Accelerating materials discovery for polymer solar cells: Data-driven insights enabled by natural language processing

We present a natural language processing pipeline that was used to extract polymer solar cell property data from the literature and simulate various active learning strategies. While data-driven methods have been well established to discover novel materials faster than Edisonian trial-and-error approaches, their benefits have not been quantified. Our approach demonstrates a potential reduction in discovery time by approximately 75 %, equivalent to a 15 year acceleration in material innovation. Our pipeline enables us to extract data from more than 3300 papers which is ~5 times larger than similar data sets reported by others. We also trained machine learning models to predict the power conversion efficiency and used our model to identify promising donor-acceptor combinations that are as yet unreported. We thus demonstrate a workflow that goes from published literature to extracted material property data which in turn is used to obtain data-driven insights. Our insights include active learning strategies that can simultaneously optimize the material system and train strong predictive models of material properties. This work provides a valuable framework for research in material science.

Diffusion Models as Constrained Samplers for Optimization with Unknown Constraints

Addressing real-world optimization problems becomes particularly challenging when analytic objective functions or constraints are unavailable. While numerous studies have addressed the issue of unknown objectives, limited research has focused on scenarios where feasibility constraints are not given explicitly. Overlooking these constraints can lead to spurious solutions that are unrealistic in practice. To deal with such unknown constraints, we propose to perform optimization within the data manifold using diffusion models. To constrain the optimization process to the data manifold, we reformulate the original optimization problem as a sampling problem from the product of the Boltzmann distribution defined by the objective function and the data distribution learned by the diffusion model. To enhance sampling efficiency, we propose a two-stage framework that begins with a guided diffusion process for warm-up, followed by a Langevin dynamics stage for further correction. Theoretical analysis shows that the initial stage results in a distribution focused on feasible solutions, thereby providing a better initialization for the later stage. Comprehensive experiments on a synthetic dataset, six real-world black-box optimization datasets, and a multi-objective optimization dataset show that our method achieves better or comparable performance with previous state-of-the-art baselines.

CLAP: Learning Transferable Binary Code Representations with Natural Language Supervision

Binary code representation learning has shown significant performance in binary analysis tasks. But existing solutions often have poor transferability, particularly in few-shot and zero-shot scenarios where few or no training samples are available for the tasks. To address this problem, we present CLAP (Contrastive Language-Assembly Pre-training), which employs natural language supervision to learn better representations of binary code (i.e., assembly code) and get better transferability. At the core, our approach boosts superior transfer learning capabilities by effectively aligning binary code with their semantics explanations (in natural language), resulting a model able to generate better embeddings for binary code. To enable this alignment training, we then propose an efficient dataset engine that could automatically generate a large and diverse dataset comprising of binary code and corresponding natural language explanations. We have generated 195 million pairs of binary code and explanations and trained a prototype of CLAP. The evaluations of CLAP across various downstream tasks in binary analysis all demonstrate exceptional performance. Notably, without any task-specific training, CLAP is often competitive with a fully supervised baseline, showing excellent transferability. We release our pre-trained model and code at https://github.com/Hustcw/CLAP.

ARL2: Aligning Retrievers for Black-box Large Language Models via Self-guided Adaptive Relevance Labeling

Retrieval-augmented generation enhances large language models (LLMs) by incorporating relevant information from external knowledge sources. This enables LLMs to adapt to specific domains and mitigate hallucinations in knowledge-intensive tasks. However, existing retrievers are often misaligned with LLMs due to their separate training processes and the black-box nature of LLMs. To address this challenge, we propose ARL2, a retriever learning technique that harnesses LLMs as labelers. ARL2 leverages LLMs to annotate and score relevant evidence, enabling learning the retriever from robust LLM supervision. Furthermore, ARL2 uses an adaptive self-training strategy for curating high-quality and diverse relevance data, which can effectively reduce the annotation cost. Extensive experiments demonstrate the effectiveness of ARL2, achieving accuracy improvements of 5.4% on NQ and 4.6% on MMLU compared to the state-of-the-art methods. Additionally, ARL2 exhibits robust transfer learning capabilities and strong zero-shot generalization abilities. Our code will be published at \url{https://github.com/zhanglingxi-cs/ARL2}.

A Simple but Effective Approach to Improve Structured Language Model Output for Information Extraction

Large language models (LLMs) have demonstrated impressive abilities in generating unstructured natural language according to instructions. However, their performance can be inconsistent when tasked with producing text that adheres to specific structured formats, which is crucial in applications like named entity recognition (NER) or relation extraction (RE). To address this issue, this paper introduces an efficient method, G&O, to enhance their structured text generation capabilities. It breaks the generation into a two-step pipeline: initially, LLMs generate answers in natural language as intermediate responses. Subsequently, LLMs are asked to organize the output into the desired structure, using the intermediate responses as context. G&O effectively separates the generation of content from the structuring process, reducing the pressure of completing two orthogonal tasks simultaneously. Tested on zero-shot NER and RE, the results indicate a significant improvement in LLM performance with minimal additional efforts. This straightforward and adaptable prompting technique can also be combined with other strategies, like self-consistency, to further elevate LLM capabilities in various structured text generation tasks.

