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Liang Si

Publications and source records attributed to Liang Si.

At least 37 records · Page 2Linked to original sources
arXiv2024

Boosting the transparency of metallic SrNbO3 through Ti doping

In recent years, various materials have been developed to reduce the reliance of industries on Indium, a primary component of transparent conducting oxides (TCOs) used in the current generation of devices. The leading candidates for indium free TCOs are strontium vanadates, niobates and molybdates -- strongly correlated perovskite systems that exhibit high intrinsic electrical conductivity and optimal transparency. In this work, we focus on the strontium niobate thin films and manipulate its optical conductivity by Ti doping, which shifts the plasma frequency and reduces electronic correlations. This allows us to achieve a low resistance for Ti doped SNO thin films, while maintaining a high transparency in the visible spectrum. We obtain the optimal figure-of-merit (FOM) of 10.3 ($10^{-3}Ω^{-1}$) for $x = 0.3$. This FOM significantly outperforms the optoelectronic capabilities of Tin-doped Indium oxide (ITO) and several other proposed transparent conductor materials. Our research paves the way for designing the next generation of transparent conductors, guided by insights from density-functional theory (DFT) and dynamical mean-field theory (DMFT).

cond-mat.mtrl-sci↗
arXiv2024

Evolution of the Coulomb interactions in correlated transition-metal perovskite oxides from the constrained random phase approximation

Determining the strength of electronic correlations of correlated electrons plays important roles in accurately describing the electronic structures and physical properties of transition-metal (TM) perovskite oxides. Here, we study the evolution of electronic interaction parameters as a function of $d$-electron occupancy in an extended class of TM perovskite oxides $AB$O$_3$ ($A$=Sr, Ca, and $B$=3$d$-5$d$ TM elements) using the constrained random-phase-approximation method adopting two distinct models: $t_{2g}$-$t_{2g}$ and $d$-$dp$. For Sr$B$O$_3$ with $B$=Fe, Ru, and Ir, the $t_{2g}$-$t_{2g}$ model faces critical challenges, as the low-energy Hamiltonian spanning $t_{2g}$ manifolds is ill-defined. The $t_{2g}$-$t_{2g}$ model suggests that, for early $AB$O$_3$ series ($B$=$d^1$-$d^3$), the bare Coulomb interaction parameters $V$ remain nearly constant due to the competition between extended $t_{2g}$ Wannier orbitals and bandwidth reduction. As the $d$-electron filling increases, both partially screened Coulomb interaction parameters $U$ and fully screened Coulomb interaction parameters $W$ decrease, which are attributed to enhanced $e_g$-$t_{2g}$ and $e_g$-$p$ screenings. In contrast to the $t_{2g}$-$t_{2g}$ model, the $d$-$dp$ model effectively handles both early and late $AB$O$_3$ perovskites and reveals different trends. Specifically, $V$ varies inversely with the spreads of $d$-orbitals. $W$ reaches its minimum at the $d^3$ occupancy due to an interplay between increasing $d$-orbital localization and increasing screening effects. An unusual trend is observed for $U$, with local maxima at both $d^1$ and $d^4$ occupations. This can be understood from two aspects: (1) the increasing full screening effects from $d^1$ to $d^3$ and (2) the strongest $d$-$d$ and the weakest $d$-$p$ screening effects near $d^4$ for Sr$B$O$_3$.

cond-mat.mtrl-sci↗
arXiv2024

Impact of rotational symmetry breaking on $d$-wave superconductivity in Hubbard models for cuprate and nickelate superconductors

