溶液中类胡萝卜素的结构与光谱性质研究
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摘要
众所周知,多烯类生物分子中的类胡萝卜素是自然界中最丰富的天然色素之一,广泛存在于包括人类在内的生物有机体内,在光合作用、预防人类疾病等方面起重要作用。β-胡萝卜素、番茄红素和角黄素是类胡萝卜素中最受关注和研究最为广泛的三种类胡萝卜素。尤其是β-胡萝卜素在光合作用中有光能采集、转移、淬灭单态氧等功能,番茄红素有预防人类老化和癌症的功能更是生物学、物理学和化学研究的热点之一。
它们是具有共轭双键结构的多烯分子,是研究共振拉曼光谱、光学非线性等分子结构的理想样品,又是实现分子导线等光电器件的重要材料。因此对其研究既有理论价值又有光明应用前景。多烯类分子的性质、功能与其分子结构关系极大,尤其这种链状多烯分子结构有序性与分子的性质、功能密切相关。
本论文采用计算机模拟结合光谱实验以及设计物理模型等方法,多角度多方面研究了多烯类线形生物分子(类胡萝卜素)在溶液中的光谱特性,涉及到计算化学、分子光谱学、溶液化学、生物物理化学等多个学科。值得一提的是,我们在研究拉曼光谱时,引进了一个重要的参量—拉曼散射截面。这是因为在拉曼光谱的研究和应用中,拉曼散射截面是一个重要的参量。正如拉曼频移和线宽一样,表现了分子的微观特性,拉曼散射截面表示了某一特定分子的光散射特性,并直接反映了分子极化率的大小及变化。散射截面不仅和激发光的频率,散射分子的结构有关,还和被散射分子所处的环境有关。
我们从单一溶剂的不同浓度下类胡萝卜素的结构有序对π-电子离域和拉曼散射截面的影响出发,再扩展到不同溶剂中类胡萝卜素的结构有序对π-电子离域和拉曼散射截面的影响。在有机溶剂—类胡萝卜素体系的研究基础上,我们进一步研究了二元水溶液(有机溶剂—水)—类胡萝卜素体系中弱相互作用对类胡萝卜素的结构有序对其光学特性的影响,主要取得了以下创新性成果：
1.在研究一元溶液对类胡萝卜素结构有序影响的研究中,测量不同浓度下类胡萝卜素的紫外—可见光谱和拉曼光谱。尤其是测量极低浓度拉曼光谱,我们采用课题组独立设计的液芯光纤内共振拉曼技术进行测量,获得了低浓度下乃至单分子状态类胡萝卜素分子结构有序性相关的性质、功能信息。我们测量β-胡萝卜素、番茄红素和角黄素等在溶液中拉曼光谱时,发现在10~(-6)—10~(-11)mol/L浓度下拉曼散射截面增加了四个数量级(达2.6×10~(-20)cm~2molecule_(-1)Sr_(-1))比一般分子拉曼散射截面大十个数量级,而且随浓度降低成指数关系增大。其紫外—可见光谱吸收峰型随浓度降低而变窄变陡。根据非线性相干弱阻尼电子—核振动模型,科学地解释了上面得到的实验结果,也为以后的研究中可以继续通过改变其他环境对类胡萝卜素结构与性质影响的研究提供参考资料和依据。
2.改变不同溶剂是研究溶剂效应的一种基本方法。通过变化溶剂可以改变物质的结构以及其物理、化学性质,这是由于分子间的作用使物质内部的分子(原子)距离拉长或缩短,改变相邻电子轨道重叠。测得不同溶剂中角黄素的的紫外—可见光谱和拉曼光谱,并利用密度泛函理(DFT)论优化角黄素分子与溶剂之间形成的三聚体几何结构。通过对实验和理论结果进行分析,了解一些结构与性质之间的关系。利用密度泛函与分子光谱对此类分子微环境测量、微结构测量有潜在的应用前景,同时该方法也为此类研究提供实验依据。
3.正是因为大多数的生物分子都是在水环境中进行其生物活性的,所以我们测量了角黄素在二元水溶液中的拉曼光谱与紫外-可见光谱。由于三元物质之间的相互作用相当复杂,我们首先利用光谱和密度泛函理论联用研究二元水溶液中有机溶剂与水之间的氢键作用。然后,我们对角黄素在二元水溶液中的拉曼光谱与紫外-可见光谱进行分析,建立了二元水溶液与角黄素的相互作用模型并解析了实验结果。这种研究思路与方法有利于深入理解水环境中生物分子结构变化和π—电子离域等的光学特性。同时,研究结果也为进一步研究复杂体系中类胡萝卜素的结构与性质提供了一定的光谱依据。
综上所述,本论文将量子化学理论与拉曼光谱与电子光谱相结合,通过改变溶液浓度和变换溶剂研究类胡萝卜素结构有序对其性质的影响,并提出一个二元水溶液体系的物理模型。这为类胡萝卜素研究提供了一个新思路,也为人们深层次探讨类胡萝卜素的结构与性质问题提供了参考资料。
To our knowledge, carotenoids are one of the most abundant pigments found in nature. They are present in most organisms including humans.Carotenoids play an important role in photosynthesis, protection against various diseases in humans, etc.β-carotene, lycopene and canthaxanthin is the most attention and he most widely studied of the three ones of carotenoids. In particular,β-carotene has two main functions, i.e. photoprotection and photon harvesting in photosynthetic systems. Lycopene has functions defense aging and cancer prevention.
