Microwave-Assisted Synthesis of Silver Nanoparticles for Multimode Colorimetric Sensing of Multiplex Metal Ions and Molecular Informatization Applications.

Plasmonic materials have been widely used in chemo/biosensing and biomedicine. However, little attention has been paid to the application of plasmonic materials in terms of the transition from molecular sensing to molecular informatization. Herein, we demonstrated that silver nanoparticles (AgNPs) prepared through facile and rapid microwave heating have multimode colorimetric sensing capabilities to different metal ions (Cr3+, Hg2+, and Ni2+), which can be further transformed into interesting and powerful molecular information technology (massively parallel molecular logic computing and molecular information protection). The prepared AgNPs can quantitatively and sensitively detect Cr3+ and Hg2+ in actual water samples. The AgNPs' multimode-guided multianalyte sensing processing was further investigated to construct a series of basic logic gates and advanced cascaded logic circuits by considering the analytes as the inputs and the colorimetric signals (like color, absorbance, wavelength shift) as the outputs. Moreover, the selective responses and molecular logic computing ability of AgNPs were also utilized to develop molecular cryptosteganography for encrypting and hiding some specific information, which proves that the molecular world and the information world are interconnected and use each other. This research not only opens the door for the transition from molecular sensing to molecular informatization but also provides an excellent opportunity for the construction of the "metaverse" of the molecular world.

Peptide-Based Sensing, Logic Computing, and Information Security on the Antimonene Platform.

Peptides have higher information density than DNA and equivalent molecular recognition ability and durability. However, there are currently no reports on the comprehensive use of peptides' recognition ability and structural diversity for sensing, logic computing, information coding, and protection. Herein, we, for the first time, demonstrate peptide-based sensing, logic computing, and information security on the antimonene platform. The molecular recognition capability and structural diversity (amino acid sequence) of peptides (Pb2+-binding peptide DHHTQQHD as a model) adsorbed on the antimonene universal fluorescence quenching platform were comprehensively utilized to sense targets (Pb2+) and give a response (fluorescence turn-on) and then to encode, encrypt, and hide information. Fluorescently labeled peptides used as the recognition probe and the information carrier were quenched and hidden by the large-plane two-dimensional material antimonene and specifically bound by Pb2+ as the stego key, resulting in fluorescence recovery. The above interaction and signal change can be considered as a peptide-based sensing and steganographic process to further implement quantitative detection of Pb2+, complex logic operation, information coding, encrypting, and hiding using a peptide sequence and the binary conversion of its selectivity. This research provides a basic paradigm for the construction of a molecular sensing and informatization platform and will inspire the development of biopolymer-based molecular information technology (processing, communication, control, security).

DNA nanosensing systems for tunable detection of metal ions and molecular crypto-steganography.

Various sensing platforms based on molecular or nanosystems are widely exploited through molecular diversity and specific recognition. However, it is extremely challenging to develop systems with tunable sensing ability and utilize the systems as information carriers/covers for communication and safety. Herein, DNA nanosensing systems based on cobalt oxyhydroxide (CoOOH) nanosheets were constructed for tunable detection and valence distinction of metal ions, molecular crypto-steganography, and information coding. CoOOH nanosheets absorb fluorescence-labeled single-stranded DNA with different bases and lengths, resulting in fluorescence quenching. The binding priority of bases with CoOOH nanosheets was guanine (G) > cytosine (C) > adenine (A) ≈ thymine (T) and the short chain excelled long chain. Due to the differences in the interaction among CoOOH, DNA, metal ions and variability of DNA bases, various DNA-CoOOH nanosystems have significantly different selective response patterns (that is selectivity) to metal ions and tunable linear ranges to Fe3+, Hg2+, Cr3+. Interestingly, by utilizing their molecular diversity, recognition, selective patterns, DNA-CoOOH sensing systems can be served as doubly cryptographic and steganographic systems to implement information encoding, encryption, and hiding and to reversely improve the selectivity of metal ions. This study provides an idea and platform for adjustable detection and valence distinction of metal ions, and gives a set of "molecular programming languages" for designing intelligent programmable sensing and molecular information communication and safety systems.

Multifunctional Carbon Nanocomposites as Nanoneurons from Multimode and Multianalyte Sensing to Molecular Logic Computing, Steganography, and Cryptography.

