TY - JOUR
T1 - First-principles study of the impact of chemical doping and functional groups on the absorption spectra of graphene
AU - Panneerselvam, Iyyappa Rajan
AU - Chakraborty, Pranay
AU - Nian, Qiong
AU - Lu, Yongfeng
AU - Liao, Yiliang
AU - Wang, Yan
N1 - Publisher Copyright:
© 2021 IOP Publishing Ltd.
PY - 2022/2
Y1 - 2022/2
N2 - The rational design of the electronic band structures and the associated properties (e.g. optical) of advanced materials has remained challenging for crucial applications in optoelectronics, solar desalination, advanced manufacturing technologies, etc. In this work, using first-principles calculations, we studied the prospects of tuning the absorption spectra of graphene via defect engineering, i.e. chemical doping and oxidation. Our computational analysis shows that graphene functionalization with single hydroxyl and carboxylic acid fails to open a band gap in graphene. While single epoxide functionalization successfully opens a bandgap in graphene and increases absorptivity, however, other optical properties such as reflection, transmission, and dielectric constants are significantly altered. Boron and nitrogen dopants lead to p- and n-type doping, respectively, while fluorine dopants or a single-carbon atomic vacancy cannot create a significant bandgap in graphene. By rigorously considering the spin-polarization effect, we find that titanium, zirconium, and hafnium dopants can create a bandgap in graphene via an induced flat band around the Fermi level as well as the collapse of the Dirac cone. In addition, silicon, germanium, and tin dopants are also effective in improving the optical characteristics. Our work is important for future experimental work on graphene for laser and optical processing applications.
AB - The rational design of the electronic band structures and the associated properties (e.g. optical) of advanced materials has remained challenging for crucial applications in optoelectronics, solar desalination, advanced manufacturing technologies, etc. In this work, using first-principles calculations, we studied the prospects of tuning the absorption spectra of graphene via defect engineering, i.e. chemical doping and oxidation. Our computational analysis shows that graphene functionalization with single hydroxyl and carboxylic acid fails to open a band gap in graphene. While single epoxide functionalization successfully opens a bandgap in graphene and increases absorptivity, however, other optical properties such as reflection, transmission, and dielectric constants are significantly altered. Boron and nitrogen dopants lead to p- and n-type doping, respectively, while fluorine dopants or a single-carbon atomic vacancy cannot create a significant bandgap in graphene. By rigorously considering the spin-polarization effect, we find that titanium, zirconium, and hafnium dopants can create a bandgap in graphene via an induced flat band around the Fermi level as well as the collapse of the Dirac cone. In addition, silicon, germanium, and tin dopants are also effective in improving the optical characteristics. Our work is important for future experimental work on graphene for laser and optical processing applications.
KW - doping
KW - functionalization
KW - graphene
KW - optical properties
KW - spin-polarization
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U2 - 10.1088/1361-6641/ac4406
DO - 10.1088/1361-6641/ac4406
M3 - Article
AN - SCOPUS:85123840755
SN - 0268-1242
VL - 37
JO - Semiconductor Science and Technology
JF - Semiconductor Science and Technology
IS - 2
M1 - 025013
ER -