arXiv subjects

Xiao-Guang Zhang

Publications and source records attributed to Xiao-Guang Zhang.

17 recordsLinked to original sources

arXiv2026

Using near-flat-band electrons for read-out of molecular spin qubit entangled states

While molecular spin qubits (MSQs) are a promising platform for quantum computing, read-out has been largely limited to electron paramagnetic resonance which is often slow and requires a global system drive. Moreover, because one prerequisite for the Elzerman and Pauli spin blockade readout mechanisms typical of semiconductor spin qubits is tunneling of electrons between sites, these read-out modalities are unavailable in MSQs. Here, we theoretically demonstrate electrical read-out of entangled MSQs via driven many-electron spin unpolarized currents. In particular, using a time-dependent density matrix renormalization group approach we simulate a maximally entangled MSQ pair between two electronic leads. Driving itinerant electrons between the two leads, we find that the conductance is greater when the MSQs are in the entangled singlet state as compared to the entangled triplet state. This contrast in conductance is enhanced when the electronic density of states at the Fermi energy is large and for narrow bandwidth. Our results are readily applicable to molecules supramolecularly functionalizing semiconductors with relatively flat bands such as single-wall carbon nanotubes under a magnetic field.

cond-mat.mes-hall↗

arXiv2025

Discovery of Spin-Crossover Candidates with Equivariant Graph Neural Networks and Relevance-Based Classification

Swift discovery of spin-crossover materials for their potential application in quantum information devices requires techniques which enable efficient identification of suitably bistable candidates. To this end, we screened the Cambridge Structural Database to develop a specialized database of 1,439 materials and computed spin-switching energies from density functional theory for each material. The database was used to train an equivariant graph convolutional neural network to predict the magnitude of the spin-conversion energy. A test mean absolute error was 360 meV. For candidate identification, we equipped the system with a relevance-based classifier. This approach leads to a nearly four-fold improvement in identifying potential spin-crossover systems of interest as compared to conventional high-throughput screening.

cond-mat.dis-nn↗

arXiv2023

Mapping Spin Interactions from Conductance Peak Splitting in Coulomb Blockade

We investigate the transport properties of a quantum dot coupled to leads interacting with a multi-spin system using the generalized master equation within the Coulomb blockade regime. We find that if two states for each scattering region electron manifold are included, several signatures of the interacting spin system appear in steady-state transport properties. We provide a theoretical mapping of differential conductance peak signatures and all spin Hamiltonian parameters related to the inclusion of excited state transitions between uncharged and charged electron manifolds. Our predictions describe a scheme of only using a quantum dot and differential conductance to measure magnetic anisotropy, inter-spin exchange coupling, exchange coupling between the spin system and itinerant electron, and applied magnetic field response.

cond-mat.mes-hall↗

arXiv2022

Demonstration of electron-nuclear decoupling at a spin clock transition

The ability to design quantum systems that decouple from environmental noise sources is highly desirable for development of quantum technologies with optimal coherence. The chemical tunability of electronic states in magnetic molecules combined with advanced electron spin resonance techniques provides excellent opportunities to address this problem. Indeed, so-called clock transitions (CTs) have been shown to protect molecular spin qubits from magnetic noise, giving rise to significantly enhanced coherence. Here we conduct a spectroscopic and computational investigation of this physics, focusing on the role of the nuclear bath. Away from the CT, linear coupling to the nuclear degrees of freedom causes a modulation and decay of electronic coherence, as quantified via electron spin echo signals generated experimentally and $\textit{in silico}$. Meanwhile, the effective hyperfine interaction vanishes at the CT, resulting in electron-nuclear decoupling and an absence of quantum information leakage to the nuclear bath, providing opportunities to characterize other decoherence sources.

quant-ph↗

arXiv2022

Scattering solution of interacting Hamiltonian for electronic control of molecular spin qubits

We theoretically study how a scattered electron can entangle molecular spin qubits (MSQs). This requires solving the inelastic transport of a single electron through a scattering region described by a tight-binding interacting Hamiltonian. We accomplish this using a Green's function solution. We can model realistic physical implementations of MSQs by parameterizing the tight-binding Hamiltonian with first-principles descriptions of magnetic anisotropy and exchange interactions. We find that for two-MSQ systems with inversion symmetry, the spin degree of freedom of the scattered electron offers probabilistic control of the degree of entanglement between the MSQs.

quant-ph↗

arXiv2022

Electronic control and switching of entangled spin state using anisotropy and exchange in the three-particle paradigm

