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- Creators: Barnaby, Hugh J
Description
Chalcogenide glass (ChG) materials have gained wide attention because of their applications in conductive bridge random access memory (CBRAM), phase change memories (PC-RAM), optical rewritable disks (CD-RW and DVD-RW), microelectromechanical systems (MEMS), microfluidics, and optical communications. One of the significant properties of ChG materials is the change in the resistivity of the material when a metal such as Ag or Cu is added to it by diffusion. This study demonstrates the potential radiation-sensing capabilities of two metal/chalcogenide glass device configurations. Lateral and vertical device configurations sense the radiation-induced migration of Ag+ ions in germanium selenide glasses via changes in electrical resistance between electrodes on the ChG. Before irradiation, these devices exhibit a high-resistance `OFF-state' (in the order of 10E12) but following irradiation, with either 60-Co gamma-rays or UV light, their resistance drops to a low-resistance `ON-state' (around 10E3). Lateral devices have exhibited cyclical recovery with room temperature annealing of the Ag doped ChG, which suggests potential uses in reusable radiation sensor applications. The feasibility of producing inexpensive flexible radiation sensors has been demonstrated by studying the effects of mechanical strain and temperature stress on sensors formed on flexible polymer substrate. The mechanisms of radiation-induced Ag/Ag+ transport and reactions in ChG have been modeled using a finite element device simulator, ATLAS. The essential reactions captured by the simulator are radiation-induced carrier generation, combined with reduction/oxidation for Ag species in the chalcogenide film. Metal-doped ChGs are solid electrolytes that have both ionic and electronic conductivity. The ChG based Programmable Metallization Cell (PMC) is a technology platform that offers electric field dependent resistance switching mechanisms by formation and dissolution of nano sized conductive filaments in a ChG solid electrolyte between oxidizable and inert electrodes. This study identifies silver anode agglomeration in PMC devices following large radiation dose exposure and considers device failure mechanisms via electrical and material characterization. The results demonstrate that by changing device structural parameters, silver agglomeration in PMC devices can be suppressed and reliable resistance switching may be maintained for extremely high doses ranging from 4 Mrad(GeSe) to more than 10 Mrad (ChG).
ContributorsDandamudi, Pradeep (Author) / Kozicki, Michael N (Thesis advisor) / Barnaby, Hugh J (Committee member) / Holbert, Keith E. (Committee member) / Goryll, Michael (Committee member) / Arizona State University (Publisher)
Created2013
Description
Layered chalcogenides are a diverse class of crystalline materials that consist of covalently bound building blocks held together by van der Waals forces, including the transition metal dichalcogenides (TMDCs) and the pnictogen chalcogenides (PCs) among all. These materials, in particular, MoS2 which is the most widely studied TMDC material, have attracted significant attention in recent years due to their unique physical, electronic, optical, and chemical properties that depend on the number of layers. Due to their high aspect ratios and extreme thinness, 2D materials are sensitive to modifications via chemistry on their surfaces. For instance, covalent functionalization can be used to robustly modify the electronic properties of 2D materials, and can also be used to attach other materials or structures. Metal adsorption on the surfaces of 2D materials can also tune their electronic structures, and can be used as a strategy for removing metal contaminants from water. Thus, there are many opportunities for studying the fundamental surface interactions of 2D materials and in particular the TMDCs and PCs.
The work reported in this dissertation represents detailed fundamental studies of the covalent functionalization and metal adsorption behavior of layered chalcogenides, which are two significant aspects of the surface interactions of 2D materials. First, we demonstrate that both the Freundlich and Temkin isotherm models, and the pseudo-second-order reaction kinetics model are good descriptors of the reaction due to the energetically inhomogeneous surface MoS2 and the indirect adsorbate-adsorbate interactions from previously attached nitrophenyl (NP) groups. Second, the covalent functionalization using aryl diazonium salts is extended to nanosheets of other representative TMDC materials MoSe2, WS2, and WSe2, and of the representative PC materials Bi2S3 and Sb2S3, demonstrated using atomic force microscopy (AFM) imaging and Fourier transform infrared spectroscopy (FTIR). Finally, using AFM and X-ray photoelectron spectroscopy (XPS), it is shown that Pb, Cd Zn and Co form nanoclusters on the MoS2 surface without affecting the structure of the MoS2 itself. The metals can also be thermally desorbed from MoS2, thus suggesting a potential application as a reusable water purification technology.
