Publications

Atomic layers deposited on semiconductor substrates introduce a platform for the realization of the extended electronic Hubbard model, where the consideration of electronic repulsion beyond the onsite term is paramount. Recently, the onset of superconductivity at 4.7K has been reported in the hole-doped triangular lattice of tin atoms on a silicon substrate. Through renormalization group methods designed for weak and intermediate coupling, we investigate the nature of the superconducting instability in hole-doped Sn/Si(111). We find that the extended Hubbard nature of interactions is crucial to yield triplet pairing, which is f-wave (p-wave) for moderate (higher) hole doping. In light of persisting challenges to tailor triplet pairing in an electronic material, our finding promises to pave unprecedented ways for engineering unconventional triplet superconductivity.

Inspired by Grimme's simplified Tamm-Dancoff density functional theory approach [S. Grimme, J. Chem. Phys.

We present a vibrational dynamical mean-field theory (VDMFT) of the dynamics of atoms in solids with anharmonic interactions. Like other flavors of DMFT, VDMFT maps the dynamics of a periodic anharmonic lattice of atoms onto those of a self-consistently defined impurity problem with local anharmonicity and coupling to a bath of harmonic oscillators. VDMFT is exact in the harmonic and molecular limits, nonperturbative, systematically improvable through its clusters extensions, and usable with classical or quantum impurity solvers, depending on the importance of nuclear quantum effects. When tested on models of anharmonic optical and acoustic phonons, we find that classical VDMFT gives good agreement with classical molecular dynamics, including the temperature dependence of phonon frequencies and lifetimes. Using a quantum impurity solver, signatures of nuclear quantum effects are observed at low temperatures.

Efficient computer implementations of the GW approximation must approximate a numerically challenging frequency integral; the integral can be performed analytically, but doing so leads to an expensive implementation whose computational cost scales as O(N

Traditional numerical methods for calculating matrix eigenvalues are prohibitively expensive for high-dimensional problems. Iterative random sparsification methods allow for the estimation of a single dominant eigenvalue at reduced cost by leveraging repeated random sampling and averaging. We present a general approach to extending such methods for the estimation of multiple eigenvalues and demonstrate its performance for several benchmark problems in quantum chemistry.

The inherent atomistic precision of synthetic chemistry enables bottom-up structural control over quantum bits, or qubits, for quantum technologies. Tuning paramagnetic molecular qubits that feature optical-spin initialization and readout is a crucial step toward designing bespoke qubits for applications in quantum sensing, networking, and computing. Here, we demonstrate that the electronic structure that enables optical-spin initialization and readout for S = 1, Cr(aryl)4, where aryl = 2,4-dimethylphenyl (1), o-tolyl (2), and 2,3-dimethylphenyl (3), is readily translated into Cr(alkyl)4 compounds, where alkyl = 2,2,2-triphenylethyl (4), (trimethylsilyl)methyl (5), and cyclohexyl (6). The small ground state zero field splitting values (<5 GHz) for 1–6 allowed for coherent spin manipulation at X-band microwave frequency, enabling temperature-, concentration-, and orientation-dependent investigations of the spin dynamics. Electronic absorption and emission spectroscopy confirmed the desired electronic structures for 4–6, which exhibit photoluminescence from 897 to 923 nm, while theoretical calculations elucidated the varied bonding interactions of the aryl and alkyl Cr4+ compounds. The combined experimental and theoretical comparison of Cr(aryl)4 and Cr(alkyl)4 systems illustrates the impact of the ligand field on both the ground state spin structure and excited state manifold, laying the groundwork for the design of structurally precise optically addressable molecular qubits.

The rapidly growing interest in simulating condensed-phase materials using quantum chemistry methods calls for a library of high-quality Gaussian basis sets suitable for periodic calculations. Unfortunately, most standard Gaussian basis sets commonly used in molecular simulation show significant linear dependencies when used in close-packed solids, leading to severe numerical issues that hamper the convergence to the complete basis set (CBS) limit, especially in correlated calculations. In this work, we revisit Dunning's strategy for construction of correlation-consistent basis sets and examine the relationship between accuracy and numerical stability in periodic settings. Specifically, we find that limiting the number of primitive functions avoids the appearance of problematic small exponents while still providing smooth convergence to the CBS limit. As an example, we generate double-, triple-, and quadruple-zeta correlation-consistent Gaussian basis sets for periodic calculations with Goedecker-Teter-Hutter (GTH) pseudopotentials. Our basis sets cover the main-group elements from the first three rows of the periodic table. Especially for atoms on the left side of the periodic table, our basis sets are less diffuse than those used in molecular calculations. We verify the fast and reliable convergence to the CBS limit in both Hartree-Fock and post-Hartree-Fock (MP2) calculations, using a diverse test set of 19 semiconductors and insulators.

We determine the spin and charge orders in the ground state of the doped two-dimensional (2D) Hubbard model in its simplest form, namely with only nearest-neighbor hopping and on-site repulsion. At half-filling, the ground state is known to be an anti-ferromagnetic Mott insulator. Doping Mott insulators is believed to be relevant to the superconductivity observed in cuprates. A variety of candidates have been proposed for the ground state of the doped 2D Hubbard model. A recent work employing a combination of several state-of-the-art numerical many-body methods, established the stripe order as the ground state near 1/8 doping at strong interactions. In this work, we apply one of these methods, the cutting-edge constrained-path auxiliary field quantum Monte Carlo method with self-consistently optimized gauge constraints, to systematically study the model as a function of doping and interaction strength. With careful finite size scaling based on large-scale computations, we map out the ground state phase diagram in terms of its spin and charge order. We find that modulated antiferromagnetic order persists from near half-filling to about 1/5 doping. At lower interaction strengths or larger doping, these ordered states are best described as spin-density waves, with essentially delocalized holes and modest oscillations in charge correlations. When the charge correlations are stronger (large interaction or small doping), they are best described as stripe states, with the holes more localized near the node in the antiferromagnetic spin order. In both cases, we find that the wavelength in the charge correlations is consistent with so-called filled stripes in the pure Hubbard model.

We perform large-scale, numerically exact calculations on the two-dimensional interacting Fermi gas with a contact attraction. Reaching much larger lattice sizes and lower temperatures than previously possible, we determine systematically the finite-temperature phase diagram of the Berezinskii-Kosterlitz-Thouless (BKT) transitions for interaction strengths ranging from BCS to crossover to BEC regimes. The evolutions of the pairing wavefunctions and the fermion and Cooper pair momentum distributions with temperature are accurately characterized. In the crossover regime, we find that the contact has a non-monotonic temperature dependence, first increasing as temperature is lowered, and then showing a slight decline below the BKT transition temperature to approach the ground-state value from above.

Leveraging cutting-edge numerical methodologies, we study the ground state of the two-dimensional spin-polarized Fermi gas in an optical lattice. We focus on systems at high density and small spin polarization, corresponding to the parameter regime believed to be most favorable to the formation of the elusive Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) superfluid phase. Our systematic study of large lattice sizes, hosting nearly 500 atoms, provides strong evidence of the stability of the FFLO state in this regime, as well as a high-accuracy characterization of its properties. Our results for the density correlation function reveal the existence of density order in the system, suggesting the possibility of an intricate coexistence of long-range orders in the ground state. The ground-state properties are seen to differ significantly from the standard mean-field description, providing a compelling avenue for future theoretical and experimental explorations of the interplay between interaction and superfluidity in an exotic phase of matter.