The ReaxFF reactive force-field : development, applications and future directions

The reactive force-field (ReaxFF) interatomic potential is a powerful computational tool for exploring, developing and optimizing material properties. Methods based on the principles of quantum mechanics (QM), while offering valuable theoretical guidance at the electronic level, are often too computationally intense for simulations that consider the full dynamic evolution of a system. Alternatively, empirical interatomic potentials that are based on classical principles require significantly fewer computational resources, which enables simulations to better describe dynamic processes over longer timeframes and on larger scales. Such methods, however, typically require a predefined connectivity between atoms, precluding simulations that involve reactive events. The ReaxFF method was developed to help bridge this gap. Approaching the gap from the classical side, ReaxFF casts the empirical interatomic potential within a bond-order formalism, thus implicitly describing chemical bonding without expensive QM calculations. This article provides an overview of the development, application, and future directions of the ReaxFF method

Scalable Reactive Molecular Dynamics Simulations for Computational Synthesis

Reactive molecular dynamics (MD) simulation is a powerful research tool for describing chemical reactions. We eliminate the speed-limiting charge iteration in MD with a novel extended-Lagrangian scheme. The extended-Lagrangian reactive MD (XRMD) code drastically improves energy conservation while substantially reducing time-to-solution. Furthermore, we introduce a new polarizable charge equilibration (PQEq) model to accurately predict atomic charges and polarization. The XRMD code based on hybrid message passing+multithreading achieves a weak-scaling parallel efficiency of 0.977 on 786 432 IBM Blue Gene/Q cores for a 67.6 billion-atom system. The performance is portable to the second-generation Intel Xeon Phi, Knights Landing. Blue Gene/Q simulations for the computational synthesis of materials via novel exfoliation mechanisms for synthesizing atomically thin transition metal dichalcogenide layers will dominate nanomaterials science in this century

An extended-Lagrangian scheme for charge equilibration in reactive molecular dynamics simulations

a b s t r a c t Reactive molecular dynamics (RMD) simulations describe chemical reactions at orders-of-magnitude faster computing speed compared with quantum molecular dynamics (QMD) simulations. A major computational bottleneck of RMD is charge-equilibration (QEq) calculation to describe charge transfer between atoms. Here, we eliminate the speed-limiting iterative minimization of the Coulombic energy in QEq calculation by adapting an extended-Lagrangian scheme that was recently proposed in the context of QMD simulations, Souvatzis and Niklasson (2014). The resulting XRMD simulation code drastically improves energy conservation compared with our previous RMD code, , while substantially reducing the time-to-solution. The XRMD code has been implemented on parallel computers based on spatial decomposition, achieving a weak-scaling parallel efficiency of 0.977 on 786,432 IBM Blue Gene/Q cores for a 67.6 billion-atom system

Recovery Act: Molecular Simulation of Dissolved Inorganic Carbons for Underground Brine CO2 Sequestration

To further our understanding and develop the method for measuring the DICs under geological sequestration conditions, we studied the infrared spectra of DICs under high pressure and temperature conditions. First principles simulations of DICs in brine conditions were performed using a highly optimized ReaxFF-DIC forcefield. The thermodynamics stability of each species were determined using the 2PT method, and shown to be consistent with the Reax simulations. More importantly, we have presented the IR spectra of DIC in real brine conditions as a function of temperature and pressure. At near earth conditions, we find a breaking of the O-C-O bending modes into asymmetric and symmetric modes, separated by 100cm{sup -1} at 400K and 5 GPa. These results can now be used to calibrate FTIR laser measurements

Experimental and numerical study of nanoparticles for potential energy applications

PhDThis thesis investigates both experimentally and numerically the oxidation, sintering, melting and solidification processes of different nanoparticles under various thermodynamic scenarios, with a background for energy applications. Two sets of main techniques are adopted in this work, which are isoconvensional kinetic analysis and molecular dynamics simulation. Based on the techniques of simultaneous Thermogravimetric Analysis (TGA) and Differential Scanning Calorimetry (DSC), for first time the isoconvensional kinetic analysis is applied to study the oxidation of nickel and tin nanoparticles. This method is demonstrated capable of modelling one-step nanoscale oxidation and revealing underling kinetic mechanisms. Moreover, some distinct features of nanoparticle oxidation compared with their bulk counterparts are found such as melting depression, oxidation kinetic change in the vicinity of Curie point of nickel and pressure-related two-step oxidation of tin nanoparticles. The detailed study from Molecular Dynamics (MD) simulation establishes a three-stage sintering process of two nickel nanoparticles, which is unable to be described by bulk continuum-level models. MD is applied to study the interaction between nickel and aluminium and its consequent thermo-mechanical and structural property evolution in a nickel-coating aluminium particle in a heating and cooling cycle. The simulation successfully predicts the atomic diffusion during melting and the formation of glass and crystal phases, and allows for the estimation of interior core-shell pressure. Reactive MD is then applied to simulate the oxidation of silicon nanoparticles. It predicts well the exothermal reaction process and experimentally reveals the oxygen exchange process

Laboratory Directed Research and Development Program FY 2004 Annual Report

The Oak Ridge National Laboratory (ORNL) Laboratory Directed Research and Development (LDRD) Program reports its status to the U.S. Department of Energy (DOE) in March of each year. The program operates under the authority of DOE Order 413.2A, 'Laboratory Directed Research and Development' (January 8, 2001), which establishes DOE's requirements for the program while providing the Laboratory Director broad flexibility for program implementation. LDRD funds are obtained through a charge to all Laboratory programs. This report describes all ORNL LDRD research activities supported during FY 2004 and includes final reports for completed projects and shorter progress reports for projects that were active, but not completed, during this period. The FY 2004 ORNL LDRD Self-Assessment (ORNL/PPA-2005/2) provides financial data about the FY 2004 projects and an internal evaluation of the program's management process. ORNL is a DOE multiprogram science, technology, and energy laboratory with distinctive capabilities in materials science and engineering, neutron science and technology, energy production and end-use technologies, biological and environmental science, and scientific computing. With these capabilities ORNL conducts basic and applied research and development (R&D) to support DOE's overarching national security mission, which encompasses science, energy resources, environmental quality, and national nuclear security. As a national resource, the Laboratory also applies its capabilities and skills to the specific needs of other federal agencies and customers through the DOE Work For Others (WFO) program. Information about the Laboratory and its programs is available on the Internet at <http://www.ornl.gov/>. LDRD is a relatively small but vital DOE program that allows ORNL, as well as other multiprogram DOE laboratories, to select a limited number of R&D projects for the purpose of: (1) maintaining the scientific and technical vitality of the Laboratory; (2) enhancing the Laboratory's ability to address future DOE missions; (3) fostering creativity and stimulating exploration of forefront science and technology; (4) serving as a proving ground for new research; and (5) supporting high-risk, potentially high-value R&D. Through LDRD the Laboratory is able to improve its distinctive capabilities and enhance its ability to conduct cutting-edge R&D for its DOE and WFO sponsors. To meet the LDRD objectives and fulfill the particular needs of the Laboratory, ORNL has established a program with two components: the Director's R&D Fund and the Seed Money Fund. As outlined in Table 1, these two funds are complementary. The Director's R&D Fund develops new capabilities in support of the Laboratory initiatives, while the Seed Money Fund is open to all innovative ideas that have the potential for enhancing the Laboratory's core scientific and technical competencies. Provision for multiple routes of access to ORNL LDRD funds maximizes the likelihood that novel and seminal ideas with scientific and technological merit will be recognized and supported