TY - JOUR
T1 - Charge Carrier Diffusion Dynamics in Multisized Quaternary Alkylammonium-Capped CsPbBr3 Perovskite Nanocrystal Solids
AU - Gutiérrez Álvarez, Sol
AU - Lin, Weihua
AU - Abdellah, Mohamed
AU - Meng, Jie
AU - Žídek, Karel
AU - Pullerits, Tõnu
AU - Zheng, Kaibo
N1 - Publisher Copyright:
© 2021 The Authors. Published by American Chemical Society.
PY - 2021/9/22
Y1 - 2021/9/22
N2 - CsPbBr3 quantum dots (QDs) are promising candidates for optoelectronic devices. The substitution of oleic acid (OA) and oleylamine (OLA) capping agents with a quaternary alkylammonium such as di-dodecyl dimethyl ammonium bromide (DDAB) has shown an increase in external quantum efficiency (EQE) from 0.19% (OA/OLA) to 13.4% (DDAB) in LED devices. The device performance significantly depends on both the diffusion length and the mobility of photoexcited charge carriers in QD solids. Therefore, we investigated the charge carrier transport dynamics in DDAB-capped CsPbBr3 QD solids by constructing a bi-sized QD mixture film. Charge carrier diffusion can be monitored by quantitatively varying the ratio between two sizes of QDs, which varies the mean free path of the carriers in each QD cluster. Excited-state dynamics of the QD solids obtained from ultrafast transient absorption spectroscopy reveals that the photogenerated electrons and holes are difficult to diffuse among small-sized QDs (4 nm) due to the strong quantum confinement. On the other hand, both photoinduced electrons and holes in large-sized QDs (10 nm) would diffuse toward the interface with the small-sized QDs, followed by a recombination process. Combining the carrier diffusion study with a Monte Carlo simulation on the QD assembly in the mixture films, we can calculate the diffusion lengths of charge carriers to be ∼239 ± 16 nm in 10 nm CsPbBr3 QDs and the mobility values of electrons and holes to be 2.1 (± 0.1) and 0.69 (± 0.03) cm2/V s, respectively. Both parameters indicate an efficient charge carrier transport in DDAB-capped QD films, which rationalized the perfect performance of their LED device application.
AB - CsPbBr3 quantum dots (QDs) are promising candidates for optoelectronic devices. The substitution of oleic acid (OA) and oleylamine (OLA) capping agents with a quaternary alkylammonium such as di-dodecyl dimethyl ammonium bromide (DDAB) has shown an increase in external quantum efficiency (EQE) from 0.19% (OA/OLA) to 13.4% (DDAB) in LED devices. The device performance significantly depends on both the diffusion length and the mobility of photoexcited charge carriers in QD solids. Therefore, we investigated the charge carrier transport dynamics in DDAB-capped CsPbBr3 QD solids by constructing a bi-sized QD mixture film. Charge carrier diffusion can be monitored by quantitatively varying the ratio between two sizes of QDs, which varies the mean free path of the carriers in each QD cluster. Excited-state dynamics of the QD solids obtained from ultrafast transient absorption spectroscopy reveals that the photogenerated electrons and holes are difficult to diffuse among small-sized QDs (4 nm) due to the strong quantum confinement. On the other hand, both photoinduced electrons and holes in large-sized QDs (10 nm) would diffuse toward the interface with the small-sized QDs, followed by a recombination process. Combining the carrier diffusion study with a Monte Carlo simulation on the QD assembly in the mixture films, we can calculate the diffusion lengths of charge carriers to be ∼239 ± 16 nm in 10 nm CsPbBr3 QDs and the mobility values of electrons and holes to be 2.1 (± 0.1) and 0.69 (± 0.03) cm2/V s, respectively. Both parameters indicate an efficient charge carrier transport in DDAB-capped QD films, which rationalized the perfect performance of their LED device application.
KW - CsPbBr
KW - DDAB
KW - carrier transport
KW - charge transfer
KW - diffusion lengths
KW - quantum dot photovoltaics
KW - ultrafast spectroscopy
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U2 - 10.1021/acsami.1c11676
DO - 10.1021/acsami.1c11676
M3 - Article
C2 - 34515458
AN - SCOPUS:85116060763
SN - 1944-8244
VL - 13
SP - 44742
EP - 44750
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 37
ER -