Daily Papers

The coupled cluster calculations with accounting for relativistic effects to study spectroscopic and chemical properties of element 120 (E120) are performed. Similar calculations for Ba are also done and they are in a good agreement with the experimental data. Dissociation energies of diatomic X-H and X-Au molecules, where X=E120, Ba, are calculated; for E120 they are found to be 1.5div2 times smaller than those for Ba.

Accurately modeling chemical reactions at the atomistic level requires high-level electronic structure theory due to the presence of unpaired electrons and the need to properly describe bond breaking and making energetics. Commonly used approaches such as Density Functional Theory (DFT) frequently fail for this task due to deficiencies that are well recognized. However, for high-fidelity approaches, creating large datasets of energies and forces for reactive processes to train machine learning interatomic potentials or force fields is daunting. For example, the use of the unrestricted coupled cluster level of theory has previously been seen as unfeasible due to high computational costs, the lack of analytical gradients in many computational codes, and additional challenges such as constructing suitable basis set corrections for forces. In this work, we develop new methods and workflows to overcome the challenges inherent to automating unrestricted coupled cluster calculations. Using these advancements, we create a dataset of gas-phase reactions containing energies and forces for 3119 different organic molecules configurations calculated at the gold-standard level of unrestricted CCSD(T) (coupled cluster singles doubles and perturbative triples). With this dataset, we provide an analysis of the differences between the density functional and unrestricted CCSD(T) descriptions. We develop a transferable machine learning interatomic potential for gas-phase reactions, trained on unrestricted CCSD(T) data, and demonstrate the advantages of transitioning away from DFT data. Transitioning from training to DFT to training to UCCSD(T) datasets yields an improvement of more than 0.1 eV/Å in force accuracy and over 0.1 eV in activation energy reproduction.

Accurate thermochemical data with sub-chemical accuracy (i.e., within pm1 kcal mol^{-1} from sufficiently accurate experimental or theoretical reference data) is essential for the development and improvement of computational chemistry methods. Challenging thermochemical properties such as heats of formation and total atomization energies (TAEs) are of particular interest because they rigorously test the ability of computational chemistry methods to accurately describe complex chemical transformations involving multiple bond rearrangements. Yet, existing thermochemical datasets that confidently reach this level of accuracy are limited in either size or scope. Datasets with highly accurate reference values include a small number of data points, and larger datasets provide less accurate data or only cover a narrow portion of the chemical space. The existing datasets are therefore insufficient for developing data-driven methods with predictive accuracy over a large chemical space. The Microsoft Research Accurate Chemistry Collection (MSR-ACC) will address this challenge. Here, it offers the MSR-ACC/TAE25 dataset of 76,879 total atomization energies obtained at the CCSD(T)/CBS level via the W1-F12 thermochemical protocol. The dataset is constructed to exhaustively cover chemical space for all elements up to argon by enumerating and sampling chemical graphs, thus avoiding bias towards any particular subspace of the chemical space (such as drug-like, organic, or experimentally observed molecules). With this first dataset in MSR-ACC, we enable data-driven approaches for developing predictive computational chemistry methods with unprecedented accuracy and scope.

Quantum many-body methods provide a systematic route to computing electronic properties of molecules and materials, but high computational costs restrict their use in large-scale applications. Due to the complexity in many-electron wavefunctions, machine learning models capable of capturing fundamental many-body physics remain limited. Here, we present a deep learning framework targeting the many-body Green's function, which unifies predictions of electronic properties in ground and excited states, while offering physical insights into many-electron correlation effects. By learning the GW or coupled-cluster self-energy from mean-field features, our graph neural network achieves competitive performance in predicting one- and two-particle excitations and quantities derivable from one-particle density matrix. We demonstrate its high data efficiency and good transferability across chemical species, system sizes, molecular conformations, and correlation strengths in bond breaking, through multiple molecular and nanomaterial benchmarks. This work opens up opportunities for utilizing machine learning to solve many-electron problems.

Training frontier-scale diffusion models often requires substantial computational resources concentrated in tightly-coupled clusters, limiting participation to well-resourced institutions. While Decentralized Diffusion Models (DDM) enable training multiple experts in isolation, existing approaches require 1176 GPU-days and homogeneous training objectives across all experts. We present an efficient framework that dramatically reduces resource requirements while supporting heterogeneous training objectives. Our approach combines three key contributions: (1) a heterogeneous decentralized training paradigm that allows experts to use different objectives (DDPM and Flow Matching), unified at inference time without any retraining; (2) pretrained checkpoint conversion from ImageNet-DDPM to Flow Matching objectives, accelerating convergence and enabling initialization without objective-specific pretraining; and (3) PixArt-α's efficient AdaLN-Single architecture, reducing parameters while maintaining quality. Experiments on LAION-Aesthetics show that, relative to the training scale reported for prior DDM work, our approach reduces the compute by 16times and data by 14times. Under aligned inference settings, our heterogeneous configuration achieves better FID and higher intra-prompt diversity than the homogeneous baseline. By eliminating synchronization requirements and enabling mixed DDPM/FM objectives, our framework makes decentralized generative model training accessible to contributors with single GPUs requiring only 24--48GB VRAM.

