Materials Science & Engineering Research Works

Permanent URI for this collectionhttp://hdl.handle.net/1903/1660

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Dataset for "Resistance of Boron Nitride Nanotubes to Radiation-Induced Oxidation" as published in The Journal of Physical Chemistry C
(2024) Chao, Hsin-Yun (Joy); Nolan, Adelaide M.; Hall, Alex T.; Golberg, Dmitri; Park, Cheol; Yang, Wei-Chang David; Mo, Yifei; Sharma, Renu; Cumings, John
Interface Diagnostics Platform for Thin-Film Solid-State Batteries
(2024-08-28) Ferrari, Victoria Castagna; Stewart, David Murdock; Rubloff, Gary
This dataset comprises electorchemical impedance spectroscopy measurements from thin film batteries comprised of LiV2O5, LiPON, and Si. The data is associated with a manuscript that describes the methodology and analysis of the data and conclusions we draw from it in complete detail. (At the time of submission, the manuscript was set to be submitted to a peer reviewed journal.) The data herein is intended to be used to model equivalent circuits for each material and the charge transfer interfaces throughout the device in order to construct the model of the full battery. The demonstrated methods to build from simple materials to a complex device are novel in the field and we hope this data and process will be used by other researchers to develop more robust analysis of batteries across academic labs and industry.
Flame retardant biogenic building insulation materials from hemp fiber
(Wiley, 2023-12-27) Jadhav, Porus Sunil; Sarkar, Arpita; Zhu, Long; Ren, Shenqiang
Biogenic thermal insulation materials are in high demand because of its carbon-sequestration nature. However, high flammability, moisture condensation, and relatively high thermal conductivity of biogenic material are major concerns for sustainable building applications. In this study, we report the fire-retardant cellulose xerogel insulation nanocomposites derived from hemp fiber recycling and silica xerogel, in which the boric acid treatment improves its fire retardancy. The as-prepared materials show a low thermal conductivity of 31.3 mW/m K, high flexural modulus of 665 MPa, hydrophobicity with the water contact angle of 115°, and fire retardancy with 30% weight loss over a period of burning time 10 min. Overall, this work provides an effective method for the synthesis of fire-retardant biogenic thermal insulation materials and shows a promising way for next-generation bio-based insulation materials.
Mitigating Electronic Conduction in Ceria-Based Electrolytes via External Structure Design
(Wiley, 2023-12-22) Robinson, Ian A.; Huang, Yi-Lin; Horlick, Samuel A.; Obenland, Jonathan; Robinson, Nicholas; Gritton, J. Evans; Hussain, A. Mohammed; Wachsman, Eric D.
Doped ceria electrolytes are the state of the art low-temperature solid oxide electrolytes because of their high ionic conductivity and good material compatibility. However, cerium tends to reduce once exposed to reducing environments, leading to an increase in electronic conduction and a decrease in efficiency. Here, the leakage current is mitigated in ceria-based electrolytes by controlling the defect chemistry through an engineered cathode side microstructure. This functional layer effectively addresses the problematic electronic conduction issue in ceria-based electrolytes without adding significant ohmic resistance and increases the ionic transference to2- number to over 0.93 in a thin 20 µm ceria-based electrolyte at 500 °C, compared to a of to2- 0.8 for an unmodified one. Based on this design, solid oxide fuel cells (SOFCs) are further demonstrated with the remarkable peak power density of 550 mW at 500 °C and excellent stability for over 2000 h. This approach enables a potential breakthrough in the development of ceria-based low-temperature solid oxide electrolytes.
Spatial and temporal control of glassy-crystalline domains in optical phase change materials
(Wiley, 2023-11-07) Lee, Chih-Yu; Lian, Chuanyu; Sun, Hongyi; Huang, Yi-Siou; Acharjee, Niloy; Takeuchi, Ichiro; Rios Ocampo, Carlos A.
Chalcogenide phase change materials (PCMs) have become one of the most promising material platforms for the Optics and Photonics community. The unparalleled combination of nonvolatility and large optical property modulation promises devices with low-energy consumption and ultra-compact form factors. At the core of all these applications lies the difficult task of precisely controlling the glassy amorphous and crystalline domains that compose the PCM microstructure and dictate the optical response. A spatially controllable glassy-crystalline domain distribution is desired for intermediate optical response (vs. binary response between fully amorphous and crystalline states), and temporally resolved domains are sought after for repeatable reconfiguration. In this perspective, we briefly review the fundamentals of PCM phase transition in various reconfiguring approaches for optical devices. We discuss each method's underpinning mechanisms, design, advantages, and downsides. Finally, we lay out current challenges and future directions in this field.
