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Title: SU-C-204-03: DFT Calculations of the Stability of DOTA-Based-Radiopharmaceuticals

Abstract

Purpose: Application of the density function theory (DFT) to investigate the structural stability of complexes applied in cancer therapy consisting of the 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA) chelated to Ac225, Fr221, At217, Bi213, and Gd68 radio-nuclei. Methods: The possibility to deliver a toxic payload directly to tumor cells is a highly desirable aim in targeted alpha particle therapy. The estimation of bond stability between radioactive atoms and the DOTA chelating agent is the key element in understanding the foundations of this delivery process. Thus, we adapted the Vienna Ab-initio Simulation Package (VASP) with the projector-augmented wave method and a plane-wave basis set in order to study the stability and electronic properties of DOTA ligand chelated to radioactive isotopes. In order to count for the relativistic effect of radioactive isotopes we included Spin-Orbit Coupling (SOC) in the DFT calculations. Five DOTA complex structures were represented as unit cells, each containing 58 atoms. The energy optimization was performed for all structures prior to calculations of electronic properties. Binding energies, electron localization functions as well as bond lengths between atoms were estimated. Results: Calculated binding energies for DOTA-radioactive atom systems were −17.792, −5.784, −8.872, −13.305, −18.467 eV for Ac, Fr, At, Bi and Gd complexesmore » respectively. The displacements of isotopes in DOTA cages were estimated from the variations in bond lengths, which were within 2.32–3.75 angstroms. The detailed representation of chemical bonding in all complexes was obtained with the Electron Localization Function (ELF). Conclusion: DOTA-Gd, DOTA-Ac and DOTA-Bi were the most stable structures in the group. Inclusion of SOC had a significant role in the improvement of DFT calculation accuracy for heavy radioactive atoms. Our approach is found to be proper for the investigation of structures with DOTA-based-radiopharmaceuticals and will enhance our understanding of processes occurring at subatomic levels.« less

Authors:
;  [1]; ; ;  [2]; ;  [1];  [3]
  1. University of South Florida, Tampa, Florida (United States)
  2. H. Lee Moffitt Cancer Center and Research Institute, Tampa, Florida (United States)
  3. (United States)
Publication Date:
OSTI Identifier:
22624301
Resource Type:
Journal Article
Resource Relation:
Journal Name: Medical Physics; Journal Volume: 43; Journal Issue: 6; Other Information: (c) 2016 American Association of Physicists in Medicine; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
62 RADIOLOGY AND NUCLEAR MEDICINE; 60 APPLIED LIFE SCIENCES; 61 RADIATION PROTECTION AND DOSIMETRY; ACTINIUM 225; ASTATINE 217; BINDING ENERGY; BISMUTH 213; BOND LENGTHS; CHELATES; CHELATING AGENTS; CHEMICAL BONDS; FRANCIUM 221; GADOLINIUM COMPLEXES; NEOPLASMS; PARTICLE BEAMS; RADIOPHARMACEUTICALS; RADIOTHERAPY; RELATIVISTIC RANGE; TUMOR CELLS

Citation Formats

Khabibullin, A.R., Woods, L.M., Karolak, A., Budzevich, M.M., Martinez, M.V., McLaughlin, M.L., Morse, D.L., and H. Lee Moffitt Cancer Center and Research Institute, Tampa, Florida. SU-C-204-03: DFT Calculations of the Stability of DOTA-Based-Radiopharmaceuticals. United States: N. p., 2016. Web. doi:10.1118/1.4955536.
Khabibullin, A.R., Woods, L.M., Karolak, A., Budzevich, M.M., Martinez, M.V., McLaughlin, M.L., Morse, D.L., & H. Lee Moffitt Cancer Center and Research Institute, Tampa, Florida. SU-C-204-03: DFT Calculations of the Stability of DOTA-Based-Radiopharmaceuticals. United States. doi:10.1118/1.4955536.
Khabibullin, A.R., Woods, L.M., Karolak, A., Budzevich, M.M., Martinez, M.V., McLaughlin, M.L., Morse, D.L., and H. Lee Moffitt Cancer Center and Research Institute, Tampa, Florida. Wed . "SU-C-204-03: DFT Calculations of the Stability of DOTA-Based-Radiopharmaceuticals". United States. doi:10.1118/1.4955536.
@article{osti_22624301,
title = {SU-C-204-03: DFT Calculations of the Stability of DOTA-Based-Radiopharmaceuticals},
author = {Khabibullin, A.R. and Woods, L.M. and Karolak, A. and Budzevich, M.M. and Martinez, M.V. and McLaughlin, M.L. and Morse, D.L. and H. Lee Moffitt Cancer Center and Research Institute, Tampa, Florida},
abstractNote = {Purpose: Application of the density function theory (DFT) to investigate the structural stability of complexes applied in cancer therapy consisting of the 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid (DOTA) chelated to Ac225, Fr221, At217, Bi213, and Gd68 radio-nuclei. Methods: The possibility to deliver a toxic payload directly to tumor cells is a highly desirable aim in targeted alpha particle therapy. The estimation of bond stability between radioactive atoms and the DOTA chelating agent is the key element in understanding the foundations of this delivery process. Thus, we adapted the Vienna Ab-initio Simulation Package (VASP) with the projector-augmented wave method and a plane-wave basis set in order to study the stability and electronic properties of DOTA ligand chelated to radioactive isotopes. In order to count for the relativistic effect of radioactive isotopes we included Spin-Orbit Coupling (SOC) in the DFT calculations. Five DOTA complex structures were represented as unit cells, each containing 58 atoms. The energy optimization was performed for all structures prior to calculations of electronic properties. Binding energies, electron localization functions as well as bond lengths between atoms were estimated. Results: Calculated binding energies for DOTA-radioactive atom systems were −17.792, −5.784, −8.872, −13.305, −18.467 eV for Ac, Fr, At, Bi and Gd complexes respectively. The displacements of isotopes in DOTA cages were estimated from the variations in bond lengths, which were within 2.32–3.75 angstroms. The detailed representation of chemical bonding in all complexes was obtained with the Electron Localization Function (ELF). Conclusion: DOTA-Gd, DOTA-Ac and DOTA-Bi were the most stable structures in the group. Inclusion of SOC had a significant role in the improvement of DFT calculation accuracy for heavy radioactive atoms. Our approach is found to be proper for the investigation of structures with DOTA-based-radiopharmaceuticals and will enhance our understanding of processes occurring at subatomic levels.},
doi = {10.1118/1.4955536},
journal = {Medical Physics},
number = 6,
volume = 43,
place = {United States},
year = {Wed Jun 15 00:00:00 EDT 2016},
month = {Wed Jun 15 00:00:00 EDT 2016}
}