Thin films provide a versatile platform to tune electron correlations and explore new physics in strongly correlated materials. Epitaxially grown thin films of the alkali-doped fulleride K$_{3+x}$C$_{60}$, for example, exhibit %various intriguing phenomena, including Mott transitions and superconductivity, depending on dimensionality and doping. Surprisingly, in the trilayer case, a strong electron-hole doping asymmetry has been observed in the superconducting phase, which is absent in the three-dimensional bulk limit. Using density-functional theory plus dynamical mean-field theory, we show that this doping asymmetry results from a substantial charge reshuffling from the top layer to the middle layer. While the nominal filling per fullerene is close to $n=3$, the top layer rapidly switches to an $n=2$ insulating state upon hole doping, which \textcolor{black}{implies a} doping asymmetry of the superconducting gap. The interlayer charge transfer and layer-selective metal-insulator transition result from the interplay between crystal field splittings, strong Coulomb interactions, and an effectively negative Hund coupling. This peculiar charge reshuffling is absent in the monolayer system, which is an $n=3$ Mott insulator, as expected from the nominal filling.
We use scanning tunneling microscopy to investigate Bi2Sr2Ca2Cu3O10+δ trilayer cuprates from the optimally doped to overdoped regime. We find that the two distinct superconducting gaps from the inner and outer CuO2 planes both decrease rapidly with doping, in sharp contrast to the nearly constant Tc. 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 CuO2 planes and the intricate interaction betwee…
The doping dependence of the themopower, in-plane resistivity rho_ab(T), out-of-plane resistivity rho_c(T), and susceptibility has been systematically measured for high-quality single crystal Bi2Sr2Ca2Cu3O10+delta. We found that the transition temperature Tc and pseudogap formation temperature T_rho_c*, below which rho_c shows a typical upturn, do not change from their optimum values in the "overdoped" region, even though doping actually proceeds. This suggests that, in overdoped region, the bulk $T_c$ is determined by the always underdoped inner plane, which have a large superconducting gap, …
Mode-selective phonon effects on magnetism and superconductivity in trilayer nickelates
Universität Würzburg（维尔茨堡大学）；Nagoya University（名古屋大学）；Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所北京凝聚态物理国家研究中心）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Hefei National Laboratory, and New Cornerstone Science Laboratory（合肥国家实验室和新基石科学实验室）；Institute of Theoretical Physics, Chinese Academy of Sciences（中国科学院理论物理研究所）
Doping Evolution of Nodal Electron Dynamics in Trilayer Cuprate Superconductor Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+δ}$ Revealed by Laser-Based Angle-Resolved Photoemission Spectroscopy
We construct a van der Waals heterostructure consisting of three graphene layers stacked with alternating twisting angles $\pmθ$. At the average twist angle $θ\sim 1.56^{\circ}$, a theoretically predicted magic angle for the formation of flat electron bands, narrow conduction and valence moiré bands appear together with a linearly dispersing Dirac band. Upon doping the half-filled moiré valence band with holes, or the half-filled moiré conduction band with electrons, displacement field tunable superconductivity emerges, reaching a maximum critical temperature of 2.1 K at optimal doping and dis…
Based on a hybrid interlayer coupling mechanism, we study the coexistence of superconductivity (SC) and antiferromagnetism (AFM) in trilayer cuprates. By introducing an interlayer magnetic scattering term, we solve the multilayer $t{-}J$ model with Josephson coupling under the framework of Gutzwiller projection. We show that both the SC and AFM orders in the multilayered system are enhanced and the range of AFM order is extended. The layer configuration of d-wave pairing gap and AFM order further plays an essential role in determining the interlayer magnetic and superconducting coupling phase …
Magic-angle twisted trilayer graphene (MATTG) recently emerged as a highly tunable platform for studying correlated phases of matter, such as correlated insulators and superconductivity. Superconductivity occurs in a range of doping levels that is bounded by van Hove singularities which stimulates the debate of the origin and nature of superconductivity in this material. In this work, we discuss the role of spin-fluctuations arising from atomic-scale correlations in MATTG for the superconducting state. We show that in a phase diagram as function of doping ($ν$) and temperature, nematic superco…
