arXiv subjects

Wenjie Dou

Publications and source records attributed to Wenjie Dou.

At least 19 recordsLinked to original sources

arXiv2026

Phonon chirality as an additive control of CISS: a symmetry-protected law

Chirality-induced spin selectivity (CISS) is usually associated with molecular handedness. The possible contribution of chiral phonons is less established. We study a helical tight-binding model in which local phonon angular momentum modulates spin-dependent nearest-neighbor hopping. Fewest-switches surface hopping calculations give the transmitted spin polarization $\mathrm{SP}=aC+b\mathrm{PH}$. Here $C$ is the molecular chirality and $\mathrm{PH}$ is the phonon chirality. A mirror symmetry reverses $C$, $\mathrm{PH}$, and $\mathrm{SP}$ simultaneously. This symmetry excludes both a chirality-independent offset and a $C\cdot\mathrm{PH}$ term. The phonon contribution can therefore enhance, cancel, or reverse the molecular CISS signal.

physics.chem-ph↗

arXiv2026

Heterogeneous Cross-Chain Transaction Tracing for Solana Bridges via Candidate-Set Selective Decision

Solana is a rapidly growing high-throughput blockchain platform that has attracted substantial liquidity and user activity. However, this expansion has also drawn the attention of illicit actors, who frequently leverage cross-chain bridges to route illicit funds onto Solana to obfuscate transaction lineage. Unlike EVM-compatible platforms, Solana features distinct execution dynamics and lacks standard event logs, creating severe semantic gaps that prevent existing tracing methods from reliably correlating cross-ledger transactions. In this paper, we formalize four types of Solana-bound cross-chain transaction modes and propose a candidate-set selective decision-based tracing method called SolTracer. SolTracer maps disparate execution semantics into a unified event space and employs candidate-set selective decision-making to reliably associate target transactions while abstaining when valid targets are absent. Extensive experiments demonstrate that SolTracer outperforms state-of-the-art (SOTA) methods across three representative scenarios: closed-world association, open-world association, and cross-source-chain generalization. In particular, under the challenging open-world setting with a 50% TA ratio, SolTracer improves the F1 score by 20.16% over the strongest SOTA baseline. Utilizing SolTracer, we conduct an empirical analysis on real-world cross-chain transfers to investigate ecosystem dynamics. Our analysis explores the stark count-value divergence across bridge mechanisms, the prevalence of cross-asset shifts, and the decoupling between on-chain settlement and explorer visibility.

cs.CR↗

arXiv2026

Nonadiabatic Dynamics near Multiple Light-Induced Conical Intersections under Bichromatic Driving: Quantum Wave-Packet Dynamics versus Floquet Surface Hopping

Light-induced conical intersections (LICIs) create externally tunable pathways for nonadiabatic transitions, enabling active control of molecular photophysical and photochemical processes. However, both the dynamics near multiple LICIs under bichromatic driving and the applicability of our recently developed two-mode Floquet fewest switches surface hopping (two-mode F-FSSH) method to this regime remain insufficiently understood. Here, we construct a minimal three-channel Floquet Hamiltonian supporting two LICIs for Na2 interacting with a bichromatic field. We characterize its static Floquet properties and investigate the associated nonadiabatic dynamics using numerically exact quantum wave-packet dynamics and two-mode F-FSSH. We find that the second photon energy controls the relative positions of the LICIs, whereas the second-field intensity primarily redistributes and broadens the derivative-coupling landscape around the second LICI. Consequently, electronic population transfer and molecular alignment exhibit distinct and often nonmonotonic responses to these two control parameters. Two-mode F-FSSH reliably captures the principal features of the early-time dynamics and provides a semiquantitative description of the post-transient time-averaged observables. These findings advance our understanding of LICI-mediated dynamics at both the physical and methodological levels.

physics.chem-ph↗

arXiv2026

Floquet Nonadiabatic Dynamics for Light-Matter Interactions: Recent Advances and Emerging Opportunities

