4.6 Article

Understanding Disorder, Vibronic Structure, and Delocalization in Electronically Coupled Dimers on DNA Duplexes

期刊

JOURNAL OF PHYSICAL CHEMISTRY A
卷 125, 期 44, 页码 9632-9644

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpca.1c07205

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资金

  1. ASEE Fellowship from the American Society for Engineering Education
  2. Naval Research Laboratory Institute for Nanoscience
  3. Office of Naval Research

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Structural DNA nanotechnology offers a promising approach to control material functions through modular structures and Hamiltonians. Characterizing parameters of chromophore networks, such as vibronic Hamiltonian, molecular positions, and environmentally induced energy broadening, is essential for optimizing their functionalities. Study methods include steady-state optical measurements, physical modeling, and genetic algorithms, with temperature-dependent optical measurements aiding in further characterization of spectral broadening. Results reveal quantum mechanical delocalization crucial for functions like coherent energy transport and quantum information applications.
Structural DNA nanotechnology is a promising approach to create chromophore networks with modular structures and Hamiltonians to control the material's functions. The functional behaviors of these systems depend on the interactions of the chromophores' vibronic states, as well as interactions with their environment. To optimize their functions, it is necessary to characterize the chromophore network's structural and energetic properties, including the electronic delocalization in some cases. In this study, parameters of interest are deduced in DNA-scaffolded Cyanine 3 and Cyanine 5 dimers. The methods include steady-state optical measurements, physical modeling, and a genetic algorithm approach. The parameters include the chromophore network's vibronic Hamiltonian, molecular positions, transition dipole orientations, and environmentally induced energy broadening. Additionally, the study uses temperature-dependent optical measurements to characterize the spectral broadening further. These combined results reveal the quantum mechanical delocalization, which is important for functions like coherent energy transport and quantum information applications.

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