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Researcher profile

Yang Li

Yang Li contributes to research discovery and scholarly infrastructure.

ResearcherAffiliation not importedOpen to collaborate
Artificial IntelligenceComputation and LanguageComputer VisionRoboticsMachine Learningphysics.chem-phcond-mat.mtrl-sciphysics.atom-phquant-phcond-mat.mes-hallcond-mat.str-elcond-mat.supr-conInformation Theorymath.ITmath.OCphysics.comp-phphysics.plasm-ph

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Published work

21 published item(s)

preprint2026arXiv

AT$^2$PO: Agentic Turn-based Policy Optimization via Tree Search

LLM agents have emerged as powerful systems for tackling multi-turn tasks by interleaving internal reasoning and external tool interactions. Agentic Reinforcement Learning has recently drawn significant research attention as a critical post-training paradigm to further refine these capabilities. In this paper, we present AT$^2$PO (Agentic Turn-based Policy Optimization via Tree Search), a unified framework for multi-turn agentic RL that addresses three core challenges: limited exploration diversity, sparse credit assignment, and misaligned policy optimization. AT$^2$PO introduces a turn-level tree structure that jointly enables Entropy-Guided Tree Expansion for strategic exploration and Turn-wise Credit Assignment for fine-grained reward propagation from sparse outcomes. Complementing this, we propose Agentic Turn-based Policy Optimization, a turn-level learning objective that aligns policy updates with the natural decision granularity of agentic interactions. ATPO is orthogonal to tree search and can be readily integrated into any multi-turn RL pipeline. Experiments across seven benchmarks demonstrate consistent improvements over the state-of-the-art baseline by up to 1.84 percentage points in average, with ablation studies validating the effectiveness of each component. Our code is available at https://github.com/zzfoutofspace/ATPO.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Beyond Mode Collapse: Distribution Matching for Diverse Reasoning

On-policy reinforcement learning methods like GRPO suffer from mode collapse: they exhibit reduced solution diversity, concentrating probability mass on a single solution once discovered and ceasing exploration of alternative strategies. We show this stems from reverse KL minimization's mode-seeking behavior, which reinforces the first high-reward trajectory found rather than maintaining a distribution over multiple diverse solutions. We propose DMPO (Distribution-Matching Policy Optimization), which prevents mode collapse through principled approximation of forward KL minimization. DMPO constructs a group level target distribution over sampled trajectories proportional to their rewards, then aligns the policy distribution to this target. This provides mode-covering behavior without requiring sampling from the intractable global target distribution, enabling sustained exploration throughout training. We validate DMPO on NP-hard combinatorial optimization, where exponentially many feasible solutions exist but only a few approach optimality, an ideal testbed for evaluating exploration. DMPO achieves 43.9% Quality Ratio on text-based NP-Bench (vs. GRPO's 40.1%) and 43.1% on vision-based NP-Bench (vs. 38.4%), demonstrating 9% and 12% relative improvements respectively. These gains generalize to mathematical reasoning (+2.0%) and out-of-domain tasks (+2.3%), showing that diversity-preserving training enhances general reasoning capabilities across modalities. Our work establishes distribution matching as a practical, principled approach to preventing mode collapse in on-policy RL, with consistent quality improvements demonstrating sustained exploration across diverse reasoning tasks.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Chain-of-Action: Trajectory Autoregressive Modeling for Robotic Manipulation

We present Chain-of-Action (CoA), a novel visuo-motor policy paradigm built upon Trajectory Autoregressive Modeling. Unlike conventional approaches that predict next step action(s) forward, CoA generates an entire trajectory by explicit backward reasoning with task-specific goals through an action-level Chain-of-Thought (CoT) process. This process is unified within a single autoregressive structure: (1) the first token corresponds to a stable keyframe action that encodes the task-specific goals; and (2) subsequent action tokens are generated autoregressively, conditioned on the initial keyframe and previously predicted actions. This backward action reasoning enforces a global-to-local structure, allowing each local action to be tightly constrained by the final goal. To further realize the action reasoning structure, CoA incorporates four complementary designs: continuous action token representation; dynamic stopping for variable-length trajectory generation; reverse temporal ensemble; and multi-token prediction to balance action chunk modeling with global structure. As a result, CoA gives strong spatial generalization capabilities while preserving the flexibility and simplicity of a visuo-motor policy. Empirically, we observe CoA achieves the state-of-the-art performance across 60 RLBench tasks and 8 real-world manipulation tasks.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Closing the Reality Gap: Zero-Shot Sim-to-Real Deployment for Dexterous Force-Based Grasping and Manipulation

