arXiv subjects

Daniel S. Dessau

Publications and source records attributed to Daniel S. Dessau.

13 recordsLinked to original sources

arXiv2025

Experimental realization of dice-lattice flat band at the Fermi level in layered electride YCl

Flat electronic bands, where interactions among electrons overwhelm their kinetic energies, hold the promise for exotic correlation physics. The dice lattice has long been theorized as a host of flat bands with intriguing band topology. However, to date, no material has ever been found to host the characteristic flat bands of a dice lattice. Here, using angle-resolved photoemission spectroscopy (ARPES), we discover a dice-lattice flat band at $E_F$ in the van der Waals (vdW) electride [YCl]$^{2+}$: 2e-. In this system, excess valence electrons from Y deconfine from the cation framework to form an interstitial anionic electron lattice that constitutes the dice lattice. Our ARPES measurements unambiguously identify two sets of dice-lattice bands in YCl, including a nearly dispersionless band at the Fermi level. The flat bands and other dispersive bands observed in ARPES find excellent agreement with first-principles calculations, and theoretical analysis reveals that the near-$E_F$ electronic structure is well captured by a simple dice-lattice model. Our findings thus end the long quest of a real dice flat band material and establish vdW electride YCl as a prototype of dice metals. Our results further demonstrate the anionic electron lattice as a novel scheme for realizing lattice geometries and electronic structures rare to find in conventional crystalline systems.

cond-mat.str-el↗

arXiv2023

Potential Lifshitz transition at optimal substitution in nematic pnictide Ba$_{1-x}$Sr$_x$Ni$_2$As$_2$

BaNi$_2$As$_2$ is a structural analog of the pnictide superconductor BaFe$_2$As$_2$, which, like the iron-based superconductors, hosts a variety of ordered phases including charge density waves (CDWs), electronic nematicity, and superconductivity. Upon isovalent Sr substitution on the Ba site, the charge and nematic orders are suppressed, followed by a sixfold enhancement of the superconducting transition temperature ($T_c$). To understand the mechanisms responsible for enhancement of $T_c$, we present high-resolution angle-resolved photoemission spectroscopy (ARPES) measurements of the Ba$_{1-x}$Sr$_{x}$Ni$_2$As$_2$ series, which agree well with our density functional theory (DFT) calculations throughout the substitution range. Analysis of our ARPES-validated DFT results indicates a Lifshitz transition and reasonably nested electron and hole Fermi pockets near optimal substitution where $T_c$ is maximum. These nested pockets host Ni $d_{xz}$/$d_{yz}$ orbital compositions, which we associate with the enhancement of nematic fluctuations, revealing unexpected connections to the iron-pnictide superconductors. This gives credence to a scenario in which nematic fluctuations drive an enhanced $T_c$.

cond-mat.supr-con↗

arXiv2023

Pb-apatite framework as a generator of novel flat-band CuO based physics

Based on DFT calculations, we present the basic electronic structure of CuPb9(PO4)6O (Cu-doped lead apatite, LK-99), in two scenarios: (1) where the structure is constrained to the P3 symmetry and (2) where no symmetry is imposed. At the DFT level, the former is predicted to be metallic while the latter is found to be a charge-transfer insulator. In both cases the filling of these states is nominally d9, consistent with the Cu2+ valence state, and Cu with a local magnetic moment ~0.7mB. In the metallic case we find these states to be unusually flat (0.2 eV dispersion), giving high DOS at EF that we argue can be a host for novel electronic physics, including potentially high temperature superconductivity. The flatness of the bands is the likely origin of symmetry-lowering gapping possibilities that would remove the spectral weight from EF. Since some experimental observations show metallic/semiconducting behavior, we propose that disorder is responsible for closing the gap. We consider a variety of possibilities that could possibly close the gap, but limit consideration to kinds of disorder that preserve electron count. For all possibilities we considered (spin disorder, O on vacancy sites, Cu on different Pb sites), the local Cu moment, and consequently the gap remains robust. We conclude that disorder responsible for metallic behavior entails some kind of doping where the electron count changes. We claim that the emergence of the flat bands should be due to weak wave function overlap between the Cu and O orbitals, owing to the directional character of the constituent orbitals. So, finding an appropriate host structure for minimizing hybridization between Cu and O while allowing them to still weakly interact should be a promising route for generating flat bands at EF which can lead to interesting electronic phenomena, regardless of whether LK-99 is a room-temperature superconductor.

cond-mat.supr-con↗

arXiv2023

Multiple Slater determinants and strong spin-fluctuations as key ingredients of the electronic structure of electron- and hole-doped Pb$_{10-x}$Cu$_x$(PO4)$_6$O

