Long-range Electron-electron Interactions Research Articles

Long-range electron-electron interactions in quantum dot systems and applications in quantum chemistry

Long-range interactions play a key role in several phenomena of quantum physics and chemistry. To study these phenomena, analog quantum simulators provide an appealing alternative to classical numerical methods. Gate-defined quantum dots have been established as a platform for quantum simulation, but for those experiments the effect of long-range interactions between the electrons did not play a crucial role. Here we present the first detailed experimental characterization of long-range electron-electron interactions in an array of gate-defined semiconductor quantum dots. We demonstrate significant interaction strength among electrons that are separated by up to four sites, and show that our theoretical prediction of the screening effects matches well the experimental results. Based on these findings, we investigate how long-range interactions in quantum-dot arrays may be utilized for analog simulations of artificial quantum matter. We numerically show that about ten quantum dots are sufficient to observe binding for a one-dimensional $H_2$-like molecule. These combined experimental and theoretical results pave the way for future quantum simulations with quantum dot arrays and benchmarks of numerical methods in quantum chemistry.

One-dimensional excitons in long phosphorene atomic chains

The electronic structure of phosphorene atomic chains (PACs) embedded in various dielectric environments is studied theoretically by using a configuration interaction approach beyond the conventional double-excitation scheme. While the nominal single-particle gap of the PACs is shown to roughly obey an expected scaling law of ${L}^{\ensuremath{-}2}$, where $L$ measures the length of PACs, the quasiparticle shift is found to gradually converge to a value that is insensitive to the dielectric environment as $L$ increases. In the meantime, exciton binding energies are revealed to obey a simple scaling law of $0.96/(\ensuremath{\kappa}L)\ensuremath{-}0.02$, with $\ensuremath{\kappa}$ being the effective dielectric constant. As $L$ goes to infinity, the quasiparticle and excitonic effect are both found to be greatly suppressed as if the long-range electron-electron interactions are quenched in long PACs.

Band structure and superconductivity in twisted trilayer graphene

We study the symmetries of twisted trilayer graphene's band structure under various extrinsic perturbations, and analyze the role of long-range electron-electron interactions near the first magic angle. The electronic structure is modified by these interactions in a similar way to twisted bilayer graphene. We analyze electron pairing due to long-wavelength charge fluctuations, which are coupled among themselves via the Coulomb interaction and additionally mediated by longitudinal acoustic phonons. We find superconducting phases with either spin-singlet/valley-triplet or spin-triplet/valley-singlet symmetry, with critical temperatures up to a few Kelvin for realistic choices of parameters.

Negative quasiparticle shifts in phosphorene quantum dots

It is commonly believed that electron correlations would open up a quasiparticle gap in semiconductors. Contrary to this intuitive expectation, here we reveal that phosphorene quantum dots (PQDs) may exhibit just the opposite effect. By using a configuration interaction approach beyond the conventional double-excitation scheme, quasiparticle energies are calculated for hexagonal and rectangular PQDs in various dielectric environments. For the hexagonal PQD with a nominal gap of 2.26 eV, it is found that the quasiparticle shift decreases by more than 500 meV and eventually becomes negative when the effective dielectric constant is reduced from 20.0 to 5.0. For other trapezoidal, triangular, and rectangular PQDs, the quasiparticle shift exhibits a similar amount of decrement after the same change in the dielectric environment. Furthermore, the calculation by adopting the Rytova-Keldysh potential, which may be more suitable to describe two-dimensional screening, also shows a very similar result, although with smaller decrement of the quasiparticle shift. The origin of this anomalous quasiparticle shift is believed to be related to the long-range electron-electron interactions in the distinctive lattice structure of PQDs, as a similar phenomenon has never been found in graphene quantum dots.

