Daily Papers

Accelerating material discovery holds the potential to greatly help mitigate the climate crisis. Discovering new solid-state materials such as electrocatalysts, super-ionic conductors or photovoltaic materials can have a crucial impact, for instance, in improving the efficiency of renewable energy production and storage. In this paper, we introduce Crystal-GFN, a generative model of crystal structures that sequentially samples structural properties of crystalline materials, namely the space group, composition and lattice parameters. This domain-inspired approach enables the flexible incorporation of physical and structural hard constraints, as well as the use of any available predictive model of a desired physicochemical property as an objective function. To design stable materials, one must target the candidates with the lowest formation energy. Here, we use as objective the formation energy per atom of a crystal structure predicted by a new proxy machine learning model trained on MatBench. The results demonstrate that Crystal-GFN is able to sample highly diverse crystals with low (median -3.1 eV/atom) predicted formation energy.

Extensive work has shown that the performance and interpretability of commonsense reasoning can be improved via knowledge-augmented reasoning methods, where the knowledge that underpins the reasoning process is explicitly verbalized and utilized. However, existing implementations, including "chain-of-thought" and its variants, fall short in capturing the introspective nature of knowledge required in commonsense reasoning, and in accounting for the mutual adaptation between the generation and utilization of knowledge. We propose a novel method to develop an introspective commonsense reasoner, Crystal. To tackle commonsense problems, it first introspects for knowledge statements related to the given question, and subsequently makes an informed prediction that is grounded in the previously introspected knowledge. The knowledge introspection and knowledge-grounded reasoning modes of the model are tuned via reinforcement learning to mutually adapt, where the reward derives from the feedback given by the model itself. Experiments show that Crystal significantly outperforms both the standard supervised finetuning and chain-of-thought distilled methods, and enhances the transparency of the commonsense reasoning process. Our work ultimately validates the feasibility and potential of reinforcing a neural model with self-feedback.

Generating the periodic structure of stable materials is a long-standing challenge for the material design community. This task is difficult because stable materials only exist in a low-dimensional subspace of all possible periodic arrangements of atoms: 1) the coordinates must lie in the local energy minimum defined by quantum mechanics, and 2) global stability also requires the structure to follow the complex, yet specific bonding preferences between different atom types. Existing methods fail to incorporate these factors and often lack proper invariances. We propose a Crystal Diffusion Variational Autoencoder (CDVAE) that captures the physical inductive bias of material stability. By learning from the data distribution of stable materials, the decoder generates materials in a diffusion process that moves atomic coordinates towards a lower energy state and updates atom types to satisfy bonding preferences between neighbors. Our model also explicitly encodes interactions across periodic boundaries and respects permutation, translation, rotation, and periodic invariances. We significantly outperform past methods in three tasks: 1) reconstructing the input structure, 2) generating valid, diverse, and realistic materials, and 3) generating materials that optimize a specific property. We also provide several standard datasets and evaluation metrics for the broader machine learning community.

Large Language Models (LLMs) specializing in code generation (which are also often referred to as code LLMs), e.g., StarCoder and Code Llama, play increasingly critical roles in various software development scenarios. It is also crucial for code LLMs to possess both code generation and natural language abilities for many specific applications, such as code snippet retrieval using natural language or code explanations. The intricate interaction between acquiring language and coding skills complicates the development of strong code LLMs. Furthermore, there is a lack of thorough prior studies on the LLM pretraining strategy that mixes code and natural language. In this work, we propose a pretraining strategy to enhance the integration of natural language and coding capabilities within a single LLM. Specifically, it includes two phases of training with appropriately adjusted code/language ratios. The resulting model, Crystal, demonstrates remarkable capabilities in both domains. Specifically, it has natural language and coding performance comparable to that of Llama 2 and Code Llama, respectively. Crystal exhibits better data efficiency, using 1.4 trillion tokens compared to the more than 2 trillion tokens used by Llama 2 and Code Llama. We verify our pretraining strategy by analyzing the training process and observe consistent improvements in most benchmarks. We also adopted a typical application adaptation phase with a code-centric data mixture, only to find that it did not lead to enhanced performance or training efficiency, underlining the importance of a carefully designed data recipe. To foster research within the community, we commit to open-sourcing every detail of the pretraining, including our training datasets, code, loggings and 136 checkpoints throughout the training.

