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Fragmentation dynamics of CS 2 dications and trications following S 2p ionization

Here, we present the results from a detailed study of the fragmentation dynamics of CS$_2^{2+}$ and CS$_2^{3+}$, formed in intense femtosecond soft x-ray pulses above the sulfur 2p edge, primarily through single core photoionization from the S 2p site, and subsequent Auger–Meitner decay(s). By combining three-dimensional velocity map imaging with covariance analysis, we determine the relative momenta of the ions produced in each two- and three-body fragmentation channel, at significantly higher ion count rates than conventional coincidence measurements. We shed new light on the wide range of fragmentation channels observed from the CS 2 dication and trication, including channels that involve ionization-induced bond formation and fragmentations producing undetected neutral cofragments. In the latter case, a “native frames” approach is used to isolate contributions from concerted and sequential fragmentations and extract dynamical information about each step of a concerted fragmentation process. While dications often fragment sequentially, the trication is dominated by concerted fragmentation. The main trication fragmentation channel into S + + C + + S + can be well-approximated by classical Coulombic simulations of the ground-state geometry distribution, reflecting both the nature of the trication potential energy surface and the rapid multiple ionization prior to substantial structural dynamics. This study demonstrates ways in which fundamental insights into the fragmentation dynamics of polycations following x-ray ionization may be extracted, which will be beneficial to future studies that employ time-resolved x-ray Coulomb explosion imaging to study ultrafast photochemistry.

Allum, Felix [Deutsches Elektronen-Synchrotron (DE↗

Intensified charge coupled devices for ultra low light level imaging

Development of a sensor incorporating a CCD and photocathode for operation in the electron bombarded mode in both a magnetic and an electrostatic focussed, gated configuration is described. Initial format size is 100 x 160 pixels with eventual growth to 400 x 400 pixels. The sensor is part of a digital camera system which includes the low level video conditioning electronics, a camera controller, a high speed buffer memory, and digital recording and display electronics. The memory uses CMOS/SOS and has a capacity of 1.6 Mbits with operating rates of 48 Mbits/sec. Individual frames are co-added to provide wide dynamic range and photometric precision better than 1%. A 4-bit video quantization is used to increase the photon counting detection rate before coincidence losses become serious.

Sobieski, S.↗

An Extremely Low Power Quantum Optical Communication Link for Autonomous Robotic Explorers

One concept for planetary exploration involves using many small robotic landers that can cover more ground than a single conventional lander. In addressing this vision, NASA has been challenged in the National Nanotechnology Initiative to research the development of miniature robots built from nano-sized components. These robots have very significant challenges, such as mobility and communication, given the small size and limited power generation capability. The research presented here has been focused on developing a communications system that has the potential for providing ultra-low power communications for robots such as these. In this paper an optical communications technique that is based on transmitting recognizable sets of photons is presented. Previously pairs of photons that have an entangled quantum state have been shown to be recognizable in ambient light. The main drawback to utilizing entangled photons is that they can only be generated through a very energy inefficient nonlinear process. In this paper a new technique that generates sets of photons from pulsed sources is described and an experimental system demonstrating this technique is presented. This technique of generating photon sets from pulsed sources has the distinct advantage in that it is much more flexible and energy efficient, and is well suited to take advantage of the very high energy efficiencies that are possible when using nano scale sources. For these reasons the communication system presented in this paper is well suited for use in very small, low power landers and rovers. In this paper a very low power optical communications system for miniature robots, as small as 1 cu cm is addressed. The communication system is a variant of photon counting communications. Instead of counting individual photons the system only counts the arrival of time coincident sets of photons. Using sets of photons significantly decreases the bit error rate because they are highly identifiable in the presence of ambient light. An experiment demonstrating reliable communication over a distance of 70 meters using less than a billionth of a watt of radiated power is presented. The components used in this system were chosen so that they could in the future be integrated into a cubic centimeter device.