Light-matter interactions provide versatile routes for probing and controlling chemical reactivity, charge transport, and material properties. Time-periodic external fields can reshape electronic states and open new dynamical pathways beyond the field-free Born-Oppenheimer (BO) picture. Floquet nonadiabatic dynamics has consequently emerged as an important framework for describing coupled electron-nuclear dynamics under periodic driving. In this Perspective, we first discuss recent developments in Floquet nonadiabatic dynamics methods for closed and open quantum systems. We then highlight how this framework provides mechanistic insights into electron transfer at molecule-metal interfaces, quantum transport in molecular junctions, carrier dynamics in crystalline solids, and multicolor Floquet engineering. Finally, we outline key conceptual and computational challenges that must be addressed to transform Floquet nonadiabatic dynamics from model-based demonstrations into predictive, first-principles simulations of realistic light-driven processes.

physics.chem-ph↗

arXiv2026

A DMFT approach to evaluate electronic frictional effects near solid surfaces of strongly correlated systems

Electronic friction-Langevin dynamics (EF-LD) provides an efficient framework for capturing nonadiabatic effects at solid surfaces, with particular relevance to electrochemistry and molecular electronics. In this work, we investigate electronic friction in the two-dimensional Hubbard-Holstein model employing dynamical mean-field theory (DMFT), where the full density-matrix numerical renormalization group (FDM-NRG) serves as the impurity solver. Our results are benchmarked against mean-field theory (MFT). DMFT yields two distinct peaks in the electronic friction, arising from electron attachment/detachment resonances with the solid Fermi level, whereas MFT is unable to capture this Fermi resonance. We further examine the dynamics of electronic friction via EF-LD simulations. Our simulations uncover significant discrepancies mainly in the electronic population evolution predicted by MFT versus DMFT, indicating that MFT is inadequate for describing nonadiabatic dynamics in strongly correlated systems. Thanks to its flexibility and computational efficiency, the proposed DMFT-based approach can be readily extended to a broad range of applications.

physics.chem-ph↗

arXiv2026

Multi-mode Floquet NEGF method for driven quantum transport

We present a non-perturbative Floquet-based non-equilibrium Green's function (NEGF) method to study electron transport in a quantum system driven simultaneously by multiple independent terms (multi-mode). We first derive the two-mode Floquet NEGF based on two-step transformations of the retarded-advanced Green's function from the Kadanoff-Baym equation. This derivation proceeds by elaborating on the expectation values of the number and current operators. The two-mode Floquet NEGF is then extended to cases with multiple drivings. The method is tested by investigating current suppression in the presence of two drivings. We show that an extra sinusoidal off-diagonal driving can cause substantial modification to the current suppression, provided careful selection of the driving frequency. Consequently, we expect that the established method has broad applications in a wide range of open quantum systems driven by complicated drivings.

cond-mat.other↗

arXiv2026

Stochastic Resolution of Identity for Correlation Energy Prediction via Doubles Connected Moments Expansion

The recently developed Doubles Connected Moments (DCM) expansion offers a tractable approach for computing correlation energy, exhibiting an noniterative O(N^6) scaling with system size N. Benchmark calculations on a set of molecules demonstrate that the DCM can outperform CCSD in terms of accuracy. To further enhance its efficiency, we present a stochastic variant of DCM by introducing a stochastic resolution-of-identity (sRI) technique, which decomposes the essential four-index intermediates. The resulting sRI-DCM scheme only involves one O(N^6) step, while all other steps do not exceed O(N^4) at each recursion, and reliably reproduces the results of conventional DCM. Our sRI-DCM achieves an overall experimental scaling of O(N^{4.46}) for series hydrogen dimer chains, demonstrating that it is attractive and practical for large systems containing hundreds of electrons.

physics.chem-ph↗

arXiv2026

Accessing the performance of CC2 for excited state dynamics: a benchmark study with pyrazine

