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Thermoelectric properties of acene molecular junctions

Xie Zhong-Xiang Yu Xia Jia Pin-Zhen Chen Xue-Kun Deng Yuan-Xiang Zhang Yong Zhou Wu-Xing

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Thermoelectric properties of acene molecular junctions

Xie Zhong-Xiang, Yu Xia, Jia Pin-Zhen, Chen Xue-Kun, Deng Yuan-Xiang, Zhang Yong, Zhou Wu-Xing
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  • By using non-equilibrium Green’s function method, we investigate the thermoelectric properties of molecular junctions based on acene-linked graphene nanoribbons. The effects of the length of the acene molecule, the contact position between the acene molecule and graphene nanoribbon electrode on the thermoelectric parameters are mainly considered in this work. It is found that the phonon contribution is dominant in the thermal conductance corresponding to the maximum of the thermoelectric figure of merit (ZTmax). As the length of the acene molecule increases, the phonon thermal conductance decreases monotonically, and eventually becomes almost independent of the acene molecule’ length. When the acene molecules contact the middle (upper) part of the left (right) electrode of graphene nanoribbon, the corresponding ZTmax is the highest. However, when the acene molecules contact the middle (middle) part of the left (right) electrode of graphene nanoribbons, the corresponding ZTmax is the lowest. As the temperature increases, ZTmax has a monotonically increasing tendency, regardless of the contact position. With the increase of the length of the acene molecule, the chemical potential corresponding to ZTmax becomes closer to the intrinsic Fermi level. The above findings may provide the valuable reference for the future design of thermoelectric devices based on the acene molecular junctions.
      Corresponding author: Xie Zhong-Xiang, xiezxhu@163.com ; Zhou Wu-Xing, wuxingzhou@hnu.edu.cn
    • Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 12074115, 11874145, 11904161) and the Natural Science Foundation of Hunan Province, China (Grant Nos. 2021JJ30202, 2021JJ30203, 2022JJ30222).
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  • 图 1  并苯连接石墨烯纳米带形成分子结的几何结构示意图. 并苯分子与石墨烯纳米带电极间的接触位置用整数1, 2, 3表示. 为了方便描述, 统一用AN(mn)来表示几何结构, 其中, “N”代表并苯分子长度(也就是苯环的数目), “m, n”分别表示左电极、右电极与中间并苯分子的接触位置. 例如: 本图可以用A5(22)表示

    Figure 1.  Schematic geometric structure of the molecule junction formed by the acene linked with graphene nanoribbons. The contact positions between the acene molecule and graphene nanoribbon electrodes are denoted by the integers 1, 2, and 3. For the sake of description, we uniformly apply “AN(mn)” to represent the geometric structures, where “N” denotes the length of the acene molecule (namely the number of benzene rings), “m, n” denote the contact position between the left, right electrodes and the acene molecule, respectively. For example, this geometric structure is denoted by A5(22).

    图 2  声子热导$ {\sigma }_{{\rm{p}}} $与温度T的关系. 右下角的插图呈现了低温时声子热导$ {\sigma }_{{\rm{p}}} $与温度T关系的细节行为

    Figure 2.  Phononic thermal conductance $ {\sigma }_{{\rm{p}}} $ versus the temperature T. The bottom-right inset shows the detailed behavior of the phononic thermal conductance $ {\sigma }_{{\rm{p}}} $ versus the temperature T at low temperatures.

    图 3  声子输运系数与入射声子能量的关系

    Figure 3.  Phononic transmission coefficient versus the energy of incident phonons.

    图 4  A3(31), A3(22), A3(21)和A3(11)的(a)电导、(b) Seebeck系数、(c)热导和(d)ZT. 实线、划线、双点划线和点划线分别对应着A3(31), A3(22), A3(21)和A3(11). 图(c)中, 四条平整的曲线对应着声子热导

    Figure 4.  (a) Electrical conductance, (b) Seebeck coefficient, (c) thermal conductance, and (d) ZT of A3(31), A3(22), A3(21)和A3(11). The solid, dashed, double-dot-dashed, and dot-dashed curves correspond to A3(31), A3(22), A3(21), and A3(11), respectively. In panel (c), four flat curves correspond to the phononic thermal conductance.

