We find the ground-state energy of the Ising model using the Cascaded Variational Quantum Eigensolver (CVQE) algorithm with the Guided-Sampling Ansatz (GSA) using up to 63 qubits on a quantum computer. We study a heavy-hex lattice to match the qubit architecture, allowing us to perform calculations in the quantum utility regime. We study both a homogeneous and random-coupling model. We locate the boundary of acceptable quantum errors as a function of the number of qubits and coupling strength. An entropic analysis is performed giving insights into the quantum computing performance. A subspace analysis is performed that suggests that the Ising model is especially suited for near-term quantum computing.

Transition metal dichalcogenide (TMD) bilayers with an interlayer twist exhibit a moiré superperiod, whose effects can manifest in both structural and electronic properties. Atomic displacements can lead to reconstruction into domains of aligned stacking, and flat bands can form that may host correlated electron states. In heterobilayers, an angular mismatch is nearly unavoidable, so understanding the consequences of an interlayer twist is essential. Using ab initio density functional theory, we find that in near-60° twisted MoSe2/WSe2 bilayers, spectrally isolated valence and conduction band flat bands emerge at ∼3° twist. Despite relatively limited reconstruction at these angles, atomic displacement creates a polarization gradient that forms a confining potential, localizing and laterally separating electrons and holes within the moiré supercell. Excitons formed from flat band electrons and holes should therefore have not only the out-of-plane dipole moment familiar from MoSe2/WSe2 interlayer excitons but an in-plane moment as well.

We propose a hybrid variational quantum algorithm that has variational parameters used by both the quantum circuit and the subsequent classical optimization. Similar to the Variational Quantum Eigensolver (VQE), this algorithm applies a parameterized unitary operator to the qubit register. We generate this operator using diabatic state preparation. The quantum measurement results then inform the classical optimization procedure used by the Cascaded Variational Quantum Eigensolver (CVQE). We demonstrate the algorithm on a system of interacting electrons and show how it can be used on long-term error-corrected as well as short-term intermediate-scale quantum computers. Our simulations performed on IBM Brisbane produced energies well within chemical accuracy.

Conjugational defects, also known as solitons, play an important role in the electronic, magnetic, and optical properties of materials. Understanding solitons can uncover intriguing physics and provide insights for designing quantum materials with tailored band structures and electronic properties. Here, we propose a framework to create and control solitons via topological phase transitions in a class of graphene nanoribbons (GNRs) called square-root GNRs, using a transverse electric field. To demonstrate the experimental feasibility, we design and synthesize a representative GNR with a bottom-up approach, with first-principles calculations revealing topological soliton states at the domain wall induced by the electric field. The framework introduced in this Letter can potentially enable direct manipulation of solitons and provide a platform to study them systematically.

Quantum computing is a promising technology because of the ability of quantum computers to process vector spaces with dimensions that increase exponentially with the simulated system size. Extracting the solution, however, is challenging as the number of quantum gate operations and quantum circuit executions must still scale at most polynomially. Consequently, choosing a good ansatz–a polynomial subset of the exponentially many possible solutions–will be critical to maintain accuracy for larger systems. To address this challenge, we introduce a class of guided sampling ansätzes (GSAs) that depend on the system interactions and measured state samples as well as a parameter space. We demonstrate a minimal ansatz for the hydronium cation H_3O^+ and found that with only 200 circuit executions per structure on the IonQ Aria quantum computer, our calculations produced total energies around the relaxed structure with errors well below 1.59×10^-3 Ha, thus exceeding chemical accuracy.

Ceramics are widely perceived as brittle. Recent research showed that the deformability of brittle ceramics can be improved by introducing defects, e.g., dislocations and stacking faults, into the ceramics using flash sintering. However, many ceramic materials, including TiO2, have limited room-temperature dislocation mobility. In this work, we explored a potential route to toughen ceramic materials by introducing oxygen vacancies into rutile TiO2. Nanoindentation method was employed to investigate the deformation behavior of the oxygen-deficient TiO2-x. Detailed post-deformation transmission electron microscopy analyses revealed a significant increase in dislocation density. The improved fracture toughness is attributed to the abundant dislocation plasticity in reduced TiO2 with abundant oxygen vacancies. This study provides insight into understanding the influence of point defects and dislocations on the deformation behavior of ceramic materials towards the future designs of ductile ceramics at room temperature.

