Strong Electron-electron Interactions Research Articles

Realizing one-dimensional moiré chains with strong electron localization in two-dimensional twisted bilayer WSe2

Two-dimensional (2D) moiré systems based on twisted bilayer graphene and transition metal dichalcogenides provide a promising platform to investigate emergent phenomena driven by strong electron-electron interactions in partially filled flat bands. A natural question arises: Is it possible to expand the 2D correlated moiré physics to one-dimensional (1D) that electron-electron correlation is expected to be further enhanced? This requires selectively doping of 1D moiré chain, which seems to be not within the grasp of today's technology. Therefore, an experimental demonstration of the 1D moiré chain with partially filled electronic states remains absent. Here, we show that we can introduce 1D boundaries, separating two regions with different twist angles, in twisted bilayer WSe2 (tWSe2) by using scanning tunneling microscopy (STM) and demonstrate that the electronic states of 1D moiré sites along the boundaries can be selectively filled. The strong localized charge states of correlated moiré electrons in the 1D moiré chain can be directly imaged and manipulated by combining a back-gate voltage with the STM bias voltage. Our results open the door for realizing new correlated electronic states of the 1D moiré chain in 2D systems.

Quantum dot based Kitaev chains: Majorana quality measures and scaling with increasing chain length

Realizing Majorana bound states (MBSs) in short, well-controllable chains of coupled quantum dots sidesteps the problem of disorder but requires finetuning and does not give the true topological protection inherent to long chains. Here, we introduce a quality measure that is also applicable in the presence of strong electron-electron interactions and that quantifies the closeness to topological protection of finetuned MBSs in short quantum dot chains. We call this measure local distinguishability (LD) because it puts a bound to the degree an arbitrary local measurement can distinguish between two states. We study the LD for quantum dot chains of different length. The three-dot chain is studied in detail, and we find that it may not always be an improvement over the two-dot case, a fact that can be understood within an effective model derived from perturbation theory. For longer chains, the LD vanishes exponentially, signaling a transition to a topological phase with two ground states that cannot be distinguished by any local measurement. Published by the American Physical Society 2024

Singlet-Triplet Inversion in Triangular Boron Carbon Nitrides.

The discovery of singlet-triplet (ST) inversion in some π-conjugated triangle-shaped boron carbon nitrides is a remarkable breakthrough that defies Hund's first rule. Deeply rooted in strong electron-electron interactions, ST inversion has garnered significant interest due to its potential to revolutionize triplet harvesting in organic LEDs. Using the well-established Pariser-Parr-Pople model for correlated electrons in π-conjugated systems, we employ a combination of CISDT and restricted active space configuration interaction calculations to investigate the photophysics of several triangular boron carbon nitrides. Our findings reveal that ST inversion in these systems is primarily driven by a network of alternating electron-donor and electron-acceptor groups in the molecular rim, rather than by the triangular molecular structure itself.

Electronic States of Single Perovskite Quantum Dots in Weak and Strong Interaction Regimes: Implications in Electrically Pumped Quantum Emitters.

We investigate the effect of Coulomb interactions on the electronic states of a single perovskite quantum dot (PQD), CsPbBr3, through scanning tunneling microscopy/spectroscopy (STM/S). Under a weak interaction regime, where the time-averaged occupation of electrons in a PQD remains zero, the peaks observed in the differential tunneling conductance (dI/dV) spectrum correspond to the single-particle density of states (DOS) without any electron-electron correlation. However, with a shorter tunnel distance between the STM tip and PQD, additional electrons are trapped in the QD, leading to a strong interaction regime with well-defined electronic fine structures due to the lifting of spin degeneracy in the conduction bands. Interestingly, we observe that the strong Coulomb interaction can modify the spin-orbit coupling (SOC) strength in the PQDs. We have concluded that the energy levels under a strong electron-electron interaction regime are of utmost importance since they will be applicable to electrically pumped PQD-based single photon quantum emitters.

Measuring the Electronic Bandgap of Carbon Nanotube Networks in Non-Ideal p-n Diodes.