Additive Manufacturing of High-Temperature Hybrid Electronics via Molecular-Decomposed Metals
(Wiley, 2023-10-20) Khuje, Saurabh; Alshatnawi, Firas; Smilgies, Detlef; Alhendi, Mohammed; Islam, Abdullah; Armstrong, Jason; Yu, Jian; Poliks, Mark; Ren, Shenqiang
As the modern electronic technology extends into operating in harsh working conditions, it calls for a system that is capable of uncompromising performance in extreme environments, thus providing a strong motivation to look for advanced materials and electronics with the capability of high-throughput and rapid prototyping. Coupled with additive manufacturing, molecular decomposition metals bypass the challenging oddities of traditional material-limited and thermally initiated metalworking, enabling high throughput and rapid prototyping of stoichiometry and composition-controlled metals. Here, a new paradigm for the design and additive manufacturing of copper metallic alloy materials onto ceramics is described by printing molecular decomposable metal materials, capable of withstanding thermo-mechanical loading, operating in extreme environments in static and dynamic conditions. The resulting printed hybrid electronics are electrically stable for 25 h of aging at 1000 °C. This curious fact paves a way for printed antenna and sensor electronics that reliably operate up to 1000 °C. These results can be further extended to establish other printable molecular decomposable materials as a platform for rapid prototyping of high temperature electronics that are suitable for harsh environments.
High-Throughput Evaluation of Hardening Coefficients of Eight Alloying Elements in Magnesium
(Wiley, 2023-08-24) Wang, Chuangye; Zhong, Wei; Garnett, Jess; Zhao, Ji-Cheng
Liquid–solid diffusion couples (LSDCs) are employed to generate a composition gradient in the single-phase hexagonal closed-packed (hcp) solid solution with compositions up to the solubility limit of various solutes in Mg. Nanoindentation scanning across the composition gradient in LSDCs allows effective evaluation of composition-dependent hardness of eight alloying elements (Al, Ca, Ce, Gd, Li, Sn, Y, and Zn) in the hcp Mg phase. The hardening coefficients, an indicator of the potency of solid-solution hardening, are evaluated from the measured composition-hardness data and correlated with various materials properties such as atomic radius, shear modulus, and elastic modulus of the solutes. The rank of hardening potency of Al, Gd, Sn, Y, and Zn measured by nanoindentation is in good agreement with that measured by microindentation reported in the literature. The hardening coefficient (potency) from the strongest to the weakest is Ce > Ca > Y ≈ Gd > Zn > Al ≈ Sn > Li in Mg-based hcp binary solid solutions. The hardening coefficient is found to be closely correlated with the strengthening potency.
Additive Manufacturing of High-Temperature Preceramic-Derived SiOC Hybrid Functional Ceramics
(Wiley, 2023-09-22) Li, Zheng; Khuje, Saurabh; Islam, Abdullah; Ren, Shenqiang
High-temperature capable materials, metals, and ceramics are attracting significant interest for applications in extreme environmental conditions. Herein, a hybrid metal-reinforced ceramic matrix material consisting of preceramic-derived high-temperature SiOC and copper nanoplates is reported, enabling the manufacturing of high-temperature sensing electronics. The preceramic polymer precursors including polydimethylsiloxane and polydimethylsilane, together with copper nanoplates, are thermally converted into durable copper-reinforced SiOC ceramics. The presence of copper in SiOC ceramics enhances its electrical conductivity, while SiOC suppresses oxygen uptake and acts as a shield for oxidation to achieve high-temperature thermal resistance and negative temperature coefficient at high temperatures. A comprehensive electric and sensing performance, combined with cost-effectiveness and scalability, can facilitate the utilization of hybrid Cu and SiOC composites in high-temperature electronics.
High Sulfur Loading and Capacity Retention in Bilayer Garnet Sulfurized-Polyacrylonitrile/Lithium-Metal Batteries with Gel Polymer Electrolytes
(Wiley, 2023-09-24) Shi, Changmin; Takeuchi, Saya; Alexander, George V.; Hamann, Tanner; O'Neill, Jonathan; Dura, Joseph A.; Wachsman, Eric D.
