arXiv subjects

Vincenzo Lordi

Publications and source records attributed to Vincenzo Lordi.

36 records · Page 2Linked to original sources

arXiv2024

Cross-scale covariance for material property prediction

A simulation can stand its ground against experiment only if its prediction uncertainty is known. The unknown accuracy of interatomic potentials (IPs) is a major source of prediction uncertainty, severely limiting the use of large-scale classical atomistic simulations in a wide range of scientific and engineering applications. Here we explore covariance between predictions of metal plasticity, from 178 large-scale ($\sim 10^8$ atoms) molecular dynamics (MD) simulations, and a variety of indicator properties computed at small-scales ($\leq 10^2$ atoms). All simulations use the same 178 IPs. In a manner similar to statistical studies in public health, we analyze correlations of strength with indicators, identify the best predictor properties, and build a cross-scale ``strength-on-predictors'' regression model. This model is then used to quantify uncertainty over the statistical pool of IPs. Small-scale predictors found to be highly covariant with strength are computed using expensive quantum-accurate calculations and used to predict flow strength, within the uncertainty bounds established in our statistical study.

cond-mat.mtrl-sci↗

arXiv2024

LTAU-FF: Loss Trajectory Analysis for Uncertainty in Atomistic Force Fields

Model ensembles are effective tools for estimating prediction uncertainty in deep learning atomistic force fields. However, their widespread adoption is hindered by high computational costs and overconfident error estimates. In this work, we address these challenges by leveraging distributions of per-sample errors obtained during training and employing a distance-based similarity search in the model latent space. Our method, which we call LTAU, efficiently estimates the full probability distribution function (PDF) of errors for any test point using the logged training errors, achieving speeds that are 2--3 orders of magnitudes faster than typical ensemble methods and allowing it to be used for tasks where training or evaluating multiple models would be infeasible. We apply LTAU towards estimating parametric uncertainty in atomistic force fields (LTAU-FF), demonstrating that its improved ensemble diversity produces well-calibrated confidence intervals and predicts errors that correlate strongly with the true errors for data near the training domain. Furthermore, we show that the errors predicted by LTAU-FF can be used in practical applications for detecting out-of-domain data, tuning model performance, and predicting failure during simulations. We believe that LTAU will be a valuable tool for uncertainty quantification (UQ) in atomistic force fields and is a promising method that should be further explored in other domains of machine learning.

cs.LG↗

arXiv2024

Direct Experimental Constraints on the Spatial Extent of a Neutrino Wavepacket

Despite their high relative abundance in our Universe, neutrinos are the least understood fundamental particles of nature. They also provide a unique system to study quantum coherence and the wavelike nature of particles in fundamental systems due to their extremely weak interaction probabilities. In fact, the quantum properties of neutrinos emitted in experimentally relevant sources are virtually unknown and the spatial extent of the neutrino wavepacket is only loosely constrained by reactor neutrino oscillation data with a spread of 13 orders of magnitude. Here, we present the first direct limits of this quantity through a new experimental concept to extract the energy width, $σ_{\textrm{N},E}$, of the recoil daughter nucleus emitted in the nuclear electron capture (EC) decay of $^7$Be. The final state in the EC decay process contains a recoiling $^7$Li nucleus and an electron neutrino ($ν_e$) which are entangled at their creation. The $^7$Li energy spectrum is measured to high precision by directly embedding $^7$Be radioisotopes into a high resolution superconducting tunnel junction that is operated as a cryogenic sensor. The lower limit on the spatial uncertainty of the recoil daughter was found to be $σ_{\textrm{N}, x} \geq 6.2$\,pm, which implies the final-state system is localized at a scale more than a thousand times larger than the nucleus itself. From this measurement, the first direct lower limits on the spatial extent of the neutrino wavepacket were extracted using two different theoretical methods. These results have wide-reaching implications in several areas including the nature of spatial localization at sub-atomic scales, interpretation of neutrino physics data, and the potential reach of future large-scale experiments.

nucl-ex↗

arXiv2023

Dangling bonds as possible contributors to charge noise in silicon and silicon-germanium quantum dot qubits

