skip to main content

Title: Radiation-resistant binary solid solutions via vacancy trapping on solute clusters
Additions of solute that trap vacancies slow down vacancy diffusion and promote point-defect recombination in alloys subjected to irradiation. Such selective alloying can thus help to minimize the detrimental consequences resulting from point defect fluxes. The current work investigates the effect of solute additions on the recombi- nation rate using kinetic Monte Carlo simulations for a model alloy system, which was parametrized to Cu-Ag in the dilute limit, but with an increased solubility limit, ≈0.86 at.% at 300 K. As the solute concentration was increased above 0.1 at.%, solute clustering was observed and led to a strong increase in recombination rate. The beneficial effects of solute clustering on reducing vacancy mobility, and reducing solute drag, were analyzed by calculating relevant transport coefficients using the KineCluE code (Schuler et al., Computational Materials Science (2020) 172,109,191). Moreover, it was observed in the KMC simulations that large recombination rates resulted in a shift of steady-state distributions of solute cluster sizes to smaller clusters compared to equilibrium distributions in the solid solution. This shift is rationalized as resulting from the irreversible character of the interstitial-vacancy recombination reaction. These results suggest a novel irradiation effect on phase stability where a high recombination rate increases the more » solubility limit of a solute at steady state over its equilibrium value. « less
Authors:
; ;
Award ID(s):
1709857
Publication Date:
NSF-PAR ID:
10312915
Journal Name:
Materialia
Volume:
20
ISSN:
2589-1529
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    Monolayer molybdenum disulfide has been previously discovered to exhibit non-volatile resistive switching behavior in a vertical metal-insulator-metal structure, featuring ultra-thin sub-nanometer active layer thickness. However, the reliability of these nascent 2D-based memory devices was not previously investigated for practical applications. Here, we employ an electron irradiation treatment on monolayer MoS2film to modify the defect properties. Raman, photoluminescence, and X-ray photoelectron spectroscopy measurements have been performed to confirm the increasing amount of sulfur vacancies introduced by the e-beam irradiation process. The statistical electrical studies reveal the reliability can be improved by up to 1.5× for yield and 11× for average DC cycling endurance in the devices with a moderate radiation dose compared to unirradiated devices. Based on our previously proposed virtual conductive-point model with the metal ion substitution into sulfur vacancy, Monte Carlo simulations have been performed to illustrate the irradiation effect on device reliability, elucidating a clustering failure mechanism. This work provides an approach by electron irradiation to enhance the reliability of 2D memory devices and inspires further research in defect engineering to precisely control the switching properties for a wide range of applications from memory computing to radio-frequency switches.

  2. Radiation damage in electronic devices is known to be influenced by physics, design, and materials system. Here, we report the effects of biasing state (such as ON and OFF) and pre-existing damage in GaN high electron mobility transistors exposed to γ radiation. Controlled and accelerated DC biasing was used to prestress the devices, which showed significant degradation in device characteristics compared to pristine devices under ON and OFF states after γ irradiation. The experiment is performed in situ for the ON-state to investigate transient effects during irradiation until the total dose reaches 10 Mrad. It shows that threshold voltage, maximum transconductance, and leakage current initially decrease with dosage but slowly converge to a steady value at higher doses. After 10 Mrad irradiation, the OFF-state device demonstrates larger RONand one order of magnitude increased leakage current compared to the ON-state irradiated device. The micro-Raman study also confirms that the ON-state operation shows more radiation hardness than OFF and prestressed devices. Prestressed devices generate the highest threshold voltage shift from −2.85 to −2.49 V and two orders of magnitude higher leakage current with decreased saturation current after irradiation. These findings indicate that high electric fields during stressing can generate defects by modifying strain distribution, andmore »higher defect density can not only create more charges during irradiation but also accelerate the diffusion process from the ionizing track to the nearest collector and consequently degrade device performances.