The measurement of the electronic bandgap and exciton binding energy in quasi-one-dimensional materials such as carbon nanotubes is challenging due to many-body effects and strong electron-electron interactions. Unlike bulk semiconductors, where the electronic bandgap is well known, the optical resonance in low-dimensional semiconductors is dominated by excitons, making their electronic bandgap more difficult to measure. In this work, we measure the electronic bandgap of networks of polymer-wrapped semiconducting single-walled carbon nanotubes (s-SWCNTs) using non-ideal p-n diodes. We show that our s-SWCNT networks have a short minority carrier lifetime due to the presence of interface trap states, making the diodes non-ideal. We use the generation and recombination leakage currents from these non-ideal diodes to measure the electronic bandgap and excitonic levels of different polymer-wrapped s-SWCNTs with varying diameters: arc discharge (~1.55 nm), (7,5) (0.83 nm), and (6,5) (0.76 nm). Our values are consistent with theoretical predictions, providing insight into the fundamental properties of networks of s-SWCNTs. The techniques outlined here demonstrate a robust strategy that can be applied to measuring the electronic bandgaps and exciton binding energies of a broad variety of nanoscale and quantum-confined semiconductors, including the most modern nanoscale transistors that rely on nanowire geometries.

Nonadiabatic dynamics of molecules interacting with metal surfaces: A quantum-classical approach based on Langevin dynamics and the hierarchical equations of motion.

A novel mixed quantum-classical approach to simulating nonadiabatic dynamics of molecules at metal surfaces is presented. The method combines the numerically exact hierarchical equations of motion approach for the quantum electronic degrees of freedom with Langevin dynamics for the classical degrees of freedom, namely, low-frequency vibrational modes within the molecule. The approach extends previous mixed quantum-classical methods based on Langevin equations to models containing strong electron-electron or quantum electronic-vibrational interactions, while maintaining a nonperturbative and non-Markovian treatment of the molecule-metal coupling. To demonstrate the approach, nonequilibrium transport observables are calculated for a molecular nanojunction containing strong interactions.

Highly entangled polyradical nanographene with coexisting strong correlation and topological frustration.

Open-shell nanographenes exhibit unconventional π-magnetism arising from topological frustration or strong electron-electron interaction. However, conventional design approaches are typically limited to a single magnetic origin, which can restrict the number of correlated spins or the type of magnetic ordering in open-shell nanographenes. Here we present a design strategy that combines topological frustration and electron-electron interactions to fabricate a large fully fused 'butterfly'-shaped tetraradical nanographene on Au(111). We employ bond-resolved scanning tunnelling microscopy and spin-excitation spectroscopy to resolve the molecular backbone and reveal the strongly correlated open-shell character, respectively. This nanographene contains four unpaired electrons with both ferromagnetic and anti-ferromagnetic interactions, harbouring a many-body singlet ground state and strong multi-spin entanglement, which is well described by many-body calculations. Furthermore, we study the magnetic properties and spin states in the nanographene using a nickelocene magnetic probe. The ability to imprint and characterize many-body strongly correlated spins in polyradical nanographenes paves the way for future advancements in quantum information technologies.

Role of Protons in and around Strongly Coupled Nitroxide Biradicals for Cross-Effect Dynamic Nuclear Polarization.

In magic angle spinning dynamic nuclear polarization (DNP), biradicals such as bis-nitroxides are used to hyperpolarize protons under microwave irradiation through the cross-effect mechanism. This mechanism relies on electron-electron spin interactions (dipolar coupling and exchange interaction) and electron-nuclear spin interactions (hyperfine coupling) to hyperpolarize the protons surrounding the biradical. This hyperpolarization is then transferred to the bulk sample via nuclear spin diffusion. However, the involvement of the protons in the biradical in the cross-effect DNP process has been under debate. In this work, we address this question by exploring the hyperpolarization pathways in and around bis-nitroxides. We demonstrate that for biradicals with strong electron-electron interactions, as in the case of the AsymPols, the protons on the biradical may not be necessary to quickly generate hyperpolarization. Instead, such biradicals can efficiently, and directly, polarize the surrounding protons of the solvent. The findings should impact the design of the next generation of biradicals.

