Large language models, physics-based modeling, experimental measurements: the trinity of data-scarce learning of polymer properties

Large language models (LLMs) bear promise as a fast and accurate material modeling paradigm for evaluation, analysis, and design. Their vast number of trainable parameters necessitates a wealth of data to achieve accuracy and mitigate overfitting. However, experimental measurements are often limited and costly to obtain in sufficient quantities for finetuning. To this end, we present a physics-based training pipeline that tackles the pathology of data scarcity. The core enabler is a physics-based modeling framework that generates a multitude of synthetic data to align the LLM to a physically consistent initial state before finetuning. Our framework features a two-phase training strategy: (1) utilizing the large-in-amount while less accurate synthetic data for supervised pretraining, and (2) finetuning the phase-1 model with limited experimental data. We empirically demonstrate that supervised pretraining is vital to obtaining accurate finetuned LLMs, via the lens of learning polymer flammability metrics where cone calorimeter data is sparse.

RankRAG: Unifying Context Ranking with Retrieval-Augmented Generation in LLMs

Large language models (LLMs) typically utilize the top-k contexts from a retriever in retrieval-augmented generation (RAG). In this work, we propose a novel instruction fine-tuning framework RankRAG, which instruction-tunes a single LLM for the dual purpose of context ranking and answer generation in RAG. In particular, the instruction-tuned LLMs work surprisingly well by adding a small fraction of ranking data into the training blend, and outperform existing expert ranking models, including the same LLM exclusively fine-tuned on a large amount of ranking data. For generation, we compare our model with many strong baselines, including GPT-4-0613, GPT-4-turbo-2024-0409, and ChatQA-1.5, an open-sourced model with the state-of-the-art performance on RAG benchmarks. Specifically, our Llama3-RankRAG significantly outperforms Llama3-ChatQA-1.5 and GPT-4 models on nine knowledge-intensive benchmarks. In addition, it also performs comparably to GPT-4 on five RAG benchmarks in the biomedical domain without instruction fine-tuning on biomedical data, demonstrating its superb capability for generalization to new domains.

Efficient Evolutionary Search Over Chemical Space with Large Language Models

Molecular discovery, when formulated as an optimization problem, presents significant computational challenges because optimization objectives can be non-differentiable. Evolutionary Algorithms (EAs), often used to optimize black-box objectives in molecular discovery, traverse chemical space by performing random mutations and crossovers, leading to a large number of expensive objective evaluations. In this work, we ameliorate this shortcoming by incorporating chemistry-aware Large Language Models (LLMs) into EAs. Namely, we redesign crossover and mutation operations in EAs using LLMs trained on large corpora of chemical information. We perform extensive empirical studies on both commercial and open-source models on multiple tasks involving property optimization, molecular rediscovery, and structure-based drug design, demonstrating that the joint usage of LLMs with EAs yields superior performance over all baseline models across single- and multi-objective settings. We demonstrate that our algorithm improves both the quality of the final solution and convergence speed, thereby reducing the number of required objective evaluations. Our code is available at http://github.com/zoom-wang112358/MOLLEO

Toward Exploring the Code Understanding Capabilities of Pre-trained Code Generation Models

Recently, large code generation models trained in a self-supervised manner on extensive unlabeled programming language data have achieved remarkable success. While these models acquire vast amounts of code knowledge, they perform poorly on code understanding tasks, such as code search and clone detection, as they are specifically trained for generation. Pre-training a larger encoder-only architecture model from scratch on massive code data can improve understanding performance. However, this approach is costly and time-consuming, making it suboptimal. In this paper, we pioneer the transfer of knowledge from pre-trained code generation models to code understanding tasks, significantly reducing training costs. We examine effective strategies for enabling decoder-only models to acquire robust code representations. Furthermore, we introduce CL4D, a contrastive learning method designed to enhance the representation capabilities of decoder-only models. Comprehensive experiments demonstrate that our approach achieves state-of-the-art performance in understanding tasks such as code search and clone detection. Our analysis shows that our method effectively reduces the distance between semantically identical samples in the representation space. These findings suggest the potential for unifying code understanding and generation tasks using a decoder-only structured model.

