Abstract:Understanding behavior of rare-earth ions (REI) in crowded environments is crucial for several nano- and bio-technological applications. Evolution of REI photoluminescence (PL) in small compartments inside a silica hydrogel, mimic to a soft matter bio-environment, has been studied and explained within a solvation model. The model uncovered the origin of high PL efficiency to be the formation of REI complexes, surrounded by bile salt (DOC) molecules. Comparative study of these REI-DOC complexes in bulk water so… Show more
“…This excludes the electrons trapped in solvated states in surrounding water. We note that the same samples showed an interesting PL behavior during the formation of the complexes with the multivalent ions [93] to be discussed elsewhere.…”
Section: Si: Discussion Of Alternative Recombination Mechanismsmentioning
SWNT ssDNADNA is capable to recover after absorbing ultraviolet (UV) radiation, for example, by autoionization (AI). Singlewall carbon nanotube (SWNT) two-color photoluminescence spectroscopy was combined with quantum mechanical calculations to explain the AI in self-assembled complexes of DNA wrapped around SWNT. DNA autoionization is a fundamental process wherein UV-photoexcited nucleobases dissipate energy by charge transfer to the environment without undergoing chemical damage. Here, single-wall carbon nanotubes (SWNT) are explored as a photoluminescent reporter for studying the mechanism and rates of DNA autoionization. Two-color photoluminescence spectroscopy allows separate photoexcitation of the DNA and the SWNTs in the UV and visible range, respectively. A strong SWNT photoluminescence quenching is observed when the UV pump is resonant with the DNA absorption, consistent with charge transfer from the excited states of the DNA to the SWNT. Semiempirical calculations of the DNA-SWNT electronic structure, combined with a Green's function theory for charge transfer, show a 20 fs autoionization rate, dominated by the hole transfer. Rate-equation analysis of the spectroscopy data confirms that the quenching rate is limited by the thermalization of the free charge carriers transferred to the nanotube reservoir. The developed approach has a great potential for monitoring DNA excitation, autoionization, and chemical damage both in vivo and in vitro arXiv:1512.00710v1 [cond-mat.mes-hall] 2 Dec 2015 2
“…This excludes the electrons trapped in solvated states in surrounding water. We note that the same samples showed an interesting PL behavior during the formation of the complexes with the multivalent ions [93] to be discussed elsewhere.…”
Section: Si: Discussion Of Alternative Recombination Mechanismsmentioning
SWNT ssDNADNA is capable to recover after absorbing ultraviolet (UV) radiation, for example, by autoionization (AI). Singlewall carbon nanotube (SWNT) two-color photoluminescence spectroscopy was combined with quantum mechanical calculations to explain the AI in self-assembled complexes of DNA wrapped around SWNT. DNA autoionization is a fundamental process wherein UV-photoexcited nucleobases dissipate energy by charge transfer to the environment without undergoing chemical damage. Here, single-wall carbon nanotubes (SWNT) are explored as a photoluminescent reporter for studying the mechanism and rates of DNA autoionization. Two-color photoluminescence spectroscopy allows separate photoexcitation of the DNA and the SWNTs in the UV and visible range, respectively. A strong SWNT photoluminescence quenching is observed when the UV pump is resonant with the DNA absorption, consistent with charge transfer from the excited states of the DNA to the SWNT. Semiempirical calculations of the DNA-SWNT electronic structure, combined with a Green's function theory for charge transfer, show a 20 fs autoionization rate, dominated by the hole transfer. Rate-equation analysis of the spectroscopy data confirms that the quenching rate is limited by the thermalization of the free charge carriers transferred to the nanotube reservoir. The developed approach has a great potential for monitoring DNA excitation, autoionization, and chemical damage both in vivo and in vitro arXiv:1512.00710v1 [cond-mat.mes-hall] 2 Dec 2015 2
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