We explore the relationship between entropy and quantum measurements and present a variational algorithm for preparing statistical ensembles on quantum computers using mid-circuit measurements. This algorithm optimizes both the entropy and variational parameters describing the state to obtain the minimum free energy of quantum systems in thermal equilibrium with some external heat bath. We demonstrate our algorithm on IBM-Q Lagos.

We present a cascaded variational quantum eigensolver algorithm that only requires the execution of a set of quantum circuits once rather than at every iteration during the parameter optimization process, thereby increasing the computational throughput. This algorithm uses a quantum processing unit to probe the needed probability mass functions and a classical processing unit perform the remaining calculations, including the energy minimization. The ansatz form does not restrict the Fock space and provides full control over the trial state, including the implementation of symmetry and other physically motivated constraints.

We demonstrate how the cascaded variational quantum eigensolver (CVQE) can be applied to study molecular systems for the family of Jastrow ansatzes. Specifically, we applied CVQE to the water molecule. We find that CVQE has a number of advantages. In particular, our results show that CVQE requires 2 to 3 orders of magnitude fewer quantum computing (QC) executions than VQE for the water molecule. Furthermore, our results indicate that CVQE might provide some robustness against two-qubit gate errors given that the number of CNOT gates used in our calculation was ∼300 and the errors in the QC calculations are still comparable to those obtained by VQE.

A Jastrow-Gutzwiller operator adds many-body correlations to a quantum state. However, the operator is nonunitary, making it difficult to implement directly on a quantum computer. We present an implementation of the Jastrow-Gutzwiller operator using the cascaded variational quantum eigensolver algorithm. We demonstrate the method on IBM Q Lagos for a Hubbard model.

We present a hybrid classical/quantum algorithm for efficiently solving the eigenvalue problem of many-particle Hamiltonians on quantum computers with limited resources by splitting the workload between classical and quantum processors. This algorithm reduces the needed number of qubits at the expense of an increased number of quantum evaluations. We demonstrate the method for the Hubbard model and show how the conservation of the z-component of the total spin allows the spin-up and spin-down configurations to be computed on classical and quantum hardware, respectively. Other symmetries can be exploited in a similar manner.

Bilayers of 2D materials offer opportunities for creating devices with tunable electronic, optical, and mechanical properties. In van der Waals heterostructures (vdWHs) where the constituent monolayers have different lattice constants, a moiré superlattice forms with a length scale larger than the lattice constant of either constituent material regardless of twist angle. Here, we report the appearance of moiré Raman modes from nearly aligned WSe2-WS2 vdWHs in the range of 240-260 cm-1, which are absent in both monolayers and homobilayers of WSe2 and WS2 and in largely misaligned WSe2-WS2 vdWHs. Using first-principles calculations and geometric arguments, we show that these moiré Raman modes are a consequence of the large moiré length scale, which results in zone-folded phonon modes that are Raman active. These modes are sensitive to changes in twist angle, but notably, they occur at identical frequencies for a given small twist angle away from either the 0-degree or 60-degree aligned heterostructure. Our measurements also show a strong Raman intensity modulation in the frequency range of interest, with near 0 and near 60-degree vdWHs exhibiting a markedly different dependence on excitation energy. In near 0-degree aligned WSe2-WS2 vdWHs, a nearly complete suppression of both the moiré Raman modes and the WSe2 A1g Raman mode (∼250 cm-1) is observed when exciting with a 532 nm CW laser at room temperature. Temperature-dependent reflectance contrast measurements demonstrate the significant Raman intensity modulation arises from resonant Raman effects.

