R. Flores-Cruz, E. Vallejo-Castañeda, J. F. Acosta-Palacios, M. Arteaga-Varela, V. Rodríguez-Lugo
{"title":"Hydrogen adsorption and sensing response of MnBi2Te4 monolayers: insights from electronic structure, magnetism, and local symmetry","authors":"R. Flores-Cruz, E. Vallejo-Castañeda, J. F. Acosta-Palacios, M. Arteaga-Varela, V. Rodríguez-Lugo","doi":"10.1007/s10853-026-13708-6","DOIUrl":null,"url":null,"abstract":"<div><p>In this work, density functional theory (DFT) calculations were performed to investigate the adsorption behavior of H<sub>2</sub> molecules on a MnBi<sub>2</sub>Te<sub>4</sub> monolayer and assess its potential for hydrogen-sensing applications. Three adsorption configurations, namely TOP (Case I), HOLLOW (Case II), and BRIDGE (Case III), were analyzed in terms of structural stability, adsorption energetics, electronic properties, magnetic response, sensitivity, recovery time, charge transfer, and dynamical stability. Structural relaxations revealed that H₂ remains molecularly adsorbed without dissociation, indicating a physisorption-dominated interaction. The HOLLOW configuration was identified as the preferred adsorption site, while the initially placed BRIDGE configuration spontaneously relaxed toward a HOLLOW-like geometry. The most favorable adsorption energies were obtained for the HOLLOW and BRIDGE-derived structures, reaching − 0.164 eV and − 0.167 eV, respectively. Electronic band-structure calculations showed a slight increase in the band gap from 0.21 eV for pristine MnBi<sub>2</sub>Te<sub>4</sub> to approximately 0.233 eV after adsorption, while the total magnetic moment remained nearly unchanged, decreasing from 45 μB to 44.896–44.897 μB. Ab initio molecular dynamics simulations confirmed the structural stability and reversible adsorption behavior of the H<sub>2</sub> molecule throughout the simulation. Additionally, a local radial-variance descriptor was introduced to rationalize adsorption-site preference. The proposed approach relates adsorption stability to the degree of local geometric symmetry surrounding the adsorbed molecule and successfully explains the tendency of H<sub>2</sub> to migrate toward energetically favorable adsorption regions. These findings, together with the proposed radial-variance descriptor, provide new insights into adsorption-site selection and highlight the potential of MnBi<sub>2</sub>Te<sub>4</sub> as a reversible hydrogen-sensing material.</p><h3>Graphical abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":645,"journal":{"name":"Journal of Materials Science","volume":"61 42","pages":"32911 - 32935"},"PeriodicalIF":4.4000,"publicationDate":"2026-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Science","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s10853-026-13708-6","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
In this work, density functional theory (DFT) calculations were performed to investigate the adsorption behavior of H2 molecules on a MnBi2Te4 monolayer and assess its potential for hydrogen-sensing applications. Three adsorption configurations, namely TOP (Case I), HOLLOW (Case II), and BRIDGE (Case III), were analyzed in terms of structural stability, adsorption energetics, electronic properties, magnetic response, sensitivity, recovery time, charge transfer, and dynamical stability. Structural relaxations revealed that H₂ remains molecularly adsorbed without dissociation, indicating a physisorption-dominated interaction. The HOLLOW configuration was identified as the preferred adsorption site, while the initially placed BRIDGE configuration spontaneously relaxed toward a HOLLOW-like geometry. The most favorable adsorption energies were obtained for the HOLLOW and BRIDGE-derived structures, reaching − 0.164 eV and − 0.167 eV, respectively. Electronic band-structure calculations showed a slight increase in the band gap from 0.21 eV for pristine MnBi2Te4 to approximately 0.233 eV after adsorption, while the total magnetic moment remained nearly unchanged, decreasing from 45 μB to 44.896–44.897 μB. Ab initio molecular dynamics simulations confirmed the structural stability and reversible adsorption behavior of the H2 molecule throughout the simulation. Additionally, a local radial-variance descriptor was introduced to rationalize adsorption-site preference. The proposed approach relates adsorption stability to the degree of local geometric symmetry surrounding the adsorbed molecule and successfully explains the tendency of H2 to migrate toward energetically favorable adsorption regions. These findings, together with the proposed radial-variance descriptor, provide new insights into adsorption-site selection and highlight the potential of MnBi2Te4 as a reversible hydrogen-sensing material.
期刊介绍：
The Journal of Materials Science publishes reviews, full-length papers, and short Communications recording original research results on, or techniques for studying the relationship between structure, properties, and uses of materials. The subjects are seen from international and interdisciplinary perspectives covering areas including metals, ceramics, glasses, polymers, electrical materials, composite materials, fibers, nanostructured materials, nanocomposites, and biological and biomedical materials. The Journal of Materials Science is now firmly established as the leading source of primary communication for scientists investigating the structure and properties of all engineering materials.
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