arXiv subjects

Junyi Zhu

Publications and source records attributed to Junyi Zhu.

At least 55 records · Page 3Linked to original sources

arXiv2019

Intrinsic long range antiferromagnetic coupling in dilutely V doped CuInTe$_2$

Despite the various magnetic orders mediated by superexchange mechanism, the existence of a long range antiferromagnetic (AFM) coupling is unknown. Based on DFT calculations, we discovered an intrinsic long range AFM coupling in V doped CuInTe$_2$. The AFM coupling is mainly due to the $p-d$ coupling and electron redistribution along the interacting chains. The relatively small energy difference between $p$ and $d$ orbitals and the small energy difference between d orbitals of the dopants and that of stepping stone sites can enhance the stability of this AFM configuration. A multi-bands Hubbard model was proposed to provide fundamental understanding to the long range AFM coupling in chalcopyrite diluted magnetic semiconductors(DMS).

cond-mat.mtrl-sci↗

arXiv2019

Towards understanding the special stability of ${\text{SrCo}\text{O}_{2.5}}$ and ${\text{HSrCo}\text{O}_{2.5}}$

Reversible hydrogen incorporation was recently attested [N. Lu, $\textit{et al.}$, Nature $\textbf{546}$, 124 (2017)] in ${\text{SrCo}\text{O}_{2.5}}$, the brownmillerite phase (BM) of strontium cobalt oxide (SCO), opening new avenues in catalysis and energy applications. However, existing theoretical studies of BM-SCO are insufficient, and that of ${\text{HSrCo}\text{O}_{2.5}}$, the newly-reported hydrogenated SCO (H-SCO), is especially scarce. In this work, we demonstrate how the electron-counting model (ECM) can be used in understanding the phases, particularly in explaining the stability of the oxygen-vacancy channels (OVCs), and in examining the Co valance problem. Using density-functional theoretical (DFT) methods, we analyze the crystalline, electronic, and magnetic structures of BM- and H-SCO. Based on our structure search, we discovered stable phases with large bandgaps (> 1 eV) for both BM-SCO and H-SCO, agreeing better with experiments on the electronic structures. Our calculations also indicate limited charge transfer from H to O that may explain the special stability of the H-SCO phase and the reversibility of H incorporation observed in experiments. In contrary to the initial study, our calculation also suggests intrinsic antiferromagnetism (AFM) of H-SCO, showing how the measured ferromagnetism (FM) has possible roots in hole doping.

cond-mat.mtrl-sci↗

arXiv2018

A protonated brownmillerite electrolyte for superior low-temperature proton conductivity

Design novel solid oxide electrolyte with enhanced ionic conductivity forms one of the Holy Grails in the field of materials science due to its great potential for wide range of energy applications. Conventional solid oxide electrolyte typically requires elevated temperature to activate the ionic transportation, while it has been increasing research interests to reduce the operating temperature due to the associated scientific and technological importance. Here, we report a conceptually new solid oxide electrolyte, HSrCoO2.5, which shows an exceptional enhanced proton conductivity at low temperature region (from room temperature to 140 oC). Combining both the experimental results and corresponding first-principles calculations, we attribute these intriguing properties to the extremely-high proton concentration as well as the well-ordered oxygen vacancy channels inherited from the novel crystalline structure of HSrCoO2.5. This result provides a new strategy to design novel solid oxide electrolyte with excellent proton conductivity for wide ranges of energy-related applications.

cond-mat.mtrl-sci↗

arXiv2018

Quasicrystalline 30° Twisted Bilayer Graphene as an Incommensurate Superlattice with Strong Interlayer Coupling

The interlayer coupling can be used to engineer the electronic structure of van der Waals heterostructures (superlattices) to obtain properties that are not possible in a single material. So far research in heterostructures has been focused on commensurate superlattices with a long-ranged Moiré period. Incommensurate heterostructures with rotational symmetry but not translational symmetry (in analogy to quasicrystals) are not only rare in nature, but also the interlayer interaction has often been assumed to be negligible due to the lack of phase coherence. Here we report the successful growth of quasicrystalline 30° twisted bilayer graphene (30°-tBLG) which is stabilized by the Pt(111) substrate, and reveal its electronic structure. The 30°-tBLG is confirmed by low energy electron diffraction and the intervalley double-resonance Raman mode at 1383 cm$^{-1}$. Moreover, the emergence of mirrored Dirac cones inside the Brillouin zone of each graphene layer and a gap opening at the zone boundary suggest that these two graphene layers are coupled via a generalized Umklapp scattering mechanism, i.e. scattering of Dirac cone in one graphene layer by the reciprocal lattice vector of the other graphene layer. Our work highlights the important role of interlayer coupling in incommensurate quasicrystalline superlattices, thereby extending band structure engineering to incommensurate superstructures.

