Plasmonic colour printing based on engineered metasurfaces has revolutionized colour display science due to its unprecedented subwavelength resolution and high-density optical data storage. However, ...advanced plasmonic displays with novel functionalities including dynamic multicolour printing, animations, and highly secure encryption have remained in their infancy. Here we demonstrate a dynamic plasmonic colour display technique that enables all the aforementioned functionalities using catalytic magnesium metasurfaces. Controlled hydrogenation and dehydrogenation of the constituent magnesium nanoparticles, which serve as dynamic pixels, allow for plasmonic colour printing, tuning, erasing and restoration of colour. Different dynamic pixels feature distinct colour transformation kinetics, enabling plasmonic animations. Through smart material processing, information encoded on selected pixels, which are indiscernible to both optical and scanning electron microscopies, can only be read out using hydrogen as a decoding key, suggesting a new generation of information encryption and anti-counterfeiting applications.
Conspectus The development of DNA nanotechnology, especially the advent of DNA origami, has made DNA ideally suited to construct nanostructures with unprecedented complexity and arbitrariness. As a ...fully addressable platform, DNA origami can be used to organize discrete entities in space through DNA hybridization with nanometer accuracy. Among a variety of functionalized particles, metal nanoparticles such as gold nanoparticles (AuNPs) feature an important pathway to endow DNA-origami-assembled nanostructures with tailored optical functionalities. When metal particles are placed in close proximity, their particle plasmons, i.e., collective oscillations of conduction electrons, can be coupled together, giving rise to a wealth of interesting optical phenomena. Nevertheless, characterization methods that can read out the optical responses from plasmonic nanostructures composed of small metal particles, and especially can optically distinguish in situ their minute conformation changes, are very few. Circular dichroism (CD) spectroscopy has proven to be a successful means to overcome these challenges because of its high sensitivity in discrimination of three-dimensional conformation changes. In this Account, we discuss a variety of static and dynamic chiral plasmonic nanostructures enabled by DNA nanotechnology. In the category of static plasmonic systems, we first show chiral plasmonic nanostructures based on spherical AuNPs, including plasmonic helices, toroids, and tetramers. To enhance the CD responses, anisotropic gold nanorods with larger extinction coefficients are utilized to create chiral plasmonic crosses and helical superstructures. Next, we highlight the inevitable evolution from static to dynamic plasmonic systems along with the fast development of this interdisciplinary field. Several dynamic plasmonic systems are reviewed according to their working mechanisms. We first elucidate a reconfigurable plasmonic cross structure that can execute DNA-regulated conformational changes on the nanoscale. Hosted by a reconfigurable DNA origami template, the plasmonic cross can be switched between a chiral locked state and an achiral relaxed state through toehold-mediated strand displacement reactions. This reconfigurable nanostructure can also be modified in response to light stimuli, leading to a noninvasive, waste-free, and all-optically controlled system. Taking one step further, we show that selective manipulations of individual structural species coexisting in one ensemble can be achieved using pH tuning of reconfigurable plasmonic nanostructures in a programmable manner. Finally, we describe an alternative to achieving dynamic plasmonic systems by driving AuNPs directly on origami. Such plasmonic walkers, inspired by the biological molecular motors in living cells, can generate dynamic CD responses when carrying out directional, progressive, and reverse nanoscale walking on DNA origami. We envision that the combination of DNA nanotechnology and plasmonics will open an avenue toward a new generation of functional plasmonic systems with tailored optical properties and useful applications, including polarization conversion devices, biomolecular sensing, surface-enhanced Raman and fluorescence spectroscopy, and diffraction-limited optics.
High-resolution multicolor printing based on pixelated optical nanostructures is of great importance for promoting advances in color display science. So far, most of the work in this field has been ...focused on achieving static colors, limiting many potential applications. This inevitably calls for the development of dynamic color displays with advanced and innovative functionalities. In this Letter, we demonstrate a novel dynamic color printing scheme using magnesium-based pixelated Fabry-Pérot cavities by gray scale nanolithography. With controlled hydrogenation and dehydrogenation, magnesium undergoes unique metal and dielectric transitions, enabling distinct blank and color states from the pixelated Fabry-Pérot resonators. Following such a scheme, we first demonstrate dynamic Ishihara plates, in which the encrypted images can only be read out using hydrogen as information decoding key. We also demonstrate a new type of dynamic color generation, which enables fascinating transformations between black/white printing and color printing with fine tonal tuning. Our work will find wide-ranging applications in full-color printing and displays, colorimetric sensing, information encryption and anticounterfeiting.
