arXiv subjects

K. Haule

Publications and source records attributed to K. Haule.

At least 19 recordsLinked to original sources

arXiv2022

Nonreciprocal directional dichroism at telecom wavelengths

Magnetoelectrics with ultra-low symmetry and spin-orbit coupling are well known to display a number of remarkable properties including nonreciprocal directional dichroism. As a polar and chiral magnet, Ni$_3$TeO$_6$ is predicted to host this effect in three fundamentally different configurations, although only two have been experimentally verified. Inspired by the opportunity to unravel the structure-property relations of such a unique light-matter interaction, we combined magneto-optical spectroscopy and first-principles calculations to reveal nonreciprocity in the toroidal geometry and compared our findings with the chiral configurations. We find that formation of Ni toroidal moments is responsible for the largest effects near 1.1 eV - a tendency that is captured by our microscopic model and computational implementation. At the same time, we demonstrate deterministic control of nonreciprocal directional dichroism in Ni$_3$TeO$_6$ across the entire telecom wavelength range. This discovery will accelerate the development of photonics applications that take advantage of unusual symmetry characteristics.

cond-mat.mtrl-sci↗

arXiv2022

Band-Mott mixing hybridizes the gap in Fe$_2$Mo$_3$O$_8$

We combined optical spectroscopy and first principles electronic structure calculations to reveal the charge gap in the polar magnet Fe$_2$Mo$_3$O$_8$. Iron occupation on the octahedral site draws the gap strongly downward compared to the Zn parent compound, and subsequent occupation of the tetrahedral site creates a narrow resonance near the Fermi energy that draws the gap downward even further. This resonance is a many-body effect that emanates from a flat valence band in a Mott-like state due to screening of the local moment - similar to expectations for a Zhang-Rice singlet, except that here, it appears in a semi-conductor. We discuss the unusual hybridization in terms of orbital occupation and character as well as the structure-property relationships that can be unveiled in various metal-substituted systems (Ni, Mn, Co, Zn).

cond-mat.str-el↗

arXiv2022

Global perspectives of the bulk electronic structure of URu$_2$Si$_2$ from angle-resolved photoemission

Previous high-resolution angle-resolved photoemission (ARPES) studies of URu$_2$Si$_2$ have characterized the temperature-dependent behavior of narrow-band states close to the Fermi level ($E_\mathrm{F}$) at low photon energies near the zone center, with an emphasis on electronic reconstruction due to Brillouin zone folding. A substantial challenge to a proper description is that these states interact with other hole-band states that are generally absent from bulk-sensitive soft x-ray ARPES measurements. Here we provide a more global $k$-space context for the presence of such states and their relation to the bulk Fermi surface topology using synchrotron-based wide-angle and photon energy-dependent ARPES mapping of the electronic structure using photon energies intermediate between the low-energy regime and the high-energy soft x-ray regime. Small-spot spatial dependence, $f$-resonant photoemission, Si 2$p$ core-levels, x-ray polarization, surface-dosing modification, and theoretical surface slab calculations are employed to assist identification of bulk versus surface state character of the $E_\mathrm{F}$-crossing bands and their relation to specific U- or Si-terminations of the cleaved surface. The bulk Fermi surface topology is critically compared to density functional theory and to dynamical mean field theory calculations. In addition to clarifying some aspects of the previously measured high symmetry $Γ$, Z and X points, incommensurate 0.6a* nested Fermi-edge states located along Z-N-Z are found to be distinctly different from the density functional theory Fermi surface prediction. The temperature evolution of these states above $T_{HO}$, combined with a more detailed theoretical investigation of this region, suggests a key role of the N-point in the hidden order transition.

cond-mat.str-el↗

arXiv2019

Protracted Kondo coherence with dilute carrier density in Cerium based nickel pnictides

Nozi$\grave{e}$res' exhaustion theory argues the temperature for coherently screening of all local moments in Kondo lattice could be much lower than the temperature of single moment screening with insufficient number of conduction electrons. Recent experiment [Luo et al, PNAS, 112,13520 (2015)] indicates the cerium based nickel pnictides $CeNi_{2-δ}As_2 (δ\approx0.28)$ with low carrier density is an ideal material to exam such protracted Kondo screening. Using the density functional theory and dynamical mean-field theory, we calculated the respective electronic structures of paramagnetic $CeNi_2As_2$/$CeNi_2P_2$. In contrast to structurally analogous layered iron pnictides, the electronic structures of the present systems show strong three-dimensionality with substantially small contributions of Ni-3d electrons to the carrier density. Moreover, we find significant Kondo resonance peaks in the compressed $CeNi_2As_2$ and $CeNi_2P_2$ at low temperatures, accompanied by topological changes of the Fermi surfaces. We also find similar quantum phase transition in $CeNi_2As_2$ driven by chemical pressure via the isovalence As$\rightarrow$P substitution.

