乙醇—水团簇分子的光谱学特征及分子结构研究
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摘要
本文采用荧光光谱分析技术，结合量子力学和量子化学理论对乙醇—水溶液中的团簇分子结构进行了研究。在讨论了乙醇—水溶液中新分子的空间取向特征、平面结构特点以及电子能级变化规律的基础上，得到了该分子结构的物理模型和空间结构信息，进而反演了团簇分子的结构。
通过对乙醇—水溶液荧光光谱特征的实验研究，得到了乙醇—水团簇分子的三种可能类型，并从荧光量子产率和光吸收度等方面对三种可能的分子结构进行了理论研究。从数学上推导了乙醇和水形成配合物的结合常数，推断配合物分子的可能结构为：5个乙醇分子和6个水分子间通过氢键相连形成环式或链式结构；一个乙醇分子和两个水分子间隔相连形成的团簇结构；或一个乙醇分子和5个水分子相互连接形成新分子结构。
通过对乙醇—水溶液偏振荧光光谱的检测，计算了该荧光的偏振度和分子各向异性度，表征了分子的空间取向行为，认为乙醇—水溶液中的团簇分子是在较大程度上具有固定取向的有序结构。理论分析认为氢键不仅对分子团簇的空间结构产生影响，而且对分子中的电子轨道也产生了影响，表现为分子的偶极矩和极性(偏振)特性的变化。
通过对长波方向上宽展谱峰的实验和理论研究，得到了处于基态和激发态的团簇分子间形成激基缔合物的结论。在求解荧光强度随时间衰变过程方程的基础上，从理论上分析了形成激基缔合物的光物理过程。利用密度泛函理论计算了乙醇—水团簇分子电子跃迁的理论值。利用碰撞复合物和激基缔合物的形成机制研究了团簇分子基态能级发生改变的过程，进而对溶液的发光机制进行了定量研究。
利用量子化学、量子力学并结合含时密度泛函理论反演了乙醇—水团簇分子的结构：多个乙醇和水分子在溶液中由氢键相连形成了环式或链式结构，且具有镶嵌型的平面结构特点和高度有序的空间结构特征。
本文的研究结果可为分子间团簇结构的研究，以及乙醇分子与生物组织相互作用的研究提供理论和实验依据。
Based on the experimental results of the fluorescence spectrum, the molecularstructure of ethanol-water clusters have been studied by using the theories of quantummechanics and quantum chemistry. The physical model and the structure information of thecluster molecules have been presented and concluded after a detailed discussion on thespatial orientation character, the planar structure feature as well as the change rule ofenergy levels. Furthermore, the cluster molecular structures have been inversed.
From the experimental results of fluorescence spectral characteristic of ethanol-watersolutions with different concentrations, a further theoretical study on the quantum yield andlight absorbency give the results of the bonding number n to form MR_n clusters ofethanol and water molecules. It is concluded that there are three possible cluster structures:five ethanol molecules and six water molecules connect with each other to form a ring orchain structures through the hydrogen bond, an ethanol molecule and two water moleculesform the chain structure with hydrogen bond, and an ethanol molecule and five watermolecules link mutually to form a new molecular structure.
Based on the polarized fluorescence spectrum of ethanol-water solution, thepolarization degree and molecular anisotropy have been calculated and the molecularspatial orientation behavior has been characterized as well. As a result, it was consideredthat the cluster molecule in the solution has an ordered structure with a fixed orientation toa large extent. The theoretical analysis reveals that the hydrogen bond not only influencesthe spatial structure of cluster, but also affects the molecular energy levels, representing bythe change in the molecular dipole moment and the polarity.
It is concluded that the clusters form the excimer by the excited state molecules andthe ground state molecules based on a broad and featureless fluorescent spectrum at longStokes shift. By solving decay process of the fluorescence intensity, the possiblephotophysical process of the excimer formation was analyzed theoretically. Furthermore,all the ground and excited energy levels of water molecule, ethanol molecules and theclusters were calculated by density functional theory (DFT) and the theoretical electrontransition value of the cluster was obtained accordingly. The change process of the energylevels and the luminescence mechanism of the solution have been presented by studying the formation mechanism of the excimer and the collision compound of two clusters in theground state.
The structure of ethanol-water cluster molecule was inversed using the quantumchemistry, the quantum mechanics and the time dependent density functional theory(TDDFT). The conclusion is that several ethanol molecules and water molecules haveconnected into ring or chain structure through hydrogen bonds, with inlaid planar structurecharacteristic and a spatial structure characteristic with high degree of order.
