Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “Mott insulator”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 181 records · Page 10
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

BCS-BEC crossover driven by small Fermi pockets of a high- T c cuprate superconductor

Fermi arcs observed in underdoped cuprates have sparked debate over whether they represent segments of a large Fermi surface or small Fermi pockets. This ambiguity has long hindered their classification as either the conventional Bardeen-Cooper-Schrieffer (BCS) regime or the strongly coupled Bose-Einstein condensation (BEC) crossover limit. Here, using angle-resolved photoemission spectroscopy and quantum oscillations, we demonstrate the coexistence of a small Fermi pocket and a large superconducting gap in the clean inner CuO 2 layers of the four-layer cuprate Ba 2 Ca 3 Cu 4 O 8 (F,O) 2 . This coexistence constitutes a hallmark of the BCS-BEC crossover and has remained elusive for decades. Despite the presence of antiferromagnetic (AF) order, the superconducting gap in the small pocket is remarkably large, yielding a gap-to-Fermi energy ratio (Δ pocket /ε F ~ 0.6) and a critical-to-Fermi temperature ratio (T c /T F ~ 0.13) that reach the theoretical upper bound for two-dimensional superconductivity. Unexpectedly, this BCS-BEC crossover emerges not as the carrier density decreases but as it increases, abruptly within a narrow doping range of less than 1%. These results provide a long-sought microscopic foundation for the d-wave pairing mechanism in doped AF-Mott insulators.

Jeong, Junhyeok [University of Tokyo, Kashiwa (Jap↗
DOE OSTI2020

Wannier–Koopmans method calculations for transition metal oxide band gaps

The widely used density functional theory (DFT) has a major drawback of underestimating the band gaps of materials. Wannier–Koopmans method (WKM) was recently developed for band gap calculations with accuracy on a par with more complicated methods. WKM has been tested for main group covalent semiconductors, alkali halides, 2D materials, and organic crystals. Here we apply the WKM to another interesting type of material system: the transition metal (TM) oxides. TM oxides can be classified as either with d 0 or d 10 closed shell occupancy or partially occupied open shell configuration, and the latter is known to be strongly correlated Mott insulators. We found that, while WKM provides adequate band gaps for the d0 and d10 TM oxides, it fails to provide correct band gaps for the group with partially occupied d states. This issue is also found in other mean-field approaches like the GW calculations. We believe that the problem comes from a strong interaction between the occupied and unoccupied d-state Wannier functions in a partially occupied d-state system. We also found that, for pseudopotential calculations including deep core levels, it is necessary to remove the electron densities of these deep core levels in the Hartree and exchange–correlation energy functional when calculating the WKM correction parameters for the d-state Wannier functions.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Adaptive finite differencing in high accuracy electronic structure calculations

Abstract A multi-order Adaptive Finite Differencing (AFD) method is developed for the kinetic energy operator in real-space, grid-based electronic structure codes. It uses atomic pseudo orbitals produced by the corresponding pseudopotential codes to optimize the standard finite difference (SFD) operators for improved precision. Results are presented for a variety of test systems and Bravais lattice types, including the well-known Δ test for 71 elements in the periodic table, the Mott insulator NiO, and borax decahydrate, which contains covalent, ionic, and hydrogen bonds. The tests show that an 8th-order AFD operator leads to the same average Δ value as that achieved by plane-wave codes and is typically far more accurate and has a much lower computational cost than a 12th-order SFD operator. The scalability of real-space electronic calculations is demonstrated for a 2016-atom NiO cell, for which the computational time decreases nearly linearly when scaled from 18 to 144 CPU-GPU nodes.

