外场（环境）对类胡萝卜素分子电子声子耦合的影响
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摘要
π共轭线性多烯分子是重要的光电材料，如研制光电二极管、太阳能电池、场效应晶体管等。类胡萝卜素分子为线性多烯类生物分子，具有光合作用，具有光能采集、吸收三重态能量，猝灭单态氧等功能。它的光电性质与其结构及其有序程度，即π电子离域程度密切相关。研究类胡萝卜素分子在共振拉曼过程中的电子—声子耦合可以获得电子、原子振动相互作用规律，对丰富分子光谱学内容、研制高质量多烯光电材料既有重要理论价值又有光明应用前景。外场对电子声子耦合影响等很多规律有待认知，很多实际应用有待开发。
本文利用共振拉曼光谱、可见吸收光谱技术、依据量子力学、分子光谱相关理论，分别研究了：β胡萝卜素溶于1，2二氯乙烷溶液温度区间为83K到323K范围内，溶液相变对β胡萝卜素拉曼光谱基频、和频、倍频强度及线宽的影响，β胡萝卜素溶于二甲基亚砜溶液中25-81oC温度范围内的拉曼和吸收光谱特性，分析了温度对电子—声子耦合的影响；研究了温度对β胡萝卜素溶于极性溶剂1，2二氯乙烷和非极性溶剂环己烷中20-60oC温度范围内，溶剂极性对β胡萝卜素电子—声子耦合的影响；研究了压强对二硫化碳中β胡萝卜素分子电子—声子耦合的影响，取得如下创新性成果：
1.利用变换温度的方法研究了β胡萝卜素溶于1，2二氯乙烷中323K到83K范围内温度对拉曼光谱基频、和频、倍频强度及线宽的影响。研究的创新之处为相变期间，和频和倍频的相对强度一直增加。这主要是由于电子声子耦合增加量大于相干弱阻尼CC键振动的减少量。
测量多烯分子β胡萝卜素在二甲基亚砜溶液中的可见吸收和拉曼光谱，分析了温度对β胡萝卜素紫外吸收带峰位，构型能，黄昆因子及电子声子耦合的影响。结果表明：随着温度的升高，β胡萝卜素CC单键和双键的拉曼散射截面值降低，可见吸收光谱发生蓝移。黄昆因子增加，拉曼半高宽增加。这是由于温度增加引起分子热运动加剧，溶液不稳定，导致β胡萝卜素熵降低，另外，温度升高所引起的有效共轭长度降低，也是吸收光谱发生蓝移的原因之一。此外，随着温度的升高，β胡萝卜素分子的结构有序性下降，CC各单、双键的键长差增加，导致半高宽增加。根据不同温度的吸收和拉曼谱，我们计算了电子声子耦合系数，随着温度的增加，有效共轭长度降低，改变了晶格振动，拉曼的电子声子耦合系数降低。
(2)研究了β胡萝卜素在极性溶剂1，2-二氯乙烷和非极性溶剂环己烷不同温度范围的电子吸收光谱和拉曼光谱，通过分析实验的光谱变化规律及理论计算，得出不同极性溶剂对β胡萝卜素分子结构有序性、π-电子离域、黄昆因子、电子声子耦合等有很大影响，在非极性溶剂环己烷中,分子间相互作用力及其种类少,分子结构有序性好,有效共轭长度大,π电子离域扩展容易, R. Tubino提出的带量纲电子声子耦合常数V小，相干弱阻尼电子-晶格振动强，拉曼活性好。在极性溶剂1,2-二氯乙烷中,存在着静电诱导能等多种作用使β胡萝卜素分子结构有序性差，有效共轭长度小，π电子离域范围小，有量纲的电子-声子耦合大，拉曼活性差。实现了电子能隙对碳碳键振动的调制作用。
(3)测量了β胡萝卜素溶于CS_2溶液中0.04-0.6Gpa下的高压紫外—可见吸收光谱和高压拉曼光谱，实验结果表明，随着压强的增加，溶液的密度和折射率的增大。分子被压缩并有序性下降，π电子能隙减小，使紫外-可见吸收光谱红移；由于压强增大，使溶质溶剂之间的相互作用增大，S1态的振动弛豫时间缩短，00带吸收光谱变宽。黄昆因子随着压强的增大而增加。随着压强的增大，由于电子能隙对碳碳键振动的调制作用变大，使得拉曼光谱中CC键的散射截面减小；根据吸收和拉曼光谱的各参数，我们计算了R. Tubino提出的带量纲电子声子耦合常数V，随着压强的增大，电子声子耦合常数增加。
综上所述，本论文通过改变温度、溶剂极性、压强等外界环境来研究电子声子耦合参数随外场（环境）变化规律，掌握其产生光学现象的机理，深入了解分子结构和分子内、分子间相互作用。明确线性多烯分子各种光电特性及光谱学机理，既能丰富多烯分子光谱学内容，也为研制高性能光电材料提供依据和参考。
π-Conjugated linear polymers are highly interesting subjects due to theiroptoelectronic applications, such as in light-emitting diodes, solar cells, andfield-effect transistors. Carotenoids have multiple roles in the photosynthetic process.They harvest incoming photons at wavelengths that chlorophyll molecules do notabsorb and are capable of accepting the energy of chlorophyll triplet states, which caninduce the formation of harmful singlet oxygen species. Its electro-optical propertiesare closely related to the structure ordered, that is π-electron delocalization extent.The researches on electron-phonon coupling of all-trans-β-carotene in resonantRaman scattering contain the important regularity between the electron and atomvibration. At the same time, it has theoretical value and bright application prospect forenriching molecule spectroscopy content and developing the high-quality polyenephotoelectric material. We need have deeper research on electron-phonon coupling,we need develop some practical application on it.
