A-Site Cation-Induced Hot-Carrier Lifetime Extension in 2D Perovskites: A New Strategy for X-Ray Detection Enhancement

Shilong Jia; Xiaolong Feng; Hanqing Zeng; Pengda Tong; Shisong Zhang; Hongjie Xu; Jiaxue You; Lu Zhang; Shengzhong Liu

doi:10.1002/smll.202513374

A-Site Cation-Induced Hot-Carrier Lifetime Extension in 2D Perovskites: A New Strategy for X-Ray Detection Enhancement

Shilong Jia
, Xiaolong Feng
, Hanqing Zeng
, Pengda Tong
, Shisong Zhang
, Hongjie Xu
, Jiaxue You
, Lu Zhang^*
, Shengzhong Liu^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

1 Citation (Scopus)

Abstract

2D metal halide perovskites exhibit exceptional potential for X-ray detection due to their high lattice stability and moisture-resistant layered structures. However, energy loss due to rapid hot carrier (HC) cooling during high-energy X-ray irradiation limits the device performance. Herein, we prolong HC lifetimes in 2D perovskites through A-site cation engineering, synthesizing single-crystalline DMePDAPbI₄ (DMePDA) and MPDAPb₂I₆ (MPDA) structures. By tailoring molecular polarity and hydrogen-bonding capability via functional group substitution, MPDA achieves enhanced lattice rigidity and suppressed low-frequency phonon modes. These structural features directly reduce carrier–phonon scattering and phonon-mediated non-radiative energy dissipation, thereby retarding HC cooling. Femtosecond transient absorption confirms MPDA extends HC cooling times to 80 ps (vs. 10 ps in DMePDA) with peak temperatures reaching 535 K. By integrating a hot-electron extraction layer, MPDA achieves 51.4% HC extraction efficiency sixfold-higher than that of DMePDA. Consequently, vertical X-ray detectors exhibit an improved sensitivity of 12834.1 µC Gy_air⁻¹ cm⁻². These results establish organic cation design as a transformative strategy for harnessing hot carriers in radiation detection. © 2026 Wiley-VCH GmbH.

Original language	English
Article number	e13374
Number of pages	9
Journal	Small
Volume	22
Issue number	13
Online published	29 Jan 2026
DOIs	https://doi.org/10.1002/smll.202513374
Publication status	Published - 3 Mar 2026

Funding

S.L. is grateful for support from Key project of National Natural Science Foundation of China (U21A20102), National Natural Science Foundation of China (62174103), and the 111 project (B21005). J.Y. is grateful for support from Hon Hai (AC-202403-02-3).

Research Keywords

2D Perovskite
hot carrier
X-ray detection

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title = "A-Site Cation-Induced Hot-Carrier Lifetime Extension in 2D Perovskites: A New Strategy for X-Ray Detection Enhancement",

abstract = "2D metal halide perovskites exhibit exceptional potential for X-ray detection due to their high lattice stability and moisture-resistant layered structures. However, energy loss due to rapid hot carrier (HC) cooling during high-energy X-ray irradiation limits the device performance. Herein, we prolong HC lifetimes in 2D perovskites through A-site cation engineering, synthesizing single-crystalline DMePDAPbI4 (DMePDA) and MPDAPb2I6 (MPDA) structures. By tailoring molecular polarity and hydrogen-bonding capability via functional group substitution, MPDA achieves enhanced lattice rigidity and suppressed low-frequency phonon modes. These structural features directly reduce carrier–phonon scattering and phonon-mediated non-radiative energy dissipation, thereby retarding HC cooling. Femtosecond transient absorption confirms MPDA extends HC cooling times to 80 ps (vs. 10 ps in DMePDA) with peak temperatures reaching 535 K. By integrating a hot-electron extraction layer, MPDA achieves 51.4\% HC extraction efficiency sixfold-higher than that of DMePDA. Consequently, vertical X-ray detectors exhibit an improved sensitivity of 12834.1 µC Gyair−1 cm−2. These results establish organic cation design as a transformative strategy for harnessing hot carriers in radiation detection. {\textcopyright} 2026 Wiley-VCH GmbH.",