We present a comprehensive overview of chirality and its optical manifestation in plasmonic nanosystems and nanostructures. We discuss top-down fabricated structures that range from solid metallic ...nanostructures to groupings of metallic nanoparticles arranged in three dimensions. We also present the large variety of bottom-up synthesized structures. Using DNA, peptides, or other scaffolds, complex nanoparticle arrangements of up to hundreds of individual nanoparticles have been realized. Beyond this static picture, we also give an overview of recent demonstrations of active chiral plasmonic systems, where the chiral optical response can be controlled by an external stimulus. We discuss the prospect of using the unique properties of complex chiral plasmonic systems for enantiomeric sensing schemes.
One of the fundamental challenges in nanophotonics is to gain full control over nanoscale optical elements. The precise spatiotemporal arrangement determines their interactions and collective ...behavior. To this end, DNA nanotechnology is employed as an unprecedented tool to create nanophotonic devices with excellent spatial addressability and temporal programmability. However, most of the current DNA-assembled nanophotonic devices can only reconfigure among random or very few defined states. Here, we demonstrate a DNA-assembled rotary plasmonic nanoclock. In this system, a rotor gold nanorod can carry out directional and reversible 360° rotation with respect to a stator gold nanorod, transitioning among 16 well-defined configurations powered by DNA fuels. The full-turn rotation process is monitored by optical spectroscopy in real time. We further demonstrate autonomous rotation of the plasmonic nanoclock powered by DNAzyme-RNA interactions. Such assembly approaches pave a viable route towards advanced nanophotonic systems entirely from the bottom-up.
Nature has developed striking light-powered proteins such as bacteriorhodopsin, which can convert light energy into conformational changes for biological functions. Such natural machines are a great ...source of inspiration for creation of their synthetic analogues. However, synthetic molecular machines typically operate at the nanometre scale or below. Translating controlled operation of individual molecular machines to a larger dimension, for example, to 10-100 nm, which features many practical applications, is highly important but remains challenging. Here we demonstrate a light-driven plasmonic nanosystem that can amplify the molecular motion of azobenzene through the host nanostructure and consequently translate it into reversible chiroptical function with large amplitude modulation. Light is exploited as both energy source and information probe. Our plasmonic nanosystem bears unique features of optical addressability, reversibility and modulability, which are crucial for developing all-optical molecular devices with desired functionalities.
Deterministic placement and dynamic manipulation of individual plasmonic nanoparticles with nanoscale precision feature an important step toward active nanoplasmonic devices with prescribed levels of ...performance and functionalities at optical frequencies. In this Letter, we demonstrate a plasmonic walker couple system, in which two gold nanorod walkers can independently or simultaneously perform stepwise walking powered by DNA hybridization along the same DNA origami track. We utilize optical spectroscopy to resolve such dynamic walking with nanoscale steps well below the optical diffraction limit. We also show that the number of walkers and the optical response of the system can be correlated. Our studies exemplify the power of plasmonics, when integrated with DNA nanotechnology for realization of advanced artificial nanomachinery with tailored optical functionalities.
Control over plasmonic colors on the nanoscale is of great interest for high-resolution display, imaging, and information encryption applications. However, so far, very limited schemes have been ...attempted for dynamic plasmonic color generation. In this paper, we demonstrate a scanning plasmonic color generation scheme, in which subwavelength plasmonic pixels can be laterally switched on/off through directional hydrogenation/dehydrogenation of a magnesium screen. We show several dynamic plasmonic color displays with different scanning functions by varying the number and geometries of the palladium gates, where hydrogen enters the scanning screens. In particular, we employ the scanning effects to create a dynamic plasmonic quick response code. The information cannot be decrypted by varying the polarization states of light or by accessing the physical features. Rather, it can only be read out using hydrogen as a decoding key. Our work advances the established design concepts for plasmonic color printing and provides insights into the development of optical information storage and anticounterfeiting features.
•lncRNA ENSG00000253385.1 is an independent prognostic factor for esophageal cancer.•lncRNA ENSG00000253385.1 plays a clear role in the invasion of esophageal cancer immune cells and the signaling ...pathways of these cells.•lncRNA ENSG00000253385.1 expression was elevated in the esophageal cancer cell lines KYSE150 and KYSE410.•Small interfering RNA (siRNA)-mediated silencing of lncRNA ENSG00000253385.1 significantly inhibited the proliferation, migration and invasion of KYSE150 and KYSE410 cells and promoted their apoptosis.
