title: Spin-conserving carrier recombination in conjugated polymers.
abstract: The ultimate efficiency of polymer light-emitting diodes is limited by the fraction of charges recombining in the molecular singlet manifold. We address the question of whether this fraction can principally exceed the fundamental limit set down by spin statistics, which requires the possibility of spin changes during exciton formation. Sensitized phosphorescence at 4-300 K enables a direct quantification of spin conversion in coulombically bound electron-hole pairs, the precursors to exciton formation. These are stabilized in external electric fields over times relevant to carrier transport, capture and recombination in devices. No interconversion of exciton intermediates between singlet and triplet configurations is observed. Static magnetic fields are equally unable to induce spin mixing in electroluminescence. Our observations imply substantial exchange splitting at all times during carrier capture. Prior statements regarding increased singlet yields above 25% merely on the basis of higher singlet than triplet formation rates should therefore be re-examined.
authors.affiliation: Photonics and Optoelectronics Group, Physics Department and CeNS, Ludwig-Maximilians-Universität, Amalienstr. 54, 80799 Munich, Germany.
authors.forename: Martin
authors.initials: M
authors.lastname: Reufer
authors.forename: Manfred J
authors.initials: MJ
authors.lastname: Walter
authors.forename: Pavlos G
authors.initials: PG
authors.lastname: Lagoudakis
authors.forename: Anne Beate
authors.initials: AB
authors.lastname: Hummel
authors.forename: Johanna S
authors.initials: JS
authors.lastname: Kolb
authors.forename: Hartmut G
authors.initials: HG
authors.lastname: Roskos
authors.forename: Ullrich
authors.initials: U
authors.lastname: Scherf
authors.forename: John M
authors.initials: JM
authors.lastname: Lupton
mesh_terms: D004583:Electrons; D006838:Hydrocarbons; D008280:Magnetics; D008956:Models, Chemical; D011108:Polymers / Q000737:chemistry*; D013696:Temperature; D013997:Time Factors
chemical_list: D006838:Hydrocarbons; D011108:Polymers