LK-99, with chemical formula Pb$_{10-x}$Cu$_x$(PO4)$_6$O, was recently reported to be a room-temperature superconductor. While this claim has met with little support in a flurry of ensuing work, a variety of calculations (mostly based on density-functional theory) have demonstrated that the system possesses some unusual characteristics in the electronic structure, in particular flat bands. We have established previously that within DFT, the system is insulating with many characteristics resembling the classic cuprates, provided the structure is not constrained to the $P$3(143) symmetry nominally assigned to it. Here we describe the basic electronic structure of LK-99 within self-consistent many-body perturbative approach, quasiparticle self-consistent GW (QSGW) approximation and their diagrammatic extensions. QSGW predicts that pristine LK-99 is indeed a Mott/charge transfer insulator, with a bandgap gap in excess of 3eV, whether or not constrained to the $P$3(143) symmetry. The highest valence bands occur as a pair, and look similar to DFT bands. The lowest conduction band is an almost dispersionless state of largely Cu $d$ character. When Pb$_9$Cu(PO$_4$)$_6$O} is hole-doped, the valence bands modify only slightly, and a hole pocket appears. However, two solutions emerge: a high-moment solution with the Cu local moment aligned parallel to neighbors, and a low-moment solution with Cu aligned antiparallel to its environment. In the electron-doped case the conduction band structure changes significantly: states of mostly Pb character merge with the formerly dispersionless Cu $d$ state, and high-spin and low spin solutions once again appear. Thus we conclude that with suitable doping, the ground state of the system is not adequately described by a band picture, and that strong correlations are likely.

cond-mat.supr-con↗

arXiv2023

Thin film TaAs: developing a platform for Weyl semimetal devices

MX monopnictide compounds (M=Nb,Ta, X = As,P) are prototypical three-dimensional Weyl semimetals (WSMs) that have been shown in bulk single crystal form to have potential for a wide variety of novel devices due to topologically protected band structures and high mobilities. However, very little is known about thin film synthesis, which is essential to enable device applications. We synthesize TaAs(001) epilayers by molecular beam epitaxy on GaAs(001) and provide an experimental phase diagram illustrating conditions for single phase, single-crystal-like growth. We investigate the relationship between nanoscale defects and electronic structure, using angle-resolved photoemission spectroscopy, Kelvin probe microscopy and transmission electron microscopy. Our results provide a roadmap and platform for developing 3D WSMs for device applications.

cond-mat.mtrl-sci↗

arXiv2022

Revised phase diagram of the high-$T_c$ cuprate superconductor Pb-doped Bi$_2$Sr$_2$CaCu$_2$O$_{8+δ}$ revealed by anisotropic transport measurements

Although phase diagrams can be leveraged to investigate high transition temperature (high-$T_c$) superconductivity, the issue has not been discussed thoroughly. In this study, we elucidate the phase diagram of the overdoped side of high-$T_c$ cuprates via systematic anisotropic transport measurements for Pb-doped Bi-2212 single crystals. We demonstrate that the characteristic temperatures of the "weak" pseudogap opening and electronic coherence cross each other at a critical doping level, while those of the "strong" pseudogap merges into that of superconducting fluctuations above the critical doping level. Our results indicate the importance of Mottness in high-$T_c$ superconductivity.

cond-mat.supr-con↗

arXiv2018

Observation of Topological Surface State in High Temperature Superconductor MgB2

The hunt for the benchmark topological superconductor (TSc) has been an extremely active research subject in condensed matter research, with quite a few candidates identified or proposed. However, low transition temperatures (Tc) and/or strong sensitivity to disorder and dopant levels in known TSc candidates have greatly hampered progress in this field. Here, we use Angle-resolved Photoemission Spectroscopy (ARPES) to show the presence of Dirac Nodal Lines (DNLs) and the corresponding topological surface states (TSS's) on the [010] faces of the Tc=39K s-wave BCS superconductor MgB2. Not only is this nearly triple the current record of superconducting Tc among all candidate TSc's, but the nature of these DNL states should make them highly tolerant against disorder and inadvertent doping variations. This makes MgB2 a promising high temperature platform for the study of topological superconductivity.

cond-mat.supr-con↗

arXiv2016

Disorder-driven topological phase transition in Bi2Se3 films

Topological insulators (TI) are a phase of matter that host unusual metallic states on their surfaces. Unlike the states that exist on the surface of conventional materials, these so-called topological surfaces states (TSS) are protected against disorder-related localization effects by time reversal symmetry through strong spin-orbit coupling. By combining transport measurements, angle-resolved photo-emission spectroscopy and scanning tunneling microscopy, we show that there exists a critical level of disorder beyond which the TI Bi2Se3 loses its ability to protect the metallic TSS and transitions to a fully insulating state. The absence of the metallic surface channels dictates that there is a change in topological character, implying that disorder can lead to a topological phase transition even without breaking the time reversal symmetry. This observation challenges the conventional notion of topologically-protected surface states, and will provoke new studies as to the fundamental nature of topological phase of matter in the presence of disorder.

cond-mat.mtrl-sci↗

arXiv2014

Controlling the electronic structure of graphene using surface-adsorbate interactions

