arXiv subjects

James N. Fry

Publications and source records attributed to James N. Fry.

13 recordsLinked to original sources

arXiv2026

Simulating decoherence of two coupled spins using the generalized cluster correlation expansion

We simulate the coherence of two coupled electron spins interacting with a bath of nuclei using the generalized cluster correlation expansion (gCCE) method. An exchange interaction between the electrons facilitates a family of entangling gates that can be spoiled by nuclear-induced dephasing. Consequently, we study the dephasing of the coherent two-electron system by characterizing the $T_2$ and $T_2^*$ of the two-electron reduced density matrix for various system parameters in the range mimicking magnetic molecules, including magnetic field strength and orientation, exchange interaction strength, distance between the two spins, minimum distance between electron and nuclei and between nuclei, and nuclei density. We find the optimal regime for each parameter in which the coherence time is maximized and provide a physical understanding of it.

quant-ph↗

arXiv2025

Tuning the Magnetic Anisotropy Energy of MoS$_2$-supported Mn$_{12}$ complexes by Electric Field: A First-Principles Study

In this work, we examine low-energy adsorption configurations of four dodecanuclear manganese single-molecule magnets [Mn$_{12}$O$_{12}$(O$_2$CR)$_{16}$(H$_2$O)$_4$] (Mn$_{12}$), where the ligand R being H, CH$_3$, CHCl$_2$ or C$_6$H$_5$, on a molybdenum disulfide (MoS$_2$) monolayer using force field and density functional theory calculations. The van der Waals interaction is shown to be crucial for determining the adsorption energy. Some electrons transfer from the substrate to the molecules upon surface adsorption, resulting in a reduction of the magnetic anisotropy energy of Mn$_{12}$. Since the lowest unoccupied molecular orbital of Mn$_{12}$ is close to the valence band of MoS$_2$, a negative electric field is more effective in modulating charge transfer and energy band alignment, and thus altering the magnetic anisotropy energy, compared with a positive electric field. A significant increase in the magnetic anisotropy energy of Mn$_{12}$ with the ligand R=CHCl$_2$ or R=C$_6$H$_5$ under a sufficiently high electric field has been predicted. Our calculations show that the molecules remain intact on the surface both before and after the electric field is applied. Finally, a two-level system formed by different adsorption configurations is evaluated, and the tunability of its energy barrier under an electric field is demonstrated. Our study sheds light on tuning the properties of single-molecule magnets using an electric field, when the molecules are supported on a surface.

cond-mat.mtrl-sci↗

arXiv2025

Machine Learning Assisted Modeling of Amorphous TiO$_2$-Doped GeO$_2$ for Advanced LIGO Mirror Coatings

The mechanical loss angle of amorphous TiO$_2$-doped GeO$_2$ can be lower than 10$^{-4}$, making it a candidate for Laser Interferometer Gravitational-wave Observatory (LIGO) mirror coatings. Amorphous oxides have complex atomic structures that are influenced by various factors, including doping concentration, preparation, and thermal history, resulting in different mass densities and physical properties. Modeling at atomistic level enables capturing these effects by generating atomic structure models according to experimental conditions. In order to obtain reliable and physical amorphous models at an affordable cost, we develop classical and machine-learning potentials (MLP) to speed up simulations. First-principles calculations are used to train and validate MLP as well as validating structure models. To better reproduce properties such as elastic modulus, radial distribution function (RDF) and the variations in mass density of doped amorphous oxides, density functional theory (DFT) calculations are used to optimize the final models. We find that the mass densities of amorphous systems are correlated with the total void volume. The experimental mass density matches the models with the most symmetric potential energy wells under volume change. The elastic response of the metal-oxygen network is also studied. The 27\% TiO$_2$ doped GeO$_2$ system shows the least number of large atom-atom distance changes, while for 44\% TiO$_2$ doped GeO$_2$, a majority of Ti-O distances are significantly changed. In response to strains, the metal-oxygen network at low mass densities prefers to adjust bond angles, while at high mass densities, the adjustment is mainly done by changing atom-atom distance.