Coulomb interactions and renormalization of semi-Dirac fermions near a topological Lifshitz transition

We aim to understand how the spectrum of semi-Dirac fermions is renormalized due to long-range Coulomb electron-electron interactions at a topological Lifshitz transition, where two Dirac cones merge. At the transition, the electronic spectrum is characterized by massive quadratic dispersion in one direction, while it remains linear in the other. We have found that, to lowest order, the unconventional log squared (double logarithmic) correction to the quasiparticle mass in bare perturbation theory leads to resummation into strong mass renormalization in the exact full solution of the perturbative renormalization group equations. This behavior effectively wipes out the curvature of the dispersion and leads to Dirac cone restoration at low energy: the system flows towards Dirac dispersion which is anisotropic but linear in momentum, with interaction-depended logarithmic modulation. The Berry phase associated with the restored critical Dirac spectrum is zero - a property guaranteed by time-reversal symmetry and unchanged by renormalization. Our results are in contrast with the behavior that has been found within the large-$N$ approach.

Excited States and Optical Properties of Hydrogen-Passivated Rectangular Graphenes: A Computational Study

In this paper, we perform large-scale electron-correlated calculations of optoelectronic properties of rectangular graphene-like polycyclic aromatic hydrocarbon molecules. Theoretical methodology employed in this work is based upon Pariser-Parr-Pople (PPP) π-electron model Hamiltonian, which includes long-range electron-electron interactions. Electron-correlation effects were incorporated using multi-reference singles-doubles configurationinteraction (MRSDCI) method, and the ground and excited state wave functions thus obtained were employed to calculate the linear optical absorption spectra of these molecules, within the electric-dipole approximation. As far as the ground state wave functions of these molecules are concerned, we find that with the increasing size, they develop a strong diradical open-shell character. Our results on optical absorption spectra are in very good agreement with the available experimental results, outlining the importance of electron-correlation effects in accurate description of the excited states. In addition to the optical gap, spin gap of each molecule was also computed using the same methodology. Calculated spin gaps exhibit a decreasing trend with the increasing sizes of the molecules, suggesting that the infinite graphene has a vanishing spin gap.

Coulomb localization in orbital degenerate, doped Mott insulators

We study electron localization in a three-band extended Hubbard model describing the t2g electrons of doped vanadium perovskites such as La1−xCaxVO3, where Ca defects are represented by Coulomb potentials. The main goal of this paper is to explore what happens when long-range electron-electron (e-e) interactions are switched on. The electronic structure of these doped Mott-Hubbard insulators is calculated using the unrestricted Hartree-Fock approximation that allows to perform the required statistical averages over many distinct defect realizations. The Mott gap is found to persist up to large doping and the defect states, appearing inside of it, are seen to develop a defect states gap centered at the Fermi energy. The internal kinetic energy of the doped holes, forming spin-orbital polarons bound to the defects, induces the defect states gap even in the absence of e-e interactions. Such kinetic gap survives disorder fluctuations and is amplified by long-range e-e interactions. A study of the inverse participation ratio reveals the small size of such spin-orbital polarons and provides an explanation for the persistence of spin and orbital order up to high doping.

Suppression of spin and optical gaps in phosphorene quantum dots

Electronic structure and optical properties of triangular phosphorene quantum dots have been investigated theoretically. Based on systematic configuration interaction calculations, the ground and excited states of the interacting many-electron system together with its optical absorption spectrum are obtained. For the nanodot with 60 phosphorus atoms in various dielectric environments, it is found that the spin gap of the correlated system surprisingly overlaps its optical gap over a large range of the effective dielectric constant. The overlapping of the spin and optical gaps can be attributed to the fact that the extra correlation energy in the spin singlet almost compensates the exchange energy in the spin triplet in the presence of strong long-range electron-electron interactions. Moreover, both the spin and optical gaps are shown to be greatly suppressed as the screening effect becomes strong. When the dielectric constant decreases below 2.65, it is seen that the spin gap becomes negative and the quantum dot undergoes a phase transition from nonmagnetic to ferromagnetic. Our results are compared with the previous experimental and theoretical works.

