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Microcalorimeters with embedded radioisotopes are an emerging category of sensor with advantages over existing methods for isotopic analysis of trace-level nuclear materials. For each nuclear decay, the energy of all decay products captured by the absorber (alpha particles, gamma rays, X-rays, electrons, daughter nuclei, etc.) is measured in one pulse. For alpha-decaying isotopes, this gives a measurement of the total nuclear reaction energy (Q value) and the spectra consist of well-separated, narrow peaks. We have demonstrated a simple mechanical alloying process to create an absorber structure consisting of a gold matrix with small inclusions of a radioactive sample. This absorber structure provides an optimized energy thermalization environment, resulting in high-resolution spectra with minimal tailing. We have applied this process to the analysis of particles collected from the surface of a plutonium metal certified reference material (CRM-126A from New Brunswick Laboratory) and demonstrated isotopic analysis by microcalorimeter Q value spectroscopy. Energy resolution from the Gaussian component of a Bortels function fit was 1.3 keV FWHM at 5244 keV. The collected particles were integrated directly into the detector absorber without any chemical processing. The $$^{238}$$ Pu/ $$^{239}$$ Pu and $$^{240}$$ Pu/ $$^{239}$$ Pu mass ratios were measured and the results confirmed against the certificate of analysis for the reference material. We also demonstrated inter-element analysis capability by measuring the $$^{241}$$ Am/ $$^{239}$$ Pu mass ratio. [ABSTRACT FROM AUTHOR]

Microcalorimeter detectors with embedded radioactive material offer many possibilities for new types of measurements and applications. We will discuss the designs and methods that we are developing for precise deposition of radioactive material and its encapsulation in the absorber of transition-edge sensor (TES) microcalorimeter detectors for two specific applications. The first application is total nuclear reaction energy (Q) spectroscopy for nuclear forensics measurements of trace actinide samples, where the goal is determination of ratios of isotopes with Q values in the range of 5-7 MeV. Simplified, rapid sample preparation and detector assembly is necessary for practical measurements, while maintaining good energy resolution. The second application is electron capture spectroscopy of isotopes with low Q values, such as $$^{163}$$ Ho, for measurement of neutrino mass. Detectors for electron capture spectroscopy are designed for measuring energies up to approximately 6 keV. Their smaller heat capacity and physical size present unique challenges. Both applications require precise deposition of radioactive material and encapsulation in an absorber with optimized thermal properties and coupling to the TES. We have made detectors for both applications with a variety of designs and assembly methods, and will present their development. [ABSTRACT FROM AUTHOR]

Ultra-high resolution alpha spectrometry by microcalorimetry has demonstrated a dramatic improvement in alpha energy resolution over silicon based detectors. To characterize the optimal resolution obtained by the microcalorimeter alpha spectrometers, high quality deposits that are virtually massless are required; electrodeposition is the preferred method for the preparation of high quality deposits. In order to better understand the factors that contribute to lower alpha energy resolution and deposit yield, we have conducted a study to determine the effect of some of the parameters that are used for preparing electrodeposits. We have compared four different electrodeposition methods and four different substrate materials to determine the effect on the deposit yield and alpha energy resolution of plutonium as measured by full width at half maximum using silicon based detectors. Furthermore, we wanted to understand the effect of contaminants from environmental samples on electrodeposits. Therefore, the effect on deposit yield and alpha energy resolution with several common soil constituents (Al, Eu, Fe, K, Lu, Mg, Na, Zn) have been studied. [ABSTRACT FROM AUTHOR]

Alpha particle spectrometry is a powerful analytical tool for nuclear forensics and environmental monitoring. Microcalorimeter detectors have been shown to yield nearly an order of magnitude better energy resolution (1.06 keV FWHM at 5.3 MeV) than current state-of-the-art silicon detectors (8-10 keV FWHM at 5.3 MeV). This superior resolution allows isotopic analysis with a single non-consumptive measurement of samples that contain multiple radioisotopes with overlapping alpha energies. Measurement of such a sample with a silicon detector would require expensive and time-consuming radiochemical separations. We are developing two alpha spectrometer systems with superconducting transition-edge sensor microcalorimeters. The first system has eight independent detector channels that measure eight different alpha sources, and is optimized for detector development experiments. The second system incorporates a prototype cryogenic load lock that allows for rapid exchange of alpha samples. This paper will present results from these two systems. [ABSTRACT FROM AUTHOR]

Alpha-particle spectrometry is a powerful analytical tool for nuclear forensics and environmental monitoring. Superconducting transition-edge sensor microcalorimeters have been shown to yield unsurpassed energy resolution for alpha spectrometry. With nearly an order of magnitude better energy resolution (1.06 keV FWHM at 5.3 MeV) than the current state-of-the-art silicon detectors (8–10 keV at 5.3 MeV), it is possible to measure samples containing multiple radioisotopes that would require expensive and time-consuming radiochemical separation prior to measurement with a silicon detector. This paper presents recent results from the Los Alamos four-channel microcalorimeter alpha spectrometer. We have prepared a source from weapons-grade plutonium and demonstrated the ability of microcalorimeter alpha spectrometry to simultaneously resolve alpha energies from ^239Pu, ^240Pu, ^238Pu, and ^241Am. The low-energy performance of the spectrometer system has been improved to allow measurement of energies as low as 5 keV, which gives a dynamic range of 1000. We have demonstrated this capability by simultaneously measuring the alpha particles and low-energy x-rays and internal conversion electrons emitted by an electroplated ^240Pu source. [ABSTRACT FROM AUTHOR]