Citation: LIU Nanshu, ZHOU Si, ZHAO Jijun. Electrical Conductance of Graphene with Point Defects[J]. Acta Physico-Chimica Sinica, ;2019, 35(10): 1142-1149. doi: 10.3866/PKU.WHXB201810040 shu

Electrical Conductance of Graphene with Point Defects

Key Laboratory of Materials Modification by Laser, Ion and Electron Beams, Ministry of Education, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China

Corresponding author: ZHOU Si, sizhou@dlut.edu.cn
Received Date: 18 October 2018
Revised Date: 4 December 2018
Accepted Date: 3 February 2019
Available Online: 21 October 2019
Fund Project: Fundamental Research Funds for the Central Universities of China DUT16LAB01Fundamental Research Funds for the Central Universities of China DUT17LAB19The project was supported by the National Natural Science Foundation of China 11504041The project was supported by the National Natural Science Foundation of China (11504041), the Fundamental Research Funds for the Central Universities of China (DUT16LAB01, DUT17LAB19), and the Supercomputing Center of Dalian University of Technology, China

Graphene is one of the most promising materials in nanotechnology and has attracted worldwide attention and research interest owing to its high electrical conductivity, good thermal stability, and excellent mechanical strength. Perfect graphene samples exhibit outstanding electrical and mechanical properties. However, point defects are commonly observed during fabrication which deteriorate the performance of graphene based-devices. The transport properties of graphene with point defects essentially depend on the imperfection of the hexagonal carbon atom network and the scattering of carriers by localized states. Furthermore, an in-depth understanding of the effect of specific point defects on the electronic and transport properties of graphene is crucial for specific applications. In this work, we employed density functional theory calculations and the non-equilibrium Green's function method to systematically elucidate the effects of various point defects on the electrical transport properties of graphene, including Stone-Waals and inverse Stone-Waals defects; and single and double vacancies. The electrical conductance highly depends on the type and concentration of point defects in graphene. Low concentrations of Stone-Waals, inverse Stone-Waals, and single-vacancy defects do not noticeably degrade electron transport. In comparison, DV585 induces a moderate reduction of 25%–34%, and DV55577 and DV5555-6-7777 induce significant suppression of 51%–62% in graphene. As the defect concentration increases, the electrical conductance reduces by a factor of 2–3 compared to the case of graphene monolayers with a low concentration of point defects. These distinct electrical transport behaviors are attributed to the variation of the graphene band structure; the point defects induce localized states near the Fermi level and result in energy splitting at the Dirac point due to the breaking of the intrinsic symmetry of the graphene honeycomb lattice. Double vacancies with larger defect concentrations exhibit more flat bands near the Fermi energy and more localized states in the defective region, resulting in the presence of resonant peaks close to the Fermi energy in the local density of states. This may cause resonant scattering of the carriers and a corresponding reduction of the conductance of graphene. Moreover, the partial charge densities for double vacancies and point defects with larger concentrations exhibit enhanced localization in the defective region that hinder the charge carriers. The electrical conductance shows an exponential decay as the defect concentration and energy splitting increase. These theoretical results provide important insights into the electrical transport properties of realistic graphene monolayers and will assist in the fabrication of high-performance graphene-based devices.
