Highly Mobile Large Polarons in Black Phase CsPbI<sub>3</sub>

Zhang, Heng; Debroye, Elke; Steele, Julian A.; Roeffaers, Maarten B. J.; Hofkens, Johan; Wang, Hai I.; Bonn, Mischa

doi:10.1021/acsenergylett.0c02482

Cited by 44 publications

(51 citation statements)

References 57 publications

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“…The is due to the assumption that the quantum efficiency (QE) of carrier photogeneration and collection is 100%. For a 10% QE, the mobility for CsPbI3 nanocrystal thin films is ~25 cm 2 /Vs, which is in the same range as that characterized by the THz TDS (11). Moreover, this high mobility value (>10 cm 2 /Vs) at room temperature is consistent with the phonon scattering mechanism in CsPbI3 films, leading to bandlike transport.…”

Section: Resultssupporting

confidence: 70%

“…The inter-nanocrystal carrier transport is tunneling transport mechanism, indicated by n = 0, and the tunneling time is ~ 0.1 ps. For reference, Zhang et al reported a scattering time in CsPbI3 of ~0.02 ps, characterized by THz-TDS (11). As a result, more than 100 scattering events in one nanocrystal can be reduced by further increasing the electric field, leading to a longer drift length.…”

Section: Carrier Transport Mechanismmentioning

confidence: 99%

“…The first is based on the photon emission mechanism, which includes time-resolved photoluminescence (TRPL) and the streak camera technique (7). The second is the pump-probe mechanism, which includes transient absorption (8), THz-time domain spectroscopy (THz-TDS) (9)(10)(11), and other pump-probe approaches (12,13). As schematically indicated in Fig.…”

Section: Introductionmentioning

confidence: 99%

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Are solution processed CsPbI3 perovskite nanocrystalline films similar to traditional crystalline semiconductors?

Kobbekaduwa¹,

Liu²,

Zhao³

et al. 2021

Preprint

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We use ultrafast photocurrent spectroscopy with a sub-25 picosecond resolution to address a long-standing question in emergent perovskite materials: are solution-processed CsPbI3 perovskites nanocrystal films similar to their counterparts semiconductors including GaAs and Si? Prior to carrier trapping, all semiconductors show similar transition of transport mechanism from the band-like transport due to the longitudinal optical (LO) phonon scattering in the higher temperature region to a combination of band-like and hopping transport mechanisms in the lower temperature region. The critical difference is that CsPbI3 demonstrate the strongest carrier-LO phonon interaction among all semiconductors, most likely due to the unique cation-halogen bond arrangements within the highly symmetric lattice structure. This ultrafast dynamics work establish a foundation of fundamental carrier transport understating for perovskite optoelectronics.

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Section: Resultssupporting

confidence: 70%

Section: Carrier Transport Mechanismmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Are solution processed CsPbI3 perovskite nanocrystalline films similar to traditional crystalline semiconductors?

Kobbekaduwa¹,

Liu²,

Zhao³

et al. 2021

Preprint

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show abstract

“…This is consistent with a charge carrier diffusion length in the range of few to tens of μm in the IP direction [38][39][40] and high charge carrier mobility (> ~1-10 cm 2 V -1 s -1 ) as measured by Hall effect, 41 a field-effect transistor, 42 TRMC, 43,44 and terahertz spectroscopy. 45,46 The defect-tolerant nature of 3D perovskites is responsible for the efficient charge transport even at the grain boundary. 47,48 In contrast, the RIP/OOP values of 2D perovskites (PEA2MA2Pb3I10, FPEA2MA2Pb3I10, BA2MA2Pb3I10, and PEA2FA2Pb3I10) prepared by NTA were decreased to 14-43.…”

Section: Resultsmentioning

confidence: 99%

Top Thermal Annealing of 2D/3D Lead Halide Perovskites: Anisotropic Photoconductivity and Vertical Gradient of Dimensionality