cond-mat.str-el↗

arXiv2019

Spectroscopic and first principle DFT+eDMFT study of complex structural, electronic, and vibrational properties of $M_2$Mo$_3$O$_8$ ($M$=Fe, Mn) polar magnets

Optical spectroscopy, X-ray diffraction measurements, density functional theory (DFT) and density functional theory + embedded dynamical mean field theory (DFT+eDMFT) have been used to characterize structural and electronic properties of hexagonal $M_2$Mo$_3$O$_8$ ($M$=Fe, Mn) polar magnets. Our experimental data are consistent with the room temperature structure belonging to the space group P6$_3$mc for both compounds. The experimental structural and electronic properties at room temperature are well reproduced within DFT+eDMFT method, thus establishing its predictive power in the paramagnetic phase. With decreasing temperature, both compounds undergo a magnetic phase transition and we argue that this transition is concurrent with a structural phase transition (symmetry change from P6$_3$mc) in the Fe compound and an isostructural transition (no symmetry change from P6$_3$mc) in the Mn compound. In addition, the unusual temperature dependent behavior of electronic d-d transitions in Fe$^{2+}$ ions is discussed.

cond-mat.str-el↗

arXiv2019

The Mott-semiconducting state in the magic angle bilayer graphene

Using non-perturbative theoretical method, we address the problem of strong correlations in twisted bilayer-layer graphene at the magic angle. We concentrate on the solution without symmetry breaking, where conventional Mott insulating state is expected for all integer fillings. At Coulomb repulsion corresponding to dielectric constant $\varepsilon\approx 5$ and several integer fillings we find a Mott-semiconducting state, which simultaneously hosts the Mott state, and inside the Mott gap, a second much smaller semiconduting gap. The presence of these Mott-ingap states, which are located at the $Γ$ point, makes the Mott state strongly temperature dependent and leads to a bad-metal phase at elevated temperatures. The system is insulating at the charge neutrality point and at even fillings away from it.

cond-mat.str-el↗

arXiv2018

Investigation into the inadequacy of cRPA in reproducing screening in strongly correlated systems

The accuracy of the constrained random phase approximation(cRPA) method is examined in multi-orbital Hubbard models containing all possible on-site density-density interactions. Using DMFT, we show that the effective model constructed using cRPA fails to reproduce the spectral properties of the original full model in a wide parameter range. By comparing quantities such as the density of states and quasiparticle residues of the full and the effective models, we show that cRPA systematically overestimates the screening of Hubbard U for DMFT impurity solvers. We instead propose a new method to investigate the screening mechanism in the system using the local polarization, which is highly successful in reproducing spectra and also shows that the true screening is far less than that predicted by RPA. Furthermore, we compare the fully screened interaction $W$ given by RPA and our new method and show that the RPA $W$ is also overscreened and misses the signatures of local screening, which are clearly present in our new method.

cond-mat.str-el↗

arXiv2018

Thermal conductivity and electrical resistivity of solid iron at Earth's core conditions from first-principles

We compute the thermal conductivity and electrical resistivity of solid hcp Fe to pressures and temperatures of Earth's core. We find significant contributions from electron-electron scattering, usually neglected at high temperatures in transition metals. Our calculations show a quasi-linear relation between electrical resistivity and temperature for hcp Fe at extreme high pressures. We obtain thermal and electrical conductivities that are consistent with experiments considering reasonable error. The predicted thermal conductivity is reduced from previous estimates that neglect electron-electron scattering. Our estimated thermal conductivity for the outer core is 77$\pm$10 W/m/K, and is consistent with a geodynamo driven by thermal convection.

cond-mat.mtrl-sci↗

arXiv2018

Valence and Spin fluctuations in Mn-doped ferroelectric BaTiO3

We study Mn substitution for Ti in BaTiO3 with and without compensating oxygen vacancies using density functional theory (DFT) in combination with dynamical mean field theory (DMFT). We find strong charge and spin fluctuations. Without compensating oxygen vacancies, the ground state is found to be a quantum superposition of two distinct atomic valences, 3d4 and 3d5. Introducing a compensating oxygen vacancy at a neighboring site reduces both charge and spin fluctuations due to the reduction of electron hopping from Mn to its ligands. As a consequence, valence fluctuations are reduced, and is closely fixed to the high spin 3d5 state. Here we show that inclusion of charge and spin fluctuations is necessary to obtain an accurate ground state of transition metal doped ferroelectrics.

cond-mat.mtrl-sci↗

arXiv2017

How correlated is the FeSe/SrTiO$_3$ system ?