GUI-WORLD: A Dataset for GUI-oriented Multimodal LLM-based Agents

Recently, Multimodal Large Language Models (MLLMs) have been used as agents to control keyboard and mouse inputs by directly perceiving the Graphical User Interface (GUI) and generating corresponding code. However, current agents primarily exhibit excellent understanding capabilities in static environments and are predominantly applied in relatively simple domains, such as Web or mobile interfaces. We argue that a robust GUI agent should be capable of perceiving temporal information on the GUI, including dynamic Web content and multi-step tasks. Additionally, it should possess a comprehensive understanding of various GUI scenarios, including desktop software and multi-window interactions. To this end, this paper introduces a new dataset, termed GUI-World, which features meticulously crafted Human-MLLM annotations, extensively covering six GUI scenarios and eight types of GUI-oriented questions in three formats. We evaluate the capabilities of current state-of-the-art MLLMs, including ImageLLMs and VideoLLMs, in understanding various types of GUI content, especially dynamic and sequential content. Our findings reveal that ImageLLMs struggle with dynamic GUI content without manually annotated keyframes or operation history. On the other hand, VideoLLMs fall short in all GUI-oriented tasks given the sparse GUI video dataset. Based on GUI-World, we take the initial step of leveraging a fine-tuned VideoLLM as a GUI agent, demonstrating an improved understanding of various GUI tasks. However, due to the limitations in the performance of base LLMs, we conclude that using VideoLLMs as GUI agents remains a significant challenge. We believe our work provides valuable insights for future research in dynamic GUI content understanding. The code and dataset are publicly available at our project homepage: https://gui-world.github.io/.

PairCFR: Enhancing Model Training on Paired Counterfactually Augmented Data through Contrastive Learning

Counterfactually Augmented Data (CAD) involves creating new data samples by applying minimal yet sufficient modifications to flip the label of existing data samples to other classes. Training with CAD enhances model robustness against spurious features that happen to correlate with labels by spreading the casual relationships across different classes. Yet, recent research reveals that training with CAD may lead models to overly focus on modified features while ignoring other important contextual information, inadvertently introducing biases that may impair performance on out-ofdistribution (OOD) datasets. To mitigate this issue, we employ contrastive learning to promote global feature alignment in addition to learning counterfactual clues. We theoretically prove that contrastive loss can encourage models to leverage a broader range of features beyond those modified ones. Comprehensive experiments on two human-edited CAD datasets demonstrate that our proposed method outperforms the state-of-the-art on OOD datasets.

HYDRA: Model Factorization Framework for Black-Box LLM Personalization

Personalization has emerged as a critical research area in modern intelligent systems, focusing on mining users' behavioral history and adapting to their preferences for delivering tailored experiences. Despite the remarkable few-shot capabilities exhibited by black-box large language models (LLMs), the inherent opacity of their model parameters presents significant challenges in aligning the generated output with individual expectations. Existing solutions have primarily focused on prompt design to incorporate user-specific profiles and behaviors; however, such approaches often struggle to generalize effectively due to their inability to capture shared knowledge among all users. To address these challenges, we propose HYDRA, a model factorization framework that captures both user-specific behavior patterns from historical data and shared general knowledge among all users to deliver personalized generation. In order to capture user-specific behavior patterns, we first train a reranker to prioritize the most useful information from top-retrieved relevant historical records. By combining the prioritized history with the corresponding query, we train an adapter to align the output with individual user-specific preferences, eliminating the reliance on access to inherent model parameters of black-box LLMs. Both the reranker and the adapter can be decomposed into a base model with multiple user-specific heads, resembling a hydra. The base model maintains shared knowledge across users, while the multiple personal heads capture user-specific preferences. Experimental results demonstrate that HYDRA outperforms existing state-of-the-art prompt-based methods by an average relative improvement of 9.01% across five diverse personalization tasks in the LaMP benchmark. Our implementation is available at https://github.com/night-chen/HYDRA.

