12 years after the introduction of DNA-templated silver nanoclusters (DNA-AgNCs), exciting progress has been made and yet we are still in the midst of trying to fully understand this nanomaterial. The prominent excellence of DNA-AgNCs is undoubtedly its modulatable emission property, of which how variation in DNA templates causes emission tuning remains elusive. Based on the up-to-date DNA-AgNCs, we aim to establish the correlation between the structure/sequence of DNA templates and emission behaviour of AgNCs. Herein, we systematically present a wide-range of DNA-AgNCs based on the structural complexity of the DNA templates, including single-stranded DNA (ssDNA), double-stranded DNA (dsDNA), triple-stranded DNA (tsDNA) and DNA nanostructures. For each DNA category, we discuss the emission property, quantum yield and synthesis condition of the respective AgNCs, before cross-comparing the impact of different DNA scaffolds on the properties of AgNCs. A future outlook for this area is given as a conclusion. By putting the information together, this review may shed new light on understanding DNA-AgNCs while we are expecting continuous breakthroughs in this field.

Significance: Nature spent millions of years to evolve electron transfer proteins that span a wide range of reduction potentials (E°′) under physiological conditions, from −1 V to 1 V vs. standard hydrogen electrode. Understanding the rules that govern such tuning within similar classes of metalloproteins enables scientists to rationally tune the E°′of their catalysts without changing the active site. An ultimate test of such understanding is to achieve the entire range of E°′ within a single protein, a feat that has not been achieved yet. Herein, we conclusively found that we can cover the entire 2-V range of E°′ using a single protein with five mutations and two metal ions. We have also provided explanations for structural features responsible for such high potential.

This communication reports a facile, fast (<10 min), and hitherto unreported drug screening method by comparing the fluorescence intensities of the in situ formed gold nanoclusters templated by drug-loaded proteins.

Cysteamine-coated gold nanoparticles (cysAuNPs) are positively charged as-synthesised and hence can interact with negatively charged DNA with ease. We have investigated the dependency of the particles' dispersion stage on different concentrations of lysozyme-binding aptamer (LBA). On top of the commonly reported phenomenon where cysAuNPs aggregate as the concentration of LBA increases, we observed that cysAuNPs redispersed after the amount of LBA achieved a certain threshold, dubbed as the critical redispersion concentration (CRC). By harnessing the aggregation and dispersion behaviour of cysAuNPs at LBA below and above the CRC, respectively, we have demonstrated a bimodal colorimetric aptasensor to detect lysozyme as a proof-of-concept study. Apart from being able to quantify the lysozyme in different ranges of concentrations with a visual change in colour, this aptasensor also demonstrated a novel concept of inverse sensitivity (i.e. higher signal with less analyte), leading to a 24-fold higher of signal-to-noise ratio (SNR), in comparison to the conventional sensors. The aptasensor can also selectively distinguish lysozyme and eliminate false results from other control proteins via both modes. The generalisability, as well as potential of cysAuNPs for bimodal colorimetric detection and inverse sensitivity behaviour have made this material an interesting alternative to citrate-coated AuNPs.