The research consequences may offer a theoretical and experimental reference tostudy the intermolecular cluster structure, as well as the interaction between ethanolmolecule and biological tissue.
通过对乙醇—水溶液荧光光谱特征的实验研究，得到了乙醇—水团簇分子的三种可能类型，并从荧光量子产率和光吸收度等方面对三种可能的分子结构进行了理论研究。从数学上推导了乙醇和水形成配合物的结合常数，推断配合物分子的可能结构为：5个乙醇分子和6个水分子间通过氢键相连形成环式或链式结构；一个乙醇分子和两个水分子间隔相连形成的团簇结构；或一个乙醇分子和5个水分子相互连接形成新分子结构。
通过对乙醇—水溶液偏振荧光光谱的检测，计算了该荧光的偏振度和分子各向异性度，表征了分子的空间取向行为，认为乙醇—水溶液中的团簇分子是在较大程度上具有固定取向的有序结构。理论分析认为氢键不仅对分子团簇的空间结构产生影响，而且对分子中的电子轨道也产生了影响，表现为分子的偶极矩和极性(偏振)特性的变化。
通过对长波方向上宽展谱峰的实验和理论研究，得到了处于基态和激发态的团簇分子间形成激基缔合物的结论。在求解荧光强度随时间衰变过程方程的基础上，从理论上分析了形成激基缔合物的光物理过程。利用密度泛函理论计算了乙醇—水团簇分子电子跃迁的理论值。利用碰撞复合物和激基缔合物的形成机制研究了团簇分子基态能级发生改变的过程，进而对溶液的发光机制进行了定量研究。
利用量子化学、量子力学并结合含时密度泛函理论反演了乙醇—水团簇分子的结构：多个乙醇和水分子在溶液中由氢键相连形成了环式或链式结构，且具有镶嵌型的平面结构特点和高度有序的空间结构特征。
本文的研究结果可为分子间团簇结构的研究，以及乙醇分子与生物组织相互作用的研究提供理论和实验依据。
Based on the experimental results of the fluorescence spectrum, the molecularstructure of ethanol-water clusters have been studied by using the theories of quantummechanics and quantum chemistry. The physical model and the structure information of thecluster molecules have been presented and concluded after a detailed discussion on thespatial orientation character, the planar structure feature as well as the change rule ofenergy levels. Furthermore, the cluster molecular structures have been inversed.
From the experimental results of fluorescence spectral characteristic of ethanol-watersolutions with different concentrations, a further theoretical study on the quantum yield andlight absorbency give the results of the bonding number n to form MR_n clusters ofethanol and water molecules. It is concluded that there are three possible cluster structures:five ethanol molecules and six water molecules connect with each other to form a ring orchain structures through the hydrogen bond, an ethanol molecule and two water moleculesform the chain structure with hydrogen bond, and an ethanol molecule and five watermolecules link mutually to form a new molecular structure.
Based on the polarized fluorescence spectrum of ethanol-water solution, thepolarization degree and molecular anisotropy have been calculated and the molecularspatial orientation behavior has been characterized as well. As a result, it was consideredthat the cluster molecule in the solution has an ordered structure with a fixed orientation toa large extent. The theoretical analysis reveals that the hydrogen bond not only influencesthe spatial structure of cluster, but also affects the molecular energy levels, representing bythe change in the molecular dipole moment and the polarity.
It is concluded that the clusters form the excimer by the excited state molecules andthe ground state molecules based on a broad and featureless fluorescent spectrum at longStokes shift. By solving decay process of the fluorescence intensity, the possiblephotophysical process of the excimer formation was analyzed theoretically. Furthermore,all the ground and excited energy levels of water molecule, ethanol molecules and theclusters were calculated by density functional theory (DFT) and the theoretical electrontransition value of the cluster was obtained accordingly. The change process of the energylevels and the luminescence mechanism of the solution have been presented by studying the formation mechanism of the excimer and the collision compound of two clusters in theground state.
The structure of ethanol-water cluster molecule was inversed using the quantumchemistry, the quantum mechanics and the time dependent density functional theory(TDDFT). The conclusion is that several ethanol molecules and water molecules haveconnected into ring or chain structure through hydrogen bonds, with inlaid planar structurecharacteristic and a spatial structure characteristic with high degree of order.
The research consequences may offer a theoretical and experimental reference tostudy the intermolecular cluster structure, as well as the interaction between ethanolmolecule and biological tissue.
引文
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