Spin qubits based on Si and Si$_{1-x}$Ge$_{x}$ quantum dot architectures exhibit among the best coherence times of competing quantum computing technologies, yet they still suffer from charge noise that limit their qubit gate fidelities. Identifying the origins of these charge fluctuations is therefore a critical step toward improving Si quantum-dot-based qubits. Here we use hybrid functional calculations to investigate possible atomistic sources of charge noise, focusing on charge trapping at Si and Ge dangling bonds (DBs). We evaluate the role of global and local environment in the defect levels associated with DBs in Si, Ge, and \sige alloys, and consider their trapping and excitation energies within the framework of configuration coordinate diagrams. We additionally consider the influence of strain and oxidation in charge-trapping energetics by analyzing Si and Ge$_{\rm Si}$ DBs in SiO$_2$ and strained Si layers in typical \sige quantum dot heterostructures. Our results identify that Ge dangling bonds are more problematic charge-trapping centers both in typical \sige alloys and associated oxidation layers, and they may be exacerbated by compositional inhomogeneities. These results suggest the importance of alloy homogeneity and possible passivation schemes for DBs in Si-based quantum dot qubits and are of general relevance to mitigating possible trap levels in other Si, Ge, and Si$_{1-x}$Ge$_{x}$-based metal-oxide-semiconductor stacks and related devices.

cond-mat.mtrl-sci↗

arXiv2023

Simulating noise on a quantum processor: interactions between a qubit and resonant two-level system bath

Material defects fundamentally limit the coherence times of superconducting qubits, and manufacturing completely defect-free devices is not yet possible. Therefore, understanding the interactions between defects and a qubit in a real quantum processor design is essential. We build a model that incorporates the standard tunneling model, the electric field distributions in the qubit, and open quantum system dynamics, and draws from the current understanding of two-level system (TLS) theory. Specifically, we start with one million TLSs distributed on the surface of a qubit and pick the 200 systems that are most strongly coupled to the qubit. We then perform a full Lindbladian simulation that explicitly includes the coherent coupling between the qubit and the TLS bath to model the time dependent density matrix of resonant TLS defects and the qubit. We find that the 200 most strongly coupled TLSs can accurately describe the qubit energy relaxation time. This work confirms that resonant TLSs located in areas where the electric field is strong can significantly affect the qubit relaxation time, even if they are located far from the Josephson junction. Similarly, a strongly-coupled resonant TLS located in the Josephson junction does not guarantee a reduced qubit relaxation time if a more strongly coupled TLS is far from the Josephson junction. In addition to the coupling strengths between TLSs and the qubit, the model predicts that the geometry of the device and the TLS relaxation time play a significant role in qubit dynamics. Our work can provide guidance for future quantum processor designs with improved qubit coherence times.

quant-ph↗

arXiv2022

Changes in electric-field noise due to thermal transformation of a surface ion trap

We aim to illuminate how the microscopic properties of a metal surface map to its electric-field noise characteristics. In our system, prolonged heat treatments of a metal film can induce a rise in the magnitude of the electric-field noise generated by the surface of that film. We refer to this heat-induced rise in noise magnitude as a thermal transformation. The underlying physics of this thermal transformation process is explored through a series of heating, milling, and electron treatments performed on a single surface ion trap. Between these treatments, $^{40}$Ca$^+$ ions trapped 70~$μ$m above the surface of the metal are used as detectors to monitor the electric-field noise at frequencies close to 1~MHz. An Auger spectrometer is used to track changes in the composition of the contaminated metal surface. With these tools we investigate contaminant deposition, chemical reactions, and atomic restructuring as possible drivers of thermal transformations.

cond-mat.mtrl-sci↗

arXiv2022

Material Effects on Electron Capture Decays in Cryogenic Sensors

Several current searches for physics beyond the standard model are based on measuring the electron capture (EC) decay of radionuclides implanted into cryogenic high-resolution sensors. The sensitivity of these experiments has already reached the level where systematic effects related to atomic-state energy changes from the host material are a limiting factor. One example is a neutrino mass study based on the nuclear EC decay of $^7$Be to $^7$Li inside cryogenic Ta-based sensors. To understand the material effects at the required level we have used density functional theory and modeled the electronic structure of lithium atoms in different atomic environments of the polycrystalline Ta absorber film. The calculations reveal that the Li 1s binding energies can vary by more than 2 eV due to insertion at different lattice sites, at grain boundaries, in disordered Ta, and in the vicinity of various impurities. However, the total range of Li 1s shifts does not exceed 4 eV, even for extreme amorphous disorder. Further, when investigating the effects on the Li 2s levels, we find broadening of more than 5 eV due to hybridization with the Ta band structure. Materials effects are shown to contribute significantly to peak broadening in Ta-based sensors that are used to search for physics beyond the standard model in the EC decay of $^7$Be, but they do not explain the full extent of observed broadening. Understanding these in-medium effects will be required for current- and future-generation experiments that observe low-energy radiation from the EC decay of implanted isotopes to evaluate potential limitations on the measurement sensitivity.

