Hierarchical materials that exhibit order over multiple length scales are ubiquitous in nature. Because hierarchy gives rise to unique properties and functions, many have sought inspiration from nature when designing and fabricating hierarchical matter. More and more, however, nature's own high-information content building blocks, proteins, peptides, and peptidomimetics, are being coopted to build hierarchy because the information that determines structure, function, and interfacial interactions can be readily encoded in these versatile macromolecules. Here, we take stock of recent progress in the rational design and characterization of hierarchical materials produced from highinformation content blocks with a focus on stimuli-responsive and "smart" architectures. We also review advances in the use of computational simulations and data-driven predictions to shed light on how the side chain chemistry and conformational flexibility of macromolecular blocks drive the emergence of order and the acquisition of hierarchy and also on how ionic, solvent, and surface effects influence the outcomes of assembly. Continued progress in the above areas will ultimately usher in an era where an understanding of designed interactions, surface effects, and solution conditions can be harnessed to achieve predictive materials synthesis across scale and drive emergent phenomena in the self-assembly and reconfiguration of high-information content building blocks.
with a proper selected optical filter. [8] Nevertheless, this method increases both the cost and complexity of the system and also is limited by the available filters. To address those issues, several strategies have been developed to achieve filterless narrowband photodetections, which include: (1) specially designing the absorber with narrowband absorption; [9][10][11] (2) utilizing the plasma effect to intentionally enhance the absorption at a designed wavelength range; [12] (3) engineering the charge collection efficiency via charge collection narrowing (CCN) mechanism. [13,14] In particular, filterless narrowband photodetectors based on CCN mechanism have been recently demonstrated with decent performance in both 2D perovskite single crystals and 3D perovskite single crystals and films. [15] While in 2D perovskite single crystals the narrowband photoresponse is assisted by the self-trapped states within bandgap, the band-tail states play the dominant role in 3D perovskite based narrowband photodetectors. [16][17][18] The CCN mechanism is to manipulate the charge collection efficiency to a desired spectral region so that the photo response can be controlled in the designed spectral range. In brief, the photogenerated carriers are mainly distributed close to the crystal surface for the above-gap photons due to the large absorption coefficient (termed as surface generation) while the light can penetrate deep into the crystal for the subgap photons because of the smaller absorption coefficient (termed as volume generation). The collection efficiency of surface-generation carriers is greatly suppressed due to the recombination loss due to the imbalanced carriers' transit time, higher local carrier density, and severe surface-charge recombination while the collection efficiency of volume-generation carriers is much less affected by those factors. As a result, the charge collection efficiency of volume-generation carriers is much larger than that of surface-generation carriers. For the photons with energy far below the bandgap energy of materials, the photons cannot be absorbed by the materials, and thus cannot contribute to the photocurrent again. Therefore, under such situation, only photons with energy near or slight below bandgap energy can significantly contribute to the photocurrent, leading to the narrowband spectral response. [4] Polarization-sensitive photodetectors can sense the polarization of light in addition to the intensity and wavelength of the Polarization-sensitive narrowband photodetectors can respond to a narrow spectral range of light together with the ability to sense the polarization of light. Traditionally, expensive filters combined with polarizers are utilized to realize the polarization-sensitive narrowband photodetections. To reduce the cost and simplify optical system, here a polarization-sensitive narrowband photodetector based on 2D perovskite single crystals without any additional optical components is reported. The photodetector shows a linear dichroic ratio of 1.56 at 552 nm under ...
Chiral objects are defined as nonsuperimposable conformations that are mirror images of each other, much like a pair of left and right hands. In fact, the word "chiral" derives from the Greek word "χειρ" (kheir), which translates to "hand." Most biomolecules exist in only one particular conformation. For example, amino acids within large protein and peptide molecules are exclusively in the l-form (left-handed). It has long been considered that the phenomenon of homochirality (predominant occurrence of one conformation) could be linked to the origin of life. [1] These phenomena have inspired chemists and biologists to isolate, synthesize, and study the properties of chiral molecules. Research interest in chiral nanostructures has escalated rapidly since the early 2000s due to visionary reports that either predicted or demonstrated the potential applications of these materials. [2,3] In 2004, Pendry predicted that chiral metamaterials could be used to achieve negative refraction (Figure 1). [2] Following this seminal work, others demonstrated that such materials lead to circular dichroism (CD), [4] negative phase velocities, [5] and intense gyrotropy, [6] generating significant excitement within this emerging field. These properties can be harnessed to realize optical materials including "perfect lenses," [7] circular polarizers, [3] chiroptical sensors, [8] and negative refractive index materials. [9,10] In addition to these optical applications, chiral metallic nanostructures have been used for detection of biomolecular disease precursors, [11] chiral catalysis, [12] and chiral separations. [13] Many of the promising applications of chiral metallic nanostructures arise in part from their plasmonic chiroptical activity. At the nanoscale, individual metallic particles exhibit unique properties due to their high surface to volume ratio and geometric confinement of electrons. One particularly important property is the localized surface plasmon resonance (LSPR), [14] which occurs when the oscillation of surface electrons matches the frequency of incident photons. The spectral position and intensity of the LSPR depends not only on the size, shape, composition, and dielectric environment of the metallic nanoparticles (NPs) [15,16] but also on their aggregation state or assembly. [17] When metallic NPs are arranged in a chiral geometry, [18] the coupling of individual plasmons leads to collective plasmon oscillation across the entire structure. [19] Chiral NP assemblies may exhibit enhanced optical chirality in Chiral nanoparticle (NP) superstructures, in which discrete NPs are assembled into chiral architectures, represent an exciting and growing class of nanomaterials. Their enantiospecific properties make them promising candidates for a variety of potential applications. Helical NP superstructures are a rapidly expanding subclass of chiral nanomaterials in which NPs are arranged in three dimensions about a screw axis. Their intrinsic asymmetry gives rise to a variety of interesting properties, including plasmonic chir...
