Skip to main content Accessibility help
×
Home
Hostname: page-component-559fc8cf4f-rz424 Total loading time: 0.322 Render date: 2021-03-02T07:13:15.491Z Has data issue: true Feature Flags: { "shouldUseShareProductTool": true, "shouldUseHypothesis": true, "isUnsiloEnabled": true, "metricsAbstractViews": false, "figures": false, "newCiteModal": false, "newCitedByModal": true }

Article contents

Towards Reliable Modeling of Challenging f Electrons Bearing Materials: Experience from Modeling of Nuclear Materials.

Published online by Cambridge University Press:  16 January 2017

Piotr M. Kowalski
Affiliation:
Institute of Nuclear Waste Management and Reactor Safety (IEK-6), Forschungszentrum Jülich, Jülich, Germany JARA High-Performance Computing, Schinkelstraße 2, 52062, Aachen, Germany
George Beridze
Affiliation:
Institute of Nuclear Waste Management and Reactor Safety (IEK-6), Forschungszentrum Jülich, Jülich, Germany JARA High-Performance Computing, Schinkelstraße 2, 52062, Aachen, Germany
Yaqi Ji
Affiliation:
Institute of Nuclear Waste Management and Reactor Safety (IEK-6), Forschungszentrum Jülich, Jülich, Germany JARA High-Performance Computing, Schinkelstraße 2, 52062, Aachen, Germany
Yan Li
Affiliation:
Institute of Nuclear Waste Management and Reactor Safety (IEK-6), Forschungszentrum Jülich, Jülich, Germany JARA High-Performance Computing, Schinkelstraße 2, 52062, Aachen, Germany
Corresponding
E-mail address:
Get access

Abstract

Because of steady increase in the availability of computing power, ab initio methods of computational materials science become everyday investigation tools in various research fields. This popularity of the first-principle-based atomistic modeling is in large part due to the performance of density functional theory (DFT), which could be used for simulations of chemically and structurally complex materials, including minerals, fluids and melts. However, because of intrinsic approximations, DFT is not always able to deliver reliable predictions. This is especially pronounced for f-elements bearing materials such as nuclear materials considered in nuclear waste management. Properties such as reaction enthalpies or electronic state are often badly predicted. In this contribution we discuss our experience with different computational methods, including the parameter free DFT+U method, in which the Hubbard U parameter is derived ab initio, for prediction of various properties of f electrons bearing materials. We show significant improvement obtained for structural and thermochemical parameters of various lanthanide-bearing ceramic materials and actinide-bearing molecular and solid compounds when the f electrons correlations are explicitly accounted for. Last, but not least, we demonstrate that complementary experimental and atomistic modeling studies result in superior and more complete characterization of challenging materials considered in nuclear waste management.

Type
Articles
Copyright
Copyright © Materials Research Society 2017 

Access options

Get access to the full version of this content by using one of the access options below.

