Our Quantum DNA research group is pioneering the use of deoxyribonucleic acid (DNA) as a programmable, self-assembling architecture to organize dye molecules for quantum information systems. In particular, we have shown DNA self-assembly to be a viable platform for arranging and controlling the organization of dye aggregates to enable exciton delocalization. Exciton delocalization, exciton-exciton interaction, and electronic coherence are mediated by several key parameters. We postulate, and show theoretically, that certain combinations of these parameters give rise to optically-accessible, entangled many-exciton states that can be tuned by tailoring the dye aggregate structure. Therefore, our project objectives are predicated on approaches to precisely control dye properties and arrangement—thereby enhancing exciton delocalization, exciton-exciton interaction, and coherence—via targeted modifications of dyes and DNA scaffolds. Specifically, we will: (1) continue to refine our design rules for materials properties as they impact key dye and dye aggregate parameters; (2) continue to develop Boise State’s instrumentation capabilities, along with associated theoretical and measurement technique advancement, and demonstrate successful measurements of key parameters (and their control) and ultimately entanglement detection; and (3) expand our theoretical treatment of the Frenkel-Holstein Hamiltonian and use of data-driven and multiscale modeling techniques, all of which will contribute to a pathway for creating, detecting, and controlling quantum entanglement.

This project (Phase III) builds on our successful Phase I and II projects. Our goals for Phase III are to: (1) define design rules for a pathway to create and control entanglement and (2) demonstrate methodologies that enable detection of entanglement. We will accomplish this goal through six primary and integrated research objectives. Integration will occur via extensive collaborations across our five research teams. Objective 1 will build on our emerging dye synthesis capabilities (initiated in Phase II) to design, synthesize, and test custom synthesized dyes exhibiting key parameter states useful for creating exciton-entangled states. Objective 2 will tailor structures of the in-house synthesized dyes, rigid dyes (less aggregate fluorescence suppression), and “super” dyes (single molecule chromophore aggregates) and higher order and rigid DNA templates to achieve nanostructures from which entangled excited states can be detected. Objective 3 will leverage its state-of-the-art advanced and ultrafast spectroscopy instrumentation and technique capabilities developed in Phases I and II to measure key parameters of interest and assist in overcoming challenges related to excited-state quenching. Whereas Objectives 1–3 build and investigate ensembles of DNA-templated dye constructs, Objective 4 will examine individual DNA-templated dye constructs to assess dye aggregate orientation control precision and approaches to reduce population heterogeneity. Objective 5 will support all other objectives by: (1) enhancing an in-house modeling tool to support theoretical treatment of entanglement and (2) applying innovative data-driven modeling and computational techniques to guide dye and aggregate design and characterization. Objective 6 will develop the theory underlying the creation and detection of entangled states in dye aggregates.

Impacts include fundamental knowledge and ultimately design rules that define key dye structure-property relationships as these impact key parameters and various timescales governing quantum entanglement, modest infrastructure development, and continued student and staff resource development at Boise State. This Phase III grant also will strengthen current and foster emerging collaborations that will advance knowledge and capability at Boise State and fuel additional innovative research, much as our previous phase awards led to a successful collaboration with the U.S. Naval Research Laboratory and subsequent funding on two grants.

Benefits include (1) increased research competitiveness and enhanced capabilities of the Quantum DNA group, Boise State, and the state of Idaho and (2) new foundational knowledge essential to creating, detecting, and controlling room-temperature, exciton quantum entanglement. The project directly addresses DOE’s Basic Energy Sciences interest in the “creation and control of coherent phenomena in quantum systems emphasizing an improved understanding of entanglement and enhanced coherence lifetimes.”