Using Graphdiyne Nanoribbons for Molecular Electronics Spectroscopy and Nucleobase Identification: A Theoretical Investigation.

Abstract

In pursuit of fast, cost-effective, and reliable DNA sequencing techniques, a variety of two-dimensional (2D) material-based nanodevices such as solid-state nanopores and nanochannels have been explored and established. Given the promising potential of graphene for the design and fabrication of nanobiosensors, other 2D carbon allotropes such as graphyne and graphdiyne have also attracted a great deal of attention as candidate materials for the development of sequencing technology. Herein, employing the 2D electronic molecular spectroscopy (2DMES) method, we investigate the capability of graphdiyne nanoribbons (GDNRs) as the building blocks of a feasible, precise, and ultrafast sequencing device. Using first-principles calculations, we study the adsorption of four canonical nucleobases (NBs), i.e., adenine (A), cytosine (C), guanine (G), and thymine (T) on an armchair GDNR (AGDNR). Our calculations reveal that compared to graphene, graphdiyne demonstrates more distinct binding energies for different NBs, indicating its more promising ability to unambiguously recognize DNA bases. Utilizing the 2DMES technique, we calculate the differential conductance (Δg) of the studied NB-AGDNR systems and show that the resulting Δg maps, unique for each NB-AGDNR complex, can be used to recognize each individual NB without ambiguity. We also investigate the conductance sensitivity of the proposed nanobiosensor and show that it exhibits high sensitivity and selectivity toward various NBs. Thus, our proposed graphdiyne-based nanodevice would hold promise for next-generation DNA sequencing technology.