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The increasing demand for large-scale integrated logic systems urges the development of multireadout molecular logic gates. Especially, it is of great significance to explore dualreadout logic devices with both fluorescence (FL) and magnetic resonance (MR) signals as measurable outputs, since the signal combination of FL/MR might render molecular logic devices better practicality in biomedical applications. In this study, holmium(III)-doped carbon nanodots (Ho-CDs), which exhibited pH-responsive behaviors in both FL and MR signals, were synthesized by a facile one-pot pyrolysis method. When triggered by H + , Fe 3+ , or Fe 2+ , the Ho-CDs served as a switch for both FL and MR signals, leading to dual-readout and multiaddressable logic gates. A series of elementary Boolean operations including YES, NOT, OR, NOR, XOR, PASS 0, and INH have been successfully demonstrated by varying the chemical inputs of H + /Fe 3+ /Fe 2+ . More importantly, multilevel integrative Boolean operations with higher functions (NOR−INH and MR (XOR + INH)−OR), which realize the concatenation of different logic gates, have also been successfully demonstrated. This study may pave an avenue to design multilevel, dual-readout molecular logic systems with better operation stability, which hold great potential for biomedical applications in the future.

Carbon nanodot (CD)-based logic gates, depending on the fluorescence response of CDs toward various chemicals and biological inputs, have attracted increasing research attention recently. However, it is still challenging to transform multicolor CD-based logic operations into convenient, reprogrammable, and independent readout sensing systems for practical applications. In this study, blue (CD-1), green (CD-2), and red (CD-3) emissive CDs were synthesized and conditioned to implement a series of logic operations, including NOT, PASS 1, NOR, NAND, and IMP. CDs served as logic gates, while Hg2+, Fe3+, H+, and OH– served as chemical inputs. In addition, logic operation information was encoded into Quick Response (QR) codes, which could be easily decoded by a smartphone, highlighting the convenience of information storage and extraction. This study demonstrates an avenue in molecular computing that enables multilevel logic operations, and a convenient and user-friendly readout system for molecular computing. The method reported here holds a great promise to simplify complicated chemo/biosensing for practical applications in the future.

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