Recent observation of $\sim$ 10 times higher critical temperature in FeSe monolayer compared with its bulk phase has drawn a great deal of attention because the electronic structure in the monolayer phase appears to be different than bulk FeSe. Using a combination of density functional theory and dynamical mean field theory, we find electronic correlations have important effects on the predicted atomic-scale geometry and the electronic structure of the monolayer FeSe on SrTiO$_3$. The electronic correlations are dominantly controlled by the Se-Fe-Se angle either in the bulk phase or the monolayer phase. But the angle sensitivity increases and the orbital differentiation decreases in the monolayer phase compared to the bulk phase. The correlations are more dependent on Hund's J than Hubbard U. The observed orbital selective incoherence to coherence crossover with temperature confirms the Hund's metallic nature of the monolayer FeSe. We also find electron doping by oxygen vacancies in SrTiO$_3$ increases the correlation strength, especially in the $d_{xy}$ orbital by reducing the Se-Fe-Se angle.

cond-mat.supr-con↗

arXiv2017

Dynamic electronic correlation effects in NbO$_2$ as compared to VO$_2$

In this work we present a comparative investigation of the electronic structures of NbO$_2$ and VO$_2$ obtained within the combination of density functional theory and cluster-dynamical mean field theory calculations. We investigate the role of dynamic electronic correlations on the electronic structure of the metallic and insulating phases of NbO$_2$ and VO$_2$, with focus on the mechanism responsible for the gap opening in the insulating phases. For the rutile metallic phases of both oxides, we obtain that electronic correlations lead to strong renormalization of the $t_{2g}$ subbands, as well as the emergence of incoherent Hubbard subbands, signaling that electronic correlations are also important in the metallic phase of NbO$_2$. Interestingly, we find that nonlocal dynamic correlations do play a role in the gap formation of the (bct) insulating phase of NbO$_2$, by a similar physical mechanism as that recently proposed by us in the case of the (M$_1$) dimerized phase of VO$_2$ (\textit{Phys. Rev. Lett. 117, 056402 (2016)}). Although the effect of nonlocal dynamic correlations in the gap opening of bct phase is less important than in the (M$_1$ and M$_2$) monoclinic phases of VO$_2$, their presence indicates that the former is not a purely Peierls-type insulator, as it was recently proposed.

cond-mat.str-el↗

arXiv2016

Analogy between the "Hidden Order" and the Orbital Antiferromagnetism in URu$_{2-x}$Fe$_x$Si$_2$

We study URu$_{2-x}$Fe$_x$Si$_2$, in which two types of staggered phases compete at low temperature as the iron concentration $x$ is varied: the nonmagnetic "hidden order" (HO) phase below the critical concentration $x_c$, and unconventional antiferromagnetic (AF) phase above $x_c$. By using polarization resolved Raman spectroscopy, we detect a collective mode of pseudovector-like $A_{2g}$ symmetry whose energy continuously evolves with increasing $x$; it monotonically decreases in the HO phase until it vanishes at $x=x_c$, and then reappears with increasing energy in the AF phase. The mode's evolution provides direct evidence for unified order parameter for both nonmagnetic and magnetic phases arising from the orbital degrees-of-freedom of the uranium-5$f$ electrons.

cond-mat.str-el↗

arXiv2016

Orbital-differentiated coherence-incoherence crossover identified by photoemission spectroscopy in LiFeAs

In the iron-based superconductors (FeSCs), orbital differentiation is an important phenomenon, whereby correlations stronger on the dxy orbital than on the dxz/yz orbital yield quasi-particles with dxy} orbital character having larger mass renormalization and abnormal temperature evolution. However, the physical origin of this orbital differentiation is debated between the Hund's coupling induced unbinding of spin and orbital degrees of freedom and the Hubbard interaction instigated orbital selective Mott transition. Here we use angle-resolved photoemission spectroscopy to identify an orbital-dependent correlation-induced quasi-particle (QP) anomaly in LiFeAs. The excellent agreement between our photoemission measurements and first-principles many-body theory calculations shows that the orbital-differentiated QP lifetime anomalies in LiFeAs are controlled by the Hund's coupling.

