Rational Design of Pore Size and Functionality in a Series of Isoreticular Zwitterionic Metal-Organic Frameworks

The isoreticular expansion and functionalization of charged-polarized porosity has been systematically explored by the rational design of 11 isostructural zwitterionic metal-organic frameworks (ZW-MOFs). This extended series of general structural composition {[M3F(L1)3(L2)1.5]·guests}n was prepared by employing the solvothermal reaction of Co and Ni tetrafluoroborates with a binary ligand system composed of zwitterionic pyridinium derivatives and traditional functionalized ditopic carboxylate auxiliary ligands (HL1·Cl = 1-(4-carboxyphenyl)-4,4′-bipyridinium chloride, Hcpb·Cl; or 1-(4-carboxyphenyl-3-hydroxyphenyl)-4,4′-bipyridinium chloride, Hchpb·Cl; and H2L2 = benzene-1,4-dicarboxylic acid, H2bdc; 2-aminobenzene-1,4-dicarboxylic acid, H2abdc; 2,5-dihydroxy-1,4-benzenedicarboxylic acid, H2dhbdc; biphenyl-4,4′-dicarboxylic acid, H2bpdc; or stilbene-4,4′-dicarboxylic acid, H2sdc). Single-crystal structure analyses revealed cubic crystal symmetry (I-43m, a = 31-36 Å) with a 3D pore system of significant void space (73-81%). The pore system features three types of pores being systematically tunable in size ranging from 17.4 to 18.8 Å (pore I), 8.2 to 12.8 Å (pore II), and 4.8 to 10.4 Å (pore III) by the choice of auxiliary ligands. All members of this series have noninterpenetrating structures and exhibit robust architectures, as evidenced by their permanent porosity and high thermal stability (up to 300 °C). The structural integrity and specific surface areas could be systematically optimized using supercritical CO2 exchange methods for framework activation resulting in BET surface areas ranging from 1250 to 2250 m2/g. Most interestingly, as a structural landmark, we found the pore surfaces lined with charge gradients employed by the pyridinium ligands. This key feature results in significant adsorption of carbon dioxide and methane which is attributed to polarization effects. With this contribution we pioneer the reticulation of pyridinium building blocks into extended zwitterionic networks in which specific properties can be targeted

Demonstration of nanoimprinted hyperlens array for high-throughput sub-diffraction imaging

11124Nsciescopu

20 K superconductivity in heavily electron doped surface layer of FeSe bulk crystal

A superconducting transition temperature Tc as high as 100 K was recently discovered in 1 monolayer (1ML) FeSe grown on SrTiO3 (STO). The discovery immediately ignited efforts to identify the mechanism for the dramatically enhanced Tc from its bulk value of 7 K. Currently, there are two main views on the origin of the enhanced Tc; in the first view, the enhancement comes from an interfacial effect while in the other it is from excess electrons with strong correlation strength. The issue is controversial and there are evidences that support each view. Finding the origin of the Tc enhancement could be the key to achieving even higher Tc and to identifying the microscopic mechanism for the superconductivity in iron-based materials. Here, we report the observation of 20 K superconductivity in the electron doped surface layer of FeSe. The electronic state of the surface layer possesses all the key spectroscopic aspects of the 1ML FeSe on STO. Without any interface effect, the surface layer state is found to have a moderate Tc of 20 K with a smaller gap opening of 4 meV. Our results clearly show that excess electrons with strong correlation strength alone cannot induce the maximum Tc, which in turn strongly suggests need for an interfacial effect to reach the enhanced Tc found in 1ML FeSe/STO.Comment: 5 pages, 4 figure

Role of the dimerized gap due to anion ordering in spin-density wave phase of (TMTSF)2_2ClO4_4 at high magnetic fields

