Excited-State
Charge Transfer, Proton Transfer, and
Exciplex Formation Revealed by Ultrafast Time-Resolved Spectroscopy
in Human Telomeric Ribonucleic Acid Quadruplex
Posted on 2023-05-26 - 13:04
Guanine quadruplexes (GQs), important for genome stability
and
biotechnology application, can form from both DNA and RNA. However,
unlike the study of DNA GQs, little research has been conducted on
excited states of GQs from RNA, which due to the ribose 2′-hydroxy
group have structures distinct from their DNA counterparts. Combining
ultrafast broadband time-resolved fluorescence and transient absorption
measurements, we report the first direct probe of excitation dynamics
for a bimolecular GQ from human telomeric repeat-containing RNA taking
the typical highly compacted parallel folding with a propeller-like
loop structure. The result revealed a multichannel decay containing
an unusual high-energy excimer featuring charge transfer deactivated
by rapid proton transfer in the tetrad core region. It also identified
an unprecedented exciplex displaying massively red-shifted fluorescence
produced from charge transfer in the loop region. The findings underscore
the role of structural conformation and base content in determining
the energy, electronic attribution, and decay dynamics of GQ excited
states.
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Ma, Chensheng; Chow, Joshua Chiu-Lok; Wong, Allen Ka-Wa; Xiong, Qingwu; Chomchoei, Jacob; Kwok, Wai-Ming (2023). Excited-State
Charge Transfer, Proton Transfer, and
Exciplex Formation Revealed by Ultrafast Time-Resolved Spectroscopy
in Human Telomeric Ribonucleic Acid Quadruplex. ACS Publications. Collection. https://doi.org/10.1021/acs.jpclett.3c00806