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DOE OSTI2023

Imaging Nanoscale Energy Transport and Conversion with Ultrafast Electron Microscopy (Final Technical Report)

Light-matter interactions are ubiquitous in nature and reside at the heart of innumerable technologies. The cascade of processes that occur when a material absorbs a photon of light are exceedingly complex and are interwoven in both space and time, rendering precise determination of the atomic-scale and ultrafast mechanisms immensely challenging. The advent of methods for generating short pulses of light several decades ago led to major advances in understanding the initial moments of light absorption and the resultant effects, though directly interrogating the response of the atoms within the material continued to prove challenging. More recently, methods for generating ultrashort pulses of X-rays and fast electrons have opened the way to probing photoinduced structural dynamics of a wide range of matter in multiple phases. An especially promising laboratory-scale method is ultrafast electron microscopy (UEM), wherein the modalities of conventional transmission electron microscopes (imaging, diffraction, spectroscopy) are extended into the femtosecond temporal regime. Here, the ultrafast imaging and diffraction modalities of UEM were used to study the transient structural aspects of photoexcitation of semiconducting materials (e.g., spatially-resolved electron-phonon coupling, excitation and emission of acoustic phonons, and discrete nanoscale scattering processes). The project had three main objectives: (1) determination of the excitation mechanisms of dense, hypersonic charge-carrier waves and the spatially mediated means by which they couple to the lattice via coherent phonon emission, especially with UEM imaging, wherein effects of nanoscale structural and morphological features on the coupling and relaxation dynamics are expected to dictate nucleation sites and preferred wave vectors, (2) elucidation of photoinduced acoustic-phonon seeding, emergence, propagation, and decay over nanoscale crystal regions and especially with respect to local strain fields and atomic-scale disruptions in lattice order, and (3) interwoven with the first two were efforts aimed at realizing combined angstrom-femtosecond spatiotemporal imaging with UEM. The outcomes and impacts of this project were the generation of new knowledge with respect to fundamental light-matter interactions and, especially, the spatially-mediated excitation and evolution of the structural response of materials following coherent photoexcitation. Importantly, the spatial and temporal resolutions of the UEM imaging modalities used are well-suited for such studies and enable spatially-resolved mechanisms to be determined as a function of atomic order, structural features, and morphology. In addition, ultrafast crystallographic measurements were used to correlate real- and reciprocal-space dynamics in order to determine atomic-scale preferential wave vectors and ultrafast scattering mechanisms, especially as dictated by specimen boundary conditions. The obtained results, as detailed in peer-reviewed publications and presentations, illustrate the importance of ultrafast, angstrom-scale real-space imaging for developing a comprehensive understanding of energy transport and conversion in materials.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Large scale SiPM testing for the Cosmic Muon Veto detector

A Cosmic Muon Veto (CMV) detector using extruded plastic scintillators is being built around the mini-Iron Calorimeter (mini-ICAL) detector at the transit campus of the India based Neutrino Observatory, Madurai. The extruded plastic scintillators will be embedded with wavelength shifting (WLS) fibres to absorb scintillating photons and propgate the re-emitted photons to the silicon-photomultipliers for the electronic signals. The CMV detector will require 760 extruded plastic scintillators to shield the mini-ICAL detector, and will require 3040 SiPMs for the readout. The design goal for the cosmic muon veto efficiency of the CMV is $>$99.99\% and fake veto rate less than 10$^{-5}$. Hence, every SiPM used in the detector needs to be characterised to satisfy the design goal of the CMV. For this, a large-scale testing system was developed, using an LED driver, to measure the gain and noise rate of each SiPM, and thus determine it's breakdown voltage ($V_{br}$) and optimum operating overvoltage ($V_{ov}$).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS1971

Techniques for gamma rays.