Crystal structures are characterized by atomic bases within a primitive unit cell that repeats along a regular lattice throughout 3D space. The periodic and infinite nature of crystals poses unique challenges for geometric graph representation learning. Specifically, constructing graphs that effectively capture the complete geometric information of crystals and handle chiral crystals remains an unsolved and challenging problem. In this paper, we introduce a novel approach that utilizes the periodic patterns of unit cells to establish the lattice-based representation for each atom, enabling efficient and expressive graph representations of crystals. Furthermore, we propose ComFormer, a SE(3) transformer designed specifically for crystalline materials. ComFormer includes two variants; namely, iComFormer that employs invariant geometric descriptors of Euclidean distances and angles, and eComFormer that utilizes equivariant vector representations. Experimental results demonstrate the state-of-the-art predictive accuracy of ComFormer variants on various tasks across three widely-used crystal benchmarks. Our code is publicly available as part of the AIRS library (https://github.com/divelab/AIRS).

Crystal Structure Prediction (CSP) is crucial in various scientific disciplines. While CSP can be addressed by employing currently-prevailing generative models (e.g. diffusion models), this task encounters unique challenges owing to the symmetric geometry of crystal structures -- the invariance of translation, rotation, and periodicity. To incorporate the above symmetries, this paper proposes DiffCSP, a novel diffusion model to learn the structure distribution from stable crystals. To be specific, DiffCSP jointly generates the lattice and atom coordinates for each crystal by employing a periodic-E(3)-equivariant denoising model, to better model the crystal geometry. Notably, different from related equivariant generative approaches, DiffCSP leverages fractional coordinates other than Cartesian coordinates to represent crystals, remarkably promoting the diffusion and the generation process of atom positions. Extensive experiments verify that our DiffCSP significantly outperforms existing CSP methods, with a much lower computation cost in contrast to DFT-based methods. Moreover, the superiority of DiffCSP is also observed when it is extended for ab initio crystal generation.

The generation of plausible crystal structures is often the first step in predicting the structure and properties of a material from its chemical composition. Quickly generating and predicting inorganic crystal structures is important for the discovery of new materials, which can target applications such as energy or electronic devices. However, most current methods for crystal structure prediction are computationally expensive, slowing the pace of innovation. Seeding structure prediction algorithms with quality generated candidates can overcome a major bottleneck. Here, we introduce CrystaLLM, a methodology for the versatile generation of crystal structures, based on the autoregressive large language modeling (LLM) of the Crystallographic Information File (CIF) format. Trained on millions of CIF files, CrystaLLM focuses on modeling crystal structures through text. CrystaLLM can produce plausible crystal structures for a wide range of inorganic compounds unseen in training, as demonstrated by ab initio simulations. The integration with predictors of formation energy permits the use of a Monte Carlo Tree Search algorithm to improve the generation of meaningful structures. Our approach challenges conventional representations of crystals, and demonstrates the potential of LLMs for learning effective 'world models' of crystal chemistry, which will lead to accelerated discovery and innovation in materials science.