Research on that they has been carried out extensively in physics, chemistry and biology. Carotenoids are the chemically simplyπ-conjugated polyene, is which the polyene chain consists of a sequences of carbon-carbon (CC) bonds (...-C=C-C=...), characterized by a strong electron-phonon (e-ph) coupling due to delocalizedπelectrons. They are the study of resonance Raman spectroscopy, optical nonlinear, the ideal molecular structure of the ideal sample, but also the realization of molecular wires and other important materials for optoelectronic devices. Therefore, the research has theoretical value and a bright application prospect. Carotenoids molecular nature of the great relationship between functional and molecular structures. In particular, this chain of molecular structure is closely related to molecular ordering properties and function.
In the paper, UV-visible spectroscopy, Raman spectroscopy and Quantum computing are combined to investigate carotenoids in solution. It is worth mentioning that we introduce an important parameter-the Raman scattering cross section for analyzing Raman spectroscopy. Raman scattering cross section (RSCS) is an important parameter in the studies and applications of the Raman spectroscopy. It relates not only to the incident frequency and the structure of a scattered molecule but also to the environment where the scattered molecule is located. It is usually obtained bycomparing the Raman intensity of an unknown molecule with that of a standard molecule with known cross section.
1. We study on Effect of the structural order of all-trans-β-carotene on the Raman scattering cross section at low concentrations. Using the technique of liquid-core optical fiber (LCOF), we measured the Raman scattering cross sections (RSCSs) of the carbon-carbon stretching vibrational modes of all-trans--carotene in carbon disulfide (CS_2) at concentrations ranging from 10~(-6) to 10~(-11) M. It was found that the RSCSs of all-trans-β-carotene were extremely high with decreasing concentration, and the absolute RSCS of C=C stretching modes of all-trans-β-carotene reached the value of 2.6×10~(-20) cm~2 molecule_(-1) Sr_(-1) at 8×10~(-11) M, which is larger than at 8×10-6 M by 4 orders of magnitude. A theoretical interpretation of the anomalous experimental results is given, which introduces a qualitative nonlinear model of coherent weakly damped electron-lattice vibrations in structural order of all-trans-β-carotene.
2. Changing solvent is one of the basic research methods of Solvent effect. Solvent has relationship with the total energy of the compressed substance, and the phase structure and reaction way may be controlled by changing solvent because the interatomic distance can be reduced or increased during compression. UV-Visible absorption spectra and Raman spectra of canthaxanthin in different solvents. Our assignments and interpretations are supported by quantum mechanical calculations of structures, which are canthaxanthin/solvents complexes. Through the analysis of experimental and theoretical results, find the relationship between structure and properties. The combination of experimental Raman data with quantum mechanical calculation leads to a better knowledge of the nature of the hydrogen bonding and the structures of the studied hydrogen-bonded complexes. The micro-environmental and micro structures measurements for such molecules of the studied the complexes, while the method is also a powerful tool for such research.
3. It is because of all the biological molecules are in the water environment to carry out its biological activity. Therefore, we measured in binary aqueous solutions of canthaxanthin in the Raman and UV-visible spectroscopy. First of all, because of the complex interaction between the ternary matter, our vibrational spectroscopic analysis on hydrogen-bonding between dimethyl sulfoxide and water comprises both experimental Raman spectra and ab initio calculations on structures of various dimethyl sulfoxide/water clusters with increasing water content.Later, we have established physical model for explaining the experimental results.At last, this method could be used as a suitable tool for investigating the structure and properties of biological molecules in aqueous environment.