Electron pairing and nematicity in LaAlO3/SrTiO3 nanostructures

Strongly correlated electronic systems exhibit a wealth of unconventional behavior stemming from strong electron-electron interactions. The LaAlO3/SrTiO3 (LAO/STO) heterostructure supports rich and varied low-temperature transport characteristics including low-density superconductivity, and electron pairing without superconductivity for which the microscopic origins is still not understood. LAO/STO also exhibits inexplicable signatures of electronic nematicity via nonlinear and anomalous Hall effects. Nanoscale control over the conductivity of the LAO/STO interface enables mesoscopic experiments that can probe these effects and address their microscopic origins. Here we report a direct correlation between electron pairing without superconductivity, anomalous Hall effect and electronic nematicity in quasi-1D ballistic nanoscale LAO/STO Hall crosses. The characteristic magnetic field at which the Hall coefficient changes directly coincides with the depairing of non-superconducting pairs showing a strong correlation between the two distinct phenomena. Angle-dependent Hall measurements further reveal an onset of electronic nematicity that again coincides with the electron pairing transition, unveiling a rotational symmetry breaking due to the transition from paired to unpaired phases at the interface. The results presented here highlights the influence of preformed electron pairs on the transport properties of LAO/STO and provide evidence of the elusive pairing “glue” that gives rise to electron pairing in SrTiO3-based systems.

Mott insulators with boundary zeros

The topological classification of electronic band structures is based on symmetry properties of Bloch eigenstates of single-particle Hamiltonians. In parallel, topological field theory has opened the doors to the formulation and characterization of non-trivial phases of matter driven by strong electron-electron interaction. Even though important examples of topological Mott insulators have been constructed, the relevance of the underlying non-interacting band topology to the physics of the Mott phase has remained unexplored. Here, we show that the momentum structure of the Green’s function zeros defining the “Luttinger surface" provides a topological characterization of the Mott phase related, in the simplest description, to the one of the single-particle electronic dispersion. Considerations on the zeros lead to the prediction of new phenomena: a topological Mott insulator with an inverted gap for the bulk zeros must possess gapless zeros at the boundary, which behave as a form of “topological antimatter” annihilating conventional edge states. Placing band and Mott topological insulators in contact produces distinctive observable signatures at the interface, revealing the otherwise spectroscopically elusive Green’s function zeros.

Effect of electron-electron interaction on polarization process of exciton and biexciton in conjugated polymers

Abstract By using the one-dimensional tight-binding model modified to include electron-electric field interaction and electron-electron interaction, we theoretically explore the polarization process of exciton and biexciton in cis-polyacetylene. The dynamical simulation is performed by adopting the non-adiabatic evolution approach. The results show that under the effect of moderate electric field, when the strength of electron-electron interaction is weak, the singlet exciton is stable but its polarization presents obvious oscillation. With the enhancement of interaction, it is dissociated into polaron pair, the spin-flip of which could be observed through modulating the interaction strength. For the triplet exciton, the strong electron-electron interaction restrains its normal polarization, but it is still stable. In case of biexciton, the strong electron-electron interaction not only dissociate it, but also flip its charge distribution. We also calculate the yield of the possible states formed after the dissociation of exciton and biexciton.

Robust Luttinger Liquid State of 1D Dirac Fermions in a Van der Waals System Nb9Si4Te18.

We report on the Tomonaga-Luttinger liquid (TLL) behavior in fully degenerate 1D Dirac Fermions. A ternary van der Waals material Nb9Si4Te18 incorporates in-plane NbTe2 chains, which produce a 1D Dirac band crossing Fermi energy. Tunneling conductance of electrons confined within NbTe2 chains is found to be substantially suppressed at Fermi energy, which follows a power law with a universal temperature scaling, hallmarking a TLL state. The obtained Luttinger parameter of ∼0.15 indicates a strong electron-electron interaction. The TLL behavior is found to be robust against atomic-scale defects, which might be related to the Dirac electron nature. These findings, combined with the tunability of the compound and the merit of a van der Waals material, offer a robust, tunable, and integrable platform to exploit non-Fermi liquid physics.

Signatures of fractional quantum anomalous Hall states in twisted MoTe2.