cond-mat.mtrl-sci↗

arXiv2021

How Correlated Adsorbate Dynamics on Realistic Substrates Can Give Rise to 1/ω Electric-Field Noise in Surface Ion Traps

Ion traps are promising architectures for implementing scalable quantum computing, but they suffer from excessive "anomalous" heating that prevents their full potential from being realized. This heating, which is orders of magnitude larger than that expected from Johnson-Nyquist noise, results in ion motion that leads to decoherence and reduced fidelity in quantum logic gates. The exact origin of anomalous heating is an open question, but experiments point to adsorbates on trap electrodes as a likely source. Many different models of anomalous heating have been proposed, but these models have yet to pinpoint the atomistic origin of the experimentally-observed $1/ω$ electric field noise scaling observed in ion traps at frequencies between 0.1-10 MHz. In this work, we perform the first computational study of the ion trap electric field noise produced by the motions of multiple monolayers of adsorbates described by first principles potentials. In so doing, we show that correlated adsorbate motions play a definitive role in producing $1/ω$ noise and identify candidate collective adsorbate motions, including translational and rotational motions of adsorbate patches and multilayer exchanges, that give rise to $1/ω$ scaling at the MHz frequencies typically employed in ion traps. These results demonstrate that multi-adsorbate systems, even simple ones, can give rise to a set of activated motions that can produce the $1/ω$ noise observed in ion traps and that collective, rather than individual, adsorbate motions are much more likely to give rise to low-frequency heating.

quant-ph↗

arXiv2019

On Quantifying Large Lattice Relaxations in Photovoltaic Devices

Temporal variations of Cu(In,Ga)Se$_2$ photovoltaic device properties during light exposure at various temperatures and voltage biases for times up to 100 h were analyzed using the kinetic theory of large lattice relaxations. Open-circuit voltage and p-type doping increased with charge injection and decreased with temperature at low injection conditions. Lattice relaxation can account for both trends and activation energies extracted from the data were approximately 0.9 and 1.2 eV for devices with lower and higher sodium content, respectively. In these devices, increased sodium content resulted in higher initial p-type doping with greater stability. First principles calculations providing revised activation energies for the ($V_{Se}-V_{Cu}$) complex suggest that this defect does not account for the metastability observed here.

physics.app-ph↗

arXiv2019

Electric-field noise from thermally-activated fluctuators in a surface ion trap

We probe electric-field noise near the metal surface of an ion trap chip in a previously unexplored high-temperature regime. We observe a non-trivial temperature dependence with the noise amplitude at 1-MHz frequency saturating around 500~K. Measurements of the noise spectrum reveal a $1/f^{α\approx1}$-dependence and a small decrease in $α$ between low and high temperatures. This behavior can be explained by considering noise from a distribution of thermally-activated two-level fluctuators with activation energies between 0.35~eV and 0.65~eV. Processes in this energy range may be relevant to understanding electric-field noise in ion traps; for example defect motion in the solid state and surface adsorbate binding energies. Studying these processes may aid in identifying the origin of excess electric-field noise in ion traps -- a major source of ion motional decoherence limiting the performance of surface traps as quantum devices.

quant-ph↗

arXiv2019

vdW-corrected density functional study of electric field noise heating in ion traps caused by electrode surface adsorbates

