

Tunable terahertz (THz) photonic devices are imperative in a wide range of applications ranging from THz signal modulation to molecular sensing. One of the currently prevailing methods is based on arrays of metallic or dielectric resonators integrated with functional materials in response to an external stimulus, in which for the purpose of sensing the external stimuli may introduce inadvertent undesirable effects into the target samples to be measured. Here we developed an alternative approach by postprocessing nanothickness macro-assembled graphene (nMAG) films with widely tunable THz conductivity, enabling versatile solid-state THz devices and sensors, showing multifunctional nMAG-based applications. The THz conductivities of free-standing nMAGs showed a broad range from 1.2 x 10 3 S/m in reduced graphene oxide before annealing to 4.0 x 10 6 S/m in a nMAG film annealed at 2800 °C. We fabricated nMAG/dielectric/metal and nMAG/dielectric/nMAG THz Salisbury absorbers with broad reflectance ranging from 0% to 80%. The highly conductive nMAG films enabled THz metasurfaces for sensing applications. Taking advantage of the resonant field enhancement arising from the plasmonic metasurface structures and the strong interactions between analyte molecules and nMAG films, we have successfully detected diphenylamine with a limit of detection of 4.2 pg. Those wafer-scale nMAG films present promising potential in high-performance THz electronics, photonics, and sensors.

36 MATERIALS SCIENCE↗

Contributions to the optical linewidth of shallow donor-bound excitonic transition in ZnO

Neutral shallow donors in zinc oxide (ZnO) are spin qubits with optical access via the donor-bound exciton. This spin–photon interface enables applications in quantum networking, memories, and transduction. Essential optical parameters which impact the spin–photon interface include radiative lifetime, optical inhomogeneous and homogeneous linewidth, and optical depth. We study the donor-bound exciton optical linewidth properties of Al, Ga, and In donors in single-crystal ZnO. The ensemble photoluminescence linewidth ranges from 4 to 11 GHz, less than two orders of magnitude larger than the expected lifetime-limited linewidth. The ensemble linewidth remains narrow in absorption through samples with an estimated optical depth up to several hundred. The primary thermal relaxation mechanism is identified and found to have a negligible contribution to the total linewidth at 2 K. We find that inhomogeneous broadening due to the disordered isotopic environment in natural ZnO is significant, contributing 2 GHz. Two-laser spectral hole burning measurements indicate that the dominant mechanism, however, is homogeneous. Despite this broadening, the high homogeneity, large optical depth, and potential for isotope purification indicate that the optical properties of the ZnO donor-bound exciton are promising for a wide range of quantum technologies, and motivate a need to improve the isotope and chemical purity of ZnO for quantum technologies.

Niaouris, Vasileios (ORCID:000000015313748X)↗

Phonon linewidths in InAs/AlSb superlattices derived from first-principles—application towards quantum well hot carrier solar cells

Hot electrons generated by the absorption of high-energy photons typically thermalize by dissipating energy through phonon mediated relaxation pathways. Existence of non-equilibrium optical phonon populations (hot phonons) can suppress thermalization of electrons by facilitating a stable hot carrier population. In this work, we derive optical phonon scattering rates in InAs/AlSb superlattices using first-principles calculations and compare them with bulk InAs. Computations are performed for the two shortest period superlattices with equal widths of InAs and AlSb. While in pure InAs, the highest optical phonon scattering rates reach 5 cm -1 ; in the superlattice, the peak scattering rates of optical phonons with frequencies above the energy gap, are much smaller, reaching ~1 cm -1 . Finally, these lower scattering rates in the superlattice have important implications for design of high efficiency hot carrier solar cells and explain some of the robust hot carriers observed recently in InAs/AlAsSb quantum wells.

14 SOLAR ENERGY↗

Simulating 50 keV X-ray Photon Detection in Silicon with a Down-Conversion Layer

Simulation results are presented that explore an innovative, new design for X-ray detection in the 20–50 keV range that is an alternative to traditional direct and indirect detection methods. Typical indirect detection using a scintillator must trade-off between absorption efficiency and spatial resolution. With a high-Z layer that down-converts incident photons on top of a silicon detector, this design has increased absorption efficiency without sacrificing spatial resolution. Simulation results elucidate the relationship between the thickness of each layer and the number of photoelectrons generated. Further, the physics behind the production of electron-hole pairs in the silicon layer is studied via a second model to shed more light on the detector’s functionality. Together, the two models provide a greater understanding of this detector and reveal the potential of this novel form of X-ray detection.