Human-like dexterous hands with multiple fingers offer human-level manipulation capabilities, but training control policies that can directly deploy on real hardware remains difficult due to contact-rich physics and imperfect actuation. We close this gap with a practical sim-to-real reinforcement learning (RL) framework that utilizes dense tactile feedback combined with joint torque sensing to explicitly regulate physical interactions. To enable effective sim-to-real transfer, we introduce (i) a computationally fast tactile simulation that computes distances between dense virtual tactile units and the object via parallel forward kinematics, providing high-rate, high-resolution touch signals needed by RL; (ii) a current-to-torque calibration that eliminates the need for torque sensors on dexterous hands by mapping motor current to joint torque; and (iii) actuator dynamics modeling to bridge the actuation gaps with randomization of non-ideal effects such as backlash, torque-speed saturation. Using an asymmetric actor-critic PPO pipeline trained entirely in simulation, our policies deploy directly to a five-finger hand. The resulting policies demonstrated two essential skills: (1) command-based, controllable grasp force tracking, and (2) reorientation of objects in the hand, both of which were robustly executed without fine-tuning on the robot. By combining tactile and torque in the observation space with effective sensing/actuation modeling, our system provides a practical solution to achieve reliable dexterous manipulation. To our knowledge, this is the first demonstration of controllable grasping on a multi-finger dexterous hand trained entirely in simulation and transferred zero-shot on real hardware.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Decide Then Retrieve: A Training-Free Framework with Uncertainty-Guided Triggering and Dual-Path Retrieval

Retrieval-augmented generation (RAG) enhances large language models (LLMs) by incorporating external knowledge, but existing approaches indiscriminately trigger retrieval and rely on single-path evidence construction, often introducing noise and limiting performance gains. In this work, we propose Decide Then Retrieve (DTR), a training-free framework that adaptively determines when retrieval is necessary and how external information should be selected. DTR leverages generation uncertainty to guide retrieval triggering and introduces a dual-path retrieval mechanism with adaptive information selection to better handle sparse and ambiguous queries. Extensive experiments across five open-domain QA benchmarks, multiple model scales, and different retrievers demonstrate that DTR consistently improves EM and F1 over standard RAG and strong retrieval-enhanced baselines, while reducing unnecessary retrievals. The code and data used in this paper are available at https://github.com/ChenWangHKU/DTR.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Decoupled interband pairing in a bilayer iron-based superconductor evidenced by ultrahigh-resolution ARPES

We present direct experimental evidence of a weakly coupled multiband superconducting state in the bilayer iron-based superconductor ACa$_2$Fe$_4$As$_4$F$_2$ (A = K, Cs) via ultrahigh-resolution angle-resolved photoemission spectroscopy (ARPES). Remarkably, the K-containing compound exhibits two distinct transition temperatures, corresponding to two separate sets of bilayer-split bands, as evidenced by temperature-dependent superconducting gap and spectral weight near the Fermi energy, while its Cs counterpart displays conventional single transition behavior. These experimental observations are well described by the weakly coupled two-band model of Eilenberger theory, which identifies suppressed interband pairing interactions between the bilayer-split bands as the key mechanism. By exploring quantum phenomena in the weak-coupling limit within a multiband system, our findings pave the way for engineering exotic superconductivity via band-selective pairing control.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

DeepH-pack: A general-purpose neural network package for deep-learning electronic structure calculations

In computational physics and materials science, first-principles methods, particularly density functional theory, have become central tools for electronic structure prediction and materials design. Recently, rapid advances in artificial intelligence (AI) have begun to reshape the research landscape, giving rise to the emerging field of deep-learning electronic structure calculations. Despite numerous pioneering studies, the field remains in its early stages; existing software implementations are often fragmented, lacking unified frameworks and standardized interfaces required for broad community adoption. Here we present DeepH-pack, a comprehensive and unified software package that integrates first-principles calculations with deep learning. By incorporating fundamental physical principles into neural-network design, such as the nearsightedness principle and the equivariance principle, DeepH-pack achieves robust cross-scale and cross-material generalizability. This allows models trained on small-scale structures to generalize to large-scale and previously unseen materials. The toolkit preserves first-principles accuracy while accelerating electronic structure calculations by several orders of magnitude, establishing an efficient and intelligent computational paradigm for large-scale materials simulation, high-throughput materials database construction, and AI-driven materials discovery.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