We present the design of a flexible quantum-chemical method development framework, which supports employing any type of basis function. This design has been implemented in the light-weight program package molsturm, yielding a basis-function-independent self-consistent field scheme. Versatile interfaces, making use of open standards like python, mediate the integration of molsturm with existing third-party packages. In this way both rapid extension of the present set of methods for electronic structure calculations as well as adding new basis function types can be readily achieved. This makes molsturm well-suitable for testing novel approaches for discretising the electronic wave function and allows comparing them to existing methods using the same software stack. This is illustrated by two examples, an implementation of coupled-cluster doubles as well as a gradient-free geometry optimisation, where in both cases, an arbitrary basis functions could be used. molsturm is open-source and can be obtained from https://molsturm.org.

The absorption and fluorescence properties in a class of oligothiophene push-pull biomarkers are investigated with a long-range-corrected (LC) density functional method. Using linear response time-dependent density functional theory (TDDFT), we calculate excitation energies, fluorescence energies, oscillator strengths, and excited-state dipole moments. To benchmark and assess the quality of the LC-TDDFT formalism, an extensive comparison is made between LC-BLYP excitation energies and approximate coupled cluster singles and doubles (CC2) calculations. When using a properly-optimized value of the range parameter, "mu", we find that the LC technique provides an accurate description of charge-transfer excitations as a function of biomarker size and chemical functionalization. In contrast, we find that re-optimizing the fraction of Hartree Fock exchange in conventional hybrid functionals still yields an inconsistent description of excitation energies and oscillator strengths for the two lowest excited states in our series of biomarkers. The results of the present study emphasize the importance of a distance-dependent contribution of exchange in TDDFT for investigating excited-state properties.

We introduce the generative quantum eigensolver (GQE), a new quantum computational framework that operates outside the variational quantum algorithm paradigm by applying classical generative models to quantum simulation. The GQE algorithm optimizes a classical generative model to produce quantum circuits with desired properties. Here, we develop a transformer-based implementation, which we name the generative pre-trained transformer-based (GPT) quantum eigensolver (GPT-QE). We show a proof-of-concept of training and pretraining of GPT-QE applied to electronic structure Hamiltonians, and demonstrate its ability illustrated by surpassing coupled cluster singles and doubles (CCSD) for the strong bond dissociation of the nitrogen molecule and approaching chemical accuracy. We also demonstrate the method on real quantum hardware.

Prefill-decode (PD) disaggregation has become the standard architecture for large-scale LLM serving, but in practice its deployment boundary is still determined by KVCache transfer. In conventional dense-attention models, prefill generates huge KVCache traffics that keep prefill and decode tightly coupled within a single high-bandwidth network domain, limiting heterogeneous deployment and resource elasticity. Recent hybrid-attention architectures substantially reduce KVCache size, making cross-cluster KVCache transport increasingly plausible. However, smaller KVCache alone does not make heterogeneous cross-datacenter PD serving practical: real workloads remain bursty, request lengths are highly skewed, prefix caches are unevenly distributed, and inter-cluster bandwidth fluctuates. A naive design that fully externalizes prefill can therefore still suffer from congestion, unstable queueing, and poor utilization. We present Prefill-as-a-Service (PrfaaS), a cross-datacenter serving architecture that selectively offloads long-context prefill to standalone, compute-dense prefill clusters and transfers the resulting KVCache over commodity Ethernet to local PD clusters for decode. Rather than treating reduced KVCache as sufficient, PrfaaS combines model-side KV efficiency with system-side selective offloading, bandwidth-aware scheduling, and cache-aware request placement. This design removes the requirement that heterogeneous accelerators share the same low-latency RDMA fabric, enabling independent scaling of prefill and decode capacity across loosely coupled clusters. In a case study using an internal 1T-parameter hybrid model, a PrfaaS-augmented heterogeneous deployment achieves 54% higher serving throughput and 64% lower P90 TTFT than a homogeneous PD baseline, with approximately 15% throughput gain at equal cost, while consuming only modest cross-datacenter bandwidth.