Lekki, John↗

Single-Volume Scatter Camera (Final Report)

This document serves as a comprehensive final report for the Single-Volume Scatter Camera (SVSC) project. Most of the work over the course of this project has been documented in journal articles, conference papers, and other reports. We therefore reference those materials for detailed presentation of our technical results. The most recent efforts on the project have not been published and are presented in detail here. We present characterizations of two neutron scatter camera prototypes; one using a monolithic geometry, and one using an optically segmented geometry. Both detectors employ plastic scintillator with SiPM-based readout. For the monolithic prototype, we present calibrations of several detector parameters made using a set of dark counts. In particular, we employ a coincidence analysis to characterize the distribution external optical crosstalk, along with the relative timing of the different SiPMs. For the optically segmented prototype we present the results of calibrations made using a tagged 22 Na source, as well as the results of an imaging measurement made using a tagged AmBe source.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

RALPH: An online computer program for acquisition and reduction of pulse height data

A background/foreground data acquisition and analysis system incorporating a high level control language was developed for acquiring both singles and dual parameter coincidence data from scintillation detectors at the Radiation Counting Laboratory at the NASA Manned Spacecraft Center in Houston, Texas. The system supports acquisition of gamma ray spectra in a 256 x 256 coincidence matrix (utilizing disk storage) and simultaneous operation of any of several background support and data analysis functions. In addition to special instruments and interfaces, the hardware consists of a PDP-9 with 24K core memory, 256K words of disk storage, and Dectape and Magtape bulk storage.

Davies, R. C.↗

A Preliminary Investigation for the Use of Digital Gamma-Gamma Coincidence Spectrometry to Determine 239 Pu

Gamma-ray spectrometry is one of the most effective ways to determine the activity of 239 Pu, depending on activity levels. However, often high backgrounds in complex spectra with low amounts of 239 Pu can increase detection limits. The effectiveness of the use of gamma-gamma spectrometry in the characterization of 239 Pu was studied for the first time. Using the XIA Pixie-16 digital pulse processor, the gamma-gamma system was studied to establish unshielded background radiation, source to detector distances, Poisson statistics and gating of several gamma-rays from 239 Pu. The results clearly show that the distance between gamma ray spectrometers has a much bigger effort in counting statistics for the gamma-gamma coincidence detectors than a single detector. In addition, measurements demonstrated the background radiation to be virtually negligible, meaning gammagamma spectroscopy can still be very effective without requiring the usual lead shielding. Other measurements were taken to assure Poisson statistics were attained in the digital system. Preliminary measurements revealed 3 orders of magnitude background reduction for the measurement of 239 Pu using gated gamma-rays.

61 RADIATION PROTECTION AND DOSIMETRY↗

A photon-counting multichannel spectrometer

A multichannel detector system is described in which the positions of individual photon events in a high-gain image intensifier are decoded in the output of a video detector. The high-gain intensifier consists of a pair of three-stage electrostatic image-tube assemblies each containing three fiber-optically-coupled tubes potted in a rugged package with an internal high-voltage supply. Operation of the electrooptical system is discussed along with the pulse-detection process and the operation of the spectrograph in which the image-tube assembly is mounted. It is noted that the spectrometer detects 1.0 count/sec per A for an object of magnitude 13.0 at the peak of its response in the visual band when no light is lost on the slit, that a 10% coincidence correction is reached at an overall count rate of 860 per sec, and that the response follows an exponential law up to count rates of about 4000 per sec. The measured spectrum of the Seyfert galaxy NGC 5548 is provided as an example of the raw data produced by the instrument on a 1.5 meter telescope.

Shectman, S. A.↗

A new algorithm for estimating radioxenon concentrations

A new algorithm (Xcounts) is introduced for estimating the activity concentrations of the xenon isotopes 131m Xe, 133m Xe, 133 Xe, and 135 Xe using beta-gamma coincidence data. The algorithm simultaneously estimates the decay counts associated with the four xenon isotopes, background, and radon in contrast to the net-counts method that uses sequential residual removal to account for background and interreferences. Calibration data for background counts are determined from gas-background measurements and simulation. In Xcounts, the false positive count rates for 131m Xe and 133m Xe are lower than the false positive rates for 133 Xe and 135 Xe. This algorithm appears to reliably detect the metastable isotopes at lower activity levels than the net-counts method and have similar performance for the other isotopes.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Fast event-based electron counting for small-molecule structure determination by MicroED

