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Patel, Maulik K.

Publications and source records attributed to Patel, Maulik K..

Ionizing vs collisional radiation damage in materials: Separated, competing, and synergistic effects in Ti 3 SiC 2

Comparison between intense radiation environments present in nuclear reactors and charged particle beams is necessary for evaluating next generation fission and fusion reactor materials. Yet, these two irradiation environments encompass different proportions of ionizing and collisional phenomena, so exploring the different energy loss pathways is needed for appropriate analysis. Using the candidate M n+1 AX n phase, Ti 3 SiC 2 , as a test case, this work separates the effects of electronic and nuclear energy loss during ion irradiation, through a combination of 4 MeV Au, 17 MeV Pt, and 14 MeV Cl ion irradiations to examine the effects independently and systematically recombine them. Nuclear energy loss (elastic collisions) is found to be primarily responsible for the formation of a face-centered-cubic phase with anti-site defects, while intense electronic energy loss (ionization) exacerbates the effect and increases lattice strain. Moreover, these dissipation pathways are found to be competing or synergistic depending on their ionization and collisional ratio.

36 MATERIALS SCIENCE↗

Influence of electronic vs nuclear energy loss in radiation damage of Ti 3 SiC 2

We report the thermal conductivity and stability of MAX phases has led to irradiation studies of these materials for their possible application in the hostile environments of high temperature and radiation. Numerous neutron and ion irradiation studies have been conducted that demonstrate that radiation induced modifications consists of lattice strain and increased formation of TiC. Ion beams have been used to simulate damage created by neutrons; however, what is not clear is the effect of varying electronic to nuclear energy loss on the damage evolution within this material. In the present work, changes in c/a within Ti 3 SiC 2 are monitored as a function of energy deposition at constant damage dose following high fluence 9 MeV Ti ion irradiations at room temperature. The results reveal that there is an apparent threshold in the electronic energy loss, above which the c/a ratio and TiC concentration starts to increase with increasing electronic energy loss. Interestingly, this change is independent of the damage dose in displacements per atom. In conclusion, this suggests that inelastic energy dissipation is of paramount importance when selecting ions for simulating damage by energetic neutrons.

36 MATERIALS SCIENCE↗

Improved high temperature radiation damage tolerance in a three-phase ceramic with heterointerfaces

Abstract Radiation damage tolerance for a variety of ceramics at high temperatures depends on the material’s resistance to nucleation and growth of extended defects. Such processes are prevalent in ceramics employed for space, nuclear fission/fusion and nuclear waste environments. This report shows that random heterointerfaces in materials with sub-micron grains can act as highly efficient sinks for point defects compared to grain boundaries in single-phase materials. The concentration of dislocation loops in a radiation damage-prone phase (Al 2 O 3 ) is significantly reduced when Al 2 O 3 is a component of a composite system as opposed to a single-phase system. These results present a novel method for designing exceptionally radiation damage tolerant ceramics at high temperatures with a stable grain size, without requiring extensive interfacial engineering or production of nanocrystalline materials.

36 MATERIALS SCIENCE↗

Semiconductor composition containing iron, dysprosium, and terbium

An amorphous semiconductor composition includes 1 to 70 atomic percent iron, 15 to 65 atomic percent dysprosium, 15 to 35 atomic percent terbium, balance X, wherein X is at least one of an oxidizing element and a reducing element. The composition has an essentially amorphous microstructure, an optical transmittance of at least 50% in at least the visible spectrum and semiconductor electrical properties.

36 MATERIALS SCIENCE↗

In situ investigation of halide incorporation into perovskite solar cells

We report on the material chemistry following crystallization in the presence of water vapor of chlorinated formamidinium lead-triiodide (NH 2 CH = NH 2 PbI 3-x Cl x ) perovskite films. We found in-situ exposure to water vapor reduces, or possibly eliminates, the retention of chlorine (Cl) inside NH 2 CH = NH 2 PbI 3-x Cl x crystals. There is a strong tendency toward Cl volatility, which indicates the sensitivity of these materials for their integration into solar cells. The requisite for additional efforts focused on the mitigation of water vapor is reported. Based on the in situ results, hot casting (<100°C) in dry conditions demonstrates improved film coverage and Cl retention with efficiencies reaching 12.07%.