We demonstrate the connection between an operator's matrix element distribution and entangling power via numerical simulations of random, pseudo-random, and quantum chaotic operators. Creating operators with a random distribution of matrix elements is more difficult than creating operators that reproduce other statistical properties of random matrices. Thus, operators that fulfill many random matrix statistical properties may not generate states of high multi-partite entanglement. To quantify the randomness of various statistical distributions and, by extension, entangling power, we use properties of interpolating ensembles that transition between integrable and random matrix ensembles.

The twist angle between the monolayers in van der Waals heterostructures provides a new degree of freedom in tuning material properties. We compare the optical properties of WSe2 homobilayers with 2H and 3R stacking using photoluminescence, Raman spectroscopy, and reflectance contrast measurements under ambient and cryogenic temperatures. Clear stacking- dependent differences are evident for all temperatures, with both photoluminescence and reflectance contrast spectra exhibiting a blue shift in spectral features in 2H compared to 3R bilayers. Density functional theory (DFT) calculations elucidate the source of the variations and the fundamental differences between 2H and 3R stackings. DFT finds larger energies for both A and B excitonic features in 2H than in 3R, consistent with experimental results. In both stacking geometries, the intensity of the dominant A1g Raman mode exhibits significant changes as a function of laser excitation wavelength. These variations in intensity are intimately linked to the stacking- and temperature-dependent optical absorption through resonant enhancement effects. The strongest enhancement is achieved when the laser excitation coincides with the C excitonic feature, leading to the largest Raman intensity under 514 nm excitation in 2H stacking and at 520 nm in 3R stacked WSe2 bilayers.

A fundamental understanding of the influence of defects in ionic ceramics at the atomic, microstructural, and macroscopic levels, before, during, and after the flash sintering event is key to the development of ceramic processing operations that lead to fast, low cost, and environmentally safe fabrication of materials. The observed phenomenology of the flash process encompasses multiple time and length scales and has resulted in a wide variety of what sometimes appears to be contradictory explanations. This article summarizes the latest developments on the modeling and simulation of flash sintering, specifically those related to the understanding of the equilibrium and kinetic properties and the corresponding microstructural evolution of ionic ceramics. Challenges and opportunities in the development of theoretical analyses that include unidentified multiphysical effects are discussed, as they pertain to the processing of technologically relevant ceramic materials for advanced structures and devices.

Locally intensified, low energy electromagnetic fields can directly affect atomic arrangements through defect-driven structural distortions.

Van der Waals layered materials, such as transition metal dichalcogenides (TMDs), are an exciting class of materials with weak interlayer bonding, which enables one to create so-called van der Waals heterostructures (vdWH). One promising attribute of vdWH is the ability to rotate the layers at arbitrary azimuthal angles relative to one another. Recent work has shown that control of the twist angle between layers can have a dramatic effect on TMD vdWH properties, but the twist angle has been treated solely through the use of rigid-lattice moiré patterns. No atomic reconstruction, that is, any rearrangement of atoms within the individual layers, has been reported experimentally to date. Here, we demonstrate that vdWH of MoSe2/WSe2 and MoS2/WS2 at twist angles ≤1° undergo significant atomic level reconstruction leading to discrete commensurate domains divided by narrow domain walls, rather than a smoothly varying rigid-lattice moiré pattern as has been assumed in prior experimental work. Using conductive atomic force microscopy (CAFM), we show that TMD vdWH at small twist angles exhibit large domains of constant conductivity. The domains in samples with R-type stacking are triangular, whereas the domains in samples with H-type stacking are hexagonal. Transmission electron microscopy provides additional evidence of atomic reconstruction in MoSe2/WSe2 structures and demonstrates the transition between a rigid-lattice moiré pattern for large angles and atomic reconstruction for small angles. We use density functional theory to calculate the band structures of the commensurate reconstructed domains and find that the modulation of the relative electronic band edges is consistent with the CAFM results and photoluminescence spectra. The presence of atomic reconstruction in TMD heterostructures and the observed impact on nanometer-scale electronic properties provide fundamental insight into the behavior of this important class of heterostructures.