Electron counting helped realize the resolution revolution in single-particle cryoEM and is now accelerating the determination of MicroED structures. Its advantages are best demonstrated by new direct electron detectors capable of fast (kilohertz) event-based electron counting (EBEC). This strategy minimizes the inaccuracies introduced by coincidence loss (CL) and promises rapid determination of accurate structures. We used the Direct Electron Apollo camera to leverage EBEC technology for MicroED data collection. Given its ability to count single electrons, the Apollo collects high-quality MicroED data from organic small-molecule crystals illuminated with incident electron beam flux densities as low as 0.01–0.045 e − /Å 2 /s. Under even the lowest flux density (0.01 e − /Å 2 /s) condition, fast EBEC data produced ab initio structures of a salen ligand (268 Da) and biotin (244 Da). Each structure was determined from a 100° wedge of data collected from a single crystal in as few as 50 s, with a delivered fluence of only ∼0.5 e − /Å 2 . Fast EBEC data collected with a fluence of 2.25 or 3.33 e − /Å 2 also facilitated a 1.5 Å structure of thiostrepton (1665 Da). While refinement of these structures appeared unaffected by CL, a CL adjustment applied to EBEC data further improved the distribution of intensities measured from the salen ligand and biotin crystals. However, CL adjustment only marginally improved the refinement of their corresponding structures, signaling the already high counting accuracy of detectors with counting rates in the kilohertz range. Overall, by delivering low-dose structure-worthy data, fast EBEC collection strategies open new possibilities for high-throughput MicroED.

EBEC↗

Distinguishing fissile uranium isotopes using an active well neutron coincidence counter

Proposed thorium-based nuclear fuel cycles are likely to require quantification and verification of 233 U within nuclear material. Because of their similar fission cross sections, active neutron nondestructive assay (NDA) systems may respond similarly to 233 U and 235 U. Traditional safeguards equipment has been optimized for 235 U and 238 U quantification associated with conventional uranium/plutonium fuel cycles and may not be directly applicable to 233 U quantification when mixed with other actinides. This work used models of the large volume active well coincidence counter (LV-AWCC) at Oak Ridge National Laboratory to evaluate the performance of this neutron NDA system to differentiate fissile uranium isotopes. The models were developed to simulate NDA system performance in response to a number of triangular radiation signature training device sources within the central cavity or well. This work predicted that the LV-AWCC can effectively differentiate 233 U from 235 U in certain modes of operation. In active mode, the LV-AWCC with the cadmium liner results in different doubles count rates between the fissile isotopes for a given fissile uranium mass. Without the cadmium liner, the uranium isotopes provide a statistically indistinguishable doubles count rate response for the fissile masses considered in this work (up to approximately 150 g). The cadmium liner serves to harden the neutron interrogation spectrum, which better exploits the notable difference in the 233 U and 235 U fission cross sections at approximately 1 eV. In passive mode, the two fissile isotopes exhibit different doubles and singles count rates regardless of liner presence because the passive source strength of 233 U is approximately 2 orders of magnitude stronger than that of 235 U due to the shorter half-life and correspondingly higher (α, n) yield. We conclude that using neutron interrogation in the LV-AWCC, two measurements are needed to quantify 233 U content in mixed uranium items. The first measurement is used to determine the total fissile uranium mass using a mode that cannot distinguish fissile isotopes (i.e., where a similar response is observed for both fissile uranium isotopes such as active doubles without cadmium or using a thermal neutron interrogation source). In conclusion, the second measurement is used to determine the 233 U content by using a differentiating technique (e.g., passive doubles, passive doubles to singles ratio, active doubles with cadmium).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The faint limit of the Hubble Space Telescope faint object spectrograph and rejection of the cosmic-ray background

