d-Penicillamine@Ag/Cu Nanocluster-Based Fluorescent Nanoneuron for Logic Screening Phosphonate-Type Organophosphate Pesticides and Steganographically Encrypting Information

Abstract

Organophosphate pesticides are used in agriculture due to their high effectiveness and low persistence in eradicating insects and pests. However, conventional detection methods encounter the limitation of undesired detection specificity. Thus, screening phosphonate-type organophosphate pesticides (OOPs) from their analogues, phosphorothioate organophosphate pesticides (SOPs), remains a challenge. Here, we reported a D-penicillamine@Ag/Cu nanocluster (DPA@Ag/Cu NCs)based fluorescence assay to screen OOPs from 21 kinds of organophosphate pesticides, which can be used for logic sensing and information encryption. Acetylthiocholine chloride was enzymatically split by acetylcholinesterase (AChE) to produce thiocholine, which reduced the fluorescence of DPA@Ag/Cu NCs due to the transmission of electrons from DPA@Ag/Cu NCs donor to the thiol group acceptor. Impressively, OOPs acted as an AChE inhibitor and retained the high fluorescence of DPA@Ag/Cu NCs due to the stronger positive electricity of the phosphorus atom. Conversely, SOPs possessed weak toxicity to AChE, which led to low fluorescence intensity. By setting 21 kinds of organophosphate pesticides as the inputs and the fluorescence of the resulting products as the outputs, DPA@Ag/Cu NCs could serve as a fluorescent nanoneuron to construct Boolean logic tree and complex logic circuit for molecular computing. As a proof of concept, by converting the selective response patterns of DPA@Ag/Cu NCs into binary strings, molecular cryptosteganography for encoding, storing, and concealing information was successfully achieved. This study is expected to advance the progress and practical application of nanoclusters in the area of logic detection and information security while also enhancing the relationship between molecular sensors and the world of information.

Photocontrollable DNA Walker-Based Molecular Circuit for the Tunable Detection of MicroRNA-21 Using Metal–Organic Frameworks as Label-Free Fluorescence Tags

“…DNA molecular computing, as a cutting-edge interdisciplinary research field, holds significant importance in contemporary biology, computer science, and analytical chemistry . Due to DNA inherent biocompatibility, ease of synthesis, sequence programmability, and low cost, the DNA computing devices exhibit significant promise in various biosensing applications .…”

Photocleavable DNA Nanotube-Based Dual-Amplified Resonance Rayleigh Scattering System for MicroRNA Detection Incorporating Molecular Computing-Cascaded Keypad Lock Functionality

“…Molecular sensing systems often integrate biomolecules (nucleic acids, enzymes, and peptides) with nanomaterials (metal–organic framework, quantum dots, graphene, noble metal nanoparticles, and nanoclusters) to regulate the sensing interface for biosensing, bioimaging, and logic gate operations. − The use of expensive labeled biomolecules, such as fluorophores and electrochemically active molecules, restricts the signal capacity and reduces bioaffinity. − Label-free sensing systems with various output signals, including electrochemistry, fluorescence, colorimetry, and so forth, hold significant potential to overcome these limitations. − Resonace Rayleigh scattering (RRS), which occurs when the wavelength of Rayleigh scattering aligns with or is near the molecular absorption band, has gained significant attention due to its notable selectivity and sensitivity. − Nonetheless, RRS sensing systems have primarily been utilized solely for detection purposes. The use of RRS sensing systems in intelligent molecular circuits, particularly in molecular keypad locks, has not yet received adequate consideration.…”