Effects of long-range disorder and electronic interactions on the optical properties of graphene quantum dots

We theoretically investigate the effects of long-range disorder and electron-electron interactions on the optical properties of hexagonal armchair graphene quantum dots consisting of up to 10806 atoms. The numerical calculations are performed using a combination of tight-binding, mean-field Hubbard and configuration interaction methods. Imperfections in the graphene quantum dots are modelled as a long-range random potential landscape, giving rise to electron-hole puddles. We show that, when the electron-hole puddles are present, tight-binding method gives a poor description of the low-energy absorption spectra compared to meanfield and configuration interaction calculation results. As the size of the graphene quantum dot is increased, the universal optical conductivity limit can be observed in the absorption spectrum. When disorder is present, calculated absorption spectrum approaches the experimental results for isolated monolayer of graphene sheet.

Magnetic phases of graphene nanoribbons under potential fluctuations

We investigate the effects of long-range potential fluctuations and electron-electron interactions on electronic and magnetic properties of graphene nanoribbons with zigzag edges using an extended mean-field Hubbard model. We show that electron-electron interactions make the edge states robust against potential fluctuations. When the disorder is strong enough, the presence of electron-hole puddles induces a magnetic phase transition from antiferromagnetically coupled edge states to ferromagnetic coupling, in agreement with recent experimental results.

Range-separated double-hybrid density-functional theory applied to periodic systems.

Quantum chemistry methods exploiting density-functional approximations for short-range electron-electron interactions and second-order Møller-Plesset (MP2) perturbation theory for long-range electron-electron interactions have been implemented for periodic systems using Gaussian-type basis functions and the local correlation framework. The performance of these range-separated double hybrids has been benchmarked on a significant set of systems including rare-gas, molecular, ionic, and covalent crystals. The use of spin-component-scaled MP2 for the long-range part has been tested as well. The results show that the value of μ = 0.5 bohr(-1) for the range-separation parameter usually used for molecular systems is also a reasonable choice for solids. Overall, these range-separated double hybrids provide a good accuracy for binding energies using basis sets of moderate sizes such as cc-pVDZ and aug-cc-pVDZ.

Long-range electron-electron interactions in graphene make its electrodynamics nonlocal

Graphene, a one-layer-thick hexagonal array of carbon atoms, when undoped, exhibits a curious mixture of properties pertinent to either metals or insulators. On the one hand, despite near absence of both charge carriers and impurities, it has a finite conductivity like a metal. On the other hand, the Coulomb interaction between electrons is unscreened like in a dielectric and hence is long range. The chemical potential is pinned right between the conical valence and conduction bands causing quasiparticles to move like massless relativistic particles. We demonstrate at small coupling that the electrodynamics of graphene exhibits nonlocality on a macroscopic level due to the combination of the long-range interactions and the linear dispersion relation. The frequency and wave vector $\mathbf{k}$-dependent conductivity tensor, in addition to a local pseudo-Ohmic part ${\ensuremath{\sigma}}_{T}{\ensuremath{\delta}}_{ij}$, possesses a nonlocal contribution ${\ensuremath{\sigma}}_{\mathrm{nl}}{k}_{i}{k}_{j}/{k}^{2}$. While the coefficient of the local part is ${\ensuremath{\sigma}}_{T}\ensuremath{\approx}{e}^{2}/4\ensuremath{\hbar}$, the coefficient of the nonlocal part is proportional to the Coulomb interaction strength $\ensuremath{\alpha}$, ${\ensuremath{\sigma}}_{\mathrm{nl}}={\ensuremath{\sigma}}_{T}\ensuremath{\alpha}$. This leads to several remarkable effects in transport and optical response. In particular, the resistance of the graphene flake depends on the location and the geometry of the source, drain, and probes. A voltage perpendicular to the current appears in a time-reversal symmetric situation and the polarization of reflected and transmitted light is modified, without either the magnetic field (like in the Faraday effect) or anisotropy.