We use the resonance Raman and visible absorption spectroscopy technology toresearch following work according to the theory of quantum mechanics and molecularspectrum. We got resonance Raman spectra of the all-trans-β-carotene dissolved in1,2-dichloroethane in the83K to323K temperature range. The fundamental,combination and harmonic modes and width of CC bonds vary with temperature. Wemeasure the Raman and absorption spectra of all-trans-β-carotene in dimethylsulfoxide (DMSO) at the temperature range from25to81oCand analysis the effectof temperature on electron-phonon coupling. The absorption and resonance Ramanspectra of all-trans-β-carotene in nonpolar cyclohexane and polar1,2-dicholoroethaneat the temperature range from20to60oChave been measured to analysis the effectof solvent’s polar on electron-phonon coupling. The effect of pressure onelectron-phonon coupling of all-trans-β-carotene in CS2has been discussed. We gotthe following innovative achievements.
1. We got resonance Raman spectra of the all-trans-β-carotene dissolved in1,2-dichloroethane through varying temperature and obtain the temperature effect onfundamental, combination and harmonic modes and width of CC bonds. The innovateresearch describes that during the solid-liquid phase transition, the Raman ScatteringCross Section(RSCS) of the fundamental CC bonds rapidly decreases but the rate ofrelative intensities increases sharply as the temperature decreases. The observed highRaman activity in segment s can be attributed to the greater electron-phonon couplingthat can rapidly arise in all-trans-β-carotene.
The temperature dependence (25-81oC) of the visible absorption and Ramanspectra of all-trans-β-carotene extremely diluted in dimethyl sulfoxide (DMSO) isinvestigated to clarify the effects of temperature on the absorption wavelength,characteristic energy, Huang-Rhys (HR) factor and electron-phonon coupling. Aprominent feature of the temperature evolution of all-trans-β-carotene is theacceleration of molecular movement, which results in a decrease in entropy andcauses the solution to become unstable. Weakening of the coherent weakly dampedCC stretching vibrations of all-trans-β-carotene caused by a decrease in thestructurally ordered properties of the molecules leads to decreases in the RSCS. Wemeasure the absorption spectra of all-trans-β-carotene at different temperatures. Aprominent feature of the all-trans-β-carotene absorption spectrum is the blueshift withincreases in temperature. We interpret the phenomenon with Lorentz-Lorenz function.Therefore, with increasing temperature, the blueshift of the all-trans-β-caroteneabsorption spectrum in the visible region could be interpreted as arising fromconcomitant decreases in the liquid density and refractive index by theLorentz-Lorenz function. The decrease in effective conjugation length (ECL) withincreasing temperature can lead to the blueshift of absorption spectra. Inaddition, we also calculated an important parameter: Huang-Rhys (HR) factor, itdescribes the degree of electron-phonon coupling. The HR factor trend in theabsorption indicates that excitons have strengthened coupling with the primaryphonon with energy of E_p when temperature is increased. The full width at half maximum (FWHM) of the Raman peak increases monotonically with increasingtemperature. We calculate electron–phonon coupling parameter combine the Ramanand absorption spectra. With increasing temperature, the degree of effectiveconjugation length, modifying the lattice configuration, electron–phonon couplingdecreases.
