We report results of large-scale quantum Monte Carlo (QMC) simulations of graphene. Using cutting-edge algorithmic improvements, we are able to consider spatial volumes, corresponding to 20808 electrons, that allow us to access energy scales of direct relevance to experiments. Using constrained random phase approximation (cRPA) estimates of short-ranged interactions combined with a Coulomb tail, we are able to successfully confront numerical and experimental estimates of the Fermi velocity renormalization, thus fixing the parameters of microscopic Hamiltonian to exactly reproduce the experimental data. Subsequent comparison of the QMC results with perturbation theory not only show the non-Fermi liquid character of graphene, but also prove the importance of lattice-scale physics and higher-order perturbative corrections beyond RPA for the quantitative description of the experimental data for the Fermi velocity renormalization in suspended graphene. The same Monte Carlo technique is subsequently employed to investigate electrical transport by computing the renormalization of the optical conductivity in freestanding graphene. The large lattice sizes and low temperatures accessible in our QMC simulations enable a clear resolution of the Dirac plateau in the spectral function, even in the presence of interactions. We demonstrate that, despite the strong renormalization of the single-particle dispersion, the optical conductivity remains essentially constant, in agreement with current experimental observations. This finding points toward the possibility of extending the theorem on the absence of optical conductivity renormalization for the Hubbard model on the hexagonal lattice to the case of long-range interactions.
We report results of large-scale quantum Monte Carlo (QMC) simulations of graphene. Using cutting-edge algorithmic improvements, we are able to consider spatial volumes, corresponding to 20808 electrons, that allow us to access energy scales of direct relevance to experiments. Using constrained random phase approximation (cRPA) estimates of short-ranged interactions combined with a Coulomb tail, we are able to successfully confront numerical and experimental estimates of the Fermi velocity renormalization, thus fixing the parameters of microscopic Hamiltonian to exactly reproduce the experimental data. Subsequent comparison of the QMC results with perturbation theory not only show the non-Fermi liquid character of graphene, but also prove the importance of lattice-scale physics and higher-order perturbative corrections beyond RPA for the quantitative description of the experimental data for the Fermi velocity renormalization in suspended graphene. The same Monte Carlo technique is subsequently employed to investigate electrical transport by computing the renormalization of the optical conductivity in freestanding graphene. The large lattice sizes and low temperatures accessible in our QMC simulations enable a clear resolution of the Dirac plateau in the spectral function, even in the presence of interactions. We demonstrate that, despite the strong renormalization of the single-particle dispersion, the optical conductivity remains essentially constant, in agreement with current experimental observations. This finding points toward the possibility of extending the theorem on the absence of optical conductivity renormalization for the Hubbard model on the hexagonal lattice to the case of long-range interactions.
We develop and apply the diagrammatic Monte Carlo technique to address the problem of the stability of the Dirac liquid state (in a graphene-type system) against the strong long-range part of the Coulomb interaction. So far, all attempts to deal with this problem in the field-theoretical framework were limited either to perturbative or random phase approximation and functional renormalization group treatments, with diametrically opposite conclusions. Our calculations aim at the approximation-free solution with controlled accuracy by computing vertex corrections from higher-order skeleton diagrams and establishing the renormalization group flow of the effective Coulomb coupling constant. We unambiguously show that with increasing the system size L (up to ln(L)∼40), the coupling constant always flows towards zero; i.e., the two-dimensional Dirac liquid is an asymptotically free T=0 state with divergent Fermi velocity.