Inspired by information exchange and logic functions of life based on molecular recognition and interaction networks, ongoing efforts are directed toward development of molecular or nanosystems for multiplexed chem/biosensing and advanced information processing. However, because of their preparation shortcomings, poor functionality, and limited paradigms, it is still a big challenge to develop advanced nanomaterials-based systems and comprehensively realize neuron-like functions from multimode sensing to molecular information processing and safety. Herein, using fish scales derived carbon nanoparticles (FSCN) as a reducing agent and stabilizer, a simple one-step synthesis method of multifunctional silver-carbon nanocomposites (AgNPs-FSCN) is developed. The prepared AgNPs-FSCN own wide antibacterial and multisignal response abilities in five channels (including color, Tyndall, absorption and fluorescence intensities, and absorption wavelength) for quantitative colorimetric and fluorescence sensing of H2 O2 , ascorbic acid, and dopamine. Benefiting from its multicoding stimuli-responsive ability, molecular concealment, and programmability, AgNPs-FSCN can be abstracted as nanoneurons for implementing batch and parallel molecular logic computing, steganography, and cryptography. This research will promote the preparation of advanced multifunctional nanocomposites and the development of their multipurpose applications, including the multireadout-guided multianalyte intelligent sensing and sophisticated molecular computing, communication, and security.

Graphene-Based Steganographically Aptasensing System for Information Computing, Encryption and Hiding, Fluorescence Sensing and in Vivo Imaging of Fish Pathogens.

Inspired by information processing and communication of life based on complex molecular interactions, some artificial (bio)chemical systems have been developed for applications in molecular information processing or chemo/biosensing and imaging. However, little attention has been paid to simultaneously and comprehensively utilize the information computing, encoding, and molecular recognition capabilities of molecular-level systems (such as DNA-based systems) for multifunctional applications. Herein, a graphene-based steganographically aptasensing system was constructed for multifunctional application, which relies on specific molecular recognition and information encoding abilities of DNA aptamers ( Aeromonas hydrophila and Edwardsiella tarda-binding aptamers as models) and the selective adsorption and fluorescence quenching capacities of graphene oxide (GO). Although graphene-DNA systems have been widely used in biosensors and diagnostics, our proposed graphene-based aptasensing system can not only be utilized for fluorescence sensing and in vivo imaging of fish pathogens ( A. hydrophila and E. tarda), but can also function as a molecular-level logic computing system where the combination of matters (specific molecules or materials) as inputs produces the resulting product (matter level) or fluorescence (energy level) changes as two outputs. More importantly and interestingly, our graphene-based steganographically aptasensing system can also serve as a generally doubly cryptographic and steganographic system for sending different secret messages by using pathogen-binding DNA aptamers as information carriers, GO as a cover, and a pair of keys, that is, target pathogen as a public key, the encryption key used to encode or decode a message in DNA as a private key. Our study not only provides a novel nanobiosensing assay for rapid and effective sensing and in vivo imaging of fish pathogens, but also demonstrates a prototype of (bio)molecular steganography as an important and interesting extension direction of molecular information technology, which is helpful in probably promoting the development of multifunctional molecular-level devices or machines.

Matter, energy and information network of a graphene-peptide-based fluorescent sensing system for molecular logic computing, detection and imaging of cancer stem cell marker CD133 in cells and tumor tissues.

Tumorigenesis, metastasis, and the recurrence of cancer, which may result from the abnormal presence or activation of cancer stem cells (CSCs), are involved in disorders of exchanged matter (biomarkers), energy and information in living organisms. Rapid and sensitive detection and imaging of CSC biomarkers (such as CD133) are helpful for early diagnosis and therapeutic evaluation of tumors. Recently, a preliminary exploration of a few affinity molecules (like peptide-based probes) has just begun for chemical measurements and imaging of CSC biomarker CD133. However, a comprehensive analysis of the matter, energy and information in an artificial molecular system has not been demonstrated and applied to biosensing and disease diagnosis. In this study, a graphene-peptide-based fluorescent sensing system was constructed by utilizing a graphene oxide platform and a CD133-specific recognition peptide and comprehensively analysed with respect to matter (molecular events), energy (fluorescence) and information flow. The molecular event interaction networks in this system were further used to perform molecular logic computing, for the sensitive detection of CSC marker CD133 (with a linear range from 0 to 630 nM and a detection limit of 7.91 nM), and for an application involving targeting the imaging of cells and tumor tissues that highly express CD133 (with a detection limit of 1.1 × 103 cells per mL for CT26 CSCs). The present report will provide more opportunities for the development and design of molecular-level intelligent complex systems and will probably promote the development of artificial intelligent sensing and treatment systems, a molecular-level "Internet of Things", and artificial life.