In summary, this work realized the combination of quantum mechanical calculation and molecular spectroscopic technique, and established physical model for explaining carotenoids in solution. This is a new technique to investigate carotenoids, and therefore opens a new approach to deeply explore physical and chemical issues.
它们是具有共轭双键结构的多烯分子,是研究共振拉曼光谱、光学非线性等分子结构的理想样品,又是实现分子导线等光电器件的重要材料。因此对其研究既有理论价值又有光明应用前景。多烯类分子的性质、功能与其分子结构关系极大,尤其这种链状多烯分子结构有序性与分子的性质、功能密切相关。
本论文采用计算机模拟结合光谱实验以及设计物理模型等方法,多角度多方面研究了多烯类线形生物分子(类胡萝卜素)在溶液中的光谱特性,涉及到计算化学、分子光谱学、溶液化学、生物物理化学等多个学科。值得一提的是,我们在研究拉曼光谱时,引进了一个重要的参量—拉曼散射截面。这是因为在拉曼光谱的研究和应用中,拉曼散射截面是一个重要的参量。正如拉曼频移和线宽一样,表现了分子的微观特性,拉曼散射截面表示了某一特定分子的光散射特性,并直接反映了分子极化率的大小及变化。散射截面不仅和激发光的频率,散射分子的结构有关,还和被散射分子所处的环境有关。
我们从单一溶剂的不同浓度下类胡萝卜素的结构有序对π-电子离域和拉曼散射截面的影响出发,再扩展到不同溶剂中类胡萝卜素的结构有序对π-电子离域和拉曼散射截面的影响。在有机溶剂—类胡萝卜素体系的研究基础上,我们进一步研究了二元水溶液(有机溶剂—水)—类胡萝卜素体系中弱相互作用对类胡萝卜素的结构有序对其光学特性的影响,主要取得了以下创新性成果：
1.在研究一元溶液对类胡萝卜素结构有序影响的研究中,测量不同浓度下类胡萝卜素的紫外—可见光谱和拉曼光谱。尤其是测量极低浓度拉曼光谱,我们采用课题组独立设计的液芯光纤内共振拉曼技术进行测量,获得了低浓度下乃至单分子状态类胡萝卜素分子结构有序性相关的性质、功能信息。我们测量β-胡萝卜素、番茄红素和角黄素等在溶液中拉曼光谱时,发现在10~(-6)—10~(-11)mol/L浓度下拉曼散射截面增加了四个数量级(达2.6×10~(-20)cm~2molecule_(-1)Sr_(-1))比一般分子拉曼散射截面大十个数量级,而且随浓度降低成指数关系增大。其紫外—可见光谱吸收峰型随浓度降低而变窄变陡。根据非线性相干弱阻尼电子—核振动模型,科学地解释了上面得到的实验结果,也为以后的研究中可以继续通过改变其他环境对类胡萝卜素结构与性质影响的研究提供参考资料和依据。
2.改变不同溶剂是研究溶剂效应的一种基本方法。通过变化溶剂可以改变物质的结构以及其物理、化学性质,这是由于分子间的作用使物质内部的分子(原子)距离拉长或缩短,改变相邻电子轨道重叠。测得不同溶剂中角黄素的的紫外—可见光谱和拉曼光谱,并利用密度泛函理(DFT)论优化角黄素分子与溶剂之间形成的三聚体几何结构。通过对实验和理论结果进行分析,了解一些结构与性质之间的关系。利用密度泛函与分子光谱对此类分子微环境测量、微结构测量有潜在的应用前景,同时该方法也为此类研究提供实验依据。
3.正是因为大多数的生物分子都是在水环境中进行其生物活性的,所以我们测量了角黄素在二元水溶液中的拉曼光谱与紫外-可见光谱。由于三元物质之间的相互作用相当复杂,我们首先利用光谱和密度泛函理论联用研究二元水溶液中有机溶剂与水之间的氢键作用。然后,我们对角黄素在二元水溶液中的拉曼光谱与紫外-可见光谱进行分析,建立了二元水溶液与角黄素的相互作用模型并解析了实验结果。这种研究思路与方法有利于深入理解水环境中生物分子结构变化和π—电子离域等的光学特性。同时,研究结果也为进一步研究复杂体系中类胡萝卜素的结构与性质提供了一定的光谱依据。
综上所述,本论文将量子化学理论与拉曼光谱与电子光谱相结合,通过改变溶液浓度和变换溶剂研究类胡萝卜素结构有序对其性质的影响,并提出一个二元水溶液体系的物理模型。这为类胡萝卜素研究提供了一个新思路,也为人们深层次探讨类胡萝卜素的结构与性质问题提供了参考资料。
To our knowledge, carotenoids are one of the most abundant pigments found in nature. They are present in most organisms including humans.Carotenoids play an important role in photosynthesis, protection against various diseases in humans, etc.β-carotene, lycopene and canthaxanthin is the most attention and he most widely studied of the three ones of carotenoids. In particular,β-carotene has two main functions, i.e. photoprotection and photon harvesting in photosynthetic systems. Lycopene has functions defense aging and cancer prevention.
