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Nuclear dynamics of singlet exciton fission in pentacene single crystals.

Hélène SeilerMarcin KrynskiDaniela ZahnSebastian HammerYoav William WindsorThomas VasileiadisJens PflaumRalph ErnstorferMariana RossiHeinrich Schwoerer
Published in: Science advances (2021)
Singlet exciton fission (SEF) is a key process for developing efficient optoelectronic devices. An aspect rarely probed directly, yet with tremendous impact on SEF properties, is the nuclear structure and dynamics involved in this process. Here, we directly observe the nuclear dynamics accompanying the SEF process in single crystal pentacene using femtosecond electron diffraction. The data reveal coherent atomic motions at 1 THz, incoherent motions, and an anisotropic lattice distortion representing the polaronic character of the triplet excitons. Combining molecular dynamics simulations, time-dependent density-functional theory, and experimental structure factor analysis, the coherent motions are identified as collective sliding motions of the pentacene molecules along their long axis. Such motions modify the excitonic coupling between adjacent molecules. Our findings reveal that long-range motions play a decisive part in the electronic decoupling of the electronically correlated triplet pairs and shed light on why SEF occurs on ultrafast time scales.
Keyphrases
  • energy transfer
  • molecular dynamics simulations
  • density functional theory
  • molecular dynamics
  • single cell
  • magnetic resonance imaging
  • electron microscopy
  • big data
  • contrast enhanced
  • data analysis