cond-mat.mtrl-sci↗

arXiv2024

RASCBEC: RAman Spectroscopy Calculation via Born Effective Charge

We advance the algorithm for ab initio calculations of Raman spectra for large systems via applying external electric field, and complement it by a code implementation we name RASCBEC. With the RASCBEC code, we have successfully benchmark crystalline materials and compute Raman spectra of large molecules, and amorphous oxides. Our results demonstrate a remarkable level of agreement with the results from other commonly used codes as well as the experimental data. The electric field approach for Raman spectra calculation is designed to overcome the computational challenges associated with the conventional approach, which requires the calculation of the macroscopic dielectric tensor at numerous molecular geometries. The key innovation in our approach lies in obtaining the first-order derivatives with respect to the external electric field directly from VASP (the Vienna Ab Initio Simulation Package), as the Born Effective Charge (BEC). The RASCBEC code not only significantly reduces computational time, up to a factor of $N/8$, compared to the conventional approach, where $N$ is the total count of atoms within the simulation box. But also maintains the same level of accuracy, employing first-order numerical derivatives that avoid the numerical noise associated with algorithms requiring second-order derivatives, as seen in other electric field-based methods. This advantage makes RASCBEC particularly beneficial for large molecules and expansive amorphous systems.

physics.comp-ph↗

arXiv2023

Spin decoherence in VOPc@graphene nanoribbon complexes

Carbon nanoribbon or nanographene qubit arrays can facilitate quantum-to-quantum transduction between light, charge, and spin, making them an excellent testbed for fundamental science in quantum coherent systems and for the construction of higher-level qubit circuits. In this work, we study spin decoherence due to coupling with a surrounding nuclear spin bath of an electronic molecular spin of a vanadyl phthalocyanine (VOPc) molecule integrated on an armchair-edged graphene nanoribbon (GNR). Density functional theory (DFT) is used to obtain ground state atomic configurations. Decay of spin coherence in Hahn echo experiments is then simulated using the cluster correlation expansion method with a spin Hamiltonian involving hyperfine and electric field gradient tensors calculated from DFT. We find that the decoherence time $T_2$ is anisotropic with respect to magnetic field orientation and determined only by the hydrogen nuclear spins both on VOPc and GNR. Large electron spin echo envelope modulation (ESEEM) due to nitrogen and vanadium nuclear spins is present at specific field ranges and can be completely suppressed by tuning the magnetic field. The relation between these field ranges and the hyperfine interactions is analyzed. The effects of interactions with the nuclear quadrupole moments are also studied, validating the applicability and limitations of the spin Hamiltonian when they are disregarded.

cond-mat.mes-hall↗

arXiv2022

Clar's goblet on graphene: field modulated charge transfer in a hydrocarbon heterostructure

In certain configurations, the aromatic properties of benzene ring structured molecules allow for unpaired, reactive valence electrons (known as radicals). Clar's goblets are such molecules. With an even number of unpaired radicals, these nanographenes are topologically frustrated hydrocarbons in which pi-bonding network and topology of edges give rise to the magnetism. Clar's goblets are therefore valued as prospective qubits provided they can be modulated between magnetic states. Using first principles DFT, we demonstrate the effects of adsorption on both molecule and substrate in a graphene-Clar's goblet heterostructure. We look at the energy difference bewteen FM and AFM states of the system and discuss underlying physical and chemical mechanisms in reference to the highest occupied molecular orbital (HOMO) and second HOMO (HOMO-1). We find that the HOMO of the molecule in the FM state is right at the Fermi surface, which leads to the hybridization between molecular state and the graphene state near the Dirac point. Furthermore, we investigate qualitative changes in charge realignment and magnetic state under variable electric field. Transitions from FM to AFM and back to FM states are observed.