Recent experiments have revealed the substantial impact of broken rotational symmetry on the superconductivity. In the pursuit of understanding the role played by this symmetry breaking particularly in cuprate and nickelate superconductors on their superconductivity, we investigated two characteristic symmetry breaking mechanisms arising from (1) structurally orthogonal distortions from $C_4$ to $C_2$ symmetry and (2) anisotropic hybridization between $d_{x^2-y^2}$ orbital and an additional metallic band within the framework of the Hubbard model by employing dynamic cluster quantum Monte Carlo calculations. We discovered that the anisotropy is generically detrimental to the $d$-wave pairing so that the experimental findings of much lower superconducting $T_c$ of infinite-layer nickelates compared with the cuprates may be connected to the intrinsic anisotropy. Our exploration sheds light on the fundamental anisotropy factors governing superconductivity in nickelates and cuprates and offer insights contributing to the broader understanding of unconventional superconductors in anisotropic environment.

cond-mat.supr-con↗
arXiv2023

Spin fluctuations sufficient to mediate superconductivity in nickelates

Infinite-layer nickelates show high-temperature superconductivity, and the experimental phase diagram agrees well with the one simulated within the dynamical vertex approximation (D$Γ$A). Here, we compare the spin-fluctuation spectrum behind these calculations to resonant inelastic X-ray scattering experiments. The overall agreement is good. This independent cross-validation of the strength of spin fluctuations strongly supports the scenario, advanced by D$Γ$A, that spin-fluctuations are the mediator of the superconductivity observed in nickelates.

cond-mat.supr-con↗
arXiv2023

Strain mediated phase crossover in Ruddlesden Popper nickelates

Recent progress on the signatures of pressure-induced high temperature superconductivity in Ruddlesden Popper (RP) nickelates (Lan+1NinO3n+1) has attracted growing interest in both theoretical calculations and experimental efforts. The fabrication of high-quality single crystalline RP nickelate thin films is critical for possible reducing the superconducting transition pressure and advancing applications in microelectronics in the future. In this study, we report the observations of an active phase transition in RP nickelate films induced by misfit strain. We found that RP nickelate films favor the perovskite structure (n = infinite) under tensile strains, while compressive strains stabilize the La3Ni2O7 (n = 2) phase. The selection of distinct phases is governed by the strain dependent formation energy and electronic configuration. In compressively strained La3Ni2O7, we experimentally determined splitting energy is ~0.2 eV and electrons prefer to occupy in-plane orbitals. First principles calculations unveil a robust coupling between strain effects and the valence state of Ni ions in RP nickelates, suggesting a dual driving force for the inevitable phase co-existence transition in RP nickelates. Our work underscores the sensitivity of RP nickelate formation to epitaxial strain, presenting a significant challenge in fabricating pure-phase RP nickelate films. Therefore, special attention to stacking defects and grain boundaries between different RP phases is essential when discussing the pressure-induced superconductivity in RP nickelates.

cond-mat.supr-con↗
arXiv2023

Unconventional superconductivity without doping: infinite-layer nickelates under pressure

High-temperature unconventional superconductivity quite generically emerges from doping a strongly correlated parent compound, often (close to) an antiferromagnetic insulator. The recently developed dynamical vertex approximation is a state-of-the-art technique that has quantitatively predicted the superconducting dome of nickelates. Here, we apply it to study the effect of pressure in the infinite-layer nickelate Sr$_x$Pr$_ {1-x}$NiO$_2$. We reproduce the increase of the critical temperature ($T_c$) under pressure found in experiment up to 12 GPa. According to our results, $T_c$ can be further increased with higher pressures. Even without Sr-doping the parent compound, PrNiO$_2$, will become a high-temperature superconductor thanks to a strongly enhanced self-doping of the \nidxsqysq{} orbital under pressure. With a maximal \Tc{} of 100\,K around 100\,GPa, nickelate superconductors can reach that of the best cuprates.

cond-mat.supr-con↗
arXiv2023

No superconductivity in Pb$_9$Cu$_1$(PO$_4$)$_6$O found in orbital and spin fluctuation exchange calculations

