Now showing1 - 10 of 12
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    Printed smart devices for anti-counterfeiting allowing precise identification with household equipment
    (2024-12-01) ;
    Tan, Rong
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    Liu, Yuxin
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    Counterfeiting has become a serious global problem, causing worldwide losses and disrupting the normal order of society. Physical unclonable functions are promising hardware-based cryptographic primitives, especially those generated by chemical processes showing a massive challenge-response pair space. However, current chemical-based physical unclonable function devices typically require complex fabrication processes or sophisticated characterization methods with only binary (bit) keys, limiting their practical applications and security properties. Here, we report a flexible laser printing method to synthesize unclonable electronics with high randomness, uniqueness, and repeatability. Hexadecimal resistive keys and binary optical keys can be obtained by the challenge with an ohmmeter and an optical microscope. These readout methods not only make the identification process available to general end users without professional expertise, but also guarantee device complexity and data capacity. An adopted open-source deep learning model guarantees precise identification with high reliability. The electrodes and connection wires are directly printed during laser writing, which allows electronics with different structures to be realized through free design. Meanwhile, the electronics exhibit excellent mechanical and thermal stability. The high physical unclonable function performance and the widely accessible readout methods, together with the flexibility and stability, make this synthesis strategy extremely attractive for practical applications.
    Publicationtype: Journal Article
      14
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    Confined Flash Printing and Synthesis of Stable Perovskite Nanofilms under Ambient Conditions
    (2024-11-14) ;
    Knaus, Tanja
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    ; ;
    The fabrication of stable perovskite nanofilm patterns is important for the development of functional optical devices. However, current production approaches are limited by the requirement for strict inert gas protection and long processing times. Here, a confined flash printing synthesis method is presented to generate perovskite nanofilms under ambient conditions, combining precursor transfer, perovskite synthesis, crystallization, and polymer protection in a single step within milliseconds. A laser simultaneously prints and induces the flash synthesis, confined in a polymer nanofilm, under normal ambient conditions. Due to its simplicity and flexibility, the method enables the combination and screening of many different perovskite precursor materials on various substrates. Besides for the development of novel perovskite materials and devices, the nanofilms can be applied for biodetection. The unique H<inf>2</inf>O<inf>2</inf>-responsive property of the ultrathin perovskite quantum dot film is applied for biomolecule detection based on oxidase-catalyzed enzymatic reactions.
    Publicationtype: Journal Article
      11
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    Metal-free photoanodes for C–H functionalization
    Organic semiconductors, such as carbon nitride, when employed as powders, show attractive photocatalytic properties, but their photoelectrochemical performance suffers from low charge transport capability, charge carrier recombination, and self-oxidation. High film-substrate affinity and well-designed heterojunction structures may address these issues, achieved through advanced film generation techniques. Here, we introduce a spin coating pretreatment of a conductive substrate with a multipurpose polymer and a supramolecular precursor, followed by chemical vapor deposition for the synthesis of dual-layer carbon nitride photoelectrodes. These photoelectrodes are composed of a porous microtubular top layer and an interlayer between the porous film and the conductive substrate. The polymer improves the polymerization degree of carbon nitride and introduces C-C bonds to increase its electrical conductivity. These carbon nitride photoelectrodes exhibit state-of-the-art photoelectrochemical performance and achieve high yield in C-H functionalization. This carbon nitride photoelectrode synthesis strategy may be readily adapted to other reported processes to optimize their performance.
    Publicationtype: Journal Article
      6
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    An all-in-one nanoprinting approach for the synthesis of a nanofilm library for unclonable anti-counterfeiting applications
    In addition to causing trillion-dollar economic losses every year, counterfeiting threatens human health, social equity and national security. Current materials for anti-counterfeiting labelling typically contain toxic inorganic quantum dots and the techniques to produce unclonable patterns require tedious fabrication or complex readout methods. Here we present a nanoprinting-assisted flash synthesis approach that generates fluorescent nanofilms with physical unclonable function micropatterns in milliseconds. This all-in-one approach yields quenching-resistant carbon dots in solid films, directly from simple monosaccharides. Moreover, we establish a nanofilm library comprising 1,920 experiments, offering conditions for various optical properties and microstructures. We produce 100 individual physical unclonable function patterns exhibiting near-ideal bit uniformity (0.492 ± 0.018), high uniqueness (0.498 ± 0.021) and excellent reliability (>93%). These unclonable patterns can be quickly and independently read out by fluorescence and topography scanning, greatly improving their security. An open-source deep-learning model guarantees precise authentication, even if patterns are challenged with different resolutions or devices.
    Publicationtype: Journal Article
      8
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    Multi-Channel Lanthanide Nanocomposites for Customized Synergistic Treatment of Orthotopic Multi-Tumor Cases
    (2023-07-24)
    Liu, Yuxin
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    Zhu, Xingjun
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    ; ;
    Simultaneous photothermal ablation of multiple tumors is limited by unpredictable photo-induced apoptosis, caused by individual intratumoral differences. Here, a multi-channel lanthanide nanocomposite was used to achieve tailored synergistic treatment of multiple subcutaneous orthotopic tumors under non-uniform whole-body infrared irradiation prescription. The nanocomposite reduces intratumoral glutathione by simultaneously activating the fluorescence and photothermal channels. The fluorescence provides individual information on different tumors, allowing customized prescriptions to be made. This enables optimal induction of hyperthermia and dosage of chemo drugs, to ensure treatment efficacy, while avoiding overtherapy. With an accessional therapeutic laser system, customized synergistic treatment of subcutaneous orthotopic cancer cases with multiple tumors is possible with both high efficacy and minimized side effects.
