The photochemical and photophysical properties of near-infrared (NIR) dyes are significantly influenced by their aggregation state and mesoscopic morphology. However, beyond chemical synthesis, the regulation mechanisms for the properties of NIR dyes, particularly with respect to photothermal properties of the aggregates, are not yet fully understood. Here, we investigate the photothermal behaviors of croconaine-based (CroA) NIR dyes containing dipeptide or amino acids moieties. The introduction of hydrogen bonding promotes π–π stacking of croconaine center, which can efficiently regulate aggregation states and assembly structures in isopropanol. Under laser irradiation, CroA aggregates undergo aggregation-dissociation transition, the in-situ monomer generation process regulates two parameters of photothermal performance: heating rates and plateau photothermal temperatures. This study reveals the regulation effect of non-covalent bonding interactions on CroA aggregates, highlighting supramolecular assembly strategy not only facilitates to construct of photothermal nanomaterials with well-defined structures, but also provides an alternative and effective method for regulating photothermal performance of NIR dyes.

There is a great interest in developing microelectronic devices based on nanostructured conducting polymers that can selectively electro-couple analytes at high sensitivity and low power. Nanostructured conducting polymers have emerged as promising candidates for this technology due to their excellent stability with low redox potential, high conductivity, and selectivity endowed by chemical functionalization. However, it remains challenging to develop cost-effective and large-scale assembly approaches for functionalized conducting polymers in the practical fabrication of electronic devices. Here, we reported a straightforward wafer-scale assembly of nanostructured hexafluoroisopropanol functionalized poly(3,4-ethylenedioxythiophene) (PEDOT-HFIP) on smooth substrates. This approach is template-free, solution-processed, and adaptable to conductive and nonconductive substrates. By this approach, the nanostructured PEDOT-HFIPs could be easily integrated onto interdigitated electrodes with intimate ohmic contact. At the optimized space-to-volume ratio, we demonstrated a low-power, sensitive, and selective nerve agent sensing technology using this platform by detecting sarin vapor with a limit of detection (LOD) of 10 ppb and signal strength of 400 times the water interference at the same concentration, offering significant advantages over existing similar technologies. We envision that its easy scale-up, micro size, small power consumption, and combination of high sensitivity and selectivity make it attractive for various wearable platforms.