- Graphene,
- Point defect,
- Electron transport,
- Electrical conductance,
- Energy splitting
1. [1]
  Novoselov, K. S.; Geim, A. K.; Morozov, S. V.; Jiang, D.; Zhang, Y.; Dubonos, S. V.; Grigorieva, I. V.; Firsov, A. A. Science 2004, 306, 666. doi: 10.1126/science.1102896 doi: 10.1126/science.1102896
2. [2]
  Geim, A. K.; Novoselov, K. S. Nat. Mater. 2007, 6, 183. doi: 10.1038/nmat1849 doi: 10.1038/nmat1849
3. [3]
  Yi, M.; Shen, Z. J. Mater. Chem. A 2015, 3, 11700. doi: 10.1039/C5TA00252D doi: 10.1039/C5TA00252D
4. [4]
  Muñoz, B. R.; Gómez-aleixandre, C. Chem. Vap. Depos. 2013, 19, 297. doi: 10.1002/cvde.201300051 doi: 10.1002/cvde.201300051
5. [5]
  Zhang, Y.; Zhang, L.; Zhou, C. Acc. Chem. Res. 2013, 46, 2329. doi: 10.1021/ar300203n doi: 10.1021/ar300203n
6. [6]
  Park, B. J.; Mitchel, W. C.; Grazulis, L.; Smith, H. E.; Eyink, K. G.; Boeckl, J. J.; Tomich, D. H.; Pacley, S. D.; Hoelscher, J. E. Adv. Mater. 2010, 45433, 4140. doi:10.1002/adma.201000756 doi: 10.1002/adma.201000756a
7. [7]
  Ugeda, M. M.; Torre, F.; Brihuega, I.; Pou, P.; Martinez-Galera, A. J.; Perez, R.; Gomez-Rodriguez, J. M. Phys. Rev. Lett. 2011, 107, 116803. doi: 10.1103/PhysRevLett.107.116803 doi: 10.1103/PhysRevLett.107.116803
8. [8]
  Banhart, F.; Kotakoski, J.; Krasheninnikov. A. V. ACS Nano 2011, 5, 26. doi: 10.1021/nn102598m doi: 10.1021/nn102598m
9. [9]
  Kotakoski, J.; Mangler, C.; Meyer. J. C. Nat. Commun. 2014, 5, 536. doi: 10.1038/ncomms4991 doi: 10.1038/ncomms4991
10. [10]
  Robertson, A. W.; Allen, C. S.; Wu, Y. A.; He, K.; Olivier, J.; Neethling, J.; Kirkland, A. I.; Warner, J. H. Nat. Commun. 2012, 3, 1144. doi:10.1038/ncomms2141 doi: 10.1038/ncomms2141
11. [11]
  Ugeda, M. M.; Brihuega, I. Phys. Rev. Lett. 2010, 104, 96804. doi: 10.1103/PhysRevLett.104.096804 doi: 10.1103/PhysRevLett.104.096804
12. [12]
  Stone, A. J.; Wales, D. J. Chem. Phys. Lett. 1986, 128, 501. doi: 10.1016/0009-2614(86)80661-3 doi: 10.1016/0009-2614[86]80661-3
13. [13]
  Chen, J. H.; Li, L.; Cullen, W. G.; Williams, E. D.; Fuhrer, M. S. Nat. Phys. 2011, 7, 535. doi: 10.1038/nphys1962 doi: 10.1038/nphys1962
14. [14]
  Barreiro, A.; Lazzeri, M.; Moser, J.; Mauri, F.; Bachtold, A. Phys. Rev. Lett. 2009, 103, 076601. doi: 10.1103/PhysRevLett.103.076601 doi: 10.1103/PhysRevLett.103.076601
15. [15]
  Meyer, J. C.; Kisielowski, C.; Erni, R.; Rossell, M. D.; Crommie, M. F.; Zettl, A. Nano Lett. 2008, 12, 3582. doi: 10.1021/nl801386m doi: 10.1021/nl801386m
16. [16]
  Kotakoski, J.; Krasheninnikov, A. V.; Kaiser, U.; Meyer, J. C. Phys. Rev. Lett. 2011, 106, 105505. doi: 10.1103/PhysRevLett.106.105505 doi: 10.1103/PhysRevLett.106.105505
17. [17]
  Lahiri, J.; Lin, Y.; Bozkurt, P.; Oleynik, I. I.; Batzill, M. Nat. Nanotechnol. 2010, 5, 326. doi: 10.1038/nnano.2010.53 doi: 10.1038/nnano.2010.53
