Abstract
AbstractMethylation of adenine at the N6 position is a crucial epigenetic modification that profoundly influences gene regulation and expression. Moreover, this modification intricately alters the excited state dynamics of adenine nucleobases. To explore the impact of N6‐methyladenine on the excited state dynamics within oligonucleotides, we conducted a comprehensive investigation of two dinucleotides containing N6‐methyladenosine, in conjunction with adenosine or guanosine. Using steady‐state and time‐resolved absorption and fluorescence spectroscopy techniques, we not only observed the customary monomer‐like and charge transfer emissive states, as reported in previous dinucleotides, but also identified an additional low‐energy emissive state. This unique state exhibits an extraordinary Stokes Shift exceeding 2.3 eV and has a relatively long lifetime of 4–5 ns. We propose that this state corresponds to a bonded exciplex state, governed by ground‐state geometries.
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