Bi-path color tunable plasmonic micro-nano hybrid structures for encrypted printing.

Colored information is crucial for humans to perceive the world. Plasmonic spectra modulation can serve as an effective means to create different colors. Although several solutions for plasmonic color-printing have been proposed, further information encryption has not received any attention. Herein, we exhibit a fine color modulation strategy to construct noble-metal-based micro-nano hybrid structures in the bi-path of photo-thermal deformation and liquid-phase-chemical reaction. Ag/Ta2O5 bi-layer films are ablated at the center of the machined lines of nanosecond pulsed laser, while silver nanoparticles are formed in other regions by thermal radiation of the infrared laser, which can be further dissolved and shape-modulated in KCl solution under different periods. The variation of size and spacing of nano-Ag particles results in a precise shift of plasmonic spectra in visible region. Colored information can be hidden by adjusting the scan number and the energy density during laser processing, and will emerge after the subsequent chemical dissolution reactions. The bi-path color adjustment strategy is easy to operate and can play a role in key information protection and color image switching.

Semi-spontaneous temporal evolution of relief/fluorescence hybrid gratings for holographic encryption.

Holographic systems can reconstruct the entire wavefront of light which are developed as an excellent platform of information encryption. Although holography has utilized multiple modulation dimensions, little attention is given to its combination with fluorescence emitting. Herein, we propose a semi-spontaneous time-dependent encryption strategy of hybrid holographic fringes with surface relief and fluorescent emission mediated by a plasmonic polymer doped with fluorescent dyes. It is found that the two kinds of optical characteristic regions exhibit unique temporal evolution from the overlapped mode to the staggered one. The mode switching is closely related to the strong quenching effect of gold ions and nanoparticles which are dominant at the early and later recording stages, respectively. Thus, the real and deceptive information are recorded at different holographic writing periods. High-secret information of texts or images is constructed by the array of different sets of holographic fringes and is identified by comparing the dual-channel results of confocal laser scanning microscopes. This work puts a bright way to dynamic holographic encryption.

Exciting-frequency-adaptive amplitude/phase hybrid holographic inscription in plasmonic polymers.

Plasmonic holography is generally regarded as an effective technology for 3D display that meets the requirements of the human visual system. However, low readout stability and large cross talk in the frequency field during a plasmonic photo-dissolution reaction set a huge obstacle for application of color holography. Herein, we propose a new, to the best of our knowledge, route toward producing exciting frequency sensitive holographic-inscription based on plasmonic nano-Ag adaptive growth. Donor-molecule-doped plasmonic polymers on polyethylene terephthalate substrates exhibit wide spectral response range, accurate optical frequency sensing, and bending durability. The resonant plasmonic particles act as optical antennas and transfer energy to surrounding organic matrices for nanocluster production and non-resonant particle growth. The surface relief hologram is also highly dependent on the excitation frequency, so we successfully obtain a controllable cross-periodic structure with amplitude/phase mixed information, as well as color holographic display. This work provides a bright way to high-density storage, information steganography, and virtual/augmented reality.

Dual-path inscription of plasmonic nano-Ag moiré fringes.

Construction of moiré surface patterns has attracted considerable attention due to the fascinating function of photoelectric manipulation. Holographic inscription offers superposition of two or more sinusoidal gratings to form moiré structures. However, the current material platforms primarily depend on a single process of photoinduced physical property change to build up multicomponent gratings. Herein, we demonstrate a strategy of bidirectional photochemical reaction on mesoporous TiO2 matrices to form plasmonic nano-Ag moiré fringes. This consists of a photoreduction grating from in situ growth of Ag nanoparticles (NPs) and a photooxidation grating utilizing the Schottky interface of Ag/TiO2. The pattern obtained under the superposition of double spatial frequencies exhibits non-equidistant moiré fringes. This Letter provides a pathway for implementing complex surface structures.

Plasmonic Optoelectronic Memristor Enabling Fully Light-Modulated Synaptic Plasticity for Neuromorphic Vision.