cond-mat.mes-hall↗

arXiv2022

Insights to negative differential resistance in \texorpdfstring{MoS\textsubscript{2}}{MoS2} Esaki diodes: a first-principles perspective

\ce{MoS_2} is a two dimensional material with a band gap depending on the number of layers and tunable by an external electric field. The experimentally observed intralayer band-to-band tunneling and interlayer band-to-band tunneling in this material present an opportunity for new electronic applications in tunnel field effect transistors. However, such a widely accepted concept has never been supported up by theoretical investigations based on first principles. In this work, using density functional theory, in conjunction with non-equilibrilibrium Green's function techniques and our electric field gating method, enabled by a large-scale computational approach, we study the relation between band alignment and transmission in planar and side-stack \ce{MoS_2} $p$-$i$-$n$ junction configurations. We demonstrate the presence of negative differential resistance for both in-plane and interlayer current, a staple characteristic of tunnel diode junctions, and analyze the physical origin of such an effect. Electrostatic potentials, the van der Waals barrier, and complex band analysis are also examined for a thorough understanding of Esaki Diodes.

cond-mat.mes-hall↗

arXiv2022

Single-Molecule Magnet Mn$_{12}$ on GaAs-supported Graphene: Gate Field Effects From First Principles

We study gate field effects on the Mn$_{12}$O$_{12}$(COOH)$_{16}$(H$_2$O)$_4$ | graphene | GaAs heterostructure via first-principles calculations. We find that under moderate doping levels electrons can be added to but not taken from the single-molecule magnet Mn$_{12}$O$_{12}$(COOH)$_{16}$(H$_2$O)$_4$ (Mn$_{12}$). The magnetic anisotropy energy (MAE) of Mn$_{12}$ decreases as the electron doping level increases, due to electron transfer from graphene to Mn$_{12}$ and change in the band alignment between Mn$_{12}$ and graphene. At an electron doping level of $-5.00 \times 10^{13}\, \textrm{cm}^{-2}$, the MAE decreases by about 18% compared with zero doping. The band alignment between graphene and GaAs is more sensitive to electron doping than to hole doping since the valence band of GaAs is close to the Fermi level. The GaAs substrate induces a small bandgap in the supported graphene under the zero gate field and a nearly strain-free configuration. Finally, we propose a vertical tunnel junction for probing the gate dependence of MAE via electron transport measurements.

cond-mat.mtrl-sci↗

arXiv2020

Multiple Control of Few-layer Janus MoSSe Systems

In this computational work based on density functional theory we study the electronic and electron transport properties of asymmetric multi-layer MoSSe junctions, known as Janus junctions. Focusing on 4-layer systems, we investigate the influence of electric field, electrostatic doping, strain, and interlayer stacking on the electronic structure. We discover that a metal to semiconductor transition can be induced by an out-of-plane electric field. The critical electric field for such a transition can be reduced by in-plane biaxial compressive strain. Due to an intrinsic electric field, a 4-layer MoSSe can rectify out-of-plane electric current. The rectifying ratio reaches 34.1 in a model junction Zr/4-layer MoSSe/Zr. This ratio can be further enhanced by increasing the number of MoSSe layers. In addition, we show a drastic sudden vertical compression of 4-layer MoSSe due to in-plane biaxial tensile strain, indicating a second phase transition. Furthermore, an odd-even effect on electron transmission at the Fermi energy for Zr/$n$-layer MoSSe/Zr junctions with $n=1, \, 2,\, 3, \,\dots,\, 10$ is observed. These findings reveal the richness of physics in this asymmetric system and strongly suggest that the properties of 4-layer MoSSe are highly tunable, thus providing a guide to future experiments relating materials research and nanoelectronics.