Finding a material that turns superconducting under ambient conditions has been the goal of over a century of research, and recently Pb$_{10-x}$Cu$_x$(PO$_4$)$_6$O aka LK-99 has been put forward as a possible contestant. In this work, we study the possibility of electronically driven superconductivity in LK-99 also allowing for electron or hole doping. We use an $\textit{ab initio}$ derived two-band model of the Cu $e_g$ orbitals for which we determine interaction values from the constrained random phase approximation (cRPA). For this two-band model we perform calculations in the fluctuation exchange (FLEX) approach to assess the strength of orbital and spin fluctuations. We scan over a broad range of parameters and enforce no magnetic or orbital symmetry breaking. Even under optimized conditions for superconductivity, spin and orbital fluctuations turn out to be too weak for superconductivity anywhere near to room-temperature. We contrast this finding to non-self-consistent RPA, where it is possible to induce spin-singlet $d$-wave superconductivity at $T_{\mathrm{c}}\geq300$ K if the system is put close enough to a magnetic instability.

cond-mat.supr-con↗
arXiv2023

Weyl points and spin-orbit coupling in copper-substituted lead phosphate apatite

We study the impact of spin-orbit coupling on the topological band-properties of copper-substituted lead phosphate apatite using a combination of group-theoretical analysis and full-relativistic density-functional theory calculations. We characterize Weyl points at time-reversal invariant momenta and find that a band-inversion due to spin-orbit coupling leads to additional Weyl points close to the Fermi-edge at general momenta. To determine the position of the altogether 66 Weyl points in the Brilouin-zone, we develop an algorithm that follows a Berry-curvature-derived vector field to its monopole: the Weyl point. The emerging surface Fermi-arcs and their spin-polarization reveal avoided crossings and a Fermi-loop detached from the Weyl points.

cond-mat.mes-hall↗
arXiv2023

Super-tetragonal Sr4Al2O7: a versatile sacrificial layer for high-integrity freestanding oxide membranes

Releasing the epitaxial oxide heterostructures from substrate constraints leads to the emergence of various correlated electronic phases and paves the way for integrations with advanced semiconductor technologies. Identifying a suitable water-soluble sacrificial layer, compatible with the high-quality epitaxial growth of oxide heterostructures, is currently the key to the development of large-scale freestanding oxide membranes. In this study, we unveil the super-tetragonal Sr4Al2O7 (SAOT) as a promising water-soluble sacrificial layer. The distinct low-symmetric crystal structure of SAOT enables a superior capability to sustain epitaxial strain, thus allowing for broad tunability in lattice constants. The resultant structural coherency and defect-free interface in perovskite ABO3/SAOT heterostructures effectively restrain crack formations during the water-assisted release of freestanding oxide membranes. For a variety of non-ferroelectric oxide membranes, the crack-free areas can span up to a few millimeters in length scale. These compelling features, combined with the inherent high-water solubility, make SAOT a versatile and feasible sacrificial layer for producing high-quality freestanding oxide membranes, thereby boosting their potential for innovative oxide electronics and flexible device designs.

cond-mat.mtrl-sci↗
arXiv2023

Electronic structure of the putative room-temperature superconductor Pb$_9$Cu(PO$_4$)$_6$O

A recent paper [Lee {\em et al.}, J. Korean Cryt. Growth Cryst. Techn. {\bf 33}, 61 (2023)] provides some experimental indications that Pb$_{10-x}$Cu$_x$(PO$_4$)$_6$O with $x\approx 1$, coined LK-99, might be a room-temperature superconductor at ambient pressure. Our density-functional theory calculations show lattice parameters and a volume contraction with $x$ -- very similar to experiment. The DFT electronic structure shows Cu$^{2+}$ in a $3d^9$ configuration with two flat Cu bands crossing the Fermi energy. This puts Pb$_{9}$Cu(PO$_4$)$_6$O in an ultra-correlated regime and suggests that, without doping, it is a Mott or charge transfer insulator. If doped such an electronic structure might support flat-band superconductivity or an correlation-enhanced electron-phonon mechanism, whereas a diamagnet without superconductivity appears to be rather at odds with our results.

cond-mat.supr-con↗
arXiv2023

Pb$_{10-x}$Cu$_x$(PO$_4$)$_6$O: a Mott or charge transfer insulator in need of further doping for (super)conductivity