Online Self-Preferring Language Models

Aligning with human preference datasets has been critical to the success of large language models (LLMs). Reinforcement learning from human feedback (RLHF) employs a costly reward model to provide feedback for on-policy sampling responses. Recently, offline methods that directly fit responses with binary preferences in the dataset have emerged as alternatives. However, existing methods do not explicitly model preference strength information, which is crucial for distinguishing different response pairs. To overcome this limitation, we propose Online Self-Preferring (OSP) language models to learn from self-generated response pairs and self-judged preference strengths. For each prompt and corresponding self-generated responses, we introduce a ranked pairing method to construct multiple response pairs with preference strength information. We then propose the soft-preference cross-entropy loss to leverage such information. Empirically, we demonstrate that leveraging preference strength is crucial for avoiding overfitting and enhancing alignment performance. OSP achieves state-of-the-art alignment performance across various metrics in two widely used human preference datasets. OSP is parameter-efficient and more robust than the dominant online method, RLHF when limited offline data are available and generalizing to out-of-domain tasks. Moreover, OSP language models established by LLMs with proficiency in self-preferring can efficiently self-improve without external supervision.

Intuitive Fine-Tuning: Towards Unifying SFT and RLHF into a Single Process

Supervised Fine-Tuning (SFT) and Reinforcement Learning from Human Feedback (RLHF) are two fundamental processes for enhancing the capabilities of Language Models (LMs) post pre-training, aligning them better with human preferences. Although SFT advances in training efficiency, RLHF delivers better alignment, thus they are often combined. However, common practices simply apply them sequentially without unifying their optimization targets, resulting in a trade-off between fitting different objectives, and ignoring the opportunities to bridge the paradigm gap and take the strength from both. To obtain a unified understanding, we interpret SFT and RLHF using two sub-processes -- Preference Estimation and Transition Optimization -- defined at token level within the Markov Decision Process (MDP) framework. This modeling shows that SFT is only a specialized case of RLHF with inferior estimation and optimization. RLHF evaluates the quality of model's entire generated answer, whereas SFT only scores predicted tokens based on preceding tokens from target answers. Therefore, SFT overestimates the ability of model, leading to inferior optimization. Building on this view, we introduce Intuitive Fine-tuning (IFT) to integrate SFT and RLHF into a single process. IFT captures LMs' intuitive sense of the entire answers through a temporal residual connection, while using a single policy and the same volume of non-preference-labeled data as SFT. Our experiments show that IFT performs comparably or even superiorly to sequential recipes of SFT and some typical alignment methods across several tasks, particularly those requires generation, reasoning, and fact-following abilities. An explainable Frozen Lake game further validates the effectiveness of IFT.

Deep Neural Operator Enabled Digital Twin Modeling for Additive Manufacturing

A digital twin (DT), with the components of a physics-based model, a data-driven model, and a machine learning (ML) enabled efficient surrogate, behaves as a virtual twin of the real-world physical process. In terms of Laser Powder Bed Fusion (L-PBF) based additive manufacturing (AM), a DT can predict the current and future states of the melt pool and the resulting defects corresponding to the input laser parameters, evolve itself by assimilating in-situ sensor data, and optimize the laser parameters to mitigate defect formation. In this paper, we present a deep neural operator enabled computational framework of the DT for closed-loop feedback control of the L-PBF process. This is accomplished by building a high-fidelity computational model to accurately represent the melt pool states, an efficient surrogate model to approximate the melt pool solution field, followed by an physics-based procedure to extract information from the computed melt pool simulation that can further be correlated to the defect quantities of interest (e.g., surface roughness). In particular, we leverage the data generated from the high-fidelity physics-based model and train a series of Fourier neural operator (FNO) based ML models to effectively learn the relation between the input laser parameters and the corresponding full temperature field of the melt pool. Subsequently, a set of physics-informed variables such as the melt pool dimensions and the peak temperature can be extracted to compute the resulting defects. An optimization algorithm is then exercised to control laser input and minimize defects. On the other hand, the constructed DT can also evolve with the physical twin via offline finetuning and online material calibration. Finally, a probabilistic framework is adopted for uncertainty quantification. The developed DT is envisioned to guide the AM process and facilitate high-quality manufacturing.