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Main Authors: Fu, Shuai, Huang, Xing, Gao, Guoquan, Petkov, Petko St., Gao, Wenpei, Zhang, Jianjun, Gao, Lei, Zhang, Heng, Liu, Min, Hambsch, Mike, Zhang, Wenjie, Zhang, Jiaxu, Li, Keming, Kaiser, Ute, Parkin, Stuart S. P., Mannsfeld, Stefan C. B., Zhu, Tong, Wang, Hai I., Wang, Zhiyong, Dong, Renhao, Feng, Xinliang, Bonn, Mischa
Format: Preprint
Published: 2025
Subjects:
Online Access:https://arxiv.org/abs/2501.08742
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author Fu, Shuai
Huang, Xing
Gao, Guoquan
Petkov, Petko St.
Gao, Wenpei
Zhang, Jianjun
Gao, Lei
Zhang, Heng
Liu, Min
Hambsch, Mike
Zhang, Wenjie
Zhang, Jiaxu
Li, Keming
Kaiser, Ute
Parkin, Stuart S. P.
Mannsfeld, Stefan C. B.
Zhu, Tong
Wang, Hai I.
Wang, Zhiyong
Dong, Renhao
Feng, Xinliang
Bonn, Mischa
author_facet Fu, Shuai
Huang, Xing
Gao, Guoquan
Petkov, Petko St.
Gao, Wenpei
Zhang, Jianjun
Gao, Lei
Zhang, Heng
Liu, Min
Hambsch, Mike
Zhang, Wenjie
Zhang, Jiaxu
Li, Keming
Kaiser, Ute
Parkin, Stuart S. P.
Mannsfeld, Stefan C. B.
Zhu, Tong
Wang, Hai I.
Wang, Zhiyong
Dong, Renhao
Feng, Xinliang
Bonn, Mischa
contents Hot carriers, inheriting excess kinetic energy from high-energy photons, underpin numerous optoelectronic applications involving non-equilibrium transport processes. Current research on hot carriers has predominantly focused on inorganic materials, with little attention paid to organic-based systems due to their ultrafast energy relaxation and inefficient charge transport. Here, we overturn this paradigm by demonstrating highly mobile hot carriers in solution-processable, highly crystalline two-dimensional conjugated coordination polymer (2D c-CP) Cu3BHT (BHT = benzenehexathiol) films. Leveraging a suite of ultrafast spectroscopic and imaging techniques, we unravel the microscopic charge transport landscape in Cu3BHT films following non-equilibrium photoexcitation across temporal, spatial, and frequency domains, revealing two distinct high-mobility transport regimes. In the non-equilibrium transport regime, hot carriers achieve ultrahigh mobility of ~2,000 cm2 V-1 s-1, traversing grain boundaries up to 300 nm within a picosecond. In the quasi-equilibrium transport regime, free carriers exhibit Drude-type band-like transport with a remarkable mobility of ~400 cm2 V-1 s-1 and an intrinsic diffusion length exceeding 1 micrometer. These findings establish 2D c-CPs as versatile platforms for exploring high-mobility non-equilibrium transport, unlocking new opportunities for organic-based hot carrier applications.
format Preprint
id arxiv_https___arxiv_org_abs_2501_08742
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Beyond the band edge: Unveiling high-mobility hot carriers in a two-dimensional conjugated coordination polymer
Fu, Shuai
Huang, Xing
Gao, Guoquan
Petkov, Petko St.
Gao, Wenpei
Zhang, Jianjun
Gao, Lei
Zhang, Heng
Liu, Min
Hambsch, Mike
Zhang, Wenjie
Zhang, Jiaxu
Li, Keming
Kaiser, Ute
Parkin, Stuart S. P.
Mannsfeld, Stefan C. B.
Zhu, Tong
Wang, Hai I.
Wang, Zhiyong
Dong, Renhao
Feng, Xinliang
Bonn, Mischa
Materials Science
Soft Condensed Matter
Hot carriers, inheriting excess kinetic energy from high-energy photons, underpin numerous optoelectronic applications involving non-equilibrium transport processes. Current research on hot carriers has predominantly focused on inorganic materials, with little attention paid to organic-based systems due to their ultrafast energy relaxation and inefficient charge transport. Here, we overturn this paradigm by demonstrating highly mobile hot carriers in solution-processable, highly crystalline two-dimensional conjugated coordination polymer (2D c-CP) Cu3BHT (BHT = benzenehexathiol) films. Leveraging a suite of ultrafast spectroscopic and imaging techniques, we unravel the microscopic charge transport landscape in Cu3BHT films following non-equilibrium photoexcitation across temporal, spatial, and frequency domains, revealing two distinct high-mobility transport regimes. In the non-equilibrium transport regime, hot carriers achieve ultrahigh mobility of ~2,000 cm2 V-1 s-1, traversing grain boundaries up to 300 nm within a picosecond. In the quasi-equilibrium transport regime, free carriers exhibit Drude-type band-like transport with a remarkable mobility of ~400 cm2 V-1 s-1 and an intrinsic diffusion length exceeding 1 micrometer. These findings establish 2D c-CPs as versatile platforms for exploring high-mobility non-equilibrium transport, unlocking new opportunities for organic-based hot carrier applications.
title Beyond the band edge: Unveiling high-mobility hot carriers in a two-dimensional conjugated coordination polymer
topic Materials Science
Soft Condensed Matter
url https://arxiv.org/abs/2501.08742