Accurate modeling of large DNA structures provided by quantum calculations would be especially useful in the burgeoning field of DNA nanotechnology, which utilizes a repeated four-way junction motif to program large-scale synthetic DNA assemblies often referred to as "DNA origami." An understanding of how to control these customized, scaffolded DNA structures has led to applications such as biological light-harvesting and energy transfer , biomedical sensing , and molecular-scale memory storage. However, the sheer sizes of these DNA origami structures restrict their theoretical and computational study to coarsegrained methods or classical all-atom molecular dynamics, which are both dependent on the accuracy of the underlying force fields. In fact, a recent study has shown that commonly used DNA force fields often give incorrect results in describing the folding mechanisms of four-way junctions. It is now easier than ever to sequence and build novel DNA origami structures using available strand routing and structural design software, but a straightforward tool to accurately analyze these DNA structures at the molecular and electronic level does not yet exist.