Many-body effects in the spin-polarized electron transport through graphene nanoislands

Spin-polarized electron transport through zigzag-edged graphene nanoislands is studied within the framework of the Pariser-Parr-Pople Hamiltonian. By including both short- and long-range electron-electron interactions, the electron conductance is calculated self-consistently for the hexagonal model on various substrates from which we are able to identify the effects of the many-body interactions in the electron transport. For the system in its lowest antiferromagnetic (AFM) state, the long-range interactions are shown to have negligible effect on the electron transport in the low-energy region in which the conductance is found quenched mainly by the short-range interactions. As the system is excited to its second AFM state, the short- and long-range interactions are found to have opposite effects on the electron transmission, i.e., the electron transmission is found to increase with either the suppression of the long-range interactions or the enhancement of the short-range interactions. When the system moves further into the ferromagnetic state, the conductance becomes spin dependent and its resonance is shown to exhibit a blue shift in an environment with stronger long-range interactions. The distinct impact of short- and long-range electron-electron interactions are attributed to their different effects on the spin polarization in the model system.

Violation of Hund's rule and quenching of long-range electron-electron interactions in graphene nanoflakes

Hund's rule of maximum multiplicity controls the spin configuration of a system with degenerate midgap states, while Lieb's theorem determines the total spin of the ground state of a bipartite lattice. Most of graphene nanostructures follow both Hund's rule and Lieb's theorem, except that a number of nanoflakes with degenerate midgap states violates Hund's rule by exhibiting antiferromagnetic ground states as predicted by Lieb's theorem. To determine why Hund's rule fails and Lieb's theorem can predict correct spin configuration beyond the Hubbard model for which it was proved, we solve the strongly correlated electron states in such graphene nanoflakes where Hund's rule is violated by using a full configuration interaction approach. We find that long-range electron-electron interactions are quenched in both the ground and low-lying excited states of these systems. As there are no interactions between electrons with parallel spins in the system where long-range interactions are absent, we point out that a graphene nanoflake with degenerate midgap states and an antiferromagnetic ground state, in fact, falls very close to an ideal Hubbard system. Quenching of long-range interactions is therefore believed to be the natural explanation for the advantage of Lieb's theorem over Hund's rule in graphene nanostructures.

Linear and Nonlinear Optical Properties of Expanded Porphyrins: A DMRG Study

We study absorption spectra and two photon absorption coefficient of expanded porphyrins (EPs) by the density matrix renormalization group (DMRG) technique. We employ the Pariser-Parr-Pople (PPP) Hamiltonian which includes long-range electron-electron interactions. We find that, in the 4n+2 EPs, there are two prominent low-lying one-photon excitations, while in 4n EPs, there is only one such excitation. We also find that 4n+2 EPs have large two-photon absorption cross sections compared to 4n EPs. The charge density rearrangement in the one-photon excited state is mostly at the pyrrole nitrogen site and at the meso carbon sites. In the two-photon states, the charge density rearrangement occurs mostly at the aza-ring sites. In the one-photon state, the C-C bond length in aza rings shows a tendency to become uniform. In the two-photon state, the bond distortions are on C-N bonds of the pyrrole ring and the adjoining C-C bonds which connect the pyrrole ring to the aza or meso carbon sites.

Effect of dimerization on dynamics of spin-charge separation in Pariser-Parr-Pople model: A time-dependent density matrix renormalization group study

We investigate the effect of static electron-phonon coupling, on real-time dynamics of spin and charge transport in $\pi$-conjugated polyene chains. The polyene chain is modeled by the Pariser-Parr-Pople Hamiltonian with dimerized nearest-neighbor parameter $t_{0}(1+\delta)$ for short bonds and $t_{0}(1-\delta)$ for long bonds, and long-range electron-electron interactions. We follow the time evolution of the spin and charge using time-dependent density matrix renormalization group technique, when a hole is injected at one end of the chain in its ground state. We find that spin and charge dynamics followed through spin and charge velocities, depend both on chain length and extent of dimerization, $\delta$. Analysis of the results requires focusing on physical quantities such as average spin and charge polarizations, particularly in the large dimerization limit. In the dimerization range 0.0 $\le$ $\delta$ $\le$ 0.15, spin-charge dynamics is found to have a well defined behavior, with spin-charge separation (measured as the ratio of charge velocity to spin velocity) as well as, the total amount of charge and spin transported in a given time, along the chain, decreasing as dimerization increases. However, in the range 0.3 $\le$ $\delta$ $\le$ 0.5, it is observed that the dynamics of spin and charge transport becomes complicated. It is observed that for large $\delta$ values, spin-charge separation is suppressed and the injected hole fails to travel the entire length of the chain.