Combining mean-field and renormalization group analyses, here we unveil the nature of recently observed superconductivity and parent metallic states in chemically doped rhombohedral trilayer graphene, subject to external electric displacement fields ($D$) [H. Zhou, \emph{et al.}, Nature (London) {\bf 598}, 434 (2021)]. We argue that close to the charge neutrality, on site Hubbard repulsion favors layer antiferromagnet, which when combined with the $D$-field induced layer polarization, produces a spin-polarized, but valley-unpolarized half-metal, conducive to the nucleation of spin-triplet $f$-…
Incipient superconductivity and tunable Chern insulators in twisted bilayer-trilayer graphene
Department of Physics, University of Washington（华盛顿大学物理系）；Department of Materials Science and Engineering, University of Washington（华盛顿大学材料科学与工程系）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（物质材料研究机构电子与光学材料研究中心）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（物质材料研究机构的材料纳米结构研究中心）
We describe a reversible, spatially-controlled doping method for cuprate films. The technique has been used to create superconductor-antiferromagnetic insulator-superconductor (S-AFI-S) junctions and optimally doped superconductor-underdoped superconductor-optimally doped superconductor (OS-US-OS) cuprate structures. We demonstrate how the S-AFI-S structure can be employed to reliably measure the transport properties of the antiferromagnetic insulator region at cryogenic temperatures using the superconductors as seamless electrical leads. We also discuss applied and fundamental issues which ma…
Orbital-selective electronic modes induced by doping and originating from distinct spin excitations: an essential feature of orbital-selective Mott transition
Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（物质纳米结构研究中心，日本国立物质材料研究所）
Magic-angle twisted trilayer graphene (MATTG) has emerged as a novel moiré material that exhibits both strong electronic correlations and unconventional superconductivity. However, spectroscopic studies of its electronic properties are lacking, and the nature of superconductivity and the corresponding order parameter in this system remain elusive. Here we perform high-resolution scanning tunneling microscopy and spectroscopy of MATTG and reveal extensive regions of atomic reconstruction that favor mirror-symmetric stacking. In these regions, we observe a cascade of symmetry-breaking electronic…
Electrically controllable valence-conduction band reversals in helical trilayer graphene
Weizmann Institute of Science（魏茨曼科学研究所）；Massachusetts Institute of Technology（麻省理工学院）；University of Texas at Dallas（德克萨斯大学达拉斯分校）；Stanford University（斯坦福大学）；SLAC National Accelerator Laboratory（斯坦福直线加速器中心）；National Institute for Materials Science（国立材料研究所）
We have studied the doping-driven orbital-selective Mott transition in multi-band Hubbard models with equal band width in the presence of crystal field splitting. Crystal field splitting lifts one of the bands while leaving the others degenerate. We use single-site dynamical mean-field theory combined with continuous time quantum Monte Carlo impurity solver to calculate a phase diagram as a function of total electron filling $N$ and crystal field splitting $Δ$. We find a large region of orbital-selective Mott phase in the phase diagram when the doping is large enough. Further analysis indicate…
A series of recent experiments have demonstrated robust superconductivity in magic-angle twisted trilayer graphene (TTG). In particular, a recent work by Cao et al. (arxiv:2103.12083) studies the behavior of the superconductor in an in-plane magnetic field and out-of-plane displacement field, finding that the superconductor is unlikely to be spin-singlet. This work also finds that at high magnetic fields and a smaller range of dopings and displacement fields, it undergoes a transition to a distinct field-induced superconducting state. Inspired by these results, we develop an understanding of s…
The moiré superlattice formed by ABC stacked trilayer graphene aligned with a hexagonal boron nitride substrate (TG/h-BN) provides an interesting system where both the bandwidth and the topology can be tuned by an applied perpendicular electric field $D$ . Thus the TG/h-BN system can simulate both Hubbard model physics and nearly flat Chern band physics within one sample. We derive lattice models for both signs of $D$ (which controls the band topology) separately through explicit Wannier orbital construction and mapping of Coulomb interaction. When the bands are topologically trivial, we discu…
Pyrochlore oxides are fascinating systems where strong, multi-orbital correlations in concert with geometrical frustration give rise to unanticipated physical properties. The detailed mechanism of the insulator-metal transitions (IMT) underpinning these phenomena is, however, ill-understood in general. Motivated thereby, we study the IMT in the pyrochlore ${\rm Hg_{2}Ru_{2}O_{7}}$ using LDA+DMFT. In contrast to the well-known examples of Mott transitions in TMO, we show that, in the negative charge-transfer situation characteristic of \hg, self-doping plays a crucial role in the emergence of a…