In this work, we access the performance of RI-CC2 for ultrafast internal conversion using pyrazine as a benchmark system. We implement analytical gradients and nonadiabatic coupling vectors for RI-CC2 in the Q-Chem package and employ them in two complementary approaches: a reduced-dimensionality vibronic coupling (VC) model and full-dimensional ab initio on-the-fly trajectory surface hopping simulations. To accelerate the on-the-fly dynamics, we employ a diabatic artificial neural network model trained on RI-CC2 data. Both the VC model and the full-dimensional dynamics reveal that the dark $A_\text{1u}$ state actively participates in the internal conversion process. RI-CC2 identifies the $Q_\text{9a}$ and $Q_\text{8a}$ vibrational modes as key drivers of the coherent population transfer between the $A_\text{1u}$ and $B_\text{3u}$. The on-the-fly dynamics reproduce the experimental $B_\text{2u}$ population decay time of 26 fs, consistent with the measured value of $22\pm3$ fs. The high-quality dataset of energies, forces, and nonadiabatic couplings generated here provides a valuable resource for future machine-learning developments, while the stochastic variant sRI-CC2 promises to extend such dynamics to larger molecular systems.

physics.chem-ph↗

arXiv2026

Generalized quantum master equation from memory kernel coupling theory

The generalized quantum master equation provides a powerful framework for non-Markovian dynamics of open quantum systems. However, the accurate and efficient evaluation of the memory kernel remains a challenge. In this work, we introduce a comprehensive tensorial extension to the Memory Kernel Coupling Theory (MKCT) to overcome this bottleneck. By elevating the original scalar formalism to a tensorial framework, the extended MKCT enables the calculation of general expectation values and cross-correlation functions. We demonstrate the numerical accuracy and efficiency of this method across multiple benchmark systems: capturing transient populations and coherences in the spin-boson model, resolving the excitonic absorption spectrum of the Fenna-Matthews-Olson complex, and simulating charge mobility in one-dimensional lattice models. These successful applications establish the tensorial MKCT as a highly efficient tool for investigating complex dynamics in open quantum systems.

physics.chem-ph↗

arXiv2026

Projection-Based Memory Kernel Coupling Theory for Quantum Dynamics: A Stable Framework for Non-Markovian Simulations

We present a projection-based, stability-preserving methodology for computing time correlation functions in open quantum systems governed by generalized quantum master equations with non-Markovian effects. Building upon the memory kernel coupling theory framework, our approach transforms the memory kernel hierarchy into a system of coupled linear differential equations through Mori-Zwanzig projection, followed by spectral projection onto stable eigenmodes to ensure numerical stability. By systematically eliminating unstable modes while preserving the physically relevant dynamics, our method guaranties long-time convergence without introducing artificial damping or ad hoc modifications. The theoretical framework maintains mathematical rigor through orthogonal projection operators and spectral decomposition. Benchmark calculations on the spin-boson model show excellent agreement with exact hierarchical equations of motion results while achieving significant computational efficiency. This approach provides a versatile and reliable framework for simulating non-Markovian dynamics in complex systems.

quant-ph↗

arXiv2026

Tunable spin-phonon polarons in a chiral molecular qubit framework

Chiral structures that produce asymmetric spin-phonon coupling can theoretically generate spin-phonon polarons -- quasiparticles exhibiting non-degenerate spin states with phonon displacements. These quasiparticles are speculated to be the origin of chirality-induced spin selectivity and presumably can display exotic dynamic behaviors. However, direct experimental evidence of spin-phonon polarons has been lacking. Using a chiral molecular qubit framework embedding stable semiquinone-like radicals, we report spin dynamic signatures that indicate the formation of spin-phonon polarons for the first time. Our non-adiabatic model reveals that these quasiparticles introduce an active spin relaxation channel when polaron reorganization energy approaches Zeeman splitting. This new channel manifests itself as anomalous, temperature-independent spin relaxation, which can be suppressed by high magnetic fields or pore-filling solvents (e.g. CH2Cl2, CS2). Such field- and guest-tunable relaxation is unattainable in conventional spin systems. Harnessing this mechanism could boost repetition rates in spin-based quantum information technologies without compromising coherence or quantum sensing performance.

