Amino-acids; Annihilation rates; Computational studies; Energy; Large clusters; Molecular mechanics method; Orbitals; Quantum mechanics/molecular mechanics; Water solutions; Zwitterionic forms; Surfaces, Coatings and Films; Physical and Theoretical Chemistry; Materials Chemistry
Abstract :
[en] We performed a computational study of positron attachment to hydrated amino acids, namely glycine, alanine, and proline in the zwitterionic form. We combined the sequential quantum mechanics/molecular mechanics (s-QM/MM) method with various levels of any particle molecular orbital (APMO) calculations. Consistent with previous studies, our calculations indicate the formation of energetically stable states for the isolated and microsolvated amino acids, in which the positron localizes around the carboxylate group. However, for the larger clusters, composed of 7 to 40 water molecules, hydrogen bonding between the solute and solvent molecules disfavors positron attachment to the amino acids, giving rise to surface states in which the positron is located around the water-vacuum interface. The analysis of positron binding energies, positronic orbitals, radial probability distributions, and annihilation rates consistently pointed out the change from positron-solute to positron-solvent states. Even with the inclusion of an electrostatic embedding around the aggregates, the positrons did not localize around the solute. Positron attachment to molecules in the gas phase is a well-established fact. The existence of hydrated positronic molecules could also be expected from the analogy with transient anion states, which are believed to participate in radiation damage. Our results indicate that positron attachment to hydrated biomolecules, even to zwitterions with negatively charged carboxylated groups, would not take place. For the larger clusters, in which positron-water interactions are favored, the calculations indicate an unexpectedly large contribution of the core orbitals to the annihilation rates, between 15 and 20%. Finally, we explored correlations between positron binding energies (PBEs) and dipole moments, as well as annihilation rates and PBEs, consistent with previous studies for smaller clusters.
Disciplines :
Chemistry Physics
Author, co-author :
Bergami, Mateus ; Instituto de Física, Universidade de São Paulo, Rua do Matão 1371, CEP 05508-090 São Paulo, SP, Brazil
Conselho Nacional de Desenvolvimento Cient?fico e Tecnol?gico Funda??o de Amparo ? Pesquisa do Estado de S?o Paulo Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior
Funding text :
M.B. acknowledges support from the Brazilian agency Coordenac\u0327a\u0303o de Aperfeic\u0327oamento de Pessoal de Ni\u0301vel Superior (CAPES). M.T.N.V. also acknowledges financial support from CNPq (Grant No 306285/2022-3) and FAPESP (Grant no. 2020/16155-7). K.C. acknowledges support from CNPq, CAPES and FAPESP (Grant no. 2021/09016-3). This work used resources of the Centro Nacional de Processamento de Alto Desempenho em Sa\u0303o Paulo (CENAPAD-SP) and STI (University of Sa\u0303o Paulo).The Article Processing Charge for the publication of this research was funded by the Coordination for the Improvement of Higher Education Personnel - CAPES (ROR identifier: 00x0ma614).
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