arXiv subjects

Jyh-Pin Chou

Publications and source records attributed to Jyh-Pin Chou.

18 recordsLinked to original sources

arXiv2026

Correlation-Converged Virtual Orbitals for Accurate and Efficient Quantum Molecular Simulations

Density functional theory with plane-wave basis sets is widely employed in computational materials science, including applications to isolated molecular systems. However, the inadequate description of electron correlation remains a fundamental limitation. Accurate correlation treatments based on many-body Hamiltonians require reliable representations of both occupied and virtual orbitals, yet virtual orbitals are often poorly described in conventional computational schemes, resulting in reduced accuracy. In this work, we introduce localized correlation-converged virtual orbitals (LCCVOs) as an efficient basis for constructing accurate many-body Hamiltonians in molecular systems. Using a substantially reduced number of orbitals, the LCCVO framework yields dissociation energies for singlet, doublet, and triplet molecules that are comparable to, and in many cases exceed, those obtained with high-level correlation-consistent basis sets such as cc-pVXZ (X = D, T, Q, 5). These results demonstrate the efficiency, scalability, and robustness of the LCCVO approach for high-accuracy quantum chemical calculations.

physics.chem-ph↗

arXiv2026

Physics-Informed 3D Atomic Reconstruction and Dynamics of Free-Standing Graphene from Single Low-Dose TEM Images

Resolving the three-dimensional (3D) atomic geometry of free-standing graphene in real time is essential for understanding how intrinsic rippling governs its electronic properties. However, the low electron doses required to mitigate radiation damage impose severe signal-to-noise constraints that limit conventional reconstruction methods. Here, we present a physics-informed computational framework that reconstructs 3D atomic coordinates of single-layer graphene from individual low-dose transmission electron microscopy (TEM) frames (8x10^3 e-/Ang^2, 1 ms temporal resolution). The approach combines simulated annealing optimisation with molecular dynamics regularisation, achieving sub-angstrom out-of-plane accuracy (sigma_z < 0.45 Ang), validated against ground-truth simulations. A Kullback-Leibler divergence-based calibration aligns the forward model with experimental image statistics, reducing systematic bias. Applied to high-speed time-series data, the framework enables simultaneous extraction of real-time ripple dynamics, strain tensors, surface curvature, bond-length distributions, and density functional theory (DFT)-derived electron localisation functions (ELF). We establish quantitative relationships linking local geometry, strain, and bond-length variations to electron localisation, demonstrating that sub-angstrom structural fluctuations drive spatially localised, millisecond-scale electronic modulation. A critical dose threshold is identified below which structural information becomes irrecoverable, providing practical guidance for experimental design. The framework is broadly applicable to beam-sensitive two-dimensional materials.

cond-mat.mtrl-sci↗

arXiv2024

Ultrafast spintronics with geometric effects in non-adiabatic wave-packet dynamics

Motivated by the intriguing possibilities of steering ultrafast non-adiabatic processes through the geometric properties of bands in quantum materials by laser pulses, we extend a wave-packet transport theory, previously well-established in the adiabatic regime that intuitively captured geometric properties of bands, to the transient and non-adiabatic regime. This extension facilitates us to investigate macroscopic ways of manifesting microscopic band-geometric effects that highlight the special capability of non-adiabatic drivings not available to adiabatic drivings. These include imprinting band-geometric properties to the current rate after switching off the laser pulses and the induction of intrinsic macroscopic spin polarisation with an orientation not accessible by adiabatic processes. In particular, the microscopic geometrically-rooted intrinsic spin coherence is shown to underlie the spin-mediated parts of the macroscopic photocurrents. Through explicit calculations of an example with Rashba spin-orbit coupling, the spin-mediated part is shown to be discernible from the non-spin-mediated part in terms of the anisotropy of the photocurrents. Working principles behind the above theoretical results allegedly applicable beyond the Rashba example are distilled to inspect experimental data collected for SnSe, exhibiting considerable anisotropic effects. Consistency between theory and experiment is observed, paving the way of further exploration into the above intended direction.