A loess landslide occurred in the morning of October 6, 2006, in Gaolou district of Daming town, Hua country, Shaanxi, China. The landslide originated from a valley side slope of the loess 'yuan' (dissected loess plateau), below which many houses are densely located. The displaced materials smashed several houses and killed 12 persons, after traveling down a long but gentle valley channel. Field surveys revealed that the displaced materials were highly fluidized. Because there was no rainfall before this event, the leakage of irrigation water from the canal on the top of the slope may be the reason for the initiation. To investigate the possible mechanisms underlying the initiation and movement of this landslide, laboratory tests on the loess samples from the source area were performed. Some preliminary research results are presented in this report.
Developing tunable and stable peroxidase mimetics with high catalytic efficiency provides a promising opportunity to improve and expand enzymatic catalysis in lignin depolymerization. A class of peptoid-based peroxidase mimetics with tunable catalytic activity and high stability is developed by constructing peptoids and hemins into self-assembled crystalline nanomaterials. By varying peptoid side chain chemistry to tailor the microenvironment of active sites, these self-assembled peptoid/hemin nanomaterials (Pep/hemin) exhibit highly modulable catalytic activities toward two lignin model substrates 2,2-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) and 3,3’,5,5’-tetramethylbenzidine. Among them, a Pep/hemin complex containing the pyridyl side chain showed the best catalytic efficiency (Vmax/Km = 5.81 × 10−3 s−1). These Pep/hemin catalysts are highly stable; kinetics studies suggest that they follow a peroxidase-like mechanism. Moreover, they exhibit a high efficacy on depolymerization of a biorefinery lignin. Because Pep/hemin catalysts are highly robust and tunable, we expect that they offer tremendous opportunities for lignin valorization to high value products.
The objective of this study is to analyze clinical manifestations, features of imaging, and laboratory assessment of patients with neuropsychiatric SLE (NPSLE) for better diagnosis and outcome prediction. One hundred eighteen NPSLE patients admitted to the Anhui Provincial Hospital in Hefei, China, between January 2006 and December 2016 were enrolled and analyzed retrospectively. All patients fulfilled the American College of Rheumatology revised classification criteria for SLE. Patients with NPSLE fulfilled the American College of Rheumatology (ACR) nomenclature and case definitions. All NPSLE patients underwent neurological investigations including MRI of nervous system, electroencephalograms, or CSF examination as part of the diagnostic evaluation of nervous system involvement. All statistical analyses were performed. According to different types of data, different statistical methods were used to determine factors associated with abnormal MRI among NPSLE patients. Statistical significance was defined as P value < 0.05(two-tailed). Twelve different neurological manifestations of NPSLE patients were shown, in which headache was most common symptom (25.95%, 34/131), followed by seizures (25.19%, 33/131), cerebrovascular disease (18.32%, 24/131), psychosis (8.40%, 11/131), and others including mood disorder, cognitive dysfunction, plexopathy, cranial neuropathy, movement disorder, myelopathy, acute confusional state, and anxiety disorder. Thirteen patients have two neurological symptoms at the same time. Cerebrospinal fluid was assessed in 76 NPSLE patients, in which 29 patients had higher pressure of cerebrospinal fluid and 66 patients had abnormal immunoglobulin in cerebrospinal fluid, predominantly with an increase of IgG (84.21%, 64/76), followed by an increase of IgA (69.74%, 53/76), and IgM accounted for 47.74% (34/76). The MRI taken by 66.10% (78/118) patients have shown abnormal lesions and/or ischemic changes in the bilateral cerebral hemisphere, thalamus, pons, brainstem, and cerebellum. The abnormal changes in MRI were correlated with antiphospholipid antibody (APL) and C3 (P = 0.026 and 0.040, respectively). The most common clinical manifestation of NPSLE is headache, followed by seizures and cerebrovascular accident. The test of cerebrospinal fluid and MRI plays an important role in the assessment of NPSLE. The abnormal intracranial lesions were correlated with the level of anti-cardiolipin antibodies (ACL) and C3.
Optical anisotropy is essential for the polarization-sensitive optoelectronic devices. Recently, in-plane anisotropy is demonstrated in various 2D layered materials. It has been proved that organic-inorganic perovskites possess excellent optical properties; however, the anisotropy of organic-inorganic perovskites is rarely reported because of the in-plane isotropic structure. Here, we report a large optical anisotropy of one-dimensional organic lead iodine perovskites C 4 N 2 H 14 PbI 4 crystals, including emission, excitation and reflection anisotropy. An emission linear dichroic ratio of 5.5 and an excitation linear dichroic ration of 7 are achieved respectively, which are much larger than the inplane anisotropy of 2D layered materials. The large optical anisotropy can be ascribed to the anisotropic dipole moment in the unique 1D chain structure. In addition, the PL of the 1D C 4 N 2 H 14 PbI 4 crystal is dominated by the broadband self-trapped exciton emission due to the quantum confinement effect and strong electron-phonon interaction. Our results advocate that 1D perovskites are promising in the application of broadband polarization-sensitive optoelectronic devices.
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