DemoBot: Efficient Learning of Bimanual Manipulation with Dexterous Hands From Third-Person Human Videos

This work presents DemoBot, a learning framework that enables a dual-arm, multi-finger robotic system to acquire complex manipulation skills from a single unannotated RGB-D video demonstration. The method extracts structured motion trajectories of both hands and objects from raw video data. These trajectories serve as motion priors for a novel reinforcement learning (RL) pipeline that learns to refine them through contact-rich interactions, thereby eliminating the need to learn from scratch. To address the challenge of learning long-horizon manipulation skills, we introduce: (1) Temporal-segment based RL to enforce temporal alignment of the current state with demonstrations; (2) Success-Gated Reset strategy to balance the refinement of readily acquired skills and the exploration of subsequent task stages; and (3) Event-Driven Reward curriculum with adaptive thresholding to guide the RL learning of high-precision manipulation. The novel video processing and RL framework successfully achieved long-horizon synchronous and asynchronous bimanual assembly tasks, offering a scalable approach for direct skill acquisition from human videos.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

DIP: Dynamic In-Context Planner For Diffusion Language Models

Diffusion language models (DLMs) have shown strong potential for general natural language tasks with in-context examples. However, due to the bidirectional attention mechanism, DLMs incur substantial computational cost as context length increases. This work addresses this issue with a key discovery: unlike the sequential generation in autoregressive language models (ARLMs), the diffusion generation paradigm in DLMs allows \textit{efficient dynamic adjustment of the context} during generation. Building on this insight, we propose \textbf{D}ynamic \textbf{I}n-Context \textbf{P}lanner (DIP), a context-optimization method that dynamically selects and inserts in-context examples during generation, rather than providing all examples in the prompt upfront. Results show DIP maintains generation quality while achieving up to 12.9$\times$ inference speedup over standard inference and 1.17$\times$ over KV cache-enhanced inference.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Enhancing Rare Codes via Probability-Biased Directed Graph Attention for Long-Tail ICD Coding

Automated international classification of diseases (ICD) coding aims to assign multiple disease codes to clinical documents and plays a critical role in healthcare informatics. However, its performance is hindered by the extreme long-tail distribution of the ICD ontology, where a few common codes dominate while thousands of rare codes have very few examples. To address this issue, we propose a Probability-Biased Directed Graph Attention model (ProBias) that partitions codes into common and rare sets and allows information to flow only from common to rare codes. Edge weights are determined by conditional co-occurrence probabilities, which guide the attention mechanism to enrich rare-code representations with clinically related signals. To provide higher-quality semantic representations as model inputs, we further employ large language models to generate enriched textual descriptions for ICD codes, offering external clinical context that complements statistical co-occurrence signals. Applied to automated ICD coding, our approach significantly improves the representation and prediction of rare codes, achieving state-of-the-art performance on three benchmark datasets. In particular, we observe substantial gains in macro-averaged F1 score, a key metric for long-tail classification.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Exploiting Task Relationships in Continual Learning via Transferability-Aware Task Embeddings

Continual learning (CL) has been a critical topic in contemporary deep neural network applications, where higher levels of both forward and backward transfer are desirable for an effective CL performance. Existing CL strategies primarily focus on task models, either by regularizing model updates or by separating task-specific and shared components, while often overlooking the potential of leveraging inter-task relationships to enhance transfer. To address this gap, we propose a transferability-aware task embedding, termed H-embedding, and construct a hypernet framework under its guidance to learn task-conditioned model weights for CL tasks. Specifically, H-embedding is derived from an information theoretic measure of transferability and is designed to be online and easy to compute. Our method is also characterized by notable practicality, requiring only the storage of a low-dimensional task embedding per task and supporting efficient end-to-end training. Extensive evaluations on benchmarks including CIFAR-100, ImageNet-R, and DomainNet show that our framework performs prominently compared to various baseline and SOTA approaches, demonstrating strong potential in capturing and utilizing intrinsic task relationships. Our code is publicly available at https://github.com/viki760/Hembedding_Guided_Hypernet.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Stabilizing, Scaling & Enhancing MeanFlow for Large-scale Diffusion Distillation