Self-supervised neural language models have recently achieved unprecedented success, from natural language processing to learning the languages of biological sequences and organic molecules. These models have demonstrated superior performance in the generation, structure classification, and functional predictions for proteins and molecules with learned representations. However, most of the masking-based pre-trained language models are not designed for generative design, and their black-box nature makes it difficult to interpret their design logic. Here we propose BLMM Crystal Transformer, a neural network based probabilistic generative model for generative and tinkering design of inorganic materials. Our model is built on the blank filling language model for text generation and has demonstrated unique advantages in learning the "materials grammars" together with high-quality generation, interpretability, and data efficiency. It can generate chemically valid materials compositions with as high as 89.7\% charge neutrality and 84.8\% balanced electronegativity, which are more than 4 and 8 times higher compared to a pseudo random sampling baseline. The probabilistic generation process of BLMM allows it to recommend tinkering operations based on learned materials chemistry and makes it useful for materials doping. Combined with the TCSP crysal structure prediction algorithm, We have applied our model to discover a set of new materials as validated using DFT calculations. Our work thus brings the unsupervised transformer language models based generative artificial intelligence to inorganic materials. A user-friendly web app has been developed for computational materials doping and can be accessed freely at www.materialsatlas.org/blmtinker.

Crystals are the foundation of numerous scientific and industrial applications. While various learning-based approaches have been proposed for crystal generation, existing methods seldom consider the space group constraint which is crucial in describing the geometry of crystals and closely relevant to many desirable properties. However, considering space group constraint is challenging owing to its diverse and nontrivial forms. In this paper, we reduce the space group constraint into an equivalent formulation that is more tractable to be handcrafted into the generation process. In particular, we translate the space group constraint into two parts: the basis constraint of the invariant logarithmic space of the lattice matrix and the Wyckoff position constraint of the fractional coordinates. Upon the derived constraints, we then propose DiffCSP++, a novel diffusion model that has enhanced a previous work DiffCSP by further taking space group constraint into account. Experiments on several popular datasets verify the benefit of the involvement of the space group constraint, and show that our DiffCSP++ achieves promising performance on crystal structure prediction, ab initio crystal generation and controllable generation with customized space groups.

Predicting physical properties of materials from their crystal structures is a fundamental problem in materials science. In peripheral areas such as the prediction of molecular properties, fully connected attention networks have been shown to be successful. However, unlike these finite atom arrangements, crystal structures are infinitely repeating, periodic arrangements of atoms, whose fully connected attention results in infinitely connected attention. In this work, we show that this infinitely connected attention can lead to a computationally tractable formulation, interpreted as neural potential summation, that performs infinite interatomic potential summations in a deeply learned feature space. We then propose a simple yet effective Transformer-based encoder architecture for crystal structures called Crystalformer. Compared to an existing Transformer-based model, the proposed model requires only 29.4% of the number of parameters, with minimal modifications to the original Transformer architecture. Despite the architectural simplicity, the proposed method outperforms state-of-the-art methods for various property regression tasks on the Materials Project and JARVIS-DFT datasets.

We introduce the use of Crystal Graph Convolutional Neural Networks (CGCNN), Fully Connected Neural Networks (FCNN) and XGBoost to predict thermoelectric properties. The dataset for the CGCNN is independent of Density Functional Theory (DFT) and only relies on the crystal and atomic information, while that for the FCNN is based on a rich attribute list mined from Materialsproject.org. The results show that the optimized FCNN is three layer deep and is able to predict the scattering-time independent thermoelectric powerfactor much better than the CGCNN (or XGBoost), suggesting that bonding and density of states descriptors informed from materials science knowledge obtained partially from DFT are vital to predict functional properties.

Normalizing flows (NF) are a class of powerful generative models that have gained popularity in recent years due to their ability to model complex distributions with high flexibility and expressiveness. In this work, we introduce a new type of normalizing flow that is tailored for modeling positions and orientations of multiple objects in three-dimensional space, such as molecules in a crystal. Our approach is based on two key ideas: first, we define smooth and expressive flows on the group of unit quaternions, which allows us to capture the continuous rotational motion of rigid bodies; second, we use the double cover property of unit quaternions to define a proper density on the rotation group. This ensures that our model can be trained using standard likelihood-based methods or variational inference with respect to a thermodynamic target density. We evaluate the method by training Boltzmann generators for two molecular examples, namely the multi-modal density of a tetrahedral system in an external field and the ice XI phase in the TIP4P water model. Our flows can be combined with flows operating on the internal degrees of freedom of molecules and constitute an important step towards the modeling of distributions of many interacting molecules.

