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      Evidence for conical intersection dynamics mediating ultrafast singlet exciton fission

      Author(s): , , , , , ,
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      Journal: Nature Physics
      Publisher: Springer Nature

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          Singlet fission.

          Millicent Smith, Josef Michl (2010)
          Article 0 comments Cited 393 times – based on 0 reviews     Review now
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            Ultrafast long-range charge separation in organic semiconductor photovoltaic diodes.

            Simon Gélinas, Akshay Rao, Abhishek Kumar … (2014)
            Understanding the charge-separation mechanism in organic photovoltaic cells (OPVs) could facilitate optimization of their overall efficiency. Here we report the time dependence of the separation of photogenerated electron hole pairs across the donor-acceptor heterojunction in OPV model systems. By tracking the modulation of the optical absorption due to the electric field generated between the charges, we measure ~200 millielectron volts of electrostatic energy arising from electron-hole separation within 40 femtoseconds of excitation, corresponding to a charge separation distance of at least 4 nanometers. At this separation, the residual Coulomb attraction between charges is at or below thermal energies, so that electron and hole separate freely. This early time behavior is consistent with charge separation through access to delocalized π-electron states in ordered regions of the fullerene acceptor material.
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              Two-dimensional spectroscopy of a molecular dimer unveils the effects of vibronic coupling on exciton coherences.

              Alexei Halpin, Philip J M Johnson, Roel Tempelaar … (2014)
              The observation of persistent oscillatory signals in multidimensional spectra of protein-pigment complexes has spurred a debate on the role of coherence-assisted electronic energy transfer as a key operating principle in photosynthesis. Vibronic coupling has recently been proposed as an explanation for the long lifetime of the observed spectral beatings. However, photosynthetic systems are inherently complicated, and tractable studies on simple molecular compounds are needed to fully understand the underlying physics. In this work, we present measurements and calculations on a solvated molecular homodimer with clearly resolvable oscillations in the corresponding two-dimensional spectra. Through analysis of the various contributions to the nonlinear response, we succeed in isolating the signal due to inter-exciton coherence. We find that although calculations predict a prolongation of this coherence due to vibronic coupling, the combination of dynamic disorder and vibrational relaxation leads to a coherence decay on a timescale comparable to the electronic dephasing time.
              Article 0 comments Cited 91 times – based on 0 reviews     Review now
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                Author and article information

                Journal
                Title: Nature Physics
                Abbreviated Title: Nat Phys
                Publisher: Springer Nature
                ISSN (Print): 1745-2473
                ISSN (Electronic): 1745-2481
                Publication date Created: March 16 2015
                Publication date (Print): March 16 2015
                Volume: 11
                Issue: 4
                Pages: 352-357
                Article
                DOI: 10.1038/nphys3241
                SO-VID: 6e81441a-13f4-4359-ab74-2b2bef332c83
                Copyright © © 2015
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