The cubic-garnet (Li7La3Zr2O12, LLZO) lithium–sulfur battery shows great promise in the pursuit of achieving high energy densities. The sulfur used in the cathodes is abundant, inexpensive, and possesses high specific capacity. In addition, LLZO displays excellent chemical stability with Li metal; however, the instabilities in the sulfur cathode/LLZO interface can lead to performance degradation that limits the development of these batteries. Therefore, it is critical to resolve these interfacial challenges to achieve stable cycling. Here, an innovative gel polymer buffer layer to stabilize the sulfur cathode/LLZO interface is created. Employing a thin bilayer LLZO (dense/porous) architecture as a solid electrolyte and significantly high sulfur loading of 5.2 mg cm−2, stable cycling is achieved with a high initial discharge capacity of 1542 mAh g−1 (discharge current density of 0.87 mA cm−2) and an average discharge capacity of 1218 mAh g−1 (discharge current density of 1.74 mA cm−2) with 80% capacity retention over 265 cycles, at room temperature (22 °C) and without applied pressure. Achieving such stability with high sulfur loading is a major step in the development of potentially commercial garnet lithium–sulfur batteries.
Design principles for sodium superionic conductors
(Nature Portfolio, 2023-11-22) Wang, Shuo; Fu, Jiamin; Liu, Yunsheng; Saravanan, Ramanuja; Luo, Jing; Deng, Sixu; Sham, Tsun-Kong; Sun, Xueliang; Mo, Yifei
Motivated by the high-performance solid-state lithium batteries enabled by lithium superionic conductors, sodium superionic conductor materials have great potential to empower sodium batteries with high energy, low cost, and sustainability. A critical challenge lies in designing and discovering sodium superionic conductors with high ionic conductivities to enable the development of solid-state sodium batteries. Here, by studying the structures and diffusion mechanisms of Li-ion versus Na-ion conducting solids, we reveal the structural feature of face-sharing high-coordination sites for fast sodium-ion conductors. By applying this feature as a design principle, we discover a number of Na-ion conductors in oxides, sulfides, and halides. Notably, we discover a chloride-based family of Na-ion conductors NaxMyCl6 (M = La–Sm) with UCl3-type structure and experimentally validate with the highest reported ionic conductivity. Our findings not only pave the way for the future development of sodium-ion conductors for sodium batteries, but also consolidate design principles of fast ion-conducting materials for a variety of energy applications.
Discrepancies and error evaluation metrics for machine learning interatomic potentials
(Springer Nature, 2023-09-26) Liu, Yunsheng; He, Xingfeng; Mo, Yifei
Machine learning interatomic potentials (MLIPs) are a promising technique for atomic modeling. While small errors are widely reported for MLIPs, an open concern is whether MLIPs can accurately reproduce atomistic dynamics and related physical properties in molecular dynamics (MD) simulations. In this study, we examine the state-of-the-art MLIPs and uncover several discrepancies related to atom dynamics, defects, and rare events (REs), compared to ab initio methods. We find that low averaged errors by current MLIP testing are insufficient, and develop quantitative metrics that better indicate the accurate prediction of atomic dynamics by MLIPs. The MLIPs optimized by the RE-based evaluation metrics are demonstrated to have improved prediction in multiple properties. The identified errors, the evaluation metrics, and the proposed process of developing such metrics are general to MLIPs, thus providing valuable guidance for future testing and improvements of accurate and reliable MLIPs for atomistic modeling.
Simplified Reflection Fabry-Perot Method for Determination of Electro-Optic Coefficients of Poled Polymer Thin Films
(MDPI, 2011-08-18) Park, Dong Hun; Luo, Jingdong; Jen, Alex K.-Y.; Herman, Warren N.
We report a simplified reflection mode Fabry-Perot interferometry method for determination of electro-optic (EO) coefficients of poled polymer thin films. Rather than fitting the detailed shape of the Fabry-Perot resonance curve, our simplification involves a technique to experimentally determine the voltage-induced shift in the angular position of the resonance minimum. Rigorous analysis based on optical properties of individual layers of the multilayer structure is not necessary in the data analysis. Although angle scans are involved, the experimental setup does not require a θ-2θ rotation stage and the simplified analysis is an advantage for polymer synthetic efforts requiring quick and reliable screening of new materials. Numerical and experimental results show that our proposed method can determine EO coefficients to within an error of ∼8% if poled values for the refractive indices are used.