14 SOLAR ENERGY↗

Combined effects of radiation damage and He accumulation on bubble nucleation in Gd2Ti2O7

Pyrochlores have long been considered as host phases for long-term immobilization of radioactive waste nuclides that would undergo ..alpha..-decay for hundreds of thousands of years. This work utilizes ion-beam irradiations to examine the combined effects of radiation damage and He accumulation on bubble formation in Gd2Ti2O7 over relevant waste-form timescales. Helium bubbles are not observed in pre-damaged Gd2Ti2O7 implanted with 2 x 1016 He/cm2, even after post-implantation irradiations with 7 MeV Au3+ at 300, 500, and 700 K. However, He bubbles with average diameters of 1.5 nm and 2.1 nm are observed in pre-damaged (amorphous) Gd2Ti2O7 and pristine Gd2Ti2O7, respectively, after implantation of 2 x 1017 He/cm2. The critical He concentration for bubble nucleation in Gd2Ti2O7 is estimated to be 6 at.% He.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Bubble Formation and Lattice Parameter Changes Resulting from He Irradiation of Defect-Fluorite Gd2Zr2O7

Pyrochlores have long been considered as potential candidates for advanced ceramic waste-forms for the immobilization of radioactive waste nuclides. This work provides evidence that Gd2Zr2O7, often considered the most radiation tolerant pyrochlore, could be susceptible to radiation damage in the form of bubble nucleation at the highest He doses expected over geological time. Ion irradiations were utilized to experimentally simulate the radiation damage and He accumulation produced by ..alpha..-decay. Samples were pre-damaged using 7 MeV Au3+ to induce the pyrochlore to defect-fluorite phase transformation, which would occur due to ..alpha..-recoil damage within several hundred years of storage in a Gd2Zr2O7 waste-form. These samples were then implanted to various He concentrations in order to study the long-term effects of He accumulation. Helium bubbles 1-3 nm in diameter were observed in TEM at a concentration of 4.6 at.% He. Some bubbles remained isolated, while others formed chains 10-30 nm in length parallel to the surface. GIXRD measurements showed lattice swelling after irradiating pristine Gd2Zr2O7 with 7 MeV Au3+ to a fluence of 2.2 x 1015 Au/cm2. An increase in lattice swelling was also measured after 2.2 x 1015 Au/cm2 + 2 x 1015 He/cm2 and 2.2 x 1015 Au/cm2 + 2 x 1016 He/cm2. A decrease in lattice swelling was measured after irradiation with 2.2 x 1015 Au/cm2 + 2 x 1017 He/cm2, the fluence where bubbles and bubble chains were observed in TEM. Bubble chains are thought to form in order to reduce lattice strain normal to the surface, which is produced by the Au and He irradiation damage.

36 MATERIALS SCIENCE↗

Revealing Surface Modifications of Potassium-Fluoride-Treated Cu(In,Ga)Se 2 : A Study of Material Structure, Chemistry, and Photovoltaic Performance

The effects of alkali post-deposition treatments and device properties for polycrystalline thin film Cu(In,Ga)Se2 have been investigated. It is reported that these surface treatments lead to differences in interface chemistry and device properties. The behavior of defects in the space charge region as a function of different growth parameters is investigated by correlative analytical microscopy. The latter combines electron microscopy based imaging, Kelvin probe force microscopy, and atom probe tomography. Alkali treatments lead to copper depletion and consequent sharpening of the compositional profiles, and the measured electric potential differences of exposed Cu(In1-x,Gax)Se2 surfaces. Measurable differences in resistivity and potential have also been observed, which are expected to relate to the improved open-circuit voltage, fill-factor, and device efficiency. This study frames one perspective as to why post-deposition alkaline treatments lead to copper depletion, a mildly n-type semiconductor interface, and higher efficiency for a Cu(In,Ga)Se2 thin-film photovoltaic device.

14 SOLAR ENERGY↗

In situ investigation of the formation and metastability of formamidinium lead tri-iodide perovskite solar cells

Organic–inorganic perovskites have emerged as an important class of next generation solar cells due to their remarkably low cost, band gap, and sub-900 nm absorption onset. Here, we show a series of in situ observations inside electron microscopes and X-ray diffractometers under device-relevant synthesis conditions focused on revealing the crystallization process of the formamidinium lead-triiodide perovskite at the optimum temperature of 175 °C. Direct in situ observations of the structure and chemistry over relevant spatial, temporal, and temperature scales enabled identification of key perovskite formation and degradation mechanisms related to grain evolution and interface chemistry. The lead composition was observed to fluctuate at grain boundaries, indicating a mobile lead-containing species, a process found to be partially reversible at a key temperature of 175 °C. Using low energy electron microscopy and valence electron energy loss spectroscopy, lead is found to be bonded in the grain interior with iodine in a tetrahedral configuration. At the grain boundaries, the binding energy associated with lead is consequently shifted by nearly 2 eV and a doublet peak is resolved due presumably to a greater degree of hybridization and the potential for several different bonding configurations. At the grain boundaries there is adsorption of hydrogen and OH¯ ions as a result of residual water vapor trapped as a non-crystalline material during formation. Lastly, insights into the relevant formation and decomposition reactions of formamidinium lead iodide at low to high temperatures, observed metastabilities, and relationship with the photovoltaic performance were obtained and used to optimize device processing resulting in conversion efficiencies of up to 17.09% within the stability period of the devices.

14 SOLAR ENERGY↗