cond-mat.mes-hall↗

arXiv2024

Molecular Ground State Simulation by Subspace Restriction and Hund's Rule

Simulation of molecular ground states on near-term quantum hardware is constrained by qubit availability and the cost of variational optimization. To address these challenges, the Subspace Restriction Scheme (SRS) is introduced as a mathematical framework that projects the molecular Hamiltonian onto a selected Fock subspace prior to qubit encoding. By enforcing molecular multiplicity and a generalized Hund's rule, the Multi-Hund Subspace (MHS) is constructed. This physically motivated restriction significantly reduces the effective Fock-space dimension, asymptotically saving $N$ qubits for a Hamiltonian of $M$ spatial orbitals and $N$ electrons. As a result, we successfully overcome classical memory bottlenecks and enable simulations of large systems, such as the $H_{22}$ chain, which requires 44 qubits under standard Jordan-Wigner (JW) encoding. While the strict pairing structure may limit accuracy in strongly correlated dissociation regimes, MHS effectively captures the essential low-energy physics of closed-shell molecules near equilibrium. In Variational Quantum Eigensolver (VQE) benchmarks, MHS enhances optimization behaviour and achieves high accuracy with a shallow ansatz. These findings demonstrate that physically motivated subspace restriction offers an effective approach to more resource-efficient quantum-chemistry simulations.

quant-ph↗

arXiv2024

Unveiling the stacking-dependent electronic properties of 2D ultrathin rare-earth metalloxenes family LnX$_2$ (Ln = Eu, Gd, Dy; X = Ge, Si)

The studies of electronic effects in reduced dimensionality have become a frontier in nanoscience due to exotic and highly tunable character of quantum phenomena. Recently, a new class of 2D ultrathin Ln$X_2$ metalloxenes composed of a triangular lattice of lanthanide ions (Ln) coupled with 2D-Xenes of silicene or germanene ($X_2$) was introduced and studied with a particular focus on magnetic and transport properties. However, the electronic properties of metalloxenes and their effective functionalization remain mainly unexplored. Here, using a number of experimental and theoretical techniques, we trace the evolution of electronic properties and magnetic ground state of metalloxenes triggered by external perturbations. We demonstrate that the band structure of Ln$X_2$ films can be uniquely modified by controlling the Xenes stacking, thickness, varying the rare-earth and host elements, and applying an external electric field. Our findings suggest new pathways to manipulate the electronic properties of 2D rare-earth magnets that can be adjusted for spintronics applications.

cond-mat.mtrl-sci↗

arXiv2023

Accurate harmonic vibrational frequencies for diatomic molecules via quantum computing

During the noisy intermediate-scale quantum (NISQ) era, quantum computational approaches refined to overcome the challenge of limited quantum resources are highly valuable. However, the accuracy of the molecular properties predicted by most of the quantum computations nowadays is still far off (not within chemical accuracy) compared to their corresponding experimental data. Here, we propose a promising qubit-efficient quantum computational approach to calculate the harmonic vibrational frequencies of a large set of neutral closed-shell diatomic molecules with results in great agreement with their experimental data. To this end, we construct the accurate Hamiltonian using molecular orbitals, derived from density functional theory to account for the electron correlation and expanded in the Daubechies wavelet basis set to allow an accurate representation in real space grid points, where an optimized compact active space is further selected so that only a reduced small number of qubits is sufficient to yield an accurate result. To justify the approach, we benchmark the performance of the Hamiltonians spanned by the selected molecular orbitals by first transforming the molecular Hamiltonians into qubit Hamiltonians and then using the exact diagonalization method to calculate the results, regarded as the best results achievable by quantum computation. Furthermore, we show that the variational quantum circuit with the chemistry-inspired UCCSD ansatz can achieve the same accuracy as the exact diagonalization method except for systems whose Mayer bond order indices are larger than 2. For those systems, we demonstrate that the heuristic hardware-efficient RealAmplitudes ansatz, even with a shorter circuit depth, can provide a significant improvement over the UCCSD ansatz, verifying that the harmonic vibrational frequencies could be calculated accurately by quantum computation in the NISQ era.

