Herein, a peripherally clamped stretched square monolayer graphene sheet with a side length of 10 nm was demonstrated as a resonator for atomic-scale mass sensing via molecular dynamics (MD) simulation. Then, a novel method of mass determination using the first three resonant modes (mode11, mode21 and mode22) was developed to avoid the disturbance of stress fluctuation in graphene. MD simulation results indicate that improving the prestress in stretched graphene increases the sensitivity significantly. Unfortunately, it is difficult to determine the mass accurately by the stress-reliant fundamental frequency shift. However, the absorbed mass in the middle of graphene sheets decreases the resonant frequency of mode11 dramatically while having negligible effect on that of mode21 and mode22, which implies that the latter two frequency modes are appropriate for compensating the stress-induced frequency shift of mode11. Hence, the absorbed mass, with a resolution of 3.3 × 10⁻²² g, is found using the frequency ratio of mode11 to mode21 or mode22, despite the unstable prestress ranging from 32 GPa to 47 GPa. This stress insensitivity contributes to the applicability of the graphene-based resonant mass sensor in real applications.

Edge mode could disturb the ultra-subtle mass detection for graphene resonators. Herein, classical molecular dynamics simulations are performed to investigate the effect of edge mode on mass sensing for a doubly clamped strained graphene resonator. Compared with the fundamental mode, the localized vibration of edge mode shows a lower frequency with a constant frequency gap of 32.6 GHz, despite the mutable inner stress ranging from 10 to 50 GPa. Furthermore, the resonant frequency of edge mode is found to be insensitive to centrally located adsorbed mass, while the frequency of the fundamental mode decreases linearly with increasing adsorbates. Thus, a mass determination method using the difference of these two modes is proposed to reduce interferences for robust mass measurement. Moreover, molecular dynamics simulations demonstrate that a stronger prestress or a higher width–length ratio of about 0.8 could increase the low-quality factor induced by edge mode, thus improving the performance in mass sensing for graphene resonators.

In consideration of the presented optical-thermally excited resonant mass detection scheme, molecular dynamics calculations are performed to investigate the thermal actuation and resonant mass sensing mechanism. The simulation results indicate that an extremely high temperature exists in a 6% central area of the graphene sheet exposed to the exciting laser. Therefore, constraining the laser driving power and enlarging the laser spot radius are essential to weaken the overheating in the middle of the graphene sheet, thus avoiding being burned through. Moreover, molecular dynamics calculations demonstrate a mass sensitivity of 214 kHz/zg for the graphene resonator with a pre-stress of 1 GPa. However, the adsorbed mass would degrade the resonant quality factor from 236 to 193. In comparison, the sensitivity and quality factor could rise by 1.3 and 4 times, respectively, for the graphene sheet with a pre-stress of 5 GPa, thus revealing the availability of enlarging pre-stress for better mass sensing performance.