Evolution of the Nature of Excitons and Electronic Couplings in Hybrid 2D Perovskites as a Function of Organic Cation π-Conjugation

Qingqing Dai, Hong Li, Gjergji Sini, Jean Luc Bredas

Research output: Contribution to journalArticlepeer-review

15 Scopus citations


2D perovskites have attracted much attention, due to their organic–inorganic hybrid nature and layered configuration. Multi-quantum-well structures then generally form since the inorganic frameworks and organic spacers have typically well-separated frontier energy levels. Here, it is focused on the opposite picture where wavefunction hybridization occurs between the frontier orbitals of the two components. Such a hybridization emerges upon tuning the strength of electronic coupling between the inorganic and organic layers. A series of model diammonium organic spacers is theoretically designed with varying extent of π-conjugation along their backbones. Wavefunction hybridization is realized in a Dion-Jacobson 2D perovskite combining PbI4 inorganic layers with anthracene-bis(ethan-1-ammonium) organic spacers. An analysis of the electronic band structures points to electronic couplings as high as 30–40 meV between the organic and inorganic components. Such couplings can lead to the formation of interfacial hybrid excitons or to the appearance of Dexter-type energy transfer conducive to phosphorescence in the organic layers. Overall, the results highlight that a variety of excitonic behaviors could be observed by tuning the degree of conjugation of the organic cations and the structural proximity and electronic couplings between the organic and inorganic constituents.

Original languageEnglish (US)
Article number2108662
JournalAdvanced Functional Materials
Issue number10
StatePublished - Mar 2 2022


  • 2D perovskites
  • DFT calculations
  • band structures
  • electronic couplings
  • excitons

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • General Chemistry
  • Condensed Matter Physics
  • General Materials Science
  • Electrochemistry
  • Biomaterials


Dive into the research topics of 'Evolution of the Nature of Excitons and Electronic Couplings in Hybrid 2D Perovskites as a Function of Organic Cation π-Conjugation'. Together they form a unique fingerprint.

Cite this