Modeling amorphous thin films: Kinetically limited minimization

Zawadzki, Paweł; Perkins, John D.; Lany, Stephan

doi:10.1103/physrevb.90.094203

Cited by 14 publications

(9 citation statements)

References 28 publications

(32 reference statements)

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“…Finding the amorphous limit requires exploring the PEL of the amorphous system to locate the low-lying basins. These atomic models of amorphous structures can be generated using a variety of procedures such as melt-quench routes and energy minimization techniques ( 39 , 40 ). We adopted a common PEL exploration strategy ( 28 , 30 ) where a certain number of independent configurations from the high-temperature parent liquid were selected and relaxed to their nearby local minima.…”

Section: Methodsmentioning

confidence: 99%

Thermodynamic limit for synthesis of metastable inorganic materials

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Section: Methodsmentioning

confidence: 99%

Thermodynamic limit for synthesis of metastable inorganic materials

et al. 2018

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“…To sample more comprehensively the Zn−Mo−N ternary space for possible compositions and their structures, we used a modified version of the Kinetically Limited Minimization (KLM) algorithm, originally designed to sample amorphous structures, 45 so to obtain a wider range of possible stoichiometries and their structures. This search was performed for many Zn i Mo j N k stoichiometries (ijk = 112, 146, 414, 213, 124, 326, 338, 313) chosen to accommodate the Zn 2+ , Mo 4+/5+/6+ , and N 3− oxidation states.…”

Section: Methodsmentioning

confidence: 99%

Redox-Mediated Stabilization in Zinc Molybdenum Nitrides

et al. 2018

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We report on the theoretical prediction and experimental realization of new ternary zinc molybdenum nitride compounds. We used theory to identify previously unknown ternary compounds in the Zn-Mo-N systems, ZnMoN and ZnMoN, and to analyze their bonding environment. Experiments show that Zn-Mo-N alloys can form in broad composition range from ZnMoN to ZnMoN in the wurtzite-derived structure, accommodating very large off-stoichiometry. Interestingly, the measured wurtzite-derived structure of the alloys is metastable for the ZnMoN stoichiometry, in contrast to the ZnMoN stoichiometry, where ordered wurtzite is predicted to be the ground state. The formation of ZnMoN-ZnMoN alloy with wurtzite-derived crystal structure is enabled by the concomitant ability of Mo to change oxidation state from +VI in ZnMoN to +IV in ZnMoN, and the capability of Zn to contribute to the bonding states of both compounds, an effect that we define as "redox-mediated stabilization". The stabilization of Mo in both the +VI and +IV oxidation states is due to the intermediate electronegativity of Zn, which enables significant polar covalent bonding in both ZnMoN and ZnMoN compounds. The smooth change in the Mo oxidation state between ZnMoN and ZnMoN stoichiometries leads to a continuous change in optoelectronic properties-from resistive and semitransparent ZnMoN to conductive and absorptive ZnMoN. The reported redox-mediated stabilization in zinc molybdenum nitrides suggests there might be many undiscovered ternary compounds with one metal having an intermediate electronegativity, enabling significant covalent bonding, and another metal capable of accommodating multiple oxidation states, enabling stoichiometric flexibility.

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“…Hence, an accurate modeling of atomic structures using cutting‐edge simulation techniques is highly desired. Some key features of AMOs have been already explored through theoretical methods, including DFT studies on the origin of defect formation, statistical depictions, and the electron transport of single‐ and multication AMOs . However, some fundamental questions regarding the nature of crystallization, transport dynamics, and carrier generation have yet to be answered, which are significant to understand the performance improvements in a variety of energy applications.…”

Section: Summary and Perspectivementioning

confidence: 99%

Research Advances of Amorphous Metal Oxides in Electrochemical Energy Storage and Conversion

Yan

Abhilash

Tang

et al. 2018

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possess lower hardness, higher strength, higher elasticity, higher tensile strength, lower internal energy, higher interatomic forces, lower viscosity coefficient, larger surface area, higher chemical stability, and strong corrosion resistance compared with their crystalline counterparts. [1][2][3] Based on the anionic constituents, amorphous materials could be categorized as oxides, sulfides, phosphates, etc. Among them, amorphous metal oxide family is of great importance owing to its widespread applications in a variety of areas such as batteries, supercapacitors, electronics, conducting films, multilayered transistors, electrochromic displays, nonvolatile memories, and the like. [4][5][6] As the basic building blocks, metaloxide (M-O) polyhedra are responsible for the essential features of the electronic band structure in amorphous metal oxides (AMOs). [3] AMO materials differ from their crystalline counterparts in the arrangement of M-O polyhedra, in which a random network arrangement of distorted polyhedra with short-range ordering is presented rather than maintaining perfect periodicity. [7,8] The coordination number of the M-O polyhedra, namely, the number of anions bonded to the metal cation, constitutes a crucially decisive factor for the unique properties of AMOs. Multiple polyhedra are interconnected through different types of sharing configurations known as edge sharing, corner sharing, and face sharing of the oxygen atoms. The combination of different sharing geometries also affects the properties of AMOs. [9] In other words, AMOs are formed by the superposition of the distorted M-O polyhedra to form network arrays through a random package. Long-range structural disorder in the AMO reduces scattering mean free path, and the lack of grain boundaries makes the electronic properties identical within large areas. These unique characteristics make them suitable for flexible electronics such as flexible films, intervening layers, thin film transistors, etc. [10][11][12] In recent years, there are numerous reports pointing out the advantages of AMOs over the crystalline counterparts in many electrochemical applications. [13][14][15][16][17] For example, the inherent disorderliness in the structural arrangement and rich defects are evidenced to be highly constructive to improve the alkali ion diffusion through the lattice. [18,19] As for intercalation-type electrodes in lithium-ion batteries (LIBs), amorphous materials Amorphous metal oxides (AMOs) have aroused great enthusiasm across multiple energy areas over recent years due to their unique properties, such as the intrinsic isotropy, versatility in compositions, absence of grain boundaries, defect distribution, flexible nature, etc. Here, the materials engineering of AMOs is systematically reviewed in different electrochemical applications and recent advances in understanding and developing AMO-based high-performance electrodes are highlighted. Attention is focused on the important roles that AMOs play in various energy storage and conversion technologies...

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Modeling amorphous thin films: Kinetically limited minimization

Cited by 14 publications

References 28 publications

Thermodynamic limit for synthesis of metastable inorganic materials

Thermodynamic limit for synthesis of metastable inorganic materials

Redox-Mediated Stabilization in Zinc Molybdenum Nitrides

Research Advances of Amorphous Metal Oxides in Electrochemical Energy Storage and Conversion

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