Diffusion models exhibit remarkable generative capability, but their high latency limits practical deployment. Many studies have attempted to reduce sampling steps to accelerate inference. Among them, MeanFlow has attracted considerable attention due to its concise formulation and remarkable performance. Nevertheless, the instability of its optimization objective and the ''mean-seeking bias'' have limited its applicability to distill large-scale industrial models. To stabilize MeanFlow for distilling large-scale models, we first introduce a warm-up technique, in which the original differential solution of MeanFlow is replaced by a discrete solution. This design avoids training collapse caused by the MeanFlow target containing a stop-gradient term from an undertrained model. Once the model acquires a preliminary ability to fit the average velocity field, we switch the optimization objective back to the differential solution, enabling further refinement. Meanwhile, to alleviate the ''mean-seeking bias'' of MeanFlow under extremely few-step inference with complex target distributions, we incorporate trajectory distribution alignment as an auxiliary objective, encouraging the student model's trajectory distribution to align more closely with that of the teacher model. Our proposed distillation framework achieves superior performance compared to existing distillation approaches when applied to the text-to-image (T2I) model FLUX.1-dev (up to 12B parameters). Furthermore, when extended to the 80B-parameter state-of-the-art (SOTA) T2I model HunyuanImage 3.0, our method continues to demonstrate robust generalization and strong performance.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

STEP3-VL-10B Technical Report

We present STEP3-VL-10B, a lightweight open-source foundation model designed to redefine the trade-off between compact efficiency and frontier-level multimodal intelligence. STEP3-VL-10B is realized through two strategic shifts: first, a unified, fully unfrozen pre-training strategy on 1.2T multimodal tokens that integrates a language-aligned Perception Encoder with a Qwen3-8B decoder to establish intrinsic vision-language synergy; and second, a scaled post-training pipeline featuring over 1k iterations of reinforcement learning. Crucially, we implement Parallel Coordinated Reasoning (PaCoRe) to scale test-time compute, allocating resources to scalable perceptual reasoning that explores and synthesizes diverse visual hypotheses. Consequently, despite its compact 10B footprint, STEP3-VL-10B rivals or surpasses models 10$\times$-20$\times$ larger (e.g., GLM-4.6V-106B, Qwen3-VL-235B) and top-tier proprietary flagships like Gemini 2.5 Pro and Seed-1.5-VL. Delivering best-in-class performance, it records 92.2% on MMBench and 80.11% on MMMU, while excelling in complex reasoning with 94.43% on AIME2025 and 75.95% on MathVision. We release the full model suite to provide the community with a powerful, efficient, and reproducible baseline.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Subjective-Objective Median-based Importance Technique (SOMIT) to Aid Multi-Criteria Renewable Energy Evaluation

Accelerating the renewable energy transition requires informed decision-making that accounts for the diverse financial, technical, environmental, and social trade-offs across different renewable energy technologies. A critical step in this multi-criteria decision-making (MCDM) process is the determination of appropriate criteria weights. However, deriving these weights often solely involves either subjective assessment from decision-makers or objective weighting methods, each of which has limitations in terms of cognitive burden, potential bias, and insufficient contextual relevance. This study proposes the subjective-objective median-based importance technique (SOMIT), a novel hybrid approach for determining criteria weights in MCDM. By tailoring SOMIT to renewable energy evaluation, the method directly supports applied energy system planning, policy analysis, and technology prioritization under carbon neutrality goals. The practical utility of SOMIT is demonstrated through two MCDM case studies on renewable energy decision-making in India and Saudi Arabia. Using the derived weights from SOMIT, the TOPSIS method ranks the renewable energy alternatives, with solar power achieving the highest performance scores in both cases. The main contributions of this work are five-fold: 1) the proposed SOMIT reduces the number of required subjective comparisons from the conventional quadratic order to a linear order; 2) SOMIT is more robust to outliers in the alternatives-criteria matrix (ACM); 3) SOMIT balances subjective expert knowledge with objective data-driven insights, thereby mitigating bias; 4) SOMIT is inherently modular, allowing both its individual parts and the complete approach to be seamlessly coupled with a wide range of MCDM methods commonly applied in energy systems and policy analysis; 5) a dedicated Python library, pysomit, is developed for SOMIT.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