The interplay between spontaneous symmetry breaking and topology can result in exotic quantum states of matter. A celebrated example is the quantum anomalous Hall (QAH) state, which exhibits an integer quantum Hall effect at zero magnetic field owing to intrinsic ferromagnetism1-3. In the presence of strong electron-electron interactions, fractional QAH (FQAH) states at zero magnetic field can emerge4-8. These states could host fractional excitations, including non-Abelian anyons-crucial building blocks for topological quantum computation9. Here we report experimental signatures of FQAH states in a twisted molybdenum ditelluride (MoTe2) bilayer. Magnetic circular dichroism measurements reveal robust ferromagnetic states at fractionally hole-filled moiré minibands. Using trion photoluminescence as a sensor10, we obtain a Landau fan diagram showing linear shifts in carrier densities corresponding to filling factor v = -2/3 and v = -3/5 ferromagnetic states with applied magnetic field. These shifts match the Streda formula dispersion of FQAH states with fractionally quantized Hall conductance of [Formula: see text] and [Formula: see text], respectively. Moreover, the v = -1 state exhibits a dispersion corresponding to Chern number -1, consistent with the predicted QAH state11-14. In comparison, several non-ferromagnetic states on the electron-doping side do not disperse, that is, they are trivial correlated insulators. The observed topological states can be electrically driven into topologically trivial states. Our findings provide evidence of the long-sought FQAH states, demonstrating MoTe2 moiré superlattices as a platform for exploring fractional excitations.

Exceptional van Hove singularities in pseudogapped metals

Motivated by the pseudogap state of the cuprates, we introduce the concept of an ``exceptional'' van Hove singularity that appears when a strong electron-electron interaction splits an otherwise simply connected Fermi surface into multiply connected pieces. The singularity describes the touching of two pieces of the split Fermi surface. We show that this singularity is proximate to a second-order van Hove singularity, which can be accessed by tuning a dispersion parameter. We argue that, in a wide class of cuprates, the endpoint of the pseudogap is accessed only by triggering the exceptional van Hove singularity. The resulting Lifshitz transition is characterized by enhanced specific heat and nematic susceptibility, as seen in experiments.

Origin of the anomalous spin resonance in a strongly correlated electron system

We study the origin of the anomalous spin resonance detected electrically in a strongly correlated two-dimensional electron system. Such resonance reveals itself around nominally nonmagnetic even filling factors $\ensuremath{\nu}$ of the integer quantum Hall effect and is a consequence of strong electron-electron interactions. We directly demonstrate that while the spin resonance at odd $\ensuremath{\nu}$ manifests itself as an increase in the longitudinal resistance of the two-dimensional channel induced by the usual heating due to the radiation absorption, the anomalous resonance around even fillings is detected as a drop in the resistance, as if the electron system is cooled. In contrast, if the magnetic field is tilted so that the ground state of the system becomes ferromagnetic at even $\ensuremath{\nu}$, the spin resonance around even fillings turns to a more conventional ``heating''-like behavior. Analysis of both the evolution of the spin resonance with increasing tilt angle and the measured temperature dependencies allowed us to put forth a possible mechanism of anomalous spin resonance around even fillings that qualitatively explains all of the puzzling experimental findings.

Pairing of holes by confining strings in antiferromagnets

In strongly correlated quantum materials, the behavior of charge carriers is dominated by strong electron-electron interactions. These can lead to insulating states with spin order, and upon doping to competing ordered states including unconventional superconductivity. The underlying pairing mechanism remains poorly understood however, even in strongly simplified theoretical models. Recent advances in quantum simulation allow to study pairing in paradigmatic settings, e.g. in the t-Jt−J and t-J_zt−Jz Hamiltonians. Even there, the most basic properties of paired states of only two dopants, such as their dispersion relation and excitation spectra, remain poorly studied in many cases. Here we provide new analytical insights into a possible string-based pairing mechanism of mobile holes in an antiferromagnet. We analyze an effective model of partons connected by a confining string and calculate the spectral properties of bound states. Our model is equally relevant for understanding Hubbard-Mott excitons consisting of a bound doublon-hole pair or confined states of dynamical matter in lattice gauge theories, which motivates our study of different parton statistics. Although an accurate semi-analytic estimation of binding energies is challenging, our theory provides a detailed understanding of the internal structure of pairs. For example, in a range of settings we predict heavy states of immobile pairs with flat-band dispersions - including for the lowest-energy dd-wave pair of fermions. Our findings shed new light on the long-standing question about the origin of pairing and competing orders in high-temperature superconductors.

Jellybean Quantum Dots in Silicon for Qubit Coupling and On-Chip Quantum Chemistry.