Decomposition Mechanisms and Kinetics of Novel Energetic Molecules BNFF-1 and ANFF-1: Quantum-Chemical Modeling
(MDPI, 2013-07-18) Tsyshevsky, Roman V.; Kuklja, Maija M.
Decomposition mechanisms, activation barriers, Arrhenius parameters, and reaction kinetics of the novel explosive compounds, 3,4-bis(4-nitro-1,2,5-oxadiazol-3-yl)-1,2,5-oxadiazole (BNFF-1), and 3-(4-amino-1,2,5-oxadiazol-3-yl)-4-(4-nitro-1,2,5-oxadiazol-3-yl)-1,2,5-oxadiazole (ANFF-1) were explored by means of density functional theory with a range of functionals combined with variational transition state theory. BNFF-1 and ANFF-1 were recently suggested to be good candidates for insensitive high energy density materials. Our modeling reveals that the decomposition initiation in both BNFF-1 and ANFF-1 molecules is triggered by ring cleavage reactions while the further process is defined by a competition between two major pathways, the fast C-NO2 homolysis and slow nitro-nitrite isomerization releasing NO. We discuss insights on design of new energetic materials with targeted properties gained from our modeling.
Topography of Photochemical Initiation in Molecular Materials
(MDPI, 2013-11-15) Aluker, Edward D.; Krechetov, Alexander G.; Mitrofanov, Anatoly Y.; Zverev, Anton S.; Kuklja, Maija M.
We propose a fluctuation model of the photochemical initiation of an explosive chain reaction in energetic materials. In accordance with the developed model, density fluctuations of photo-excited molecules serve as reaction nucleation sites due to the stochastic character of interactions between photons and energetic molecules. A further development of the reaction is determined by a competition of two processes. The first process is growth in size of the isolated reaction cell, leading to a micro-explosion and release of the material from the cell towards the sample surface. The second process is the overlap of reaction cells due to an increase in their size, leading to the formation of a continuous reaction zone and culminating in a macro-explosion, i.e., explosion of the entire area, covering a large part of the volume of the sample. Within the proposed analytical model, we derived expressions of the explosion probability and the duration of the induction period as a function of the initiation energy (exposure). An experimental verification of the model was performed by exploring the initiation of pentaerythritol tetranitrate (PETN) with the first harmonic of YAG: Nd laser excitation (1,064 nm, 10 ns), which has confirmed the adequacy of the model. This validation allowed us to make a few quantitative assessments and predictions. For example, there must be a few dozen optically excited molecules produced by the initial fluctuations for the explosive decomposition reaction to occur and the life-time of an isolated cell before the micro-explosion must be of the order of microseconds.
Directed Kinetic Self-Assembly of Mounds on Patterned GaAs (001): Tunable Arrangement, Pattern Amplification and Self-Limiting Growth
(MDPI, 2014-05-12) Lin, Chuan-Fu; Kan, Hung-Chih; Kanakaraju, Subramaniam; Richardson, Christopher; Phaneuf, Raymond
We present results demonstrating directed self-assembly of nanometer-scale mounds during molecular beam epitaxial growth on patterned GaAs (001) surfaces. The mound arrangement is tunable via the growth temperature, with an inverse spacing or spatial frequency which can exceed that of the features of the template. We find that the range of film thickness over which particular mound arrangements persist is finite, due to an evolution of the shape of the mounds which causes their growth to self-limit. A difference in the film thickness at which mounds at different sites self-limit provides a means by which different arrangements can be produced.
3-(4-Amino-1,2,5-oxadiazol-3-yl)-4-(4-nitro-1,2,5-oxadiazol-3-yl)-1,2,5-oxadiazole
(MDPI, 2014-05-22) Pagoria, Philip; Zhang, Maoxi; Racoveanu, Ana; DeHope, Alan; Tsyshevsky, Roman V.; Kuklja, Maija M.
The title compound 3-(4-amino-1,2,5-oxadiazol-3-yl)-4-(4-nitro-1,2,5-oxadiazol-3-yl)-1,2,5-oxadiazole (ANFF-1) was synthesized by: (1) by reaction of 3,4-bis(4-nitro-1,2,5-oxadiazol-3-yl)-1,2,5-oxadiazole (BNFF-1) with gaseous ammonia in toluene and (2) by partial oxidation of 3,4-bis(4-amino-1,2,5-oxadiazol-3-yl)-1,2,5-oxadiazole (BAFF-1) with 35% H2O2 in concentrated H2SO4.
