Implementation of Digital Computing by Colloidal Crystal Engineering with DNA

Toehold-mediated strand displacement (TMSD) provides a versatile toolbox for developing DNA digital computing systems. Although different logic circuits with diverse functions have achieved good performance in terms of complexity and scalability, most previous DNA logic circuits perform information processing only at the molecular level, and nonspecific signal leakages are often difficult to avoid. Here, we demonstrate the feasibility of constructing leakless digital computing systems in three-dimensionally ordered colloidal supercrystals. These systems possess a unique signal leakage resistance by integrating different TMSD-based logic gates with the catalytic assembly of DNA-functionalized gold colloids. A complete set of basic Boolean logic gates and different cascaded logic circuits is constructed on the basis of the catalytic assembly strategy enabled by a facilely designed catassembler, where the output signals are recognized by determining whether specific colloidal supercrystals are formed or not. In addition, a half adder is built through a combination of XOR and AND logic gates with two distinct crystal types as readouts. Finally, a leakless two-digit DNA keypad lock for information security protection is demonstrated. The combination of TMSD-based logic circuits with the universal nanoparticle catalytic assembly offers the possibility to develop highly complicated and leakage-free digital computing systems and promotes macroscopic colloidal superlattice materials with programmable logic functions.