The melting point of lithium: an orbital-free first-principles molecular dynamics study

Chen, Mohan; Hung, Linda; Huang, Chen; Xia, Junchao; Carter, Emily A.

doi:10.1080/00268976.2013.828379

Cited by 45 publications

(61 citation statements)

References 57 publications

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“…Despite this limitation, large defects in crystals (e.g., dislocations, grain boundaries) and large nanostructures (e.g., nanowires, quantum dots) are too computationally costly to treat with most first principles approaches, and so OF‐DFT offers an appealing alternative for such systems. The code has been used to simulate more than 1 million atoms of bulk Al and to study melting of Li using MD …”

Section: Large Scale Qm: Methodological and Computational Approachesmentioning

confidence: 99%

Challenges in large scale quantum mechanical calculations

Ratcliff

Mohr

Huhs

et al. 2016

WIREs Comput Mol Sci

110

103

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During the past decades, quantum mechanical methods have undergone an amazing transition from pioneering investigations of experts into a wide range of practical applications, made by a vast community of researchers. First principles calculations of systems containing up to a few hundred atoms have become a standard in many branches of science. The sizes of the systems which can be simulated have increased even further during recent years, and quantum-mechanical calculations of systems up to many thousands of atoms are nowadays possible. This opens up new appealing possibilities, in particular for interdisciplinary work, bridging together communities of different needs and sensibilities. In this review we will present the current status of this topic, and will also give an outlook on the vast multitude of applications, challenges, and opportunities stimulated by electronic structure calculations, making this field an important working tool and bringing together researchers of many different domains.We would like to thank Modesto Orozco and Hansel Gómez for fruitful discussions and Fátima Lucas for providing various test systems and helping with some visualizations. This work was supported by the EXTMOS\ud project, grant agreement number 646176, and the Energy oriented Centre of Excellence (EoCoE), grant agreement number 676629, funded both within the Horizon2020 framework of the European Union. This research\ud used resources of the Argonne Leadership Computing Facility at Argonne National Laboratory, which is supported by the Ofﬁce of Science of the U.S. Department of Energy under contract DE-AC02-06CH11357.Peer ReviewedPostprint (author's final draft

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Section: Large Scale Qm: Methodological and Computational Approachesmentioning

confidence: 99%

Challenges in large scale quantum mechanical calculations

Ratcliff

Mohr

Huhs

et al. 2016

WIREs Comput Mol Sci

110

103

View full text Add to dashboard Cite

show abstract

“…The Perdew-Burke-Ernzerhof (PBE) [90] generalized gradient approximation (GGA) XC functional and previous GGA-PBE Si [84] and Li [44] BLPSs are used for direct comparison to previously published results [85] of KSDFT-PAW (projector augmented wave) [91], KSDFT-BLPS, and OFDFT-BLPS with the original WGCD KEDF. All OFDFT calculations are performed within PROFESS 3.0 [92][93][94].…”

Section: Swgcd Testsmentioning

confidence: 99%

Orbital-free density functional theory study of amorphous Li–Si alloys and introduction of a simple density decomposition formalism

Xia¹,

Carter²

2016

Modelling Simul. Mater. Sci. Eng.

Self Cite

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We propose a simple density decomposition formalism within orbital-free (OF) density functional theory (DFT) based on the Wang-Govind-Carter-decomposition (WGCD) kinetic energy density functional (KEDF). The resulting simple-WGCD (sWGCD) KEDF provides efficient density optimization, full cell relaxation, reasonable bulk properties for various materials compared to both the original OFDFT-WGCD and the Kohn-Sham (KS) DFT values, and has various numerical benefits including more stable convergence and lower computational cost (twice as fast as the WGCD KEDF).We also study amorphous (a-) Li-Si alloys with KSDFT and OFDFT using the HuangCarter (HC), WGCD, and sWGCD KEDFs. The a-Li-Si alloy samples are prepared with the anneal-and-quench method using NVT molecular dynamics simulations. We report structural properties, equilibrium volumes, bulk moduli, and alloy formation energies for each a-alloy. The HC, WGCD, and sWGCD KEDFs within OFDFT all predict accurate equilibrium volumes compared against KSDFT benchmarks. The HC KEDF bulk moduli 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 2 agree with KSDFT benchmarks whereas the WGCD/sWGCD KEDFs generally overestimate the bulk moduli, especially for alloys with low Li concentrations. All three KEDFs show limited ability to predict alloy formation energies, which indicates the lack of transferability of these KEDFs among such systems and motivates future developments in OFDFT and KEDF formalisms.

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“…However, this is an area of ongoing developments 18 and there have been applications in specific cases such as the physical properties of liquid Li. 19 The majority of DFT calculations are performed with the Kohn-Sham approach which describes the energy of the system as a functional of the electronic density n(r) and molecular orbitals {ψ i },…”

Section: Density Functional Theory For Metallic Systemsmentioning

confidence: 99%

Perspective: Methods for large-scale density functional calculations on metallic systems

Aarons

Sarwar

Thompsett

et al. 2016

The Journal of Chemical Physics

113

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Perspective: Explicitly correlated electronic structure theory for complex systems The Journal of Chemical Physics 146, 080901 (2017) Current research challenges in areas such as energy and bioscience have created a strong need for Density Functional Theory (DFT) calculations on metallic nanostructures of hundreds to thousands of atoms to provide understanding at the atomic level in technologically important processes such as catalysis and magnetic materials. Linear-scaling DFT methods for calculations with thousands of atoms on insulators are now reaching a level of maturity. However such methods are not applicable to metals, where the continuum of states through the chemical potential and their partial occupancies provide significant hurdles which have yet to be fully overcome. Within this perspective we outline the theory of DFT calculations on metallic systems with a focus on methods for large-scale calculations, as required for the study of metallic nanoparticles. We present early approaches for electronic energy minimization in metallic systems as well as approaches which can impose partial state occupancies from a thermal distribution without access to the electronic Hamiltonian eigenvalues, such as the classes of Fermi operator expansions and integral expansions. We then focus on the significant progress which has been made in the last decade with developments which promise to better tackle the lengthscale problem in metals. We discuss the challenges presented by each method, the likely future directions that could be followed and whether an accurate linear-scaling DFT method for metals is in sight. Published by AIP Publishing. [http://dx

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The melting point of lithium: an orbital-free first-principles molecular dynamics study

Cited by 45 publications

References 57 publications

Challenges in large scale quantum mechanical calculations

Challenges in large scale quantum mechanical calculations

Orbital-free density functional theory study of amorphous Li–Si alloys and introduction of a simple density decomposition formalism

Perspective: Methods for large-scale density functional calculations on metallic systems

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