    « less
  3. Two-dimensional transition metal dichalcogenides (2D-TMDs) hold a great potential to platform future flexible optoelectronics. The beating hearts of these materials are their excitons known as XA and XB, which arise from transitions between spin-orbit split (SOS) levels in the conduction and valence bands at the K-point. The functionality of 2D-TMD-based devices is determined by the dynamics of these excitons. One of the most consequential channels of exciton decay on the device functionality is the defect-assisted recombination (DAR). Here, we employ steady-state absorption and emission spectroscopies, and pump density-dependent femtosecond transient absorption spectroscopy to report on the effect of DAR on the lifetime of excitons in monolayers of tungsten disulfide (2D-WS2) and diselenide (2D-WSe2). These pump-probe measurements suggested that while exciton decay dynamics in both monolayers are driven by DAR, in 2D-WS2, defect states near the XB exciton fill up before those near the XA exciton. However, in the 2D-WSe2 monolayer, the defect states fill up similarly. Understanding the contribution of DAR on the lifetime of excitons and the partition of this decay channel between XA and XB excitons may open new horizons for the incorporation of 2D-TMD materials in future optoelectronics.
  4. Multiple silicon solar cell technologies have surpassed or are close to surpassing 26% efficiency. Dielectric and amorphous silicon-based passivation layers combined with minimal metal/silicon contact areas were responsible for reducing the surface saturation current density below 3 fA cm −2 . At open-circuit, in passivated contact solar cells, the recombination is mainly from fundamental mechanisms (Auger and radiative) representing over 3/4 of the total recombination. At the maximum power point, the fundamental recombination fraction can drop to half, as surface and bulk Shockley–Read–Hall step in. As a result, to further increase the performance at the operating point, it is paramount to reduce the bulk dependence and secure proper surface passivation. Bulk recombination can be mitigated either by reducing bulk defect density or by reducing the wafer thickness. We demonstrate that for commercially-viable solar-grade silicon, thinner wafers and surface saturation current densities below 1 fA cm −2 , are required to significantly increase the practical efficiency limit of solar cells up to 0.6% absolute. For a high-quality n-type bulk silicon minority-carrier lifetime of 10 ms, the optimum wafer thickness range is 40–60 μm, a very different value from 110 μm previously calculated assuming undoped substrates and solely Auger and radiative recombination.more »In this thickness range surface saturation current densities near 0.1 fA cm −2 are required to narrow the gap towards the fundamental efficiency limit. We experimentally demonstrate surface saturation currents below 0.5 fA cm −2 on pi/CZ/in structures across different wafer thicknesses (35–170 μm), with potential to reach open-circuit voltages close to 770 mV and bandgap-voltage offsets near 350 mV. Finally, we use the bandgap-voltage offset as a metric to compare the quality of champion experimental solar cells in the literature, for the most commercially-relevant photovoltaic cell absorbers and architectures.« less
  5. The remarkable optoelectronic properties of metal halide perovskites have generated intense research interest over the last few years. The ability to control and manipulate the crystallisation and stoichiometry of perovskite thin-films has allowed for impressive strides in the development of highly efficient perovskite solar cells. However, being able to effectively modify the interfaces of metal halide perovskites, and to controllably p- or n-type dope the surfaces, may be key to further improvements in the efficiency and long-term stability of these devices. In this study, we use surface doping of the mixed-cation, mixed-halide perovskite FA 0.85 MA 0.15 Pb(I 0.85 Br 0.15 ) 3 (FA – formamidinium; MA – methylammonium) to improve the hole extraction from the perovskite solar cell. By treating the surface of the perovskite film with a strongly oxidizing molybdenum tris(dithiolene) complex, we achieve a shift in the work function that is indicative of p-doping, and a twofold increase in the total conductivity throughout the film. We probe the associated interfacial chemistry through photoelectron and solid-state nuclear magnetic resonance spectroscopies and confirm that charge-transfer occurs between the perovskite and dopant complex. The resulting p-doped interface constitutes a homojunction with increased hole-selectivity. With charge-selective layers, we show that thismore »surface doping enhances the device performance of perovskite solar cells resulting in steady-state efficiencies approaching 21%. Finally, we demonstrate that a surface treatment with this dopant produces the same effect as the commonly employed additive 4- tert butylpyridine ( t BP), allowing us to achieve “ t BP-free” devices with steady-state efficiencies of over 20%, and enhanced thermal stability as compared to devices processed using t BP. Our findings therefore demonstrate that molecular doping is a feasible route to tune and control the surface properties of metal halide perovskites.« less