The many-body correlation between electrons is the origin of many fascinating phenomena in condensed matter systems, such as high temperature superconductivity, superfluidity, fractional quantum Hall effect, and Mott insulator. Strongly correlated systems have been an important subject of condensed matter physics for several decades, especially after the discovery of high temperature cuprate superconductors. In this thesis, we apply first principles quantum Monte Carlo (QMC) method to several representative systems to study the electron correlations in transition metal oxides (vanadium dioxide) and low dimensional electronic systems (graphene and graphene-like two dimensional systems). Vanadium dioxide (VO2) is a paradigmatic example of a strongly correlated system that undergoes a metal-insulator transition at a structural phase transition. To date, this transition has necessitated significant post-hoc adjustments to theory in order to be described properly. We apply first principles quantum Monte Carlo (QMC) to study the structural dependence of the properties of VO2. Using this technique, we simulate the interactions between electrons explicitly, which allows for the metal-insulator transition to naturally emerge, importantly without ad-hoc adjustments. The QMC calculations show that the structural transition directly causes the metal-insulator transition and a change in the coupling of vanadium spins. This change in the spin coupling results in a prediction of a momentum-independent magnetic excitation in the insulating state. While two-body correlations are important to set the stage for this transition, they do not change significantly when VO2 becomes an insulator. These results show that it is now possible to account for electron correlations in a quantitatively accurate way that is also specific to materials. Electron correlation in graphene is unique because of the interplay of the Dirac cone dispersion of pi electrons with long range Coulomb interaction. The random phase approximation predicts no metallic screening at long distances and low energies because of the zero density of states at Fermi level. It is thus interesting to see how screening takes place in graphene at different length scales. We addressed this problem by computing the structure factor S(q) and S(q, ω) of freestanding graphene using ab initio fixed-node diffusion Monte Carlo and the random phase approximation. The X-ray measured structure factor is reproduced very accurately using both techniques, provided that sigma-bonding electrons are included in the simulations. Strong dielectric screening from sigma electrons are observed, which redshifts the pi plasmons resonance frequency at long distance and reduces the effective interactions between pi electrons at short distance. The short distance screening makes suspended graphene a weakly correlated semimetal which otherwise would be an insulator. The third piece of works is dedicated to studying the low energy excitation of many-body systems using extended Koopmans' theorem (EKT). The EKT provides a straight forward way to compute charge excitation spectra, such as ionization potentials, electron affinities from any level of theory. We implemented the EKT within the QMC framework, and performed systematic benchmark studies of ionization potentials of the second- and third-row atoms, and closed- and open-shell molecules. We also applied it to compute the quasiparticle band structure of solids (graphene). For complex correlated systems, identifying relevant low energy physics degrees of freedom is extremely important to understanding the system's collective behavior at different length scales. In this sense, bridging the realistic systems to lower energy effective lattice models that involve fewer but important degrees of freedom is significant to understanding correlated systems. We have formulated three ab initio density matrix based downfolding (AIDMD) methods to downfold the ab initio systems into effective lattice models. We have demonstrated the successfulness of these methods by applying them to molecules (H2) and periodic systems (hydrogen chain and graphene).
We report an implementation of the momentum space quantum Monte Carlo (QMC) method on the interaction model for the twisted bilayer graphene (TBG). The long-range Coulomb repulsion is treated exactly with the flat bands, spin and valley degrees of freedom of electrons taking into account. We prove the absence of the minus sign problem for QMC simulation when either the two valleys or the two spin degrees of freedom are considered. By taking the realistic parameters of the twist angle and interlayer tunnelings into the simulation, we benchmark the QMC data with the exact band gap obtained at the chiral limit, to reveal the insulating ground states at the charge neutrality point (CNP). Then, with the exact Green’s functions from QMC, we perform stochastic analytic continuation to obtain the first set of single-particle spectral function for the TBG model at CNP. Our momentum space QMC scheme therefore offers the controlled computation pathway for systematic investigation of the electronic states in realistic TBG model at various electron fillings.
Both insulating and conducting electronic behaviors have been experimentally seen in clean bilayer graphene samples at low temperature, and there is still no consensus on the nature of the interacting ground state at half filling and in the absence of a magnetic field. Theoretically, several possibilities for the insulating ground states have been predicted for weak interaction strength. However, a recent renormalization-group calculation on a Hubbard model for charge-neutral bilayer graphene with short-range interactions suggests the emergence of low-energy Dirac fermions that would stabilize the metallic phase for weak interactions. Using a nonperturbative projective quantum Monte Carlo, we calculate the ground state for bilayer graphene using a realistic model for the Coulomb interaction that includes both short-range and long-range contributions. We find that a finite critical on-site interaction is needed to gap bilayer graphene and the transition belongs to the Gross-Neveu universality class, thereby confirming the Hubbard model expectations even in the presence of a long-range Coulomb potential, in agreement with our theoretical analysis. In addition, we also find that the critical on-site interactions necessary to destabilize the metallic ground state decrease with increasing interlayer coupling.
