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Jonathan D. Denlinger

Publications and source records attributed to Jonathan D. Denlinger.

At least 55 records · Page 3Linked to original sources

Electric field driven octahedral rotation in perovskite

Rotation of MO6 (M = transition metal) octahedra is a key determinant of the physical properties of perovskite materials. Therefore, tuning physical properties, one of the most important goals in condensed matter research, may be accomplished by controlling octahedral rotation (OR). In this study, it is demonstrated that OR can be driven by an electric field in Sr$_2$RuO$_4$. Rotated octahedra in the surface layer of Sr$_2$RuO$_4$ are restored to the unrotated bulk structure upon dosing the surface with K. Theoretical investigation shows that OR in Sr$_2$RuO$_4$ originates from the surface electric field, which can be tuned via the screening effect of the overlaid K layer. This work establishes not only that variation in the OR angle can be induced by an electric field, but also provides a way to control OR, which is an important step towards in situ control of the physical properties of perovskite oxides.

cond-mat.mtrl-sci↗

Absence of a Dirac gap in ferromagnetic Cr$_x$(Bi$_{0.1}$Sb$_{0.9}$)$_{2-x}$Te$_3$

Magnetism breaks the time reversal symmetry expected to open a Dirac gap in 3D topological insulators that consequently leads to quantum anomalous Hall effect. The most common approach of inducing ferromagnetic state is by doping magnetic 3$d$ elements into bulk of 3D topological insulators. In Cr$_{0.15}$(Bi$_{0.1}$Sb$_{0.9}$)$_{1.85}$Te$_3$, the material where the quantum anomalous Hall effect was initially discovered at temperatures much lower than the ferromagnetic transition, $T_C$, the scanning tunneling microscopy studies have reported a large Dirac gap $\sim20-100$ meV. The discrepancy between the low temperature of quantum anomalous Hall effect ($\ll T_C$) and large spectroscopic Dirac gaps ($\gg T_C$) found in magnetic topological insulators remains puzzling. Here, we used angle-resolved photoemission spectroscopy to study the surface electronic structure of pristine and potassium doped surface of Cr$_{0.15}$(Bi$_{0.1}$Sb$_{0.9}$)$_{1.85}$Te$_3$. Upon potassium deposition, the $p$-type surface state of pristine sample was turned into an $n$-type, allowing spectroscopic observation of Dirac point. We find a gapless surface state, with no evidence of a large Dirac gap reported in tunneling studies.

cond-mat.mtrl-sci↗

A weak topological insulator state in quasi-one-dimensional superconductor TaSe$_3$

A well-established way to find novel Majorana particles in a solid-state system is to have superconductivity arising from the topological electronic structure. To this end, the heterostructure systems that consist of normal superconductor and topological material have been actively explored in the past decade. However, a search for the single material system that simultaneously exhibits intrinsic superconductivity and topological phase has been largely limited, although such a system is far more favorable especially for the quantum device applications. Here, we report the electronic structure study of a quasi-one-dimensional (q1D) superconductor TaSe$_3$. Our results of angle-resolved photoemission spectroscopy (ARPES) and first-principles calculation clearly show that TaSe$_3$ is a topological superconductor. The characteristic bulk inversion gap, in-gap state and its shape of non-Dirac dispersion concurrently point to the topologically nontrivial nature of this material. The further investigations of the Z$_2$ indices and the topologically distinctive surface band crossings disclose that it belongs to the weak topological insulator (WTI) class. Hereby, TaSe$_3$ becomes the first verified example of an intrinsic 1D topological superconductor. It hopefully provides a promising platform for future applications utilizing Majorana bound states localized at the end of 1D intrinsic topological superconductors.

cond-mat.supr-con↗

Crystalline symmetry-protected non-trivial topology in prototype compound BaAl$_4$

The BaAl$_4$ prototype crystal structure is the most populous of all structure types, and is the building block for a diverse set of sub-structures including the famous ThCr$_2$Si$_2$ family that hosts high-temperature superconductivity and numerous magnetic and strongly correlated electron systems. The MA$_4$ family of materials (M=Sr, Ba, Eu; A=Al, Ga, In) themselves present an intriguing set of ground states including charge and spin orders, but have largely been considered as uninteresting metals. Using electronic structure calculations, symmetry analysis and topological quantum chemistry techniques, we predict the exemplary compound BaAl$_4$ to harbor a three-dimensional Dirac spectrum with non-trivial topology and possible nodal lines crossing the Brillouin zone, wherein one pair of semi-Dirac points with linear dispersion along the $k_z$ direction and quadratic dispersion along the $k_x/k_y$ direction resides on the rotational axis with $C_{4v}$ point group symmetry. Electrical transport measurements reveal the presence of an extremely large, unsaturating positive magnetoresistance in BaAl$_4$ despite an uncompensated band structure, and quantum oscillations and angle-resolved photoemission spectroscopy measurements confirm the predicted multiband semimetal structure with pockets of Dirac holes and a Van Hove singularity (VHS) remarkably consistent with the theoretical prediction. We thus present BaAl$_4$ as a new topological semimetal, casting its prototype status into a new role as building block for a vast array of new topological materials.