Magnetoresistance measurements have been carried out along the highly conducting a axis in the FISDW phase of hydrogened and deuterated (TMTSF)$_2$ClO$_4$ for various cooling rates through the anion ordering temperature. With increasing the cooling rate, a) the high field phase boundary $\beta_{\rm {HI}}$, observed at 27 T in hydrogened samples for slowly cooled, is shifted towards a lower field, b) the last semimetallic SDW phase below $\beta_{\rm {HI}}$ is suppressed, and c) the FISDW insulating phase above $\beta_{\rm {HI}}$ is enhanced in both salts. The cooling rate dependence of the FISDW transition and of $\beta_{\rm {HI}}$ in both salts can be explained by taking into account the peculiar SDW nesting vector stabilized by the dimerized gap due to anion ordering.Comment: 6pages,6figures(EPS), accepted for publication in PR

Extended Formulations in Mixed-integer Convex Programming

We present a unifying framework for generating extended formulations for the polyhedral outer approximations used in algorithms for mixed-integer convex programming (MICP). Extended formulations lead to fewer iterations of outer approximation algorithms and generally faster solution times. First, we observe that all MICP instances from the MINLPLIB2 benchmark library are conic representable with standard symmetric and nonsymmetric cones. Conic reformulations are shown to be effective extended formulations themselves because they encode separability structure. For mixed-integer conic-representable problems, we provide the first outer approximation algorithm with finite-time convergence guarantees, opening a path for the use of conic solvers for continuous relaxations. We then connect the popular modeling framework of disciplined convex programming (DCP) to the existence of extended formulations independent of conic representability. We present evidence that our approach can yield significant gains in practice, with the solution of a number of open instances from the MINLPLIB2 benchmark library.Comment: To be presented at IPCO 201

Field-induced spin density wave in (TMTSF)2_2NO3_3

Interlayer magnetoresistance of the Bechgaard salt (TMTSF)$_2$NO$_3$ is investigated up to 50 teslas under pressures of a few kilobars. This compound, the Fermi surface of which is quasi two-dimensional at low temperature, is a semi metal under pressure. Nevertheless, a field-induced spin density wave is evidenced at 8.5 kbar above $\sim$ 20 T. This state is characterized by a drastically different spectrum of the quantum oscillations compared to the low pressure spin density wave state.Comment: to be published in Phys. Rev. B 71 (2005

Nearest pattern interaction and global pattern formation

We studied the effect of nearest pattern interaction on a globally pattern formation in a 2-dimensional space, where patterns are to grow initially from a noise in the presence of periodic supply of energy. Although our approach is general, we found that this study is relevant in particular to the pattern formation on a periodically vibrated granular layer, as it gives a unified perspective of the experimentally observed pattern dynamics such as oscillon and stripe formations, skew-varicose and crossroll instabilities, and also a kink formation and decoration

Possible role of bonding angle and orbital mixing in iron pnictide superconductivity: Comparative electronic structure studies of LiFeAs and Sr2VO3FeAs

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Biosolids application and soil organic carbon dynamics: a meta-analysis.

Soil carbon sequestration has been recognized as a potential “direct action” tool in mitigating climate change. Organic matter rich biosolids from wastewater industry has been applied to soils as one of the strategies to the carbon sequestration. However, most of the short- and long-term studies as influenced by land application of biosolids have been showed quite inconsistent results in carbon increments in soils. Therefore, soil carbon sequestration resulted by biosolids application is yet to be needed further studies to elucidate. This study presents a comprehensive MetaAnalysis (MA) on soil carbon sequestration as influenced by biosolids application. Datasets comprised with 175 independent paired-treatments across 25 countries were fed in to Comprehensive Meta-Analysis (version 3) programme and modelled. The MA compared Soil Organic Carbon (SOC as g/kg) changes as the functions of time after biosolids application and its rate over twelve groups under two categories: application age (time after application) as 11 year, and cumulative application rate as 251 tonnes/ha.The fixed model is applied to explicate overall effects of analysed data derived from the MA. The MA showed overall positive influences on soil carbon sequestration towards increasing SOC. For example, the highest effect on SOC was observed at 1-3 age group suggesting the need of short term biosolids application to develop carbon storage in soils. Overall, this study shows that land application of biosolids can be used to increase soil carbon storage and therefore has the potential to be a strategy for mitigating climate change towards carbon sequestration in soils