Perspective and Prospects for Ordered Functional Materials.

Many functional materials are approaching their performance limits due to inherent trade-offs between essential physical properties. Such trade-offs can be overcome by engineering a material that has an ordered arrangement of structural units, including constituent components/phases, grains, and domains. By rationally manipulating the ordering with abundant structural units at multiple length scales, the structural ordering opens up unprecedented opportunities to create transformative functional materials, as amplified properties or disruptive functionalities can be realized. In this perspective article, a brief overview of recent advances in the emerging ordered functional materials across catalytic, thermoelectric, and magnetic materials regarding the fabrication, structure, and property is presented. Then the possibility of applying this structural ordering strategy to highly efficient neuromorphic computing devices and durable battery materials is discussed. Finally, remaining scientific challenges are highlighted, and the prospects for ordered functional materials are made. This perspective aims to draw the attention of the scientific community to the emerging ordered functional materials and trigger intense studies on this topic.

Efficient Probabilistic Computing with Stochastic Perovskite Nickelates.

Probabilistic computing has emerged as a viable approach to solve hard optimization problems. Devices with inherent stochasticity can greatly simplify their implementation in electronic hardware. Here, we demonstrate intrinsic stochastic resistance switching controlled via electric fields in perovskite nickelates doped with hydrogen. The ability of hydrogen ions to reside in various metastable configurations in the lattice leads to a distribution of transport gaps. With experimentally characterized p-bits, a shared-synapse p-bit architecture demonstrates highly parallelized and energy-efficient solutions to optimization problems such as integer factorization and Boolean satisfiability. The results introduce perovskite nickelates as scalable potential candidates for probabilistic computing and showcase the potential of light-element dopants in next-generation correlated semiconductors.

Macroscopic Gradient Ordered α-Fe/Pr2Fe14B Nanocomposites with Ultrahigh Energy Density.

Nanoparticle self-assembly enables the generation of complex ordered nanostructures with enhanced properties or new functionalities. However, the ordering is often limited to the micrometer scale with chemical strategies due to the relative weak supramolecular interactions that govern the self-assembly process. Here a physical strategy via temperature-gradient-assisted self-assembly is reported to create three-dimensional (3D) macroscopic ordered nanocomposites with different gradient variations in grain size, constituent content, and crystal orientation. The resulting α-Fe/Pr2Fe14B ordered nanostructure with reverse gradients in both the grain size and α-Fe content exhibits a record-high energy density of about 25 MGOe for isotropic α-Fe/Pr2Fe14B systems, approximately 130% higher than that of its disordered counterpart. Both experiments and micromagnetic simulations demonstrate that creating ordered nanostructures is an alternative approach to develop high-performance permanent-magnet materials. Our findings make a significant step toward creating 3D macroscopic ordered nanostructures and will stimulate the development of ordered nanomaterials.

Reconfigurable perovskite nickelate electronics for artificial intelligence.

Reconfigurable devices offer the ability to program electronic circuits on demand. In this work, we demonstrated on-demand creation of artificial neurons, synapses, and memory capacitors in post-fabricated perovskite NdNiO3 devices that can be simply reconfigured for a specific purpose by single-shot electric pulses. The sensitivity of electronic properties of perovskite nickelates to the local distribution of hydrogen ions enabled these results. With experimental data from our memory capacitors, simulation results of a reservoir computing framework showed excellent performance for tasks such as digit recognition and classification of electrocardiogram heartbeat activity. Using our reconfigurable artificial neurons and synapses, simulated dynamic networks outperformed static networks for incremental learning scenarios. The ability to fashion the building blocks of brain-inspired computers on demand opens up new directions in adaptive networks.

Rewritable Nanoplasmonics through Room-Temperature Phase Manipulations of Vanadium Dioxide.

The interactions between light and plasmonic charge oscillations in conducting materials are important venues for realizing nanoscale light manipulations. Conventional metal-based plasmonic devices lack tunability due to the fixed material permittivities. Here, we show that reconfigurable plasmonic functionalities can be achieved using the spatially controlled phase transitions in strongly correlated oxide films. The experimental results discussed here are enabled by a recently developed scanning probe-based technique that allows a nonvolatile, monoclinic-metal VO2 phase to be reversibly patterned at the nanoscale in ambient conditions. Using this technique, rewritable waveguides, spatially modulated plasmonic resonators, and reconfigurable wire-grid polarizers are successfully demonstrated. These structures, effectively controlling infrared lights through spatially confined mobile carriers, showcase a great potential for building programmable nanoplasmonic devices on correlated oxide platforms.

