Lower Hubbard Band Research Articles

Gate-driven transition temperatures of electron hopping behaviors in Hubbard bands formed by dopant-induced QD array in silicon nanowire

Abstract Dopant atoms confined in silicon nanoscale channel can be ionized to form quantum dots (QDs). Several dopant atoms couple with each other forming energy bands, where the electron hopping behavior can be described by the Hubbard model. This characteristic renders dopant-induced quantum dots particularly appealing for applications in nanoelectronic and quantum devices. Herein we study the gate-driven transition temperatures of electron hopping behavior in upper and lower Hubbard bands formed by dopant-induced QD array in junctionless silicon nanowire transistors. The gate-dependent transition temperatures are calculated for three stages of electron hopping behaviors including Efros-Shklovskii Variable Range Hopping (ES-VRH), Mott Variable Range Hopping (Mott-VRH) and Nearest Neighbor Hopping (NNH). Our experimental results indicate that the ES-VRH in arrays of dopant atoms occurs in the domination of a long-range Coulomb interaction, in which the hopping distance relies on the Coulomb gap. Furthermore, the localization length of ES-VRH can be modulated by gate voltages.Those factors lead to the significant difference of transition temperatures between the upper and lower Hubbard bands. In addition, we find that the source-drain bias voltage can effectively modulate the transition temperatures between VRH and NNH by thermal activation energies under different bias voltages Vds.

Ce-4f as an electron-modulation reservoir weakening Fe-O bond to induce iron vacancies in CeFevNi hydroxide for enhancing oxygen evolution reaction

Designing novel rare-earth-transition metal composites is at the forefront of electrocatalyst research. However, the modulation of transition metal electronic structures by rare earths to induce vacancy defects and enhance electrochemical performance has rarely been reported. In this study, we systematically investigate the mechanism by which Ce-4f electron modulation weakens the Fe-O bond, thereby altering the electronic structure in CeFevNi hydroxide to improve oxygen evolution reaction (OER) performance. Theoretical calculations and experimental characterizations reveal that Ce-4f orbitals function as electron-modulation reservoirs, capable not only of retaining or donating electrons but also of influencing the material's electronic structure. Moreover, Ce-4f bands optimize the Fe lower Hubbard bands (LHB) and O-2p bands, leading to weakened Fe-O bonds and the formation of cationic vacancies. This change results in the upshift of the d-band center at the active sites, favoring the reaction energy barrier for oxygen intermediates in the OER process. The synthesized catalyst demonstrated an overpotential of 201 mV at 10 mA cm−2 and a lifetime exceeding 200 h at 100 mA cm−2 under alkaline conditions. This work offers a proof-of-concept for the application of the mechanism of rare earth-induced transition metal vacancy defects, providing a general guideline for the design and development of novel highly efficient catalysts.

Band Structure Engineering Promotes Anionic Redox Reversibility of Cobalt-Free Li-Rich Layered Oxides Cathodes.

Li-rich layered oxides cathodes (LLOs) have prevailed as the promising high-energy-density cathode materials due to their distinctive anionic redox chemistry. However, uncontrollable anionic redox process usually leads to structural deterioration and electrochemical degradation. Herein, a Mo/Cl co-doping strategy is proposed to regulate the relative position of energy band for modulating the anionic redox chemistry and strengthening the structural stability of Co-free Li1.16Mn0.56Ni0.28O2 cathodes. The incorporation of Mo with high d state orbit and Cl with low electronegativity can narrow the band energy gap between bonding and antibonding bands via increasing the filled lower-Hubbard band (LHB) and decreasing the non-bonding O 2p energy bands, promoting the anionic redox reversibility. In addition, strong covalent Mo─O and Mn─Cl bonding further increases the covalency of Mn─O band to further stabilize the O2 n- species and enhance the reversible distortion of MnO6 octahedron. The strengthening electronic conductivity, together with the epitaxial structure Li2MoO4 facilitates the fast Li+ kinetics. As a result, the dual doping material exhibits enhanced anionic redox reversibility and suppressed oxygen release with increased cyclic stability and excellent rate performance. This strategy provides some guidance to design high-energy-density LLOs with desirable anionic redox reversibility and stable crystal structure via band structure engineering.

Mapping charge excitations in generalized Wigner crystals.