In order to realize the full potential of ion trap quantum computers, an improved understanding is required of the motional heating that trapped ions experience. Experimental studies of the temperature-, frequency-, and ion--electrode distance-dependence of the electric field noise responsible for motional heating, as well as the noise before and after ion bombardment cleaning of trap electrodes, suggest that fluctuations of adsorbate dipoles are a likely source of so-called `anomalous heating,' or motional heating of the trapped ions at a rate much higher than the Johnson noise limit. Previous computational studies have investigated how the fluctuation of model adsorbate dipoles affects anomalous heating. However, the way in which specific adsorbates affect the electric field noise has not yet been examined, and an electric dipole model employed in previous studies is only accurate for a small subset of possible adsorbates. Here, we analyze the behavior of both in-plane and out-of-plane vibrational modes of fifteen adsorbate--electrode combinations within the independent fluctuating dipole model, utilizing accurate first principles computational methods to determine the surface-induced dipole moments. We find the chemical specificity of the adsorbate can change the electric field noise by seven orders of magnitude and specifically that soft in-plane modes of weakly-adsorbed hydrocarbons produce the greatest noise and ion heating. We discuss the dynamics captured by the fluctuating dipole model, namely the adsorbate dependent turn-on temperature and electric field noise magnitude, and also discuss the model's failure to reproduce the measured 1/$ω$ noise frequency scaling with a single adsorbate species. We suggest future research directions for improved, quantitatively predictive models based on extensions of the present framework to multiple interacting adsorbates.

physics.atom-ph↗

arXiv2018

Anomalous Diffusion along Metal/Ceramic Interfaces

Hole formation in a polycrystalline Ni film on an $α$-Al$_2$O$_3$ substrate coupled with a continuum diffusion analysis demonstrates that Ni diffusion along the Ni/$α$-Al$_2$O$_3$ interface is surprisingly fast. Ab initio calculations demonstrate that both Ni vacancy formation and migration energies at the coherent Ni/$α$-Al$_2$O$_3$ interface are much smaller than in bulk Ni, suggesting that the activation energy for diffusion along coherent Ni/$α$-Al$_2$O$_3$ interfaces is comparable to that along (incoherent/high angle) grain boundaries. Based on these results, we develop a simple model for diffusion along metal/ceramic interfaces, apply to a wide range of metal/ceramic systems and validate it with several ab initio calculations. These results suggest that fast metal diffusion along metal/ceramic interfaces should be common, but is not universal.

cond-mat.mtrl-sci↗

arXiv2015

Lithium Ion Solvation and Diffusion in Bulk Organic Electrolytes from First Principles and Classical Reactive Molecular Dynamics

Lithium-ion battery performance is strongly influenced by the ionic conductivity of the electrolyte, which depends on the speed at which Li ions migrate across the cell and relates to their solvation structure. The choice of solvent can greatly impact both solvation and diffusivity of Li ions. We use first principles molecular dynamics to examine the solvation and diffusion of Li ions in the bulk organic solvents ethylene carbonate (EC), ethyl methyl carbonate (EMC), and a mixture of EC/EMC. We find that Li ions are solvated by either carbonyl or ether oxygen atoms of the solvents and sometimes by the PF$_6^-$ anion. Li$^+$ prefers a tetrahedrally-coordinated first solvation shell regardless of which species are involved, with the specific preferred solvation structure dependent on the organic solvent. In addition, we calculate Li diffusion coefficients in each electrolyte, finding slightly larger diffusivities in the linear carbonate EMC compared to the cyclic carbonate EC. The magnitude of the diffusion coefficient correlates with the strength of Li$^+$ solvation. Corresponding analysis for the PF$_6^-$ anion shows greater diffusivity associated with a weakly-bound, poorly defined first solvation shell. These results may be used to aid in the design of new electrolytes to improve Li-ion battery performance.

cond-mat.mtrl-sci↗

arXiv2014

Electronic and optical properties of GaSb:N from first principles

GaSb:N displays promise towards realization of optoelectronic devices accessing the mid-infrared wavelength regime. Theoretical and experimental results on its electronic and optical properties are however few. To address this, we present a first principles, density functional theory study using the hybrid HSE06 exchange-correlation functional of GaSb doped with 1.6$\%$ nitrogen. To study dilute-nitrides with small band gaps, the local density approximation (LDA) is insufficient and more accurate techniques such as HSE06 are needed. We conduct a comparative study on GaAs:N, also with 1.6$\%$ nitrogen mole fraction, and find that GaSb:N has a smaller band gap and displays more band gap bowing than GaAs:N. In addition we examine the orbital character of the bands, finding the lowest conduction band to be quasi-delocalized, with a large N-$3s$ contribution. At high concentrations, the N atoms interact via the host matrix, forming a dispersive band of their own which governs optoelectronic properties and dominates band gap bowing. While this band drives the optical and electronic properties of GaSb:N, its physics is not captured by traditional models for dilute-nitrides. We thus propose that a complete theory of dilute-nitrides should incorporate orbital character examination, especially at high N concentrations.

