Variations of topological surface states of nodal line semimetal AlB<sub>2</sub> after adsorption in aqueous environment

Zhu Pang-Dong; Wang Chang-Hao; Wang Ru-Zhi

doi:10.7498/aps.73.20240404

Abstract

Topological semimetals have aroused great research interest due to their intrinsic topological physics and potential applications in devices. A key feature for all topological materials is the so-called bulk-boundary correspondence, which means that if there is non-trivial band topology in the bulk, then we can expect unique topologically protected conducting states in the surface, i.e. the topological surface state (TSS). Previously, the studies of the surface states of topological materials mainly focused on the pristine surfaces, while the topological nodal line semimetal surface states with adsorbates are rarely systematically studied. In this paper, the topological properties of the topological semimetal AlB₂ are studied by first-principles calculations, and the TSS position is calculated by constructing the Al- and B-terminated slab models. Observing the topological surface state, it is found that the drumhead-like TSS connects two Dirac nodes with no energy gaps on the node line, and the TSS of the Al end-terminated slab has a smaller energy dispersion than that of the B-terminated slab. The adsorption characteristics of AlB₂ (010) surface are studied, and it is found that the Gibbs free energy ($ {\Delta }{G}_{{{\mathrm{H}}}^{*}} $) for hydrogen adsorption on the surface of Al is only –0.031 eV, demonstrating excellent hydrogen evolution reaction (HER) performance. The changes of TSS after H, OH and H₂O are adsorbed on the surface of AlB₂ in aqueous solution environment are observed. The TSS change is the most significant when H is adsorbed, followed by OH adsorption. And the influence of H₂O on TSS due to its electrical neutrality and weak surface adsorption is very weak. Before and after adsorption, because the topology protection TSS still exists, only the energy changes, which confirms its robustness in the environment. The results of this work provide a systematic understanding of the effects of different adsorbents on the TSS of AlB₂, paving the way for future theoretical and experimental research in related fields, and alsopresent theoretical support for putting the topological materials into practical applications .

Keywords:

Authors and contacts

Key Laboratory of Advanced Functional Materials of Education Ministry of China, Institute of New Energy Materials and College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China

Corresponding author: Wang Chang-Hao, wangch33@bjut.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11804012) and the Urban Carbon Neutral Science and Technology Innovation Fund Project of Beijing University of Technology, China (Grant No. 048000514123695).

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References

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图 1 (a) AlB₂晶体结构; (b) 体相BZ和 (010)表面BZ, 绿线为不同k_sy值的$ \bar{X}—\bar{\varGamma } $高对称路径

Figure 1. (a) AlB₂ crystal structure; (b) bulk BZ and (010) surface BZ, the green line is the $ \bar{X}-\bar{\varGamma } $ high symmetry path with different k_sy values.

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图 2 (a) AlB₂的体相材料电子能带结构; (b) AlB₂节线分布示意图, 其中K点处的红圈为贝里相位计算路径

Figure 2. (a) Band structure of AlB₂; (b) schematic diagram of the node line distribution of AlB₂, where the red circle at K point is the calculation path of Berry phase.

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图 3 AlB₂ (010) 20层平板的能带结构　(a)表面BZ中k_sy = 0, 0.06, 0.15和0.3时, Al端面能带结构图; (b) k_sy = 0, 0.1, 0.15和0.3处B端面能带结构图, 动量位置如图1(b)所示; (c) Al端面平板模型在图3(a)中红色标记的能带$ \bar{X} $高对称点处的部分电荷密度图; (d) B端面平板模型在图3(b)中红色标记的能带$ \bar{\varGamma } $高对称点处的部分电荷密度图

Figure 3. Band structure of AlB₂ (010) 20-layer slab: (a) Band structure of Al-terminated slab when k_sy = 0, 0.06, 0.15 and 0.3 in surface BZ; (b) band structure of B-terminated slab at k_sy = 0, 0.1, 0.15 and 0.3, and the position of high symmetry path, as shown in Fig. 1(b); (c) partial charge density of Al-terminated slab at the high symmetry point $ \bar{X} $ of the energy band marked in red in Fig. 3(a); (d) partial charge density diagram of B-terminated slab at the high symmetry point $ \bar{\varGamma } $ of the energy band marked in red in Fig. 3(b).

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图 4 AlB₂ (010)表面吸附最佳位点图　(a) Al端面top点位吸附H; (b) Al端面top点位吸附OH; (c) Al端面top点位吸附H₂O; (d) B端面top点位吸附H; (e) B端面top点位吸附OH; (f) B端面top点位吸附H₂O

Figure 4. Optimal sites for the adsorption of AlB₂ (010) surface: (a) Al-terminated slab adsorbing H on the top site; (b) Al-terminated slab adsorbing OH on the top site; (c) Al-terminated slab adsorbing H₂O on the top site; (d) B-terminated slab adsorbing H on the top site; (e) B-terminated slab adsorbing OH on the top site; (f) B-terminated slab adsorbing H₂O on the top site.

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图 5 AlB₂ (010) 表面TSS吸附H后的变化　(a) Al端面平板单侧吸附H; (b) Al端面平板两侧吸附H; (c) B端面平板单侧吸附H; (d) B端面平板两侧吸附H; 红色标记处为两节线间的鼓膜状TSS

Figure 5. Changes of TSS adsorbing H of AlB₂ (010) surface: (a) Al-terminated slab adsorbing H on a single side; (b) Al-terminated slab adsorbing H on both sides; (c) B-terminated slab adsorbing H on a single side; (d) B-terminated slab adsorbing H on both sides. The red line represents the drumhead-like TSS between two nodal lines.