References

Ewing, R. C., PNAS 96, 3432-3439 (1999)CrossRef
Chroneos, A., Rushton, M., Jiang, C. and Tsoukalas, L., J. Nucl. Mater. 441, 29 (2013).CrossRef
Jahn, S. and Kowalski, P. M., Rev. Mineral. Geochem. 78, 691 (2014).CrossRef
Becke, A. D., Phys. Rev. A 38, 30983100 (1988).CrossRef
Wen, X.-D., Martin, R. L., Henderson, T. M. and Scuseria, G. E., Chem. Rev. 113, 1063 (2013).CrossRef
Shamov, G. A., Schreckenbach, G. and Vo, T. N., Chem. Eur. J. 13, 4932 (2007).CrossRef
Iche-Tarrat, N. and Marsden, C. J., J. Phys. Chem. A 112, 7632 (2008).CrossRef
Beridze, G. and Kowalski, P. M., J. Phys. Chem. A 118, 11797 (2014).CrossRef
Cococcioni, M. and de Gironcoli, S., Phys. Rev. B 71, 035105 (2005).CrossRef
Giannozzi, P. et al., J. Phys. Condens. Matter 21, 395502 (2009), http://www.quantum-espresso.org (accessed on 25.11.2016).CrossRef
Perdew, J. P., Burke, K. and Ernzerhof, M., Phys. Rev. Lett. 77, 3865 (1996).CrossRef
Perdew, J. P. et al., Phys. Rev. Lett. 100, 136406 (2008).CrossRef
Vanderbilt, D., Phys. Rev. B 41, 7892 (1990).CrossRef
Baer, Y. and Schoenes, J., Solid State Commun. 33, 885 (1980).CrossRef
Yu, J., Devanathan, R. and Weber, W. J., J. Phys. Conden. Matter 21, 435401 (2009).CrossRef
Beridze, G., Birnie, A., Koniski, S., Ji, Y. and Kowalski, P. M., Prog. Nucl. Energy 92, 142 (2016).CrossRef
Kowalski, P. M., Beridze, G., Li, Y., Ji, Y., Friedrich, C., Sasioglu, E. and Blügel, S., Ceram. Trans. 258, 207 (2016).
Ewing, R. and Wang, L., Rev. Mineral. Geochem. 48, 673 (2002).CrossRef
Blanca-Romero, A., Kowalski, P. M., Beridze, G., Schlenz, H. and Bosbach, D., J. Comput. Chem. 35, 1339 (2014).CrossRef
Kowalski, P. M., Beridze, G., Vinograd, V. L. and Bosbach, D., J. Nucl. Mater. 464, 147 (2015).CrossRef
Li, Y., Kowalski, P. M., Blanca-Romero, A., Vinograd, V. L. and Bosbach, D., J. Solid State Chem. 220, 137 (2014).CrossRef
Kowalski, P. M. and Li, Y., J. Eur. Ceram. Soc. 36, 2093 (2016).CrossRef
Li, Y., Kowalski, P. M., Beridze, G., Birnie, A. R., Finkeldei, S. and Bosbach, D., Scr. Mater. 107, 18 (2015).CrossRef
24. Finkeldei, S., Kegler, P., Kowalski, P. M. et al., Acta Materialia, in press (2016).
Wu, S. et al., Inorganic Chemistry, 53, 7650 (2014).CrossRef
Murphy, G. et al., Inorganic Chemistry 55, 9329 (2016).CrossRef
Xiao, B. et al., Chemistry – European Journal, 22, 946 (2016).CrossRef

Full text views

Full text views reflects PDF downloads, PDFs sent to Google Drive, Dropbox and Kindle and HTML full text views.

Total number of HTML views: 0
Total number of PDF views: 22 *
View data table for this chart

* Views captured on Cambridge Core between 16th January 2017 - 2nd March 2021. This data will be updated every 24 hours.

Send article to Kindle

To send this article to your Kindle, first ensure no-reply@cambridge.org is added to your Approved Personal Document E-mail List under your Personal Document Settings on the Manage Your Content and Devices page of your Amazon account. Then enter the ‘name’ part of your Kindle email address below. Find out more about sending to your Kindle. Find out more about sending to your Kindle.

Note you can select to send to either the @free.kindle.com or @kindle.com variations. ‘@free.kindle.com’ emails are free but can only be sent to your device when it is connected to wi-fi. ‘@kindle.com’ emails can be delivered even when you are not connected to wi-fi, but note that service fees apply.

Find out more about the Kindle Personal Document Service.

Towards Reliable Modeling of Challenging f Electrons Bearing Materials: Experience from Modeling of Nuclear Materials.
Available formats
×

Send article to Dropbox

To send this article to your Dropbox account, please select one or more formats and confirm that you agree to abide by our usage policies. If this is the first time you use this feature, you will be asked to authorise Cambridge Core to connect with your <service> account. Find out more about sending content to Dropbox.

Towards Reliable Modeling of Challenging f Electrons Bearing Materials: Experience from Modeling of Nuclear Materials.
Available formats
×

Send article to Google Drive

To send this article to your Google Drive account, please select one or more formats and confirm that you agree to abide by our usage policies. If this is the first time you use this feature, you will be asked to authorise Cambridge Core to connect with your <service> account. Find out more about sending content to Google Drive.

Towards Reliable Modeling of Challenging f Electrons Bearing Materials: Experience from Modeling of Nuclear Materials.
Available formats
×
×

Reply to: Submit a response


Your details


Conflicting interests

Do you have any conflicting interests? *