The small size and excellent integrability of silicon metal-oxide-semiconductor (SiMOS) quantum dot spin qubits make them an attractive system for mass-manufacturable, scaled-up quantum processors. Furthermore, classical control electronics can be integrated on-chip, in-between the qubits, if an architecture with sparse arrays of qubits is chosen. In such an architecture qubits are either transported across the chip via shuttling or coupled via mediating quantum systems over short-to-intermediate distances. This paper investigates the charge and spin characteristics of an elongated quantum dot-a so-called jellybean quantum dot-for the prospects of acting as a qubit-qubit coupler. Charge transport, charge sensing, and magneto-spectroscopy measurements are performed on a SiMOS quantum dot device at mK temperature and compared to Hartree-Fock multi-electron simulations. At low electron occupancies where disorder effects and strong electron-electron interaction dominate over the electrostatic confinement potential, the data reveals the formation of three coupled dots, akin to a tunable, artificial molecule. One dot is formed centrally under the gate and two are formed at the edges. At high electron occupancies, these dots merge into one large dot with well-defined spin states, verifying that jellybean dots have the potential to be used as qubit couplers in future quantum computingarchitectures.

Fractional second-order topological insulator from a three-dimensional coupled-wires construction

We construct a three-dimensional second-order topological insulator with gapless helical hinge states from an array of weakly tunnel-coupled Rashba nanowires. For suitably chosen interwire tunnelings, we demonstrate that the system has a fully gapped bulk as well as fully gapped surfaces, but hosts a Kramers pair of gapless helical hinge states propagating along a path of hinges that is determined by the hierarchy of interwire tunnelings and the boundary termination of the system. Furthermore, the coupled-wires approach allows us to incorporate electron-electron interactions into our description. At suitable filling factors of the individual wires, we show that sufficiently strong electron-electron interactions can drive the system into a fractional second-order topological insulator phase with hinge states carrying only a fraction $e/p$ of the electronic charge $e$ for an odd integer $p$.

Coherent control of the photoinduced transition in a strongly correlated material

The use of intense tailored light fields is the perfect tool to achieve ultrafast control of electronic properties in quantum materials. Among them, Mott insulators are materials in which strong electron-electron interactions drive the material into an insulating phase. When shining a Mott insulator with a strong laser pulse, the electric field may induce the creation of doublon-hole pairs, triggering a photoinduced transition into a metallic state. In this paper, we take advantage of the threshold character of this photoinduced transition and we propose a setup that consists of a midinfrared laser pulse and a train of short pulses separated by a half period of the midinfrared with alternating phases. By varying the time delay between the two pulses and the internal carrier envelope phase of the short pulses, we achieve control of the phase transition, which leaves its fingerprint at its high harmonic spectrum.

Valleytronic full configuration-interaction approach: Application to the excitation spectra of Si double-dot qubits

The influence of strong electron-electron interactions and Wigner-molecule (WM) formation on the spectra of $2e$ singlet-triplet double-dot Si qubits is presented based on a full configuration interaction (FCI) approach that incorporates the valley degree of freedom (VDOF) in the context of the continuous (effective mass) description of semiconductor materials. Our FCI treats the VDOF as an isospin in addition to the regular spin. Our treatment is able to assign to each energy curve in the qubit's spectrum a complete set of good quantum numbers for both the spin and the valley isospin. This reveals an underlying SU(4) $\supset$ SU(2) $\times$ SU(2) group-chain organization in the Si double-dot spectra. With parameters in the range of actual experimental situations, we demonstrate in a double-dot qubit that, in the (2,0) charge configuration and compared to the expected large, and dot-size determined, single-particle (orbital) energy gap, the strong $e-e$ interactions drastically quench the spin-singlet$-$spin-triplet energy gap, $E_{\rm ST}$, within the same valley, making it competitive to the small energy gap, $E_V$, between the two valleys. We present results for both the $E_{\rm ST} < E_V$ and $E_{\rm ST} > E_V$ cases. We investigate the spectra as a function of detuning and demonstrate the strengthening of the avoided crossings due to a lowering of the interdot barrier and/or the influence of valley-orbit coupling. We further demonstrate, as a function of an applied magnetic field, the emergence of avoided crossings in the (1,1) charge configuration due to the spin-valley coupling. The valleytronic FCI formulated here, and implementeded for two electrons confined in a tunable double quantum dot, offers also a most effective tool for analyzing the spectra of Si qubits with more than two wells and/or more than two electrons.