quant-ph↗

arXiv2023

\emph{Ab initio} study of (100) diamond surface spins

Unpaired electronic spins at diamond surfaces are ubiquitous and can lead to excess magnetic noise. They have been observed in several studies to date, but their exact chemical nature is still unknown. We propose a simple model to explain the existence and chemical stability of surface spins associated with the $sp^3$ dangling bond on the (100) diamond surface using density functional theory. We find that the (111) facet, which is naturally generated at a step edge of (100) crystalline diamond surface, can sterically protect a spinful defect. Our study reveals a mechanism for annihilation of these surface spins upon annealing, consistent with recent experimental results. We also demonstrate that the Fermi-contact term in the hyperfine coupling is not negligible between the surface spins and the surrounding nuclear spins, and thus \textit{ab initio} simulation can be used to devise a sensing protocol where the surface spins act as reporter spins to sense nuclear spins on the surface.

quant-ph↗

arXiv2022

Accurate and Efficient Quantum Computations of Molecular Properties Using Daubechies Wavelet Molecular Orbitals: A Benchmark Study against Experimental Data

Although quantum computation (QC) is regarded as a promising numerical method for computational quantum chemistry, current applications of quantum-chemistry calculations on quantum computers are limited to small molecules. This limitation can be ascribed to technical problems in building and manipulating more qubits and the associated complicated operations of quantum gates in a quantum circuit when the size of the molecular system becomes large. As a result, reducing the number of required qubits is necessary to make QC practical. Currently, the minimal STO-3G basis set is commonly used in benchmark studies because it requires the minimum number of spin orbitals. Nonetheless, the accuracy of using STO-3G is generally low and thus cannot provide useful predictions. We propose to adopt Daubechies wavelet functions as an accurate and efficient method for QCs of molecular electronic properties. We demonstrate that a minimal basis set constructed from Daubechies wavelet basis can yield accurate results through a better description of the molecular Hamiltonian, while keeping the number of spin orbitals minimal. With the improved Hamiltonian through Daubechies wavelets, we calculate vibrational frequencies for H$_2$ and LiH using quantum-computing algorithm to show that the results are in excellent agreement with experimental data. As a result, we achieve quantum calculations in which accuracy is comparable with that of the full configuration interaction calculation using the cc-pVDZ basis set, whereas the computational cost is the same as that of a STO-3G calculation. Thus, our work provides a more efficient and accurate representation of the molecular Hamiltonian for efficient QCs of molecular systems, and for the first time demonstrates that predictions in agreement with experimental measurements are possible to be achieved with quantum resources available in near-term quantum computers.

quant-ph↗

arXiv2021

Find The Optimized Structure of 5CBs

We use density functional theory (DFT) to investigate the geometric and electronic structures of multiple 5CB molecules. There are three parts for this research, test of the arrangement property of the 5CB molecule, calculation of two 4-n-pentyl-4-cyanobiphenyl (5CB), and four molecules 5CB structure arrangement. First part reveals the result, which the two 5CBs pointing in opposite directions case possesses lower total energy, that has the same result of the optimized caused by the nematic property of 5CBs. In the result of two 5CBs calculation, two 5CBs optimized structures always appears at least one pair of parallel plains formed by the head benzene of one 5CB and the carbon chain. In the four 5CBs optimized structure case, we can find out several pairs of parallel plains consist of benzene plains and one parallel plain in two carbon chain.

cond-mat.mtrl-sci↗

arXiv2021

Probing spin dynamics on diamond surfaces using a single quantum sensor

Understanding the dynamics of a quantum bit's environment is essential for the realization of practical systems for quantum information processing and metrology. We use single nitrogen-vacancy (NV) centers in diamond to study the dynamics of a disordered spin ensemble at the diamond surface. Specifically, we tune the density of "dark" surface spins to interrogate their contribution to the decoherence of shallow NV center spin qubits. When the average surface spin spacing exceeds the NV center depth, we find that the surface spin contribution to the NV center free induction decay can be described by a stretched exponential with variable power n. We show that these observations are consistent with a model in which the spatial positions of the surface spins are fixed for each measurement, but some of them reconfigure between measurements. In particular, we observe a depth-dependent critical time associated with a dynamical transition from Gaussian (n=2) decay to n=2/3, and show that this transition arises from the competition between the small decay contributions of many distant spins and strong coupling to a few proximal spins at the surface. These observations demonstrate the potential of a local sensor for understanding complex systems and elucidate pathways for improving and controlling spin qubits at the surface.