    Publicationtype: Journal Article
      5
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    Solid Ink Laser Patterning for High-Resolution Information Labels with Supervised Learning Readout
    (2023-04-25) ; ;
    Liu, Yuxin
    ;
    Tagging, tracking, or validation of products are often facilitated by inkjet-printed optical information labels. However, this requires thorough substrate pretreatment, ink optimization, and often lacks in printing precision/resolution. Herein, a printing method based on laser-driven deposition of solid polymer ink that allows for printing on various substrates without pretreatment is demonstrated. Since the deposition process has a precision of <1 µm, it can introduce the concept of sub-positions with overlapping spots. This enables high-resolution fluorescent labels with comparable spot-to-spot distance of down to 15 µm (444,444 spots cm<sup>−2</sup>) and rapid machine learning-supported readout based on low-resolution fluorescence imaging. Furthermore, the defined thickness of the printed polymer ink spots can be used to fabricate multi-channel information labels. Additional information can be stored in different fluorescence channels or in a hidden topography channel of the label that is independent of the fluorescence.
    Publicationtype: Journal Article
      4
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    Nanolayer Laser Absorber for Femtoliter Chemistry in Polymer Reactors
    Laser-induced forward transfer (LIFT) has the potential to be an alternative approach to atomic force microscopy based scanning probe lithography techniques, which have limitations in high-speed and large-scale patterning. However, traditional donor slides limit the resolution and chemical flexibility of LIFT. Here, a hematite nanolayer absorber for donor slides to achieve high-resolution transfers down to sub-femtoliters is proposed. Being wettable by both aqueous and organic solvents, this new donor significantly increases the chemical scope for the LIFT process. For parallel amino acid coupling reactions, the patterning resolution can now be increased more than five times (>111 000 spots cm<sup>−</sup><sup>2</sup> for hematite donor vs 20 000 spots cm<sup>−</sup><sup>2</sup> for standard polyimide donor) with even faster scanning (2 vs 6 ms per spot). Due to the increased chemical flexibility, other types of reactions inside ultrasmall polymer reactors: copper (I) catalyzed click chemistry and laser-driven oxidation of a tetrahydroisoquinoline derivative, suggesting the potential of LIFT for both deposition of chemicals, and laser-driven photochemical synthesis in femtoliters within milliseconds can be explored. Since the hematite shows no damage after typical laser transfer, donors can be regenerated by heat treatment. These findings will transform the LIFT process into an automatable, precise, and highly efficient technology for high-throughput femtoliter chemistry.
    Publicationtype: Journal Article
      8
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    Laser-driven growth of structurally defined transition metal oxide nanocrystals on carbon nitride photoelectrodes in milliseconds
    (2021-12-01) ;
    Zou, Yajun
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    ; ;
    Fabrication of hybrid photoelectrodes on a subsecond timescale with low energy consumption and possessing high photocurrent densities remains a centerpiece for successful implementation of photoelectrocatalytic synthesis of fuels and value-added chemicals. Here, we introduce a laser-driven technology to print sensitizers with desired morphologies and layer thickness onto different substrates, such as glass, carbon, or carbon nitride (CN). The specially designed process uses a thin polymer reactor impregnated with transition metal salts, confining the growth of transition metal oxide (TMO) nanostructures on the interface in milliseconds, while their morphology can be tuned by the laser. Multiple nano-p-n junctions at the interface increase the electron/hole lifetime by efficient charge trapping. A hybrid copper oxide/CN photoanode with optimal architecture reaches 10 times higher photocurrents than the pristine CN photoanode. This technology provides a modular approach to build a library of TMO-based composite films, enabling the creation of materials for diverse applications.
    Publicationtype: Journal Article
      3
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    Alkanes as Intelligent Surface Thermometers: A Facile Approach to Characterize Short-Lived Temperature Gradients on the Micrometer Scale
    Short-lived micro-sized thermal gradients are challenging to measure. Especially, in thin film processes and devices, it is important to know the exact temperature profile to assure process parameters and the stability of sensitive materials. Many theoretical models try to describe the occurring temperatures, but still lack in profound experimental data. Here, a facile approach is presented, which allows to measure confined temperature gradients with millisecond and micrometer precision. By casting a thin alkane film onto a substrate of interest, it is possible to reconstruct local temperature gradients by imaging the phase behavior and morphology of the alkane film with a simple optical microscope setup. Alkanes are inert and their melting and boiling temperatures depend on the chain length. This allows to measure temperatures between 37 and 522 °C on any surface. Furthermore, after thorough characterization of laser-induced temperature gradients, this approach can be used to measure the phase transition behavior of complex thin film polymer mixtures.
    Publicationtype: Journal Article
      7
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    Laser-induced forward transfer of soft material nanolayers with millisecond pulses shows contact-based material deposition
    In this work, we present a qualitative and quantitative experimental analysis, as well as a numerical model, of a novel variant of the laser-induced forward transfer, which uses millisecond laser pulses. In this process, soft material nanolayer spots are transferred from a donor slide, which is coated with the soft material layer, to an acceptor slide via laser irradiation. This method offers a highly flexible material transfer to perform high-throughput combinatorial chemistry for the generation of biomolecule arrays. For the first time, we show visual evidence that the main transfer mechanism is contact-based, due to thermal surface expansion of the donor layer. Thus, the process is different from the many known variants of laser-induced forward transfer. We characterize the maximum axial surface expansion in relation to laser power and pulse duration. On this basis, we derive a numerical model that approximates the axial surface expansion within measurement tolerances. Finally, we analyze the topology of the transferred soft material nanolayer spots by fluorescence imaging and vertical scanning interferometry to determine width, height, and shape of the transferred material. Concluding from this experimental and numerical data, we can now predict the amount of transferred material in this process.
    Publicationtype: Journal Article
      9