Electronic origin of the preferential NH3 response of N-substituted SnS2 monolayers: a first-principles study with machine learning force field-assisted assessment of structural stability
11 affiliations
- 1International PhD Program in Plasma and Thin Film Technology, Ming Chi University of Technology New Taipei City 243303 Taiwan
- 2Center for Plasma and Thin Film Technologies, Ming Chi University of Technology New Taipei City 243303 Taiwan
- 3Faculty of Chemistry, University of Science 227 Nguyen Van Cu, Cho Quan Ward Ho Chi Minh City Vietnam
- 4Vietnam National University Vo Truong Toan Street, Quarter 33, Linh Xuan Ward Ho Chi Minh City Vietnam
- 5International University Quarter 33, Linh Xuan Ward Ho Chi Minh City Vietnam
- 6Institute of Theoretical and Applied Research, Duy Tan University Ha Noi 100000 Vietnam
- 7School of Engineering and Technology, Duy Tan University Da Nang 550000 Vietnam
- 8Faculty of Basic Sciences, Nam Can Tho University Can Tho City Vietnam
- 9Department of Chemical System Engineering, School of Engineering, The University of Tokyo Japan
- 10Laboratory for Computational Physics, Institute for Computational Science and Artificial Intelligence, Van Lang University Ho Chi Minh City Vietnam
- 11Faculty of Mechanical, Electrical, and Computer Engineering, Van Lang School of Technology, Van Lang University Ho Chi Minh City Vietnam
Abstract
Spin-polarized density functional theory (DFT) was employed to investigate the adsorption and electronic responses of pristine and N-substituted SnS2 monolayers toward CO, CO2, and NH3. In parallel, a machine learning force field (MLFF) was developed and evaluated against DFT reference data to assess the structural and dynamical stability of the pristine and N-substituted substrates. The MLFF was not employed to predict gas adsorption or sensing properties, which were investigated exclusively using first-principles calculations. Among the three investigated gases, NH3 exhibits the strongest interaction with N-substituted SnS2, with an adsorption energy of −0.55 eV, an adsorption height of 1.712 Å, a Bader charge transfer of −0.22e, and a work-function change of −0.80 eV. Projected density of states and charge-density analyses reveal pronounced interfacial electronic redistribution for NH3, consistent with a stronger perturbation of the N-centered electronic states. This molecular differentiation is further reflected in the calculated relative conductivity-change metric at the Fermi level, which reaches 97.5% for NH3, compared with 44.8% for CO and 13.8% for CO2. MLFF calculations, phonon analysis, and molecular dynamics simulations further support the structural and dynamical stability of the modeled lattices. Collectively, these results establish a consistent relationship between substitutional nitrogen, spin-polarized electronic states, and the preferential electronic response toward NH3, providing a mechanistic basis for engineering N-substituted SnS2 for gas-sensing applications.
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BibTeX
@article{kha2026electronic,
title = {{Electronic origin of the preferential NH3 response of N-substituted SnS2 monolayers: a first-principles study with machine learning force field-assisted assessment of structural stability}},
author = {Truong Do Anh Kha and Tam V.-T. Mai and Lam K. Huynh and Truong Tuan Vu and D. M. Hoat and Nguyen Hai Dang and Minh-Thuan Pham and Duy Khanh Nguyen},
journal = {RSC Advances},
year = {2026},
month = nov,
doi = {10.1039/d6ra07435a},
url = {https://doi.org/10.1039/d6ra07435a},
note = {CC BY-NC 3.0},
}
RIS
TY - JOUR
TI - Electronic origin of the preferential NH3 response of N-substituted SnS2 monolayers: a first-principles study with machine learning force field-assisted assessment of structural stability
AU - Truong Do Anh Kha
AU - Tam V.-T. Mai
AU - Lam K. Huynh
AU - Truong Tuan Vu
AU - D. M. Hoat
AU - Nguyen Hai Dang
AU - Minh-Thuan Pham
AU - Duy Khanh Nguyen
PY - 2026
DA - 2026/11/04
JO - RSC Advances
DO - 10.1039/d6ra07435a
UR - https://doi.org/10.1039/d6ra07435a
AB - Spin-polarized density functional theory (DFT) was employed to investigate the adsorption and electronic responses of pristine and N-substituted SnS2 monolayers toward CO, CO2, and NH3. In parallel, a machine learning force field (MLFF) was developed and evaluated against DFT reference data to assess the structural and dynamical stability of the pristine and N-substituted substrates. The MLFF was not employed to predict gas adsorption or sensing properties, which were investigated exclusively using first-principles calculations. Among the three investigated gases, NH3 exhibits the strongest interaction with N-substituted SnS2, with an adsorption energy of −0.55 eV, an adsorption height of 1.712 Å, a Bader charge transfer of −0.22e, and a work-function change of −0.80 eV. Projected density of states and charge-density analyses reveal pronounced interfacial electronic redistribution for NH3, consistent with a stronger perturbation of the N-centered electronic states. This molecular differentiation is further reflected in the calculated relative conductivity-change metric at the Fermi level, which reaches 97.5% for NH3, compared with 44.8% for CO and 13.8% for CO2. MLFF calculations, phonon analysis, and molecular dynamics simulations further support the structural and dynamical stability of the modeled lattices. Collectively, these results establish a consistent relationship between substitutional nitrogen, spin-polarized electronic states, and the preferential electronic response toward NH3, providing a mechanistic basis for engineering N-substituted SnS2 for gas-sensing applications.
SN - 2046-2069
ER -