quant-ph↗

arXiv2020

Material Platforms for Defect Qubits and Single Photon Emitters

Quantum technology has grown out of quantum information theory and now provides a valuable tool that researchers from numerous fields can add to their toolbox of research methods. To date, various systems have been exploited to promote the application of quantum information processing. The systems that can be used for quantum technology include superconducting circuits, ultra-cold atoms, trapped ions, semiconductor quantum dots, and solid-state spins and emitters. In this review, we will discuss the state of the art on material platforms for spin-based quantum technology, with a focus on the progress in solid-state spins and emitters in several leading host materials, including diamond, silicon carbide, boron nitride, silicon, two-dimensional semiconductors, and other materials. We will highlight how first-principles calculations can serve as an exceptionally robust tool for finding the novel defect qubits and single photon emitters in solids, through detailed predictions of the electronic, magnetic and optical properties.

cond-mat.mtrl-sci↗

arXiv2020

Giant shift upon strain on the fluorescence spectrum of V$_{\rm N}$N$_{\rm B}$ color centers in $h$-BN

We study the effect of strain on the physical properties of the nitrogen antisite-vacancy pair in hexagonal boron nitride ($h$-BN), a color center that may be employed as a quantum bit in a two-dimensional material. With group theory and ab-initio analysis we show that strong electron-phonon coupling plays a key role in the optical activation of this color center. We find a giant shift on the zero-phonon-line (ZPL) emission of the nitrogen antisite-vacancy pair defect upon applying strain that is typical of $h$-BN samples. Our results provide a plausible explanation for the experimental observation of quantum emitters with similar optical properties but widely scattered ZPL wavelengths and the experimentally observed dependence of the ZPL on the strain.

cond-mat.mtrl-sci↗

arXiv2019

Ab initio theory of negatively charged boron vacancy qubit in hBN

Highly correlated orbitals coupled with phonons in two-dimension are identified for paramagnetic and optically active boron vacancy in hexagonal boron nitride by first principles methods which are responsible for recently observed optically detected magnetic resonance signal. We report ab initio analysis of the correlated electronic structure of this center by density matrix renormalization group and Kohn-Sham density functional theory methods. By establishing the nature of the bright and dark states as well as the position of the energy levels, we provide a complete description of the magneto-optical properties and corresponding radiative and non-radiative routes which are responsible for the optical spin polarization and spin dependent luminescence of the defect. Our findings pave the way toward advancing the identification and characterization of room temperature quantum bits in two-dimensional solids.

cond-mat.mes-hall↗

arXiv2019

Oxygenated (113) diamond surface for nitrogen-vacancy quantum sensors with preferential alignment and long coherence time from first principles

Shallow nitrogen-vacancy (NV) center in diamond is promising in quantum sensing applications however its sensitivity has been limited by surface terminators and defects. There is an immediate quest to find suitable diamond surfaces for NV sensors. In this work, the surface terminators of (113) diamond to host shallow NV centers are studied by means of first principles calculations. Results indicate that complete oxygen termination of (113) diamond creates positive electron affinity with neither strain on the surface nor in-gap levels. This is a very surprising result as the commonly employed oxygenated (001) diamond surface is often defective due to the disorder created by the strain of ether groups at the surface that seriously undermine the coherence properties of the shallow NV centers. The special atomic configurations on (113) diamond surface are favorable for oxygen bonding, in contrast to (001) and (111) diamond surfaces. These simulations imply that oxygenated diamond (113) surface can be produced by conventional diamond chemical vapor deposition growth. Combining this with the ~73% preferential alignment of as-grown NV centers in (113) oriented diamond, oxygenated (113) diamond is presently supposed to be the most prospective host for NV quantum sensors.

