Classical and Quantum Mechanical Calculations of the Stacking Interaction of Nd III Complexes with Regular and Mismatched DNA Sequences

María J. Beltrán-Leiva, Isabel Fuenzalida-Valdivia, Plinio Cantero-López, Ana Bulhoes-Figueira, Jans Alzate-Morales, Dayán Páez-Hernández, Ramiro Arratia-Pérez

Research output: Contribution to journalArticle

Abstract

The design of organometallic complexes used as selective intercalators to bind and react at DNA mismatch sites has concentrated efforts in the last few years. In this context, lanthanides have received attention to be employed as active optical centers due to their spectroscopic properties. Despite the fact that there are several experimental data about synthesis and DNA binding of these compounds, theoretical analyses describing their interaction with DNA are scarce. To understand the binding to regular and mismatched DNA sequences as well as to determine the effect of the intercalation on the spectroscopic properties of the complexes, a complete theoretical study going from classical to relativistic quantum mechanics calculations has been performed on some lanthanide complexes with phenanthroline derivatives synthesized and characterized herein, viz. [Nd(NO 3 ) 3 (H 2 O)(dppz-R)] with R = H, NO 2 - , CN - and their [Nd(NO 3 ) 3 (H 2 O)(dpq)] analogue, which was computationally modeled. The results were in correct agreement with the available experimental data showing that dppz complexes have higher binding affinities to DNA than dpq one and supporting the idea that these complexes are not selective to mismatch sites in the sampled time scale. Finally, the spectroscopic analysis evidence an intercalative binding mode and made possible the elucidation of the emission mechanism of these systems. This approach is proposed as a benchmark study to extend this methodology on similar systems and constitutes the first theoretical insight in the interaction between DNA and lanthanide complexes.

Original languageEnglish
Pages (from-to)3219-3231
Number of pages13
JournalJournal of Physical Chemistry B
Volume123
Issue number15
DOIs
Publication statusPublished - 18 Apr 2019

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DNA sequences
DNA
deoxyribonucleic acid
Lanthanoid Series Elements
Rare earth elements
interactions
Intercalating Agents
Spectroscopic analysis
Phenanthrolines
Quantum theory
Organometallics
Intercalation
spectroscopic analysis
intercalation
affinity
quantum mechanics
Derivatives
methodology
analogs
synthesis

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films
  • Materials Chemistry

Cite this

Beltrán-Leiva, María J. ; Fuenzalida-Valdivia, Isabel ; Cantero-López, Plinio ; Bulhoes-Figueira, Ana ; Alzate-Morales, Jans ; Páez-Hernández, Dayán ; Arratia-Pérez, Ramiro. / Classical and Quantum Mechanical Calculations of the Stacking Interaction of Nd III Complexes with Regular and Mismatched DNA Sequences. In: Journal of Physical Chemistry B. 2019 ; Vol. 123, No. 15. pp. 3219-3231.
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Classical and Quantum Mechanical Calculations of the Stacking Interaction of Nd III Complexes with Regular and Mismatched DNA Sequences. / Beltrán-Leiva, María J.; Fuenzalida-Valdivia, Isabel; Cantero-López, Plinio; Bulhoes-Figueira, Ana; Alzate-Morales, Jans; Páez-Hernández, Dayán; Arratia-Pérez, Ramiro.

In: Journal of Physical Chemistry B, Vol. 123, No. 15, 18.04.2019, p. 3219-3231.

Research output: Contribution to journalArticle

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AU - Fuenzalida-Valdivia, Isabel

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AU - Bulhoes-Figueira, Ana

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AU - Arratia-Pérez, Ramiro

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