Exploration of optoelectronic memristors with the capability to combine sensing and processing functions is required to promote development of efficient neuromorphic vision. In this work, the authors develop a plasmonic optoelectronic memristor that relies on the effects of localized surface plasmon resonance (LSPR) and optical excitation in an Ag-TiO2 nanocomposite film. Fully light-induced synaptic plasticity (e.g., potentiation and depression) under visible and ultraviolet light stimulations is demonstrated, which enables the functional combination of visual sensing and low-level image pre-processing (including contrast enhancement and noise reduction) in a single device. Furthermore, the light-gated and electrically-driven synaptic plasticity can be performed in the same device, in which the spike-timing-dependent plasticity (STDP) learning functions can be reversibly modulated by visible and ultraviolet light illuminations. Thereby, the high-level image processing function, i.e., image recognition, can also be performed in this memristor, whose recognition rate and accuracy are obviously enhanced as a result of image pre-processing and light-gated STDP enhancement. Experimental analysis shows that the memristive switching mechanism under optical stimulation can be attributed to the oxidation/reduction of Ag nanoparticles due to the effects of LSPR and optical excitation. The authors' work proposes a new type of plasmonic optoelectronic memristor with fully light-modulated capability that may promote the future development of efficient neuromorphic vision.

Adjustable color response during plasmon resonance by monochromatic light irradiation.

A combination of plasmonic nanoparticles with a semiconductor is a feasible approach to realize multiple color exhibitions. The phenomenon is based on plasmon-driven charge separation between electrons and metal ions, but suitable only for light excitation with different wavelengths. Here, we introduce a color-adjustable method under monochromatic light irradiation. A smart strategy is proposed to construct sandwich structures of a hydrogel coating layer, thermally deposited Ag nanoparticles, and mesoporous TiO2 matrices. The contacting mode of TiO2 and nano-Ag at the Schottky interface is strongly dependent on the pore morphology of the oxide. Surface and interface plasmon resonances result in sample color switching from cyan to green and from brown to purple, respectively. The color response ability is further controlled by hydrogel coating, besides the exciting light wavelength. This Letter paves a bright way for colorful displays and information encryption.

Plasmon-driven light harvesting in poly(vinyl alcohol) films for precise surface topography modulation.

Efficient light harvesting is essential for advanced photonic devices. Complex micro/nano surface relief structures can be produced via light-triggered mechanical movement, but limited in organic active molecular units. In this Letter, we propose to embed noble-metal particles into light-inactive polyvinyl alcohol matrix to construct a light harvesting system driven by plasmon for inscription of surface relief gratings. Ultra-small-sized silver nuclei are generated in the polymer by pre-thermal treatment, acting as an accelerator for the subsequent photoinduced particle growth, hydrogen group cleavage, and matrix softening. Based on such properties, a complex plasmonic array carrying ultra-high-density information is achieved with peristrophic multiplexing holography. This Letter paves a bright way to realize data storage, information encryption, and optical microcavity.

Enhancing hologram memory via deposition of plasmonic nanocubes on orderly mesoporous titania.

Hologram is regarded as a key platform for large-volume data storage and information encryption. Diversity of plasmonic nanostructures makes it being a kind of vibrant hologram memory media. However, recording of amplitude, phase and polarization of light is restricted by difficulty to obtain anisotropic morphology of metal particles. Photocatalysis approach allows wide size distribution of Ag plasmonic nanoparticles after a long growth time on titania but suffers from the disadvantage that the shape of plasmonic nanostructures is mostly isotropic, which weakens optical vector sensitivity and information stability. Herein, Ag nanocubes exhibiting high polarization response ability are deposited on orderly mesoporous titania via UV photocatalysis. Recording efficiency of hologram by orthogonally linearly polarized lights is enhanced and the memorized information can be resistant to UV-erasure, both benefiting from the distal resonance of Ag nanocubes. This work delivers a guideline for long-term data storage and high-efficiency display devices.

Bidirectional Photochromism via Anchoring of Carbon Dots to TiO2 Porous Films.

Photochromic materials present photocontrollable properties, which is of great interest for potential applications including high-density storage and optical displays. Herein, we demonstrate a promising pathway toward smart photochromic nanocomposite exploration by anchoring of carbon dots (CDs) to titanium dioxide (TiO2) porous films. This study reveals that the color of the CDs/TiO2 film obtained by dropping anchoring becomes darker and that obtained by immersion anchoring becomes lighter, both under blue light irradiation. For the photobleaching material system, the spectral response is strongly dependent on wavelength and polarization of the exciting light, which provides new dimensions for optical information encryption and memory. This work lays the foundation for the materials platform in the integration of advanced information processing in the future.

Bi-photonic reduction of anisotropic Ag nanoparticles for color-tunable hologram reconstruction.