The work reported in this dissertation represents detailed fundamental studies of the covalent functionalization and metal adsorption behavior of layered chalcogenides, which are two significant aspects of the surface interactions of 2D materials. First, we demonstrate that both the Freundlich and Temkin isotherm models, and the pseudo-second-order reaction kinetics model are good descriptors of the reaction due to the energetically inhomogeneous surface MoS2 and the indirect adsorbate-adsorbate interactions from previously attached nitrophenyl (NP) groups. Second, the covalent functionalization using aryl diazonium salts is extended to nanosheets of other representative TMDC materials MoSe2, WS2, and WSe2, and of the representative PC materials Bi2S3 and Sb2S3, demonstrated using atomic force microscopy (AFM) imaging and Fourier transform infrared spectroscopy (FTIR). Finally, using AFM and X-ray photoelectron spectroscopy (XPS), it is shown that Pb, Cd Zn and Co form nanoclusters on the MoS2 surface without affecting the structure of the MoS2 itself. The metals can also be thermally desorbed from MoS2, thus suggesting a potential application as a reusable water purification technology.
ContributorsLi, Duo, Ph.D (Author) / Wang, Qing Hua (Thesis advisor) / Green, Alexander A. (Committee member) / Chan, Candace K. (Committee member) / Jiao, Yang (Committee member) / Arizona State University (Publisher)
Created2019
Description
As photons, electrons, and neutrons traverse a medium, they impart their energy in ways that are analytically difficult to describe. Monte Carlo methods provide valuable insight into understanding this behavior, especially when the radiation source or environment is too complex to simplify. This research investigates simulating various radiation sources using the Monte Carlo N-Particle (MCNP) transport code, characterizing their impact on various materials, and comparing the simulation results to general theory and measurements.
A total of five sources were of interest: two photon sources of different incident particle energies (3.83 eV and 1.25 MeV), two electron sources also of different energies (30 keV and 100 keV), and a californium-252 (Cf-252) spontaneous fission neutron source. Lateral and vertical programmable metallization cells (PMCs) were developed by other researchers for exposure to these photon and electron sources, so simplified PMC models were implemented in MCNP to estimate the doses and fluences. Dose rates measured around the neutron source and the predicted maximum activity of activation foils exposed to the neutrons were determined using MCNP and compared to experimental results obtained from gamma-ray spectroscopy.
The analytical fluence calculations for the photon and electron cases agreed with MCNP results, and differences are due to MCNP considering particle movements that hand calculations do not. Doses for the photon cases agreed between the analytical and simulated results, while the electron cases differed by a factor of up to 4.8. Physical dose rate measurements taken from the neutron source agreed with MCNP within the 10% tolerance of the measurement device. The activity results had a percent error of up to 50%, which suggests a need to further evaluate the spectroscopy setup.
A total of five sources were of interest: two photon sources of different incident particle energies (3.83 eV and 1.25 MeV), two electron sources also of different energies (30 keV and 100 keV), and a californium-252 (Cf-252) spontaneous fission neutron source. Lateral and vertical programmable metallization cells (PMCs) were developed by other researchers for exposure to these photon and electron sources, so simplified PMC models were implemented in MCNP to estimate the doses and fluences. Dose rates measured around the neutron source and the predicted maximum activity of activation foils exposed to the neutrons were determined using MCNP and compared to experimental results obtained from gamma-ray spectroscopy.
The analytical fluence calculations for the photon and electron cases agreed with MCNP results, and differences are due to MCNP considering particle movements that hand calculations do not. Doses for the photon cases agreed between the analytical and simulated results, while the electron cases differed by a factor of up to 4.8. Physical dose rate measurements taken from the neutron source agreed with MCNP within the 10% tolerance of the measurement device. The activity results had a percent error of up to 50%, which suggests a need to further evaluate the spectroscopy setup.
ContributorsBowler, Herbert (Author) / Holbert, Keith E. (Thesis advisor) / Barnaby, Hugh J (Committee member) / Clark, Lawrence T (Committee member) / Arizona State University (Publisher)
Created2014