Effect of Extended Extinction from Gold Nanopillar Arrays on the Absorbance Spectrum of a Bulk Heterojunction Organic Solar Cell
(MDPI, 2015-02-18) Tsai, Shu-Ju; Ballarotto, Mihaela; Kan, Hung-Chih; Phaneuf, Raymond J.
We report on the effects of enhanced absorption/scattering from arrays of Au nanopillars of varied size and spacing on the spectral response of a P3HT:PCBM bulk heterojunction solar cell. Nanopillar array-patterned devices do show increased optical extinction within a narrow range of wavelengths compared to control samples without such arrays. The measured external quantum efficiency and calculated absorbance, however, both show a decrease near the corresponding wavelengths. Numerical simulations indicate that for relatively narrow nanopillars, the increased optical extinction is dominated by absorption within the nanopillars, rather than scattering, and is likely dissipated by Joule heating.
Molecular Theory of Detonation Initiation: Insight from First Principles Modeling of the Decomposition Mechanisms of Organic Nitro Energetic Materials
(MDPI, 2016-02-19) Tsyshevsky, Roman V.; Sharia, Onise; Kuklja, Maija M.
This review presents a concept, which assumes that thermal decomposition processes play a major role in defining the sensitivity of organic energetic materials to detonation initiation. As a science and engineering community we are still far away from having a comprehensive molecular detonation initiation theory in a widely agreed upon form. However, recent advances in experimental and theoretical methods allow for a constructive and rigorous approach to design and test the theory or at least some of its fundamental building blocks. In this review, we analyzed a set of select experimental and theoretical articles, which were augmented by our own first principles modeling and simulations, to reveal new trends in energetic materials and to refine known existing correlations between their structures, properties, and functions. Our consideration is intentionally limited to the processes of thermally stimulated chemical reactions at the earliest stage of decomposition of molecules and materials containing defects.
Photochemistry of the α-Al2O3-PETN Interface
(MDPI, 2016-02-29) Tsyshevsky, Roman V.; Zverev, Anton; Mitrofanov, Anatoly; Rashkeev, Sergey N.; Kuklja, Maija M.
Optical absorption measurements are combined with electronic structure calculations to explore photochemistry of an α-Al2O3-PETN interface formed by a nitroester (pentaerythritol tetranitrate, PETN, C5H8N4O12) and a wide band gap aluminum oxide (α-Al2O3) substrate. The first principles modeling is used to deconstruct and interpret the α-Al2O3-PETN absorption spectrum that has distinct peaks attributed to surface F0-centers and surface—PETN transitions. We predict the low energy α-Al2O3 F0-center—PETN transition, producing the excited triplet state, and α-Al2O3 F0-center—PETN charge transfer, generating the PETN anion radical. This implies that irradiation by commonly used lasers can easily initiate photodecomposition of both excited and charged PETN at the interface. The feasible mechanism of the photodecomposition is proposed.
A Review of Metastable Beta Titanium Alloys
(MDPI, 2018-06-30) Kolli, R. Prakash; Devaraj, Arun
In this article, we provide a broad and extensive review of beta titanium alloys. Beta titanium alloys are an important class of alloys that have found use in demanding applications such as aircraft structures and engines, and orthopedic and orthodontic implants. Their high strength, good corrosion resistance, excellent biocompatibility, and ease of fabrication provide significant advantages compared to other high performance alloys. The body-centered cubic (bcc) β-phase is metastable at temperatures below the beta transus temperature, providing these alloys with a wide range of microstructures and mechanical properties through processing and heat treatment. One attribute important for biomedical applications is the ability to adjust the modulus of elasticity through alloying and altering phase volume fractions. Furthermore, since these alloys are metastable, they experience stress-induced transformations in response to deformation. The attributes of these alloys make them the subject of many recent studies. In addition, researchers are pursuing development of new metastable and near-beta Ti alloys for advanced applications. In this article, we review several important topics of these alloys including phase stability, development history, thermo-mechanical processing and heat treatment, and stress-induced transformations. In addition, we address recent developments in new alloys, phase stability, superelasticity, and additive manufacturing.

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