Efficient optical phase modulation is essential for information processing. The polarization response of metallic nanoparticles plays a key role in the formation of vector hologram. Commonly, Ag nanoparticles reduced by incoherent UV lamp tend to grow in isotropy, which is unsuitable for the formation of polarization hologram and the resultant multicolor holograms recording-readout in polarization channels. Here, the Ag nanoparticles storage with high polarization-sensitivity and anti-radiation interference are realized via bi-photonic irradiation from UV and visible lasers with participation of electron-acceptor. For the first time, the orthogonal polarization storage efficiency of the system is higher than that of the parallel mode. Color-tunable holographic reconstruction by polarization-multiplexing is achieved. This work provides a significant research strategy for stable, high-density data storage and advanced display.

Graphene-oxide/TiO2 nanocomposite films with electron-donors for multicolor holography.

Graphene oxide (GO) with an ideal two-dimensional structure, presents outstanding optical, electric, and mechanical properties which draws great attention in advanced information devices. Recently, GO-based films were found to show photochromic behavior, especially for the TiO2 involved system which has potential data processing capability, such as storing holograms. However, expanding spectral response range and increasing exposure sensitivity are still challenges for such a film, due to the limited photo-quantum efficiency in reduction reaction. Here, an innovative method of "Immersion-Dropping" technology is proposed to fabricate GO-based continuous films. We, for the first time, achieve colored holography from violet to yellow regions on GO/TiO2 nanocomposite films with introduction of weak acid molecules. A "diffraction self-enhancement" is observed. The obtained results benefit from the broadband photo-response of weak acid molecules and photo-triggered transferring of electrons in multi-channels. This work provides a research strategy for the large-capacity information storage and colorful display device.

Fluorescent Holographic Fringes with a Surface Relief Structure Based on Merocyanine Aggregation Driven by Blue-violet Laser.

Stability and integration are the goals for developing photonic devices. Spirooxazines have the property of photoinduced merocyanine-aggregation in polymer matrix, which can be applied to fluorescence emission and stable information storage. Although visible light coherent radiation with UV-assist has been used to achieve polarization-modulated holographic memory in spirooxazine doped PMMA films, the complexity of optical systems is increased and the aggregation ability of merocyanine is decreased. Here, we report that fluorescent holographic gratings with a surface relief structure can be inscribed in the film via sole irradiation of 403.4 nm. Time-dependent photo-anisotropy and holographic dynamics were both investigated with different power densities of the near-UV laser. The non-exponential photokinetics was explained by the sequential formation of mono- and aggregate-merocyanine molecules. The appearance of merocyanine aggregates is found to be beneficial to the long-term holographic memory with fluorescent emission. This work provides a research strategy for the integrity of storage, display and micro-fabrication of organic functional-devices.

Visible laser-assisted reduction of plasmonic Ag nanoparticles with narrow-band optical absorption for colored holographic reconstruction.

Noble metal plasmonic resonance has been utilized in optical data storage widely for its excellent photo-transformation efficiency. TiO2 nanoporous films deposited with Ag nanoparticles present outstanding polarization-response and color-modulation ability. However, the low exposure-sensitivity at single wavelength inhibits their application in optical information processing, which is urgent to be improved by innovative methods. Here, we report that Ag nanoparticles were deposited efficiently via continuous laser irradiation in the TiO2 nanoporous film treated by tannic acid, presenting high-efficient monochromic absorption property. As a result, two sets of holograms were recorded sequentially at the same point of the film with orthogonal circular polarization configurations. The colored reconstruction of the mixed holograms was achieved by utilizing laser polarization state as chrominance segmentation channel. Our method provides a distinctive route for enhancing the photo-energy conversion efficiency of plasmonic nanoparticles, and paves a way to develop advanced display device.

Selective photo-oxidation induced bi-periodic plasmonic structures for high-density data storage.

Stable and controllable optical memory is necessary for the development of current information technology. In this context, Ag/TiO2 films have received much attention for their photosensitivity in wavelength and polarization, which can be applied to high-density optical storage. Here, we carried out dual-wavelength holographic recording using 403.4 nm and 532 nm lasers, and obtained mixed microfringes based on selective photodissolution of Ag nanoparticles of various sizes in TiO2 nanoporous films. Two recording methods of simultaneous and sequential multiplexing were investigated. It was found that using simultaneous irradiation it is easier to obtain equivalent efficiency in both spectral hole burning and multiplexed grating diffraction, compared with the sequential one. The results can be explained by the Time-accumulation effect during Ag+ ion diffusion and migration in holographic recordings. Based on such properties, multiplexed-holographic fringes with uniform contrast were reserved by simultaneous recording in Ag/TiO2 films. This work provides a new strategy for fabrication of photonic devices with complex microstructures.