The faintest object which can be observed with the Hubble Space Telescope (HST) Faint Object Spectrograph (FOS) is set by the detector cosmic-ray background and not by object flux. We use data from Beaver and Lyons to show that 48% of the background counts are from cosmic rays which each generate a near instantaneous burst of two or more counts. Setting the FOS threshold parameter REJLIM = 1, which rejects all frames with more than one count increases the ratio of signal-to-dark counts (S/D) by a factor of 1.94, regardless of the frame time or the object signal, because half of the dark counts which arrive in single counts (from either cosmic-ray bursts or thermal dark current photoemission) are rejected at the same rate as the object signal. But the signal-to-noise ratio (SNR proportional to S/square root of S + D) increases by at most a factor of 1.35, and for realistic parameters and taking into account dead time, we expect a gain in SNR of only 1.18. If a diode has failed and now emits noise, no data at all will be recorded. The chance of this occurring is approximately = 10% , and for this reason we do not recommend the use of REJLIM. The two-point correlation function of dark counts per pixel has strong peaks every four pixels, caused by the action of quarter-stepping on the counts from large bursts. The counts from such bursts spread over at least 80-100 diodes, and we show that such bursts can be rejected during data reduction if the data are recorded in RAPID mode with individual exposures of about 35 seconds. The SNR of the spectrum can also be improved by weighting each exposure by its SNR (a function ofthe mean dark count rate at that time), since dark varies by a factor of 2 around an orbit. These two procedures together increase the SNR by a factor of 1.1.3 (a 28% gain in exposure time) in regions of a spectrum where the object is much fainter than the background. We find that the Ly-alpha and O I sky emission lines give at most 4 (counts/array/s/sq arcsec), and typically half this number. With a small frame time and a small entrance aperture, these counts cause REJLIM = 1 to reject only a few percent of the data. We discuss only the HST FOS blue side detector, but the same ideas apply to any photon counter which records bursts of noise, and the calculations resemble those for the loss of signal due to coincidences in photon counters. In the ideal photon counter the dark counts are readily distinguished from photons. One way to do this is to add detectors which records only dark current, so that every cosmic ray produces more than one count and the instrument can be operated in an anti-coincidence mode.

Tytler, David↗

Deep Learning Approach for High-accuracy Electron Counting of Monolithic Active Pixel Sensor-type Direct Electron Detectors at Increased Electron Dose

Abstract Electron counting can be performed algorithmically for monolithic active pixel sensor direct electron detectors to eliminate readout noise and Landau noise arising from the variability in the amount of deposited energy for each electron. Errors in existing counting algorithms include mistakenly counting a multielectron strike as a single electron event, and inaccurately locating the incident position of the electron due to lateral spread of deposited energy and dark noise. Here, we report a supervised deep learning (DL) approach based on Faster region-based convolutional neural network (R-CNN) to recognize single electron events at varying electron doses and voltages. The DL approach shows high accuracy according to the near-ideal modulation transfer function (MTF) and detector quantum efficiency for sparse images. It predicts, on average, 0.47 pixel deviation from the incident positions for 200 kV electrons versus 0.59 pixel using the conventional counting method. The DL approach also shows better robustness against coincidence loss as the electron dose increases, maintaining the MTF at half Nyquist frequency above 0.83 as the electron density increases to 0.06 e−/pixel. Thus, the DL model extends the advantages of counting analysis to higher dose rates than conventional methods.

Materials Science↗

Novel Photon-Counting Detectors for Free-Space Communication

We present performance data for novel photon-counting detectors for free space optical communication. NASA GSFC is testing the performance of two types of novel photon-counting detectors 1) a 2x8 mercury cadmium telluride (HgCdTe) avalanche array made by DRS Inc., and a 2) a commercial 2880-element silicon avalanche photodiode (APD) array. We present and compare dark count, photon-detection efficiency, wavelength response and communication performance data for these detectors. We successfully measured real-time communication performance using both the 2 detected-photon threshold and AND-gate coincidence methods. Use of these methods allows mitigation of dark count, after-pulsing and background noise effects. The HgCdTe APD array routinely demonstrated photon detection efficiencies of greater than 50% across 5 arrays, with one array reaching a maximum PDE of 70%. We performed high-resolution pixel-surface spot scans and measured the junction diameters of its diodes. We found that decreasing the junction diameter from 31 micrometers to 25 micrometers doubled the e- APD gain from 470 for an array produced in the year 2010 to a gain of 1100 on an array delivered to NASA GSFC recently. The mean single-photon SNR was over 12 and the excess noise factors measurements were 1.2-1.3. The commercial silicon APD array exhibited a fast output with rise times of 300 ps and pulse widths of 600 ps. On-chip individually filtered signals from the entire array were multiplexed onto a single fast output.

