Observing the Fluctuation Dynamics of Dative Bonds Using Two-Dimensional Electronic Spectroscopy
Journal of Physical Chemistry Letters, ISSN: 1948-7185, Vol: 12, Issue: 1, Page: 165-170
2021
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Article Description
We perform two-dimensional electronic spectroscopy on chlorophyll (Chl) a and b molecules in aprotic solvents of different Lewis basicity. By analyzing the ultrafast spectral diffusion dynamics of the Qy transition, we show that a certain timescale of the spectral diffusion dynamics is affected by the solvents' Lewis basicity. Control experiments with Chlorin-e6 - a Chl molecule analog - and ab initio time-dependent density functional theory calculations confirm that we are directly probing the fluctuation dynamics of the dative bond between the solvent's lone pair and the Mg2+ center in Chls that is responsible for the Lewis basicity. The observation is indicative of dative bond length and angular fluctuations with timescales ranging between ∼30 and 150 ps and the dative bond-strength-dependent perturbation on the Qy transition frequency of Chls.
Bibliographic Details
American Chemical Society (ACS)
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