Briggs, E. L. (ORCID:0000000343983492)↗
DOE OSTI2020

The range of non-Kitaev terms and fractional particles in α-RuCl 3

Significant efforts have focused on the magnetic excitations of relativistic Mott insulators, predicted to realize the Kitaev quantum spin liquid (QSL). This exactly solvable model involves a highly entangled state resulting from bond-dependent Ising interactions that produce excitations which are non-local in terms of spin flips. A key challenge in real materials is identifying the relative size of the non-Kitaev terms and their role in the emergence or suppression of fractional excitations. Here, we identify the energy and temperature boundaries of non-Kitaev interactions by direct comparison of the Raman susceptibility of α-RuCl 3 with quantum Monte Carlo (QMC) results for the Kitaev QSL. Moreover, we further confirm the fractional nature of the magnetic excitations, which is given by creating a pair of fermionic quasiparticles. Interestingly, this fermionic response remains valid in the non-Kitaev range. Our results and focus on the use of the Raman susceptibility provide a stringent new test for future theoretical and experimental studies of QSLs.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Melting of charge order in the low-temperature state of an electronic ferroelectric-like system

Strong electronic interactions can drive a system into a state with a symmetry breaking. Lattice frustration or competing interactions tend to prevent symmetry breaking, leading to quantum disordered phases. In spin systems frustration can produce a spin liquid state. Frustration of a charge degree of freedom also can result in various exotic states, however, experimental data on these effects is scarce. In this work we demonstrate how in a Mott insulator on a weakly anisotropic triangular lattice a charge ordered state melts on cooling down to low temperatures. Raman scattering spectroscopy finds that κ -(BEDT-TTF) 2 Hg(SCN) 2 Cl enters an insulating “dipole solid” state at T =30K, but below T =15K the order melts, while preserving the insulating energy gap. Based on these observations, we suggest a phase diagram relevant to other quantum paraelectric materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Electromagnetic signatures of a chiral quantum spin liquid

Quantum spin liquids (QSL) have emerged as a captivating subject within interacting spin systems that exhibit no magnetic ordering even at the lowest temperature accessible experimentally. However, definitive experimental evidence remains elusive. In light of the recent surge in theoretical and experimental interest in the half-filled Hubbard model on a triangular lattice, which offers the potential for stabilizing a chiral QSL, we investigate the electromagnetic signatures of this phase to facilitate experimental detection. Utilizing a combination of parton mean-field theory and unbiased density-matrix renormalization group calculations, we systematically examine the electrical charge and orbital electrical current associated with a spinon excitation in the chiral QSL. Additionally, we calculate the longitudinal and transverse optical conductivities below the Mott gap. Furthermore, employing quantum field theory analysis, we unravel the connection between spinon excitations and emergent as well as physical gauge fields. Our results demonstrate that the chiral QSL phase exhibits a distinct electromagnetic response, even within a Mott insulator regime. This finding holds great potential for enabling the experimental detection of this long-sought-after phase.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Multipole polaron roams the devil’s staircase

We report Electron–boson interaction (EBI) has an important role in the properties of materials. Electron–phonon interaction in good metals can give rise to superconductivity, where electrons flow without dissipation below a critical temperature. In ionic crystals such as organic semiconductors, the coupling of low-energy electrons (or holes) with the atomic vibrations can drive the formation of polarons — an electron dressed with a phonon cloud, with lower mobility and heavy effective mass. The same notion can be applied to strongly correlated electron systems. Electron–spin fluctuation coupling drives unconventional superconductivity in high-temperature cuprates, iron-based superconductors and heavy-fermion systems. Magnetic polarons can form around charged dopants in an otherwise antiferromagnetic background of a Mott insulator, while an electron–polaron is also possible, via electron–plasmon coupling, when a Kondo hole is introduced in a heavy-fermion material, similar to a plasmaron in doped graphene.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Quantum control of Hubbard excitons

