Outer Planes Research Articles

Synthesis of Ti1‐xWx Solid Solution MAX Phases and Derived MXenes for Sodium‐Ion Battery Anodes

AbstractA distinguishing feature of MAX phases and their MXene derivatives is their remarkable chemical diversity. This diversity, coupled with the 2D nature of MXenes, positions them as outstanding candidates for a wide range of electrochemical applications. Chemical disorder introduced by a solid solution can improve electrochemical behavior. Up to now, adding considerable amount of tungsten (W) in MAX phase and MXenes solid solutions, which can enhance electrochemical performance, proved challenging. In this study, the synthesis of M site Ti1‐xWx solid solution MAX phases are reported. The 211‐type (Ti1‐xWx)2AlC exhibits a disordered solid solution, whereas the 312‐type (Ti1‐xWx)3AlC2 displays a near‐ordered structure, resembling o‐MAX, with W atoms preferentially occupying the outer planes. Solid‐solution MXenes, Ti2.4W0.6C2Tz, and Ti1.6W0.4CTz, are synthesized via selective etching of high‐purity MAX powder precursors containing 20% W. These MXenes are evaluated as sodium‐ion battery anodes, with Ti1.6W0.4CTz showing exceptional capacity, outperforming existing multilayer MXene chemistries. This work not only demonstrates the successful integration of W in meaningful quantities into a double transition metal solid solution MAX phase, but also paves the way for the development of cost‐effective MXenes containing W. Such advancements significantly widen their application spectrum by fine‐tuning their physical, electronic, mechanical, electrochemical, and catalytic properties.

Enhanced mechanical and thermal properties in 3D printed Al2O3 lattice/ epoxy interpenetrating phase composites

Interpenetrating phase composites (IPCs) with 3D printed alumina microlattices infiltrated with epoxy have been fabricated. Mechanical analysis shows that the IPCs under quasi-static compression generally exhibit fracture behaviour similar to that of their ceramic-lattice constituent but in a gradual manner. The IPCs with Simple Cubic lattices initiate the fractures at the struts in the outer lattice planes, while IPCs with Octet Truss and Kelvin Cell lattices tend to fracture at their (110) or (111) planes. The compressive strength and energy absorption of IPCs follow the order of Simple Cubic > Kelvin Cells > Octet Truss when the ceramic volume fraction is 0.3. The IPCs display compressive strengths up to 120% higher and energy absorption 100% greater than the iso-strain combined properties of the lattice and epoxy. The factors governing the fracture behaviour and the strengthening and energy absorption mechanisms are thoroughly discussed. Furthermore, the IPCs show much better retention of mechanical strength and dimensional stability at elevated temperatures compared with many commonly used particle or fiber-reinforced epoxy matrix composites.

Four new compact triply eclipsing triples found with Gaia and TESS

ABSTRACT This paper presents a comprehensive analysis of four triply eclipsing triple star systems, namely TIC 88206187, TIC 14839347, TIC 298714297, and TIC 66893949. The four systems with third-body eclipses were found in the TESS light curves from among a sample of ∼400 matches between known eclipsing binaries and the Gaia DR3 Non-Single Star solution data base. We combined photometric light curves, eclipse timing variations, archival spectral energy distributions, and theoretical evolution tracks in a robust photodynamical analysis to determine the orbital and system parameters. The triples have outer periods of 52.9 d, 85.5 d, 117 d, and 471 d, respectively. All dozen stars have masses ≲ 2.6 M⊙. The systems are quite flat with mutual inclination angles between the inner and outer orbital planes that are all ≲ 4°. The outer mass ratios (q ≡ M3/Mbin) range from 0.39 to 0.76, consistent with our earlier collection of compact triply eclipsing triples. TIC 88206187 exhibits a fractional radius of the outer tertiary component (rB ≡ RB/aout) exceeding 0.1 (only the third such system known), and we consider its future evolution. Finally, we compare our photodynamical analysis results and the orbital parameters given in the Gaia DR3 NSS solutions, indicating decent agreement, but with the photodynamical results being more accurate.

