A reconfigurable plasmonic nanosystem combines an active plasmonic structure with a regulated physical or chemical control input. There have been considerable e orts on integration of plasmonic nanostructures with active platforms using topdown techniques. The active media include phase-transition materials, graphene, liquid crystals and carrier-modulated semiconductors, which can respond to thermal 1 , electrical 2 and optical stimuli 3-5 . However, these plasmonic nanostructures are often restricted to two-dimensional substrates, showing desired optical response only along specific excitation directions. Alternatively, bottom-up techniques o er a new pathway to impart reconfigurability and functionality to passive systems. In particular, DNA has proven to be one of the most versatile and robust building blocks 6-9 for construction of complex three-dimensional architectures with high fidelity 10-14 . Here we show the creation of reconfigurable three-dimensional plasmonic metamolecules, which execute DNA-regulated conformational changes at the nanoscale. DNA serves as both a construction material to organize plasmonic nanoparticles in three dimensions, as well as fuel for driving the metamolecules to distinct conformational states. Simultaneously, the threedimensional plasmonic metamolecules can work as optical reporters, which transduce their conformational changes in situ into circular dichroism changes in the visible wavelength range.Circular dichroism (CD), that is, differential absorption of left-and right-handed circularly polarized light, of natural chiral macromolecules is highly sensitive to their three-dimensional (3D) conformations 15 . Taking a similar strategy, we create 3D reconfigurable plasmonic chiral metamolecules 4,16 , whose conformation changes are highly correlated with their pronounced and distinct CD spectral changes in the visible wavelength range. Figure 1a shows the design schematic. Two gold nanorods (AuNRs) are hosted on a reconfigurable DNA origami template 7,10 , which consists of two 14-helix bundles (80 nm × 16 nm × 8 nm) folded from a long single-stranded DNA (ssDNA) scaffold with the help of hundreds of staple strands 13 . The two origami bundles are linked together by the scaffold strand passing twice between them at one point. To ensure the mobility of the DNA bundles and avoid the formation of a Holliday junction 17 , 8 unpaired bases are introduced to each ssDNA connector (Supplementary Note 1). Twelve binding sites are extended from each origami bundle for robust assembly of one AuNR (38 nm × 10 nm) functionalized with complementary DNA (Supplementary Note 2). The surface to surface distance of the two AuNRs is roughly 25 nm. Owing to close proximity, the excited plasmons in the two AuNRs can be strongly coupled 18 . The two crossed AuNRs constitute a 3D plasmonic chiral object [19][20][21][22] , which generates a theme of handedness when interacting with left-and right-handed circularly polarized light, giving rise to strong CD.
Left-handedRight-handed Two gold nanorods (...