Transition metal dichalcogenide-based moiré superlattices exhibit strong electron-electron correlations, thus giving rise to strongly correlated quantum phenomena such as generalized Wigner crystal states. Evidence of Wigner crystals in transition metal dichalcogenide moire superlattices has been widely reported from various optical spectroscopy and electrical conductivity measurements, while their microscopic nature has been limited to the basic lattice structure. Theoretical studies predict that unusual quasiparticle excitations across the correlated gap between upper and lower Hubbard bands can arise due to long-range Coulomb interactions in generalized Wigner crystal states. However, the microscopic proof of such quasiparticle excitations is challenging because of the low excitation energy of the Wigner crystal. Here we describe a scanning single-electron charging spectroscopy technique with nanometre spatial resolution and single-electron charge resolution that enables us to directly image electron and hole wavefunctions and to determine the thermodynamic gap of generalized Wigner crystal states in twisted WS2 moiré heterostructures. High-resolution scanning single-electron charging spectroscopy combines scanning tunnelling microscopy with a monolayer graphene sensing layer, thus enabling the generation of individual electron and hole quasiparticles in generalized Wigner crystals. We show that electron and hole quasiparticles have complementary wavefunction distributions and that thermodynamic gaps of ∼50 meV exist for the 1/3 and 2/3 generalized Wigner crystal states in twisted WS2.

A Suggestion Scheme to Reduce the Lower Hubbard Band and Increase the Tc of Unconventional Superconductor -- a Tip from Lk-99

A Suggestion Scheme to Reduce the Lower Hubbard Band and Increase the Tc of Unconventional Superconductor -- a Tip from Lk-99

Thermoelectric Power and Hall Effect in Correlated Metals and Doped Mott–Hubbard Insulators: DMFT Approximation

We present comparative theoretical investigation of thermoelectric power and Hall effect in the Hubbard model for correlated metal and Mott insulator (considered as prototype cuprate superconductor) for different concentrations of current carriers. Analysis is performed within standard DMFT approximation. For Mott insulator we consider the typical case of partial filling of the lower Hubbard band (hole doping). We calculate the dependence of thermopower on doping level and determine the critical concentration of carriers corresponding to sign change of thermopower. An anomalous dependence of thermopower on temperature is obtained significantly different from linear temperature dependence typical for the usual metals. The role of disorder scattering is analyzed on qualitative level. The comparison with similar studies of the Hall effect shows, that breaking of electron-hole symmetry leads to the appearance of the relatively large interval of band-fillings (close to the half-filling) where thermopower and Hall effects have different signs. We propose a certain scheme allowing to determine the number of carriers from ARPES data and perform semi-quantitative estimate of both thermopower and Hall coefficient using the usual DFT calculations of electronic spectrum.

Rubidium-induced phase transitions among metallic, band-insulating, Mott-insulating phases in 1T -TaS2

Realizing phase transitions via non-thermal sample manipulations is important not only for applications, but also for uncovering the underlying physics. Here, we report on the discovery of two distinct metal–insulator transitions in 1T-TaS2 via angle-resolved photoemission spectroscopy and in-situ rubidium deposition. At 205 K, the rubidium deposition drives a normal metal–insulator transition via filling electrons into the conduction band. While at 225 K, however, the rubidium deposition drives a bandwidth-controlled Mott transition as characterized by a rapid collapsing of Mott gap and a loss of spectral weight of the lower Hubbard band. Our result, from a doping-controlled perspective, succeeds in distinguishing the metallic, band-insulating, and Mott-insulating phases of 1T-TaS2, manifesting a delicate balance among the electron-itineracy, interlayer-coupling and Coulomb repulsion. We also establish an effective method to tune the balance between these interactions, which is useful in seeking exotic electronic phases and designing functional phase-changing devices.

Hall Effect in Doped Mott–Hubbard Insulator

We present theoretical analysis of Hall effect in doped Mott–Hubbard insulator, considered as a prototype of cuprate superconductor. We consider the standard Hubbard model within DMFT approximation. As a typical case we consider the partially filled (hole doping) lower Hubbard band. We calculate the doping dependence of both the Hall coefficient and Hall number and determine the value of carrier concentration, where Hall effect changes its sign. We obtain a significant dependence of Hall effect parameters on temperature. Disorder effects are taken into account in a qualitative way. We also perform a comparison of our theoretical results with some known experiments on doping dependence of Hall number in the normal state of YBCO and Nd-LSCO, demonstrating rather satisfactory agreement of theory and experiment. Thus the doping dependence of Hall effect parameters obtained within Hubbard model can be considered as an alternative to a popular model of the quantum critical point.