We study the quantum many-body ground states of electrons on the half-filled honeycomb lattice with short- and long-ranged density-density interactions as a model for graphene. To this end, we employ the recently developed truncated-unity functional renormalization group (TU-fRG) approach which allows for a high resolution of the interaction vertex' wave vector dependence. We connect to previous lattice quantum Monte Carlo (QMC) results which predict a stabilization of the semimetallic phase for realistic ab initio interaction parameters and confirm that the application of a finite biaxial strain can induce a quantum phase transition towards an ordered ground state. In contrast to lattice QMC simulations, the TU-fRG is not limited in the choice of tight-binding and interaction parameters to avoid the occurrence of a sign problem. Therefore, we also investigate a range of parameters relevant to the realistic graphene material which are not accessible by numerically exact methods. Although a plethora of charge-density waves arises under medium-range interactions, we find the antiferromagnetic spin-density wave to be the prevailing instability for long-range interactions. We further explore the impact of an extended tight-binding Hamiltonian with second-nearest-neighbor hopping and a finite chemical potential for a more accurate description of the band structure of graphene's pz electrons.
After its first isolation by Geim and Novoselov in 2004, graphene has grown quickly into an independent subfield of contemporary condensed matter physics, counting thousands of publications. This material has attracted so much attention not only because it is truly two-dimensional -- a feature long thought to be impossible to be realized in nature -- but also because it is the prime representative of a new class of condensed matter systems, the Dirac materials, whose electronic spectrum disperses linearly around isolated points in the Brillouin zone. An outstanding consequence of this linear energy-momentum dispersion is the collapse of the Fermi surface to isolated points at charge neutrality, accompanied by a vanishing single-particle density of states. While this feature of the noninteracting model is what separates graphene from most other, more conventional condensed matter systems, giving rise to many of its astounding physical properties, it leads to severe computational complications when extending the model to contain two-body interactions and/or disorder. In this thesis we consider both extensions separately. After rigorously deriving the low-energy quantum field theory from a tight-binding model and establishing the one-particle irreducible (1PI) vertex functions as the fundamental building blocks of correlation functions, we construct a nonperturbative formalism for the calculation of these vertex functions using the well-established functional renormalization group (fRG). By combining the fRG with the Keldysh formalism, accounting for possible external electromagnetic fields and nontrivial initial correlations, this framework is capable of handling thermal equilibrium and true nonequilibrium alike. To circumvent some of the technical problems of the standard fRG formalism when treating fermionic systems at finite density, we also explore a variant of the fRG, where the chemical potential is interpreted as a flow parameter. We obtain hierarchical sets of flow equations, which describe the change of the 1PI vertex functions upon varying an artificial cutoff scale or the chemical potential, respectively. These nonperturbative formalisms have been used to calculate the renormalization of the Fermi velocity and the static dielectric function at finite temperature and density in the strong coupling regime as an explicit demonstration of their capabilities. Since the Keldysh fRG is an exact formulation of quantum field theory, in particular when external magnetic fields are present, it should be possible to describe the fractional quantum Hall effect in this framework. However, the typical truncation schemes that are currently available to approximately solve the fRG flow equation fail to account for the nontrivial correlation effects necessary to access the fractional quantum Hall regime. To circumvent this problem we consider a modified field theory, where these correlations are implemented ``by hand'' via a Chern-Simons gauge field, coupling to the fermions in addition to the Coulomb interaction term. This modified field theory is analyzed in a stationary phase approximation including Gaussian fluctuations. The electromagnetic response tensor is calculated in the random phase approximation, yielding the Hall conductivities. In the second part of this thesis we consider disordered Dirac fermions in the absence of two-particle interactions. After sketching how the most general disorder potential for Dirac fermions arises from a tight-binding model, we first consider an explicit physical scenario, a disordered graphene pn junction in the presence of a quantizing magnetic field perpendicular to the graphene sheet. We derive an effective one-dimensional theory for the chiral states that propagate along the junction interface and calculate the full conductance distribution in the crossover between the clean and the strong-disorder limit, via an exact solution of a Fokker-Planck equation. Lastly, we develop a nonperturbative approach to calculate the disorder induced self-energy that is based on exact Schwinger-Dyson equations and Ward identities, not only for graphene, but also for other paradigmatic semimetals with a nodal point dispersion.