cond-mat.mtrl-sci↗

arXiv2014

Magnetic fluctuation from oxygen deficiency centers on the SiO$_2$ surface

The magnetic stability of oxygen deficiency centers on the surface of α-quartz is investigated with first- principles calculations to understand their role in contributing to magnetic flux noise in superconducting qubits (SQs) and superconducting quantum interference devices (SQUIDs) fabricated on amorphous silica substrates. Magnetic defects on the substrate are likely responsible for some of the 1/f noise that plagues these systems. Dangling-bonds associated with three-coordinated Si atoms allow electron density transfer between spin up and down channels, resulting in low energy magnetic states. Such under-coordinated Si defects are common in both stoichiometric and oxygen deficient silica and quartz and are a probable source of magnetic flux fluctuations in SQs and SQUIDs.

cond-mat.mtrl-sci↗

arXiv2012

Contributions of point defects, chemical disorder, and thermal vibrations to electronic properties of Cd(1-x)Zn(x)Te alloys

We present a first principles study based on density functional theory of thermodynamic and electronic properties of the most important intrinsic defects in the semiconductor alloy Cd(1-x)Zn(x)Te with x<0.13. The alloy is represented by a set of supercells with disorder on the Cd/Zn sublattice. Defect formation energies as well as electronic and optical transition levels are analyzed as a function of composition. We show that defect formation energies increase with Zn content with the exception of the neutral Te vacancy. This behavior is qualitatively similar to but quantitatively rather different from the effect of volumetric strain on defect properties in pure CdTe. Finally, the relative carrier scattering strengths of point defects, alloy disorder, and phonons are obtained. It is demonstrated that for realistic defect concentrations carrier mobilities are limited by phonon scattering for temperature above approximately 150 K.

cond-mat.mtrl-sci↗

arXiv2010

Intrinsic point defects in aluminum antimonide

Calculations within density functional theory on the basis of the local density approximation are carried out to study the properties of intrinsic point defects in aluminum antimonide. Special care is taken to address finite-size effects, band gap error, and symmetry reduction in the defect structures. The correction of the band gap is based on a set of GW calculations. The most important defects are identified to be the aluminum interstitial $Al_{i,Al}^{1+}$, the antimony antisites $Sb_{Al}^0$ and $Sb_{Al}^{1+}$, and the aluminum vacancy $V_{Al}^{3-}$. The intrinsic defect and charge carrier concentrations in the impurity-free material are calculated by self-consistently solving the charge neutrality equation. The impurity-free material is found to be n-type conducting at finite temperatures.

cond-mat.mtrl-sci↗

arXiv2010

Extrinsic point defects in aluminum antimonide

We investigate thermodynamic and electronic properties of group IV (C, Si, Ge, Sn) and group VI (O, S, Se, Te) impurities as well as P and H in aluminum antimonide (AlSb) using first-principles calculations. To this end, we compute the formation energies of a broad range of possible defect configurations including defect complexes with the most important intrinsic defects. We also obtain relative scattering cross strengths for these defects to determine their impact on charge carrier mobility. Furthermore, we employ a self-consistent charge equilibration scheme to determine the net charge carrier concentrations for different temperatures and impurity concentrations. Thereby, we are able to study the effect of impurities incorporated during growth and identify optimal processing conditions for achieving compensated material. The key findings are summarized as follows. Among the group IV elements, C, Si, and Ge substitute for Sb and act as shallow acceptors, while Sn can substitute for either Sb or Al and displays amphoteric character. Among the group VI elements, S, Se, and Te substitute for Sb and act as deep donors. In contrast, O is most likely to be incorporated as an interstitial and predominantly acts as an acceptor. As a group V element, P substitutes for Sb and is electrically inactive. C and O are the most detrimental impurities to carrier transport, while Sn, Se, and Te have a modest to low impact. Therefore, Te can be used to compensate C and O impurities, which are unintentionally incorporated during the growth process, with minimal effect on the carrier mobilities.

cond-mat.mtrl-sci↗