cond-mat.mtrl-sci↗

arXiv2018

Missing links towards understanding equilibrium shapes of hexagonal boron nitride: algorithm, hydrogen passivation, and temperature effects

There is a large discrepancy between the experimental observations and the theoretical predictions in the morphology of hexagonal boron nitride (h-BN) nanosheets. Theoretically-predicted hexagons terminated by armchair edges are not observed in experiments; and experimentally-observed triangles terminated by zigzag edges are found theoretically unstable. There are two key issues in theoretical investigations, namely, an efficient and accurate algorithm of absolute formation energy of h-BN edges, and a good understanding of the role of hydrogen passivation during h-BN growth. Here, we first proposed an efficient algorithm to calculate asymmetric edges with a self-consistent accuracy of about 0.0014 eV/Å. This method can also potentially serve as a standard approach for other two-dimensional (2D) compound materials. Then, by using this method, we discovered that only when edges are passivated by hydrogen atoms and temperature effects are taken into account can experimental morphology be explained. We further employed Wulff construction to obtain the equilibrium shapes of H-passivated h-BN nanosheets under its typical growth conditions at T = 1300 K and p = 1 bar, and found out that the equilibrium shapes are sensitive to hydrogen passivation and the growth conditions. Our results resolved long-standing discrepancies between experimental observations and theoretical analysis, explaining the thermodynamic driving force of the triangular, truncated triangular, and hexagonal shapes, and revealing the key role of hydrogen in h-BN growth. These discoveries and the advancement in algorithm may open the gateway towards the realization of 2D electronic and spintronic devices based on h-BN.

cond-mat.mtrl-sci↗

arXiv2018

Stability of wurtzite semi-polar surfaces: algorithms and practices

A complete knowledge of absolute surface energies with any arbitrary crystal orientation is important for the improvements of semiconductor devices because it determines the equilibrium and nonequilibrium crystal shapes of thin films and nanostructures. It is also crucial in the control of thin film crystal growth and surface effect studies in broad research fields. However, obtaining accurate absolute formation energies is still a huge challenge for the semi-polar surfaces of compound semiconductors. It mainly results from the asymmetry nature of crystal structures and the complicated step morphologies and related reconstructions of these surface configurations. Here we propose a general approach to calculate the absolute formation energies of wurtzite semi-polar surfaces by first-principles calculations, taking GaN as an example. We mainly focused on two commonly seen sets of semi-polar surfaces: a-family (11-2X) and m-family (10-1X). For all the semi-polar surfaces that we have calculated in this paper, the self-consistent accuracy is within 1.5 meV/Å^2. Our work fills the last technical gap to fully investigate and understand the shape and morphology of compound semiconductors.

cond-mat.mtrl-sci↗

arXiv2018

Gate-tunable Room-temperature Ferromagnetism in Two-dimensional Fe$_3$GeTe$_2$

Material research has been a major driving force in the development of modern nano-electronic devices. In particular, research in magnetic thin films has revolutionized the development of spintronic devices; identifying new magnetic materials is key to better device performance and new device paradigm. The advent of two-dimensional van der Waals crystals creates new possibilities. This family of materials retain their chemical stability and structural integrity down to monolayers and, being atomically thin, are readily tuned by various kinds of gate modulation. Recent experiments have demonstrated that it is possible to obtain two-dimensional ferromagnetic order in insulating Cr$_2$Ge$_2$Te$_6$ and CrI$_3$ at low temperatures. Here, we developed a new device fabrication technique, and successfully isolated monolayers from layered metallic magnet Fe$_3$GeTe$_2$ for magnetotransport study. We found that the itinerant ferromagnetism persists in Fe$_3$GeTe$_2$ down to monolayer with an out-of-plane magnetocrystalline anisotropy. The ferromagnetic transition temperature, $T_c$, is suppressed in pristine Fe$_3$GeTe$_2$ thin flakes. An ionic gate, however, dramatically raises the $T_c$ up to room temperature, significantly higher than the bulk $T_c$ of 205 Kelvin. The gate-tunable room-temperature ferromagnetism in two-dimensional Fe$_3$GeTe$_2$ opens up opportunities for potential voltage-controlled magnetoelectronics based on atomically thin van der Waals crystals.

cond-mat.mtrl-sci↗

arXiv2018

Long Range Magnetic order stabilized by acceptors

Tuning magnetic order in magnetic semiconductors is a long sought goal. A proper concentration of acceptors can dramatically suppress local magnetic order in favor of the long one. Using Mn and an acceptor codoped LiZnAs as an example, we demonstrate, by first-principles calculation, the emergence of a long-range magnetic order. This intriguing phenomenon can be understood from an interplay between an acceptor-free magnetism and a band coupling magnetism. Our observation thus lays the ground for a precise control of the magnetic order in future spintronic devices.

