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Area of Science:

  • Chemistry
  • Biophysics
  • Materials Science

Background:

  • DNA-templated silver clusters function as chromophores.
  • Nucleobases within DNA dictate the spectral properties and brightness of these silver clusters.
  • Understanding the coordination environment is key to controlling chromophore behavior.

Purpose of the Study:

  • To investigate the coordination environments of two similar silver clusters (Ag106+) formed with specific DNA sequences.
  • To correlate nucleobase vibrational modes with the electronic excitation of the silver clusters using time-resolved spectroscopy.
  • To establish a link between DNA sequence, silver cluster structure, and optical properties.

Main Methods:

  • Synthesis of DNA-templated silver clusters using 18-nucleotide DNA strands.
  • Femtosecond time-resolved infrared (TRIR) spectroscopy with visible excitation and mid-infrared probing.
  • Analysis of transient infrared peaks in the 1400-1720 cm−1 range.

Main Results:

  • Two nearly identical Ag106+ clusters were characterized with DNA ligands.
  • TRIR spectroscopy revealed transient peaks decaying synchronously with visible emission.
  • Specific infrared signatures were observed for guanosine, inosine, and a subset of cytidines, but not thymidines.

Conclusions:

  • The study demonstrates that nucleobases, particularly guanosine, inosine, and cytidines, play a crucial role in the vibrational response and electronic excitation of DNA-templated silver clusters.
  • These findings suggest that the DNA-silver cluster network can be deciphered to rationally tune the coordination and spectral characteristics of molecular silver chromophores.
  • This work opens avenues for designing novel molecular materials with tailored optical properties based on DNA-metal interactions.