Three-dimensional flow structures and scalar mixing of a sand dune-inspired jet in crossflow

This paper performed particle image velocimetry (PIV) measurements and delayed detached-eddy simulations (DDES) to comprehensively investigate the flow and mixing behaviors of a sand dune(SD)-inspired JICF (jet in crossflow). PIV measurements were conducted in planes parallel to the mid-plane (Z/D = 0, 0.5, and 1), and three velocity ratios (VR = 0.4, 0.8, and 1.2) were studied. The time-averaged and turbulent flow features behind the sand dune-inspired JICF is strongly three-dimensional: the jet tends to move from the mid-plane to the outer planes and can stay attached well to the wall even at Z/D = 1. Then DDES method was applied to reveal detailed three-dimensional flow structures and mixing characteristics of the SD-inspired JICF, and a cylindrical JICF was also simulated as a benchmark for comparison. The horseshoe vortex, arch-shaped shear layer vortices, and streamwise rollers are mainly responsible for the formation of the anti-counter rotating vortex pair (anti-CRVP) observed in the mean flow field of SD configuration. Analysis of concentration distributions indicates that scalar mixing between the jet and the mainstream is highly correlated to the flow features and vortex structures, and the mixing strength of the sand dune-inspired JICF is generally weaker than that of the cylindrical JICF.

Photocatalytic and thermoelectric performance of asymmetrical two-dimensional Janus aluminum chalcogenides

Through a density functional theory-driven survey, a comprehensive investigation of two-dimensional (2D) Janus aluminum-based monochalcogenides (Al2XY with X/Y = S, Se, and Te) has been performed within this study. To begin with, it is established that the examined phase, in which the Al-atoms are located at the two inner planes while the (S, Se, and Te)-atoms occupy the two outer planes in the unit cell, are energetically, mechanically, dynamically, and thermally stable. To address the electronic and optical properties, the hybrid function HSE06 has been employed. It is at first revealed that all three monolayers display a semiconducting nature with an indirect band gap ranging from 1.82 to 2.79 eV with a refractive index greater than 1.5, which implies that they would be transparent materials. Furthermore, the monolayers feature strong absorption spectra of around 105 cm−1 within the visible and ultraviolet regions, suggesting their potential use in optoelectronic devices. Concerning the photocatalytic performance, the conduction band-edge positions straddle the hydrogen evolution reaction redox level. Also, it is observed that the computed Gibbs free energy is around 1.15 eV, which is lower and comparable to some recently reported 2D-based Janus monolayers. Additionally, the thermoelectric properties are further investigated and found to offer a large thermal power as well as a high figure of merit (ZT) around 1.03. The aforementioned results strongly suggest that the 2D Janus Al-based monochalcogenide exhibits suitable characteristics as a potential material for high-performance optoelectronic and thermoelectric applications.

Limitation of solid-reaction technique in a controlled experiment: Characterization of polycrystalline LaCe0·9Th0.1CuOy compound

Solid-state reactions are the most prominent method to synthesize compounds in physics, chemistry, and material science because of their simplicity to scale up or down. Its uneven chemical reactions result in wide variances in the optical and microstructural properties of the material. There is therefore a need to adopt computational techniques to filter out anomalies. This research considers the polycrystalline growth of LaCe0·9Th0.1CuOy via the solid-state reaction. Its chemical and morphology properties were investigated by considering the phasal change and orientation of LaCeTh0·1CuOy. The material was characterized using scanning electron microscopy (SEM), transition electron microscopy (TEM), and X-ray diffractometry (XRD). The structural formulations of the generated phases have a unique combination of phases that yields new electronic properties. It was observed through the surface and bulk scans that the LaCeTh0.1CuOy has approximately 72% homogeneity and about 28% heterogeneity. Copper, oxygen, and cerium were observed to influence the surface morphology of LaCeTh0·1CuOy. Hence, aside from the outer and inner CuO2 planes that possess four and five coordination numbers, it could be inferred that the ratio of structural impact of the inner and outer CuO2 planes in LaCeTh0.1CuOy is 5:1. This anomaly may be responsible for the unresolved mechanism in a few solid-state devices or compounds.

A study on the detection of bulging disease in ancient city walls based on fitted initial outer planes from 3D point cloud data

Bulging is a common disease suffered by ancient city walls, especially clay brick walls. Bulging affects or even threatens the stability of outer structures of ancient city walls. Therefore, accurate identification of bulges is one of the urgent issues to be addressed in ancient city wall conservation. In this study, a novel method is proposed for detecting and identifying bulge information using point cloud data collected from the outer surface of an ancient city wall. The non-bulging points are identified in the sliced point cloud of a city wall, and then the initial plane of the city wall is fitted more accurately with the aid of spatial constraints. Finally, the bulging damage is identified and extracted by comparing the initial plane with the original point cloud. This method was applied to the project of ancient city wall conservation and was compared with other existing methods in effectiveness and accuracy. The results show that the proposed method can detect efficiently budging disease in ancient city walls for architectural heritage conservation.