Perovskite neural trees.

Trees are used by animals, humans and machines to classify information and make decisions. Natural tree structures displayed by synapses of the brain involves potentiation and depression capable of branching and is essential for survival and learning. Demonstration of such features in synthetic matter is challenging due to the need to host a complex energy landscape capable of learning, memory and electrical interrogation. We report experimental realization of tree-like conductance states at room temperature in strongly correlated perovskite nickelates by modulating proton distribution under high speed electric pulses. This demonstration represents physical realization of ultrametric trees, a concept from number theory applied to the study of spin glasses in physics that inspired early neural network theory dating almost forty years ago. We apply the tree-like memory features in spiking neural networks to demonstrate high fidelity object recognition, and in future can open new directions for neuromorphic computing and artificial intelligence.

Perovskite nickelates as bio-electronic interfaces.

Functional interfaces between electronics and biological matter are essential to diverse fields including health sciences and bio-engineering. Here, we report the discovery of spontaneous (no external energy input) hydrogen transfer from biological glucose reactions into SmNiO3, an archetypal perovskite quantum material. The enzymatic oxidation of glucose is monitored down to ~5 × 10-16 M concentration via hydrogen transfer to the nickelate lattice. The hydrogen atoms donate electrons to the Ni d orbital and induce electron localization through strong electron correlations. By enzyme specific modification, spontaneous transfer of hydrogen from the neurotransmitter dopamine can be monitored in physiological media. We then directly interface an acute mouse brain slice onto the nickelate devices and demonstrate measurement of neurotransmitter release upon electrical stimulation of the striatum region. These results open up avenues for use of emergent physics present in quantum materials in trace detection and conveyance of bio-matter, bio-chemical sciences, and brain-machine interfaces.

Engineering Bulk, Layered, Multicomponent Nanostructures with High Energy Density.

The precise control of individual components in multicomponent nanostructures is crucial to realizing their fascinating functionalities for applications in electronics, energy-conversion devices, and biotechnologies. However, this control remains particularly challenging for bulk, multicomponent nanomaterials because the desired structures of the constitute components often conflict. Herein, a strategy is reported for simultaneously controlling the structural properties of the constituent components in bulk multicomponent nanostructures through layered structural design. The power of this approach is illustrated by generating the desired structures of each constituent in a bulk multicomponent nanomaterial (SmCo + FeCo)/NdFeB, which cannot be attained with existing methods. The resulting nanostructure exhibits a record high energy density (31 MGOe) for this class of bulk nanocomposites composed of both hard and soft magnetic materials, with the soft magnetic fraction exceeding 20 wt%. It is anticipated that other properties beyond magnetism, such as the thermoelectric and mechanical properties, can also be tuned by engineering such layered architectures.

Associations between the HLA-A/B/DRB1 polymorphisms and aplastic anemia: evidence from 17 case-control studies.

OBJECTIVE: To estimate the associations between HLA-A/B/DRB1 polymorphisms and aplastic anemia (AA), we carried out the meta-analysis. METHODS: In this meta-analysis, all publications in English and Chinese were considered up to 30 September 2015. The electronic databases we searched were Pubmed, Science Direct, Embase, Web of Science, CNKI, Wanfang Data and VIP. We conducted all statistical data analyses in the Stata11.0 software. RESULTS: A total of 17 studies including 9164 subjects (containing 1372 cases and 7792 controls) were retrieved, which studied the relationship between HLA-A/B/DRB1 and AA. Odds ratios (ORs) with 95% confidence intervals (CIs) for the comparisons between cases and controls were calculated. The result revealed that HLA-A*02 and HLA-DRB1 (*0407, *15 and *1501) polymorphisms might increase the risk of AA. Otherwise, HLA-DRB1 (*0301, *04, *0406, *0802, *1301, *1302 and *14) were protective against AA. But, other sites of HLA-A/B/DRB1 in our study had no correlations with AA (all Pc > 0.05). CONCLUSION: In conclusion, HLA-A/B/DRB1 polymorphisms may play an important role in AA, but higher quality and larger sample studies are needed to confirm.

Modeling of flux, binding and substitution of urea molecules in the urea transporter dvUT.