We explore the control and switching of the entangled spin states of multi-spin particle qubit coupled to an electron using a three-particle spin model described by $S_i$ ($i=1,2,3$), in which $S_1=\tfrac{1}{2}$ is an electron and $S_{2,3}$ can have any spin with both exchange coupling and magnetic anisotropy. We derive a general formula for the existence of a switching (DJ) resonance for any spin $S_{2,3}$. We further contrast the entanglement switching mechanisms for the $S_{2,3}=\tfrac{1}{2}$ and $S_{2,3}=1$ spin models. We find that while the onsite magnetic anisotropy in the case of $S_{2,3}>\tfrac{1}{2}$ allows full control of their spin states via interaction with $S_1$, in order to achieve acceptable control of a Bloch vector within the $S_{2,3}=\tfrac{1}{2}$ model, additional mechanisms, such as anisotropic exchange coupling, are required.

quant-ph↗

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↗

arXiv2021

Majorana Zero Modes Emulated in a Magnetic Molecule Chain

We propose molecular magnets as a platform to emulate Majorana zero modes (MZMs). Using a quantum chemistry approach, we identify several candidates and predict a Co trimer to have sufficient properties to host MZMs. Parameters of the quantum spin Hamiltonian describing the three coupled magnetic centers are extracted from ab initio calculations. The low-energy subspace of this material realizes an effective anisotropic spin-1/2 chain. We show the presence of MZMs in this system and find that their response to electronic paramagnetic resonance provides an experimentally realizable signature.

cond-mat.mes-hall↗

arXiv2021

Anisotropy-Exchange Resonance as a Mechanism for Entangled State Switching

We explore the three-particle spin model of an $S_{1}=\frac{1}{2}$ particle (e.g. a stationary electron) interacting with two spin-coupled $S_{\text{2,3}}$ particles with exchange coupling and magnetic anisotropy. We find that in the case of $S_{2,3}=1$ particles, the coupled particle entanglement states can be prepared, controlled, and read by the $S_{1}$ particle. We also find that for particular resonance conditions of the magnetic anisotropy strength $D$ and exchange coupling strength $J$, the entanglement state switching behavior is maximized and is robust against a range of anisotropic application of the exchange coupling.

quant-ph↗

arXiv2021

First-Principles Theory for Schottky Barrier Physics

We develop a first-principles theory for Schottky barrier physics. The Poisson equation is solved completely self-consistently with the electrostatic charge density and outside the normal density functional theory (DFT) electronic structure iteration loop, allowing computation of a Schottky barrier entirely from DFT involving thousands of atomic layers in the semiconductor. The induced charge in the bulk consists of conduction and valence band charges from doping and band bending, as well as charge from the evanescent states in the gap of the semiconductor. The Schottky barrier height is determined when the induced charge density and the induced electrostatic potential reach self-consistency.

cond-mat.mtrl-sci↗

arXiv2020

Long-Range Magnetic Exchange Pathways in Complex Clusters from First-Principles

This work builds a bridge between density functional theory (DFT) and model interpretations of Anderson's superexchange theory by constructing a $f$-$d$-$p$ model with DFT Wannier functions to enable a direct quantum many-body solution within an embedding approach. When applied to long-range magnetic interactions in a Mn-Ce magnetic molecule, we are able to obtain numerical insights about double exchange and superexchange interactions. Direct metal-metal charge transfer processes are generally weak in this molecule, which leads to small contributions from double exchange interactions. For long-range interactions, Mn-Ce charge transfer is not significant compared to Ce-O charge transfer. The unusual superexchange between Mn atoms with different valence states is identified as the dominant mechanism. This procedure opens a path for quantitative understanding of different exchange interactions in complex magnetic systems, including molecular magnets, transition metal organic frameworks, and other solid materials.

cond-mat.mtrl-sci↗

arXiv2020

Three Jahn-Teller states of matter in the spin-crossover system Mn(taa)

Three high-spin phases recently discovered in the spin-crossover system Mn(taa) are identified through analysis by a combination of first-principles calculations and Monte Carlo simulation as a low-temperature Jahn-Teller ordered (solid) phase, an intermediate-temperature dynamically correlated (liquid) phase, and an uncorrelated (gas) phase. In particular, the Jahn-Teller liquid phase arises from competition between mixing with low-spin impurities, which drive the disorder, and inter-molecular strain interactions. The latter are a key factor in both the spin-crossover phase transition and the magnetoelectric coupling. Jahn-Teller liquids may exist in other spin-crossover materials and materials that have multiple equivalent Jahn-Teller axes.

cond-mat.mtrl-sci↗

arXiv2019

Decoherence in Molecular Electron Spin Qubits: Insights from Quantum Many-Body Simulations