Transport through Graphene onSrTiO3

We report transport measurements through graphene on SrTiO(3) substrates as a function of magnetic field B, carrier density n, and temperature T. The large dielectric constant of SrTiO(3) very effectively screens long-range electron-electron interactions and potential fluctuations, making Dirac electrons in graphene virtually noninteracting. The absence of interactions results in an unexpected behavior of the longitudinal resistance in the N=0 Landau level and in a large suppression of the transport gap in nanoribbons. The "bulk" transport properties of graphene at B=0 T, on the contrary, are completely unaffected by the substrate dielectric constant.

Double time window targeting technique: Real-time DMRG dynamics in the Pariser-Parr-Pople model

We present a generalized adaptive time-dependent density matrix renormalization group (DMRG) scheme, called the {\it double time window targeting} (DTWT) technique, which gives accurate results with nominal computational resources, within reasonable computational time. This procedure originates from the amalgamation of the features of pace keeping DMRG algorithm, first proposed by Luo {\it et. al}, [Phys.Rev. Lett. {\bf 91}, 049701 (2003)], and the time-step targeting (TST) algorithm by Feiguin and White [Phys. Rev. B {\bf 72}, 020404 (2005)]. Using the DTWT technique, we study the phenomena of spin-charge separation in conjugated polymers (materials for molecular electronics and spintronics), which have long-range electron-electron interactions and belong to the class of strongly correlated low-dimensional many-body systems. The issue of real time dynamics within the Pariser-Parr-Pople (PPP) model which includes long-range electron correlations has not been addressed in the literature so far. The present study on PPP chains has revealed that, (i) long-range electron correlations enable both the charge and spin degree of freedom of the electron, to propagate faster in the PPP model compared to Hubbard model, (ii) for standard parameters of the PPP model as applied to conjugated polymers, the charge velocity is almost twice that of the spin velocity and, (iii) the simplistic interpretation of long-range correlations by merely renormalizing the {\it U} value of the Hubbard model fails to explain the dynamics of doped holes/electrons in the PPP model.

Charge Response Function and a Novel Plasmon Mode in Graphene

Polarizability of noninteracting 2D Dirac electrons has a 1/square root(qv-omega) singularity at the boundary of electron-hole excitations. The screening of this singularity by long-range electron-electron interactions is usually treated within the random phase approximation. The latter is exact only in the limit of N-->infinity, where N is the "color" degeneracy. We find that the ladder-type vertex corrections become crucial close to the threshold as the ratio of the nth order ladder term to the same order random phase approximation contribution is ln(n)|qv-omega|/N(n). We perform an analytical summation of the infinite series of ladder diagrams which describe the excitonic effect. Beyond the threshold, qv>omega, the real part of the polarization operator is found to be positive leading to the appearance of a strong and narrow plasmon resonance.

Coulomb Interaction, Ripples, and the Minimal Conductivity of Graphene

We argue that the unscreened Coulomb interaction in graphene provides a positive, universal, and logarithmic correction to scaling of zero-temperature conductivity with frequency. The combined effect of the disorder due to wrinkling of the graphene sheet and the long-range electron-electron interactions is a finite positive contribution to the dc conductivity. This contribution is disorder strength dependent and thus nonuniversal. The low-energy behavior of such a system is governed by the line of fixed points at which both the interaction and disorder are finite, and the density of states is exactly linear. An estimate of the typical random vector potential representing ripples in graphene brings the theoretical value of the minimal conductivity into the vicinity of 4e2/h.