Urea transporters (UTs) are transmembrane proteins that transport urea molecules across cell membranes and play a crucial role in urea excretion and water balance. Modeling the functional characteristics of UTs helps us understand how their structures accomplish the functions at the atomic level, and facilitates future therapeutic design targeting the UTs. This study was based on the crystal structure of Desulfovibrio vulgaris urea transporter (dvUT). To model the binding behavior of urea molecules in dvUT, we constructed a cooperative binding model. To model the substitution of urea by the urea analogue N,N'-dimethylurea (DMU) in dvUT, we calculated the occupation probability of DMU along the urea pore and the ratio of the occupation probabilities of DMU at the external (Sext) and internal (Sint) binding sites, and we established the mutual substitution rule for binding and substitution of urea and DMU. Based on these calculations and modelings, together with the use of the Monte Carlo (MC) method, we further modeled the urea flux in dvUT, equilibrium urea binding to dvUT, and the substitution of urea by DMU in the dvUT. Our modeling results are in good agreement with the existing experimental functional data. Furthermore, the modelings have discovered the microscopic process and mechanisms of those functional characteristics. The methods and the results would help our future understanding of the underlying mechanisms of the diseases associated with impaired UT functions and rational drug design for the treatment of these diseases.

Controllably Manipulating Three-Dimensional Hybrid Nanostructures for Bulk Nanocomposites with Large Energy Products.

Hybrid nanostructures that comprise two or more nanoscale functional components are fascinating for applications in electronics, energy conversion devices, and biotechnologies. Their performances are strongly dependent on the characteristics of the individual components including the size, morphology, orientation, and distribution. However, it remains challenging to simultaneously control these structural properties in a three-dimensional (3D) hybrid nanostructure. Here, we introduce a robust strategy for concurrently manipulating these characteristics in a bulk SmCo/Fe(Co) nanocomposite. This method can tune nanocrystals in size (down to sub-10 nm), morphology (sphere, rod, or disc), and crystallographic orientation (isotropic or anisotropic). We have therefore achieved the desired nanostructures: oriented hard magnetic SmCo grains and homogeneously distributed soft magnetic Fe(Co) grains with high fractions (∼26 wt %) and small sizes (∼12.5 nm). The resulting anisotropic nanocomposite exhibits an energy product that is approximately 50% greater than that of its corresponding pure SmCo magnet and 35% higher than the reported largest value in isotropic SmCo/Fe(Co) systems. Our findings pave a new way to manipulating 3D hybrid nanostructures in a controllable manner.

High-Quality LaVO3 Films as Solar Energy Conversion Material.

Mott insulating oxides and their heterostructures have recently been identified as potential photovoltaic materials with favorable absorption properties and an intrinsic built-in electric field that can efficiently separate excited electron-hole pairs. At the same time, they are predicted to overcome the Shockley-Queisser limit due to strong electron-electron interaction present. Despite these premises a high concentration of defects commonly observed in Mott insulating films acting as recombination centers can derogate the photovoltaic conversion efficiency. With use of the self-regulated growth kinetics in hybrid molecular beam epitaxy, this obstacle can be overcome. High-quality, stoichiometric LaVO3 films were grown with defect densities of in-gap states up to 2 orders of magnitude lower compared to the films in the literature, and a factor of 3 lower than LaVO3 bulk single crystals. Photoconductivity measurements revealed a significant photoresponsivity increase as high as tenfold of stoichiometric LaVO3 films compared to their nonstoichiometric counterparts. This work marks a critical step toward the realization of high-performance Mott insulator solar cells beyond conventional semiconductors.

Novel Bimorphological Anisotropic Bulk Nanocomposite Materials with High Energy Products.

Nanostructuring of magnetically hard and soft materials is fascinating for exploring next-generation ultrastrong permanent magnets with less expensive rare-earth elements. However, the resulting hard/soft nanocomposites often exhibit random crystallographic orientations and monomorphological equiaxed grains, leading to inferior magnetic performances compared to corresponding pure rare-earth magnets. This study describes the first fabrication of a novel bimorphological anisotropic bulk nanocomposite using a multistep deformation approach, which consists of oriented hard-phase SmCo rod-shaped grains and soft-phase Fe(Co) equiaxed grains with a high fraction (≈28 wt%) and small size (≈10 nm). The nanocomposite exhibits a record-high energy product (28 MGOe) for this class of bulk materials with less rare-earth elements and outperforms, for the first time, the corresponding pure rare-earth magnet with 58% enhancement in energy product. These findings open up the door to moving from a pure permanent-magnet system to a stronger nanocomposite system at lower costs.

