Effect of edge on nonlinear optical property of graphene quantum dots

Li Hai-Peng; Zhou Jia-Sheng; Ji Wei; Yang Zi-Qiang; Ding Hui-Min; Zhang Zi-Tao; Shen Xiao-Peng; Han Kui

doi:10.7498/aps.70.20201643

Abstract

Graphene is a two-dimensional material with single-layer honeycomb lattice structure formed by sp² hybrid connection of carbon atoms. Graphene has excellent optical, electrical, thermal and mechanical properties, and it is considered to be an ideal material for future flexible optoelectronic devices. In recent years, the nonlinear optical properties and regulation of graphene nanostructures have attracted experimental and theoretical interest. Graphene has good delocalization of π-electrons and its unique plane structure, showing good nonlinear optical properties. Graphene quantum dots can be regarded as small graphene nanoflakes. Their unique electronic structure is closely related to the non-bond orbitals on the boundary/edge. Therefore, it is very important to study the boundary/edge effect on the electronic and optical properties of nanographene. In this paper, effects of the number of edge C=C double bonds and Borazine (B₃N₃) doping on the nonlinear optical properties and UV-Vis absorption spectrum of graphene quantum dots are studied by the quantum chemical calculation methods, respectively. It is found that the symmetry of hexagonal graphene quantum dots decreases and the symmetry of charge distribution is broken when C=C double bond is introduced into the armchair edge, which leads the second-order nonlinear optical activity to be enhanced. During the transition from armchair to zigzag edge, the polarizability and the second hyperpolarizability of hexagonal graphene quantum dots and B₃N₃-doped graphene quantum dots increase linearly with the number of introduced C=C double bonds incrrasing. In addition, the edge also has an important influence on the absorption spectrum of graphene quantum dots. For graphene quantum dots and B₃N₃-doped graphene quantum dots, the introduction of C=C double bond at the armchair edge increases the highest occupied molecular orbital energy level and also reduces the lowest unoccupied molecular orbital energy level, which reduces the energy gap between the frontier molecular orbitals, and thus resulting in the red-shift of the maximum absorption wavelength. The doping of B₃N₃ ring will increase the energy gap between molecular frontier orbitals of graphene quantum dots, leading the UV-Vis absorption spectrum of graphene quantum dots to be blue-shifted. This study provides theoretical guidance for controlling the nonlinear optical response of graphene quantum dots by edge modification.

Keywords:

Authors and contacts

School of Materials Science and Physics, China University of Mining and Technology, Xuzhou 221116, China

Corresponding author: Li Hai-Peng, haipli@cumt.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 11504418) and the Fundamental Research Funds for the Central Universities of China (Grant No. 2019ZDPY16)

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References

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图 1 石墨烯量子点和B₃N₃掺杂石墨烯量子点的结构

Figure 1. Structures of graphene quantum dots and B₃N₃-doped graphene quantum dots.

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图 2 GQD-n和B₃N₃-GQD-n的极化率α

Figure 2. The polarizabilities α of GQD-n and B₃N₃ -GQD-n.

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图 3 GQD-n和B₃N₃-GQD-n的第二超极化率γ

Figure 3. The second hyperpolarizabilities γ of GQD-n and B₃N₃-GQD-n.

DownLoad: Full-Size Img PowerPoint

图 4 GQD-0, GQD-6, B₃N₃-GQD-0和B₃N₃-GQD-6的紫外-可见吸收光谱

Figure 4. Ultraviolet-visible absorption spectra of GQD-0, GQD-6, B₃N₃-GQD-0 and B₃N₃-GQD-6.

DownLoad: Full-Size Img PowerPoint

表 1 GQD-n和B₃N₃-GQD-n的极化率α、第一超极化率β和第二超极化率γ计算值

Table 1. Calculated polarizability α, first hyperpolarizability β, second hyperpolarizability γ of GQD-n and B₃N₃-GQD-n.

