Two-dimensional polyaniline crystal with metallic out-of-plane conductivity

Tao Zhang, Shu Chen, Petko St. Petkov, Peng Zhang, Haoyuan Qi, Nguyen Ngan Nguyen, Wenjie Zhang, Jiho Yoon, Peining Li, Thomas Brumme, Alexey Alfonsov, Zhongquan Liao, Mike Hambsch, Shunqi Xu, Lars Mester, Vladislav Kataev, Bernd Büchner, Stefan C. B. Mannsfeld, Ehrenfried Zschech, Stuart S. P. Parkin, Ute Kaiser, Thomas Heine (), Renhao Dong (), Rainer Hillenbrand () and Xinliang Feng ()
Additional contact information
Tao Zhang: Technische Universität Dresden
Shu Chen: CIC nanoGUNE BRTA
Petko St. Petkov: Faculty of Chemistry and Pharmacy
Peng Zhang: Technische Universität Dresden
Haoyuan Qi: Technische Universität Dresden
Nguyen Ngan Nguyen: Technische Universität Dresden
Wenjie Zhang: Max Planck Institute of Microstructure Physics
Jiho Yoon: Max Planck Institute of Microstructure Physics
Peining Li: CIC nanoGUNE BRTA
Thomas Brumme: Technische Universität Dresden
Alexey Alfonsov: Leibniz Institute for Solid State and Materials Research Dresden
Zhongquan Liao: Fraunhofer Institute for Ceramic Technologies and Systems (IKTS)
Mike Hambsch: Technische Universität Dresden
Shunqi Xu: Technische Universität Dresden
Lars Mester: CIC nanoGUNE BRTA
Vladislav Kataev: Leibniz Institute for Solid State and Materials Research Dresden
Bernd Büchner: Leibniz Institute for Solid State and Materials Research Dresden
Stefan C. B. Mannsfeld: Technische Universität Dresden
Ehrenfried Zschech: Technische Universität Dresden
Stuart S. P. Parkin: Max Planck Institute of Microstructure Physics
Ute Kaiser: Universität Ulm
Thomas Heine: Technische Universität Dresden
Renhao Dong: Technische Universität Dresden
Rainer Hillenbrand: CIC nanoGUNE BRTA and EHU/UPV
Xinliang Feng: Technische Universität Dresden

Nature, 2025, vol. 638, issue 8050, 411-417

Abstract: Abstract Linear conducting polymers show ballistic transport, imposed by mobile carriers moving along the polymer chains1,2, whereas conductance in the extended dimension, that is, between polymer strands or layers, remains weak due to the lack of intermolecular ordering and electronic coupling3–5. Here we report a multilayer-stacked two-dimensional polyaniline (2DPANI) crystal, which shows metallic out-of-plane charge transport with high electrical conductivity. The material comprises columnar π arrays with an interlayer distance of 3.59 Å and periodic rhombohedral lattices formed by interwoven polyaniline chains. Electron spin resonance spectroscopy reveals significant electron delocalization in the 2DPANI lattices. First-principles calculations indicate the in-plane 2D conjugation and strong interlayer electronic coupling in 2DPANI facilitated by the Cl-bridged layer stacking. To assess the local optical conductivity, we used terahertz and infrared nanospectroscopy to unravel a Drude-type conductivity with an infrared plasma frequency and an extrapolated local d.c. conductivity of around 200 S cm−1. Conductive scanning probe microscopy showed an unusually high out-of-plane conductivity of roughly 15 S cm−1. Transport measurements through vertical and lateral micro-devices revealed comparable high out-of-plane (roughly 7 S cm−1) and in-plane conductivity (roughly 16 S cm−1). The vertical micro-devices further showed increasing conductivity with decreasing temperature, demonstrating unique out-of-plane metallic transport behaviour. By using this multilayer-stacked 2D conducting polymer design, we predict the achievement of strong electronic coupling beyond in-plane interactions, potentially reaching three-dimensional metallic conductivity6,7.

Date: 2025
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DOI: 10.1038/s41586-024-08387-9

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