Publications

The method of fundamental solutions (MFS) is known to be effective for solving 3D Laplace and Stokes Dirichlet boundary value problems in the exterior of a large collection of simple smooth objects. Here we present new scalable MFS formulations for the corresponding elastance and mobility problems. The elastance problem computes the potentials of conductors with given net charges, while the mobility problem -- crucial to rheology and complex fluid applications -- computes rigid body velocities given net forces and torques on the particles. The key idea is orthogonal projection of the net charge (or forces and torques) in a rectangular variant of a "completion flow". The proposal is compatible with one-body preconditioning, resulting in well-conditioned square linear systems amenable to fast multipole accelerated iterative solution, thus a cost linear in the particle number. For large suspensions with moderate lubrication forces, MFS sources on inner proxy-surfaces give accuracy on par with a well-resolved boundary integral formulation. Our several numerical tests include a suspension of 10000 nearby ellipsoids, using 26 million total preconditioned degrees of freedom, where GMRES converges to five digits of accuracy in under two hours on one workstation.

The application of an external, oriented electric field has emerged as an attractive technique for manipulating chemical reactions. Because most applications occur in solution, a theory of electric field catalysis requires treatment of the solvent, whose interaction with both the external field and the reacting species modifies the reaction energetics and thus the reaction rate. Here, we formulate such a transition state theory using a dielectric continuum model, and we incorporate dynamical effects due to solvent motion via Grote–Hynes corrections. We apply our theory to the Menshutkin reaction between CH3I and pyridine, which is catalyzed by polar solvents, and to the symmetric SN2 reaction of F– with CH3F, which is inhibited by polar solvents. At low applied field strengths when the solvent responds linearly, our theory predicts near-complete quenching of electric field catalysis. However, a qualitative treatment of the nonlinear response (i.e., dielectric saturation) shows that catalysis can be recovered at appreciable field strengths as solvent molecules begin to align with the applied field direction. The dynamical correction to the rate constant is seen to vary nonmonotonically with increasing solvent polarity due to contrasting effects of the screening ability and the longitudinal relaxation time of the solvent.

We study the interplay between intrinsic topological order and superconductivity in a two-component Haldane bilayer, where the two layers are coupled by an attractive force. We obtain the phase diagram of the model with exact diagonalization in finite size, and develop arguments to assess the stability of the observed phases in the thermodynamic limit. Our main result is that a finite critical attraction strength is needed to pair fermions forming a fractional topological order. This behavior can be harnessed to create clean interfaces between a fractional topological insulator and a superconductor by gating, wherein non-Abelian parafermionic modes are trapped. We discuss realization of such interfaces in the bulk of double bilayers of transition metal dichalcogenides by inhomogenous electrostatic gating, which should mitigate the spurious effects of disorder and crystalline defects present on physical edges.

The phase diagrams of quasi two-dimensional organic superconductors display a plethora of fundamental phenomena associated with strong electron correlations, such as unconventional superconductivity, metal-insulator transitions, frustrated magnetism and spin liquid behavior. We analyze a minimal model for these compounds, the Hubbard model on an anisotropic triangular lattice, using cutting-edge quantum embedding methods respecting the lattice symmetry. We demonstrate the existence of unconventional superconductivity by directly entering the symmetry-broken phase. We show that the crossover from the Fermi liquid metal to the Mott insulator is associated with the formation of a pseudogap. The predicted momentum-selective destruction of the Fermi surface into hot and cold regions provides motivation for further spectroscopic studies. Our results are in remarkable agreement with experimental phase diagrams of κ-BEDT organics.

It has been reported that upon doping a Mott insulator, there can be a crossover to a pseudogaped metallic phase followed by a first-order transition to another thermodynamically stable metallic phase. We call this first-order metal-metal transition the Sordi transition. It was argued that the initial reports of Sordi transitions at finite temperature could be explained by finite size effects and biases related to the model and method used. In this work, we report the Sordi transition on larger clusters at finite temperature on a triangular lattice, where long-range antiferromagnetic fluctuations are frustrated, using a different method, the dynamical cluster approximation instead of the cellular dynamical mean-field theory. This demonstrates that this first-order transition is a directly observable transition in doped Mott insulators and that it is relevant for experiments on candidate spin-liquid organic materials.