Quantum control of the many-body wavefunction is a central challenge in quantum materials research, as it could yield a precise control knob to manipulate emergent phenomena. Floquet engineering, the coherent dressing of quantum states with periodic non-resonant optical fields, has become an important strategy for quantum control. Most applications to solid-state systems have targeted weakly interacting or single-ion states, leaving the manipulation of many-body wavefunctions largely unexplored. Here, in this work, we use Floquet engineering to achieve quantum control of a strongly correlated Hubbard exciton in the one-dimensional Mott insulator Sr 2 CuO 3 . A nonresonant midinfrared optical field coherently dresses the exciton wavefunction, driving its rotation between bright and dark states. We use resonant third-harmonic generation to quantify ultrafast π/2 rotations on the Bloch sphere spanned by these exciton states. Our work advances the quest towards programmable control of correlated states and exciton-based quantum sensing.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Imaging local discharge cascades for correlated electrons in WS 2 /WSe 2 moiré superlattices

Transition metal dichalcogenide moiré heterostructures provide an ideal platform to explore the extended Hubbard model, where long-range Coulomb interactions play a critical role in determining strongly correlated electron states. This has led to experimental observations of Mott insulator states at half filling as well as a variety of extended Wigner crystal states at different fractional fillings. However, a microscopic understanding of these emerging quantum phases is still lacking. Here we describe a scanning tunnelling microscopy (STM) technique for the local sensing and manipulation of correlated electrons in a gated WS 2 /WSe 2 moiré superlattice, which enables the experimental extraction of fundamental extended Hubbard model parameters. We demonstrate that the charge state of the local moiré sites can be imaged by their influence on the STM tunnelling current. In addition to imaging, we are also able to manipulate the charge state of correlated electrons. When we ramp the bias on the STM tip, there is a local discharge cascade of correlated electrons in the moiré superlattice, which allows us to estimate the nearest-neighbour Coulomb interaction. Two-dimensional mapping of the moiré electron charge states also enables us to determine the on-site energy fluctuations at different moiré sites. Furthermore, our technique should be broadly applicable to many semiconductor moiré systems, offering a powerful tool for the microscopic characterization and control of strongly correlated states in moiré superlattices.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Evidence for a spinon Kondo effect in cobalt atoms on single-layer 1T-TaSe 2

Quantum spin liquids are highly entangled, disordered magnetic states that are expected to arise in frustrated Mott insulators and to exhibit exotic fractional excitations such as spinons and chargons. Despite being electrical insulators, some quantum spin liquids are predicted to exhibit gapless itinerant spinons that yield metallic behaviour in the charge-neutral spin channel. For this study, we deposited isolated magnetic atoms onto single-layer 1T-TaSe 2 , a candidate gapless spin liquid, to probe how itinerant spinons couple to impurity spin centres. Using scanning tunnelling spectroscopy, we observe the emergence of new, impurity-induced resonance peaks at the 1T-TaSe 2 Hubbard band edges when cobalt adatoms are positioned to have maximal spatial overlap with the local charge distribution. These resonance peaks disappear when the spatial overlap is reduced or when the magnetic impurities are replaced with nonmagnetic impurities. Theoretical simulations of a modified Anderson impurity model show that the observed peaks are consistent with a Kondo resonance induced by spinons combined with spin-charge binding effects that arise due to fluctuations of an emergent gauge field.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Evidence for chiral superconductivity on a silicon surface

Tin adatoms on a Si(111) substrate with a one-third monolayer coverage form a two-dimensional triangular lattice with one unpaired electron per site. These electrons order into an antiferromagnetic Mott-insulating state, but doping the Sn layer with holes creates a two-dimensional conductor that becomes superconducting at low temperatures. Although the pairing symmetry of the superconducting state is currently unknown, the combination of repulsive interactions and frustration inherent in the triangular adatom lattice opens up the possibility of a chiral order parameter. Here we study the superconducting state of Sn/Si(111) using scanning tunneling microscopy, scanning tunneling spectroscopy and quasiparticle interference imaging. Here we find evidence for a doping-dependent superconducting critical temperature with a fully gapped order parameter, the presence of time-reversal symmetry breaking and a strong enhancement in zero-bias conductance near the edges of the superconducting domains. Although each individual piece of evidence could have a more mundane interpretation, our combined results suggest the possibility that Sn/Si(111) is an unconventional chiral d-wave superconductor.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Signatures of moiré trions in WSe 2 /MoSe 2 heterobilayers

