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Molecular beam deposition of a new layered pnictide with distorted Sb square nets

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 Added by Masaki Uchida
 Publication date 2021
  fields Physics
and research's language is English




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While the family of layered pnictides $ABX_2$ ($A$ : rare or alkaline earth metals, $B$ : transition metals, $X$ : Sb/Bi) can host Dirac dispersions based on Sb/Bi square nets, nearly half of them has not been synthesized yet for possible combinations of the $A$ and $B$ cations. Here we report the fabrication of EuCdSb$_{mathrm{2}}$ with the largest $B$-site ionic radius, which is stabilized for the first time in thin film form by molecular beam deposition. EuCdSb$_{mathrm{2}}$ crystallizes in an orthorhombic $Pnma$ structure and exhibits antiferromagnetic ordering of the Eu magnetic moments at $T_mathrm{N}=15$K. Our successful growth will be an important step for further exploring novel Dirac materials using film techniques.



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Dirac states hosted by Sb/Bi square nets are known to exist in the layered antiferromagnetic AMnX$_2$ (A = Ca/Sr/Ba/Eu/Yb, X=Sb/Bi) material family the space group to be P4/nmm or I4/mmm. In this paper, we present a comprehensive study of quantum transport behaviors, angle-resolved photoemission spectroscopy (ARPES) and first-principles calculations on SrZnSb2, a nonmagnetic analogue to AMnX2, which crystallizes in the pnma space group with distorted square nets. From the quantum oscillation measurements up to 35 T, three major frequencies including F$_1$ = 103 T, F$_2$ = 127 T and F$_3$ = 160 T, are identified. The effective masses of the quasiparticles associated with these frequencies are extracted, namely, m*$_1$ = 0.1 m$_e$, m*$_2$ = 0.1 m$_e$ and m*$_3$ = 0.09m$_e$, where m$_e$ is the free electron mass. From the three-band Lifshitz-Kosevich fit, the Berry phases accumulated along the cyclotron orbit of the quasiparticles are 0.06$pi$, 1.2$pi$ and 0.74$pi$ for F$_1$, F$_2$ and F$_3$, respectively. Combined with the ARPES data and the first-principles calculations, we reveal that F2 and F3 are associated with the two nontrivial Fermi pockets at the Brillouin zone edge while F1 is associated with the trivial Fermi pocket at the zone center. In addition, the first-principles calculations further suggest the existence of Dirac nodal line in the band structure of SrZnSb$_2$.
Dedicated control of oxygen vacancies is an important route to functionalizing complex oxide films. It is well-known that tensile strain significantly lowers the oxygen vacancy formation energy, whereas compressive strain plays a minor role. Thus, atomically reconstruction by extracting oxygen from a compressive-strained film is challenging. Here we report an unexpected LaCoO2.5 phase with a zigzag-like oxygen vacancy ordering through annealing a compressive-strained LaCoO3 in vacuum. The synergetic tilt and distortion of CoO5 square pyramids with large La and Co shifts are quantified using scanning transmission electron microscopy. The large in-plane expansion of CoO5 square pyramids weaken the crystal-field splitting and facilitated the ordered high-spin state of Co2+, which produces an insulating ferromagnetic state with a Curie temperature of ~284 K and a saturation magnetization of ~0.25 {mu}B/Co. These results demonstrate that extracting targeted oxygen from a compressive-strained oxide provides an opportunity for creating unexpected crystal structures and novel functionalities.
Using first-principles calculations, we identify the origin of the observed charge density wave (CDW) formation in a layered kagome metal CsV$_3$Sb$_5$. It is revealed that the structural distortion of kagome lattice forming the trimeric and hexameric V atoms is accompanied by the stabilization of quasimolecular states, which gives rise to the opening of CDW gaps for the V-derived multibands lying around the Fermi level. This Jahn-Teller-like instability having the local lattice distortion and its derived quasimolecular states is a driving force of the CDW order. Specifically, the saddle points of multiple Dirac bands near the Fermi level, located at the $M$ point, are hybridized to disappear along the $k_z$ direction, therefore not supporting the widely accepted Peierls-like electronic instability due to Fermi surface nesting. It is further demonstrated that applied hydrostatic pressure significantly reduces the interlayer spacing to destabilize the quasimolecular states, leading to a disappearance of the CDW phase at a pressure of ${sim}$2 GPa. The presently proposed underlying mechanism of the CDW order in CsV$_3$Sb$_5$ can also be applicable to other isostructural kagome lattices such as KV$_3$Sb$_5$ and RbV$_3$Sb$_5$.
260 - K. Zhao , Z. Deng , X. C. Wang 2013
Diluted magnetic semiconductors (DMS) have received much attention due to its potential applications to spintronics devices. A prototypical system (Ga,Mn)As has been widely studied since 1990s. The simultaneous spin and charge doping via hetero-valence (Ga3+,Mn2+) substitution, however, resulted in severely limited solubility without availability of bulk specimens. Previously we synthesized a new diluted ferromagnetic semiconductor of bulk Li(Zn,Mn)As with Tc up to 50K, where isovalent (Zn,Mn) spin doping was separated from charge control via Li concentrations. Here we report the synthesis of a new diluted ferromagnetic semiconductor (Ba1-xKx)(Zn1-yMny)2As2, isostructural to iron 122 system, where holes are doped via (Ba2+, K1+), while spins via (Zn2+,Mn2+) substitutions. Bulk samples with x=0.1-0.3 and y=0.05-0.15 exhibit ferromagnetic order with TC up to 180K, comparable to that of record high Tc for Ga(MnAs), significantly enhanced than Li(Zn,Mn)As. Moreover the (Ba,K)(Zn,Mn)2As2 shares the same 122 crystal structure with semiconducting BaZn2As2, antiferromagnetic BaMn2As2, and superconducting (Ba,K)Fe2As2, which makes them promising to the development of multilayer functional devices.
Compositionally tunable vanadium oxyhydrides Sr2VO4-xHx (x = 0 - 1) without considerable anion vacancy were synthesized by high-pressure solid state reaction. The crystal structures and their properties were characterized by powder neutron diffraction, synchrotron X-ray diffraction, thermal desorption spectroscopy, and first-principles density functional theory (DFT) calculations. The hydrogen anions selectively replaced equatorial oxygen sites in the VO6 layers via statistical substitution of hydrogen in the low x region (x < 0.2). A new orthorhombic phase (Immm) with an almost entirely hydrogen-ordered structure formed from the K2NiF4-type tetragonal phase with x > 0.7. Based on the DFT calculations, the degree of oxygen/hydrogen anion ordering is strongly correlated with the bonding interaction between vanadium and the ligands.
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