Magnetotransport signatures of antiferromagnetism coexisting with charge order in the trilayer cuprate HgBa2Ca2Cu3O8+\u03b4

Multilayered cuprates possess not only the highest superconducting temperature transition but also offer a unique platform to study disorder-free CuO2 planes and the interplay between competing orders with superconductivity. Here, we study the underdoped trilayer cuprate HgBa2Ca2Cu3O8+δ and we report quantum oscillation and Hall effect measurements in magnetic field up to 88 T. A careful analysis of the complex spectra of quantum oscillations strongly supports the coexistence of an antiferromagnetic order in the inner plane and a charge order in the outer planes. The presence of an ordered antiferromagnetic metallic state that extends deep in the superconducting phase is a key ingredient that supports magnetically mediated pairing interaction in cuprates.

Drastic reduction of thermal conductivity in hexagonal AX (A = Ga, In & Tl, X = S, Se & Te) monolayers due to alternative atomic configuration

Several two-dimensional chalcogenide materials have been in the limelight in the recent past for their promising thermoelectric properties. It is well established that the thermoelectric performance of materials improves on reducing the physical dimensionality of the system. Two-dimensional hexagonal chalcogen (S, Se and Te) bearing compounds of Ga, In and Tl have already been studied extensively in literature. But in those phases, the group-13 non-chalcogen atoms occupy the two inner planes while the chalcogens occupy the two outer planes of the unit cell. In this work, we have proposed the alternate arrangement in which the chalcogen atoms occupy the two inner planes while the group-13 atoms occupy the two outer planes of the unit cell. Unprecedentedly, this alternate arrangement shows much lower thermal conductivity that leads to superior thermoelectric performance. In this work we have studied in details the thermoelectric properties of hexagonal AX (A = Ga, In & Tl, X = S, Se & Te) monolayers and compare the results having both the atomic arrangements. The very low lattice thermal conductivity of this new arrangement is due to the outermost valence s-orbital lone pair of the chalcogens which leads to enhanced anharmonicity. We have explained these results from the anti-crossing of the phonon branches as well. The electronic, dynamical, thermodynamical and elastic properties have also been studied. We think that these results should have significant impact on the synthesis of high-performance thermoelectric materials based on chalcogenides of gallium, indium and thallium. • The position of the group 13 and chalcogen atoms in AX (A = Ga, In & Tl, X = S, Se & Te) have been flipped. • Ab initio calculations of thermal conductivity, electronic properties and mechanical properties have been determined. • The new configuration yields dynamically stable structures too with much lower elastic constants and Debye temperatures. • The high anharmonic scattering and weak bonds lead to ultralow thermal conductivity due to the lattice vibrations. • The ultralow thermal conductivity lead to extremely high values of thermoelectric figure of merit.

Rotating co-flow jets with horizontal lip and shape transition

Purpose Control over large-scale coherent structures and stream-wise vortices lead to enhanced entrainment/conservation of the jet which is desirable for most free jet applications such as design of combustion chamber in jet engines and flame length elongation of welding torch used for metal cutting. Design/methodology/approach A co-flow nozzle with lip thickness of 2 mm, between the primary (inner) and secondary (outer) flow, is selected. Three nozzle combinations are used, i.e. C–C (circle–circle), C–E (circle–ellipse) and C–S (circle–square) for acquiring comparative data. For these nozzle combinations, inner nozzle exit plane is kept as a circle, whereas the outer nozzle exit planes are varied to circle, ellipse and square. The exit plane area of outer nozzle for the nozzle combinations has equivalent diameter, De. The nozzles are fabricated in a way that the outer nozzle can be rotated along the longitudinal axis, keeping the inner nozzle intact. Findings The C–C nozzle combination is effective in low Mach number regime in decaying the jet, when the rotational component is introduced. Around 30% reduction in the jet core length is observed for the C–C nozzle combinations without any lip. The C–E nozzle shows sedative result in decaying or preserving the jet. The C–S nozzle combination shows interesting phenomenon, whereby the low subsonic case tends to conserve the jet by 15% and the higher subsonic case tends to decay the jet by 10%. Originality/value The developed nozzle systems show both conservative and destructive effect on the jet, which is desirable for the mentioned applications.