Near-sensor data analytics is a promising direction for IoT endpoints, as it minimizes energy spent on communication and reduces network load - but it also poses security concerns, as valuable data is stored or sent over the network at various stages of the analytics pipeline. Using encryption to protect sensitive data at the boundary of the on-chip analytics engine is a way to address data security issues. To cope with the combined workload of analytics and encryption in a tight power envelope, we propose Fulmine, a System-on-Chip based on a tightly-coupled multi-core cluster augmented with specialized blocks for compute-intensive data processing and encryption functions, supporting software programmability for regular computing tasks. The Fulmine SoC, fabricated in 65nm technology, consumes less than 20mW on average at 0.8V achieving an efficiency of up to 70pJ/B in encryption, 50pJ/px in convolution, or up to 25MIPS/mW in software. As a strong argument for real-life flexible application of our platform, we show experimental results for three secure analytics use cases: secure autonomous aerial surveillance with a state-of-the-art deep CNN consuming 3.16pJ per equivalent RISC op; local CNN-based face detection with secured remote recognition in 5.74pJ/op; and seizure detection with encrypted data collection from EEG within 12.7pJ/op.

Outliers have emerged as a fundamental bottleneck in preserving accuracy for low-precision large models, particularly within Mixture-of-Experts (MoE) architectures that are increasingly central to large-scale language modeling. Under post-training quantization (PTQ), these outliers induce substantial quantization errors, leading to severe accuracy degradation. While recent rotation-based smoothing techniques alleviate the problem by redistributing outlier magnitudes, residual errors remain and continue to impede reliable low-precision deployment. In this work, we tackle this challenge by introducing CodeQuant, a unified quantization-and-clustering scheme that contains smoothing activation outliers via learnable rotation and absorbing weight outliers into fine-tuned cluster centroids for MoE. This design reduces the influence of extreme values by fitting them within cluster centroids, thereby lowering quantization error while maintaining expressive capacity. Coupled with a dedicated kernel design for GPU and CPU, CodeQuant achieves up to 4.15times speedup while delivering significantly higher accuracy than state-of-the-art quantization approaches across diverse MoE models. Our results highlight CodeQuant as a promising direction for efficient and accurate deployment of MoE-based large language models under low-precision constraints. Our code is available at https://github.com/SAI-Lab-NYU/CodeQuant.

Learning primitive (i.e., attribute and object) concepts from seen compositions is the primary challenge of Compositional Zero-Shot Learning (CZSL). Existing CZSL solutions typically rely on oversimplified data assumptions, e.g., modeling each primitive with a single centroid primitive representation, ignoring the natural diversities of the attribute (resp. object) when coupled with different objects (resp. attribute). In this work, we develop ClusPro, a robust clustering-based prototype mining framework for CZSL that defines the conceptual boundaries of primitives through a set of diversified prototypes. Specifically, ClusPro conducts within-primitive clustering on the embedding space for automatically discovering and dynamically updating prototypes. These representative prototypes are subsequently used to repaint a well-structured and independent primitive embedding space, ensuring intra-primitive separation and inter-primitive decorrelation through prototype-based contrastive learning and decorrelation learning. Moreover, ClusPro efficiently performs prototype clustering in a non-parametric fashion without the introduction of additional learnable parameters or computational budget during testing. Experiments on three benchmarks demonstrate ClusPro outperforms various top-leading CZSL solutions under both closed-world and open-world settings.

Spectrum of ^7Li and elastic scattering reaction ^4He(^3H, ^3H)^4He are studied using the unified description of the Gamow shell model in the coupled-channel formulation (GSMCC). The reaction channels are constructed using the cluster expansion with the two mass partitions [^4He + ^3H], [^6Li + n].

The rapid growth of large language models (LLMs) has outpaced the evolution of single-GPU hardware, making model scale increasingly constrained by memory capacity rather than computation. While modern training systems extend GPU memory through distributed parallelism and offloading across CPU and storage tiers, they fundamentally retain a GPU-centric execution paradigm in which GPUs host persistent model replicas and full autograd graphs. As a result, scaling large models remains tightly coupled to multi-GPU clusters, complex distributed runtimes, and unpredictable host memory consumption, creating substantial barriers for node-scale post-training workloads such as instruction tuning, alignment, and domain adaptation. We present Horizon-LM, a memory-centric training system that redefines the roles of CPU and GPU for large-model optimization. Horizon-LM treats host memory as the authoritative parameter store and uses GPUs solely as transient compute engines through a CPU-master, GPU-template execution model. By eliminating persistent GPU-resident modules and autograd graphs, employing explicit recomputation with manual gradient propagation, and introducing a pipelined double-buffered execution engine, Horizon-LM decouples model scale from GPU count and bounds memory usage to the theoretical parameter footprint. On a single H200 GPU with 1.5\,TB host RAM, Horizon-LM reliably trains models up to 120B parameters. On a standard single A100 machine, Horizon-LM achieves up to 12.2times higher training throughput than DeepSpeed ZeRO-3 with CPU offloading while preserving numerical correctness. Across platforms and scales, Horizon-LM sustains high device utilization and predictable memory growth, demonstrating that host memory, not GPU memory, defines the true feasibility boundary for node-scale large-model training.

