Detecting the chemical limits of the Universe with microwave and synchrotron infrared spectroscopy

该提案概述了一种独特的综合方法，以探索从台式到远程天文物体的宇宙化学复杂性的极限。作为化学家，我们接受的训练是识别模式，并将我们的知识外推到新的化合物上，但我们理所当然地认为，我们的首选模型在很大程度上受到元素周期表顶部元素之间的键合图的影响。通过我们的研究，我们寻求通过开发涉及较大元素的结构和键合的稳健预测模型来解决这一缺陷。在接下来的五年里，我的团队将为此奠定基础，使用我们的现代实验和计算工具，以前所未有的细节描述第15和16组中碳和更重的p块元素之间的相互作用。我们的研究的动机是迫切需要利用独特的结构图案和物理性质，以创造下一代催化和光电子学的主基团材料。主题1研究了稳定型有机氧原和磷的势能面控制因素。主题2探索在无碰撞射流中冻结的短寿命中间体中的新键基序（连通性，键序，结构），主题3将这些研究扩展到高活性气体混合物。许多目标化合物的灵感来自最近添加到天文学目录中的分子，并揭示了我们宇宙在极端环境下的化学演化。近年来，随着新的天文探测的步伐加快，对精确光谱数据的需求激增，以支持新的发现。van Wijngaarden团队拥有解决这一迫切需求的工具和专业知识。我们的综合研究设计利用了现代计算和光谱工具在微波（MW）和远红外（FIR）区域之间的协同作用。这使我们能够以极高的准确度和精度探测不断变化的化学环境，以阐明平衡分子结构和反应性的因素。我们独特的设置包括最先进的，定制的MW光谱仪，以解开丰富构象和反应混合物的旋转特征。这种方法的一个核心特点是，它稳定了超冷射流中的瞬态物质，使我们能够对化学物质进行高分辨率的光谱快照，而这些光谱快照在实验台上是无法分离的。这些研究指导我们在加拿大最大的国家科学设施加拿大光源（CLS）同步加速器上对短寿命分子的FIR振动指纹进行调查，使用由我的团队设计和建造的定制设置来模拟恶劣的反应条件。通过对该项目有影响力的研究贡献，学员将在仪器设计和计算建模方面发展先进的专业知识，与从材料科学到天文学等不同领域的研究人员进行互动，并准备好引领未来的全球科学探索。

This proposal outlines a unique integrative approach to exploring the limits of chemical complexity of the Universe from the benchtop to remote astronomical objects. As chemists, we are trained to recognize patterns and extrapolate our knowledge to new compounds, but we take for granted that our go-to models are heavily influenced by our picture of bonding between elements near the top of the periodic table. Through our research, we seek to address this deficiency by developing robust, predictive models for structure and bonding involving larger elements. In the next five years, my group will lay the foundation for this using our suite of modern experimental and computational tools to describe, with unprecedented detail, the interactions between carbon and heavier p-block elements in groups 15 and 16. Our research is motivated by a pressing need to harness unique structural motifs and physical properties in order to create next generation main group materials for catalysis and optoelectronics. Theme 1 investigates the factors controlling the potential energy surfaces of stable organochalcogens and phosphanes. Theme 2 explores novel bonding motifs (connectivity, bond order, structure) in short-lived intermediates frozen in collision-free jets and Theme 3 expands these studies to highly reactive gas mixtures. Many of the targeted compounds are inspired by molecules recently added to astronomy catalogs and shed light on the chemical evolution of our Universe in extreme environments. As the pace of new astronomical detections has accelerated in recent years, the demand for accurate spectroscopic data to support new discoveries has exploded. The van Wijngaarden group has the tools and expertise to address this urgent need. Our integrative research design exploits the synergy between modern computational and spectroscopic tools in the microwave (MW) and far infrared (FIR) regions. This allows us to probe changing chemical environments with exceptional accuracy and precision to elucidate the factors that balance molecular structure and reactivity. Our unique setup involves state-of-the-art, custom-built MW spectrometers to unravel rotational signatures from rich conformational and reaction mixtures. A central feature of this approach is that it stabilizes transient species in ultracold jets allowing us to take high resolution spectral snapshots of chemistry that cannot be isolated on the benchtop. These studies guide our investigation of FIR vibrational fingerprints of short-lived molecules at the Canadian Light Source (CLS) synchrotron, Canada's largest national science facility, using a custom setup designed and built by my team to mimic harsh reaction conditions. Through impactful research contributions to this program, trainees will develop advanced expertise in instrument design and computational modelling, interact with researchers in diverse fields from materials science to astronomy, and be poised to lead future global scientific quests.