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, Gary Rumbles, Jeffrey L. Blackburn

Research output: Contribution to journalArticle

35 Citations (Scopus)

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 languageEnglish
Pages (from-to)603-609
Number of pages7
JournalNature Chemistry
Volume8
Issue number6
DOIs
Publication statusPublished - Jun 1 2016

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Single-walled carbon nanotubes (SWCN)
Excitons
Heterojunctions
Tuning
Electrons
Fullerenes
Thermodynamics
Fuel systems
Kinetics
Energy storage
Charge transfer
Energy dissipation
Microwaves
LDS 751
Derivatives

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

Cite this

Ihly, R., Mistry, K. S., Ferguson, A. J., Clikeman, T. T., Larson, B. W., Reid, O., ... Blackburn, J. L. (2016). Tuning the driving force for exciton dissociation in single-walled carbon nanotube heterojunctions. Nature Chemistry, 8(6), 603-609. https://doi.org/10.1038/nchem.2496

Tuning the driving force for exciton dissociation in single-walled carbon nanotube heterojunctions. / Ihly, Rachelle; Mistry, Kevin S.; Ferguson, Andrew J.; Clikeman, Tyler T.; Larson, Bryon W.; Reid, Obadiah; Boltalina, Olga V.; Strauss, Steven H.; Rumbles, Gary; Blackburn, Jeffrey L.

In: Nature Chemistry, Vol. 8, No. 6, 01.06.2016, p. 603-609.

Research output: Contribution to journalArticle

Ihly, R, Mistry, KS, Ferguson, AJ, Clikeman, TT, Larson, BW, Reid, O, Boltalina, OV, Strauss, SH, Rumbles, G & Blackburn, JL 2016, 'Tuning the driving force for exciton dissociation in single-walled carbon nanotube heterojunctions', Nature Chemistry, vol. 8, no. 6, pp. 603-609. https://doi.org/10.1038/nchem.2496
Ihly R, Mistry KS, Ferguson AJ, Clikeman TT, Larson BW, Reid O et al. Tuning the driving force for exciton dissociation in single-walled carbon nanotube heterojunctions. Nature Chemistry. 2016 Jun 1;8(6):603-609. https://doi.org/10.1038/nchem.2496
Ihly, Rachelle ; Mistry, Kevin S. ; Ferguson, Andrew J. ; Clikeman, Tyler T. ; Larson, Bryon W. ; Reid, Obadiah ; Boltalina, Olga V. ; Strauss, Steven H. ; Rumbles, Gary ; Blackburn, Jeffrey L. / Tuning the driving force for exciton dissociation in single-walled carbon nanotube heterojunctions. In: Nature Chemistry. 2016 ; Vol. 8, No. 6. pp. 603-609.
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