Abstract

Ultrafast transient absorption and quantum chemistry calculations are combined to demonstrate singlet fission in newly functionalized TIPS-Tetracenes. The coupling strength (but not the energy gap) between Si and ’(TT) states gauges singlet fission efficiency and rate.

Highlights

  • The efficiency limit of organic photovoltaic devices can be overcome by Singlet Fission (SF), a photoinduced processes where two triplet states result from the “fission” of one excited singlet state [1]

  • A broad excited state absorption (ESA) band with maximum at 560 nm is observed at earliest time

  • The band decays on the way towards longer delays while a second ESA band rises concomitantly at 620 nm (Fig 2a)

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Summary

Introduction

The efficiency limit of organic photovoltaic devices can be overcome by Singlet Fission (SF), a photoinduced processes where two triplet states result from the “fission” of one excited singlet state [1]. This is shown by quantum chemical calculations, which suggest minor changes upon halogen substitution. Ultrafast broadband transient absorption provides experimental evidence and supports the correlation between key molecular properties and SF rates. Broadband transient absorption (TA) is performed with fs pump pulses and supercontinuum probing at 1 kHz repetition rate.

Results
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