Moiré superlattices formed by van der Waals materials can support a wide range of electronic phases, including Mott insulators superconductors and generalized Wigner crystals2. When excitons are confined by a moiré superlattice, a new class of exciton emerges, which holds promise for realizing artificial excitonic crystals and quantum optical effects. When such moiré excitons are coupled to charge carriers, correlated states may arise. However, no experimental evidence exists for charge-coupled moiré exciton states, nor have their properties been predicted by theory. In this work, we report the optical signatures of trions coupled to the moiré potential in tungsten diselenide/molybdenum diselenide heterobilayers. The moiré trions show multiple sharp emission lines with a complex charge-density dependence, in stark contrast to the behaviour of conventional trions. We infer distinct contributions to the trion emission from radiative decay in which the remaining carrier resides in different moiré minibands. Variation of the trion features is observed in different devices and sample areas, indicating high sensitivity to sample inhomogeneity and variability. The observation of these trion features motivates further theoretical and experimental studies of higher-order electron correlation effects in moiré superlattices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

An electro-optical Mott neuron based on niobium dioxide

Various applications—including brain-like computing and on-chip artificial vision—increasingly demand a combination of electronic and photonic techniques. However, integrating both approaches on a single chip is challenging, and solutions typically rely on disparate components with power-hungry signal conversions. Here, in this paper, we report electro-optical Mott neurons that combine visible light emission with electrical threshold switching, as well as neuron-like oscillations. The devices are based on thin films of sputtered niobium dioxide (NbO 2 ), a Mott insulator–metal transition material, operating at room temperature and emitting light that peaks around 810 nm. Operando measurements reveal an electronic origin to the light emission: charge carrier relaxation initiated by high-field transport in the NbO 2 . Our devices combine electrical and optical functions within a single material, thereby expanding the options available for future artificial intelligence hardware.

electrical engineering↗
DOE OSTI2021

Layer-resolved many-electron interactions in delafossite PdCoO2 from standing-wave photoemission spectroscopy

Abstract When a three-dimensional material is constructed by stacking different two-dimensional layers into an ordered structure, new and unique physical properties can emerge. An example is the delafossite PdCoO 2 , which consists of alternating layers of metallic Pd and Mott-insulating CoO 2 sheets. To understand the nature of the electronic coupling between the layers that gives rise to the unique properties of PdCoO 2 , we revealed its layer-resolved electronic structure combining standing-wave X-ray photoemission spectroscopy and ab initio many-body calculations. Experimentally, we have decomposed the measured VB spectrum into contributions from Pd and CoO 2 layers. Computationally, we find that many-body interactions in Pd and CoO 2 layers are highly different. Holes in the CoO 2 layer interact strongly with charge-transfer excitons in the same layer, whereas holes in the Pd layer couple to plasmons in the Pd layer. Interestingly, we find that holes in states hybridized across both layers couple to both types of excitations (charge-transfer excitons or plasmons), with the intensity of photoemission satellites being proportional to the projection of the state onto a given layer. This establishes satellites as a sensitive probe for inter-layer hybridization. These findings pave the way towards a better understanding of complex many-electron interactions in layered quantum materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ultrafast signatures of spin and orbital order in antiferromagnetic α-Sr2CrO4

