Long-Lived Hot Carriers in Two-Dimensional Perovskites: The Role of Alternating Cations in Interlayer Space

Qi Wei; Hui Ren; Jinjie Liu; Qi Liu; Chenhao Wang; Ting Wai Lau; Luwei Zhou; Tieyuan Bian; Yifan Zhou; Pengzhi Wang; Qiong Lei; Omar F. Mohammed; Mingjie Li; Jun Yin

doi:10.1021/acsenergylett.3c01691

Long-Lived Hot Carriers in Two-Dimensional Perovskites: The Role of Alternating Cations in Interlayer Space

Qi Wei, Hui Ren, Jinjie Liu, Qi Liu, Chenhao Wang, Ting Wai Lau, Luwei Zhou, Tieyuan Bian, Yifan Zhou, Pengzhi Wang, Qiong Lei, Omar F. Mohammed, Mingjie Li, Jun Yin

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Abstract

Solar absorbers featuring prolonged hot-carrier (HC) cooling are highly desired for the development of HC solar cells. Two-dimensional (2D) hybrid perovskites are known for their exceptional stability and tunable optoelectronic properties. Nevertheless, their hot-carrier dynamics have been inadequately investigated. Here, we demonstrate ultraslow hot-carrier cooling with a lifetime >2 ns and long HC diffusion length in 2D (ACA)(MA)PbI4 (ACA = acetamidinium) with alternating cations in the interlayer space (ACI), surpassing those of 3D MAPbBr3 and 2D Ruddlesden–Popper (PEA)2PbI4. Our nonadiabatic molecular dynamics simulations with spin–orbit coupling show that the enhanced HC cooling in the ACI-phase 2D perovskite is due to multiple split-off bands and reduced electron–phonon coupling. Furthermore, the hot electrons can be efficiently extracted from (ACA)(MA)PbI4 and then transferred to the electron-transporting layer. These new insights highlight the benefit of manipulating interlayer cations in 2D perovskites as an advantageous approach to control long-lived hot carriers, thus potentially enhancing photovoltaic device performance.

Original language	English (US)
Pages (from-to)	4315-4322
Number of pages	8
Journal	ACS Energy Letters
DOIs	https://doi.org/10.1021/acsenergylett.3c01691
State	Published - Sep 22 2023

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10.1021/acsenergylett.3c01691

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@article{62b75274c03f4d7f9bbca14c00f96334,

title = "Long-Lived Hot Carriers in Two-Dimensional Perovskites: The Role of Alternating Cations in Interlayer Space",

abstract = "Solar absorbers featuring prolonged hot-carrier (HC) cooling are highly desired for the development of HC solar cells. Two-dimensional (2D) hybrid perovskites are known for their exceptional stability and tunable optoelectronic properties. Nevertheless, their hot-carrier dynamics have been inadequately investigated. Here, we demonstrate ultraslow hot-carrier cooling with a lifetime >2 ns and long HC diffusion length in 2D (ACA)(MA)PbI4 (ACA = acetamidinium) with alternating cations in the interlayer space (ACI), surpassing those of 3D MAPbBr3 and 2D Ruddlesden–Popper (PEA)2PbI4. Our nonadiabatic molecular dynamics simulations with spin–orbit coupling show that the enhanced HC cooling in the ACI-phase 2D perovskite is due to multiple split-off bands and reduced electron–phonon coupling. Furthermore, the hot electrons can be efficiently extracted from (ACA)(MA)PbI4 and then transferred to the electron-transporting layer. These new insights highlight the benefit of manipulating interlayer cations in 2D perovskites as an advantageous approach to control long-lived hot carriers, thus potentially enhancing photovoltaic device performance.",

author = "Qi Wei and Hui Ren and Jinjie Liu and Qi Liu and Chenhao Wang and Lau, {Ting Wai} and Luwei Zhou and Tieyuan Bian and Yifan Zhou and Pengzhi Wang and Qiong Lei and Mohammed, {Omar F.} and Mingjie Li and Jun Yin",

note = "KAUST Repository Item: Exported on 2023-09-26 Acknowledgements: J.Y. acknowledges financial support from Hong Kong Polytechnic University (Grant no. P0042930) and a grant from the Research Grants Council of the Hong Kong Special Administrative Region, China (Project No. PolyU 25300823). M.L. acknowledges financial support from the Shenzhen Science, Technology and Innovation Commission (JCYJ20210324131806018), the Research Grants Council of the Hong Kong Special Administrative Region, China (Project No. PolyU 25301522 and PolyU 15301323), and the National Natural Science Foundation of China (22373081). Q.W. acknowledges support from the Natural Science Foundation of China (61904152). This work was also supported by King Abdullah University of Science and Technology (KAUST).",

year = "2023",

month = sep,

day = "22",

doi = "10.1021/acsenergylett.3c01691",

language = "English (US)",

pages = "4315--4322",

journal = "ACS Energy Letters",

issn = "2380-8195",

publisher = "AMER CHEMICAL SOC",

}

TY - JOUR

T1 - Long-Lived Hot Carriers in Two-Dimensional Perovskites: The Role of Alternating Cations in Interlayer Space

