Unprecedented data manipulation employed using a pH-stimuli responsive hydrogel was developed to achieve reversible data encryption–decryption.

Featured by prominent flexibility and fidelity in producing sophisticated stereoscopic structures transdimensionally, three-dimensional (3D) laser printing techniques have vastly extended the toolkit for delivering diverse functional devices. Yet chiral nanoemitters heavily resorting to artificial structures that manifest efficient emission and tightly confined light–matter interactions simultaneously remain alluring but dauntingly challenging for this technique at this moment. In this study, we assert that the chiral photoluminescence is implemented from silver nanostructures with optical duality in one go via a two-fold three-dimensional laser printing scheme. Such laser printing protocol allows the highly desired duality by simultaneously producing uniformly distributed fluorescent silver nanoclusters and aggregated plasmonic silver nanoparticles to tightly confine chiral interactions at the nanoscale. A helical emitter of 550 nm helix-diameter as fabricated has seen a record-high luminescence anisotropic factor with the absolute value up to 0.58, which is two orders of magnitude greater than fluorescent chiral silver clusters. This method holds great promise for future versatile applications in chiroptical nanodevices.

Based on degradable pH-responsive hydrogel, we report on an enhanced three-dimensional data encryption security technique in which a pH value is used for information manipulation. Featuring three types of states upon the pH value variation, namely, shrinkage, expansion and degradation, the hydrogel renders a limited pH value window as the “key” for information decryption. The pH-dependent shrinkage-to-expansion conversion of the hydrogel leads to a threshold pH value for retrieving the recorded data, whilst the degradability of the hydrogel, which can be tuned by adjusting the composition ratio of PEGDA/AAc, gives rise to a second threshold pH value for irreversibly sabotaging the retrieved data. Pre-doping silver ions in the hydrogel facilitates explicit recording and reading of binary data in forms of three-dimensional silver patterns through photoreduction and scattering, respectively, with a femtosecond laser. By accurately matching the vertical spacing of the encoded silver nanopatterns with the diffraction-limited focal depth of the decryption microscope, we can tune the pH value to encrypt and retrieve information recorded in layers and set a critical pH value to smash encoded information, which proves a highly secured 3D data encoding protocol. This strategy can effectively enrich data encryption techniques, vastly enhancing data security within unattained chemical dimensions.

Recent demonstrations of metasurfaces present their great potential to implement flat and multifunctional optical elements, which are accomplished with the designs of planar optics and micro-/nano- fabrications. Integrating metasurfaces in three dimensions has manifested drastically increasing advantages in manipulating light fields by extending design freedom. However, fabricating three-dimensional metasurfaces remain a tough challenge due to the lack of stereo printing protocols. Herein, we demonstrate laser nanoprinting of floated silver nanoparticle array in transparent hydrogel films for 3D metasurface to achieve color patterning. It is found that spatially resolved nanoparticles can be produced through laser induced photoreduction of silver ions and robustly anchored to the gel backbones by a focused femtosecond laser beam within a pH-responsive smart hydrogel matrix. With the aid of expansion properties of the pH-responsive hydrogel, repetitive coloration of the patterned plasmonic nanoparticle array over a wide spectrum range is achieved via reversible regulation of nanoparticle spacing from 550 to 350 nm and vice versa. This approach allows broadband 3D color-regulation in nanoscale for applications in active spectral filtering, information encryption, security tagging and biological colorimetric sensing, etc.