The RoboSense Challenge: Sense Anything, Navigate Anywhere, Adapt Across Platforms

Autonomous systems are increasingly deployed in open and dynamic environments -- from city streets to aerial and indoor spaces -- where perception models must remain reliable under sensor noise, environmental variation, and platform shifts. However, even state-of-the-art methods often degrade under unseen conditions, highlighting the need for robust and generalizable robot sensing. The RoboSense 2025 Challenge is designed to advance robustness and adaptability in robot perception across diverse sensing scenarios. It unifies five complementary research tracks spanning language-grounded decision making, socially compliant navigation, sensor configuration generalization, cross-view and cross-modal correspondence, and cross-platform 3D perception. Together, these tasks form a comprehensive benchmark for evaluating real-world sensing reliability under domain shifts, sensor failures, and platform discrepancies. RoboSense 2025 provides standardized datasets, baseline models, and unified evaluation protocols, enabling large-scale and reproducible comparison of robust perception methods. The challenge attracted 143 teams from 85 institutions across 16 countries, reflecting broad community engagement. By consolidating insights from 23 winning solutions, this report highlights emerging methodological trends, shared design principles, and open challenges across all tracks, marking a step toward building robots that can sense reliably, act robustly, and adapt across platforms in real-world environments.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Theoretical research on low-frequency drift Alfvén waves in general Tokamak equilibria

We developed kinetic models based on general fishbone-like dispersion relations. Firstly, a general model for arbitrary magnetic configuration and ion orbit width is presented. Then, by disregarding ion orbit width and approximating the magnetic geometry as circular, we introduce a simplified model that fully incorporates circulating/trapped ion effects. Finally, by considering the limit of ions being well-circulating or deeply trapped, the results directly revert to those observed in earlier theoretical studies.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: A Time-Domain Generalization of Extended Koopmans' Theorem

We introduce a framework for resolving electron-hole dynamics within wavefunction-based multiconfigurational time-dependent Hartree-Fock (MCTDHF) theory. Central to this framework is a time-domain generalization of the extended Koopmans' theorem, which rigorously defines time-dependent hole states through single-electron removal. From this foundation, we prove the existence of exact equations of motion for time-dependent Dyson orbitals, enabling instantaneous construction of photofragments' reduced density matrices. The formalism further yields a systematic procedure to extract hole-resolved observables, such as channel-resolved photoelectron momentum distributions, directly from time-dependent \textit{ab initio} wavefunctions. As a demonstration, we employ an attosecond $ω-2ω$ laser strategy to control hole dynamics, thereby resolving a long-standing challenge in MCTDHF simulations. This advance opens a pathway for exploring correlated multielectron dynamics in atoms and molecules under ultrafast laser fields.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Two-dimensional Intrinsic Janus Structures: Design Principle and Anomalous Nonlinear Optics

Two-dimensional Janus structures have garnered rapidly growing attention across multidisciplinary fields. However, despite extensive theoretical and experimental efforts, a principle for designing intrinsic Janus materials remains elusive. Here, we propose a first-principles alloy theory based on cluster expansion, incorporating a strong repulsive interaction of a cation-mediated anion-pair cluster and refined short-range cluster-cluster competitions, to unravel the formation mechanism of intrinsic Janus structures with a distorted 1T phase among numerous competing phases. Our theory not only explains why intrinsic Janus structures are accidentally observed in RhSeCl and BiTeI which are composed of alloyed elements from different groups, but also accurately predicts a wide range of 1T-like intrinsic Janus materials that are ready for synthesis. Intriguingly, as demonstrated in the case of RhSeCl, we reveal that intrinsic Janus materials can exhibit anomalous second-harmonic generation (SHG) with a distinct quantum geometric effect, originating from strong lattice and chemical-potential mirror asymmetry. Furthermore, a novel skin effect unexpectedly emerges in finite-thickness RhSeCl, accompanied by a hidden SHG effect within the bulk region. Our theory paves the way for the ab initio design of intrinsic Janus materials, significantly accelerating progress in Janus science.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Unique Decoding of Extended Subcodes of GRS Codes Using Error-Correcting Pairs