    图 5  电子输运系数和对应的投影局域态密度. (a1)和(a2), (b1)和(b2), (c1)和(c2), (d1)和(d2)分别对应着A3(31), A3(22), A3(21), A3(11)

    Figure 5.  Electronic transmission coefficient and projected local density of states. (a1) and (a2), (b1) and (b2), (c1) and (c2), (d1) and (d2) correspond to A3(31), A3(22), A3(21), A3(11), respectively.

    图 6  $ {ZT}_{{\rm{m}}{\rm{a}}{\rm{x}}} $与温度T的关系

    Figure 6.  $ {ZT}_{{\rm{m}}{\rm{a}}{\rm{x}}} $ versus the temperature T.

    图 7  (a) 电导$ G $和(b) 电子热导$ {\sigma }_{{\rm{e}}} $与化学势$ \mu $的关系. 实线、划线、双点划线、点划线分别对应着并三苯(N = 3)、并五苯(N = 5)、并七苯(N = 7)、并九苯(N = 9). 图(b)中插图表示的是温度为300 K时的声子热导

    Figure 7.  (a) Electrical conductance and (b) electronic thermal conductance versus the versus the chemical potential $ \mu $. The solid, dashed, double-dot-dashed, and dot-dashed curves correspond to anthracene (N = 3), pentacene (N = 5), heptacene (N = 7), and nonacene (N = 9). The inset in (b) denotes the phononic thermal conductance at T = 300 K.

    图 8  (a) Seebeck系数和(b) 热电优值ZT与化学势$ \mu $的关系. 实线、划线、双点划线、点划线分别对应着并三苯(N = 3)、并五苯(N = 5)、并七苯(N = 7)、并九苯(N = 9)

    Figure 8.  (a) Seebeck coefficient and (b) $ {ZT}_{{\rm{m}}{\rm{a}}{\rm{x}}} $versus the versus the chemical potential $ \mu $. The solid, dashed, double-dot-dashed, and dot-dashed curves correspond to anthracene (N = 3), pentacene (N = 5), heptacene (N = 7), and nonacene (N = 9), respectively.

    表 1  最大热电优值ZT($ {ZT}_{{\rm{m}}{\rm{a}}{\rm{x}}} $)对应的热电参数

    Table 1.  Thermoelectric parameters corresponding to the maximum of the thermoelectric figure of merit (ZTmax).

    N接触位置$ {ZT}_{{\rm{m}}{\rm{a}}{\rm{x}}} $G/mSS/(mV·K–1)σp/(nW·K–1)σe/(nW·K–1)σp+σe/(nW·K–1)
    N = 3(31)0.340.012–0.1940.3420.0440.385
    (22)0.090.0370.0650.2640.2460.510
    (21)0.510.0320.1500.2420.1840.425
    (11)0.160.0460.0850.3360.2930.630
    N = 5(31)0.280.015–0.1550.3140.0760.390
    (22)0.100.0300.0710.2320.2170.449
    (21)0.320.0100.1740.2310.0520.283
    (11)0.140.027–0.0920.3110.1710.483
    N = 7(31)0.420.017–0.1780.3050.0800.385
    (22)0.230.0250.1030.2100.1440.350
    (21)0.440.0120.1830.2210.0530.274
    (11)0.400.0170.1760.3040.0860.390
    N = 9(31)0.410.0230.1490.3010.0690.370
    (22)0.350.017–0.1410.2050.0860.291
    (21)0.440.018–0.1550.2170.0760.293
    (11)0.360.0160.1630.2980.0550.353
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    Jia P Z, Xie Z X, Deng Y X, Zhang Y, Tang L M, Zhou W X, Chen K Q 2022 Appl. Phys. Lett. 121 043901Google Scholar

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    Wang T, Zhang C, Snoussi H, Zhang G 2020 Adv. Funct. Mater. 30 1906041Google Scholar

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    宗志成, 潘东楷, 邓世琛, 万骁, 杨哩娜, 马登科, 杨诺 2023 物理学报 72 034401Google Scholar

    Zong Z C, Pan D K, Deng S C, Wan X, Yang L N, Ma D K, Yang N 2023 Acta Phys. Sin. 72 034401Google Scholar

    [21]

    Markussen T, Jauho A P, Brandbyge M 2009 Phys. Rev. Lett. 103 055502Google Scholar

    [22]

    Hochbaum A I, Chen R, Delgado R D, Liang W, Garnett E C, Najarian M, Majumdar A, Yang P 2008 Nature 451 163Google Scholar