The detecting systems used in high energy astrophysics are generally more similar to particle detectors than to optical devices. The basic design of the gamma ray instrument depends on whether the energy range is below about 10 MeV and therefore in the region where the Compton effect predominates in the absorption of the gamma-rays, or above that energy where electron-positron pair production is most important. The most usual approach to the detector system in the lower of the two energy intervals is to use a scintillation counter in the center of the detector system to absorb the photons and permit a measure of their energy, and to surround it by another detector which is employed as an active anticoincidence shield to discriminate against charged particles. In the gamma-ray interval above about 10 MeV, the very low flux of gamma rays and the high particle background has directed the development of high energy gamma-ray telescopes towards complicated techniques and large detector arrays. As a result, several investigators have now turned to the spark chamber as the heart of a detector system. Generally, it is surrounded by an anticoincidence system and is triggered by a counter telescope.

Fichtel, C. E.↗

NASA NTRS1980

Effective depth of spectral line formation in planetary atmospheres

The effective level of line formation for spectroscopic absorption lines has long been regarded as a useful parameter for determining average atmospheric values of the quantities involved in line formation. The identity of this parameter was recently disputed. The dependence of this parameter on the average depth where photons are absorbed in a semi-infinite atmosphere is established. It is shown that the mean depths derived by others are similar in nature and behavior.

Lestrade, J. P.↗

NASA NTRS1980

Effective depth of spectral line formation in planetary atmospheres

The effective level of line formation for spectroscopic absorption lines has long been regarded as a useful parameter for determining average atmospheric values of the quantities involved in line formation. The identity of this parameter has recently been disputed. This paper reestablishes the dependence of this parameter on the average depth at which photons are absorbed in a semi-infinite atmosphere and shows that the mean depths derived by others are similar in nature and behavior.

Lestrade, J. P.↗

NASA NTRS1987

Resonant enhanced multiphoton ionization studies of atomic oxygen

In resonant enhanced multiphoton ionization (REMPI), an atom absorbs several photons making a transition to a resonant intermediate state and subsequently ionizing out of it. With currently available tunable narrow-band lasers, the extreme sensitivity of REMPI to the specific arrangement of levels can be used to selectively probe minute amounts of a single species (atom) in a host of background material. Determination of the number density of atoms from the observed REMPI signal requires a knowledge of the multiphoton ionization cross sections. The REMPI of atomic oxygen was investigated through various excitation schemes that are feasible with available light sources. Using quantum defect theory (QDT) to estimate the various atomic parameters, the REMPI dynamics in atomic oxygen were studied incorporating the effects of saturation and a.c. Stark shifts. Results are presented for REMPI probabilities for excitation through various 2p(3) (4S sup o) np(3)P and 2p(3) (4S sup o) nf(3)F levels.

Dixit, S. N.↗

NASA NTRS1988

A new laboratory source of ozone and its potential atmospheric implications

Although 248-nm radiation falls 0.12 eV short of the energy needed to dissociate O2, large densities of ozone (O3) can be produced from unfocused 248-nm KrF excimer laser irradiation of pure O2. As soon as any O3 is present, it strongly absorbs the 248-nanometer radiation and dissociates to vibrationally excited ground state O2 (among other products), with a quantum yield of 0.1 to 0.15. During the laser pulse, a portion of these molecules absorb a photon and dissociate, which results in the production of three oxygen atoms for one O3 molecule destroyed. Recombination then converts these atoms to O3, and thus O3 production in the system is autocatalytic. A deficiency exists in current models of O3 photochemistry in the upper stratosphere and mesosphere, in that more O3 is found than can be explained. A detailed analysis of the system as it applies to the upper atmosphere is not yet possible, but with reasonable assumptions about O2 vibrational distributions resulting from O3 photodissociation and about relaxation rates of vibrationally excited O2, a case can be made for the importance of including this mechanism in the models.