Extended Han-Zhang codes are a class of linear codes where each code is either a non-generalized Reed-Solomon (non-GRS) maximum distance separable (MDS) code or a near MDS (NMDS) code. They have important applications in communication, cryptography, and storage systems. While many algebraic properties and explicit constructions of extended Han-Zhang codes have been well studied in the literature, their decoding has been unexplored. In this paper, we focus on their decoding problems in terms of $\ell$-error-correcting pairs ($\ell$-ECPs) and deep holes. On the one hand, we determine the existence and specific forms of their $\ell$-ECPs, and further present an explicit decoding algorithm for extended Han-Zhang codes based on these $\ell$-ECPs, which can correct up to $\ell$ errors in polynomial time, with $\ell$ about half of the minimum distance. On the other hand, we determine the covering radius of extended Han-Zhang codes and characterize two classes of their deep holes, which are closely related to the maximum-likelihood decoding method. By employing these deep holes, we also construct more non-GRS MDS codes with larger lengths and dimensions, and discuss the monomial equivalence between them and the well-known Roth-Lempel codes. Some concrete examples are also given to support these results.

0 citations0 reviewsNo code linkedOpen access
preprint2026arXiv

Video-MSR: Benchmarking Multi-hop Spatial Reasoning Capabilities of MLLMs

Spatial reasoning has emerged as a critical capability for Multimodal Large Language Models (MLLMs), drawing increasing attention and rapid advancement. However, existing benchmarks primarily focus on single-step perception-to-judgment tasks, leaving scenarios requiring complex visual-spatial logical chains significantly underexplored. To bridge this gap, we introduce Video-MSR, the first benchmark specifically designed to evaluate Multi-hop Spatial Reasoning (MSR) in dynamic video scenarios. Video-MSR systematically probes MSR capabilities through four distinct tasks: Constrained Localization, Chain-based Reference Retrieval, Route Planning, and Counterfactual Physical Deduction. Our benchmark comprises 3,052 high-quality video instances with 4,993 question-answer pairs, constructed via a scalable, visually-grounded pipeline combining advanced model generation with rigorous human verification. Through a comprehensive evaluation of 20 state-of-the-art MLLMs, we uncover significant limitations, revealing that while models demonstrate proficiency in surface-level perception, they exhibit distinct performance drops in MSR tasks, frequently suffering from spatial disorientation and hallucination during multi-step deductions. To mitigate these shortcomings and empower models with stronger MSR capabilities, we further curate MSR-9K, a specialized instruction-tuning dataset, and fine-tune Qwen-VL, achieving a +7.82% absolute improvement on Video-MSR. Our results underscore the efficacy of multi-hop spatial instruction data and establish Video-MSR as a vital foundation for future research. The code and data will be available at https://github.com/ruiz-nju/Video-MSR.

0 citations0 reviewsNo code linkedOpen access
preprint2025arXiv

Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule

By simulating the real-time multielectron wavefunction with the multi-configurational time-dependent Hartree-Fock (MCTDHF) approach, we conduct an \textit{ab initio} study of the single-photon ionization process of a body-fixed water molecule ($\mathrm{H_2O}$) driven by attosecond pulses. To this end, we present a full-dimensional implementation of the MCTDHF method based on one-center expansions, allowing for the simulation of arbitrarily polarized lasers and multi-center polyatomic potentials. With a rigorous definition of the time-dependent hole state (TDHS) using the time-domain generalization of extended Koopmans' theorem (TD-EKT), we derive the reduced ion density matrix within the MCTDHF framework, which inherently encodes the total and channel-resolved photoionization cross sections of $\mathrm{H_2O}$. The cross sections obtained are benchmarked against existing experimental and theoretical results, validating the TDHS formalism. Furthermore, by adjusting the phase delay and intensity ratio of a pair of orthogonally polarized attosecond pulses, we explore the ultrafast control of attosecond coherence between electronic states of $\mathrm{H_2O^+}$.

0 citations0 reviewsNo code linkedOpen access