cond-mat.mes-hall↗

arXiv2026

Two-Mode Floquet Fewest Switches Surface Hopping for Nonadiabatic Dynamics Driven by Two-Frequency Laser Fields

Two-frequency (two-color) laser fields provide a powerful and flexible means for steering molecular dynamics. However, quantitatively reliable and scalable theoretical tools for simulating laser-driven nonadiabatic processes under such fields remain limited. Here, we develop a two-mode Floquet fewest switches surface hopping (two-mode F-FSSH) approach for two-frequency driving within a mixed quantum-classical framework. We validate the algorithm on three driven one-dimensional two-state models: a Rabi model and two avoided-crossing scattering models. The electronic and nuclear dynamics are benchmarked against numerically exact results from split-operator calculations, showing good agreement across a broad range of field parameters and initial conditions. These results establish two-mode F-FSSH as a practical framework for simulating and designing two-frequency control protocols and motivate extensions to more realistic experimental settings.

physics.chem-ph↗

arXiv2026

Implicitly Restarted Lanczos Enables Chemically-Accurate Shallow Neural Quantum States

The variational optimization of high-dimensional neural network models, such as those used in neural quantum states (NQS), presents a significant challenge in machine intelligence. Conventional first-order stochastic methods (e.g., Adam) are plagued by slow convergence, sensitivity to hyperparameters, and numerical instability, preventing NQS from reaching the high accuracy required for fundamental science. We address this fundamental optimization bottleneck by introducing the implicitly restarted Lanczos (IRL) method as the core engine for NQS training. Our key innovation is an inherently stable second-order optimization framework that recasts the ill-conditioned parameter update problem into a small, well-posed Hermitian eigenvalue problem. By solving this problem efficiently and robustly with IRL, our approach automatically determines the optimal descent direction and step size, circumventing the need for demanding hyperparameter tuning and eliminating the numerical instabilities common in standard iterative solvers. We demonstrate that IRL enables shallow NQS architectures (with orders of magnitude fewer parameters) to consistently achieve extreme precision (1e-12 kcal/mol) in just 3 to 5 optimization steps. For the F2 molecule, this translates to an approximate 17,900-fold speed-up in total runtime compared to Adam. This work establishes IRL as a superior, robust, and efficient second-order optimization strategy for variational quantum models, paving the way for the practical, high-fidelity application of neural networks in quantum physics and chemistry.

quant-ph↗

arXiv2025

Orbital Surface Hopping with an Electron Thermostat Yields Accurate Dynamics and Detailed Balance

In mixed quantum-classical simulations of molecule-metal surface interactions, the discretization of the metallic electronic continuum typically results in a closed-system representation that fails to capture the open-system nature of the true physical process. This approximation can introduce significant artifacts, including deviations in the dynamical evolution and a violation of the principle of detailed balance. To address this fundamental challenge, we introduce an electronic thermostat into our previously developed orbital surface hopping (OSH) framework, generalizing the method to efficiently handle many discrete electronic states. We first outline the derivation of electronic thermostat orbital surface hopping, where the amplitude of the electronic thermostat is well justified. We then demonstrate that this method can reproduce accurate dynamics and detailed balance in long time, whereas without electronic thermostat the detailed balance is violated. Thus, this method offers a reliable tool for studying nonadiabatic dynamics near metal surfaces.

physics.chem-ph↗

arXiv2025

Two-mode Floquet Redfield quantum master approach for quantum transport

Simultaneous driving by two periodic oscillations yields a practical technique for further engineering quantum systems. For quantum transport through mesoscopic systems driven by two strong periodic terms, a non-perturbative Floquet-based quantum master equation (QME) approach is developed using a set of dissipative time-dependent terms and the reduced density matrix of the system. This work extends our previous Floquet approach for transport through quantum dots (at finite temperature and arbitrary bias) driven periodically by a single frequency. In a pedagogical way, we derive explicit time-dependent dissipative terms. Our theory begins with the derivation of the two-mode Floquet Liouville-von Neumann equation. We then explain the second-order Wangsness-Bloch-Redfield QME with a slightly modified definition of the interaction picture. Subsequently, the two-mode Shirley time evolution formula is applied, allowing for the integration of reservoir dynamics. Consequently, the established formalism has a wide range of applications in open quantum systems driven by two modes in the weak coupling regime. The formalism's potential applications are demonstrated through various examples.