Slanger, T. G.↗

NASA NTRS1989

Dust energetics in the gas phases of the interstellar medium - The origin of the Galactic large-scale far-infrared emission observed by IRAS

The large-scale Galactic properties within the most massive gas phases of the ISM are derived along with the distribution of total Galactic FIR luminosity among the three phases. Most of the Galaxy's total FIR luminosity is found to be emitted by cold dust associated with diffuse H I clouds and molecular gas. The total FIR luminosity of dust associated with extended low-density H II regions accounts for less than 10 percent of the Galaxy's total FIR output. The absence of a significant variation with longitude in the observed temperature of the dust associated with H I gas suggests that diffuse neutral clouds contain very small dust grains that are stochastically heated by the interstellar radiation field. The results are consistent with a model in which most of the FIR luminosity of molecular clouds arises from dust that is associated with giant molecular clouds and heated by embedded and nearby OB stars. H II regions in the inner Galaxy have a mean IR excess ratio of about 2.5, suggesting that the dust in these regions is heated primarily by directly absorbed stellar photons.

Sodroski, T. J.↗

NASA NTRS1989

Photo-thermo-dissociation. I - A general mechanism for destroying molecules

Photothermodissociation (PTD) of an isolated molecule is the name of the process when a photon is absorbed by an electronic transition, the energy is transferred to the vibrations (hot molecule) and then an atom or a fragment is ejected. A statistical physics treatment is presented that goes beyond the thermal approximation and fully takes into account the isolation of the system. A model is given that permits an explicit calculation of the ejection rates of hydrogen and carbon fragments from aromatic molecules as a function of their size and internal energy. Then, the lifetime of species against PTD in different astronomical radiation fields will result when a precise dynamical evolution of their internal energy can be established.

Leger, A.↗

NASA NTRS1989

Angular motion of a PAH molecule in interstellar environment

Polycyclic aromatic hydrocarbon (PAH) molecules have recently been proposed as an important and hitherto undetected component of the Interstellar Medium (ISM). The theory was based on an explanation of the Unidentified IR Emission Bands by Leger et al. It has already led to a verified prediction on extended galactic and extragalactic emissions measured by IRAS, or by a recent balloon borne experiment. The physics that rules the motion of such molecules in the ISM was studied, taking into account their coupling with the ambient gas, the radiation field (absorption and emission) and the static magnetic field. This is important for many implications of the PAH theory such as the radio emission by these molecules or the expected polarization of their IR emission. A reflection nebulae is considered where the situation is rather well known. Every day life of a mean PAH molecule in such a region is as follows: every 3 hrs a UV photon is absorbed heating the molecule to a thousand degs; the temperature decay due to cooling by IR emission follows then within a few seconds. A collision with a molecule of gas occurs typically once a week, while an H atom is ejected or captured at the same rate. A typical cooling cycle after a heat impulse is given. The PAH molecules studied as representative of the family has typically 50 atoms, a radius of 4.5 A, is circular and has a molecular mass of M = 300; its permanent dipole moment is 3 Debye.

Rouan, D.↗

NASA NTRS1993

Green icebergs formed by freezing of organic-rich seawater to the base of Antarctic ice shelves

Samples of Antarctic seawater, basal ice, and green ice from ice cliffs and green icebergs are analyzed in order to examine green icebergs formed by the freezing of organic-rich seawater to the base of Antarctic ice shelves. Spectral reflectance of a green iceberg measured near 67 deg S, 62 deg E confirms that the color is inherent in the ice, not an artifact of the illumination. A constituent that absorbs blue photons is identified by spectrophotometric analysis of core samples from this iceberg and from the Amery basal ice, and of seawater samples from Prydz Bay off the Amery Ice Shelf. Analysis of the samples by fluorescence spectroscopy indicates that the blue absorption, and hence the inherent green color, is due to the presence of marine-derived organic matter in the green iceberg, basal ice, and seawater. Thick accumulations of green ice, in icebergs, and at the base of ice shelves indicate that high concentrations of organic matter exist in seawater for centuries at the depth of basal freezing.