Research on that they has been carried out extensively in physics, chemistry and biology. Carotenoids are the chemically simplyπ-conjugated polyene, is which the polyene chain consists of a sequences of carbon-carbon (CC) bonds (...-C=C-C=...), characterized by a strong electron-phonon (e-ph) coupling due to delocalizedπelectrons. They are the study of resonance Raman spectroscopy, optical nonlinear, the ideal molecular structure of the ideal sample, but also the realization of molecular wires and other important materials for optoelectronic devices. Therefore, the research has theoretical value and a bright application prospect. Carotenoids molecular nature of the great relationship between functional and molecular structures. In particular, this chain of molecular structure is closely related to molecular ordering properties and function.
In the paper, UV-visible spectroscopy, Raman spectroscopy and Quantum computing are combined to investigate carotenoids in solution. It is worth mentioning that we introduce an important parameter-the Raman scattering cross section for analyzing Raman spectroscopy. Raman scattering cross section (RSCS) is an important parameter in the studies and applications of the Raman spectroscopy. It relates not only to the incident frequency and the structure of a scattered molecule but also to the environment where the scattered molecule is located. It is usually obtained bycomparing the Raman intensity of an unknown molecule with that of a standard molecule with known cross section.
1. We study on Effect of the structural order of all-trans-β-carotene on the Raman scattering cross section at low concentrations. Using the technique of liquid-core optical fiber (LCOF), we measured the Raman scattering cross sections (RSCSs) of the carbon-carbon stretching vibrational modes of all-trans--carotene in carbon disulfide (CS_2) at concentrations ranging from 10~(-6) to 10~(-11) M. It was found that the RSCSs of all-trans-β-carotene were extremely high with decreasing concentration, and the absolute RSCS of C=C stretching modes of all-trans-β-carotene reached the value of 2.6×10~(-20) cm~2 molecule_(-1) Sr_(-1) at 8×10~(-11) M, which is larger than at 8×10-6 M by 4 orders of magnitude. A theoretical interpretation of the anomalous experimental results is given, which introduces a qualitative nonlinear model of coherent weakly damped electron-lattice vibrations in structural order of all-trans-β-carotene.
2. Changing solvent is one of the basic research methods of Solvent effect. Solvent has relationship with the total energy of the compressed substance, and the phase structure and reaction way may be controlled by changing solvent because the interatomic distance can be reduced or increased during compression. UV-Visible absorption spectra and Raman spectra of canthaxanthin in different solvents. Our assignments and interpretations are supported by quantum mechanical calculations of structures, which are canthaxanthin/solvents complexes. Through the analysis of experimental and theoretical results, find the relationship between structure and properties. The combination of experimental Raman data with quantum mechanical calculation leads to a better knowledge of the nature of the hydrogen bonding and the structures of the studied hydrogen-bonded complexes. The micro-environmental and micro structures measurements for such molecules of the studied the complexes, while the method is also a powerful tool for such research.
3. It is because of all the biological molecules are in the water environment to carry out its biological activity. Therefore, we measured in binary aqueous solutions of canthaxanthin in the Raman and UV-visible spectroscopy. First of all, because of the complex interaction between the ternary matter, our vibrational spectroscopic analysis on hydrogen-bonding between dimethyl sulfoxide and water comprises both experimental Raman spectra and ab initio calculations on structures of various dimethyl sulfoxide/water clusters with increasing water content.Later, we have established physical model for explaining the experimental results.At last, this method could be used as a suitable tool for investigating the structure and properties of biological molecules in aqueous environment.
In summary, this work realized the combination of quantum mechanical calculation and molecular spectroscopic technique, and established physical model for explaining carotenoids in solution. This is a new technique to investigate carotenoids, and therefore opens a new approach to deeply explore physical and chemical issues.
引文
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