Previous studies have shown that necroptosis-related long noncoding RNA (lncRNA) risk models can be used to predict prognosis and immune infiltration in patients with esophageal cancer. However, further analysis of the regulatory mechanisms of necroptosis-related lncRNAs used in risk models remains to be conducted. The purpose of the present study was to identify valuable necroptosis-related lncRNAs in esophageal cancer and to verify their molecular and cellular functions.
Esophageal cancer data were downloaded from The Cancer Genome Atlas (TCGA). The expression of eight genes (LINC00299, AC090912.2, AC244197.2, AL158166.1, AC079684.1, AP003696.1, AC079684.1 and AP003696.1) in the necroptosis-related lncRNA risk model, their relationships with clinicopathological stage, and their diagnostic receiver operating characteristic (ROC) curves were analyzed. The prognostic value of these lncRNAs for overall survival (OS) and disease specific survival (DSS) was analyzed, and time-dependent ROC curves were generated. The AP003696.1 target gene (lncRNA ENSG00000253385.1) was further investigated through immune infiltration analysis, Gene Ontology/Kyoto Encyclopedia of Genes and Genomes (GO/KEGG) enrichment analyses, and gene coexpression analysis. Finally, in vitro functional assays based on lncRNA ENSG00000253385.1 were conducted to explore its regulatory role in esophageal cancer.
A bioinformatics approach was used to study the eight genes in the necroptosis-related lncRNA risk model. AP003696.1 (lncRNA ENSG00000253385.1) was highly expressed in esophageal cancer tissues, and its high expression was correlated with poor OS and DFdS. Both univariate and multivariate Cox regression analyses revealed that lncRNA ENSG00000253385.1 is an independent prognostic factor. The lncRNA ENSG00000253385.1 gene was demonstrated to play a definite role in the invasion of esophageal cancer immune cells and in signaling pathways in these cells. In vitro cell functional assays revealed that lncRNA ENSG00000253385.1 expression was elevated in the KYSE150 and KYSE410 esophageal cancer cell lines. Small interfering RNA (siRNA)-mediated silencing of lncRNA ENSG00000253385.1 significantly inhibited the proliferation, migration, and invasion of KYSE150 and KYSE410 cells, as well as promoted their apoptosis.
The ENSG00000253385.1 gene may be a key gene in the occurrence, development, and prognosis of esophageal cancer. These findings provide new ideas and references for the screening of therapeutic targets, as well as the development of targeted drugs, for esophageal cancer treatment.
Conspectus The key component of nanoplasmonics is metals. For a long time, gold and silver have been the metals of choice for constructing plasmonic nanodevices because of their excellent optical ...properties. However, these metals possess a common characteristic, i.e., their optical responses are static. The past decade has been witnessed tremendous interest in dynamic control of the optical properties of plasmonic nanostructures. To enable dynamic functionality, several approaches have been proposed and implemented. For instance, plasmonic nanostructures can be fabricated on stretchable substrates or on programmable templates so that the interactions between the constituent metal nanoparticles and therefore the optical responses of the plasmonic systems can be dynamically changed. Also, plasmonic nanostructures can be embedded in tunable dielectric materials, taking advantage of the sensitive dependence of the localized surface plasmon resonances on the neighboring environment. Another approach, which is probably the most intriguing one, is to directly regulate the carrier densities and dielectric functions of the metals themselves. In this Account, we discuss a relatively new metal in nanoplasmonics, magnesium, and its important role in the development of dynamic plasmonic nanodevices at visible frequencies. We first elucidate the basic optical properties of Mg and compare it with conventional plasmonic materials such as Au, Ag, and others. Then we describe a unique characteristic of Mg, i.e., its reversible phase transitions between the metallic state and a dielectric state, magnesium hydride, through hydrogenation and dehydrogenation. This sets the basis for Mg in dynamic nanoplasmonics. In particular, the structural properties and dielectric functions of the two distinct states are discussed in detail. Subsequently, we highlight the experimental investigations of the physical mechanisms and nanoscale understanding of Mg nanoparticles during hydrogenation and dehydrogenation. We then introduce a plethora of newly developed Mg-based dynamic optical nanodevices for applications in plasmonic chirality switching, dynamic color displays with Mg nanoparticles and films, and dynamic metasurfaces for ultrathin and flat optical elements. We also outline strategies to enhance the stability, reversibility, and durability of Mg-based nanodevices. Finally, we end this Account by outlining the remaining challenges, possible solutions, and promising applications in the field of Mg-based dynamic nanoplasmonics. We envision that Mg-based dynamic nanoplasmonics will not only provide insights into understanding the catalytic processes of hydrogen diffusion in metals by optical means but also will open an avenue toward functional plasmonic nanodevices with tailored optical properties for real-world applications.
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