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Title: Unraveling the structural stability and the electronic structure of ThO 2 clusters

Abstract

Unraveling the correlations between the geometry, the relative energy and the electronic structure of actinide oxide nanostructures is crucial for a better control of their size, shape and properties.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Theoretical Division, Los Alamos National Laboratory, Los Alamos, USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1647388
Grant/Contract Number:  
U.S. Department of Energy, Chemical Sciences, Geosciences, and Biosciences Division, Heavy Element Chemistry program, under contract DE-AC52-06NA25396; Los Alamos National Laboratory is operated by Triad National Security, LLC, for the National Nuclear Security Administration of U.S. Department of Energy (Contract No. 89233218CNA000001); NFA acknowledges the support from G.T. Seaborg Postdoctoral Fellowship and JJ acknowledges the support from a Director's Postdoctoral Fellowship.
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Volume: 22 Journal Issue: 33; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English

Citation Formats

Aguirre, Néstor F., Jung, Julie, and Yang, Ping. Unraveling the structural stability and the electronic structure of ThO 2 clusters. United Kingdom: N. p., 2020. Web. https://doi.org/10.1039/D0CP00478B.
Aguirre, Néstor F., Jung, Julie, & Yang, Ping. Unraveling the structural stability and the electronic structure of ThO 2 clusters. United Kingdom. https://doi.org/10.1039/D0CP00478B
Aguirre, Néstor F., Jung, Julie, and Yang, Ping. Tue . "Unraveling the structural stability and the electronic structure of ThO 2 clusters". United Kingdom. https://doi.org/10.1039/D0CP00478B.
@article{osti_1647388,
title = {Unraveling the structural stability and the electronic structure of ThO 2 clusters},
author = {Aguirre, Néstor F. and Jung, Julie and Yang, Ping},
abstractNote = {Unraveling the correlations between the geometry, the relative energy and the electronic structure of actinide oxide nanostructures is crucial for a better control of their size, shape and properties.},
doi = {10.1039/D0CP00478B},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 33,
volume = 22,
place = {United Kingdom},
year = {2020},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/D0CP00478B

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Works referenced in this record:

Thorium(IV) Molecular Clusters with a Hexanuclear Th Core
journal, October 2011

  • Knope, Karah E.; Wilson, Richard E.; Vasiliu, Monica
  • Inorganic Chemistry, Vol. 50, Issue 19
  • DOI: 10.1021/ic2014946

Infrared spectra and pseudopotential calculations for NUO+, NUO, and NThO in solid neon
journal, December 1999

  • Zhou, Mingfei; Andrews, Lester
  • The Journal of Chemical Physics, Vol. 111, Issue 24
  • DOI: 10.1063/1.480463

Anisotropic nanomaterials for shape-dependent physicochemical and biomedical applications
journal, January 2019

  • Yang, Lijiao; Zhou, Zijian; Song, Jibin
  • Chemical Society Reviews, Vol. 48, Issue 19
  • DOI: 10.1039/C9CS00011A

Infrared spectra and structure of some matrix‐isolated lanthanide and actinide oxides
journal, February 1974

  • Gabelnick, S. D.; Reedy, G. T.; Chasanov, M. G.
  • The Journal of Chemical Physics, Vol. 60, Issue 3
  • DOI: 10.1063/1.1681128

Perspectives of the thorium fuel cycle
journal, March 1998


Bulk-nanocrystalline oxide nuclear fuels – An innovative material option for increasing fission gas retention, plasticity and radiation-tolerance
journal, March 2012


Design of Hollow Nanostructures for Energy Storage, Conversion and Production
journal, July 2018


Transition metal oxide nanoparticles as efficient catalysts in oxidation reactions
journal, April 2018


Sensitivity evaluations of design parameters for various thorium based epithermal reactor (TBER) concepts
journal, June 2018


Investigation of the Ligand–Nanoparticle Interface: A Cryogenic Approach for Preserving Surface Chemistry
journal, February 2018

  • Karakoti, Ajay S.; Yang, Ping; Wang, Weina
  • The Journal of Physical Chemistry C, Vol. 122, Issue 6
  • DOI: 10.1021/acs.jpcc.7b09930

Exploring the Actinide−Actinide Bond:  Theoretical Studies of the Chemical Bond in Ac 2 , Th 2 , Pa 2 , and U 2
journal, December 2006

  • Roos, Björn O.; Malmqvist, Per-Åke; Gagliardi, Laura
  • Journal of the American Chemical Society, Vol. 128, Issue 51
  • DOI: 10.1021/ja066615z

Prediction of Vibrational Frequencies of UO 2 2+ at the CCSD(T) Level
journal, May 2008