Abstract The antiferromagnetic Mott insulator α -Sr 2 CrO 4 possesses multiple spin and orbital ordered phases, but their unique interplay is still relatively unexplored. Here, we used femtosecond optical spectroscopy to study ultrafast spin and orbital ordering dynamics in α -Sr 2 CrO 4 through their non-equilibrium response to photoexcitation. By varying the pump photon energy, we selectively drove inter-site spin hopping between neighboring Cr t 2 g orbitals and charge transfer-type transitions between oxygen 2 p and Cr e g orbitals. The resulting transient reflectivity dynamics revealed temperature-dependent anomalies across the Néel temperature for spin ordering as well as the transition temperatures linked to different types of orbital order. Our results reveal distinct relaxation timescales for spin and orbital orders in α -Sr 2 CrO 4 and provide experimental evidence for the phase transition at T O , possibly related to antiferro-type orbital ordering.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Leveraging the redox activities of cerium and dibenzotetrathiafulvalene to discover a photo-responsive magnetic material

Stimuli-responsive changes in lanthanide-based materials are a promising research direction. In this study, [DBTTF] 4 [Ce 2 Cl 10 ] DBTTF = dibenzotetrathiafulvalene (1) was synthesized by a light-induced crystallization, where photo-oxidation of DBTTF enables formation of the cerium dimer [Ce 2 Cl 10 ] 4− . Intermolecular interactions between the stacked organic units of the crystal result in charge transfer bands in the visible-NIR (near-infrared) region, evident in the solid-state absorption spectrum upon comparison with the solution spectrum. The assignments of the sublattice oxidation states were made with single-crystal X-ray diffraction (SC-XRD) structural characterization, Raman spectroscopy, X-ray absorption spectroscopy, and magnetometry. Continuous 532 nm laser irradiation of the microcrystalline solid modulates the redox states in 1, leading to ∼40% reduction in the observed magnetization at 2 K. Density functional theory PBE+U/HSE06 band structure calculations predict Mott insulating behavior in 1, with a bandgap of 0.54/0.81 eV, and further support the conjecture that the observed photo-induced change in magnetization results from electron transfer from the [Ce 2 Cl 10 ] 4− anions to the π-stacked [DBTTF] 2 2+ organic dimer subunits. An enhancement in conductivity is similarly observed upon 532 nm irradiation, determined by single-crystal transport measurements. The findings reveal that photo-responsive lanthanide-based materials can be achieved by integration of redox-active organic moieties with redox-active lanthanide cations for the realization of switchable, photo-magnetic materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Magnetoelastic effects in the hyperhoneycomb Kitaev spin liquid

In recent years, several magnetic Mott insulators with strong spin-orbit coupling were suggested to be proximate to the Kitaev quantum spin liquid, whose one of the most exciting features is the fractionalization of spin excitations into itinerant Majorana fermions and static Z 2 fluxes. Unfortunately, the ground states of these systems cannot be easily captured by experiment, remaining featureless to conventional local probes. Here, we propose to study the signatures of fractionalized excitations by exploiting their coupling to the lattice vibrations, dubbed magnetoelastic coupling, which arises from the fact that the interaction between spins depends on the relative distance between them. We argue that the magnetoelastic coupling can lead to the distinct modification of the phonon dynamics, which can be observed by measuring renormalized phonon spectrum, the sound attenuation, and the phonon Hall viscosity. This makes the phonon dynamics a promising tool for the characterization and identification of quantum spin liquid phases. In this work, we focus on the magnetoelastic effects in the three-dimensional Kitaev model realized on the hyperhoneycomb lattice. Here, the hyperhoneycomb Kitaev spin liquid is particularly interesting since the strong Kitaev interaction was observed in the Kitaev magnet β-Li 2 IrO 3 , for which the spin-orbit entangled J eff = 1/2 moments of iridium ions form precisely the hyperhoneycomb lattice.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

An interface-controlled Mott memristor in α -RuCl 3

Memristor devices have history-dependent charge transport properties that are ideal for neuromorphic computing applications. We reveal a memristor material and mechanism in the layered Mott insulator α-RuCl 3 . The pinched hysteresis loops and S-shaped negative differential resistance in bulk crystals verify memristor behavior and are attributed to a nonlinear coupling between charge injection over a Schottky barrier at the electrical contacts and concurrent Joule heating. Direct simulations of this coupling can reproduce the device characteristics.

Physics↗