Norm-Conserving Pseudopotentials and Basis Sets to Explore Actinide Chemistry in Complex Environments

Lu, Jun-Bo1,2,3; Cantu, David C.4; Xu, Cong-Qiao3; Manh-Thuong Nguyen5; Hu, Han-Shi1,2; Glezakou, Vassiliki-Alexandra5; Rousseau, Roger5; Li, Jun1,2,3

2021-06-08

10.1021/acs.jctc.1c00026

Journal of Chemical Theory and Computation   影响因子和分区

1549-9618

1549-9626

We have developed a new set of norm-conserving pseudopotentials and companion Gaussian basis sets for the actinide (An) series (Ac-Lr) using the Goedecker, Teter, and Hutter (GTH) formalism with the Perdew, Burke, and Ernzerhof (PBE) exchange-correlation functional of generalized gradient approximation. To test the accuracy and reliability of the newly parameterized An-GTH pseudopotentials and basis sets, a variety of benchmarks on actinide-containing molecules were carried out and compared to all-electron and available experimental results. The new pseudopotentials include both medium- ([Xe]4f(14)) and large-core ([Xe]4f(14)5d(10)) options that successfully reproduce the structures and energetics, particularly redox processes. The medium-core size set, in particular, reproduces all-electron calculations over multiple oxidation states from 0 to VII, whereas the large-core set is suitable only for the early series elements and low oxidation states. The underlying reason for these transferability issues is discussed in detail. This work fills a critical void in the literature for studying the chemistry of 5f-block elements in the condensed phase.

SCI

英语

通讯

National Natural Science Foundation of China[22033005,21590792] ; US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division[72353] ; US Department of Energy[DE-AC05-76RL01830] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002] ; National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility[DE-AC02-05CH11231]

Chemistry ; Physics

Chemistry, Physical ; Physics, Atomic, Molecular & Chemical

WOS:000661542700011

AMER CHEMICAL SOC

Web of Science

1.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
2.Tsinghua Univ, Key Lab Organ Optoelect & Mol Engn, Minist Educ, Beijing 100084, Peoples R China
3.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
4.Univ Nevada, Chem & Mat Engn, Reno, NV 89557 USA
5.Pacific Northwest Natl Lab, Basic & Appl Mol Fdn, Richland, WA 99352 USA

Lu, Jun-Bo,Cantu, David C.,Xu, Cong-Qiao,et al. Norm-Conserving Pseudopotentials and Basis Sets to Explore Actinide Chemistry in Complex Environments[J]. Journal of Chemical Theory and Computation,2021,17(6).

Lu, Jun-Bo.,Cantu, David C..,Xu, Cong-Qiao.,Manh-Thuong Nguyen.,Hu, Han-Shi.,...&Li, Jun.(2021).Norm-Conserving Pseudopotentials and Basis Sets to Explore Actinide Chemistry in Complex Environments.Journal of Chemical Theory and Computation,17(6).

Lu, Jun-Bo,et al."Norm-Conserving Pseudopotentials and Basis Sets to Explore Actinide Chemistry in Complex Environments".Journal of Chemical Theory and Computation 17.6(2021).