  • Jackson, Virgil E.; Craciun, Raluca; Dixon, David A.
  • The Journal of Physical Chemistry A, Vol. 112, Issue 17
  • DOI: 10.1021/jp710334b

Metal–dioxygen and metal–dinitrogen complexes: where are the electrons?
journal, January 2010

  • Holland, Patrick L.
  • Dalton Transactions, Vol. 39, Issue 23
  • DOI: 10.1039/c001397h

Clusters of Actinides with Oxide, Peroxide, or Hydroxide Bridges
journal, October 2012

  • Qiu, Jie; Burns, Peter C.
  • Chemical Reviews, Vol. 113, Issue 2
  • DOI: 10.1021/cr300159x

Synthesis of thoria nano-particles at low temperature through base electrogeneration on steel 316L surface: Effect of current density
journal, October 2016


Ligand induced shape transformation of thorium dioxide nanocrystals
journal, January 2018

  • Wang, Gaoxue; Batista, Enrique R.; Yang, Ping
  • Physical Chemistry Chemical Physics, Vol. 20, Issue 26
  • DOI: 10.1039/C8CP00240A

Why uranyl ion(2+) is linear and isoelectronic thorium dioxide is bent
journal, October 1981

  • Wadt, Willard R.
  • Journal of the American Chemical Society, Vol. 103, Issue 20
  • DOI: 10.1021/ja00410a011

Low temperature decomposition of U(IV) and Th(IV) oxalates to nanograined oxide powders
journal, May 2015


Approaching nanoscale oxides: models and theoretical methods
journal, January 2009

  • Bromley, Stefan T.; Moreira, Ibério de P. R.; Neyman, Konstantin M.
  • Chemical Society Reviews, Vol. 38, Issue 9
  • DOI: 10.1039/b806400h

Bonding and bending in the actinyls
journal, February 1999


On the Origin of Covalent Bonding in Heavy Actinides
journal, July 2017

  • Kelley, Morgan P.; Su, Jing; Urban, Matthew
  • Journal of the American Chemical Society, Vol. 139, Issue 29
  • DOI: 10.1021/jacs.7b03251

Thorium(IV)–Selenate Clusters Containing an Octanuclear Th(IV) Hydroxide/Oxide Core
journal, March 2012

  • Knope, Karah E.; Vasiliu, Monica; Dixon, David A.
  • Inorganic Chemistry, Vol. 51, Issue 7
  • DOI: 10.1021/ic202706s

Actinide Colloids and Particles of Environmental Concern
journal, October 2012

  • Walther, Clemens; Denecke, Melissa A.
  • Chemical Reviews, Vol. 113, Issue 2
  • DOI: 10.1021/cr300343c

Transitions from Stable to Metastable States in the Cr 2 O n and Cr 2 O n Series, n = 1–14
journal, October 2016

  • Gutsev, G. L.; Bozhenko, K. V.; Gutsev, L. G.
  • The Journal of Physical Chemistry A, Vol. 121, Issue 4
  • DOI: 10.1021/acs.jpca.6b11036

Controlled Synthesis of Thorium and Uranium Oxide Nanocrystals
journal, March 2013

  • Hudry, Damien; Apostolidis, Christos; Walter, Olaf
  • Chemistry - A European Journal, Vol. 19, Issue 17
  • DOI: 10.1002/chem.201203888

Stability of oxygen point defects in UO 2 by first-principles DFT + U calculations: Occupation matrix control and Jahn-Teller distortion
journal, July 2010


M 3 C: A Computational Approach To Describe Statistical Fragmentation of Excited Molecules and Clusters
journal, February 2017

  • Aguirre, Néstor F.; Díaz-Tendero, Sergio; Hervieux, Paul-Antoine
  • Journal of Chemical Theory and Computation, Vol. 13, Issue 3
  • DOI: 10.1021/acs.jctc.6b00984

Understanding the size effects on the electronic structure of ThO 2 nanoparticles
journal, January 2019

  • Amidani, Lucia; Plakhova, Tatiana V.; Romanchuk, Anna Yu.
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 20
  • DOI: 10.1039/C9CP01283D

DFT + U calculations of the ground state and metastable states of uranium dioxide
journal, June 2009


Atomic Structure of the Magic (ZnO) 60 Cluster: First-Principles Prediction of a Sodalite Motif for ZnO Nanoclusters
journal, March 2010

  • Wang, Baolin; Wang, Xiaoqiu; Zhao, Jijun
  • The Journal of Physical Chemistry C, Vol. 114, Issue 13
  • DOI: 10.1021/jp908472h

Thorium fuel cycle of a thorium-basedadvanced nuclear energy system
journal, January 2004


Thorium Fuel for Nuclear Energy
journal, January 2003


Chemistry of Actinide Centers in Heterogeneous Catalytic Transformations of Small Molecules
journal, April 2019


