arXiv:2510.20615cs.LG2025-10NeurIPS被引 11

用统一模型同时处理质谱和分子结构,提升未知物解析准确率。

MS-BART: Unified Modeling of Mass Spectra and Molecules for Structure Elucidation

  • 将质谱与分子结构映射到同一词表,实现跨模态预训练。
  • 在5个关键指标上达当前最优,速度比扩散模型快10倍。
  • 引入化学反馈机制,减少分子生成中的错误偏差,适合科研人员使用。

质谱在分子鉴定中至关重要,但基于质谱数据的结构解析仍因标注谱图稀缺而困难。尽管大规模预训练在其他领域有效缓解数据不足问题,但在质谱领域受限于原始信号的复杂性和异质性。为此,我们提出MS-BART,一种统一建模框架,将质谱与分子结构映射至共享词表,通过在可靠计算的指纹-分子数据集上进行大规模预训练,实现跨模态学习。多任务预训练目标联合优化去噪与翻译任务,增强模型泛化能力。预训练模型通过在MIST(一个预训练的谱图推断模型)生成的指纹预测上微调,以适应真实谱图的变异性。尽管微调缓解了分布差异,MS-BART仍存在分子幻觉问题,需进一步对齐。因此,我们引入化学反馈机制,引导模型生成更接近参考结构的分子。大量评估表明,MS-BART在MassSpecGym和NPLIB1的5/12个关键指标上达到当前最优性能,且比竞争的扩散方法快一个数量级;全面的消融实验系统验证了模型的有效性与鲁棒性。

原文摘要 · Abstract (English)

Mass spectrometry (MS) plays a critical role in molecular identification, significantly advancing scientific discovery. However, structure elucidation from MS data remains challenging due to the scarcity of annotated spectra. While large-scale pretraining has proven effective in addressing data scarcity in other domains, applying this paradigm to mass spectrometry is hindered by the complexity and heterogeneity of raw spectral signals. To address this, we propose MS-BART, a unified modeling framework that maps mass spectra and molecular structures into a shared token vocabulary, enabling cross-modal learning through large-scale pretraining on reliably computed fingerprint-molecule datasets. Multi-task pretraining objectives further enhance MS-BART's generalization by jointly optimizing denoising and translation task. The pretrained model is subsequently transferred to experimental spectra through finetuning on fingerprint predictions generated with MIST, a pre-trained spectral inference model, thereby enhancing robustness to real-world spectral variability. While finetuning alleviates the distributional difference, MS-BART still suffers molecular hallucination and requires further alignment. We therefore introduce a chemical feedback mechanism that guides the model toward generating molecules closer to the reference structure. Extensive evaluations demonstrate that MS-BART achieves SOTA performance across 5/12 key metrics on MassSpecGym and NPLIB1 and is faster by one order of magnitude than competing diffusion-based methods, while comprehensive ablation studies systematically validate the model's effectiveness and robustness.

质谱分析分子生成跨模态学习

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