Hall Effect in Doped Mott–Hubbard Insulator

We present theoretical analysis of Hall effect in doped Mott-Hubbard insulator, considered as a prototype of cuprate superconductor. We consider the standard Hubbard model within DMFT approximation. As a typical case we consider the partially filled (hole doping) lower Hubbard band. We calculate the doping dependence of both the Hall coefficient and Hall number and determine the value of carrier concentration, where Hall effect changes its sign. We obtain a significant dependence of Hall effect parameters on temperature. Disorder effects are taken into account in a qualitative way.We also perform a comparison of our theoretical results with some known experiments on doping dependence of Hall number in the normal state of YBCO and Nd-LSCO, demonstrating rather satisfactory agreement of theory and experiment. Thus the doping dependence of Hall effect parameters obtained within Hubbard model can be considered as an alternative to a popular model of the quantum critical point.

Instanton gas approach to the Hubbard model

In this paper, we consider a path integral formulation of the Hubbard model based on a Hubbard-Stratonovich transformation that couples the auxiliary field to the local electronic density. This decoupling is known to have a saddle-point structure that shows a remarkable regularity: The field configuration at each saddle point can be understood in terms of a set of elementary field configurations localized in space and imaginary time which we coin instantons. The interaction between instantons is short ranged. Here, we formulate a classical partition function for the instanton gas that has predictive power. For a given set of physical parameters, we can predict the distribution of instantons and show that the instanton number is sharply defined in the thermodynamic limit, thereby defining a unique dominant saddle point. Decoupling in the charge channel conserves SU(2) spin symmetry for each field configurations. Hence, the instanton approach provides an SU(2) spin-symmetric approximation to the Hubbard model. It fails, however, to capture the magnetic transition inherent to the Hubbard model on the honeycomb lattice despite being able to describe local moment formation. In fact, the instanton itself corresponds to local moment formation and concomitant short-ranged antiferromagnetic correlations. This aspect is also seen in the single particle spectral function that shows clear signs of the upper and lower Hubbard bands. Our instanton approach bears remarkable similarities to local dynamical approaches, such as dynamical mean-field theory, in the sense that it has the unique property of allowing for local moment formation without breaking the SU(2) spin symmetry. In contrast to local approaches, it captures short-ranged magnetic fluctuations. Furthermore, it also offers possibilities for systematic improvements by taking into account fluctuations around the dominant saddle point. Finally, we show that the saddle point structure depends upon the choice of lattice geometry. For the square lattice at half filling, the saddle-point structure reflects the itinerant to localized nature of the magnetism as a function of the coupling strength. The implications of our results for Lefschetz thimble approaches to alleviate the sign problem are also discussed.

Transport spectroscopy from Hubbard bands of dopant-induced quantum dot array to one-dimensional conduction subband

Arrays of dopant-induced quantum dots (QDs) are promising candidates as quantum bit platforms. We have achieved quantum transport spectroscopy of a junctionless silicon (Si) nanowire transistor with dual physical channels with a diameter of 10 nm fabricated by novel femtosecond laser projection exposure together with thermal oxidation. The spectroscopy demonstrates the evolution of the quantum transport process from Hubbard bands of dopant-induced QD array to one-dimensional (1D) conduction subbands. Eight pairs of current splitting peaks were observed at the initial stage of the drain current, representing the upper and lower Hubbard bands formed by the coupling of eight QDs. The current oscillation peaks in the 1D conduction subband elucidate the interference of reflected electron waves between the gate-defined barriers, which are proved by the mean wave vector interval matching the gate length. Our experimental results demonstrate the evolution of the quantum transport process in sub 10 nm dual Si channels with randomly doped dopant atoms, opening a new perspective for quantum states by dopant band engineering in Si nanoscale devices for scalable quantum computation.

