Laser spectroscopy of isolated molecules and systems: structure, dynamics and analysis

孤立分子和系统的激光光谱：结构、动力学和分析

• 批准号: 312481-2008
• 负责人: Grant, EdwardR
• 金额: $ 5.61万
• 依托单位: University of British Columbia
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2012
• 资助国家: 加拿大
• 起止时间: 2012-01-01 至 2013-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=514910
• 关键词: Laser; spectroscopy; isolated; molecules; systems

This proposal requests funds to extend and expand a program of NSERC sponsored research in basic and applied molecular spectroscopy. Research in physical chemistry at the interface with molecular physics will use pulsed laser radiation, tuned in multiresonant excitation sequences, to investigate the relaxation dynamics of superexcited small molecules - in isolation and in cold ensembles. Here, we will work spectroscopically to study the coupling of the orbital energy and angular momentum of state-selected extravalent electrons with the rovibrionic degrees of freedom of isolated molecular cations. We will maintain a focus on an important set of energetic, open-shell polyatomic free-radical intermediates with the objective of characterizing excited-state structure and dynamics. By charting rovibronic positions and lineshapes, we will obtain experimental information on electron-cation scattering for comparison with theory. Other experiments will extend further to study the nonadiabatic intermolecular scattering dynamics by which a gas of state-selected high-Rydberg molecules relaxes to form a cold plasma. We have succeeded in establishing conditions under which such a transformation occurs in NO. New work employing spatial and velocity map imaging techniques together with spectroscopic probes in the THz frequency domain will explore multiscale structural and dynamical manifestations of this quantum phase transition. Our research in analytical chemistry will explore novel instrumental and informatics methodologies that facilitate the application of Raman spectroscopy for multivariate materials classification in contexts ranging from industrial process monitoring to molecular biology. Research using dynamic alignment by means of actuated objectives will enable us to devise new mapping and spatial averaging approaches. We will develop and characterize powerful multivariate classification algorithms to enable us to track subtle spectral variations with the aim of isolating targeted signatures in the presence of uncorrelated variance. Information processing will extend to incorporate bright-field optical cues to establish new chemometrically driven smart-scanning modalities.

该提案要求提供资金，以扩展和扩大NSERC赞助的基础和应用分子光谱学研究计划。在与分子物理学的接口物理化学的研究将使用脉冲激光辐射，在多共振激发序列调谐，研究超激发小分子的弛豫动力学-在隔离和冷合奏。 在这里，我们将工作光谱研究的轨道能量和角动量的状态选择的额外的电子与孤立的分子阳离子的rovibrionic自由度的耦合。我们将继续专注于一组重要的充满活力的，开壳层的多原子自由基中间体，其目标是表征激发态结构和动力学。通过绘制振子位置和线型，我们将获得电子-阳离子散射的实验信息，以与理论进行比较。 其他实验将进一步扩展到研究非绝热分子间散射动力学，通过该动力学，气体的状态选择高里德伯分子弛豫形成冷等离子体。我们已经成功地建立了条件下，这种转变发生在NO.新的工作采用空间和速度图成像技术，连同光谱探头在太赫兹频域将探索多尺度结构和动力学表现的量子相变。 我们在分析化学的研究将探索新的仪器和信息学方法，促进应用拉曼光谱的多元材料分类的背景下，从工业过程监测到分子生物学。研究使用动态对齐的驱动目标的手段，将使我们能够设计新的映射和空间平均的方法。我们将开发和表征功能强大的多元分类算法，使我们能够跟踪微妙的光谱变化，目的是在不相关方差的存在下隔离目标特征。信息处理将扩展到包括明场光学线索，以建立新的化学计量驱动的智能扫描模式。