Vertical position of Sr dopants in the SrxBi2Se3 superconductor

The discovery of topological superconductivity in doped ${\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$ made this class of materials highly important for the field of condensed matter physics. However, the structural origin of the superconducting state remained elusive, despite being investigated intensively in recent years. We use scanning tunneling microscopy and the normal incidence x-ray standing wave (NIXSW) technique in order to determine the vertical position of the dopants---one of the key parameters for understanding topological superconductivity in this material--- for the case of ${\mathrm{Sr}}_{x}{\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$. In particular, we analyze the NIXSW data in consideration of the inelastic mean free path of the photoemitted electrons, which allows us to distinguish between symmetry-equivalent sites. We find that Sr atoms are not situated inside the van der Waals gap between the ${\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$ quintuple layers but rather in the quintuple layer close to the outer Se planes.

TIC 168789840: A Sextuply Eclipsing Sextuple Star System

Abstract We report the discovery of a sextuply eclipsing sextuple star system from TESS data, TIC 168789840, also known as TYC 7037-89-1, the first known sextuple system consisting of three eclipsing binaries. The target was observed in Sectors 4 and 5 during Cycle 1, with lightcurves extracted from TESS Full Frame Image data. It was also previously observed by the WASP survey and ASAS-SN. The system consists of three gravitationally bound eclipsing binaries in a hierarchical structure of an inner quadruple system with an outer binary subsystem. Follow-up observations from several different observatories were conducted as a means of determining additional parameters. The system was resolved by speckle interferometry with a 0.″42 separation between the inner quadruple and outer binary, inferring an estimated outer period of ∼2 kyr. It was determined that the fainter of the two resolved components is an 8.217 day eclipsing binary, which orbits the inner quadruple that contains two eclipsing binaries with periods of 1.570 days and 1.306 days. Markov Chain Monte Carlo (MCMC) analysis of the stellar parameters has shown that the three binaries of TIC 168789840 are “triplets,” as each binary is quite similar to the others in terms of mass, radius, and T eff. As a consequence of its rare composition, structure, and orientation, this object can provide important new insight into the formation, dynamics, and evolution of multiple star systems. Future observations could reveal if the intermediate and outer orbital planes are all aligned with the planes of the three inner eclipsing binaries.

Anomalous Doping Evolution of Superconductivity and Quasiparticle Interference in Bi_{2}Sr_{2}Ca_{2}Cu_{3}O_{10+δ} Trilayer Cuprates.

We use scanning tunneling microscopy to investigate Bi_{2}Sr_{2}Ca_{2}Cu_{3}O_{10+δ} trilayer cuprates from the optimally doped to overdoped regime. We find that the two distinct superconducting gaps from the inner and outer CuO_{2} planes both decrease rapidly with doping, in sharp contrast to the nearly constant T_{C}. Spectroscopic imaging reveals the absence of quasiparticle interference in the antinodal region of overdoped samples, showing an opposite trend to that in single- and double-layer compounds. We propose that the existence of two types of inequivalent CuO_{2} planes and the intricate interaction between them are responsible for these anomalies in trilayer cuprates.

A Miniaturized Butler Matrix Based Switched Beamforming Antenna System in a Two-Layer Hybrid Stackup Substrate for 5G Applications

This work presents a Butler matrix based four-directional switched beamforming antenna system realized in a two-layer hybrid stackup substrate for 28-GHz mm-Wave 5G wireless applications. The hybrid stackup substrate is composed of two layers with different electrical and thermal properties. It is formed by attaching two layers by using prepreg, in which the circuit components are placed in both outer planes and the ground layers are placed in the middle. The upper layer that is used as antenna substrate has εr = 2.17, tanδ = 0.0009 and h = 0.254 mm. The lower layer that is used as a Butler matrix substrate has εr = 6.15, tanδ = 0.0028 and h = 0.254 mm. By realizing the antenna array on the lower-εr layer while the Butler matrix on the higher-εr layer, the Butler matrix dimension is significantly reduced without sacrificing the array antenna performance, leading to significant overall antenna system size reduction. The two-layer substrate approach also significantly suppresses parasitic radiation leaking from the Butler matrix toward the antenna side, allowing overall radiation pattern improvement. The fabricated beamforming antenna is composed of 1 × 4 patch antenna array and a 4 × 4 Butler matrix. The measured return loss is lower than −8 dB at all ports in 28-GHz. It demonstrates the switched beam steering toward four distinct angles of—16°, +36°, −39°, and +7°, with the sidelobe levels of −12, −11.7, −6, and −13.8 dB, respectively. Antenna gain is found to be about 10 dBi. Due to the two-layer hybrid stackup substrate, the total antenna system is realized only in 1.7λ × 2.1λ, which shows the smallest form factor compared to similar other works.