The recent detailed study of quasi-one-dimensional iron-based ladders, with the $3d$ iron electronic density $n = 6$, has unveiled surprises, such as orbital-selective phases. However, similar studies for $n=6$ iron chains are still rare. Here, a three-orbital electronic Hubbard model was constructed to study the magnetic and electronic properties of the quasi-one-dimensional $n=6$ iron chain Ce$_2$O$_2$FeSe$_2$, with focus on the effect of doping. Specifically, introducing the Hubbard $U$ and Hund $J_{H}$ couplings and studying the model via the density matrix renormalization group, we report…
Kekulé spirals and charge transfer cascades in twisted symmetric trilayer graphene
Princeton Center for Theoretical Science, Princeton University（普林斯顿大学理论科学中心）；Department of Physics, University of Zurich（苏黎世大学物理系）；Department of Physics, Ghent University（根特大学物理系）
At interfaces between polar and nonpolar perovskite oxides, an unusual electron-doping has been previously observed, due to electronic reconstructions. We report on remote hole-doping at an interface composed of only polar layers, revealed by high-resolution hard x-ray core-level photoemission spectroscopy. In LaAlO3/LaVO3/LaAlO3 trilayers, the vanadium valence systematically evolves from the bulk value of V3+ to higher oxidation states with decreasing LaAlO3 cap layer thickness. These results provide a synthetic approach to hole-doping transition metal oxide heterointerfaces without invoking …
Starting with twisted bilayer graphene, graphene-based moiré materials have recently been established as a new platform for studying strong electron correlations. In this paper, we study twisted graphene monolayers on trilayer graphene and demonstrate that this system can host flat bands when the twist angle is close to the magic-angle of 1.16$^\circ$. When monolayer graphene is twisted on ABA trilayer graphene, the flat bands are not isolated, but are intersected by a Dirac cone with a large Fermi velocity. In contrast, graphene twisted on ABC trilayer graphene (denoted AtABC) exhibits a gap …
We present a computational study of PbCoO$_3$ at ambient and elevated pressure. We employ the static and dynamic treatment of local correlation in form of density functional theory + $U$ (DFT+$U$) and + dynamical mean-field theory (DFT+DMFT). Our results capture the experimentally observed crystal structures and identify the unsaturated Pb $6s$ - O $2p$ bonds as the driving force beyond the complex physics of PbCoO$_3$. We provide a geometrical analysis of the structural distortions and we discuss their implications, in particular, the internal doping, which triggers transition between phases …
The nature of the correlated phases found in some graphene heterostructures is under debate. We use dynamical mean-field theory (DMFT) to analyze the effect of local correlations close to half-filling on one of such systems, the ABC trilayer graphene aligned with hexagonal boron nitride (ABC/hBN), which presents a moiré superlattice. This system has shown insulating phases at integer fillings of the moiré lattice, precisely the fillings at which a sufficiently strong Coulomb interaction (U$_{\rm Mott}$) may produce a metal-insulator Mott transition. Our calculations show that the electronic st…
Tailoring transport properties of strongly correlated electron systems in a controlled fashion counts among the dreams of materials scientists. In copper oxides, varying the carrier concentration is a tool to obtain high-temperature superconducting phases. In manganites, doping results in exotic physics such as insulator-metal transitions (IMT), colossal magnetoresistance (CMR), orbital- or charge-ordered (CO) or charge-disproportionate (CD) states. In most oxides, antiferromagnetic order and charge-disproportionation are asssociated with insulating behavior. Here we report the realization of …
Barlowite $Cu_4(OH)_6FBr$ is a newly found mineral containing $Cu^{2+}$ kagome planes. Despite similarities in many aspects to Herbertsmithite $Cu_3Zn(OH)_6Cl_2$, the well-known quantum spin liquid (QSL) candidate, intrinsic Barlowite turns out not to be a QSL, possibly due to the presence of $Cu^{2+}$ ions in between kagome planes that induce interkagome magnetic interaction [PRL, 113, 227203 (2014)]. Using first-principles calculation, we systematically study the feasibility of selective substitution of the interkagome Cu ions with isovalent nonmagnetic ions. Unlike previous speculation of u…
