4.6 Article

Unveiling Ultrafast Carrier Extraction in Highly Efficient 2D/3D Bilayer Perovskite Solar Cells

Journal

ACS PHOTONICS
Volume -, Issue -, Pages -

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsphotonics.2c00982

Keywords

2D; 3D bilayer perovskites; perovskite solar cells; pump-probe transient absorption spectroscopy; hot carrier extraction; ultrafast carrier dynamics

Funding

  1. National Science and Technology Council, Taiwan [NSTC 109-2112-M-001-043-MY3, NSTC 110-2124-M-001-008-MY3, NSTC 110-2124-MA49-009-MY3, NSTC 111-2221-E001-006]
  2. Academia Sinica, Taiwan [AS-CDA-108-M08]
  3. King Abdullah University of Science and Technology (KAUST) [OSR-2018-CARF/CCF-3079]

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The development of multidimensional heterostructure lead halide perovskites has shown promise in enhancing the efficiency and stability of perovskite solar cells. In this study, the ultrafast carrier extraction in highly efficient 2D/3D bilayer perovskite solar cells was observed, shedding light on the advanced working mechanism of these solar cells.
The development of multidimensional heterostructure (2D/3D) lead halide perovskites has emerged as an effective approach to enhancing the efficiency and long-term stability of perovskite solar cells (PSCs). However, a fundamental understanding of the working mechanisms, such as carrier extraction, and carrier transfer dynamics in the multidimensional perovskites heterostructures remains elusive. Here, we observe the ultrafast carrier extraction in highly efficient 2D/ 3D bilayer PSCs (power conversion efficiency of 21.12%) via femtosecond time-resolved pump-probe transient absorption spec-troscopy (TAS). Notably, the formation of quasi-equilibrium states resulting in a subband absorption feature with an ultrafast lifetime of 440 fs was observed, and this feature is found only in 2D/3D perovskite heterostructure. The short-lived feature gives rise to the local electric-field-induced electroabsorption, resulting in an enhanced power conversion efficiency in 2D/3D PSCs. These findings can help comprehend the advanced working mechanism of highly efficient solar cells and other 2D/3D bilayer perovskite-based optoelectronic devices.

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