We briefly review the status quo of research on the putative superconductor Pb$_9$Cu(PO$_4$)$_6$O also known as LK-99. Further, we provide {\em ab initio} derived tight-binding parameters for a two- and five-band model, and solve these in dynamical-mean-field theory. The ratio interaction-to-bandwidth makes LK-99 a Mott or charge transfer insulator. Electron or hole doping (which is different from substituting Pb by Cu and thus differs from LK-99) is required to make it metallic and potentially superconducting.

cond-mat.supr-con↗
arXiv2023

Ru doping induced spin frustration and enhancement of the room-temperature anomalous Hall effect in La2/3Sr1/3MnO3 films

In transition-metal-oxide heterostructures, the anomalous Hall effect (AHE) is a powerful tool for detecting the magnetic state and revealing intriguing interfacial magnetic orderings. However, achieving a larger AHE at room temperature in oxide heterostructures is still challenging due to the dilemma of mutually strong spin-orbit coupling and magnetic exchange interactions. Here, we exploit the Ru doping-enhanced AHE in LSMRO epitaxial films. As the B-site Ru doping level increases up to 20 percent, the anomalous Hall resistivity at room temperature can be enhanced from nOhmcm to uOhmcm scale. Ru doping leads to strong competition between ferromagnetic double-exchange interaction and antiferromagnetic super-exchange interaction. The resultant spin frustration and spin-glass state facilitate a strong skew-scattering process, thus significantly enhancing the extrinsic AHE. Our findings could pave a feasible approach for boosting the controllability and reliability of oxide-based spintronic devices.

cond-mat.mtrl-sci↗
arXiv2023

Effects of different concentrations of topotactic hydrogen impurities on the electronic structure of nickelate superconductors

Infinite-layer nickelate superconductors have recently been discovered to share both similarities and differences with cuprate superconductors. Notably, the incorporation of hydrogen (H) through topotactic reduction has been found to play a critical role in their electronic structure and, consequently, their superconductivity. In this study, we utilized a theoretical approach combining density-functional theory and impurity approximation to design three characteristic multi-orbital Hubbard models representing low, moderate, and high concentrations of topotactic-hydrogen. Consistent with experimental findings, our simulations revealed that both low and high concentrations of topotactic-hydrogen induce high-spin states ($S$=1) that are composed by holes at $d_{x^2-y^2}$ and $d_{z^2}$ orbitals and consequently the emergent inter-site hopping between $d_{z^2}$ to $d_{x^2-y^2}$ is unfavorable for superconductivity. Conversely, an optimal concentration of 25\% H aligns with the single Ni-$d_{x^2-y^2}$ band picture of superconductivity in infinite-layer nickelates, demonstrating its beneficial effect on promoting superconducting behavior.

cond-mat.supr-con↗
arXiv2023

Chiral magnetism and ordering of oxygen vacancies in SrTiO$_{2.5}$

Oxygen vacancies in the perovskite insulator SrTiO$_3$ free electrons that couple with other physical degrees of freedom such as lattice, orbital, and spin. This leads to the emergence of exotic quantum states such as superconductivity and unusual ferromagnetism. We perform density-functional theory and dynamical mean-field theory calculations and demonstrate that the orientation and ordering of the TiO$_5$ pentahedra plays a crucial role. Specifically, for vacancy-rich SrTiO$_{3-δ}$ ($δ\sim$0.5), we find a chiral ordering of the TiO$_5$ pentahedra in a sixfold superlattice. This chiral structure is accompanied by a chiral magnetic state with a net moment in the (111) direction at room temperature, which can explain several experimental observations.

