▎ 摘　　要

Hybrid structures of graphene and metal nanoparticles (NPs) have been actively investigated as higher quality surface enhanced Raman spectroscopy (SERS) substrates. Compared with SERS substrates, which only contain metal NPs, the additional graphene layer provides structural, chemical, and optical advantages. However, the two-dimensional (2D) nature of graphene limits the fabrication of the hybrid structure of graphene and NPs to 2D. Introducing three-dimensionality to the hybrid structure would allow higher detection sensitivity of target analytes by utilizing the three-dimensional (3D) focal volume. Here, we report a mechanical self-assembly strategy to enable a new class of 3D crumpled graphene-gold (Au) NPs hybrid nanoplasmonic structures for SERS applications. We achieve a 3D crumpled graphene-Au NPs hybrid structure by the delamination and buckling of graphene on a thermally activated, shrinking polymer substrate. We also show the precise control and optimization of the size and spacing of integrated Au NPs on crumpled graphene and demonstrate the optimized NPs' size and spacing for higher SERS enhancement. The 3D crumpled graphene-Au NPs exhibits at least 1 order of magnitude higher SERS detection sensitivity than that of conventional, flat graphene-Au NPs. The hybrid structure is further adapted to arbitrary curvilinear structures for advanced, in situ, nonconventional, nanoplasmonic sensing applications. We believe that our approach shows a promising material platform for universally adaptable SERS substrate with high sensitivity.