With their non-Abelian topological charges, real multi-bandgap systems challenge the conventional topological phase classifications. As the minimal sector of multi-bandgap systems, real triple degeneracies (RTPs), which serve as real 'Weyl points', lay the foundation for the research on real topological phases. However, experimental demonstration of physical systems with global band configurations consisting of multiple RTPs in crystals has not been reported. Here we present experimental evidence of RTPs in photonic meta-crystals, characterizing them using the Euler number, and establishing their connection with both Abelian and non-Abelian charges. By considering RTPs as the basic elements, we further propose the concept of a topological compound, akin to a chemical compound, where we find that certain phases are not topologically allowed. The topological classification of RTPs in crystals demonstrated in our work plays a similar role as the 'no-go' theorem in Weyl systems.

Matbench Discovery simulates the deployment of machine learning (ML) energy models in a high-throughput search for stable inorganic crystals. We address the disconnect between (i) thermodynamic stability and formation energy and (ii) in-domain vs out-of-distribution performance. Alongside this paper, we publish a Python package to aid with future model submissions and a growing online leaderboard with further insights into trade-offs between various performance metrics. To answer the question which ML methodology performs best at materials discovery, our initial release explores a variety of models including random forests, graph neural networks (GNN), one-shot predictors, iterative Bayesian optimizers and universal interatomic potentials (UIP). Ranked best-to-worst by their test set F1 score on thermodynamic stability prediction, we find CHGNet > M3GNet > MACE > ALIGNN > MEGNet > CGCNN > CGCNN+P > Wrenformer > BOWSR > Voronoi tessellation fingerprints with random forest. The top 3 models are UIPs, the winning methodology for ML-guided materials discovery, achieving F1 scores of ~0.6 for crystal stability classification and discovery acceleration factors (DAF) of up to 5x on the first 10k most stable predictions compared to dummy selection from our test set. We also highlight a sharp disconnect between commonly used global regression metrics and more task-relevant classification metrics. Accurate regressors are susceptible to unexpectedly high false-positive rates if those accurate predictions lie close to the decision boundary at 0 eV/atom above the convex hull where most materials are. Our results highlight the need to focus on classification metrics that actually correlate with improved stability hit rate.

We present a computational framework that transforms single images into 3D physical objects. The visual geometry of a physical object in an image is determined by three orthogonal attributes: mechanical properties, external forces, and rest-shape geometry. Existing single-view 3D reconstruction methods often overlook this underlying composition, presuming rigidity or neglecting external forces. Consequently, the reconstructed objects fail to withstand real-world physical forces, resulting in instability or undesirable deformation -- diverging from their intended designs as depicted in the image. Our optimization framework addresses this by embedding physical compatibility into the reconstruction process. We explicitly decompose the three physical attributes and link them through static equilibrium, which serves as a hard constraint, ensuring that the optimized physical shapes exhibit desired physical behaviors. Evaluations on a dataset collected from Objaverse demonstrate that our framework consistently enhances the physical realism of 3D models over existing methods. The utility of our framework extends to practical applications in dynamic simulations and 3D printing, where adherence to physical compatibility is paramount.

Language models (LMs) have become ubiquitous in both NLP research and in commercial product offerings. As their commercial importance has surged, the most powerful models have become closed off, gated behind proprietary interfaces, with important details of their training data, architectures, and development undisclosed. Given the importance of these details in scientifically studying these models, including their biases and potential risks, we believe it is essential for the research community to have access to powerful, truly open LMs. To this end, this technical report details the first release of OLMo, a state-of-the-art, truly Open Language Model and its framework to build and study the science of language modeling. Unlike most prior efforts that have only released model weights and inference code, we release OLMo and the whole framework, including training data and training and evaluation code. We hope this release will empower and strengthen the open research community and inspire a new wave of innovation.

