arXiv subjects

Manolo C. Per

Publications and source records attributed to Manolo C. Per.

6 recordsLinked to original sources

arXiv2025

Moments-based quantum computation of the electric dipole moment of molecular systems

With rapid progress being made in the development of platforms for quantum computation, there has been considerable interest in whether present-day and near-term devices can be used to solve problems of relevance. A commonly cited application area is the domain of quantum chemistry. While most experimental demonstrations of quantum chemical calculations on quantum devices have focused on the ground-state electronic energy of the system, other properties of the ground-state, such as the electric dipole moment, are also of interest. Here we employ the quantum computed moments (QCM) method, based on the Lanczos cluster expansion, to estimate the dipole moment of the water molecule on an IBM Quantum superconducting quantum device. The noise-mitigated results agree with full configuration interaction (FCI) calculations to within 0.03 $\pm$ 0.007 debye (2% $\pm$ 0.5%), compared to direct expectation value determination (i.e. VQE) with errors on the order of 0.07 debye (5%), even when the VQE calculation is performed without noise. This demonstrates that moments-based energy estimation techniques can be adapted to noise-robust evaluation of non-energetic ground-state properties of chemical systems.

quant-ph↗

arXiv2025

Chemically-Accurate Prediction of the Ionisation Potential of Helium Using a Quantum Processor

Quantum computers have the potential to revolutionise our understanding of the microscopic behaviour of materials and chemical processes by enabling high-accuracy electronic structure calculations to scale more efficiently than is possible using classical computers. Current quantum computing hardware devices suffer from the dual challenges of noise and cost, which raises the question of what practical value these devices might offer before full fault tolerance is achieved and economies of scale enable cheaper access. Here we examine the practical value of noisy quantum computers as tools for high-accuracy electronic structure, by using a Quantinuum ion-trap quantum computer to predict the ionisation potential of helium. By combining a series of techniques suited for use with current hardware including qubit-efficient encoding coupled with chemical insight, low-cost variational optimisation with hardware-adapted quantum circuits, and moments-based corrections, we obtain an ionisation potential of 24.5536 (+0.0011, -0.0005) eV, which agrees with the experimentally measured value to within true chemical accuracy, and with high statistical confidence. The methods employed here can be generalised to predict other properties and expand our understanding of the value that might be provided by near-term quantum computers.

quant-ph↗

arXiv2025

Reproducibility of fixed-node diffusion Monte Carlo across diverse community codes: The case of water-methane dimer

Fixed-node diffusion quantum Monte Carlo (FN-DMC) is a widely-trusted many-body method for solving the Schr\"{o}dinger equation, known for its reliable predictions of material and molecular properties. Furthermore, its excellent scalability with system complexity and near-perfect utilization of computational power makes FN-DMC ideally positioned to leverage new advances in computing to address increasingly complex scientific problems. Even though the method is widely used as a computational gold standard, reproducibility across the numerous FN-DMC code implementations has yet to be demonstrated. This difficulty stems from the diverse array of DMC algorithms and trial wave functions, compounded by the method's inherent stochastic nature. This study represents a community-wide effort to assess the reproducibility of the method, affirming that: Yes, FN-DMC is reproducible (when handled with care). Using the water-methane dimer as the canonical test case, we compare results from eleven different FN-DMC codes and show that the approximations to treat the non-locality of pseudopotentials are the primary source of the discrepancies between them. In particular, we demonstrate that, for the same choice of determinantal component in the trial wave function, reliable and reproducible predictions can be achieved by employing the T-move (TM), the determinant locality approximation (DLA), or the determinant T-move (DTM) schemes, while the older locality approximation (LA) leads to considerable variability in results. These findings demonstrate that, with appropriate choices of algorithmic details, fixed-node DMC is reproducible across diverse community codes-highlighting the maturity and robustness of the method as a tool for open and reliable computational science.

physics.comp-ph↗

arXiv2023

Reducing the time-step errors in diffusion Monte Carlo

We modify the reweighting factor of the projector used in diffusion Monte Carlo to reduce the time-step error of the total energy. Further, we present a reweighting scheme that has the desirable feature that it is exactly size-consistent, i.e, the energy of a system containing widely separated fragments is the same as the sum of the energies of the individual fragments. The practical utility of the latter improvement is that it reduces the time-step error of the binding energies of some weakly interacting systems.

physics.chem-ph↗

arXiv2012

Delocalised oxygen as the origin of two-level defects in Josephson junctions

One of the key problems facing superconducting qubits and other Josephson junction devices is the decohering effects of bi-stable material defects. Although a variety of phenomenological models exist, the true microscopic origin of these defects remains elusive. For the first time we show that these defects may arise from delocalisation of the atomic position of the oxygen in the oxide forming the Josephson junction barrier. Using a microscopic model, we compute experimentally observable parameters for phase qubits. Such defects are charge neutral but have non-zero response to both applied electric field and strain. This may explain the observed long coherence time of two-level defects in the presence of charge noise, while still coupling to the junction electric field and substrate phonons.

cond-mat.mes-hall↗

arXiv2012

Ab initio calculation of valley splitting in monolayer δ-doped phosphorus in silicon

The differences in energy between electronic bands due to valley splitting are of paramount importance in interpreting transport spectroscopy experiments on state-of-the-art quantum devices defined by scanning tunneling microscope lithography. We develop a plane-wave density functional theory description of these systems which is size-limited due to computational tractability. We then develop a less resource-intensive alternative via localized basis functions, retaining the physics of the plane-wave description, and extend this model beyond the capability of plane-wave methods to determine the ab initio valley splitting of well-isolated δ-layers. In obtaining agreement between plane-wave and delocalized methods, we show that the valley splitting has been overestimated in previous ab initio calculations by more than 50%.

cond-mat.mtrl-sci↗