cond-mat.str-el↗
arXiv2023

Optimizing superconductivity: from cuprates via nickelates to palladates

Motivated by cuprate and nickelate superconductors, we perform a comprehensive study of the superconducting instability in the single-band Hubbard model. We calculate the spectrum and superconducting transition temperature $T_{\rm c}$ as a function of filling and Coulomb interaction for a range of hopping parameters, using the dynamical vertex approximation. We find the sweet spot for high $T_{\rm c}$ to be at intermediate coupling, moderate Fermi surface warping, and low hole doping. Combining these results with first principles calculations, neither nickelates nor cuprates are close to this optimum within the single-band description. Instead, we identify some palladates, notably RbSr$_2$PdO$_3$ and $A^{\prime}_2$PdO$_2$Cl$_2$ ($A^{\prime}$=Ba$_{0.5}$La$_{0.5}$), to be virtually optimal, while others, such as NdPdO$_2$, are too weakly correlated.

cond-mat.supr-con↗
arXiv2023

Absence of electron-phonon-mediated superconductivity in hydrogen-intercalated nickelates

A recent experiment [X. Ding et al., Nature 615, 50 (2023)] indicates that superconductivity in nickelates is restricted to a narrow window of hydrogen concentration: 0.22 < x < 0.28 in Nd$_{0.8}$Sr$_{0.2}$NiO$_{2}$H$_{x}$. This reported necessity of hydrogen suggests that it plays a crucial role for superconductivity, as it does in the vast field of hydride superconductors. Using density-functional theory and its extensions, we explore the effect of topotactic hydrogen on the electronic structure and phonon-mediated superconductivity in nickelate superconductors. Our calculations show that the electron-phonon coupling in hydrogen-intercalated nickelates is not strong enough to drive the electron pairing, and thus cannot explain the reported superconductivity.

cond-mat.supr-con↗
arXiv2023

Topotactic-hydrogen forms chains in $AB$O$_2$ nickelate superconductors

Despite enormous experimental and theoretical efforts, obtaining generally accepted conclusions regarding the intrinsic magnetic and electronic properties of superconducting nickelates remains exceptionally challenging. Experiments show a significant degree of uncertainty, indicating hidden factors in the synthesized films, which call for further investigations. One of those "hidden factors" is the possibility of intercalating hydrogen during the chemical reduction process from Nd(La)NiO$_3$ to Nd(La)NiO$_2$ using CaH$_2$. While hydrogen has been detected in experimental samples, not much is known about its distribution through the crystal and its influence on the electronic environment. Here, we show the tendency toward the formation of one-dimensional hydrogen chains in infinite-layers LaNiO$_2$ superconductors using density-functional theory (DFT) supplemented by dynamical mean-field theory (DMFT). The formation of such hydrogen chains induces a coexistence of different oxidation states of Ni and competing magnetic phases, and possibly explains the recently observed charge order states in nickelate superconductors. Furthermore, it contributes to the difficulty of synthesizing homogeneous nickelates and determining their ground states. The smoking gun to detect excess hydrogen in nickelates are flat phonon modes, which are infrared active and quite insensitive to the exact arrangement of the H atoms.

cond-mat.mtrl-sci↗
arXiv2022

Magnetism in doped infinite-layer NdNiO2 studied by combined density functional theory and dynamical mean-field theory

The recent observation of superconductivity in infinite-layer nickelates has brought intense debate on the established knowledge of unconventional superconductivity based on the cuprates. Despite many similarities, the nickelates differ from the cuprates in many characteristics, the most notable one among which is the magnetism. Instead of a canonical antiferromagnetic Mott insulator as the undoped cuprates, from which the superconductivity is generally believed to arise upon doping, the undoped nickelates show no sign of magnetic ordering in experiments. Through a combined density functional theory, dynamical mean-field theory, and model study, we show that although the increased energy splitting between O-$p$ orbital and Cu/Ni-$d$ orbital ($Δ_{dp}$) results in larger magnetic moment in nickelates, it also leads to stronger antiferromagnetism/ferromagnetism competition, and weaker magnetic exchange coupling. Meanwhile, the self-doping effect caused by Nd-$d$ orbital screens the magnetic moment of Ni. The Janus-faced effect of $Δ_{dp}$ and self-doping effect together give a systematic understanding of magnetic behavior in nickelates and explain recent experimental observations.

cond-mat.supr-con↗