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图 6 AlB₂ TSS吸附OH后的变化　(a) Al端面平板单侧吸附OH; (b) Al端面平板两侧吸附OH; (c) B端面单侧吸附OH; (d) B端面平板两侧吸附OH; 红色标记处为两节线间的鼓膜状TSS

Figure 6. Changes of TSS adsorbing OH of AlB₂ (010) surface: (a) Al-terminated slab adsorbing OH on a single side; (b) Al-terminated slab adsorbing OH on both sides; (c) B-terminated slab adsorbing OH on a single side; (d) B-terminated slab adsorbing OH on both sides. The red line represents the drumhead-like TSS between two nodal lines.

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图 7 AlB₂ TSS吸附H₂O后的变化　(a) Al端面平板单侧吸附H₂O; (b) Al端面平板两侧吸附H₂O; (c) B端面平板单侧吸附H₂O; (d) B端面平板两侧吸附H₂O; 红色标记处为两节线间的鼓膜状TSS

Figure 7. Changes of TSS adsorbing H₂O of AlB₂ (010) surface: (a) Al-terminated slab adsorbing H₂O on a single side; (b) Al-terminated slab adsorbing H₂O on both sides; (c) B-terminated slab adsorbing H₂O on a single side; (d) B-terminated slab adsorbing H₂O on both sides. The red line represents the drumhead-like TSS between two nodal lines.

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表 1 AlB₂ (010) 表面吸附性能参数表, 对于Bader电荷分析“+”表示电荷的增益, 而“–”表示电荷的损失(单位为$ {{\mathrm{e}}}^{-} $)

Table 1. Parameters of adsorption properties of AlB₂ (010) surface. For the Bader charge analysis, “+” means the gain of the charge, while “–” means the loss of the charge (unit in $ {{\mathrm{e}}}^{-} $).

材料	端面	吸附物	最佳位点	$ \Delta G/{\mathrm{eV}}$	Bader电荷分析/e^–
材料	端面	吸附物	最佳位点	$ \Delta G/{\mathrm{eV}}$	吸附物	B	Al
AlB₂	Al	H	top	–0.031	+0.543	+0.073	–0.553
		OH	top	–0.253	+0.737	+0.002	–0.751
		H₂O	top	0.682	+0.368	+0.178	–0.556
	B	H	top	–1.659	+0.517	–0.174	–0.019
		OH	top	–1.815	+0.717	–0.244	–0.008
		H₂O	top	0.009	+0.384	–0.127	–0.001

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[1]	Ando Y 2013 J. Phys. Soc. Jpn. 82 102001 Google Scholar
[2]	Sato M, Ando Y 2017 Rep. Prog. Phys. 80 076501 Google Scholar
[3]	Gao H, Venderbos J W F, Kim Y, Rappe A M 2019 Annu. Rev. Mater. Res. 49 153 Google Scholar
[4]	Yan B, Felser C 2017 Annu. Rev. Conden. Ma. P. 8 337 Google Scholar
[5]	Wang Z J, Sun Y, Chen X Q, Franchini C, Xu G, Weng H M, Dai X, Fang Z 2012 Phys. Rev. B 85 195320 Google Scholar
[6]	Fang C, Weng H M, Dai X, Fang Z 2016 Chin. Phys. B 25 117106 Google Scholar
[7]	Liu Z K, Zhou B, Zhang Y, Wang Z J, Weng H M, Prabhakaran D, Mo S K, Shen Z X, Fang Z, Dai X, Hussain Z, Chen Y L 2014 Science 343 864 Google Scholar
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[19]	Li G W, Huang J, Yang Q, Zhang L G, Mu Q G, Sun Y, Parkin S, Chang K, Felser C 2021 J. Energy Chem. 62 516 Google Scholar
[20]	Wei Y H, Ma D S, Yuan H K, Wang X, Kuang M Q 2023 Phys. Rev. B 107 235414 Google Scholar
[21]	Rajamathi C R, Gupta U, Kumar N, Yang H, Sun Y, Süß V, Shekhar C, Schmidt M, Blumtritt H, Werner P, Yan B, Parkin S, Felser C, Rao C N R 2017 Adv. Mater. 29 1606202 Google Scholar
[22]	Liu W, Zhang X M, Meng W Z, Liu Y, Dai X F, Liu G D 2022 iScience 25 103543 Google Scholar
[23]	Kong X P, Jiang T, Gao J J, Shi X B, Shao J, Yuan Y H, Qiu H J, Zhao W W 2021 J. Phys. Chem. Lett. 12 3740 Google Scholar
[24]	Li J X, Ma H, Xie Q, Feng S B, Ullah S, Li R H, Dong J H, Li D Z, Li Y Y, Chen X Q 2018 Sci. China Mater. 61 23 Google Scholar
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[26]	Wang L R, Zhang X M, Meng W Z, Liu Y, Dai X F, Liu G D 2021 J. Mater. Chem. A 9 22453 Google Scholar
[27]	Ren Z B, Zhang H N, Wang S H, Huang B B, Dai Y, Wei W 2022 J. Mater. Chem. A 10 8568 Google Scholar
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[31]	Loa I, Kunc K, Syassen K, Bouvier P 2002 Phys. Rev. B 66 134101 Google Scholar
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[33]	Greeley J, Jaramillo T F, Bonde J, Chorkendorff I B, Norskov J K 2006 Nat. Mater. 5 909 Google Scholar

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Variations of topological surface states of nodal line semimetal AlB₂ after adsorption in aqueous environment

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Corresponding author: Wang Chang-Hao, wangch33@bjut.edu.cn

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Variations of topological surface states of nodal line semimetal AlB2 after adsorption in aqueous environment

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Corresponding author: Wang Chang-Hao, wangch33@bjut.edu.cn

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Variations of topological surface states of nodal line semimetal AlB₂ after adsorption in aqueous environment