Abstract
<title>Abstract</title> <p>Living systems sustain complex, far-from-equilibrium structures through the continuous consumption of high-energy chemical fuels, a phenomenon known as dissipative self-assembly (DSA). While DSA has enabled the design of adaptive amorphous materials driven by a single fuel source, the construction of dissipative (opto-)electronic crystals utilizing different fuel inputs acting simultaneously remains a significant challenge. Here, we report a strategy for constructing out-of-equilibrium (opto-)electronic crystals driven by synergetic dual-fuel inputs (chemical and light). Using a bioorganic NG building block, chemical fuel consumption induces a transient condensation reaction that orchestrates successive hydration states of DSA, including colloidal particles and the formation of chiral crystals. Remarkably, the resulting dissipative crystals exhibit light-triggered transient generation of radical anions, providing an additional level of spatiotemporal regulation. Molecular dynamics simulations reveal the atomistic assembly features underlying the various states of the DSA process. Notably, this dual-fuel DSA platform endows the materials with spatiotemporally programmable multifunctionality, enabling self-erasable writing, boolean-logic-based out-of-equilibrium patterning, and dissipative (opto-)electronic device properties. These findings establish a route toward life-like programmable molecular materials with adaptive responses and autonomous information-processing capabilities, offering new opportunities for smart materials and sustainable (opto-)electronic technologies.</p>