cond-mat.mes-hall↗

arXiv2018

Evidence for Primal sp2 Defects at the Diamond Surface: Candidates for Electron Trapping and Noise Sources

Diamond materials are central to an increasing range of advanced technological demonstrations, from high power electronics, to nano-scale quantum bio-imaging with unprecedented sensitivity. However, the full exploitation of diamond for these applications is often limited by the uncontrolled nature of the diamond material surface, which suffers from Fermi-level pinning and hosts a significant density of electro-magnetic noise sources. These issues occur despite the oxide-free and air-stable nature of the diamond crystal surface, which should be an ideal candidate for functionalization and chemical-engineering. In this work we reveal a family of previously unidentified and near-ubiquitous primal surface defects which we assign to differently reconstructed surface vacancies. The density of these defects is quantified with X-ray absorption spectroscopy, their energy structures are elucidated by ab initio calculations, and their effect on near-surface quantum probes is measured directly. Subsequent ab-initio calculation of band-bending from these defects suggest they are the source of Fermi-level pinning at most diamond surfaces. Finally, an investigation is conducted on a broad range of post-growth surface treatments and concludes that none of them can reproducibly reduce this defect density below the Fermi-pinning threshold, making this defect a prime candidate as the source for decoherence-limiting noise in near-surface quantum probes.

cond-mat.mes-hall↗

arXiv2018

Color centers in hexagonal boron nitride monolayers: A group theory and ab-initio analysis

We theoretically study physical properties of the most promising color center candidates for the recently observed single-photon emissions in hexagonal boron nitride (h-BN) monolayers. Through our group theory analysis combined with density functional theory (DFT) calculations we provide several pieces of evidence that the electronic properties of the color centers match the characters of the experimentally observed emitters. We calculate the symmetry-adapted multi-electron wavefunctions of the defects using group theory methods and analyze the spin-orbit and spin-spin interactions in detail. We also identify the radiative and non-radiative transition channels for each color center. An advanced ab-initio DFT method is then used to compute energy levels of the color centers and their zero-phonon-line (ZPL) emissions. The computed ZPLs, the profile of excitation and emission dipole polarizations, and the competing relaxation processes are discussed and matched with the observed emission lines. By providing evidence for the relation between single-photon emitters and local defects in h-BN, this work provides the first steps towards harnessing quantum dynamics of these color centers.

cond-mat.mes-hall↗

arXiv2018

First principles study of charge diffusion between proximate solid state qubits and its implications on sensor applications

Solid state qubits from paramagnetic point defects in solids are promising platforms to realize quantum networks and novel nanoscale sensors. Recent advances in materials engineering make possible to create proximate qubits in solids that might interact with each other, leading to electron spin/charge fluctuation. Here we develop a method to calculate the tunneling-mediated charge diffusion between point defects from first principles, and apply it to nitrogen-vacancy (NV) qubits in diamond. The calculated tunneling rates are in quantitative agreement with previous experimental data. Our results suggest that proximate neutral and negatively charged NV defect pairs can form an NV--NV molecule. A tunneling-mediated model for the source of decoherence of the near-surface NV qubits is developed based on our findings on the interacting qubits in diamond.

cond-mat.mes-hall↗

arXiv2017

All-optical hyperpolarization of electron and nuclear spins in diamond

Low thermal polarization of nuclear spins is a primary sensitivity limitation for nuclear magnetic resonance. Here we demonstrate optically pumped (microwave-free) nuclear spin polarization of $^{13}\mathrm{C}$ and $^{15}\mathrm{N}$ in $^{15}\mathrm{N}$-doped diamond. $^{15}\mathrm{N}$ polarization enhancements up to $-2000$ above thermal equilibrium are observed in the paramagnetic system $\mathrm{N_s}^{0}$. Nuclear spin polarization is shown to diffuse to bulk $^{13}\mathrm{C}$ with NMR enhancements of $-200$ at room temperature and $-500$ at $\mathrm{240~K}$, enabling a route to microwave-free high-sensitivity NMR study of biological samples in ambient conditions.

cond-mat.mes-hall↗