To address the slow recombination of photogenerated charges in tetragonal CH3NH3PbI3, the evolution of extra electrons and holes is simulated through advanced ab initio molecular dynamics. We show that the localization of the charge carriers and their hopping from one polaronic state to another occur on a subpicosecond time scale. The localization, attended by weak bond contractions and elongations in the inorganic sublattice, is induced by thermal vibrations and only moderately perturbed by the disordered field generated by the organic cations. The simultaneous simulation of extra electrons and holes shows that they preferentially localize in spatially distinct regions. As determined by the overlap between the electron and hole wave functions, the probability of radiative bimolecular recombination is lowered by two orders of magnitude compared with that of optical generation. The separate polaronic localization of electrons and holes emerges as the key feature for achieving exceptional photovoltaic properties.

Origin of low electron-hole recombination rate in metal halide perovskites

Ambrosio F;
2018-01-01

Abstract

To address the slow recombination of photogenerated charges in tetragonal CH3NH3PbI3, the evolution of extra electrons and holes is simulated through advanced ab initio molecular dynamics. We show that the localization of the charge carriers and their hopping from one polaronic state to another occur on a subpicosecond time scale. The localization, attended by weak bond contractions and elongations in the inorganic sublattice, is induced by thermal vibrations and only moderately perturbed by the disordered field generated by the organic cations. The simultaneous simulation of extra electrons and holes shows that they preferentially localize in spatially distinct regions. As determined by the overlap between the electron and hole wave functions, the probability of radiative bimolecular recombination is lowered by two orders of magnitude compared with that of optical generation. The separate polaronic localization of electrons and holes emerges as the key feature for achieving exceptional photovoltaic properties.
File in questo prodotto:
Non ci sono file associati a questo prodotto.

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11386/4783487
 Attenzione

Attenzione! I dati visualizzati non sono stati sottoposti a validazione da parte dell'ateneo

Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 93
  • ???jsp.display-item.citation.isi??? 91
social impact