cond-mat.mtrl-sci↗

Spin-orbit-controlled metal-insulator transition in Sr$_2$IrO$_4$

In the context of correlated insulators, where electron-electron interactions (U) drive the localization of charge carriers, the metal-insulator transition (MIT) is described as either bandwidth (BC) or filling (FC) controlled. Motivated by the challenge of the insulating phase in Sr$_2$IrO$_4$, a new class of correlated insulators has been proposed, in which spin-orbit coupling (SOC) is believed to renormalize the bandwidth of the half-filled $j_{\mathrm{eff}} = 1/2$ doublet, allowing a modest U to induce a charge-localized phase. Although this framework has been tacitly assumed, a thorough characterization of the ground state has been elusive. Furthermore, direct evidence for the role of SOC in stabilizing the insulating state has not been established, since previous attempts at revealing the role of SOC have been hindered by concurrently occurring changes to the filling. We overcome this challenge by employing multiple substituents that introduce well defined changes to the signatures of SOC and carrier concentration in the electronic structure, as well as a new methodology that allows us to monitor SOC directly. Specifically, we study Sr$_2$Ir$_{1-x}$T$_x$O$_4$ (T = Ru, Rh) by angle-resolved photoemission spectroscopy (ARPES), combined with ab-initio and supercell tight-binding calculations. This allows us to distinguish relativistic and filling effects, thereby establishing conclusively the central role of SOC in stabilizing the insulating state of Sr$_2$IrO$_4$. Most importantly, we estimate the critical value for spin-orbit coupling in this system to be $λ_c = 0.42 \pm 0.01$ eV, and provide the first demonstration of a spin-orbit-controlled MIT.

cond-mat.str-el↗

Low energy band structure and symmetries of UTe2 from angle resolved photoemission spectroscopy

The compound UTe2 has recently been shown to realize spin triplet superconductivity from a non-magnetic normal state. This has sparked intense research activity, including theoretical analyses that suggest the superconducting order parameter to be topologically nontrivial. However, the underlying electronic band structure is a critical factor for these analyses, and remains poorly understood. Here, we present high resolution angle resolved photoemission (ARPES) measurements covering multiple planes in the 3D Brillouin zone of UTe2, revealing distinct Fermi-level features from two orthogonal quasi-one dimensional light electron bands and one heavy band. The electronic symmetries are evaluated in comparison with numerical simulations, and the resulting picture is discussed as a platform for unconventional many-body order.

cond-mat.str-el↗

High temperature singlet-based magnetism from Hund's rule correlations

Uranium compounds can manifest a wide range of fascinating many-body phenomena, and are often thought to be poised at a crossover between localized and itinerant regimes for 5f electrons. The antiferromagnetic dipnictide USb2 has been of recent interest due to the discovery of rich proximate phase diagrams and unusual quantum coherence phenomena. Here, linear-dichroic X-ray absorption and elastic neutron scattering are used to characterize electronic symmetries on uranium in USb2 and isostructural UBi2. Of these two materials, only USb2 is found to enable strong Hund's rule alignment of local magnetic degrees of freedom, and to undergo distinctive changes in local atomic multiplet symmetry across the magnetic phase transition. Theoretical analysis reveals that these and other anomalous properties of the material may be understood by attributing it as the first known high temperature realization of a singlet ground state magnet, in which magnetism occurs through a process that resembles exciton condensation.

cond-mat.str-el↗

Orbital character effects in the photon energy and polarization dependence of pure C60 photoemission

Recent direct experimental observation of multiple highly-dispersive C$_{60}$ valence bands has allowed for a detailed analysis of the unique photoemission traits of these features through photon energy- and polarization-dependent measurements. Previously obscured dispersions and strong photoemission traits are now revealed by specific light polarizations. The observed intensity effects prove the locking in place of the C$_{60}$ molecules at low temperatures and the existence of an orientational order imposed by the substrate chosen. Most importantly, photon energy- and polarization-dependent effects are shown to be intimately linked with the orbital character of the C$_{60}$ band manifolds which allows for a more precise determination of the orbital character within the HOMO-2. Our observations and analysis provide important considerations for the connection between molecular and crystalline C$_{60}$ electronic structure, past and future band structure studies, and for increasingly popular C$_{60}$ electronic device applications, especially those making use of heterostructures.

