Unravelling a Zigzag Pathway for Hot Carrier Collection with Graphene Electrode.
J Phys Chem Lett
; 12(11): 2886-2891, 2021 Mar 25.
Article
em En
| MEDLINE
| ID: mdl-33724034
ABSTRACT
The capture of photoexcited deep-band hot carriers, excited by photons with energies far above the bandgap, is of significant importance for photovoltaic and photoelectronic applications because it is directly related to the quantum efficiency of photon-to-electron conversion. By employing time-resolved photoluminescence and state-of-the-art time-domain density functional theory, we reveal that photoexcited hot carriers in organic-inorganic hybrid perovskites prefer a zigzag interfacial charge-transfer pathway, i.e., the hot carriers transfer back and forth between CH3NH3PbI3 and graphene electrode, before they reach a charge-separated state. Driven by quantum coherence and interlayer vibrational modes, this pathway at the semiconductor-graphene interface takes about 400 fs, much faster than the relaxation process within CH3NH3PbI3 (several picoseconds). Our work provides new insight into the fundamental understanding and precise manipulation of hot carrier dynamics at the complex interfaces, paving the way for highly efficient photovoltaic and photoelectric device optimization.
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01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
J Phys Chem Lett
Ano de publicação:
2021
Tipo de documento:
Article