Handling Ambiguity in Emotion: From Out-of-Domain Detection to Distribution Estimation

The subjective perception of emotion leads to inconsistent labels from human annotators. Typically, utterances lacking majority-agreed labels are excluded when training an emotion classifier, which cause problems when encountering ambiguous emotional expressions during testing. This paper investigates three methods to handle ambiguous emotion. First, we show that incorporating utterances without majority-agreed labels as an additional class in the classifier reduces the classification performance of the other emotion classes. Then, we propose detecting utterances with ambiguous emotions as out-of-domain samples by quantifying the uncertainty in emotion classification using evidential deep learning. This approach retains the classification accuracy while effectively detects ambiguous emotion expressions. Furthermore, to obtain fine-grained distinctions among ambiguous emotions, we propose representing emotion as a distribution instead of a single class label. The task is thus re-framed from classification to distribution estimation where every individual annotation is taken into account, not just the majority opinion. The evidential uncertainty measure is extended to quantify the uncertainty in emotion distribution estimation. Experimental results on the IEMOCAP and CREMA-D datasets demonstrate the superior capability of the proposed method in terms of majority class prediction, emotion distribution estimation, and uncertainty estimation.

BBox-Adapter: Lightweight Adapting for Black-Box Large Language Models

Adapting state-of-the-art Large Language Models (LLMs) like GPT-4 and Gemini for specific tasks is challenging. Due to the opacity in their parameters, embeddings, and even output probabilities, existing fine-tuning adaptation methods are inapplicable. Consequently, adapting these black-box LLMs is only possible through their API services, raising concerns about transparency, privacy, and cost. To address these challenges, we introduce BBox-Adapter, a novel lightweight adapter for black-box LLMs. BBox-Adapter distinguishes target and source domain data by treating target data as positive and source data as negative. It employs a ranking-based Noise Contrastive Estimation (NCE) loss to promote the likelihood of target domain data while penalizing that of the source domain. Furthermore, it features an online adaptation mechanism, which incorporates real-time positive data sampling from ground-truth, human, or AI feedback, coupled with negative data from previous adaptations. Extensive experiments demonstrate BBox-Adapter's effectiveness and cost efficiency. It improves model performance by up to 6.77% across diverse tasks and domains, while reducing training and inference costs by 31.30x and 1.84x, respectively.

EAGLE: Speculative Sampling Requires Rethinking Feature Uncertainty

Autoregressive decoding makes the inference of Large Language Models (LLMs) time-consuming. In this paper, we reconsider speculative sampling and derive two key observations. Firstly, autoregression at the feature (second-to-top-layer) level is more straightforward than at the token level. Secondly, the inherent uncertainty in feature (second-to-top-layer) level autoregression constrains its performance. Based on these insights, we introduce EAGLE (Extrapolation Algorithm for Greater Language-model Efficiency), a simple yet highly efficient speculative sampling framework. By incorporating a token sequence advanced by one time step, EAGLE effectively resolves the uncertainty, enabling precise second-to-top-layer feature prediction with minimal overhead. We conducted comprehensive evaluations of EAGLE, including all models from the Vicuna and LLaMA2-Chat series, the MoE model Mixtral 8x7B Instruct, and tasks in dialogue, code generation, mathematical reasoning, and instruction following. For LLaMA2-Chat 70B, EAGLE achieved a latency speedup ratio of 2.7x-3.5x, doubled throughput, while maintaining the distribution of the generated text.

Neural Sinkhorn Gradient Flow

Wasserstein Gradient Flows (WGF) with respect to specific functionals have been widely used in the machine learning literature. Recently, neural networks have been adopted to approximate certain intractable parts of the underlying Wasserstein gradient flow and result in efficient inference procedures. In this paper, we introduce the Neural Sinkhorn Gradient Flow (NSGF) model, which parametrizes the time-varying velocity field of the Wasserstein gradient flow w.r.t. the Sinkhorn divergence to the target distribution starting a given source distribution. We utilize the velocity field matching training scheme in NSGF, which only requires samples from the source and target distribution to compute an empirical velocity field approximation. Our theoretical analyses show that as the sample size increases to infinity, the mean-field limit of the empirical approximation converges to the true underlying velocity field. To further enhance model efficiency on high-dimensional tasks, a two-phase NSGF++ model is devised, which first follows the Sinkhorn flow to approach the image manifold quickly ($\le 5$ NFEs) and then refines the samples along a simple straight flow. Numerical experiments with synthetic and real-world benchmark datasets support our theoretical results and demonstrate the effectiveness of the proposed methods.