Enhanced Energy Transfer from Nitrogen‐Vacancy Centers to Three‐Dimensional Graphene Heterostructures by Laser Nanoshaping

Graphene, a well‐studied 2D material, is used to tailor the emission behavior of proximal light emitters by controlling the energy flow to modulate the related relaxation rates, with potentials in fields of biosensing and photovoltaics. Good interface between emitters and 2D materials are important to efficiently modulate the photon emission behavior. However, seamless integration of quantum light emitters and atomically thin materials is challenging due to fabrication limitation. In this paper, the utilization of laser nanoshaping approaches to “wrap” the atomically thin graphene on nanodiamond particles is reported. Compared with 2D layout, the 3D integration enhances the energy transfer by 45%. Furthermore, it is found that the energy transfer efficiency of nitrogen‐vacancy (NV) centers to the 3D graphene can reach a maximum value of 80% over a long distance (≈25 nm), under intense laser excitation. The authors’ analysis indicates that the photon‐generated carrier density of graphene enhances the nonradiative decay rate of NV centers. Besides contributing new insight on the fundamentals of interactions between graphene and quantum emitters, the effort undertaken furthermore holds tremendous promise in developing the graphene‐based nano‐cavities for various applications ranging from sensing, to photovoltaics, to lasing, and to quantum communications. This work reports the utilization of laser nanoshaping approaches to “wrap” the atomically thin graphene on nanodiamond particles. Compared with the 2D layout, the 3D integration enhances the energy transfer by 45%. This effort holds tremendous promise in developing the graphene‐based nano‐cavities for various applications ranging from sensing, to photovoltaics, to lasing, and to quantum communications.