cond-mat.mes-hall↗

Observation of highly dispersive bands in pure thin film C$_{60}$

While long-theorized, the direct observation of multiple highly dispersive C$_{60}$ valence bands has eluded researchers for more than two decades due to a variety of intrinsic and extrinsic factors. Here we report a realization of multiple highly dispersive (330-520 meV) valence bands in pure thin film C$_{60}$ on a novel substrate--the three-dimensional topological insulator Bi$_{2}$Se$_{3}$--through the use of angle-resolved photoemission spectroscopy (ARPES) and first-principles calculations. The effects of this novel substrate reducing C$_{60}$ rotational disorder are discussed. Our results provide important considerations for past and future band structure studies as well as the increasingly popular C$_{60}$ electronic device applications, especially those making use of heterostructures.

cond-mat.mes-hall↗

A setup for extreme-ultraviolet ultrafast angle-resolved photoelectron spectroscopy at 50-kHz repetition rate

Time- and angle-resolved photoelectron spectroscopy (trARPES) is a powerful method to track the ultrafast dynamics of quasiparticles and electronic bands in energy and momentum space. We present a setup for trARPES with 22.3 eV extreme-ultraviolet (XUV) femtosecond pulses at 50-kHz repetition rate, which enables fast data acquisition and access to dynamics across momentum space with high sensitivity. The design and operation of the XUV beamline, pump-probe setup, and UHV endstation are described in detail. By characterizing the effect of space-charge broadening, we determine an ultimate source-limited energy resolution of 60 meV, with typically 80-100 meV obtained at 1-2e10 photons/s probe flux on the sample. The instrument capabilities are demonstrated via both equilibrium and time-resolved ARPES studies of transition-metal dichalcogenides. The 50-kHz repetition rate enables sensitive measurements of quasiparticles at low excitation fluences in semiconducting MoSe$_2$, with an instrumental time resolution of 65 fs. Moreover, photo-induced phase transitions can be driven with the available pump fluence, as shown by charge density wave melting in 1T-TiSe$_2$. The high repetition-rate setup thus provides a versatile platform for sensitive XUV trARPES, from quenching of electronic phases down to the perturbative limit.

physics.ins-det↗

Evidence for quasi-one-dimensional charge density wave in CuTe by angle-resolved photoemission spectroscopy

We report the electronic structure of CuTe with a high charge density wave (CDW) transition temperature Tc = 335 K by angle-resolved photoemission spectroscopy (ARPES). An anisotropic charge density wave gap with a maximum value of 190 meV is observed in the quasi-one-dimensional band formed by Te px orbitals. The CDW gap can be filled by increasing temperature or electron doping through in situ potassium deposition. Combining the experimental results with calculated electron scattering susceptibility and phonon dispersion, we suggest that both Fermi surface nesting and electron-phonon coupling play important roles in the emergence of the CDW.

cond-mat.mtrl-sci↗

In-situ strain tuning of the Dirac surface states in Bi2Se3 films

Elastic strain has the potential for a controlled manipulation of the band gap and spin-polarized Dirac states of topological materials, which can lead to pseudo-magnetic-field effects, helical flat bands and topological phase transitions. However, practical realization of these exotic phenomena is challenging and yet to be achieved. Here, we show that the Dirac surface states of the topological insulator Bi2Se3 can be reversibly tuned by an externally applied elastic strain. Performing in-situ x-ray diffraction and in-situ angle-resolved photoemission spectroscopy measurements during tensile testing of epitaxial Bi2Se3 films bonded onto a flexible substrate, we demonstrate elastic strains of up to 2.1% and quantify the resulting reversible changes in the topological surface state. Our study establishes the functional relationship between the lattice and electronic structures of Bi2Se3 and, more generally, demonstrates a new route toward momentum-resolved mapping of strain-induced band structure changes.

cond-mat.mtrl-sci↗

Observation of a Topological Insulator Dirac Cone Reshaped by Non-magnetic Impurity Resonance

The massless Dirac electrons found at topological insulator surfaces are thought to be influenced very little by weak, non-magnetic disorder. However, a resonance effect of strongly perturbing non-magnetic impurities has been theoretically predicted to change the dispersion and physical nature of low-energy quasiparticles, resulting in unique particle-like states that lack microscopic translational symmetry. Here we report the direct observation of impurities reshaping the surface Dirac cone of the model 3D topological insulator Bi2Se3. For the first time, a pronounced kink-like dispersion feature is observed in disorder-enriched samples, and found to be closely associated with the anomaly caused by impurity resonance in the surface state density of states, as observed by dichroic angle resolved photoemission spectroscopy (ARPES). The experimental observation of these features, which closely resemble theoretical predictions, has significant implications for the properties of topological Dirac cones in applied scenarios that commonly feature point defect disorder at surfaces or interfaces.