Language models have become a critical technology to tackling a wide range of natural language processing tasks, yet many details about how the best-performing language models were developed are not reported. In particular, information about their pretraining corpora is seldom discussed: commercial language models rarely provide any information about their data; even open models rarely release datasets they are trained on, or an exact recipe to reproduce them. As a result, it is challenging to conduct certain threads of language modeling research, such as understanding how training data impacts model capabilities and shapes their limitations. To facilitate open research on language model pretraining, we release Dolma, a three trillion tokens English corpus, built from a diverse mixture of web content, scientific papers, code, public-domain books, social media, and encyclopedic materials. In addition, we open source our data curation toolkit to enable further experimentation and reproduction of our work. In this report, we document Dolma, including its design principles, details about its construction, and a summary of its contents. We interleave this report with analyses and experimental results from training language models on intermediate states of Dolma to share what we have learned about important data curation practices, including the role of content or quality filters, deduplication, and multi-source mixing. Dolma has been used to train OLMo, a state-of-the-art, open language model and framework designed to build and study the science of language modeling.

Today's most advanced multimodal models remain proprietary. The strongest open-weight models rely heavily on synthetic data from proprietary VLMs to achieve good performance, effectively distilling these closed models into open ones. As a result, the community is still missing foundational knowledge about how to build performant VLMs from scratch. We present Molmo, a new family of VLMs that are state-of-the-art in their class of openness. Our key innovation is a novel, highly detailed image caption dataset collected entirely from human annotators using speech-based descriptions. To enable a wide array of user interactions, we also introduce a diverse dataset mixture for fine-tuning that includes in-the-wild Q&A and innovative 2D pointing data. The success of our approach relies on careful choices for the model architecture details, a well-tuned training pipeline, and, most critically, the quality of our newly collected datasets, all of which will be released. The best-in-class 72B model within the Molmo family not only outperforms others in the class of open weight and data models but also compares favorably against proprietary systems like GPT-4o, Claude 3.5, and Gemini 1.5 on both academic benchmarks and human evaluation. We will be releasing all of our model weights, captioning and fine-tuning data, and source code in the near future. Select model weights, inference code, and demo are available at https://molmo.allenai.org.

We present OLMo 2, the next generation of our fully open language models. OLMo 2 includes dense autoregressive models with improved architecture and training recipe, pretraining data mixtures, and instruction tuning recipes. Our modified model architecture and training recipe achieve both better training stability and improved per-token efficiency. Our updated pretraining data mixture introduces a new, specialized data mix called Dolmino Mix 1124, which significantly improves model capabilities across many downstream task benchmarks when introduced via late-stage curriculum training (i.e. specialized data during the annealing phase of pretraining). Finally, we incorporate best practices from T\"ulu 3 to develop OLMo 2-Instruct, focusing on permissive data and extending our final-stage reinforcement learning with verifiable rewards (RLVR). Our OLMo 2 base models sit at the Pareto frontier of performance to compute, often matching or outperforming open-weight only models like Llama 3.1 and Qwen 2.5 while using fewer FLOPs and with fully transparent training data, code, and recipe. Our fully open OLMo 2-Instruct models are competitive with or surpassing open-weight only models of comparable size, including Qwen 2.5, Llama 3.1 and Gemma 2. We release all OLMo 2 artifacts openly -- models at 7B and 13B scales, both pretrained and post-trained, including their full training data, training code and recipes, training logs and thousands of intermediate checkpoints. The final instruction model is available on the Ai2 Playground as a free research demo.

