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Molecular Dynamical and Quantum Mechanical Exploration of the Site-Specific Dynamics of Cy3 Dimers Internally Linked to dsDNA.
Sorour, Mohammed I; Kistler, Kurt A; Marcus, Andrew H; Matsika, Spiridoula.
Afiliación
  • Sorour MI; Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United States.
  • Kistler KA; Department of Chemistry, Pennsylvania State University, Brandywine Campus, Media, Pennsylvania 19063, United States.
  • Marcus AH; Department of Chemistry and Biochemistry, University of Oregon, Eugene, Oregon 97403, United States.
  • Matsika S; Department of Chemistry, Temple University, Philadelphia, Pennsylvania 19122, United States.
J Phys Chem B ; 128(32): 7750-7760, 2024 Aug 15.
Article en En | MEDLINE | ID: mdl-39105720
ABSTRACT
Performing spectroscopic measurements on biomolecules labeled with fluorescent probes is a powerful approach to locating the molecular behavior and dynamics of large systems at specific sites within their local environments. The indocarbocyanine dye Cy3 has emerged as one of the most commonly used chromophores. The incorporation of Cy3 dimers into DNA enhances experimental resolution owing to the spectral characteristics influenced by the geometric orientation of excitonically coupled monomeric units. Various theoretical models and simulations have been utilized to aid in the interpretation of the experimental spectra. In this study, we employ all-atom molecular dynamics simulations to study the structural dynamics of Cy3 dimers internally linked to the dsDNA backbone. We used quantum mechanical calculations to derive insights from both the linear absorption spectra and the circular dichroism data. Furthermore, we explore potential limitations within a commonly used force field for cyanine dyes. The molecular dynamics simulations suggest the presence of four possible Cy3 dimeric populations. The spectral simulations on the four populations show one of them to agree better with the experimental signatures, suggesting it to be the dominant population. The relative orientation of Cy3 in this population compares very well with previous predictions from the Holstein-Frenkel Hamiltonian model.
Asunto(s)

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Teoría Cuántica / ADN / Carbocianinas / Dimerización / Simulación de Dinámica Molecular Idioma: En Revista: J Phys Chem B Asunto de la revista: QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Teoría Cuántica / ADN / Carbocianinas / Dimerización / Simulación de Dinámica Molecular Idioma: En Revista: J Phys Chem B Asunto de la revista: QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos