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In this paper, the first-principles method based on density functional theory and non-equilibrium Green’s function is used to investigate the modulation of quantum interference and spin transport in N and B atom substituted meta-phenylene (M-OPE) molecular devices. The zero bias spin transmission spectrum of M-OPE molecular device shows that highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) are located at higher energy positions on both sides of the Fermi level, and there is a clear transmission spectrum valley (anti resonance peak) on the right side of the Fermi level. This indicates that M-OPE molecules are typical destructive quantum interference molecular systems. Research has found that N and B atoms replace carbon atoms at positions 1, 2, and 3 on the central ring of the molecule, which suppress the original destructive quantum interference of M-OPE molecular device to different extents. The substitution of N and B atoms at position 1 has no effect on the original destructive quantum interference of M-OPE molecular device, while the substitution of N and B atoms at positions 2 and 3 significantly suppresses the original destructive quantum interference of M-OPE molecular device. Therefore, there is a significant difference in the electrical conductivity of devices with N and B atoms at different positions, with the order of electrical conductivity values being N2 > N3 > N1 and B2 > B3 > B1. In this study, it is also found that the spin current value of device with B atom substitution is significantly higher than that of device with N atom substitution. After the substitution of B atom at position 2, the spin current value of the device under negative bias is significantly greater than that under positive bias, exhibiting a significant spin rectification effect. Based on the extended curled arrow rule proposed by O’Driscoll et al. to predict the behavior of quantum interference effects, we explain the physical mechanism by which N and B protons at different positions have different effects on the suppression of quantum interference in M-OPE molecular device. The results of the quantum interference and spin transport regulation of molecular systems by the substitution of B and N atoms can provide theoretical guidance for realizing the further application of heterocyclic aromatic hydrocarbons in molecular electronics.
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Keywords:
- first principles /
- density functional theory /
- molecular device /
- quantum interference /
- spin-transport
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图 1 N或B原子取代后M-OPE分子结示意图
Figure 1. Schematic diagram of M-OPE molecular junction after N or B atom substitution.
图 2 零偏压下(a) M-OPE和(b) N1的自旋透射谱. 红线和蓝线分别代表自旋向上和自旋向下
Figure 2. Spin transmission spectra of (a) M-OPE and (b) N1 under zero bias. Red and blue lines represent spin up and spin down, respectively.
图 3 (a) 零偏压下N2的自旋透射谱; (b) HOMO-up和HOMO-down位置的透射本征态. Isovalue的取值固定为0.35
Figure 3. (a) Spin transmission spectrum of N2 under zero bias; (b) transmission eigenstates of HOMO-up and HOMO-down. The isovalue is fixed at 0.35.
图 4 (a) 零偏压下N3的自旋透射谱; (b) LUMO-up和LUMO-down位置的透射本征态. Isovalue的取值固定为0.35
Figure 4. (a) Spin transmission spectrum of N3 under zero bias; (b) transmission eigenstates of LUMO-up and LUMO-down. The isovalue is fixed at 0.35.
图 5 零偏压下(a) B1和(b) B3的自旋透射谱
Figure 5. Spin transmission spectra of (a) B1 and (b) B3 under zero bias.
图 6 (a) 零偏压下B2的自旋透射谱; (b) LUMO-up和LUMO-down位置的透射本征态. Isovalue的取值固定为0.35
Figure 6. (a) Spin transmission spectrum of B2 under zero bias; (b) transmission eigenstates of LUMO-up and LUMO-down. The isovalue is fixed at 0.35.
图 7 器件的自旋电流-电压特性 (a) N1; (b) N2; (c) N3; (d) B1; (e) B2; (f) B3
Figure 7. Spin-resolved current-voltage characteristics of devices: (a) N1; (b) N2; (c) N3; (d) B1; (e) B2; (f) B3.
图 8 B原子在1, 2, 3位置取代的量子干涉效应行为预测
Figure 8. Prediction of quantum interference behavior of B atom substitution at positions 1, 2, and 3.