cond-mat.mtrl-sci↗

arXiv2018

Kuznetsov-Ma solution and Akhmediev breather for TD equation

We present the inverse scattering transform for the TD equation, which is related to the Heisenberg spin equation. We note that the TD equation is an integrable model with high nonlinearity, and has singularity at zero. Thus a nonzero boundary condition is introduced in the direct scattering problem. We obtain the $N$-solitonic solution of the TD equation, and give the Kuznetsov-Ma type solution, rational solution and Akhmediev type breather.

nlin.SI↗

arXiv2017

Hydrogen Surfactant Assisted Coherent Growth of GaN on ZnO Substrate

Heterostructures of wurtzite based devices have attracted great research interests since the tremendous success of GaN in light emitting diodes (LED) industry. Among the possible heterostructure material candidates, high quality GaN thin films on inexpensive and lattice matched ZnO substrate are both commercially and technologically desirable. However, the energy of ZnO polar surfaces is much lower than that of GaN polar surfaces. Therefore, the intrinsic wetting condition forbids such heterostructures. As a result, poor crystal quality and 3D growth mode were obtained. To dramatically change the growth mode of the heterostructure, we propose to use hydrogen as a surfactant, confirmed by our first principles calculations. Stable H involved surface configurations and interfaces are investigated, with the help of newly developed algorithms. By applying the experimental Gibbs free energy of H$_2$, we also predict the temperature and chemical potential of H, which is critical in experimental realizations of our strategy. This novel approach will for the first time make the growth of high quality GaN thin films on ZnO substrates possible. We believe that our new strategy may reduce the manufactory cost and improve the crystal quality and the efficiency of GaN based devices.

cond-mat.mtrl-sci↗

arXiv2017

Defect Properties of Na and K in Cu2ZnSnS4 from Hybrid Functional Calculation

In-growth or post-deposition treatment of $Cu_{2}ZnSnS_{4}$ (CZTS) absorber layer had led to improved photovoltaic efficiency, however, the underlying physical mechanism of such improvements are less studied. In this study, the thermodynamics of Na and K related defects in CZTS are investigated from first principle approach using hybrid functional, with chemical potential of Na and K established from various phases of their polysulphides. Both Na and K predominantly substitute on Cu sites similar to their behavior in $Cu(In,Ga)Se_{2}$, in contrast to previous results using the generalized gradient approximation (GGA). All substitutional and interstitial defects are shown to be either shallow levels or highly energetically unfavorable. Defect complexing between Na and abundant intrinsic defects did not show possibility of significant incorporation enhancement or introducing deep n-type levels. The possible benefit of Na incorporation on enhancing photovoltaic efficiency is discussed. The negligible defect solubility of K in CZTS also suggests possible surfactant candidate.

cond-mat.mtrl-sci↗

arXiv2017

A novel strategy to control defects and secondary phases of CZTS by surfactant Potassium

Cu2ZnSnS4 (CZTS) is a promising photovoltaic absorber material with earth abundant and nontoxic elements. However, the detrimental native defects and secondary phases of CSTS will largely reduce the energy conversion efficiencies. To understand the origin of these problems during the growth of CZTS, we investigated the kinetic processes on CZTS (-1-1-2) surface, using first principles calculations. A surface Zn atom was found to occupy the subsurface Cu site easily due to a low reaction barrier, which may lead to a high ZnCu concentration and a secondary phase of ZnS. These n-type defects may create deep electron traps near the interface and become detrimental to device performance. To reduce the population of ZnCu and the secondary phase, we propose to use K as a surfactant to alter surface kinetic processes. Improvements on crystal quality and device performance based on this surfactant are consistent with early experimental observations.

cond-mat.mtrl-sci↗

arXiv2017

Line-soliton and rational solutions to (2+1)-dimensional Boussinesq equation by Dbar-problem

We present a generalized (2+1)-dimensional Boussinesq equation, including two cases which are called the plus Boussinesq equation and the minus one. To investigate these equations, we apply the $\bar{\partial}$ approach to a coupled (2+1)-dimensional nonlinear equation, which reduces to the Boussinesq equation. For the plus equation, we give the line-solitons and rational solutions, for the minus one, we give some freak solutions.

nlin.SI↗

arXiv2017

Step Stone Effect: A sp anti-bonding Mediated Long-Range Ferromagnetism in Cr-doped Carrier-Free Bi2Te3