Nonvolatile plasmonic holographic memory based on photo-driven ion migration.

Stability of data storage is essential for optical information processing. TiO2 nanoporous films loaded with small-sized Ag nanoparticles thus attracted much attention due to their fast and polarization-sensitive photochemical response, which is able to realize optical phase modulation and high-density optical memory. However, little attention was given to the modulation of the silver ion migration, which plays a key role in anti-erasure of the recorded hologram. In this paper, the strong coupling of two phase gratings was achieved by long-term recording in the Ag-TiO2 film irradiated with a pair of coherent left- and right-hand circular polarization lights from a Blu-ray (∼405 nm) laser. The migration of Ag+ ions was enhanced by the electronic field gradient force. A stable polarization holographic grating was obtained by this method and observed by a polarizing microscope. This work provided a strategy for a nonvolatile device based on photo-driven ion migration.

Blu-ray-sensitive localized surface plasmon resonance for high-density optical memory.

Tunable spectrum-response is desired for efficient photo-energy transformation. Blu-ray (~405 nm) and polarization sensitive Ag/TiO2 nanocomposite films are thus fascinating in application of fast-response and high-density optical memory device. The Ag/TiO2 film has the ability of replicating hologram based on optical coherence by laser-stimulated dissolution of Ag nanoparticles (NPs). The rate and efficiency of the dissolution are supposed to be enhanced by introducing uniform and small-sized Ag NPs in TiO2 nanoporous films. However, no effective methods have been proposed to resolve this issue by now. Here, we develop a simple method of thermal-reduction to obtain high-density, space-dispersed and extremely small-sized Ag NPs in TiO2 nanoporous films pretreated with tannic acid. The film shows both high and narrow absorbance band centered at ~405 nm. Diffraction efficiency of the blu-ray holographic storage in the Ag/TiO2 film is improved by one order of magnitude compared to the traditional UV-reduced sample. Based on such properties, polarization-multiplexing holograms are able to be written at 405 nm and readout with little crosstalk. This work provides effective solutions for sensitizing localized surface plasmon resonance at near-UV region, extending the growth range of Ag NPs in the volume of TiO2, and resultantly, realizing high-density optical memory.

Biphotonic holographic grating recordings for different polarization configurations in spirooxazine-doped polymers.

Spirooxazine-doped polymers exhibit a fast photochromism response and high polarization sensitivity after irradiation in the short-wavelength range. Based on such properties, holographic grating recordings accompanying a linearly polarized blue-violet beam (405 nm) in a photochromic film were performed by two coherent green beams (532 nm) for s-s, p-p, s-p left-to-right circular polarization and right-to-right circular polarization. Under the biphotonic action of 405 and 532 nm, the temporal evolution of the diffraction efficiency was strongly dependent on the polarization configuration of the recording beams. It was found that the blue-violet irradiation plays a dual role in holographic recordings: generation of merocyanine aggregation and induction of anisotropy. The experimental results were precisely fitted with a phenomenological model, assuming the simultaneous formation of one absorption grating induced by the 532 nm light and two coupling phase gratings generated from the refractive index changes by recording and auxiliary beams. The existence of absorption and phase gratings was proved by observing the florescence emission of holographic gratings and testing the dependence of the diffraction efficiency on the reading beam polarization state, respectively. The results provided a good deal of insight into the photochromic behavior of spirooxazine in polymers and created a new range of applications in the field of high-density optical storage.

Photoinduced anisotropy and polarization holographic gratings formed in Ag/TiO2 nanocomposite films.

Formation of anisotropy and polarization holographic gratings (s-s, p-p, and s-p) in Ag/TiO2 nanocomposite films were investigated using Nd:YAG lasers (532 nm) as pumping and writing source, respectively. The observations can be well explained by the anisotropic photodissolution of Ag nanoparticles, the photomobility and reduction of Ag+ ions, and the light scattering induced by Ag nanoparticles. Taking these effects into account, a phenomenological model based on simultaneous formation of the absorption grating and the two coupling phase gratings is proposed and found to be in good agreement with the measurements. The main differences in the three polarization grating formation processes are also discussed.