18. [18]
  Blanc, N.; Jean, F.; Krasheninnikov, A. V; Renaud, G.; Coraux, J. Phys. Rev. Lett. 2013, 111, 085501. doi: 10.1103/PhysRevLett.111.085501 doi: 10.1103/PhysRevLett.111.085501
19. [19]
  Robertson, A. W.; Montanari, B.; He, K.; Allen, C. S.; Wu, Y. A.; Harrison, N. M.; Kirkland, A. I.; Warner, J. H. ACS Nano 2013, 7, 4495. doi: 10.1021/nn401113r doi: 10.1021/nn401113r
20. [20]
  Tan, Y. W.; Zhang, Y.; Bolotin, K.; Zhao, Y.; Adam, S.; Hwang, E. H.; Sarma, S. D.; Stormer, H. L.; Kim, P. Phys. Rev. Lett. 2007, 99, 246803. doi: 10.1103/PhysRevLett.99.246803 doi: 10.1103/PhysRevLett.99.246803
21. [21]
  Moktadir, Z.; Hang, S.; Mizuta, H. Carbon 2015, 93, 325. doi: 10.1016/j.carbon.2015.05.049 doi: 10.1016/j.carbon.2015.05.049
22. [22]
  Chen, J. H.; Cullen, W. G.; Jang, C.; Fuhrer, M. S.; Williams, E. D. Phys. Rev. Lett. 2009, 102, 236805. doi: 10.1103/PhysRevLett.102.236805 doi: 10.1103/PhysRevLett.102.236805
23. [23]
  Cretu, O.; Krasheninnikov, A. V.; Rodríguez-Manzo, J. A.; Sun, L.; Nieminen, R. M.; Banhart, F. Phys. Rev. Lett. 2010, 105, 196102. doi: 10.1103/PhysRevLett.105.196102 doi: 10.1103/PhysRevLett.105.196102
24. [24]
  Hou, Z.; Wang, X.; Ikeda, T.; Terakura, K.; Oshima, M.; Kakimoto, M. Phys. Rev. B 2013, 87, 165401. doi: 10.1103/PhysRevB.87.165401 doi: 10.1103/PhysRevB.87.165401
25. [25]
  Zaminpayma, E.; Razavi, M. E.; Nayebi, P. Appl. Surf. Sci. 2017, 414, 101. doi: 10.1016/j.apsusc.2017.04.065 doi: 10.1016/j.apsusc.2017.04.065
26. [26]
  Pereira, V. M.; Guinea, F.; Lopes Dos Santos, J. M. B.; Peres, N. M. R.; Castro Neto, A. H. Phys. Rev. Lett. 2006, 96, 036801. doi: 10.1103/PhysRevLett.96.036801 doi: 10.1103/PhysRevLett.96.036801
27. [27]
  Nanda, B. R. K.; Sherafati, M.; Popović, Z. S.; Satpathy, S. New J. Phys. 2012, 14, 400. doi:10.1088/1367-2630/15/3/039501 doi: 10.1088/1367-2630/15/3/039501
28. [28]
  Lherbier, A.; Dubois, S. M. M.; Declerck, X.; Roche, S.; Niquet, Y. M.; Charlier, J. C. Phys. Rev. Lett. 2011, 106, 046803. doi: 10.1103/PhysRevLett.106.046803 doi: 10.1103/PhysRevLett.106.046803
29. [29]
  Skrypnyk, Y. V.; Loktev, V. M. Phys. Rev. B 2010, 82, 085436. doi: 10.1103/PhysRevB.82.085436 doi: 10.1103/PhysRevB.82.085436
30. [30]
  Kolasiński, K.; Mreńca-Kolasińska, A.; Szafran, B. Phys. Rev. B 2016, 94, 115406. doi: 10.1103/PhysRevB.94.115406 doi: 10.1103/PhysRevB.94.115406
31. [31]
  Gorjizadeh, N.; Farajian, A. A; Kawazoe, Y. Nanotechnology 2009, 20, 015201. doi: 10.1088/0957-4484/20/1/015201 doi: 10.1088/0957-4484/20/1/015201
32. [32]
  Deretzis, I.; Fiori, G.; Iannaccone, G.; Piccitto, G.; Magna, A. L. Phys. E 2012, 44, 981. doi: 10.1016/j.physe.2010.06.024 doi: 10.1016/j.physe.2010.06.024
33. [33]
  Taluja, Y.; SanthiBhushan, B.; Yadav, S.; Srivastava, A. Superlattices Microstruct. 2016, 98, 306. doi: 10.1016/j.spmi.2016.08.044 doi: 10.1016/j.spmi.2016.08.044