We show that strong coupling between graphene and the substrate is mitigated when 0.8 monolayer of Na is adsorbed and consolidated on top graphene-on-Ni(111). Specifically, the π state is partially restored near the K-point and the energy gap between the π and π* states reduced to 1.3 eV after adsorption, as measured by angle-resolved photoemission spectroscopy. We show that this change is not caused by intercalation of Na to underneath graphene but it is caused by an electronic coupling between Na on top and graphene. We show further that graphene can be decoupled to a much higher extent when Na is intercalated to underneath graphene. After intercalation, the energy gap between the π and π* states is reduced to 0 eV and these states are identical as in freestanding and n-doped graphene. We conclude thus that two mechanisms of decoupling exist: a strong decoupling through intercalation, which is the same as one found using noble metals, and a weak decoupling caused by electronic interaction with the adsorbate on top.

cond-mat.mtrl-sci↗

arXiv2014

Hallmarks of the Mott-Metal Crossover in the Hole Doped J=1/2 Mott insulator Sr2IrO4

The physics of doped Mott insulators remains controversial after decades of active research, hindered by the interplay among possible competing orders and fluctuations. It is thus highly desired to distinguish the intrinsic characters of the Mott-metal crossover from those of other origins. We investigate the evolution of electronic structure and dynamics of the hole-doped J=1/2 Mott insulator Sr2IrO4. The effective hole doping is achieved by replacing Ir with Rh atoms, with the chemical potential immediately jumping to or near the top of the lower Hubbard band. The doped iridates exhibit multiple exotic features previously observed in doped cuprates - pseudogaps, Fermi "arcs", and marginal-Fermi-liquid-like electronic scattering rates, despite different mechanisms that forbid electron double-occupancy. We argue these universal features of the Mott-metal crossover are not related to preformed electron pairing, quantum criticality or density-wave formation as most commonly discussed. Instead, short-range antiferromagnetic correlations may play an indispensible role.

cond-mat.str-el↗

arXiv2014

Robust topological surface states of Bi2Se3 thin films on amorphous SiO2/Si substrate and a large ambipolar gating effect

The recent emergence of topological insulators (TI) has spurred intensive efforts to grow TI thin films on various substrates. However, little is known about how robust the topological surface states (TSS) are against disorders and other detrimental effects originating from the substrates. Here, we report observation of a well-defined TSS on Bi2Se3 films grown on amorphous SiO2 (a-SiO2) substrates and a large gating effect on these films using the underneath doped-Si substrate as the back gate. The films on a-SiO2 were composed of c-axis ordered but random in-plane domains. However, despite the in-plane randomness induced by the amorphous substrate, the transport properties of these films were superior to those of similar films grown on single-crystalline Si(111) substrates, which are structurally better matched but chemically reactive with the films. This work sheds light on the importance of chemical compatibility, compared to lattice matching, for the growth of TI thin films, and also demonstrates that the technologically-important and gatable a-SiO2/Si substrate is a promising platform for TI films.

cond-mat.mtrl-sci↗

arXiv2012

In-Plane Orbital Texture Switch at the Dirac Point in the Topological Insulator Bi2Se3

Topological insulators are novel macroscopic quantum-mechanical phase of matter, which hold promise for realizing some of the most exotic particles in physics as well as application towards spintronics and quantum computation. In all the known topological insulators, strong spin-orbit coupling is critical for the generation of the protected massless surface states. Consequently, a complete description of the Dirac state should include both the spin and orbital (spatial) parts of the wavefunction. For the family of materials with a single Dirac cone, theories and experiments agree qualitatively, showing the topological state has a chiral spin texture that changes handedness across the Dirac point (DP), but they differ quantitatively on how the spin is polarized. Limited existing theoretical ideas predict chiral local orbital angular momentum on the two sides of the DP. However, there have been neither direct measurements nor calculations identifying the global symmetry of the spatial wavefunction. Here we present the first results from angle-resolved photoemission experiment and first-principles calculation that both show, counter to current predictions, the in-plane orbital wavefunctions for the surface states of Bi2Se3 are asymmetric relative to the DP, switching from being tangential to the k-space constant energy surfaces above DP, to being radial to them below the DP. Because the orbital texture switch occurs exactly at the DP this effect should be intrinsic to the topological physics, constituting an essential yet missing aspect in the description of the topological Dirac state. Our results also indicate that the spin texture may be more complex than previously reported, helping to reconcile earlier conflicting spin resolved measurements.

cond-mat.mtrl-sci↗

arXiv2010

Uniaxial "nematic-like" electronic structure and Fermi surface of untwinned CaFe2As2

Obtaining the electronic structure of the newly discovered iron-based superconductors is the key to understanding the mechanism of their high-temperature superconductivity. We used angle-resolved photoemission spectroscopy (ARPES) to make direct measurements of the electronic structure and Fermi surface (FS) of the untwinned uniaxial state of CaFe2As2, the parent compound of iron-based superconductors. We observed unequal dispersions and FS geometries along the orthogonal Fe-Fe bond directions. More importantly, unidirectional straight and flat FS segments are observed near the zone center, which indicates the existence of a unidirectional nematic charge density wave order, strengthening the case for a quantum electronic liquid crystalline "nematic" phase. Further, the doping dependence extrapolates to a possible quantum critical point of the disappearance of this order in the heavily overdoped regime of these materials.

cond-mat.supr-con↗