Role of the inner copper oxide plane in interlayer Josephson effects in multilayered cuprate superconductors

We find systematic signatures suggesting a different superconducting nature for a triple-layered cuprate Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+\delta}$ with respect to a double-layer through the properties of intrinsic Josephson junctions (IJJs). Our measurements on the current-voltage characteristics reveal that the $c$-axis maximum Josephson current density is sensitive to the superfluid density in outer planes while the critical temperature and the superconducting gap remain unaffected. Switching dynamics of stacked IJJs exhibit that the fluctuation in gauge-invariant phase difference of an IJJ implies that the inner plane completely shields the capacitive coupling between adjacent IJJs, which is essential for mono- and bilayered cuprates.

(Invited) Nanoscale (XPEEM) Spectroscopy Unveils the Complex Local (Electro-) Chemical Surface Reactions of Cycled Electrodes in Li-Ion Batteries

Understanding the electrode-electrolyte interface evolution during cycling as well as the surface structural change of the active materials is crucial to improve the safety and the life-cycle of Li-ion batteries. Despite the large effort directed at elucidating the nature and origin of the surface reactivity of the electrodes in liquid organic electrolytes, there is still no complete knowledge of the various mechanisms that take place at such interfaces. The lack of agreement in the reported findings is caused mainly by the surface complexity of the commercial electrodes (multiple particles, high roughness and porosity) and by the intrinsic limitations of the commonly used surface characterization techniques, (mainly the poor lateral resolution). Thus, in this contribution the recent development on X-Ray Photoelectron Emission Spectroscopy (XPEEM) will be presented, as a surface analytical technique capable of providing local information on single particles of anode and cathode materials, while maintaining the complex formulation of composite electrodes. The unique combination of the nanoscale lateral resolution and the spectroscopic capability, confined to within the depth analysis range of 3-4 nm, enable us to provide the missing piece of the exact mechanism of the electrolyte-electrode interactions. Two commercially-relevant electrodes for Li-ion battery will be presented during the talk, namely Li4Ti5O12 (LTO) and the high-voltage cathode lithium rich Li1+x (NiaCobMn1-a-b)1-xO2 (Li-rich NCM) after cycling in the conventional liquid carbonate electrolytes. In the first system, the controversial surface reactivity of LTO when is cycled in carbonate-based electrolyte is resolved. Despite the theoretical prediction of a stable electrochemical interface, the electrolyte reduction is found to occurs solely on LTO particles during lithiation. With the support of density functional theory (DFT) calculations, we show that this behavior is caused by the solvents adsorbed on the LTO outer planes driven by the Li-ion insertion. The DFT calculation indicates that Li-ion insertion leads to a shift of the LUMO of the adsorbed solvents to energies below the Fermi level position of lithiated Li7Ti5O12 and thus to chemical instability.[1]In the second system, at the Li-rich NCM interface, two major parasitic reactions were identified at high potential. The first reaction is related to the electrolyte oxidation, whereas the second is associated with the Li-rich NCM surface degradation.[2] Those parasitic reactions are caused mainly by the oxidation of oxygen leading to the chemical oxidation of the electrolyte solvents and to the formation of a surface layer containing reduced transition metals (TMs).[3] The presence of electrolyte by-products and TMs "cross-talk" is also demonstrated between the cathode and the anode, creating on the latter a layer rich of micrometer-sized agglomerates of TMs. The impact of these parasitic reactions on the electrodes electrochemical cycling performance will be discussed. Finally, as a further development of the technique, operando XPEEM will be presented and discussed on all-solid-state batteries for the working electrode LiCoO2 mixed with (Li2S)3-P2S5 (LPS), used as a solid electrolyte. [1] D. Leanza, C. A. F. Vaz, I. Czekaj, P. Novák, M. El Kazzi, Journal of Material Chemistry A, 2018, 6, 3534–3542. [2] D. Leanza, C. A. F. Vaz, G. Melinte, X. Mu, P. Novák, M. El Kazzi, ACS Appl. Mater. Interfaces, 2019, 11, 6054−6065. [3] D. Leanza, M. Mirolo, C. A. F. Vaz, P. Novák, M. El Kazzi, Batteries & Supercaps, 2019, 2, 1-12.