Magnetic impurity as a local probe of the U (1) quantum spin liquid with spinon Fermi surface

We solve the problem of a magnetic impurity coupled to a $U(1)$ quantum spin liquid with a spinon Fermi surface, and we compute the impurity spectral function. Using the slave rotor mean-field approach combined with gauge field fluctuations, we find that a peak located at the top of the lower Hubbard band and one at the bottom of the upper Hubbard band can emerge in the impurity spectral function. The peaks at the Hubbard band edges arise from the gauge field fluctuation-induced spinon-chargon binding inside the spinon Kondo screening cloud of the magnetic impurity. For a magnetic impurity embedded in a Mott insulator, our findings suggest that the emergence of a pair of peaks at the Hubbard band edges in the impurity density of states spectra provides strong evidence that the host Mott insulator is a $U(1)$ quantum spin liquid with a spinon Fermi surface.

Quantum Anomalous Hall Effect from Inverted Charge Transfer Gap

A general mechanism is presented by which topological physics arises in strongly correlated systems without flat bands. Starting from a charge transfer insulator, topology emerges when the charge transfer energy between the cation and anion is reduced to invert the lower Hubbard band and the spin-degenerate charge transfer band. A universal low-energy theory is developed for the inversion of the charge transfer gap in a quantum antiferromagnet. The inverted state is found to be a quantum anomalous Hall (QAH) insulator with noncoplanar magnetism. Interactions play two essential roles in this mechanism: producing the insulating gap and quasiparticle bands prior to the band inversion, and causing the change of magnetic order necessary for the QAH effect after inversion. Our theory explains the electric-field-induced transition from a correlated insulator to a QAH state in AB-stacked transition-metal-dichalcogenides bilayer MoTe2/WSe2.3 MoreReceived 3 November 2021Revised 24 January 2022Accepted 9 March 2022DOI:https://doi.org/10.1103/PhysRevX.12.021031Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasQuantum anomalous Hall effectPhysical SystemsBilayer filmsCharge-transfer insulatorsTransition metal dichalcogenidesTechniquesDensity matrix renormalization groupHartree-Fock methodsHubbard modelCondensed Matter, Materials & Applied Physics

Effect of Impurity on the Doping-Induced in-Gap States in a Mott Insulator

Motivated by the recent measurements of the spatial distribution of single particle excitation states in a hole-doped Mott insulator, we study the effects of impurity on the in-gap states, induced by the doped holes, in the Hubbard model on the square lattice by the cluster perturbation theory. We find that a repulsive impurity potential can move the in-gap state from the lower Hubbard band towards the upper Hubbard band, providing a good account for the experimental observation. The distribution of the spectral function in the momentum space can be used to discriminate the in-gap state induced by doped holes and that by the impurity. The spatial characters of the in-gap states in the presence of two impurities are also discussed and compared to the experiment.

Hall Effect in a Doped Mott Insulator: DMFT Approximation

In the framework of dynamical mean-field theory, we analyze the Hall effect in a doped Mott insulator as a parent cuprate superconductor. We consider the partial filling (hole doping) of the lower Hubbard band and calculate the dependence of the Hall coefficient and Hall number on hole doping, determining the critical concentration for sign change of the Hall coefficient. Significant temperature dependence of the Hall effect is noted. Good agreement is demonstrated with the concentration dependence of the Hall number obtained in experiments in the normal state of YBCO.

Charge dynamics in magnetically disordered Mott insulators

With the aid of both a semianalytical and a numerically exact method, we investigate the charge dynamics in the vicinity of half-filling in the one- and two-dimensional $t\text{\ensuremath{-}}J$ model derived from a Fermi-Hubbard model in the limit of large interaction $U$ and hence small exchange coupling $J$. The spin degrees of freedom are taken to be disordered. So we consider the limit $0<J\ensuremath{\ll}T\ensuremath{\ll}W$, where $W$ is the bandwidth. We focus on evaluating the local spectral density of a single hole excitation and the charge gap that separates the upper and the lower Hubbard band. We find indications that no band edges exist if the magnetic exchange is taken into account; instead of band edges, Gaussian tails seem to appear. A discussion of the underlying physics is provided.