We present Chimera, a flexible and scalable Microcontroller Unit (MCU) designed to accelerate real-time inference of rapidly evolving transformer-based models at the ultra-low-power edge (hundred of mW). The chip, implemented in 22 nm FDX technology, integrates a transformer accelerator tightly coupled within a compute cluster featuring nine general-purpose RV32IMA cores. Scalability extends to the memory hierarchy through a novel L2 memory island subsystem, which enables data sharing across multiple clusters while delivering 563 Gb/s aggregate bandwidth. The L2 subsystem enforces quality-of-service guarantees for latency-critical traffic, achieving up to 16x latency reduction. Chimera achieves peak energy and area efficiencies of 3.1 TOPS/W and 281 GOPS/mm2, demonstrating 1.37x higher energy efficiency and up to 100x higher area efficiency compared to State of the Art (SoA) SoCs. Compared to SoA standalone accelerators, Chimera achieves comparable energy efficiency and up to 1.8x higher area efficiency.

Inverse Reinforcement Learning (IRL) seeks to infer reward functions from expert demonstrations. When demonstrations originate from multiple experts with different intentions, the problem is known as Multi-Intention IRL (MI-IRL). Recent deep generative MI-IRL approaches couple behavior clustering and reward learning, but typically require prior knowledge of the number of true behavioral modes K^*. This reliance on expert knowledge limits their adaptability to new behaviors, and only enables analysis related to the learned rewards, and not across the behavior modes used to train them. We propose Contrastive Multi-Intention IRL (CoMI-IRL), a transformer-based unsupervised framework that decouples behavior representation and clustering from downstream reward learning. Our experiments show that CoMI-IRL outperforms existing approaches without a priori knowledge of K^* or labels, while allowing for visual interpretation of behavior relationships and adaptation to unseen behavior without full retraining.

Document clustering and topic modeling are two closely related tasks which can mutually benefit each other. Topic modeling can project documents into a topic space which facilitates effective document clustering. Cluster labels discovered by document clustering can be incorporated into topic models to extract local topics specific to each cluster and global topics shared by all clusters. In this paper, we propose a multi-grain clustering topic model (MGCTM) which integrates document clustering and topic modeling into a unified framework and jointly performs the two tasks to achieve the overall best performance. Our model tightly couples two components: a mixture component used for discovering latent groups in document collection and a topic model component used for mining multi-grain topics including local topics specific to each cluster and global topics shared across clusters.We employ variational inference to approximate the posterior of hidden variables and learn model parameters. Experiments on two datasets demonstrate the effectiveness of our model.

In real-world scenarios, a text classification task often begins with a cold start, when labeled data is scarce. In such cases, the common practice of fine-tuning pre-trained models, such as BERT, for a target classification task, is prone to produce poor performance. We suggest a method to boost the performance of such models by adding an intermediate unsupervised classification task, between the pre-training and fine-tuning phases. As such an intermediate task, we perform clustering and train the pre-trained model on predicting the cluster labels. We test this hypothesis on various data sets, and show that this additional classification phase can significantly improve performance, mainly for topical classification tasks, when the number of labeled instances available for fine-tuning is only a couple of dozen to a few hundred.

A complex system with cluttered observations may be a coupled mixture of multiple simple sub-systems corresponding to latent entities. Such sub-systems may hold distinct dynamics in the continuous-time domain; therein, complicated interactions between sub-systems also evolve over time. This setting is fairly common in the real world but has been less considered. In this paper, we propose a sequential learning approach under this setting by decoupling a complex system for handling irregularly sampled and cluttered sequential observations. Such decoupling brings about not only subsystems describing the dynamics of each latent entity but also a meta-system capturing the interaction between entities over time. Specifically, we argue that the meta-system evolving within a simplex is governed by projected differential equations (ProjDEs). We further analyze and provide neural-friendly projection operators in the context of Bregman divergence. Experimental results on synthetic and real-world datasets show the advantages of our approach when facing complex and cluttered sequential data compared to the state-of-the-art.