Daily Papers

Rigorous performance evaluation is essential for developing robust algorithms for high-throughput computational chemistry. Traditional benchmarking, however, often struggles to account for system-specific variability, making it difficult to form actionable conclusions. We present a Bayesian hierarchical modeling framework that rigorously quantifies performance metrics and their uncertainty, enabling a nuanced comparison of algorithmic strategies. We apply this framework to analyze the Dimer method, comparing Conjugate Gradient (CG) and L-BFGS rotation optimizers, with and without the removal of external rotations, across a benchmark of 500 molecular systems. Our analysis confirms that CG offers higher overall robustness than L-BFGS in this context. While the theoretically-motivated removal of external rotations led to higher computational cost (>40% more energy and force calls) for most systems in this set, our models also reveal a subtle interplay, hinting that this feature may improve the reliability of the L-BFGS optimizer. Rather than identifying a single superior method, our findings support the design of adaptive "chain of methods" workflows. This work showcases how a robust statistical paradigm can move beyond simple performance rankings to inform the intelligent, context-dependent application of computational chemistry methods.

The task of locating first order saddle points on high-dimensional surfaces describing the variation of energy as a function of atomic coordinates is an essential step for identifying the mechanism and estimating the rate of thermally activated events within the harmonic approximation of transition state theory. When combined directly with electronic structure calculations, the number of energy and atomic force evaluations needed for convergence is a primary issue. Here, we describe an efficient implementation of Gaussian process regression (GPR) acceleration of the minimum mode following method where a dimer is used to estimate the lowest eigenmode of the Hessian. A surrogate energy surface is constructed and updated after each electronic structure calculation. The method is applied to a test set of 500 molecular reactions previously generated by Hermez and coworkers [J. Chem. Theory Comput. 18, 6974 (2022)]. An order of magnitude reduction in the number of electronic structure calculations needed to reach the saddle point configurations is obtained by using the GPR compared to the dimer method. Despite the wide range in stiffness of the molecular degrees of freedom, the calculations are carried out using Cartesian coordinates and are found to require similar number of electronic structure calculations as an elaborate internal coordinate method implemented in the Sella software package. The present implementation of the GPR surrogate model in C++ is efficient enough for the wall time of the saddle point searches to be reduced in 3 out of 4 cases even though the calculations are carried out at a low Hartree-Fock level.

With the advent of large-scale 3D datasets, feed-forward 3D generative models, such as the Large Reconstruction Model (LRM), have gained significant attention and achieved remarkable success. However, we observe that RGB images often lead to conflicting training objectives and lack the necessary clarity for geometry reconstruction. In this paper, we revisit the inductive biases associated with mesh reconstruction and introduce DiMeR, a novel disentangled dual-stream feed-forward model for sparse-view mesh reconstruction. The key idea is to disentangle both the input and framework into geometry and texture parts, thereby reducing the training difficulty for each part according to the Principle of Occam's Razor. Given that normal maps are strictly consistent with geometry and accurately capture surface variations, we utilize normal maps as exclusive input for the geometry branch to reduce the complexity between the network's input and output. Moreover, we improve the mesh extraction algorithm to introduce 3D ground truth supervision. As for texture branch, we use RGB images as input to obtain the textured mesh. Overall, DiMeR demonstrates robust capabilities across various tasks, including sparse-view reconstruction, single-image-to-3D, and text-to-3D. Numerous experiments show that DiMeR significantly outperforms previous methods, achieving over 30% improvement in Chamfer Distance on the GSO and OmniObject3D dataset.

Dynamic Music Emotion Recognition (DMER) aims to predict the emotion of different moments in music, playing a crucial role in music information retrieval. The existing DMER methods struggle to capture long-term dependencies when dealing with sequence data, which limits their performance. Furthermore, these methods often overlook the influence of individual differences on emotion perception, even though everyone has their own personalized emotional perception in the real world. Motivated by these issues, we explore more effective sequence processing methods and introduce the Personalized DMER (PDMER) problem, which requires models to predict emotions that align with personalized perception. Specifically, we propose a Dual-Scale Attention-Based Meta-Learning (DSAML) method. This method fuses features from a dual-scale feature extractor and captures both short and long-term dependencies using a dual-scale attention transformer, improving the performance in traditional DMER. To achieve PDMER, we design a novel task construction strategy that divides tasks by annotators. Samples in a task are annotated by the same annotator, ensuring consistent perception. Leveraging this strategy alongside meta-learning, DSAML can predict personalized perception of emotions with just one personalized annotation sample. Our objective and subjective experiments demonstrate that our method can achieve state-of-the-art performance in both traditional DMER and PDMER.