The recently discovered layered kagome metals AV$_3$Sb$_5$ (A = K, Rb, and Cs) with vanadium kagome networks provide a novel platform to explore correlated quantum states intertwined with topological band structures. Here we report the prominent effect of hole doping on both superconductivity and charge density wave (CDW) order, achieved by selective oxidation of exfoliated thin flakes. A superconducting dome is revealed as a function of the effective doping content. The superconducting transition temperature ($T_{\mathrm{c}}$) and upper critical field in thin flakes are significantly enhanced…
Multiorbital character of the density wave in trilayer nickelate superconductors
Max-Planck-Institute for Solid State Research（马克斯·普朗克固体研究所）；Facultad de Ciencias Exactas, Ingeniería y Agrimensura and Instituto de Física Rosario (UNR-CONICET)（罗萨里奥大学精确科学、工程与测量学院及罗萨里奥物理研究所（UNR-CONICET））；RIKEN Interdisciplinary Theoretical and Mathematical Sciences (iTHEMS)（理化学研究所跨学科理论与数学科学中心 (iTHEMS)）
We theoretically study the magnetic properties of pyrochlore iridate bilayer and trilayer thin films grown along the $[111]$ direction using a strong coupling approach. We find the ground state magnetic configurations on a mean field level and carry out a spin-wave analysis about them. In the trilayer case the ground state is found to be the all-in-all-out (AIAO) state, whereas the bilayer has a deformed AIAO state. For all parameters of the spin-orbit coupled Hamiltonian we study, the lowest magnon band in the trilayer case has a nonzero Chern number. In the bilayer case we also find a parame…
Study of the strongly correlated states in van der Waals heterostructures is one of the central topics in modern condensed matter physics. Among these, the rhombohedral trilayer graphene (RTG) occupies a prominent place since it hosts a variety of interaction-driven phases, with the metallic ones yielding exotic superconducting orders upon doping. Motivated by these experimental findings, we show within the framework of the low-energy Dirac theory that the optical conductivity can distinguish different candidates for a paramagnetic metallic ground state in this system. In particular, this obse…
Momentum-Selective Two-Component Excitations in Electron-Doped Mott Insulators
Institute for Advanced Study, Tsinghua University（清华大学高等研究院）；French American Center for Theoretical Science, CNRS（法国美国理论科学中心，法国国家科学研究中心）；Kavli Institute for Theoretical Physics, University of California, Santa Barbara（加州大学圣塔芭芭拉分校卡弗里理论物理研究所）
Using a combination of th local-density approximtion (LDA) and dynamicla mean-field theory (DMFT) calculations, we explore the correlated electronic structure of a member of the layered Iron oxychalcogenide Na_{2}Fe_{2}OSe_{2}. We find that the parent compund is a multi-orbital Mott insulator. Surprisingly, and somewhat reminiscent of the doped high-T_{c} cuprates, carrier localization is found to persist upon weak hole doping because the chemical potential lies in a gap structure wit almost vanishing density-of-states (DOS). On the other hand, in remarkable contrast, electron doping drives an…
We outline a general mechanism for Orbital-selective Mott transition (OSMT), the coexistence of both itinerant and localized conduction electrons, and show how it can take place in a wide range of realistic situations, even for bands of identical width and correlation, provided a crystal field splits the energy levels in manifolds with different degeneracies and the exchange coupling is large enough to reduce orbital fluctuations. The mechanism relies on the different kinetic energy in manifolds with different degeneracy. This phase has Curie-Weiss susceptibility and non Fermi-liquid behavior,…
The phase diagram of the high-Tc cuprates is dominated by the Mott insulating phase of the parent compounds. As we approach it from large doping, a standard Fermi-liquid gradually turns into a bad non-Fermi liquid metal, a process which culminates in the pseudogap regime, in which the antinodal region in momentum space acquires a gap before reaching a fully gapped Mott state. Here we show that experiments for electron- and hole-doped BaFe2As2 support an analogous scenario. The doping evolution is dominated by the influence of a Mott insulator that would be realized for half-filled conduction b…
Ferromagnetism is most common in transition metal compounds but may also arise in low-density two-dimensional electron systems, with signatures observed in silicon, III-V semiconductor systems, and graphene moiré heterostructures. Here we show that gate-tuned van Hove singularities in rhombohedral trilayer graphene drive the spontaneous ferromagnetic polarization of the electron system into one or more spin- and valley flavors. Using capacitance measurements on graphite-gated van der Waals heterostructures, we find a cascade of density- and electronic displacement field tuned phase transitions…
Hund's coupling assisted orbital-selective superconductivity in Ba1-xKxFe2As2
Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory（斯坦福材料能源科学研究所，SLAC国家加速器实验室）；Geballe Laboratory for Advanced Materials, Department of Applied Physics and Physics, Stanford University（斯坦福大学应用物理与物理系，Geballe先进材料实验室）；Department of Applied Physics, Stanford University（斯坦福大学应用物理系）；Department of Applied Physics, KTH-Royal Institute of Technology（瑞典皇家理工学院应用物理系）；National Institute of Advanced Industrial Science and Technology (AIST)（日本产业技术综合研究所）；Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory（SLAC国家加速器实验室斯坦福同步辐射光源）；Department of Material Science, Stanford University（斯坦福大学材料科学系）
The recent observation of superconductivity in infinite-layer Nd$_{1-x}$Sr$_x$NiO$_2$ thin films has attracted a lot of attention, since this compound is electronically and structurally analogous to the superconducting cuprates. Due to the challenges in the phase stabilization upon chemical doping with Sr, we synthesized artificial superlattices of LaNiO$_3$ embedded in insulating LaGaO$_3$, and used layer-selective topotactic reactions to reduce the nickelate layers to LaNiO$_{2}$. Hole doping is achieved via interfacial oxygen atoms and tuned via the layer thickness. We used electrical trans…
We studied the relationship between the charge doping and the correlation, and its effects on the spectral function of the BaFe$_2$As$_2$ compound in the framework of the density functional theory combined with the dynamical mean field theory (DFT+DMFT). The calculated mass enhancements showed that the electronic correlation varies systematically from weak to strong when moving from the heavily electron-doped regime to the heavily hole-doped one. Since the compound has a multi-orbital nature, the correlation is orbital-dependent and it increases as hole-doping increases. The Fe-3d$_{xy}$ (xy) …
We present an approach to the normal state of cuprate superconductors which is based on a minimal cluster extension of dynamical mean-field theory. Our approach is based on an effective two-impurity model embedded in a self-consistent bath. The two degrees of freedom of this effective model can be associated to the nodal and antinodal regions of momentum space. We find a metal-insulator transition which is selective in momentum space: At low doping quasiparticles are destroyed in the antinodal region, while they remain protected in the nodal region, leading to the formation of apparent Fermi a…
We study the effects of electron-electron interactions and hole doping on the electronic structure of Cu-doped NaFeAs using the density functional theory plus dynamical mean-field theory (DFT+DMFT) method. In particular, we employ an effective multi-orbital Hubbard model with a realistic bandstructure of NaFeAs in which Cu-doping was modeled within a rigid band approximation and compute the evolution of the spectral properties, orbital-dependent electronic mass renormalizations, and magnetic properties of NaFeAs upon doping with Cu. In addition, we perform fully charge self-consistent DFT+DMFT…
Motivated by recent experiments [H. Zhou, \emph{et al.}, Science {\bf 375}, 774 (2022) and S. C. de la Barrera, \emph{et al.}, arXiv:2110.13907], here we propose a general mechanism for valley and/or spin degeneracy lifting of the electronic bands in doped Bernal bilayer graphene, subject to electric displacement ($D$) fields. A $D$-field induced layer polarization (LP), when accompanied by Hubbard repulsion driven layer antiferromagnet (LAF) and next-nearest-neighbor repulsion driven quantum anomalous Hall (QAH) orders, lifts the four-fold degeneracy of electronic bands, yielding a quarter me…
Mott insulator plays a central role in strongly correlated physics, where the repulsive Coulomb interaction dominates over the electron kinetic energy and leads to insulating states with one electron occupying each unit cell. Doped Mott insulator is often described by the Hubbard model3, which can give rise to other correlated phenomena such as unusual magnetism and even high-temperature superconductivity. A tunable Mott insulator, where the competition between the Coulomb interaction and the kinetic energy can be varied in situ, can provide an invaluable model system for the study of Mott phy…
Magnetic ordering of the first row transition metal intercalates of NbS$_2$ due to coupling between the conduction electrons and the intercalated ions has been explained in terms of Fermi surface nesting. We use angle-resolved photoelectron spectroscopy to investigate the Fermi surface topology and the valence band structure of the quasi-two-dimensional layer compounds Mn$_{1/3}$NbS$_2$ and Ni$_{1/3}$NbS$_2$. Charge transfer from the intercalant species to the host layer leads to non-uniform, pocket selective doping of the Fermi surface. The implication of our results on the nesting properties…