Warren, Stephen G.↗

NASA NTRS1997

Evidence for a Multiphase ISM in Early Type Galaxies and Elliptical Galaxies with Strong Radio Continuum

We have observed NGC 1316 (Fornax A) with the ROSAT HRI. In this paper, we present the results of these observations and we complement them with the spectral analysis of the archival PSPC data. The spectral properties suggest the presence of a significant component of thermal X-ray emission (greater than 60%), amounting to approx. 10(exp 9) solar mass of hot ISM. Within 3 feet from the nucleus of NGC 1316, the HRI X-ray surface brightness falls as r(exp -2) following the stellar light. In the inner approx. 30 inch., however, the X-ray surface brightness is significantly elongated, contrary to the distribution of stellar light, which is significantly rounder within 10 inch. This again argues for a non-stellar origin of the X-ray emission. This flattened X-ray feature is suggestive of either the disk-like geometry of a rotating cooling flow and/or the presence of extended, elongated dark matter. By comparing the morphology of the X-ray emission with the distribution of optical dust patches, we find that the X-ray emission is significantly reduced at the locations where the dust patches are more pronounced, indicating that at least some of the X-ray photons are absorbed by the cold ISM. We also compare the distribution of the hot and cold ISM with that of the ionized gas, using recently obtained H(sub alpha) CCD data. We find that the ionized gas is distributed roughly along the dust patches and follows the large scale X-ray distribution at r greater than 1 foot from the nucleus. However, there is no one-to-one correspondence between ionized gas and hot gas. Both morphological relations and kinematics suggest different origins for hot and cold ISM. The radio jets in projection appear to pass perpendicularly through the central X-ray ellipsoid. Comparison of thermal and radio pressures suggests that the radio jets are confined by the surrounding hot gaseous medium.

Kim, Dong Woo↗

NASA NTRS1995

Time-Dependent Photodissociation Regions

We present theoretical models of the time-dependent thermal and chemical structure of molecular gas suddenly exposed to far-ultraviolet (FUV) (6 eV less than hv less than 13.6 eV) radiation fields and the consequent time- dependent infrared emission of the gas. We focus on the response of molecular hydrogen for cloud densities ranging from n = 10(exp 3) to 10(exp 6)/cu cm and FUV fluxes G(sub 0) = 10(exp 3)-10(exp 6) times the local FUV interstellar flux. For G(sub 0)/n greater than 10(exp -2) cu cm, the emergent H(sub 2) vibrational line intensities are initially larger than the final equilibrium values. The H(sub 2) lines are excited by FUV fluorescence and by collisional excitation in warm gas. Most of the H(sub 2) intensity is generated at a characteristic hydrogen column density of N approximately 10(exp 21)/sq cm, which corresponds to an FUV optical depth of unity caused by dust opacity. The time dependence of the H(sub 2) intensities arises because the initial abundances of H(sub 2) at these depths is much higher than the equilibrium values, so that H(sub 2) initially competes more effectively with dust in absorbing FUV photons. Considerable column densities of warm (T approximately 1000) K H(sub 2) gas can be produced by the FUV pumping of H(sub 2) vibrational levels followed by collisional de-excitation, which transfers the energy to heat. In dense (n greater than or approximately 10(exp 5)/cu cm) gas exposed to high (G(sub 0) greater than or approximately 10(exp 4)) fluxes, this warm gas produces a 2-1 S(1)/1-0 S(l) H(sub 2) line ratio of approximately 0.1, which mimics the ratio found in shocked gas. In lower density regions, the FUV pumping produces a pure-fluorescent ratio of approximately 0.5. We also present calculations of the time dependence of the atomic hydrogen column densities and of the intensities of 0 I 6300 A, S II 6730 A, Fe II 1.64 microns, and rotational OH and H20 emission. Potential applications include star-forming regions, clouds near active galactic nuclei, and planetary nebulae. We apply our models to five planetary nebulae and conclude that only BD +30deg3639 shows evidence of enhanced H(sub 2) emission due to (high) nonequilibrium H(sub 2) abundances.

