Biomolecular operations, which involve
the conversion
of molecular
signals or interactions into specific functional outputs, are fundamental
to the field of biology and serve as the important foundation for
the design of diagnostic and therapeutic systems. To maximize their
functionalities and broaden their applicability, it is crucial to
develop novel outputs and facile chemical transformation methods.
With this aim, in this study, we present a straightforward method
for converting nucleic acid signals into fluorescein outputs that
exhibit a wide range of functionalities. This operation is designed
through a DNA-templated reaction based on riboflavin-photocatalyzed
oxidation of dihydrofluorescein, which is readily prepared by simple
NaBH4 reduction of the fluorescein with no complicated
chemical caging steps. The templated photooxidation exhibits high
efficiency (k
app = 2.7 × 10–3/s), generating a clear fluorescein output signal distinguishable
from a low background, originating from the high stability of the
synthesized dihydrofluorescein. This facile and efficient operation
allows the nucleic acid-initiated activation of various fluorescein
functions, such as fluorescence and artificial oxidase activity, which
are applied in the design of novel bioanalytical systems, including
fluorescent and colorimetric DNA sensors. The operation presented
herein would expand the scope of biomolecular circuit systems for
diagnostic and therapeutic applications.