期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 11, 期 21, 页码 8958-8963出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c02486
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资金
- U.S. National Science Foundation [CHE-1800471]
- Ohio State University
- National Science Foundation [CHE-1611451, CHE-2002910]
- Furman Advantage program
- National Science Foundation EPSCoR Program [OIA-1655740]
DNA-templated silver clusters are chromophores in which the nucleobases encode the cluster spectra and brightness. We describe the coordination environments of two nearly identical Ag-10(6+) clusters that form with 18-nucleotide strands CCCCA CCCCT CCCX TTTT, with X = guanosine and inosine. For the first time, femtosecond time-resolved infrared (TRIR) spectroscopy with visible excitation and mid-infrared probing is used to correlate the response of nucleobase vibrational modes to electronic excitation of the metal cluster. A rich pattern of transient TRIR peaks in the 1400-1720 cm(-1) range decays synchronously with the visible emission. Specific infrared signatures associated with the single guanosine/inosine along with a subset of cytidines, but not the thymidines, are observed. These fingerprints suggest that the network of bonds between a silver cluster adduct and its polydentate DNA ligands can be deciphered to rationally tune the coordination and thus spectra of molecular silver chromophores.
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