4 years ago

Excitonic Coupling Modulated by Mechanical Stimuli

Excitonic Coupling Modulated by Mechanical Stimuli
Ignacio Franco, Alessandro Pirrotta, Alessandro Troisi, Gemma C. Solomon
Understanding energy transfer is of vital importance in a diverse range of applications from biological systems to photovoltaics. The ability to tune excitonic coupling in any of these systems, however, is generally limited. In this work, we have simulated a new class of single-molecule spectroscopy in which force microscopy is used to control the excitonic coupling between chromophores. Here we demonstrate that the excitonic coupling can be controlled by mechanical manipulation of the molecule (perylenediimide dimers and terrylenediimide-perylenediimide heterodimers) and can be tuned over a broad range of values (0.02–0.15 eV) that correspond to different regimes of exciton dynamics going from the folded to the elongated structure of the dimer. In all of the systems considered here, the switching from high to low coupling takes place simultaneously with the mechanical deformation detected by a strong increase and subsequent decay of the force. These simulations suggest that single-molecule force spectroscopy can be used to understand and eventually aid the design of excitonic devices.

Publisher URL: http://dx.doi.org/10.1021/acs.jpclett.7b01828

DOI: 10.1021/acs.jpclett.7b01828

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