分子	α/(10^–39 C²·m²·J^–1)	β/(10^–51 C³·m³·J^–2)	γ/(10^–59 C⁴·m⁴·J^–3)
GQD-0	8.856	0	1.807
GQD-1	9.455	4.167	2.069
GQD-2	10.070	4.630	2.312
GQD-3	10.666	7.037	2.521
GQD-4	11.298	8.505	2.875
GQD-5	11.928	2.332	3.185
GQD-6	12.549	0	3.380
B₃N₃-GQD-0	8.206	0	1.381
B₃N₃-GQD-1	8.803	3.871	1.735
B₃N₃-GQD-2	9.413	0.330	2.011
B₃N₃-GQD-3	10.019	10.875	2.310
B₃N₃-GQD-4	10.629	6.387	2.689
B₃N₃-GQD-5	11.259	9.293	3.157
B₃N₃-GQD-6	11.883	0	3.446

DownLoad: CSV

表 2 GQD-n和B₃N₃-GQD-n的HOMO能级、LUMO能级、HOMO-LUMO能级差(HLG)和最大吸收波长λ_max计算值

Table 2. Calculated HOMO energy level, LUMO energy level, HOMO-LUMO energy gap (HLG) and maximum absorption wavelength λ_max of GQD-n and B₃N₃-GQD-n.

分子	HOMO/eV	LUMO/eV	HLG/eV	λ_max/nm
GQD-0	–6.606	–0.995	5.611	308.6
GQD-1	–6.324	–1.287	5.037	316.7
GQD-2	–6.203	–1.419	4.784	334.1
GQD-3	–6.266	–1.387	4.878	353.3
GQD-4	–6.078	–1.584	4.493	355.1
GQD-5	–6.038	–1.627	4.411	354.8
GQD-6	–6.126	–1.554	4.572	365.3
B₃N₃-GQD-0	–6.982	–0.778	6.204	254.6
B₃N₃-GQD-1	–6.594	–0.987	5.607	253.4
B₃N₃-GQD-2	–6.593	–1.227	5.366	256.9
B₃N₃-GQD-3	–6.403	–1.207	5.196	252.2
B₃N₃-GQD-4	–6.443	–1.398	5.044	263.6
B₃N₃-GQD-5	–6.273	–1.370	4.903	268.4
B₃N₃-GQD-6	–6.348	–1.307	5.041	320.6