Quantum states are described by wave functions whose phases cannot be directly measured, but which play a vital role in quantum effects such as interference and entanglement. The loss of the relative phase information, termed decoherence, arises from the interactions between a quantum system and its environment. Decoherence is perhaps the biggest obstacle on the path to reliable quantum computing. Here we show that decoherence occurs even in an isolated molecule although not all phase information is lost via a theoretical study of a central electron spin qubit interacting with nearby nuclear spins in prototypical magnetic molecules. The residual coherence, which is molecule-dependent, provides a microscopic rationalization for the nuclear spin diffusion barrier proposed to explain experiments. The contribution of nearby molecules to the decoherence has a non-trivial dependence on separation, peaking at intermediate distances. Molecules that are far away only affect the long-time behavior. Because the residual coherence is simple to calculate and correlates well with the coherence time, it can be used as a descriptor for coherence in magnetic molecules. This work will help establish design principles for enhancing coherence in molecular spin qubits and serve to motivate further theoretical work.

physics.chem-ph↗

arXiv2019

Formation energies of charged defects in two-dimensional materials -- resolution of long-standing difficulties

Formation energies of charged point defects in semiconductors are calculated using periodic supercells, which entail a divergence arising from long-range Coulombic interactions. The divergence is typically removed by the so-called jellium approach. Recently, Wu, Zhang and Pantelides [WZP, Phys. Rev. Lett. 119, 105501 (2017)] traced the origin of the divergence to the assumption that charged defects are formed by physically removing electrons from or adding electrons to the crystal, violating charge neutrality, a key principle of statistical mechanics that determines the Fermi level. An alternative theory was constructed by recognizing that "charged" defects form by trading carriers with the energy bands, whereby supercells are always charge-neutral so that no divergence is present and no ad-hoc procedures need to be adopted for calculations. Here we give a more detailed exposition of the foundations of both methods and show that the jellium approach can be derived from the statistical-mechanics-backed WZP definition by steps whose validity cannot be assessed a priori. In particular, the divergence appears when the charge density of band carriers is dropped, leaving a supercharged crystal. In the case of charged defects in two-dimensional (2D) materials, unphysical fields appear in vacuum regions. None of these pathological features are present in the reformulated theory. Finally, we report new calculations in both bulk and 2D materials. The WZP approach yields formation energies that differ from jellium values by up to ~1 eV. By analyzing the spatial distribution of wave functions and defect potentials, we provide insights into the inner workings of both methods and demonstrate that the failure of the jellium approach to include the neutralizing electron density of band carriers, as is the case in the physical system, is responsible for the numerical differences between the two methods.

cond-mat.mtrl-sci↗

arXiv2016

Fully integrated 3.2 Gbps quantum random number generator with real-time extraction

We present a real-time and fully integrated quantum random number generator (QRNG) by measuring laser phase fluctuations. The QRNG scheme based on laser phase fluctuations is featured for its capability of generating ultra high-speed random numbers. However, the speed bottleneck of a practical QRNG lies on the limited speed of randomness extraction. To close the gap between the fast randomness generation and the slow post-processing, we propose a pipeline extraction algorithm based on Toeplitz matrix hashing and implement it in a high-speed field-programmable gate array. Further, all the QRNG components are integrated into a module, including a compact and actively stabilized interferometer, high-speed data acquisition, and real-time data post-processing and transmission. The final generation rate of the QRNG module with real-time extraction can reach 3.2 Gbps.

quant-ph↗

arXiv2013

Influence of Reciprocal links in Social Networks

In this Letter, we empirically study the influence of reciprocal links, in order to understand its role in affecting the structure and function of directed social networks. Experimental results on two representative datesets, Sina Weibo and Douban, demonstrate that the reciprocal links indeed play a more important role than non-reciprocal ones in both spreading information and maintaining the network robustness. In particular, the information spreading process can be significantly enhanced by considering the reciprocal effect. In addition, reciprocal links are largely responsible for the connectivity and efficiency of directed networks. This work may shed some light on the in-depth understanding and application of the reciprocal effect in directed online social networks.

physics.soc-ph↗

arXiv2012

Molecular Magnetocapacitance

Capacitance of a nanoscale system is usually thought of having two contributions, a classical electrostatic contribution and a quantum contribution dependent on the density of states and/or molecular orbitals close to the Fermi energy. In this letter we demonstrate that in molecular nano-magnets and other magnetic nanoscale systems, the quantum part of the capacitance becomes spin-dependent, and is tunable by an external magnetic field. This molecular magnetocapacitance can be realized using single molecule nano-magnets and/or other nano-structures that have antiferromagnetic ground states. As a proof of principle, first-principles calculation of the nano-magnet [Mn3O(sao)3(O2CMe)(H2O)(py)3] shows that the charging energy of the high-spin state is 260 meV lower than that of the low-spin state, yielding a 6% difference in capacitance. A magnetic field of ~40T can switch the spin state, thus changing the molecular capacitance. A smaller switching field may be achieved using nanostructures whose physical properties such as magnetic moment are size-dependent. Molecular magnetocapacitance may lead to revolutionary device designs, e.g., by exploiting the Coulomb blockade magnetoresistance whereby a small change in capacitance can lead to a huge change in resistance.

cond-mat.mes-hall↗