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[1] 闫瑞, 吴泽文, 谢稳泽, 李丹, 王音 2018 67 097301
Google Scholar
Yan R, Wu Z W, Xie W Z, Li D, Wang Y 2018 Acta Phys. Sin. 67 097301
Google Scholar
[2] Haidar E A, Tawfik S A, Stampfl C, Hirao K, Yoshizawa K, Nakajima T, Nakajima T, Soliman K A, El-Nahas A M 2021 Adv. Theor. Simul. 4 2000203
Google Scholar
[3] Su T A, Neupane M, Steigerwald M L, Venkataraman L, Nuckolls C 2016 Nat. Rev. Mater. 1 16002
Google Scholar
[4] Li Y, Zhou Y, Li Y, Hong W, Li H 2022 J. Phys. Chem. C 126 6420
Google Scholar
[5] 李瑞豪, 刘俊扬, 洪文晶 2022 71 067303
Google Scholar
Li R H, Liu J Y, Hong W J 2022 Acta Phys. Sin. 71 067303
Google Scholar
[6] Liu J, Huang X, Wang F, Hong W 2019 Acc. Chem. Res. 52 151
Google Scholar
[7] Fan Z, Chen K 2010 Appl. Phys. Lett. 96 053509
Google Scholar
[8] Hirai M, Tanaka N, Sakai M, Yamaguchi S 2019 Chem. Rev. 119 8291
Google Scholar
[9] Liu Q, Li J J, Wu D, Deng X Q, Zhang Z H, Fan Z Q, Chen K Q 2021 Phys. Rev. B 104 045412
Google Scholar
[10] Tsuji Y, Okazawa K, Kurino K, Yoshizawa K 2022 J. Phys. Chem. C 126 3244
Google Scholar
[11] Shubin N, Emelianov A, Uspenskii Y, Gorbatsevich A 2021 Phys. Chem. Chem. Phys. 23 20854
Google Scholar
[12] Ding Z K, Zeng Y J, Pan H, Luo N N, Zeng J, Tang L M, Chen K Q 2022 Phys. Rev. B 106 L121401
Google Scholar
[13] Pedersen K G L, Strange M, Leijnse M, Hedegård P, Solomon G C, Paaske J 2014 Phys. Rev. B 90 125413
Google Scholar
[14] Polakovsky A, Showman J, Valdiviezo J, Palma J L 2021 Phys. Chem. Chem. Phys. 23 1550
Google Scholar
[15] Pan H, Ding Z K, Zeng B W, Luo N N, Zeng J, Tang L M, Chen K Q 2023 Phys. Rev. B 107 104303
Google Scholar
[16] Qu F Y, Zhao Z H, Ren X R, Zhang S F, Wang L, Wang D 2022 Phys. Chem. Chem. Phys. 24 26795
Google Scholar
[17] Baer R, Neuhauser D 2002 J. Am. Chem. Soc. 124 4200
Google Scholar
[18] He R, Wang D, Luo N, Zeng J, Chen K Q, Tang L M 2023 Phys. Rev. Lett. 130 046401
Google Scholar
[19] 彭淑平, 黄旭东, 刘乾, 任鹏, 伍丹, 范志强 2023 72 058501
Google Scholar
Peng S P, Huang X D, Liu Q, Ren P, Wu D, Fan Z Q 2023 Acta Phys. Sin. 72 058501
Google Scholar
[20] Zhang W, Zhao Z B, Tan M, Adijiang A, Zhong S, Xu X, Zhao T, Ramya E, Sun L, Zhao X, Fan Z, Xiang D 2023 Chem. Sci. 14 11456
Google Scholar
[21] Zhang X J, Long M Q, Chen K Q, Shuai Z, Wan Q, Zou B S, Zhang Y 2009 Appl. Phys. Lett. 94 073503
Google Scholar
[22] Yang Y, Gantenbein M, Alqorashi A, Wei J, Sangtarash S, Hu D 2018 J. Phys. Chem. C 122 14965
Google Scholar
[23] Fan Z Q, Zhang Z H, Deng X Q, Tang G P, Chen K Q 2013 Appl. Phys. Lett. 102 023508
Google Scholar
[24] Wang Y H, Huang H, Yu Z, Zheng J F, Shao Y, Zhou X S, Chen J Z, Li J F 2020 J. Mater. Chem. C 8 6826
Google Scholar
[25] Wang X Y, Yao X, Narita A, Müllen K 2019 Acc. Chem. Res. 52 2491
Google Scholar
[26] Liu X S, Sangtarash S, Reber D, Zhang D, Sadeghi H, Shi J, Xiao Z Y, Hong W J, Lambert C J, Liu S X 2017 Angew. Chem. Int. Ed. 56 173
Google Scholar
[27] Chen Z Z, Wu S D, Lin J L, Chen L C, Cao J J, Shao X, Lambert C J, Zhang H L 2023 Adv. Electron. Mater. 9 2201024
Google Scholar
[28] Manrique D Z, Huang C, Baghernejad M, Zhao X, Al-Owaedi O A, Sadeghi H 2015 Nat. Commun. 6 6389
Google Scholar
[29] Büttiker M, Imry Y, Landauer R, Pinhas S 1985 Phys. Rev. B 31 6207
Google Scholar
[30] Smidstrup S, Markussen T, Vancraeyveld P, et al. 2019 J. Phys. Condens. Matter 32 015901
Google Scholar
[31] Deng X Q, Zhang Z H, Tang G P, Fan Z Q, Qiu M, Guo C 2012 Appl. Phys. Lett. 100 063107
Google Scholar
[32] O’Driscoll L J, Bryce M R 2021 Nanoscale 13 1103
Google Scholar
[33] O’Driscoll L J, Sangtarash S, Xu W, Daaoub A, Hong W J, Sadeghi H, Bryce M R 2021 J. Phys. Chem. C 125 17385
Google Scholar
[34] Markussen T, Stadler R, Thygesen K S 2010 Nano Lett. 10 4260
Google Scholar
[35] von Grotthuss E, John A, Kaese T, Wagner M 2018 Asian J. Org. Chem. 7 37
Google Scholar
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