keywords = "2D Perovskite, hot carrier, X-ray detection",

author = "Shilong Jia and Xiaolong Feng and Hanqing Zeng and Pengda Tong and Shisong Zhang and Hongjie Xu and Jiaxue You and Lu Zhang and Shengzhong Liu",

year = "2026",

month = mar,

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doi = "10.1002/smll.202513374",

language = "English",

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TY - JOUR

T1 - A-Site Cation-Induced Hot-Carrier Lifetime Extension in 2D Perovskites

T2 - A New Strategy for X-Ray Detection Enhancement

AU - Jia, Shilong

AU - Feng, Xiaolong

AU - Zeng, Hanqing

AU - Tong, Pengda

AU - Zhang, Shisong

AU - Xu, Hongjie

AU - You, Jiaxue

AU - Zhang, Lu

AU - Liu, Shengzhong

PY - 2026/3/3

Y1 - 2026/3/3

N2 - 2D metal halide perovskites exhibit exceptional potential for X-ray detection due to their high lattice stability and moisture-resistant layered structures. However, energy loss due to rapid hot carrier (HC) cooling during high-energy X-ray irradiation limits the device performance. Herein, we prolong HC lifetimes in 2D perovskites through A-site cation engineering, synthesizing single-crystalline DMePDAPbI4 (DMePDA) and MPDAPb2I6 (MPDA) structures. By tailoring molecular polarity and hydrogen-bonding capability via functional group substitution, MPDA achieves enhanced lattice rigidity and suppressed low-frequency phonon modes. These structural features directly reduce carrier–phonon scattering and phonon-mediated non-radiative energy dissipation, thereby retarding HC cooling. Femtosecond transient absorption confirms MPDA extends HC cooling times to 80 ps (vs. 10 ps in DMePDA) with peak temperatures reaching 535 K. By integrating a hot-electron extraction layer, MPDA achieves 51.4% HC extraction efficiency sixfold-higher than that of DMePDA. Consequently, vertical X-ray detectors exhibit an improved sensitivity of 12834.1 µC Gyair−1 cm−2. These results establish organic cation design as a transformative strategy for harnessing hot carriers in radiation detection. © 2026 Wiley-VCH GmbH.

AB - 2D metal halide perovskites exhibit exceptional potential for X-ray detection due to their high lattice stability and moisture-resistant layered structures. However, energy loss due to rapid hot carrier (HC) cooling during high-energy X-ray irradiation limits the device performance. Herein, we prolong HC lifetimes in 2D perovskites through A-site cation engineering, synthesizing single-crystalline DMePDAPbI4 (DMePDA) and MPDAPb2I6 (MPDA) structures. By tailoring molecular polarity and hydrogen-bonding capability via functional group substitution, MPDA achieves enhanced lattice rigidity and suppressed low-frequency phonon modes. These structural features directly reduce carrier–phonon scattering and phonon-mediated non-radiative energy dissipation, thereby retarding HC cooling. Femtosecond transient absorption confirms MPDA extends HC cooling times to 80 ps (vs. 10 ps in DMePDA) with peak temperatures reaching 535 K. By integrating a hot-electron extraction layer, MPDA achieves 51.4% HC extraction efficiency sixfold-higher than that of DMePDA. Consequently, vertical X-ray detectors exhibit an improved sensitivity of 12834.1 µC Gyair−1 cm−2. These results establish organic cation design as a transformative strategy for harnessing hot carriers in radiation detection. © 2026 Wiley-VCH GmbH.

KW - 2D Perovskite

KW - hot carrier

KW - X-ray detection

UR - https://www.scopus.com/pages/publications/105028990221

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-105028990221&origin=recordpage

U2 - 10.1002/smll.202513374

DO - 10.1002/smll.202513374

M3 - RGC 21 - Publication in refereed journal

SN - 1613-6810

VL - 22

JO - Small

JF - Small

IS - 13

M1 - e13374

ER -

A-Site Cation-Induced Hot-Carrier Lifetime Extension in 2D Perovskites: A New Strategy for X-Ray Detection Enhancement

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