Effect of strong intersite Coulomb interaction on the topological properties of a superconducting nanowire

For superconducting nanowire with the pairing of extended s-type symmetry, Rashba spin-orbit interaction in a magnetic field, the influence of strong intersite charge correlations on single-particle Majorana excitations is analyzed. This problem is investigated on the basis of the density matrix renormalization group numerical method. It is shown that with an increase in the repulsion intensity of electrons located at the neighboring sites, two subbands emerge in the lower Hubbard band of the open system. Based on calculations of the Majorana polarization and degeneracy of the entanglement spectrum, it was found that a topologically nontrivial phase with one edge state survives at the edge of each of the subbands where the concentration of electrons or holes is minimal. Keywords: superconducting nanowires, Majorana zero modes, strong electron correlations.

Effect of strong intersite Coulomb interaction on the topological properties of a superconducting nanowire

For superconducting nanowire with the pairing of extended s-type symmetry, Rashba spin-orbit interaction in a magnetic field, the influence of strong intersite charge correlations on single-particle Majorana excitations is analyzed. This problem is investigated on the basis of the density matrix renormalization group numerical method. It is shown that with an increase in the repulsion intensity of electrons located at the neighboring sites, two subbands emerge in the lower Hubbard band of the open system. Based on calculations of the Majorana polarization and degeneracy of the entanglement spectrum, it was found that a topologically nontrivial phase with one edge state survives at the edge of each of the subbands where the concentration of electrons or holes is minimal. Keywords: superconducting nanowires, Majorana zero modes, strong electron correlations.

Robust charge-density wave strengthened by electron correlations in monolayer 1T-TaSe2 and 1T-NbSe2

Combination of low-dimensionality and electron correlation is vital for exotic quantum phenomena such as the Mott-insulating phase and high-temperature superconductivity. Transition-metal dichalcogenide (TMD) 1T-TaS2 has evoked great interest owing to its unique nonmagnetic Mott-insulator nature coupled with a charge-density-wave (CDW). To functionalize such a complex phase, it is essential to enhance the CDW-Mott transition temperature TCDW-Mott, whereas this was difficult for bulk TMDs with TCDW-Mott < 200 K. Here we report a strong-coupling 2D CDW-Mott phase with a transition temperature onset of ~530 K in monolayer 1T-TaSe2. Furthermore, the electron correlation derived lower Hubbard band survives under external perturbations such as carrier doping and photoexcitation, in contrast to the bulk counterpart. The enhanced Mott-Hubbard and CDW gaps for monolayer TaSe2 compared to NbSe2, originating in the lattice distortion assisted by strengthened correlations and disappearance of interlayer hopping, suggest stabilization of a likely nonmagnetic CDW-Mott insulator phase well above the room temperature. The present result lays the foundation for realizing monolayer CDW-Mott insulator based devices operating at room temperature.

Electronic structure of SrTi1−xVxO3 films studied by in situ photoemission spectroscopy: Screening for a transparent electrode material

This study investigated the electronic structure of SrTi$_{1-x}$V$_x$O$_3$ (STVO) thin films, which are solid solutions of strongly correlated transparent conductive oxide (TCO) SrVO$_3$ and oxide semiconductor SrTiO$_3$, using ${in situ}$ photoemission spectroscopy. STVO is one of the most promising candidates for correlated-metal TCO because it has the capability of optimizing the performance of transparent electrodes by varying ${x}$. Systematic and significant spectral changes were found near the Fermi level (${E_{\rm F}}$) as a function of ${x}$, while the overall electronic structure of STVO is in good agreement with the prediction of band structure calculations. As ${x}$ decreases from 1.0, spectral weight transfer occurs from the coherent band near ${E_{\rm F}}$ to the incoherent states (lower Hubbard band) around 1.0-1.5 eV. Simultaneously, a pseudogap is formed at ${E_{\rm F}}$, indicating a significant reduction in quasiparticle spectral weight within close vicinity of ${E_{\rm F}}$. This pseudogap seems to evolve into an energy gap at ${x}$ = 0.4, suggesting the occurrence of a composition-driven metal-insulator transition. From angle-resolved photoemission spectroscopic results, the carrier concentration ${n}$ changes proportionally as a function of ${x}$ in the metallic range of ${x}$ = 0.6-1.0. In contrast, the mass enhancement factor, which is proportional to the effective mass (${m^*}$), does not change significantly with varying ${x}$. These results suggest that the key factor of ${n/m^*}$ in optimizing the performance of correlated-metal TCO is tuned by ${x}$, highlighting the potential of STVO to achieve the desired TCO performance in the metallic region.