Matrix Infrared Spectra and Theoretical Studies of Thorium Oxide Species: ThO x and Th 2 O y
journal, December 2011

  • Andrews, Lester; Gong, Yu; Liang, Binyong
  • The Journal of Physical Chemistry A, Vol. 115, Issue 50
  • DOI: 10.1021/jp208926m

Binding Energy of Metal Oxide Nanoparticles
journal, March 2009

  • Parra, R. D.; Farrell, H. H.
  • The Journal of Physical Chemistry C, Vol. 113, Issue 12
  • DOI: 10.1021/jp807070a

Variable character of O--O and M--O bonding in side-on ( 2) 1:1 metal complexes of O2
journal, March 2003

  • Cramer, C. J.; Tolman, W. B.; Theopold, K. H.
  • Proceedings of the National Academy of Sciences, Vol. 100, Issue 7
  • DOI: 10.1073/pnas.0535926100

Geometrical Structures of Gas-Phase Cerium Oxide Cluster Cations Studied by Ion Mobility Mass Spectrometry
journal, June 2019

  • Nagata, Toshiaki; Wu, Jenna W. J.; Nakano, Motoyoshi
  • The Journal of Physical Chemistry C, Vol. 123, Issue 27
  • DOI: 10.1021/acs.jpcc.9b01378

Reactions of Laser-Ablated U and Th with CO 2 :  Neon Matrix Infrared Spectra and Density Functional Calculations of OUCO, OThCO, and Other Products
journal, November 2000

  • Andrews, Lester; Zhou, Mingfei; Liang, Binyong
  • Journal of the American Chemical Society, Vol. 122, Issue 46
  • DOI: 10.1021/ja0016699

Computed Vibrational Frequencies of Actinide Oxides AnO 0/+/2+ and AnO 2 0/+/2+ (An = Th, Pa, U, Np, Pu, Am, Cm)
journal, June 2011

  • Kovács, Attila; Konings, Rudy J. M.
  • The Journal of Physical Chemistry A, Vol. 115, Issue 24
  • DOI: 10.1021/jp202538k

Metal oxides for optoelectronic applications
journal, March 2016

  • Yu, Xinge; Marks, Tobin J.; Facchetti, Antonio
  • Nature Materials, Vol. 15, Issue 4
  • DOI: 10.1038/nmat4599

Systematic Study of Oxo, Peroxo, and Superoxo Isomers of 3d-Metal Dioxides and Their Anions
journal, December 2000

  • Gutsev, G. L.; Rao, B. K.; Jena, P.
  • The Journal of Physical Chemistry A, Vol. 104, Issue 51
  • DOI: 10.1021/jp002252s

Relativistic Density Functional Study on Uranium(IV) and Thorium(IV) Oxide Clusters of Zonohedral Geometry
journal, June 2012


Thorium breeder reactors as a power source for 21st century and beyond
journal, December 2017

  • Jagannathan, Viswanathan
  • International Journal of Energy Research, Vol. 42, Issue 1
  • DOI: 10.1002/er.3951

Ab Initio Ligand-Field Theory Analysis and Covalency Trends in Actinide and Lanthanide Free Ions and Octahedral Complexes
journal, July 2017


Metal and Metal Oxide Nanoparticles: A Lever for C–H Functionalization
journal, May 2016


Electronic structure of oxide, peroxide, and superoxide clusters of the 3d elements: A comparative density functional study
journal, March 2008

  • Uzunova, Ellie L.; Mikosch, Hans; Nikolov, Georgi St.
  • The Journal of Chemical Physics, Vol. 128, Issue 9
  • DOI: 10.1063/1.2831583

A theoretical investigation into the first-row transition metal–O 2 adducts
journal, January 2019

  • Li, Xiao-Xi; Cho, Kyung-Bin; Nam, Wonwoo
  • Inorganic Chemistry Frontiers, Vol. 6, Issue 8
  • DOI: 10.1039/C9QI00407F

Theoretical Investigations of Geometry, Electronic Structure and Stability of UO 6 : Octahedral Uranium Hexoxide and Its Isomers
journal, August 2010

  • Xiao, Hai; Hu, Han-Shi; Schwarz, W. H. Eugen
  • The Journal of Physical Chemistry A, Vol. 114, Issue 33
  • DOI: 10.1021/jp102107n

Probing the Electronic Structure of Early Transition-Metal Oxide Clusters:  Polyhedral Cages of (V 2 O 5 ) n - ( n = 2−4) and (M 2 O 5 ) 2 - (M = Nb, Ta)
journal, October 2007

  • Zhai, Hua-Jin; Döbler, Jens; Sauer, Joachim
  • Journal of the American Chemical Society, Vol. 129, Issue 43
  • DOI: 10.1021/ja0750874