DownLoad: CSV

map

[1]	Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, Dubonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666 Google Scholar
[2]	Li H, Yu X, Shen X, Tang G, Han K 2019 J. Phys. Chem. C 123 20020 Google Scholar
[3]	吴晨晨, 郭相东, 胡海, 杨晓霞, 戴庆 2019 68 148103 Google Scholar Wu C C, Guo X D, Hu H, Yang X X, Dai Q 2019 Acta Phys. Sin. 68 148103 Google Scholar
[4]	白家豪, 郭建刚 2020 69 056201 Google Scholar Bai J H, Guo J G 2020 Acta Phys. Sin. 69 056201 Google Scholar
[5]	Guo Z, Zhang D, Gong X G 2009 Appl. Phys. Lett. 95 163103 Google Scholar
[6]	蔡乐, 王华平, 于贵 2016 物理学进展 36 21 Google Scholar Cai L, Wang H P, Yu G 2016 Prog. Phys. 36 21 Google Scholar
[7]	徐小志, 余佳晨, 张智宏, 刘开辉 2017 科学通报 62 2220 Google Scholar Xu X Z, Yu J C, Zhang Z H, Liu K H 2017 Chinese Sci. Bull. 62 2220 Google Scholar
[8]	张华林, 孙琳, 王鼎 2016 65 016101 Google Scholar Zhang H L, Sun L, Wang D 2016 Acta Phys. Sin. 65 016101 Google Scholar
[9]	Mei F, Zhang D W, Zhu S L 2013 Chin. Phys. B 22 116106 Google Scholar
[10]	Ouyang F P, Chen L, Jin X, Zhang H 2011 Chin. Phys. Lett. 28 047304 Google Scholar
[11]	Otero N, El-kelany K E, Pouchan C, Rérata M, Karamanis P 2016 Phys.Chem.Chem.Phys. 18 25315 Google Scholar
[12]	Zhang M, Li G, Li L 2014 J. Mater. Chem. C 2 1482 Google Scholar
[13]	Krieg M, Reicherter F, Haiss P, Ströbele M, Eichele K, Treanor M J, Schaub R, Bettinger H F 2015 Angew. Chem. Int. Ed. 54 8284 Google Scholar
[14]	You J W, Bongu S R, Bao Q, Panoiu N C 2018 Nanophotonics 8 63 Google Scholar
[15]	Bonifazi D, Fasano F, Marinelli D 2015 Chem. Comm. 51 15222 Google Scholar
[16]	Dosso J, Marinelli D, Demitri N, Bonifazi D 2019 ACS Omega 4 9343 Google Scholar
[17]	Kan M, Li Y, Sun Q 2016 WIREs Comput. Mol. Sci. 6 65 Google Scholar
[18]	Xia F, Mueller T, Lin Y M, Valdes-Garcia A, Avouris P 2009 Nat. Nanotechn. 4 839 Google Scholar
[19]	Hwang M S, Kim H R, Kim K H, Jeong K Y, Park J S, Choi J H, Kang J H, Lee J M, Park W, Song J H, Seo M K, Par H G 2017 Nano Lett. 17 1892 Google Scholar
[20]	Sun Z P, Hasan T, Torrisi F 2010 ACS Nano 4 803 Google Scholar
[21]	Li H P, Bi Z T, Xu R F, Han K, Li M X, Shen X P, Wu Y X 2017 Carbon 122 756 Google Scholar
[22]	Hong S Y, Dadap J I, Petrone N, Yeh P C, Hone J, Osgood R M 2013 Phys. Rev. X 3 021014 Google Scholar
[23]	Xia F, Wang H, Xiao D, Dubey M, Ramasubramaniam A 2014 Nat. Photonics 8 899 Google Scholar
[24]	Karamanis P, Otero N, Pouchan C 2014 J. Am. Chem. Soc. 136 7464 Google Scholar
[25]	Jiang T, Huang D, Cheng J L, Fan X D, Zhang Z H, Shan Y W, Yi Y F, Dai Y Y, Shi L, Liu K H, Zeng C G, Zi J, Sipe J E, Shen Y R, Liu W T, Wu S W 2018 Nat. Photonics 12 430 Google Scholar
[26]	Liaros N, Bourlinos A B, Zboril R, Couris S 2013 Opt. Exp. 21 21027 Google Scholar
[27]	Bendikov M, Duong H M, Starkey K, Houk K N, Carter E A, Wudl F 2004 J. Am. Chem. Soc. 126 7416 Google Scholar
[28]	Hachmann J, Dorando J J, Aviles M, Chan K L 2007 J. Chem. Phys. 127 134309 Google Scholar
[29]	Zhang B X, Gao H, Li X L 2014 New J. Chem. 38 4615 Google Scholar
[30]	Zheng X Q, Feng M, Li Z G, Song Y L, Zhang H B 2014 J. Mater. Chem. C 2 4121 Google Scholar
[31]	Hu Y Y, Li W Q, Li Y, Feng J K, Tian W Q 2016 Can. J. Chem. 94 620 Google Scholar
[32]	Otero N, Karamanis P, El-Kelany K E, Rérat M, Maschio L, Civalleri B, Kirtman B 2017 J. Phys. Chem. C 121 709 Google Scholar
[33]	Otero N, Pouchan C, Karamanis P 2017 J. Mater. Chem. C 5 8273 Google Scholar
[34]	Karamanis P, Otero N, Pouchan C 2015 J. Phys. Chem. C 119 11872 Google Scholar
[35]	Li H, Zhang Y, Bi Z, Xu R, Li M, Shen X, Tang G, Han K 2017 Mol. Phys. 115 3164 Google Scholar
[36]	李海鹏, 韩奎, 逯振平, 沈晓鹏, 黄志敏, 张文涛, 白磊 2006 55 1827 Google Scholar Li H P, Han K, Lu Z P, Shen X P, Huang Z M, Zhang W T, Bai L 2006 Acta Phys. Sin. 55 1827 Google Scholar
[37]	梁飞, 林哲帅, 吴以成 2018 67 114203 Google Scholar Liang F, Lin Z S, Wu Y C 2018 Acta Phys. Sin. 67 114203 Google Scholar
[38]	马勇, 邹斌, 李宗良, 王传奎, 罗毅 2006 55 1974 Google Scholar Ma Y, Zou B, Li Z L, Wang C K, Luo Y 2006 Acta Phys. Sin. 55 1974 Google Scholar
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[41]	Zhang Y P, Ma J M, Yang Y S, Ru J X, Liu X Y, Ma Y, Guo H C 2019 Spectrochim. Acta A 217 60 Google Scholar

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