cond-mat.mtrl-sci↗

arXiv2020

Gate field effects on the topological insulator BiSbTeSe2 interface

Interfaces between two topological insulators are of fundamental interest in condensed matter physics. Inspired by experimental efforts, we study interfacial processes between two slabs of BiSbTeSe2 (BSTS) via first principles calculations. Topological surface states are absent for the BSTS interface at its equilibrium separation, but our calculations show that they appear if the inter-slab distance is greater than 6 Ang. More importantly, we find that topological interface states can be preserved by inserting two or more layers of hexagonal boron nitride between the two BSTS slabs. In experiments, the electric current tunneling through the interface is insensitive to back gate voltage when the bias voltage is small. Using a first-principles based method that allows us to simulate gate field, we show that at low bias the extra charge induced by a gate voltage resides on the surface that is closest to the gate electrode, leaving the interface almost undoped. This provides clues to understand the origin of the observed insensitivity of transport properties to back voltage at low bias. Our study resolves a few questions raised in experiment, which does not yet offer a clear correlation between microscopic physics and transport data. We provide a road map for the design of vertical tunneling junctions involving the interface between two topological insulators.

cond-mat.mtrl-sci↗

arXiv2012

Gaussianizing the non-Gaussian lensing convergence field II: the applicability to noisy data

In paper I (Yu et al. [1]), we show through N-body simulation that a local monotonic Gaussian transformation can significantly reduce non-Gaussianity in a noise-free lensing convergence field. This makes the Gaussianization a promising theoretical tool to understand high-order lensing statistics. Here we present a study of its applicability in lensing data analysis, in particular when shape measurement noise is presented in lensing convergence maps. (i) We find that shape measurement noise significantly degrades the Gaussianization performance and the degradation increases for shallower surveys. (ii) The Wiener filter is efficient in reducing the impact of shape measurement noise. The Gaussianization of the Wiener-filtered lensing maps is able to suppress skewness, kurtosis, and the 5th- and 6th-order cumulants by a factor of 10 or more. It also works efficiently to reduce the bispectrum to zero.

astro-ph.CO↗

arXiv2011

Gaussianizing the non-Gaussian lensing convergence field I: the performance of the Gaussianization

Motivated by recent works of Neyrinck et al. 2009 and Scherrer et al. 2010, we proposed a Gaussianization transform to Gaussianize the non-Gaussian lensing convergence field $κ$. It performs a local monotonic transformation $κ\rightarrow y$ pixel by pixel to make the unsmoothed one-point probability distribution function of the new variable $y$ Gaussian. We tested whether the whole $y$ field is Gaussian against N-body simulations. (1) We found that the proposed Gaussianization suppresses the non-Gaussianity by orders of magnitude, in measures of the skewness, the kurtosis, the 5th- and 6th-order cumulants of the $y$ field smoothed over various angular scales relative to that of the corresponding smoothed $κ$ field. The residual non-Gaussianities are often consistent with zero within the statistical errors. (2) The Gaussianization significantly suppresses the bispectrum. Furthermore, the residual scatters around zero, depending on the configuration in the Fourier space. (3) The Gaussianization works with even better performance for the 2D fields of the matter density projected over $\sim 300 \mpch$ distance interval centered at $z\in(0,2)$, which can be reconstructed from the weak lensing tomography. (4) We identified imperfectness and complexities of the proposed Gaussianization. We noticed weak residual non-Gaussianity in the $y$ field. We verified the widely used logarithmic transformation as a good approximation to the Gaussianization transformation. However, we also found noticeable deviations.

astro-ph.CO↗

arXiv2003

An estimate of Ω_m without priors

Using mean relative peculiar velocity measurements for pairs of galaxies, we estimate the cosmological density parameter $Ω_m$ and the amplitude of density fluctuations $σ_8$. Our results suggest that our statistic is a robust and reproducible measure of the mean pairwise velocity and thereby the $Ω_m$ parameter. We get $Ω_m = 0.30^{+0.17}_{-0.07}$ and $σ_8 = 1.13^{+0.22}_{-0.23}$. These estimates do not depend on prior assumptions on the adiabaticity of the initial density fluctuations, the ionization history, or the values of other cosmological parameters.

astro-ph↗