Photons↗

233 U oxide Measurement Campaign Data: Passive and Active Neutron Multiplicity Measurements of Uranium Oxide Samples at Oak Ridge National Laboratory

During FY2023, three measurement campaigns were conducted at Oak Ridge National Laboratory. The goal was to quantify the neutron signatures of samples of uranium oxide containing uranium 233 and uranium-235. This report presents the neutron multiplicity data obtained using the large volume active well coincidence counter (LV-AWCC).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Probable detection of solar neutrons by ground-level neutron monitors during STIP interval 16

The third solar neutron event detected by Earth-orbiting spacecraft was observed during STIP Interval XVI. The solar flare beginning at 2356 UT on 24 April l984 produced a variety of emissions including gamma rays and solar neutrons. The neutrons were observed by the SMM satellite and the neutron-decay protons were observed on the ISEE-3 spacecraft. Between 0000 and 0010 UT on 25 April an increase of 0.7 and 1.7 percent was recorded by neutron monitors at Tokyo (Itabashi) and Morioka, Japan. These stations were located about 42 degrees from the sub-solar point, and consequently, these is approximately 1400 grams of atmosphere between the incident neutrons at the top of the atmosphere and their detection on the Earth's surface. Nevertheless, the time coincidence of a small increase in the total counting rate of two independent neutron monitors indicates the presence of solar neutrons with energies greater than 400 MeV at the top of the Earth's atmosphere. The small increases in the counting rate emphasize the difficulty in identifying similar events using historical neutron monitor data.

Shea, M. A.↗

Analysis of counting errors in the phase/Doppler particle analyzer

NASA is investigating the application of the Phase Doppler measurement technique to provide improved drop sizing and liquid water content measurements in icing research. The magnitude of counting errors were analyzed because these errors contribute to inaccurate liquid water content measurements. The Phase Doppler Particle Analyzer counting errors due to data transfer losses and coincidence losses were analyzed for data input rates from 10 samples/sec to 70,000 samples/sec. Coincidence losses were calculated by determining the Poisson probability of having more than one event occurring during the droplet signal time. The magnitude of the coincidence loss can be determined, and for less than a 15 percent loss, corrections can be made. The data transfer losses were estimated for representative data transfer rates. With direct memory access enabled, data transfer losses are less than 5 percent for input rates below 2000 samples/sec. With direct memory access disabled losses exceeded 20 percent at a rate of 50 samples/sec preventing accurate number density or mass flux measurements. The data transfer losses of a new signal processor were analyzed and found to be less than 1 percent for rates under 65,000 samples/sec.

Oldenburg, John R.↗

Low-Noise Free-Running High-Rate Photon-Counting for Space Communication and Ranging

We present performance data for low-noise free-running high-rate photon counting method for space optical communication and ranging. NASA GSFC is testing the performance of two types of novel photon-counting detectors 1) a 2x8 mercury cadmium telluride (HgCdTe) avalanche array made by DRS Inc., and a 2) a commercial 2880-element silicon avalanche photodiode (APD) array. We successfully measured real-time communication performance using both the 2 detected-photon threshold and logic AND-gate coincidence methods. Use of these methods allows mitigation of dark count, after-pulsing and background noise effects without using other method of Time Gating The HgCdTe APD array routinely demonstrated very high photon detection efficiencies (50) at near infrared wavelength. The commercial silicon APD array exhibited a fast output with rise times of 300 ps and pulse widths of 600 ps. On-chip individually filtered signals from the entire array were multiplexed onto a single fast output. NASA GSFC has tested both detectors for their potential application for space communications and ranging. We developed and compare their performances using both the 2 detected photon threshold and coincidence methods.

Photons↗