Tuning the Driving Force for Exciton Dissociation in Single-Walled Carbon Nanotube Heterojunctions

Rachelle Ihly, Kevin S. Mistry, Andrew J. Ferguson, Tyler T. Clikeman, Bryon W. Larson, Obadiah Reid, Olga V. Boltalina, Steven H. Strauss, Garry Rumbles, Jeffrey L. Blackburn

Research output: Contribution to journalArticlepeer-review

78 Scopus Citations

Abstract

Understanding the kinetics and energetics of interfacial electron transfer in molecular systems is crucial for the development of a broad array of technologies, including photovoltaics, solar fuel systems and energy storage. The Marcus formulation for electron transfer relates the thermodynamic driving force and reorganization energy for charge transfer between a given donor/acceptor pair to the kinetics and yield of electron transfer. Here we investigated the influence of the thermodynamic driving force for photoinduced electron transfer (PET) between single-walled carbon nanotubes (SWCNTs) and fullerene derivatives by employing time-resolved microwave conductivity as a sensitive probe of interfacial exciton dissociation. For the first time, we observed the Marcus inverted region (in which driving force exceeds reorganization energy) and quantified the reorganization energy for PET for a model SWCNT/acceptor system. The small reorganization energies (about 130meV, most of which probably arises from the fullerene acceptors) are beneficial in minimizing energy loss in photoconversion schemes.

Original languageAmerican English
Pages (from-to)603-609
Number of pages7
JournalNature Chemistry
Volume8
Issue number6
DOIs
StatePublished - 1 Jun 2016

Bibliographical note

Publisher Copyright:
© 2016 Macmillan Publishers Limited. All rights reserved.

NREL Publication Number

  • NREL/JA-5900-64877

Keywords

  • carbon nanotubes
  • fullerenes
  • Marcus formulation
  • photoinduced electron transfer
  • solar-photochemistry

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