Despite the recent success in the realization of the quantum anomalous Hall effect, the underlying physical mechanism of the long range Ferromagnetism is still unclear. Based on our density functional theory calculations, we discovered an intriguing long-range ferromagnetic order in Cr-doped, carrier-free Bi2Te3, with the separation between dopants more than 8 Å. We found that this magnetic coupling is facilitated by an anti-bonding state originated from the lone pair of a Te 5p state and a Bi 6s state, despite this anti-bonding state lies below the valence band maximum. Such a state serves as a hidden step stone merged in the electron sea and mediates the long-range magnetic order. An effective electron hopping model is proposed to explain this mechanism. This novel mechanism sheds light on the understanding of long-range ferromagnetism in insulators and may lead to the realization of the long-range magnetic order in dilute magnetic semiconductors.

cond-mat.mtrl-sci↗

arXiv2016

Surfactant Antimony enhanced Indium incorporation on InGaN (000-1) surface: a DFT study

InGaN is an ideal alloy system for optoelectronic devices due its tunable band gap. Yet high-quality InGaN requires high In concentration, which is a challenging issue that limits its use in green-light LEDs and other devices. In this paper, we investigated the surfactant effect of Sb on the In incorporation on InGaN (000-1) surface via first-principles approaches. Surface phase diagram was also constructed to determine surface structures under different growth conditions. By analyzing surface stress under different structures, we found that Sb adatom can induce tensile sites in the cation layer, enhancing the In incorporation. These fi ndings may provide fundamental understandings and guidelines for the growth of InGaN with high In concentration.

cond-mat.mtrl-sci↗

arXiv2015

Induced effects by the substitution of Zn in Cu2ZnSnX4 (X = S and Se)

Based on the density functional theory with hybrid functional approach, we have studied the structural and thermodynamic stabilities of Cu2MSnX4 (M = Zn, Mg, and Ca; X = S and Se) alloy, and have further investigated the electronic and optical properties of stable Cu2MgSnS4 and Cu2MgSnSe4 phases. Thermal stability analysis indicates that Cu2MgSnS4 and Cu2MgSnSe4 are thermodynamically stable, while Cu2CaSnS4 and Cu2CaSnSe4 are unstable. The ground state configuration of the compound changes from kesterite into stannite structure when Zn atoms are substitued by larger Mg or Ca atoms. An energy separation between stannite and kesterite phase similar to that of CZTS is observed. Calculated electronic structures and optical properties suggest that Cu2MgSnS4 and Cu2MgSnSe4 can be efficient photovoltaic materials.

cond-mat.mtrl-sci↗

arXiv2015

Realization of Stable Ferromagnetic Order in Topological Insulator: Codoping Enhanced Magnetism in 4f Transition Metal Doped Bi2Se3

The realization of long range and insulating ferromagnetic states in topological insulator (TI) has been a pressing issue since its discovery. Only recently, such state was achieved in Cr-doped Bi2-xSbxTe3, leading to the discovery of quantum anomalous Hall effect (QAHE). However, the effect is only observed at extremely low temperatures mainly due to the limited magnetism. To fully understand the mechanism of the ferromagnetic ordering whereby improving the ferromagnetism, we investigated 4f transition metal-doped Bi2Se3, using density-functional-theory approaches. We found that Eu and Sm prefer the Bi substitutional sites with large magnetic moments to ensure stable long-range ferromagnetic states. Additionally, codoping can be a novel strategy to preserve the insulating property of the host material as well as improving the incorporation of magnetic dopants. Our findings thus offer the critical step in facilitating the realization of QAHE in TI systems.

cond-mat.mtrl-sci↗

arXiv2015

Surface energy calculations from Zinc blende (111)/(-1-1-1) to Wurtzite (0001)/(000-1):a study of ZnO and GaN

The accurate absolute surface energies of (0001)/(000-1) surfaces of wurtzite structures are crucial in determining the thin film growth mode of important energy materials. However, the surface energies still remain to be solved due to the intrinsic difficulty of calculating dangling bond energy of asymmetrically bonded surface atoms. In this study, we used a pseudo-hydrogen passivation method to estimate the dangling bond energy and calculate the polar surfaces of ZnO and GaN. The calculations were based on the pseudo chemical potentials obtained from a set of tetrahedral clusters or simple pseudo-molecules, using density functional theory approaches. And the surface energies of (0001)/(000-1) surfaces of wurtzite ZnO and GaN we obtained showed relatively high self-consistencies. A wedge structure calculation with a new bottom surface passivation scheme of group I and group VII elements was also proposed and performed to show converged absolute surface energy of wurtzite ZnO polar surfaces, and the result were also compared with the above method. These calculations and comparisons may provide important insights to crystal growths of the above materials, thereby leading to significant performance enhancements of semiconductor devices.

cond-mat.mtrl-sci↗