Delocalized electron and phonon structures are directives for rationally tuning the intrinsic physicochemical properties of 2D materials by redistributing electronic density. However, it is still challenging to accurately manipulate the delocalized electron and systematically study the relationships between physiochemical properties and practical nanodevices. Herein, the effects of delocalized electrons engineering on blue-arsenic-phosphorus (β-AsP)-based practical devices are systematically investigated via implementing vacancies or heteroatom doping. A tendency of carrier conductivity property from “half-metal” to “metal” is initially found when tuning the electronic structure of β-AsP with adjustable vacancy concentrations below 2 at% or above 3 at%, which can be ascribed to the introduction of delocalized electrons that cause asymmetric contributions to the electronic states near the implementation site. In optical logic device simulations, broadband response, triangular wave circuit system signal, and reverse polarization anisotropy are achieved by adjusting the vacancy concentration, while extinction ratios are as high as 1561. The electric and thermic-logic devices realize the highest available reported giant magnetoresistance (MR) up to 1013% and 1039% at vacancy concentrations of 1.67% and 0.89%, respectively, which is significantly superior to the reports. The results shed light on the electronic delocalization strategy of regulating internal structures to achieve highly efficient nanodevices.
