Electrical control of nanoscale functionalization in graphene by the scanning probe technique

Abstract

Functionalized graphene is a versatile material that has well-known physical and chemical properties depending on functional groups and their coverage. However, selective control of functional groups on the nanoscale is hardly achievable by conventional methods utilizing chemical modifications. We demonstrate electrical control of nanoscale functionalization of graphene with the desired chemical coverage of a selective functional group by atomic force microscopy (AFM) lithography and their full recovery through moderate thermal treatments. Surprisingly, our controlled coverage of functional groups can reach 94.9% for oxygen and 49.0% for hydrogen, respectively, well beyond those achieved by conventional methods. This coverage is almost at the theoretical maximum, which is verified through scanning photoelectron microscope measurements as well as first-principles calculations. We believe that the present method is now ready to realize 'chemical pencil drawing' of atomically defined circuit devices on top of a monolayer of graphene.

Experimental analysis and theoretical studies by density functional theory of aminopropyl-modified ordered mesoporous carbon

“…Projected augmented wave (PAW) method [16] is applied in this work. All calculations are performed using the local density approximation, which is feasible for modeling the graphite surface functionalization [17,18]. Interlayer distance is 3.35 Å by LDA approach and that is in good agreement with experimental value (3.33 Å) [19].…”

Surface modification of graphene and graphite by nitrogen plasma: Determination of chemical state alterations and assignments by quantitative X-ray photoelectron spectroscopy

“…7 and in Table S1 of the Supplementary Information. The epoxy and part of the OH groups are believed to be attached on top of the graphene planes, while all the other bonding configurations are located predominantly on the Imre Bertóti, Miklós Mohai, Krisztina László Surface modification of graphene and graphite by nitrogen plasma: Determination of chemical state alterations and assignments by quantitative X-ray photoelectron spectroscopy Carbon, 84, 185-196, 2015 edges of the planes or attached to the carbon atoms surrounding the in-plane defect sites around carbon vacancies [14,50].…”

“…Before discussing a recently published set of data [5,14,40,41,47,48,[53][54][55][56][57] of surface treated nanocarbon materials, depicted in Fig. 7 (and in Table 1 in the Supplementary Information), several problems associated with the published peak-synthesis procedure and the following assignments have to be emphasized.…”

“…In their use as reinforcing polymer matrices, tailored surface treatment not only improves their dispersion, but also assists their chemical bonding to the matrix [9,12]. Nanometric scale surface modification has been achieved recently by a novel atmospheric plasma AFM lithography technique, with the objective of preparing atomically defined electronic circuit devices on top of a graphene monolayer [14].…”

Oxidation of a Graphite Surface: The Role of Water

“…9 Recent experimental 26,27 and theoretical works 27 demonstrate that the oxidation of graphene bi-and trilayers is different from that of monolayer. These results demand the modeling of graphite oxidation to build a proper model of the GO formation process.…”