cond-mat.str-el↗

arXiv2016

Metal-insulator Transition in VO2: a DFT+DMFT perspective

We present a theoretical investigation of the electronic structure of rutile (metallic) and M$_1$ and M$_2$ monoclinic (insulating) phases of VO$_2$ employing a fully self-consistent combination of density functional theory and embedded dynamical mean field theory calculations. We describe the electronic structure of the metallic and both insulating phases of VO$_2$, and propose a distinct mechanism for the gap opening. We show that Mott physics plays an essential role in all phases of VO$_2$: undimerized vanadium atoms undergo classical Mott transition through local moment formation (in the M$_2$ phase), while strong superexchange within V-dimers adds significant dynamic intersite correlations, which remove the singularity of self-energy for dimerized V-atoms. The resulting transition from rutile to dimerized M$_1$ phase is adiabatically connected to Peierls-like transition, but is better characterized as the Mott transition in the presence of strong intersite exchange. As a consequence of Mott physics, the gap in the dimerized M$_1$ phase is temperature dependent. The sole increase of electronic temperature collapses the gap, reminiscent of recent experiments.

cond-mat.str-el↗

arXiv2015

The Valence-Fluctuating Ground State of Plutonium

A central issue in material science is to obtain understanding of the electronic correlations that control complex materials. Such electronic correlations frequently arise due to the competition of localized and itinerant electronic degrees of freedom. While the respective limits of well-localized or entirely itinerant ground states are well-understood, the intermediate regime that controls the functional properties of complex materials continues to challenge theoretical understanding. We have used neutron spectroscopy to investigate plutonium, which is a prototypical material at the brink between bonding and non-bonding configurations. Our study reveals that the ground state of plutonium is governed by valence fluctuations, that is, a quantum-mechanical superposition of localized and itinerant electronic configurations as recently predicted by dynamical mean field theory. Our results not only resolve the long-standing controversy between experiment and theory on plutonium's magnetism, but also suggest an improved understanding of the effects of such electronic dichotomy in complex materials.

cond-mat.str-el↗

arXiv2015

First-principles study of the Kondo physics of a single Pu impurity in a Th host

Based on its condensed-matter properties, crystal structure, and metallurgy, which includes a phase diagram with six allotropic phases, plutonium is one of the most complicated pure elements in its solid state. Its anomalous properties, which are indicative of a very strongly correlated state, are related to its special position in the periodic table, which is at the boundary between the light actinides that have itinerant 5$f$ electrons and the heavy actinides that have localized 5$f$ electrons. As a foundational study to probe the role of local electronic correlations in Pu, we use the local-density approximation together with a continuous-time quantum Monte Carlo simulation to investigate the electronic structure of a single Pu atom that is either substitutionally embedded in the bulk and or adsorbed on the surface of a Th host. This is a simpler case than the solid phases of Pu metal, which must also include the interactions between Pu 5$f$ electrons on different Pu atoms. For the Pu impurity atom we have found a Kondo resonance peak, which is an important signature of electronic correlations, in the local density of states around the Fermi energy. Furthermore, we show that the peak width of this resonance is narrower for Pu atoms at the surface of Th than for those in the bulk due to a weakened Pu 5$f$-ligand hybridization at the surface.

cond-mat.str-el↗

arXiv2014

Fermi surface of IrTe2 in the valence-bond state as determined by quantum oscillations

We report the observation of the de Haas-van Alphen effect in IrTe2 measured using torque magnetometry at low temperatures down to 0.4 K and in high magnetic fields up to 33T. IrTe2 undergoes a major structural transition around 283 K due to the formation of planes of Ir and Te dimers that cut diagonally through the lattice planes, with its electronic structure predicted to change significantly from a layered system with predominantly three-dimensional character to a tilted quasi-two dimensional Fermi surface. Quantum oscillations provide direct confirmation of this unusual tilted Fermi surface and also reveal very light quasiparticle masses (less than 1 me), with no significant enhancement due to electronic correlations. We find good agreement between the angular dependence of the observed and calculated de Haas-van Alphen frequencies, taking into account the contribution of different structural domains that form while cooling IrTe2.

cond-mat.supr-con↗

arXiv2014

Chirality density wave of the 'hidden order' phase in URu$_2$Si$_2$

A second-order phase transition is associated with emergence of an "order parameter" and a spontaneous symmetry breaking. For the heavy fermion superconductor URu$_2$Si$_2$, the symmetry of the order parameter associated with its ordered phase below 17.5 K has remained ambiguous despite 30 years of research, and hence is called "hidden order" (HO). Here we use polarization resolved Raman spectroscopy to specify the symmetry of the low energy excitations above and below the HO transition. These excitations involve transitions between interacting heavy uranium 5f orbitals, responsible for the broken symmetry in the HO phase. From the symmetry analysis of the collective mode, we determine that the HO parameter breaks local vertical and diagonal reflection symmetries at the uranium sites, resulting in crystal field states with distinct chiral properties, which order to a commensurate chirality density wave ground state.

cond-mat.str-el↗