Parametric resonances and amplification have led to extraordinary photoinduced phenomena in pump-probe experiments. While these phenomena manifest themselves in out-of-equilibrium settings, here, we present the striking result of parametric amplification in equilibrium. In particular, we demonstrate that quantum and thermal fluctuations of a Raman-active mode amplifies light inside a cavity, at equilibrium, when the Raman mode frequency is twice the cavity mode frequency. This noise-driven amplification leads to the creation of an unusual parametric Raman polariton, intertwining the Raman mode with cavity squeezing fluctuations, with smoking gun signatures in Raman spectroscopy. In the resonant regime, we show the emergence of not only quantum light amplification but also localization and static shift of the Raman mode. Apart from the fundamental interest of equilibrium parametric amplification our study suggests a resonant mechanism for controlling Raman modes and thus matter properties by cavity fluctuations. We conclude by outlining how to compute the Raman-cavity coupling, and suggest possible experimental realization

In magic angle twisted bilayer graphene, transport, thermodynamic and spectroscopic experiments pinpoint at a competition between distinct low-energy states with and without electronic order. We use Dynamical Mean Field Theory (DMFT) on the topological heavy Fermion (THF) model of twisted bilayer graphene to investigate the emergence of electronic correlations and long-range order in the absence of strain. We contrast moment formation, Kondo screening and ordering on a temperature basis and explain the nature of emergent correlated states based on three central phenomena: (i) the formation of local spin and valley isospin moments around 100K, (ii) the ordering of the local isospin moments around 10K preempting Kondo screening, and (iii) a cascadic redistribution of charge between localized and delocalized electronic states upon doping. At integer fillings, we find that low energy spectral weight is depleted in the symmetric phase, while we find insulating states with gaps enhanced by exchange coupling in the zero-strain ordered phases. Doping away from integer filling results in distinct metallic states: a "bad metal" above the ordering temperature, where scattering off the disordered local moments suppresses electronic coherence, and a "good metal" in the ordered states with coherence of quasiparticles facilitated by isospin order. This finding reveals coherence from order as the microscopic mechanism behind the Pomeranchuk effect observed experimentally. Upon doping, there is a periodic charge reshuffling between localized and delocalized electronic orbitals leading to cascades of doping-induced Lifshitz transitions, local spectral weight redistributions and periodic variations of the electronic compressibility. Our findings provide a unified understanding of the most puzzling aspects of scanning tunneling spectroscopy, transport, and compressibility experiments.

The phase diagrams of quasi two-dimensional organic superconductors display a plethora of fundamental phenomena associated with strong electron correlations, such as unconventional superconductivity, metal-insulator transitions, frustrated magnetism and spin liquid behavior. We analyze a minimal model for these compounds, the Hubbard model on an anisotropic triangular lattice, using cutting-edge quantum embedding methods respecting the lattice symmetry. We demonstrate the existence of unconventional superconductivity by directly entering the symmetry-broken phase. We show that the crossover from the Fermi liquid metal to the Mott insulator is associated with the formation of a pseudogap. The predicted momentum-selective destruction of the Fermi surface into hot and cold regions provides motivation for further spectroscopic studies. Our results are in remarkable agreement with experimental phase diagrams of κ-BEDT organics.

We study the interplay between intrinsic topological order and superconductivity in a two-component Haldane bilayer, where the two layers are coupled by an attractive force. We obtain the phase diagram of the model with exact diagonalization in finite size, and develop arguments to assess the stability of the observed phases in the thermodynamic limit. Our main result is that a finite critical attraction strength is needed to pair fermions forming a fractional topological order. This behavior can be harnessed to create clean interfaces between a fractional topological insulator and a superconductor by gating, wherein non-Abelian parafermionic modes are trapped. We discuss realization of such interfaces in the bulk of double bilayers of transition metal dichalcogenides by inhomogenous electrostatic gating, which should mitigate the spurious effects of disorder and crystalline defects present on physical edges.

Parametric resonances and amplification have led to extraordinary photoinduced phenomena in pump-probe experiments. While these phenomena manifest themselves in out-of-equilibrium settings, here, we present the striking result of parametric amplification in equilibrium. In particular, we demonstrate that quantum and thermal fluctuations of a Raman-active mode amplifies light inside a cavity, at equilibrium, when the Raman mode frequency is twice the cavity mode frequency. This noise-driven amplification leads to the creation of an unusual parametric Raman polariton, intertwining the Raman mode with cavity squeezing fluctuations, with smoking gun signatures in Raman spectroscopy. In the resonant regime, we show the emergence of not only quantum light amplification but also localization and static shift of the Raman mode. Apart from the fundamental interest of equilibrium parametric amplification our study suggests a resonant mechanism for controlling Raman modes and thus matter properties by cavity fluctuations. We conclude by outlining how to compute the Raman-cavity coupling, and suggest possible experimental realization