cond-mat.mes-hall↗

arXiv2025

Noise-reduced stochastic resolution of identity to CC2 for large-scale calculations via tensor hypercontraction

The stochastic resolution of identity (sRI) approximation significantly reduces the computational scaling of CC2 from O(N^5) to O(N^3), where N is a measure of system size. However, the inherent stochastic noise, while controllable, can introduce substantial errors in energy derivatives, limiting its reliability for molecular dynamics simulations. To mitigate this limitation, we introduce a noise-reduced approach, termed THC-sRI-CC2, which synergistically combines the sRI framework with tensor hypercontraction (THC). In this formulation, the expensive Coulomb term, which scales as O(N^4), is decoupled via THC, while the time-determining exchange term with an O(N^5) cost is addressed through the sRI scheme, collectively yielding an overall O(N^3) scaling. Benchmarks demonstrate that our THC-sRI-CC2 implementation achieves greater accuracy and markedly reduced stochastic noise compared to conventional sRI-CC2 with identical computational samplings. The resulting O(N^3) scaling substantially extends the applicability of CC2 for excited-state energy calculations and nonadiabatic dynamics simulations of large molecular systems. Furthermore, this work establishes a general THC-sRI hybrid strategy for the development of reduced-scaling electronic structure methods.

physics.chem-ph↗

arXiv2025

From higher-order moments to time correlation functions in strongly correlated systems: A DMRG-based memory kernel coupling theory

We introduce a hybrid approach for computing dynamical observables in strongly correlated systems using higher-order moments. This method integrates memory kernel coupling theory (MKCT) with the density matrix renormalization group (DMRG), extending our recent work on MKCT to strongly correlated systems. The method establishes that correlation functions can be derived from the moments. Within our framework, operators and wavefunctions are represented as matrix product operators (MPOs) and matrix product states (MPSs), respectively. Crucially, the repeated application of the Liouville operator is achieved through an iterative procedure analogous to the DMRG algorithm itself. We demonstrate the effectiveness and efficiency of MKCT-DMRG by computing the spectral function of the Hubbard model. Furthermore, we successfully apply the method to compute the electronic friction in the Hubbard-Holstein model. In all cases, the results show excellent agreement with time-dependent DMRG (TD-DMRG) benchmarks. The advantage of MKCT-DMRG over TD-DMRG is the computational efficiency, which avoids expensive real-time propagation in TD-DMRG. These findings establish MKCT-DMRG as a promising and accurate framework for simulating challenging dynamical properties in strongly correlated quantum systems.

physics.comp-ph↗

arXiv2025

Mixed Quantum-Classical Approaches to Spin Current and Polarization Dynamics in Chiral Molecular Junctions

Chiral molecular junctions offer a promising platform for realizing chiral-induced spin selectivity (CISS), where spin filtering occurs without external magnetic fields. Here, we investigate spin transport in such junctions by combining quantum master equation (QME) methods for purely electronic dynamics with surface hopping (SH) and mean-field Ehrenfest (MF) approaches to incorporate electron-phonon coupling. Our results show that transient spin polarization arises but ultimately decays to zero at long times. We find that bias voltage, molecular length, and spin-orbit coupling (SOC) strongly influence the spin current dynamics: higher bias enhances spin current but reduces polarization, while longer molecules and stronger SOC amplify transient polarization. Including electron-phonon coupling modifies current-voltage characteristics, enhancing spin currents at intermediate bias but suppressing them at high bias, while leaving the polarization dynamics largely unchanged. These findings highlight the interplay between electronic and vibrational effects in CISS and provide guidance for designing molecular spintronic devices.

cond-mat.mes-hall↗