47 OTHER INSTRUMENTATION↗

Density Functional Theory Study of Controllable Optical Absorptions and Magneto-Optical Properties of Magnetic CrI 3 Nanoribbons: Implications for Compact 2D Magnetic Devices

A chromium triiodide (CrI 3 ) monolayer has an interesting ferromagnetic ground-state. In this work, we calculate band structures and magnetic moments of tensile-strained and bent zigzag CrI 3 nanoribbons with density functional theory. The edge iodine atoms form flat low-lying conduction bands and couple with chromium atoms ferromagnetically, while the non-edge iodine atoms weakly couple antiferromagnetically. Narrow CrI 3 nanoribbons have two locally stable magnetic moment orientations, namely out-of-plane and in-plane (along the nanoribbon periodic direction) configurations. This enables four magnetization states in CrI 3 nanoribbons, including two out-of-plane ones (up and down) and two in-plane ones (forward and backward along the nanoribbon periodical direction), increasing the operating controllability. Based on the one-dimensional Ising spin chain model, the spin correlation length of the narrow CrI 3 nanoribbon is estimated as about 10 Å at its estimated Curie temperature of 27 Kelvin, which is lower than the measured 45 Kelvin of the monolayer CrI 3 . The optical absorption and magneto-optical properties of CrI 3 nanoribbons are investigated with many-body perturbation GW-BSE (Bethe-Salpeter equation), including magnetic dichroism, Faraday and magneto-optical Kerr effects. Here, the low-energy dark excitons are mainly from transitions between electrons and holes with unlike spins and are non-Frenkel-like, while the bright excitons have mixed spin configurations. The intrinsic lifetime of excitons can be over one nanosecond, suitable for quantum information processes. Tensile strains and bending manifestly modulate the absorption spectra and magneto-optical properties of CrI 3 nanoribbons within a technologically important photon energy-range of ~1.0-2.0 eV. The CrI 3 nanoribbons can be used in 1D or 2D magnetic storage nanodevices, tunable magnetic optoelectronics, and spin-based quantum information controls.

36 MATERIALS SCIENCE↗

Near-field photonic thermal diode based on hBN and InSb films

A thermal diode is a two-terminal device that allows heat to transfer more easily in one direction (forward bias) than in the opposite direction (reverse bias). A photonic thermal diode operates in a contactless mode and may afford a large operating temperature range. Here, a near-field photonic thermal diode based on hexagonal boron nitride (hBN) and indium antimonide (InSb) films is theoretically demonstrated. In this work, the temperature dependence of the interband absorption of InSb is used to couple (or decouple) with the hyperbolic phonon polaritons in hBN. The numerical analysis predicts a rectification ratio greater than 17 for a 10 nm vacuum gap, when operating at an average temperature of 300 K and a temperature difference of 200 K. The calculated rectification ratio exceeds 35 at higher average temperatures with larger temperature differences.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Spin photovoltaic effect in magnetic van der Waals heterostructures

The development of van der Waals (vdW) crystals and their heterostructures has created a fascinating platform for exploring optoelectronic properties in the two-dimensional (2D) limit. With the recent discovery of 2D magnets, the control of the spin degree of freedom can be integrated to realize 2D spin-optoelectronics. Here, we report spin photovoltaic effects in vdW heterostructures of 2D magnet chromium triiodide (CrI 3 ) sandwiched by graphene contacts. The photocurrent displays a distinct dependence on light helicity, which can be tuned by varying the magnetic states and photon energy. Circular polarization–resolved absorption measurements reveal that these observations originate from magnetic order–coupled and, thus, helicity-dependent charge-transfer excitons. The photocurrent displays multiple plateaus as the magnetic field is swept, associated with different CrI 3 spin configurations. Giant photo-magnetocurrent is observed, which tends to infinity for a small applied bias. Our results pave the way to explore emergent photospintronics by engineering magnetic vdW heterostructures.