AU - Wei, Qi

AU - Ren, Hui

AU - Liu, Jinjie

AU - Liu, Qi

AU - Wang, Chenhao

AU - Lau, Ting Wai

AU - Zhou, Luwei

AU - Bian, Tieyuan

AU - Zhou, Yifan

AU - Wang, Pengzhi

AU - Lei, Qiong

AU - Mohammed, Omar F.

AU - Li, Mingjie

AU - Yin, Jun

N1 - KAUST Repository Item: Exported on 2023-09-26 Acknowledgements: J.Y. acknowledges financial support from Hong Kong Polytechnic University (Grant no. P0042930) and a grant from the Research Grants Council of the Hong Kong Special Administrative Region, China (Project No. PolyU 25300823). M.L. acknowledges financial support from the Shenzhen Science, Technology and Innovation Commission (JCYJ20210324131806018), the Research Grants Council of the Hong Kong Special Administrative Region, China (Project No. PolyU 25301522 and PolyU 15301323), and the National Natural Science Foundation of China (22373081). Q.W. acknowledges support from the Natural Science Foundation of China (61904152). This work was also supported by King Abdullah University of Science and Technology (KAUST).

PY - 2023/9/22

Y1 - 2023/9/22

N2 - Solar absorbers featuring prolonged hot-carrier (HC) cooling are highly desired for the development of HC solar cells. Two-dimensional (2D) hybrid perovskites are known for their exceptional stability and tunable optoelectronic properties. Nevertheless, their hot-carrier dynamics have been inadequately investigated. Here, we demonstrate ultraslow hot-carrier cooling with a lifetime >2 ns and long HC diffusion length in 2D (ACA)(MA)PbI4 (ACA = acetamidinium) with alternating cations in the interlayer space (ACI), surpassing those of 3D MAPbBr3 and 2D Ruddlesden–Popper (PEA)2PbI4. Our nonadiabatic molecular dynamics simulations with spin–orbit coupling show that the enhanced HC cooling in the ACI-phase 2D perovskite is due to multiple split-off bands and reduced electron–phonon coupling. Furthermore, the hot electrons can be efficiently extracted from (ACA)(MA)PbI4 and then transferred to the electron-transporting layer. These new insights highlight the benefit of manipulating interlayer cations in 2D perovskites as an advantageous approach to control long-lived hot carriers, thus potentially enhancing photovoltaic device performance.

AB - Solar absorbers featuring prolonged hot-carrier (HC) cooling are highly desired for the development of HC solar cells. Two-dimensional (2D) hybrid perovskites are known for their exceptional stability and tunable optoelectronic properties. Nevertheless, their hot-carrier dynamics have been inadequately investigated. Here, we demonstrate ultraslow hot-carrier cooling with a lifetime >2 ns and long HC diffusion length in 2D (ACA)(MA)PbI4 (ACA = acetamidinium) with alternating cations in the interlayer space (ACI), surpassing those of 3D MAPbBr3 and 2D Ruddlesden–Popper (PEA)2PbI4. Our nonadiabatic molecular dynamics simulations with spin–orbit coupling show that the enhanced HC cooling in the ACI-phase 2D perovskite is due to multiple split-off bands and reduced electron–phonon coupling. Furthermore, the hot electrons can be efficiently extracted from (ACA)(MA)PbI4 and then transferred to the electron-transporting layer. These new insights highlight the benefit of manipulating interlayer cations in 2D perovskites as an advantageous approach to control long-lived hot carriers, thus potentially enhancing photovoltaic device performance.

UR - http://hdl.handle.net/10754/694620

UR - https://pubs.acs.org/doi/10.1021/acsenergylett.3c01691

U2 - 10.1021/acsenergylett.3c01691

DO - 10.1021/acsenergylett.3c01691

M3 - Article

SN - 2380-8195

SP - 4315

EP - 4322

JO - ACS Energy Letters

JF - ACS Energy Letters

ER -

Long-Lived Hot Carriers in Two-Dimensional Perovskites: The Role of Alternating Cations in Interlayer Space

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