Shimono

Nishikubo

Ishiwari

et al. 2021

J. Photopol. Sci. Technol.

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“…CsPbX 3 inorganic perovskite solar cells (PSCs) have emerged as burgeoning light harvesters and gained widespread attention by virtue of the highest power conversion efficiency (PCE) beyond 20% for their outstanding photophysical properties, including superior thermal stability, suitable bandgap, and high carrier mobility. [ 1–4 ] Unfortunately, the phase transition problem, caused by the mismatched radius between Cs + , Pb 2+ , and X − ions, is a notable obstacle to block their potential commercialization. [ 5,6 ] Recently, numerous efforts have been made to increase their phase stability through ionic incorporation, steric hindrance, metastable phases and reducing dimension.…”

Section: Introductionmentioning

confidence: 99%

N‐methyl‐2‐pyrrolidone Iodide as Functional Precursor Additive for Record Efficiency 2D Ruddlesden‐Popper (PEA)₂(Cs)_n₋₁Pb_nI₃_n₊₁ Solar Cells

et al. 2021

Adv Funct Materials

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2D perovskite (PEA)2(Cs)n−1PbnI3n+1 (PEA: phenylethylammonium) exhibits more strengthened phase stability than its 3D components under ambient conditions and hence gained great attention in recent years. However, uncontrollable crystallization kinetics in (PEA)2(Cs)n−1PbnI3n+1 leads to difficulty in controlling film morphology and phase‐orientation regulation, resulting in poor power conversion efficiency (PCE). Herein, by incorporating precursor additive N‐methyl‐2‐pyrrolidone iodide (NMPI), the crystallization rate during the deposition of (PEA)2(Cs)n−1PbnI3n+1 film is efficiently regulated. As a result, the 2D or quasi‐2D perovskite solar cell (PSC) delivers record PCEs in all reported 2D or quasi‐2D CsPbX3 families, for instance, the quasi‐2D (n = 20) CsPbI3 PSC exhibits a record PCE of 14.59%, showing significantly enhanced stability. Detailed characterization reveals that the NMPI forms hydrogen bonds with dimethylammonium iodide (DMAI) in the precursor to control crystallization rate for a smooth morphology with small fluctuation, which leads to improved carrier lifetime and reduced trap‐density. More importantly, femtosecond transient absorption (fs‐TA) measurements confirm an improved phase purity and the suppressed nonradiative recombination in quasi‐2D perovskite film. It is believed that this simple additive strategy paves a new route for solving phase transition and crystallization kinetic problems in 2D and quasi‐2D CsPbX3.

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Highly Mobile Large Polarons in Black Phase CsPbI₃

Cited by 44 publications

References 57 publications

Are solution processed CsPbI3 perovskite nanocrystalline films similar to traditional crystalline semiconductors?

Are solution processed CsPbI3 perovskite nanocrystalline films similar to traditional crystalline semiconductors?

Top Thermal Annealing of 2D/3D Lead Halide Perovskites: Anisotropic Photoconductivity and Vertical Gradient of Dimensionality

N‐methyl‐2‐pyrrolidone Iodide as Functional Precursor Additive for Record Efficiency 2D Ruddlesden‐Popper (PEA)₂(Cs)_n₋₁Pb_nI₃_n₊₁ Solar Cells

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Highly Mobile Large Polarons in Black Phase CsPbI3

Cited by 44 publications

References 57 publications

Are solution processed CsPbI3 perovskite nanocrystalline films similar to traditional crystalline semiconductors?

Are solution processed CsPbI3 perovskite nanocrystalline films similar to traditional crystalline semiconductors?

Top Thermal Annealing of 2D/3D Lead Halide Perovskites: Anisotropic Photoconductivity and Vertical Gradient of Dimensionality

N‐methyl‐2‐pyrrolidone Iodide as Functional Precursor Additive for Record Efficiency 2D Ruddlesden‐Popper (PEA)2(Cs)n−1PbnI3n+1 Solar Cells

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Highly Mobile Large Polarons in Black Phase CsPbI₃

N‐methyl‐2‐pyrrolidone Iodide as Functional Precursor Additive for Record Efficiency 2D Ruddlesden‐Popper (PEA)₂(Cs)_n₋₁Pb_nI₃_n₊₁ Solar Cells