Hollenbach, David↗

NASA NTRS2000

Nebular Hydrogen Absorption in the Ejecta of Eta Carinae

Space Telescope Imaging Spectrograph (STIS) observations of Eta Carinae and immediate ejecta reveal narrow Balmer absorption lines in addition to the nebular-scattered broad P-Cygni absorptions. The narrow absorption correlates with apparent disk structure that separates the two Homunculus lobes. We trace these features about half way up the Northern lobe until the scattered stellar Balmer line doppler-shifts redward beyond the nebular absorption feature. Three-dimensional data cubes, made by mapping the Homunculus at Balmer alpha and Balmer beta with the 52 x 0.1 arcsecond aperture and about 5000 spectral resolving power, demonstrate that the absorption feature changes slowly in velocity with nebular position. We have monitored the stellar Balmer alpha line profile of the central source over the past four years. The equivalent width of the nebular absorption feature changes considerably between observations. The changes do not correlate with measured brightness of Eta Carinae. Likely clumps of neutral hydrogen with a scale size comparable to the stellar disk diameter are passing through the intervening light path on the timescales less than several months. The excitation mechanism involves Lyman alpha radiation (possibly the Lyman series plus Lyman continuum) and collisions leading to populating the 2S metastable state. Before the electron can jump to the ground state by two photon emission (lifetime about 1/8 second), a stellar Balmer photon is absorbed and the electron shifts to an NP level. We see the absorption feature in higher Balmer lines, and but not in Paschen lines. Indeed we see narrow nebular Paschen emission lines. At present, we do not completely understand the details of the absorption. Better understanding should lead to improved insight of the unique conditions around Eta Carinae that leads to these absorptions.

Gull, Theodore R.↗

NASA NTRS2004

Position Sensitive Microcalorimeters

A Position Sensitive Transition-Edge Sensor (PoST) is a microcalorimeter device capable of one-dimensional imaging spectroscopy. The device consists of two Transition-Edge Sensors (TESs) connected to the ends of a long X-ray absorbing strip. The energy of a photon hitting the absorber and the position of the absorption event along the strip is measured from the response in the two sensors by analyzing the relative signal sizes, pulse rise times, and the sum of the pulses measured at each sensor, We report on the recent PoST effort at Goddard for applications to large field of view, high-energy- resolution, X-ray astrophysics.

Sadleir, J. E.↗

NASA NTRS2007

Interband cascade detectors

A device for detecting radiation, typically in the infrared. Photons are absorbed in an active region of a semiconductor device such that the absorption induces an interband electronic transition and generates photo-excited charge carriers. The charge carriers are coupled into a carrier transport region having multiple quantum wells and characterized by intersubband relaxation that provides rapid charge carrier collection. The photo-excited carriers are collected from the carrier transport region at a conducting contact region. Another carrier transport region characterized by interband tunneling for multiple stages draws charge carriers from another conducting contact and replenishes the charge carriers to the active region for photo-excitation. A photocurrent is generated between the conducting contacts through the active region of the device.

Chuang, Shun Lien↗

NASA NTRS1999

Ozone Depletion, UVB and Atmospheric Chemistry

The primary constituents of the Earth's atmosphere are molecular nitrogen and molecular oxygen. Ozone is created when ultraviolet light from the sun photodissociates molecular oxygen into two oxygen atoms. The oxygen atoms undergo many collisions but eventually combine with a molecular oxygen to form ozone (O3). The ozone molecules absorb ultraviolet solar radiation, primarily in the wavelength region between 200 and 300 nanometers, resulting in the dissociation of ozone back into atomic oxygen and molecular oxygen. The oxygen atom reattaches to an O2 molecule, reforming ozone which can then absorb another ultraviolet photon. This sequence goes back and forth between atomic oxygen and ozone, each time absorbing a uv photon, until the oxygen atom collides with and ozone molecule to reform two oxygen molecules.

Stolarski, Richard S.↗

NASA NTRS1999

Ozone Depletion, UVB and Atmospheric Chemistry

Stolarski, Richard S.↗