34. [34]
  Chowdhury, S.; Jana, D.; Mookerjee, A. Phys. E 2015, 74, 347. doi: 10.1016/j.physe.2015.07.019 doi: 10.1016/j.physe.2015.07.019
35. [35]
  Jamaati, M.; Namiranian, A. Comput. Mater. Sci. 2015, 101, 156. doi: 10.1016/j.commatsci.2015.01.037 doi: 10.1016/j.commatsci.2015.01.037
36. [36]
  Do, V. N.; Dollfus, P. J. Appl. Phys. 2009, 106, 023719. doi: 10.1063/1.3176956 doi: 10.1063/1.3176956
37. [37]
  Peng, X. Y.; Ahuja, R. Nano Lett. 2008, 8, 4464. doi: 10.1021/nl802409q doi: 10.1021/nl802409q
38. [38]
  Appelhans, D. J.; Carr, L. D.; Lusk, M. T. New J. Phys. 2010, 12, 135. doi: 10.1088/1367-2630/12/12/125006 doi: 10.1088/1367-2630/12/12/125006
39. [39]
  Datta, S. Superlattices Microstruct. 2000, 28, 253. doi: 10.1006/spmi.2000.0920 doi: 10.1006/spmi.2000.0920
40. [40]
  Brandbyge, M.; Mozos, J. L.; Ordejón, P.; Taylor, J.; Stokbro, K. Phys. Rev. B -Condens. Matter Mater. Phys. 2002, 65, 165401. doi: 10.1103/PhysRevB.65.165401 doi: 10.1103/PhysRevB.65.165401
41. [41]
  Taylor, J.; Guo, H.; Wang, J. Phys. Rev. B 2001, 63, 245407. doi: 10.1103/PhysRevB.63.245407 doi: 10.1103/PhysRevB.63.245407
42. [42]
  Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77, 3865. doi: 10.1103/PhysRevLett.77.3865 doi: 10.1103/PhysRevLett.77.3865
43. [43]
  Datta, S. Electronic Transport in Mesoscopic Systems; Cambridge University Press: Cambridge, UK, 1995; pp. 88-89.
44. [44]
  Li, T. C.; Lu, S. Phys. Rev. B 2008, 77, 085408. doi: 10.1103/PhysRevB.77.085408. doi: 10.1103/PhysRevB.77.085408
45. [45]
  Carlsson, J. M.; Scheffler, M. Phys. Rev. Lett. 2006, 96, 046806. doi: 10.1103/PhysRevLett.96.046806 doi: 10.1103/PhysRevLett.96.046806
46. [46]
  Kang, J.; Bang, J.; Ryu, B.; Chang, K. J. Phys. Rev. B 2008, 77, 115453. doi: 10.1103/PhysRevB.77.115453 doi: 10.1103/PhysRevB.77.115453
1. [1]
  Cheng Guo , Xiaoxiao Zhang , Xiujuan Hong , Yiqiu Hu , Lingna Mao , Kezhi Jiang . Graphene as adsorbent for highly efficient extraction of modified nucleosides in urine prior to liquid chromatography-tandem mass spectrometry analysis. Chinese Chemical Letters, 2024, 35(4): 108867-. doi: 10.1016/j.cclet.2023.108867
2. [2]
  Sanmei Wang , Yong Zhou , Hengxin Fang , Chunyang Nie , Chang Q Sun , Biao Wang . Constant-potential simulation of electrocatalytic N₂ reduction over atomic metal-N-graphene catalysts. Chinese Chemical Letters, 2025, 36(3): 110476-. doi: 10.1016/j.cclet.2024.110476
3. [3]
  Sanmei Wang , Dengxin Yan , Wenhua Zhang , Liangbing Wang . Graphene-supported isolated platinum atoms and platinum dimers for CO₂ hydrogenation: Catalytic activity and selectivity variations. Chinese Chemical Letters, 2025, 36(4): 110611-. doi: 10.1016/j.cclet.2024.110611
4. [4]