    [23]

    Chen I J, Burke A, Svilans A, Linke H, Thelander C 2018 Phys. Rev. Lett. 120 177703Google Scholar

    [24]

    Ohnishi M, Shiga T, and Shiomi J 2017 Phys. Rev. B 95 155405Google Scholar

    [25]

    Zhou G, Li L, Li G H 2010 Appl. Phys. Lett. 97 023112Google Scholar

    [26]

    Dash A, Scheunemann D, Kemerink M 2022 Phys. Rev. Appl. 18 064022Google Scholar

    [27]

    Huang N T, Nugraha A R T, Saito R 2019 Energies 12 4561Google Scholar

    [28]

    Yang N X, Yan Q, Sun Q F 2020 Phys. Rev. B 102 245412Google Scholar

    [29]

    Tang H, Wang X, Xiong Y, Zhao Y, Zhang Y, Zhang Y, Yang J, Xu D 2015 Nanoscale 7 6683Google Scholar

    [30]

    Fan D D, Liu H J, Cheng L, Jiang P H, Shi J, Tang X F 2014 Appl. Phys. Lett. 105 133113Google Scholar

    [31]

    Zberecki K, Wierzbicki M, Barnaś J, Swirkowicz R 2013 Phys. Rev. B 88 115404Google Scholar

    [32]

    Liu W, Yan X, Chen G, Ren Z 2012 Nano Energy 1 42Google Scholar

    [33]

    Tang J, Chen Y, McCuskey S R, Chen L, Bazan G C, Liang Z 2019 Adv. Electron. Mater. 5 1800943Google Scholar

    [34]

    Foster S, Thesberg M, Neophytou N 2017 Phys. Rev. B 96 195425Google Scholar

    [35]

    Huang W, Wang J S, Liang G 2011 Phys. Rev. B 84 045410Google Scholar

    [36]

    Liang L, Cruz-Silva E, Girão E C, Meunier V 2012 Phys. Rev. B 86 115438Google Scholar

    [37]

    Liang L, Meunier V 2013 Appl. Phys. Lett. 102 143101Google Scholar

    [38]

    Sevinçli H, Cuniberti G 2010 Phys. Rev. B 81 113401Google Scholar

    [39]

    Mazzamuto F, Nguyen V H, Apertet Y, Caër C, Chassat C, Martin J S, Dollfus P 2011 Phys. Rev. B 83 235426Google Scholar

    [40]

    Karamitaheri H, Neophytou N, Pourfath M, Faez R, Kosina H 2012 J. Appl. Phys. 111 054501Google Scholar

    [41]

    Anno Y, Imakita Y, Takei K, Akita S, Arie T 2017 2D Materials 4 025019Google Scholar

    [42]

    Xiao H, Cao W, Ouyang T, Xu X, Ding Y C, Zhong J X 2018 Appl. Phys. Lett. 112 233107Google Scholar

    [43]

    Dollfus P, Nguyen V H, Saint-Martin J 2015 J. Phys. Condens. Matter 27 133204Google Scholar

    [44]

    Xu Y, Li Z, Duan W 2014 Small 10 2182Google Scholar

    [45]

    Li D, Gong Y, Chen Y, Lin J, Khan Q, Zhang Y, Li Y, Zhang H, Xie H 2020 Nano-Micro Lett. 12 36Google Scholar

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    Hippalgaonkar K, Wang Y, Ye Y, Qiu D Y, Zhu H, Wang Y, Moore J, Louie S G, Zhang X 2017 Phys. Rev. B 95 115407Google Scholar

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    Zhu X L, Hou C H, Zhang P, Liu P F, Xie G F, Wang B T 2020 J. Phys. Chem. C 124 1812Google Scholar

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    Zhang G, Zhang Y W 2017 J. Mater. Chem. C 5 7684Google Scholar

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    Zhang G, Zhang Y W 2015 Mech. Mater. 91 382Google Scholar

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    Zeng Y J, Wu D, Cao X H, Zhou W X, Tang L M, Chen K Q 2020 Adv. Funct. Mater. 30 1903873Google Scholar

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Metrics
  • Abstract views:  3107
  • PDF Downloads:  78
  • Cited By: 0
Publishing process
  • Received Date:  09 March 2023
  • Accepted Date:  03 April 2023
  • Available Online:  15 April 2023
  • Published Online:  20 June 2023

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