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DNA autoionization is a fundamental process wherein UV-photoexcitednucleobases dissipate energy by charge transfer to the environment withoutundergoing chemical damage. Here, single-wall carbon nanotubes (SWNT) areexplored as a photoluminescent reporter for studying the mechanism and rates ofDNA autoionization. Two-color photoluminescence spectroscopy allows separatephotoexcitation of the DNA and the SWNTs in the UV and visible range,respectively. A strong SWNT photoluminescence quenching is observed when the UVpump is resonant with the DNA absorption, consistent with charge transfer fromthe excited states of the DNA to the SWNT. Semiempirical calculations of theDNA-SWNT electronic structure, combined with a Green's function theory forcharge transfer, show a 20 fs autoionization rate, dominated by the holetransfer. Rate-equation analysis of the spectroscopy data confirms that thequenching rate is limited by the thermalization of the free charge carrierstransferred to the nanotube reservoir. The developed approach has a greatpotential for monitoring DNA excitation, autoionization, and chemical damageboth {\it in vivo} and {\it in vitro}.

Two-color spectroscopy of UV excited ssDNA complex with a single-wall nanotube probe: Fast nucleobase autoionization mechanism