  Wenjing Xiong , Yulin Xu , Fangzhou Zhao , Baokai Xia , Hongqiang Wang , Wei Liu , Sheng Chen , Yongzhi Zhang . Graphene architecture interpenetrated with mesoporous carbon nanosheets promotes fast and stable potassium storage. Chinese Chemical Letters, 2025, 36(4): 109738-. doi: 10.1016/j.cclet.2024.109738
5. [5]
  Caili Yang , Tao Long , Ruotong Li , Chunyang Wu , Yuan-Li Ding . Pseudocapacitance dominated Li₃VO₄ encapsulated in N-doped graphene via 2D nanospace confined synthesis for superior lithium ion capacitors. Chinese Chemical Letters, 2025, 36(2): 109675-. doi: 10.1016/j.cclet.2024.109675
6. [6]
  Chaozheng He , Pei Shi , Donglin Pang , Zhanying Zhang , Long Lin , Yingchun Ding . First-principles study of the relationship between the formation of single atom catalysts and lattice thermal conductivity. Chinese Chemical Letters, 2024, 35(6): 109116-. doi: 10.1016/j.cclet.2023.109116
7. [7]
  Zuyou Song , Yong Jiang , Qiao Gou , Yini Mao , Yimin Jiang , Wei Shen , Ming Li , Rongxing He . Promoting the generation of active sites through "Co-O-Ru" electron transport bridges for efficient water splitting. Chinese Chemical Letters, 2025, 36(4): 109793-. doi: 10.1016/j.cclet.2024.109793
8. [8]
  Limin Wang , Feiyi Huang , Xinyi Liang , Rajkumar Devasenathipathy , Xiaotian Liu , Qiulan Huang , Zhongyun Yang , Dujuan Huang , Xinglan Peng , Du-Hong Chen , Youjun Fan , Wei Chen . Photoelectric synergy induced synchronous functionalization of graphene and its applications in water splitting and desalination. Chinese Journal of Structural Chemistry, 2025, 44(2): 100501-100501. doi: 10.1016/j.cjsc.2024.100501
9. [9]
  Zhaorui Song , Qiulian Hao , Bing Li , Yuwei Yuan , Shanshan Zhang , Yongkuan Suo , Hai-Hao Han , Zhen Cheng . NIR-Ⅱ fluorescence lateral flow immunosensor based on efficient energy transfer probe for point-of-care testing of tumor biomarkers. Chinese Chemical Letters, 2025, 36(1): 109834-. doi: 10.1016/j.cclet.2024.109834
10. [10]
  Jieqiong Qin , Zhi Yang , Jiaxin Ma , Liangzhu Zhang , Feifei Xing , Hongtao Zhang , Shuxia Tian , Shuanghao Zheng , Zhong-Shuai Wu . Interfacial assembly of 2D polydopamine/graphene heterostructures with well-defined mesopore and tunable thickness for high-energy planar micro-supercapacitors. Chinese Chemical Letters, 2024, 35(7): 108845-. doi: 10.1016/j.cclet.2023.108845
11. [11]
  Shaonan Liu , Shuixing Dai , Minghua Huang . The impact of ester groups on 1,8-naphthalimide electron transport material in organic solar cells. Chinese Journal of Structural Chemistry, 2024, 43(6): 100277-100277. doi: 10.1016/j.cjsc.2024.100277
12. [12]
  Jiangqi Ning , Junhan Huang , Yuhang Liu , Yanlei Chen , Qing Niu , Qingqing Lin , Yajun He , Zheyuan Liu , Yan Yu , Liuyi Li . Alkyl-linked TiO2@COF heterostructure facilitating photocatalytic CO2 reduction by targeted electron transport. Chinese Journal of Structural Chemistry, 2024, 43(12): 100453-100453. doi: 10.1016/j.cjsc.2024.100453
