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Fabrication, characterization and simulation of 4H-SiC Schottky diode alpha particle detectors for pyroprocessing actinide monitoring

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2014, Doctor of Philosophy, Ohio State University, Nuclear Engineering.
Pyroprocessing is a method of using high-temperature molten salts and electric fields to separate and collect fuel isotopes of used nuclear fuel. It has been has been tested in the U.S. at Idaho National Laboratory as a key step in closing the nuclear fuel cycle. One technical problem with the pyroprocessing method is a lack of knowledge regarding the actinide concentrations in the salt bath during operation, since on-line techniques for measuring these concentrations are not presently available. 4H-SiC Schottky diode detectors can potentially fulfill this need. Such detectors would operate in contact with the molten salt, and measure concentrations via alpha-particle spectroscopy. This work seeks to fabricate and characterize 4H-SiC Schottky diode detectors at high temperature, model the alpha particle spectrum expected in a molten salt, and model the operation of the detectors to confirm the physics of operation is as expected. In this work, 4H-SiC Schottky diode detectors were fabricated at OSU Nanotech West. After fabrication, these detectors were characterized using both I-V curves and Am-241 alpha-particle energy spectra. All measurements were made as a function of temperature, from room temperature up to 500°C. The average energy required to create an electron-hole pair was observed to decrease with an increase of temperature, due to a decrease of both the 4H-SiC bandgap and non-linear energy loss terms. Furthermore, the FWHM of the spectra was observed to be dependent on the leakage current at a certain temperature, and not dependent on the temperature itself. Secondly, the alpha particle energy spectrum in the pyroprocessing environment was modeled using SRIM. The molten salt was modeled in 3 different geometries, with or without a protective cover material on top of the detector. Due to the loss of alpha-particle energy in the molten salt itself, a high-energy alpha emitter may completely cover the spectrum from a lower-energy alpha emitter. Each of the geometries simulated showed a different sensitivity to the lower-energy alpha emitter. Regardless of which geometry was modeled, it was observed that it is possible to measure both the emission energy of the alpha particles, as well as the concentration of the alpha emitter in the liquid. Lastly, Sentaurus TCAD was used to simulate the detection of alpha-particle charge collection in situations that are relevant to the molten salt alpha particle energy spectra. The effect of electric field negation was investigated, as well as velocity saturation. Finally, the dependence of charge recombination on temperature, alpha particle energy, and angle of incidence was investigated. These simulations captured the measurements performed at room temperature. With changed angle of incidence, the change in the amount of charge collected was less than 1 percent, indicating a weak dependence. Also, the amount of charge lost to Auger recombination was seen to increase with temperature. This disagrees with observations from experiment, indicating that the temperature dependence of one or more parameters of the model may not be accurate.
Thomas Blue, Ph.D. (Advisor)
Wolfgang Windl, Ph.D. (Committee Member)
Lei Cao, Ph.D. (Committee Member)
285 p.

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Citations

  • Garcia, T. R. (2014). Fabrication, characterization and simulation of 4H-SiC Schottky diode alpha particle detectors for pyroprocessing actinide monitoring [Doctoral dissertation, Ohio State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=osu1387490688

    APA Style (7th edition)

  • Garcia, Timothy. Fabrication, characterization and simulation of 4H-SiC Schottky diode alpha particle detectors for pyroprocessing actinide monitoring. 2014. Ohio State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=osu1387490688.

    MLA Style (8th edition)

  • Garcia, Timothy. "Fabrication, characterization and simulation of 4H-SiC Schottky diode alpha particle detectors for pyroprocessing actinide monitoring." Doctoral dissertation, Ohio State University, 2014. http://rave.ohiolink.edu/etdc/view?acc_num=osu1387490688

    Chicago Manual of Style (17th edition)