Abstract
AbstractThe remarkable advances in molecular logic reported in the last decade demonstrate the potential of luminescent molecules for logical operations, a paradigm‐changing concerning silicon‐based electronics. Trivalent lanthanide (Ln3+) ions, with their characteristic narrow line emissions, long‐lived excited states, and photostability under illumination, may improve the state‐of‐the‐art molecular logical devices. Here, the use of monolithic silicon‐based structures incorporating Ln3+ complexes for performing logical functions is reported. Elementary logic gates (AND, INH, and DEMUX), sequential logic (KEYPAD LOCK), and arithmetic operations (HALF ADDER and HALF SUBTRACTOR) exhibiting a switching ratio >60% are demonstrated for the first time using nonwet conditions. Additionally, this is the first report showing sequential logic and arithmetic operations combining molecular Ln3+ complexes and physical inputs. Contrary to chemical inputs, physical inputs may enable the future concatenation of distinct logical functions and reuse of the logical devices, a clear step forward toward input–output homogeneity that is precluding the integration of nowadays molecular logic devices.
Highlights
In a period of a few decades, the computers and related systems become smaller and smaller due to the substantial scaling shrinkage of silicon-based technology components.[1,2,3,4,5] Whereas the first field-effect transistor has the dimensions of a palm of a hand, nowadays over 100 million equivalent components per mm2 are packaged in a chip using state-of-the-art 10 nm lithography.[6]
It was recognized that the molecules can perform logical operations of higher complexity, such as molecular multiplexers and demultiplexers or molecular binary adders and subtractors[18, 20,21,22,23,24,25] All the above-mentioned molecular devices operate in wet conditions, so its immediate use was in biomedicine
By exploiting a Eu3+/Tb3+-functionalized Si platform, that produces narrow and stable emission lines and that is fully compatible with existent Si-based electronic devices, we fabricate molecular logical arrays performing basic (AND, INH, DEMUX), sequential (KEYPAD LOCK), and arithmetic (HALF ADDER and HALF SUBTRACTOR) logic operations
Summary
In a period of a few decades, the computers and related systems become smaller and smaller due to the substantial scaling shrinkage of silicon-based technology components.[1,2,3,4,5] Whereas the first field-effect transistor has the dimensions of a palm of a hand, nowadays over 100 million equivalent components per mm are packaged in a chip using state-of-the-art 10 nm lithography.[6]. Despite it is nowadays recognized that Ln3+ ions can improve the state-of-the-art of molecular logical devices, only a handful of papers have been published so far.[11, 32,33,34,35,36] Up to now, all the logical gates based on Ln3+ ions respond to chemical inputs and operate exclusively in wet conditions, except the Eu3+/Tb3+ based selfassembled polymer monolayer functionalized Si surface proposed by some of us in 2016.[36]. The optical inputs signals can be remotely delivered and read from the molecular devices as time-gated pulses (covering time ranges until the picosecond,[37] faster cycling even in comparison to the electronic counterparts) All these potential benefits motivate the transfer of molecular logic devices from wet (chemical or physical inputs and physical outputs) to dry (exclusively physical inputs and outputs) operation conditions. By exploiting a Eu3+/Tb3+-functionalized Si platform, that produces narrow and stable emission lines and that is fully compatible with existent Si-based electronic devices, we fabricate molecular logical arrays performing basic (AND, INH, DEMUX), sequential (KEYPAD LOCK), and arithmetic (HALF ADDER and HALF SUBTRACTOR) logic operations
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