Understanding Chemical Complexity and Diversity Through Collaboration and Integration

项目名称：“通过整合和协作了解化学的复杂性和多样性”项目编号：CHE-07-17518原理研究员：哥伦比亚大学Nicholas J.Turro摘要拟议的研究是基于这样一个假设，即分子化学的结构-反应相关性原理(基于组成分子的原子之间的分子内键的范例)可以通过整合领域的基本概念和涉及PI的实验室和国内和国际合作者小组的合作成功地扩展到超分子化学(基于分子间键的范例)。除了作为分子和超分子化学基础的电子相互作用外，分子还具有与电子自旋和核自旋相关的磁性。电子自旋取向的变化速度可以控制电子激发态和自由基物种的反应。核自旋取向的变化是核磁共振波谱研究的基础。拟议的研究将调查电子自旋对控制与化学合成相关的化学过程的能力，以及核自旋对控制与磁共振成像(MRI)相关的核磁共振光谱特征的能力。具体的例子包括(1)研究富勒烯、C60分子中包含的氢分子(H2)的核自旋取向的变化；以及(2)在涉及活细胞中的信使核糖核酸靶标的发光分子探针的系统中，研究电子自旋取向的变化以确定能量转移的速度。除了这些研究外，拟议的研究还将探索(3)通过选择性聚合和偶联反应结合聚合物网络的光化学裂解来合成新型聚合物网络；以及(4)合成具有配体的纳米颗粒，这种配体允许根据纳米颗粒的期望应用而进行一般和普遍的修饰。在更广泛的影响和外展方面，国际和平研究所将(1)继续确定和建立来自学术机构和行业的资深合作者及其学生的跨学科和全球网络；(2)为合作者在哥伦比亚大学提供一个多用户友好的实验室，包括具有发光、电子自旋共振、红外和紫外-可见吸收检测的最先进的稳态和时间分辨激光闪光光解；(3)举办一系列关于通过范式进行科学运作的方式的公开讲座；(4)通过指导本科生、研究生、博士后助理、访问学者和纽约市高中教师，开发人力资源并鼓励代表不足的群体参与。

Project title: "Understanding Chemical Complexity and Diversity Through Integration and Collaborations"Project Number: CHE-07-17518Principle Investigator: Nicholas J. Turro, Columbia UniversityAbstractThe proposed research is based on the hypothesis that the principles of structure-reactivity correlations of molecular chemistry (which is based on the paradigm of intramolecular bonds between the atoms that make up a molecule) can be successfully extended to supramolecular chemistry (which is based on the paradigm of intermolecular bonds between molecules) through the integration of the fundamental concepts of the fields and collaborations involving the PI's laboratory and a national and international group of collaborators. In addition to the electrical interactions between which are the basis for both molecular and supramolecular chemistry, molecules also possess magnetic properties that are related to electron spins and nuclear spins. The rate of change of orientation of electrons spins can control the reactions of electronically excited states and of radical species. The change of the orientation of nuclear spins is the basis of nuclear magnetic resonance spectroscopy. The proposed research will investigate the ability of pairs of electron spins to control chemical processes that are relevant to chemical synthesis and of pairs of nuclear spins to control features of nuclear magnetic resonance spectroscopy that are relevant to magnetic resonance imaging (MRI). Specific examples include (1) the study of the change in nuclear spin orientation of hydrogen molecules (H2) that are contained inside a fullerene, C60 molecule; and (2) the study of the change of electron spin orientation in determining the rate of energy transfer in systems involving luminescent molecular probes of mRNA targets in living cells. In addition to these studies, the proposed research will investigate (3) the synthesis of novel polymer networks by selective polymerization and coupling reactions combined with photochemical cleavage of the polymer networks; and (4) the synthesis of nanoparticles possessing ligands that allow a general and universal modification depending on the desire application of the nanoparticle. In terms of broader impact and outreach, the PI will (1) continue to identify and establish a interdisciplinary and global network of senior collaborators and their students, from academic institutions and industry; (2) provide collaborators with a multi-user-friendly laboratory at Columbia consisting of state of the art steady state and time resolved laser flash photolysis with luminescence, ESR, IR and UV-VIS absorption detection; (3) present a series of public lectures on the way science operates through paradigms; (4) develop human resources and encouragement of the participation of underrepresented groups through his mentoring of undergraduates, graduate students, postdoctoral associates, visiting scholars and New York City high school teachers.