Photoluminescence of monolayer transition metal dichalcogenides integrated with VO2.

Integrating a phase transition material with two-dimensional semiconductors can provide a route towards tunable opto-electronic metamaterials. Here, we integrate monolayer transition metal dichalcogenides with vanadium dioxide (VO2) thin films grown via molecular beam epitaxy to form a 2D/3D heterostructure. Vanadium dioxide undergoes an insulator-to-metal transition at 60-70 °C, which changes the band alignment between MoS2 and VO2 from a semiconductor-insulator junction to a semiconductor-metal junction. By switching VO2 between insulating and metallic phases, the modulation of photoluminescence emission in the 2D semiconductors was observed. This study demonstrates the feasibility to combine TMDs and functional oxides to create unconventional hybrid optoelectronic properties derived from 2D semiconductors that are linked to functional properties of oxides through proximity coupling.

Correlated metals as transparent conductors.

The fundamental challenge for designing transparent conductors used in photovoltaics, displays and solid-state lighting is the ideal combination of high optical transparency and high electrical conductivity. Satisfying these competing demands is commonly achieved by increasing carrier concentration in a wide-bandgap semiconductor with low effective carrier mass through heavy doping, as in the case of tin-doped indium oxide (ITO). Here, an alternative design strategy for identifying high-conductivity, high-transparency metals is proposed, which relies on strong electron-electron interactions resulting in an enhancement in the carrier effective mass. This approach is experimentally verified using the correlated metals SrVO3 and CaVO3, which, despite their high carrier concentration (>2.2 × 10(22) cm(-3)), have low screened plasma energies (<1.33 eV), and demonstrate excellent performance when benchmarked against ITO. A method is outlined to rapidly identify other candidates among correlated metals, and strategies are proposed to further enhance their performance, thereby opening up new avenues to develop transparent conductors.

Wafer-scale growth of VO2 thin films using a combinatorial approach.

Transition metal oxides offer functional properties beyond conventional semiconductors. Bridging the gap between the fundamental research frontier in oxide electronics and their realization in commercial devices demands a wafer-scale growth approach for high-quality transition metal oxide thin films. Such a method requires excellent control over the transition metal valence state to avoid performance deterioration, which has been proved challenging. Here we present a scalable growth approach that enables a precise valence state control. By creating an oxygen activity gradient across the wafer, a continuous valence state library is established to directly identify the optimal growth condition. Single-crystalline VO2 thin films have been grown on wafer scale, exhibiting more than four orders of magnitude change in resistivity across the metal-to-insulator transition. It is demonstrated that 'electronic grade' transition metal oxide films can be realized on a large scale using a combinatorial growth approach, which can be extended to other multivalent oxide systems.

[Study of BRCA1 and BRCA2 gene mutations in human sporadic breast cancers].

OBJECTIVE: To detect the mutations of BRCA1 and BRCA2 in sporadic breast cancer and study the relationship between BRCA1 and BRCA2 mutations and breast cancer. METHODS: Breast cancer tissues of 144 patients and breast tissues of 30 cases of healthy people who were treated from December 2000 to September 2005 were studied. DNA was extracted by the phenol-chloroform method. Fragments of exon 2, exon 3, exon 5, exon 6, exon 7, exon 8, exon 9, exon 10, exon 11, exon 12, exon 13, exon 14, exon 15, exon 16, exon 17, exon 18, exon 19, exon 20, exon 21, exon 22, exon 23 and exon 24 in the BRCA1 gene and exon 10 and exon 14 in the BRCA2 gene were amplified by polymerase chain reaction. Mutation screening was performed by single-strand conformation polymorphism analysis and alterations were confirmed by DNA sequencing. RESULTS: A total of 20 single nucleotide changes in BRCA1 were detected in the 144 cases of breast cancer patients. The total mutation rate was 13.9% and missense mutation rate was 11.1%. No mutation was detected in the BRCA2 and controls. CONCLUSIONS: Mutations in BRCA1 may play an important role in evaluation of sick risk, earlier diagnosis and gene therapy of breast cancer in southern Chinese populations.