Multiscale simulation on a light-harvesting molecular triad

Su, Guoxiong; Czader, Arkadiusz; Homouz, Dirar; Bernardes, Gabriela; Mateen, Sana; Cheung, Margaret S.

doi:10.1021/jp212273n

Multiscale simulation on a light-harvesting molecular triad

Journal Article · Tue Feb 21 23:00:00 EST 2012 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/jp212273n· OSTI ID:1358258

Su, Guoxiong ^[1]; Czader, Arkadiusz ^[2]; Homouz, Dirar ^[3]; Bernardes, Gabriela ^[2]; Mateen, Sana ^[2]; Cheung, Margaret S. ^[2]

Univ. of Houston, Houston, TX (United States); University of Houston
Univ. of Houston, Houston, TX (United States)
Khalifa Univ., Abu Dhabi (United Arab Emirates)

Here, we have investigated the effect of solvation and confinement on an artificial photosynthetic material, carotenoid-porphyrin-C60 molecular triad, by a multiscale approach and an enhanced sampling technique. We have developed a combined approach of quantum chemistry, statistical physics, and all-atomistic molecular dynamics simulation to determine the partial atomic charges of the ground-state triad. To fully explore the free energy landscape of triad, the replica exchange method was applied to enhance the sampling efficiency of the simulations. The confinement effects on the triad were modeled by imposing three sizes of spherocylindrical nanocapsules. The triad is structurally flexible under ambient conditions, and its conformation distribution is manipulated by the choice of water models and confinement. Two types of water models (SPC/E and TIP3P) are used for solvation. When solvated by SPC/E water, whose HOH angle follows an ideal tetrahedron, the structural characteristics of triad is compact in the bulk systems. However, under a certain nanosized confinement that drastically disrupts hydrogen bond networks in solvent, the triad favors an extended configuration. By contrast, the triad solvated by TIP3P water shows a set of U-shaped conformations in the confinement. We have shown that a slight structural difference in the two water models with the same dipole moment can have great distinction in water density, water orientation, and the number of hydrogen bonds in the proximity of a large flexible compound such as the triad. Subsequently, it has direct impact on the position of the triad in a confinement as well as the distribution of conformations at the interface of liquid and solid in a finite-size system.

Research Organization:: Univ. of Houston, Houston, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

DOE Contract Number:: SC0004832

OSTI ID:: 1358258

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Journal Name: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry Journal Issue: 29 Vol. 116; ISSN 1520-6106

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

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