13. [13]
  Haowen Shang , Yujie Yang , Bingjie Xue , Yikai Wang , Zhiyi Su , Wenlong Liu , Youzhi Wu , Xinjun Xu . Efficient solution-processed near-infrared organic light-emitting diodes with a binary-mixed electron transport layer. Chinese Chemical Letters, 2025, 36(4): 110511-. doi: 10.1016/j.cclet.2024.110511
14. [14]
  Fei Jin , Bolin Yang , Xuanpu Wang , Teng Li , Noritatsu Tsubaki , Zhiliang Jin . Facilitating efficient photocatalytic hydrogen evolution via enhanced carrier migration at MOF-on-MOF S-scheme heterojunction interfaces through a graphdiyne (CnH2n-2) electron transport layer. Chinese Journal of Structural Chemistry, 2023, 42(12): 100198-100198. doi: 10.1016/j.cjsc.2023.100198
15. [15]
  Tian Cao , Xuyin Ding , Qiwen Peng , Min Zhang , Guoyue Shi . Intelligent laser-induced graphene sensor for multiplex probing catechol isomers. Chinese Chemical Letters, 2024, 35(7): 109238-. doi: 10.1016/j.cclet.2023.109238
16. [16]
  Rui Liu , Jinbo Pang , Weijia Zhou . Monolayer water shepherding supertight MXene/graphene composite films. Chinese Journal of Structural Chemistry, 2024, 43(10): 100329-100329. doi: 10.1016/j.cjsc.2024.100329
17. [17]
  Hanqing Zhang , Xiaoxia Wang , Chen Chen , Xianfeng Yang , Chungli Dong , Yucheng Huang , Xiaoliang Zhao , Dongjiang Yang . Selective CO2-to-formic acid electrochemical conversion by modulating electronic environment of copper phthalocyanine with defective graphene. Chinese Journal of Structural Chemistry, 2023, 42(10): 100089-100089. doi: 10.1016/j.cjsc.2023.100089
18. [18]
  Ying Chen , Li Li , Junyao Zhang , Tongrui Sun , Xuan Zhang , Shiqi Zhang , Jia Huang , Yidong Zou . Tailored ionically conductive graphene oxide-encased metal ions for ultrasensitive cadaverine sensor. Chinese Chemical Letters, 2024, 35(8): 109102-. doi: 10.1016/j.cclet.2023.109102
19. [19]
  Jia-Li Xie , Tian-Jin Xie , Yu-Jie Luo , Kai Mao , Cheng-Zhi Huang , Yuan-Fang Li , Shu-Jun Zhen . Octopus-like DNA nanostructure coupled with graphene oxide enhanced fluorescence anisotropy for hepatitis B virus DNA detection. Chinese Chemical Letters, 2024, 35(6): 109137-. doi: 10.1016/j.cclet.2023.109137
20. [20]
  Qiang Cao , Xue-Feng Cheng , Jia Wang , Chang Zhou , Liu-Jun Yang , Guan Wang , Dong-Yun Chen , Jing-Hui He , Jian-Mei Lu . Graphene from microwave-initiated upcycling of waste polyethylene for electrocatalytic reduction of chloramphenicol. Chinese Chemical Letters, 2024, 35(4): 108759-. doi: 10.1016/j.cclet.2023.108759

Get Citation

PDF

XML

Metrics

PDF Downloads(16)
Abstract views(697)
HTML views(111)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142