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Abstract：
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 dual-readout 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+, Fe3+, or Fe2+, 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+/Fe3+/Fe2+. 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.
摘要：
对大规模集成逻辑系统的需求不断增长，促使多读出分子逻辑门的发展。尤其是,探索同时具有荧光（FL）和磁共振（MR）信号作为可测量输出的双读出逻辑器件具有重要意义，因为FL/MR的信号组合可能使分子逻辑设备在生物医学应用中具有更好的实用性。在这项研究中,掺钬（III）的碳纳米点（Ho-CD），在FL和MR信号中均表现出pH响应行为，通过简单的一锅热解法合成。当被H+触发时，Fe3+,或Fe2+，Ho-CD用作FL和MR信号的开关，导致双读出和多寻址逻辑门。一系列基本布尔运算，包括YES，NOT,OR,NOR,XOR,通过改变H+/Fe3+/Fe2+的化学输入,已经成功地证明了PASS0和INH。更重要的是,具有更高函数(NOR-INH和MR(XOR+INH)-OR)的多级积分布尔运算，实现不同逻辑门的串联，也得到了成功的证明。这项研究可能为多层次设计铺平道路，双读出分子逻辑系统具有更好的操作稳定性，这在未来的生物医学应用中具有巨大的潜力。
