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sawaya-aspuru-excitonics-chemrxiv-170814.pdf (4.57 MB)

Excitonics: A universal set of binary gates for molecular exciton processing and signaling

preprint
submitted on 14.08.2017, 19:46 and posted on 15.08.2017, 15:57 by Nicolas Sawaya, Dmitrij Rappoport, Daniel Tabor, Alan Aspuru-Guzik
The ability to regulate energy transfer pathways through materials is an important goal of nanotechnology, as a greater degree of control is crucial for developing sensing, solar energy, and bioimaging applications. Such control necessitates a toolbox of actuation methods that can direct energy transfer based on user input. Here we propose a novel molecular exciton gate, analogous to a traditional transistor, for controlling exciton migration in chromophoric systems. The gate may be activated with an input of light or an input flow of excitons. Unlike previous gates and switches that control exciton transfer, our proposal does not require isomerization or molecular rearrangement, instead relying on excitation migration via the second singlet (S2) state of the gate molecule--hence the system is named an "S2 exciton gate." After presenting a set of system properties required for proper function of the S2 exciton gate, we show how one would overcome the two possible challenges: short-lived excited states and suppression of false positives. Precision and error rates are studied computationally in a model system with respect to excited-state decay rates and variations in molecular orientation. Finally, we demonstrate that the S2 exciton gate gate can be used to produce binary logical AND, OR, and NOT operations, providing a universal excitonic computation platform with a range of potential applications, including e.g. in signal processing for microscopy.

Funding

U.S. DOE DE-SC0001088, U.S. NSF DMR-1231319, CIFAR

History

Topic

  • Photochemistry (Physical Chem.)
  • Physical and Chemical Processes
  • Transport phenomena (Physical Chem.)
  • Spectroscopy (Physical Chem.)
  • Quasiparticles and Excitations
  • Biophysical Chemistry

Email Address of Submitting Author

sawayanicolas@gmail.com

Email Address(es) for Other Author(s)

aspuru@chemistry.harvard.edu

Institution

Harvard University

Country

United States

ORCID For Submitting Author

0000-0001-8510-8480

Declaration of Conflict of Interest

No conflict of interest.

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