cond-mat.mtrl-sci↗

Beyond Triplet: Unconventional Superconductivity in a Spin-3/2 Topological Semimetal

In all known fermionic superfluids, Cooper pairs are composed of spin-1/2 quasi-particles that pair to form either spin-singlet or spin-triplet bound states. The "spin" of a Bloch electron, however, is fixed by the symmetries of the crystal and the atomic orbitals from which it is derived, and in some cases can behave as if it were a spin-3/2 particle. The superconducting state of such a system allows pairing beyond spin-triplet, with higher spin quasi-particles combining to form quintet or septet pairs. Here, we report evidence of unconventional superconductivity emerging from a spin-3/2 quasiparticle electronic structure in the half-Heusler semimetal YPtBi, a low-carrier density noncentrosymmetric cubic material with a high symmetry that preserves the $p$-like $j=3/2$ manifold in the Bi-based $Γ_8$ band in the presence of strong spin-orbit coupling. With a striking linear temperature dependence of the London penetration depth, the existence of line nodes in the superconducting order parameter $Δ$ is directly explained by a mixed-parity Cooper pairing model with high total angular momentum, consistent with a high-spin fermionic superfluid state. We propose a $\mathbf{k\cdot p}$ model of the $j=3/2$ fermions to explain how a dominant $J$=3 septet pairing state is the simplest solution that naturally produces nodes in the mixed even-odd parity gap. Together with the underlying topologically non-trivial band structure, the unconventional pairing in this system represents a truly novel form of superfluidity that has strong potential for leading the development of a new generation of topological superconductors.

cond-mat.supr-con↗

A Novel Quasi-One-Dimensional Topological Insulator in Bismuth Iodide $β$-Bi$_4$I$_4$

Recent progress in the field of topological states of matter(1,2) has largely been initiated by the discovery of bismuth and antimony chalcogenide bulk topological insulators (TIs)(3-6), followed by closely related ternary compounds(7-16) and predictions of several weak TIs(17-19). However, both the conceptual richness of Z$_2$ classification of TIs as well as their structural and compositional diversity are far from being fully exploited. Here, a new Z$_2$ topological insulator is theoretically predicted and experimentally confirmed in the $β$-phase of quasi-one-dimensional bismuth iodide Bi$_4$I$_4$. The electronic structure of $β$-Bi$_4$I$_4$, characterized by Z$_2$ invariants (1;110), is in proximity of both the weak TI phase (0;001) and the trivial insulator phase (0;000). Our angle-resolved photoemission spectroscopy measurements on the (001) surface reveal a highly anisotropic band-crossing feature located at the point of the surface Brillouin zone and showing no dispersion with the photon energy, thus being fully consistent with the theoretical prediction.

cond-mat.mtrl-sci↗

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↗

Observation of monolayer valence band spin-orbit effect and induced quantum well states (QWS) in MoX2

Transition metal dichalcogenides have attracted much attention recently due to their potential applications in spintronics and photonics as a result of the indirect to direct band gap transition and the emergence of the spin-valley coupling phenomenon upon moving from the bulk to monolayer limit. Here, we report high-resolution angle-resolved photoemission spectroscopy on MoSe2 (molybdenum diselenide) single crystals and monolayer films of MoS2 grown on Highly Ordered Pyrolytic Graphite substrate. Our experimental results, for the first time, resolve the two distinct bands at the Brillouin zone corner of the bulk MoSe2, and provide evidence for the critically important spin-orbit split bands of the monolayer MoS2. Moreover, by depositing potassium on cleaved surfaces of these materials, the process through which quantum well states form on the surfaces of transition metal dichalcogenides is systematically imaged. We present a theoretical model to account for the observed spin-orbit splitting and the rich spectrum of the quantum well states observed in our experiments. Our findings taken together provide important insights into future applications of transition metal dichalcogenides in nanoelectronics, spintronics, and photonics devices as they critically depend on the spin-orbit physics of these materials.

cond-mat.mes-hall↗

SmB6 Photoemission: Past and Present

Recent renewed interest in the mixed valent insulator SmB6 comes from topological theory predictions and surface transport measurements of possible in-gap surface states whose existence is most directly probed by angle-resolved photoemission spectroscopy (ARPES). Early photoemission leading up to a recent flurry of ARPES studies of in-gap states is reviewed. Conflicting interpretations about the nature of the Sm 4f-5d hybridization gap and observed X-point bands between the f-states and the Fermi level are critically assessed using the important tools of photon polarization and spatial dependence which also provide additional insight into the origin of the more ambiguous Γ-point in-gap states.

cond-mat.str-el↗