3-Methyl-1-{(E)-[1-(4-methyl-pyridin-2-yl)ethyl-idene]amino}-thio-urea: crystal structure and Hirshfeld surface analysis.

The title disubstituted thio-urea derivative, C10H14N4S, features an almost planar imine (E configuration, C3N) core flanked by thio-urea (CN2S) and methyl-pyridyl (C5N) residues (each plane has a r.m.s. deviation of the respective fitted atoms of 0.0066 Å). The dihedral angles between the core and the thio-urea and pyridyl residues are 20.25 (8) and 7.60 (9)°, respectively, indicating twists in the mol-ecule; the dihedral angle between the outer planes is 13.62 (7)°. There is an anti-disposition of the amine-N-H atoms which allows for the formation of an intra-molecular amine-N-H⋯N(imine) hydrogen bond that closes an S(5) loop. In the crystal, amine-N-H⋯N(pyrid-yl) hydrogen bonds lead to zigzag (glide symmetry) supra-molecular chains along the c-axis direction. These are connected into a supra-molecular layer propagating in the bc plane by thio-amide-N-H⋯S(thione) hydrogen bonds via eight-membered thio-amide {⋯HNCS}2 synthons.

Solving the puzzle of Li4Ti5O12 surface reactivity in aprotic electrolytes in Li-ion batteries by nanoscale XPEEM spectromicroscopy

Preferential reduction of solvents solely on LTO particles, caused by their adsorption at the outer surface planes during lithiation.

Larger sized planar wire arrays of complex configuration on 1.5–1.8 MA Z-pinch generator

Two new approaches of (i) simultaneous study of implosion and radiative characteristics of different materials in wire array Z-pinch plasmas in one shot and (ii) investigation of larger sized wire arrays (to enhance energy coupling to plasmas and provide better diagnostic access) were developed in experiments with 1.5–1.8 MA Zebra with a Load Current Multiplier. In particular, the larger sized multi-plane Planar Wire Arrays with two outer planes placed at 9 and 15 mm from each other and then as far as at 19 mm (compared with 6 mm studied before at standard 1 MA current) and with a modified central plane with 8 to 12 empty slots were investigated. Though K-shell Al and L-shell Ni, Cu plasmas have similar electron temperatures and densities, the ablation dynamics and radiation of Al and Ni, Cu planes are somewhat different, which was investigated in detail using the full set of diagnostics and modeling. Advantages of using such wire arrays at higher currents to study plasma flow and radiation from different materials and jets are highlighted.

Novel Interplay between High-TcSuperconductivity and Antiferromagnetism in Tl-Based Six-CuO2-Layered Cuprates:205Tl- and63Cu-NMR Probes

We report $^{63}$Cu- and $^{205}$Tl-NMR studies on six-layered ($n$=6) high-$T_c$ superconducting (SC) cuprate TlBa$_2$Ca$_5$Cu$_6$O$_{14+\delta}$ (Tl1256) with $T_c\sim$100 K, which reveal that antiferromagnetic (AFM) order takes place below $T_{\rm N}\sim$170 K. In this compound, four underdoped inner CuO$_2$ planes ($n$(IP)=4) sandwiched by two outer planes (OPs) are responsible for the onset of AFM order, whereas the nearly optimally-doped OPs responsible for the onset of bulk SC. It is pointed out that an increase in the out-of-plane magnetic interaction within an intra-unit-cell causes $T_{\rm N}\sim$ 45 K for Tl1245 with $n$(IP)=3 to increase to $\sim$170 K for Tl1256 with $n$(IP)=4. It is remarkable that the marked increase in $T_{\rm N}$ and the AFM moments for the IPs does not bring about any reduction in $T_c$, since $T_c\sim 100$ K is maintained for both compounds with nearly optimally doped OP. We highlight the fact that the SC order for $n\ge5$ is mostly dominated by the long-range in-plane SC correlation even in the multilayered structure, which is insensitive to the magnitude of $T_{\rm N}$ and the AFM moments at the IPs or the AFM interaction among the IPs. These results demonstrate a novel interplay between the SC and AFM orders when the charge imbalance between the IPs and OP is significantly large.