skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: A crystal plasticity model based on transition state theory

ORCiD logo; ; ;
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
Grant/Contract Number:
FWP 06SCPE401; AC52-06NA25396; AC05-00OR22725
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
International Journal of Plasticity
Additional Journal Information:
Journal Volume: 93; Journal Issue: C; Related Information: CHORUS Timestamp: 2018-01-12 11:59:09; Journal ID: ISSN 0749-6419
Country of Publication:
United States

Citation Formats

Wang, H., Capolungo, L., Clausen, B., and Tomé, C. N. A crystal plasticity model based on transition state theory. United States: N. p., 2017. Web. doi:10.1016/j.ijplas.2016.05.003.
Wang, H., Capolungo, L., Clausen, B., & Tomé, C. N. A crystal plasticity model based on transition state theory. United States. doi:10.1016/j.ijplas.2016.05.003.
Wang, H., Capolungo, L., Clausen, B., and Tomé, C. N. 2017. "A crystal plasticity model based on transition state theory". United States. doi:10.1016/j.ijplas.2016.05.003.
title = {A crystal plasticity model based on transition state theory},
author = {Wang, H. and Capolungo, L. and Clausen, B. and Tomé, C. N.},
abstractNote = {},
doi = {10.1016/j.ijplas.2016.05.003},
journal = {International Journal of Plasticity},
number = C,
volume = 93,
place = {United States},
year = 2017,
month = 6

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on May 13, 2018
Publisher's Accepted Manuscript

Save / Share:
  • Abstract not provided.
  • Cited by 19
  • The inosine monophosphate cyclohydrolase (IMPCH) component (residues 1-199) of the bifunctional enzyme aminoimidazole-4-carboxamide ribonucleotide transformylase (AICAR Tfase, residues 200-593)/IMPCH (ATIC) catalyzes the final step in the de novo purine biosynthesis pathway that produces IMP. As a potential target for antineoplastic intervention, we designed IMPCH inhibitors, 1,5-dihydroimidazo[4,5-c][1,2,6]thiadiazin-4(3H)-one 2,2-dioxide (heterocycle, 1), the corresponding nucleoside (2), and the nucleoside monophosphate (nucleotide) (3), as mimics of the tetrahedral intermediate in the cyclization reaction. All compounds are competitive inhibitors against IMPCH (K(i) values = 0.13-0.23 microm) with the simple heterocycle 1 exhibiting the most potent inhibition (K(i) = 0.13 microm). Crystal structures of bifunctional ATICmore » in complex with nucleoside 2 and nucleotide 3 revealed IMPCH binding modes similar to that of the IMPCH feedback inhibitor, xanthosine 5'-monophosphate. Surprisingly, the simpler heterocycle 1 had a completely different IMPCH binding mode and was relocated to the phosphate binding pocket that was identified from previous xanthosine 5'-monophosphate structures. The aromatic imidazole ring interacts with a helix dipole, similar to the interaction with the phosphate moiety of 3. The crystal structures not only revealed the mechanism of inhibition of these compounds, but they now serve as a platform for future inhibitor improvements. Importantly, the nucleoside-complexed structure supports the notion that inhibitors lacking a negatively charged phosphate can still inhibit IMPCH activity with comparable potency to phosphate-containing inhibitors. Provocatively, the nucleotide inhibitor 3 also binds to the AICAR Tfase domain of ATIC, which now provides a lead compound for the design of inhibitors that simultaneously target both active sites of this bifunctional enzyme.« less
  • Final state-selected spectra in unimolecular decomposition are obtained by a random matrix version of Feshbach`s optical model. The number of final states which are independently coupled to the molecular quasibound states is identified with the number of states at the dividing surface of transition state theory (TST). The coupling of the transition state to the molecular complex is modeled via a universal random matrix effective Hamiltonian which is characterized by its resonance eigenstates and provides the correct average unimolecular decay rate. The transition from nonoverlapping resonances which are associated with isolated Lorentzian spectral peaks, to overlapping resonances, associated with moremore » complex spectra, is characterized in terms of deviations from a {chi}{sup 2}-like distribution of the resonance widths and the approach to a random phase-distribution of the resonance scattering amplitudes. The evolution of the system from a tight transition state to reaction products is treated explicitly as a scattering process where specific dynamics can be incorporated. Comparisons with recently measured final state-selected spectra and rotational distributions for the unimolecular reaction of NO{sub 2} show that the present model provides a useful new approach for understanding and interpreting experimental results which are dominated by overlapping resonances.« less
  • Multistate generalizations of Landau-Zener model are studied by summing entire series of perturbation theory. A technique for analysis of the series is developed. Analytical expressions for probabilities of survival at the diabatic potential curves with extreme slope are proved. Degenerate situations are considered when there are several potential curves with extreme slope. Expressions for some state-to-state transition probabilities are derived in degenerate cases.