Remote Plasma‐Enabled Vertical Asymmetry Engineering of 2D PtSe 2 via Phase‐Preserving Chalcogen Exchange

ABSTRACT Vertical asymmetry in two‐dimensional (2D) transition metal dichalcogenides induces intrinsic dipoles, symmetry‐breaking functionalities, and interface‐specific electronic reconstruction. However, existing Janus synthesis processes rely on sequential treatments, high‐temperature substitution, or solid‐phase precursors. These approaches often cause phase transitions, lattice degradation, or defect formation, limiting scalability and device performance. Here, we introduce a remote plasma‐enabled strategy for phase‐preserving vertical asymmetry engineering in 2D Platinum Diselenide (PtSe 2 ) via one‐step chalcogen exchange. Using a single‐reactor H 2 S remote plasma, treatment at near‐room‐temperature (∼50°C) selectively substitutes top‐layer chalcogen atoms, forming Janus PtSSe with preserved crystallinity and minimal lattice perturbation. Increasing the temperature to 200–300°C enables complete conversion to crystalline 2D Platinum Disulfide (PtS 2 ). Janus PtSSe monolayers derived from exfoliated PtSe 2 exhibit an out‐of‐plane dipole and piezoresponse, with enhanced surface‐enhanced Raman scattering relative to corresponding PtSe 2 and PtS 2 monolayers. Extending this approach from monolayers to four‐layer (4L) PtSe 2 grown by metal‐organic chemical vapor deposition, selective sulfurization produces Janus PtSSe/3L‐PtSe 2 heterostructures with improved hydrogen evolution reaction kinetics relative to 4L‐PtSe 2 and fully sulfurized 4L‐PtS 2 . Our results establish remote plasma‐driven chalcogen exchange as a generalizable platform for symmetry‐controlled 2D materials, enabling scalable engineering of vertical polarity, interfacial charge distribution, and functional responses.

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Small
Published
2026-10-27
DOI
https://doi.org/10.1002/smll.76465
Primary Topic
2D Materials and Applications
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article
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Remote Plasma‐Enabled Vertical Asymmetry Engineering of 2D PtSe 2 via Phase‐Preserving Chalcogen Exchange

Heesuk Rho, Gwan‐Hyoung Lee, Sooyeon Ra, 박민지 et al.
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Small
2D Materials and Applications
article

Remote Plasma‐Enabled Vertical Asymmetry Engineering of 2D PtSe 2 via Phase‐Preserving Chalcogen Exchange

Heesuk Rho, Gwan‐Hyoung Lee, Sooyeon Ra, 박민지, Yuseok Kim, Lee DaeKwon, Sangmin An, Sukang Bae, Yunjo Jeong, Changheon Kim, Minseung Gyeon, Dongchul Sung, Sanghan Lee, Suklyun Hong, Hunsu Lee, Seok‐Ki Hyeong, Unseok Jung, Min Ji Im, Kibum Kang, Byung Joon Moon, Jangyup Son, Jaehyung Yu, Sang Kyu Park, Jinwoo Kim, Taesung Kim, Changgu Lee, Jimin Jang, Han-Koo Lee, Dong‐hyun Kim
article en

Abstract

ABSTRACT Vertical asymmetry in two‐dimensional (2D) transition metal dichalcogenides induces intrinsic dipoles, symmetry‐breaking functionalities, and interface‐specific electronic reconstruction. However, existing Janus synthesis processes rely on sequential treatments, high‐temperature substitution, or solid‐phase precursors. These approaches often cause phase transitions, lattice degradation, or defect formation, limiting scalability and device performance. Here, we introduce a remote plasma‐enabled strategy for phase‐preserving vertical asymmetry engineering in 2D Platinum Diselenide (PtSe 2 ) via one‐step chalcogen exchange. Using a single‐reactor H 2 S remote plasma, treatment at near‐room‐temperature (∼50°C) selectively substitutes top‐layer chalcogen atoms, forming Janus PtSSe with preserved crystallinity and minimal lattice perturbation. Increasing the temperature to 200–300°C enables complete conversion to crystalline 2D Platinum Disulfide (PtS 2 ). Janus PtSSe monolayers derived from exfoliated PtSe 2 exhibit an out‐of‐plane dipole and piezoresponse, with enhanced surface‐enhanced Raman scattering relative to corresponding PtSe 2 and PtS 2 monolayers. Extending this approach from monolayers to four‐layer (4L) PtSe 2 grown by metal‐organic chemical vapor deposition, selective sulfurization produces Janus PtSSe/3L‐PtSe 2 heterostructures with improved hydrogen evolution reaction kinetics relative to 4L‐PtSe 2 and fully sulfurized 4L‐PtS 2 . Our results establish remote plasma‐driven chalcogen exchange as a generalizable platform for symmetry‐controlled 2D materials, enabling scalable engineering of vertical polarity, interfacial charge distribution, and functional responses.

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Pohang University of Science and Technology (KR), Seoul National University (KR), Korea Advanced Institute of Science and Technology (KR), Sejong University (KR), Gwangju Institute of Science and Technology (KR), Quantum Devices (United States) (US), Pohang Accelerator Laboratory (KR), Institute of Engineering Research (KR), Korea Institute of Science and Technology (KR), Chung-Ang University (KR), Jeonbuk National University (KR), Sungkyunkwan University (KR), Korea University of Science and Technology (KR), Texas A&M University (US)
National Research Foundation of Korea, Ministry of Education, India, National Research Council of Science and Technology, Ministry of Science and ICT, South Korea, Institute for Information and Communications Technology Promotion
Openalex Percentile: Top 29%
2D Materials and Applications
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