In this letter, we report the discovery of the highest redshift, heavily obscured, radio-loud QSO candidate selected using JWST NIRCam/MIRI, mid-IR, sub-mm, and radio imaging in the COSMOS-Web field. Using multi-frequency radio observations and mid-IR photometry, we identify a powerful, radio-loud (RL), growing supermassive black hole (SMBH) with significant spectral steepening of the radio SED (f_{1.32 GHz} sim 2 mJy, q_{24mu m} = -1.1, alpha_{1.32-3GHz}=-1.2, Delta alpha = -0.4). In conjunction with ALMA, deep ground-based observations, ancillary space-based data, and the unprecedented resolution and sensitivity of JWST, we find no evidence of QSO contribution to the UV/optical/NIR data and thus infer heavy amounts of obscuration (N_{H} > 10^{23} cm^{-2}). Using the wealth of deep UV to sub-mm photometric data, we report a singular solution photo-z of z_phot = 7.65^{+0.4}_{-0.3} and estimate an extremely massive host-galaxy (log M_{star} = 11.92 pm 0.06,M_{odot}). This source represents the furthest known obscured RL QSO candidate, and its level of obscuration aligns with the most representative but observationally scarce population of QSOs at these epochs.

Crystalline materials are a fundamental component in next-generation technologies, yet modeling their distribution presents unique computational challenges. Of the plausible arrangements of atoms in a periodic lattice only a vanishingly small percentage are thermodynamically stable, which is a key indicator of the materials that can be experimentally realized. Two fundamental tasks in this area are to (a) predict the stable crystal structure of a known composition of elements and (b) propose novel compositions along with their stable structures. We present FlowMM, a pair of generative models that achieve state-of-the-art performance on both tasks while being more efficient and more flexible than competing methods. We generalize Riemannian Flow Matching to suit the symmetries inherent to crystals: translation, rotation, permutation, and periodic boundary conditions. Our framework enables the freedom to choose the flow base distributions, drastically simplifying the problem of learning crystal structures compared with diffusion models. In addition to standard benchmarks, we validate FlowMM's generated structures with quantum chemistry calculations, demonstrating that it is about 3x more efficient, in terms of integration steps, at finding stable materials compared to previous open methods.

The crystallization of modeling methods around the Transformer architecture has been a boon for practitioners. Simple, well-motivated architectural variations can transfer across tasks and scale, increasing the impact of modeling research. However, with the emergence of state-of-the-art 100B+ parameters models, large language models are increasingly expensive to accurately design and train. Notably, it can be difficult to evaluate how modeling decisions may impact emergent capabilities, given that these capabilities arise mainly from sheer scale alone. In the process of building BLOOM--the Big Science Large Open-science Open-access Multilingual language model--our goal is to identify an architecture and training setup that makes the best use of our 1,000,000 A100-GPU-hours budget. Specifically, we perform an ablation study at the billion-parameter scale comparing different modeling practices and their impact on zero-shot generalization. In addition, we study the impact of various popular pre-training corpora on zero-shot generalization. We also study the performance of a multilingual model and how it compares to the English-only one. Finally, we consider the scaling behaviour of Transformers to choose the target model size, shape, and training setup. All our models and code are open-sourced at https://huggingface.co/bigscience .

Can a mere next-token predictor faithfully model human intelligence? We crystallize this intuitive concern, which is fragmented in the literature. As a starting point, we argue that the two often-conflated phases of next-token prediction -- autoregressive inference and teacher-forced training -- must be treated distinctly. The popular criticism that errors can compound during autoregressive inference, crucially assumes that teacher-forcing has learned an accurate next-token predictor. This assumption sidesteps a more deep-rooted problem we expose: in certain classes of tasks, teacher-forcing can simply fail to learn an accurate next-token predictor in the first place. We describe a general mechanism of how teacher-forcing can fail, and design a minimal planning task where both the Transformer and the Mamba architecture empirically fail in that manner -- remarkably, despite the task being straightforward to learn. We provide preliminary evidence that this failure can be resolved when training to predict multiple tokens in advance. We hope this finding can ground future debates and inspire explorations beyond the next-token prediction paradigm. We make our code available under https://github.com/gregorbachmann/Next-Token-Failures