36 MATERIALS SCIENCE↗

Photochemistry sample sticks for inelastic neutron scattering

Every material experiences atomic and molecular motions that are generally termed vibrations in gases and liquids or phonons in solid state materials. Optical spectroscopy techniques, such as Raman, infrared absorption spectroscopy, or inelastic neutron scattering (INS), can be used to measure the vibrational/phonon spectrum of ground state materials properties. A variety of optical pump probe spectroscopies enable the measurement of excited states or elucidate photochemical reaction pathways and kinetics. So far, it has not been possible to study photoactive materials or processes in situ using INS due to the mismatch between neutron and photon penetration depths, differences between the flux density of photons and neutrons, cryogenic temperatures for INS measurements, vacuum conditions, and a lack of optical access to the sample space. These experimental hurdles have resulted in very limited photochemistry studies using INS. Here we report on the design of two different photochemistry sample sticks that overcome these experimental hurdles to enable in situ photochemical studies using INS, specifically at the VISION instrument at Oak Ridge National Laboratory. We demonstrate the use of these new measurement capabilities through (1) the in situ photodimerization of anthracene and (2) the in situ photopolymerization of a 405 nm photoresin using 405 nm excitation as simple test cases. Furthermore, these new measurement apparatus broaden the science enabled by INS to include photoactive materials, optically excited states, and photoinitiated reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dispersion-Engineered Deep Sub-Wavelength Plasmonic Metasurfaces for Broadband Seira Applications

Surface enhanced infrared absorption (SEIRA) spectroscopy is a powerful tool in which plasmonically enhanced electromagnetic fields provide high-sensitivity molecular detection. Most SEIRA platforms operate at a single resonant frequency, which must be tuned to match that of the target molecule, and commonly rely on time-consuming lithographic techniques. This study presents a high-throughput and cost-effective plasmonic metasurface for broadband, tunable, and strong infrared signal enhancement. The platform is built upon the principle of dispersion-engineered plasmonic Fabry–Pérot (FP) nanocavity arrays. It offers 1) tight squeezing of infrared (IR) photons into deep sub-wavelength nano-volumes and 2) spectrally tunable near-field enhancements of up to ≈10 6 , two to three orders of magnitude higher than most optical metasurface systems. By coupling multilayer nano-thin film deposition and nanoskiving fabrication techniques, the dispersive FP metasurfaces can be rapidly and reproducibly constructed in a scalable and lithography-free manner. Using IR spectroscopy, the selective and sensitive label-free detection of a molecular monolayer is achieved at a range of frequencies. An enhancement factor of nearly 10 5 is measured at the carbonyl (C = O) vibrational marker band of the molecule. The confluence of high field enhancement, broadband plasmonic response, and facile fabrication makes this metasurface a promising platform for SEIRA spectroscopy.

36 MATERIALS SCIENCE↗

MicroPulse DIAL (MPD) – a diode-laser-based lidar architecture for quantitative atmospheric profiling

Abstract. Continuous water vapor and temperature profiles are critically needed for improved understanding of the lower atmosphere and potential advances in weather forecasting skill. Ground-based, national-scale profiling networks are part of a suite of instruments to provide such observations; however, the technological method must be cost-effective and quantitative. We have been developing an active remote sensing technology based on a diode-laser-based lidar technology to address this observational need. Narrowband, high-spectral-fidelity diode lasers enable accurate and calibration-free measurements requiring a minimal set of assumptions based on direct absorption (Beer–Lambert law) and a ratio of two signals. These well-proven quantitative methods are known as differential absorption lidar (DIAL) and high-spectral-resolution lidar (HSRL). This diode-laser-based architecture, characterized by less powerful laser transmitters than those historically used for atmospheric studies, can be made eye-safe and robust. Nevertheless, it also requires solar background suppression techniques such as narrow-field-of-view receivers with an ultra-narrow bandpass to observe individual photons backscattered from the atmosphere. We discuss this diode-laser-based lidar architecture's latest generation and analyze how it addresses a national-scale profiling network's need to provide continuous thermodynamic observations. The work presented focuses on general architecture changes that pertain to both the water vapor and the temperature profiling capabilities of the MicroPulse DIAL (MPD). However, the specific subcomponent testing and instrument validation presented are for the water vapor measurements only. A fiber-coupled seed laser transmitter optimization is performed and shown to meet all of the requirements for the DIAL technique. Further improvements – such as a fiber-coupled near-range receiver, the ability to perform quality control via automatic receiver scanning, advanced multi-channel scalar capabilities, and advanced processing techniques – are discussed. These new developments increase narrowband DIAL technology readiness and are shown to allow higher-quality water vapor measurements closer to the surface via preliminary intercomparisons within the MPD network itself and with radiosondes.

Spuler, Scott M.↗