(2) We measure the absorption and resonance Raman spectra ofall-trans-β-carotene in nonpolar cyclohexane and polar1,2-dicholoroethane at thetemperature range from20to60oC. We get the effect of solvent polar on structureordered, πelectron delocalization, HR factor and electron–phonon coupling ofall-trans-β-carotene. The few species of interaction force between the molecules makethe structure ordered better in a non-polar solvent cyclohexane. The ECL increases,πelectron delocalization extended and coherent weakly electron-lattice vibrationenhanced lead to the high Raman activity. The electron-phonon coupling constant ofall-trans-β-carotene in non-polar solvent cyclohexane is smaller than that in polarsolvent1,2-dicholoroethane. However, the electrostatic induction ofall-trans-β-carotene in decreases the structural ordered, shorten the ECL, diminishedπelectron delocalization. All-trans-β-carotene has low Raman activity in polar solvent1,2-dicholoroethane.
(3) Visible absorption and Raman spectra of all-trans-β-carotene are measured inCS2at pressure range from0.04-0.6Gpa. The results indicated that the visibleabsorption spectra are red-shifted, FWHM increases, the RSCS decreases,Huang-Rhys factor increases, the electron-phonon coupling constants of CC bondvibration modes increases. The reasons for these phenomena are the molecularstructural order of β-carotene decreased and π electron energy gap diminished withthe pressure increased. The visible absorption spectra are red-shifted. Otherwise, thedensity and refractive index increase with the increasing pressure. It makescontribution on the red shift. The FWHM of the0-0peak increases monotonicallywith increasing pressure. The intermolecular electrostatic interactions enhanced withthe increasing pressure. The broader bandwidth of this band in S1relative to its width in S_0is ascribed to the shorter vibrational relaxation time in the S1state. Thevibrational relaxation is due to the intermolecular electrostatic interactions betweenthe transition dipoles of the solute molecules. Weakening of the coherent weaklydamped CC stretching vibrations of all-trans-β-carotene caused by a decrease in thestructurally ordered properties of the molecules leads to decreases in the Ramanscattering cross section. We combine the absorption spectra with the Raman spectra tocalculate the electron-phonon coupling constants. The electron-phonon couplingconstant of CC bond vibration modes which is proposed by R. Tubino increases withincreasing pressure.
In summary, we analyse the effect of external field such as temperature, solventpolarity, pressure on electron-phonon coupling parameter. The mechanism ofgenerating optical phenomenon and the interactions between intramolecular andintermolecular have been grasped. It has theoretical value and bright applicationprospect for enriching molecule spectroscopy content and developing the high-qualitypolyene photoelectric material.
本文利用共振拉曼光谱、可见吸收光谱技术、依据量子力学、分子光谱相关理论，分别研究了：β胡萝卜素溶于1，2二氯乙烷溶液温度区间为83K到323K范围内，溶液相变对β胡萝卜素拉曼光谱基频、和频、倍频强度及线宽的影响，β胡萝卜素溶于二甲基亚砜溶液中25-81oC温度范围内的拉曼和吸收光谱特性，分析了温度对电子—声子耦合的影响；研究了温度对β胡萝卜素溶于极性溶剂1，2二氯乙烷和非极性溶剂环己烷中20-60oC温度范围内，溶剂极性对β胡萝卜素电子—声子耦合的影响；研究了压强对二硫化碳中β胡萝卜素分子电子—声子耦合的影响，取得如下创新性成果：
1.利用变换温度的方法研究了β胡萝卜素溶于1，2二氯乙烷中323K到83K范围内温度对拉曼光谱基频、和频、倍频强度及线宽的影响。研究的创新之处为相变期间，和频和倍频的相对强度一直增加。这主要是由于电子声子耦合增加量大于相干弱阻尼CC键振动的减少量。
测量多烯分子β胡萝卜素在二甲基亚砜溶液中的可见吸收和拉曼光谱，分析了温度对β胡萝卜素紫外吸收带峰位，构型能，黄昆因子及电子声子耦合的影响。结果表明：随着温度的升高，β胡萝卜素CC单键和双键的拉曼散射截面值降低，可见吸收光谱发生蓝移。黄昆因子增加，拉曼半高宽增加。这是由于温度增加引起分子热运动加剧，溶液不稳定，导致β胡萝卜素熵降低，另外，温度升高所引起的有效共轭长度降低，也是吸收光谱发生蓝移的原因之一。此外，随着温度的升高，β胡萝卜素分子的结构有序性下降，CC各单、双键的键长差增加，导致半高宽增加。根据不同温度的吸收和拉曼谱，我们计算了电子声子耦合系数，随着温度的增加，有效共轭长度降低，改变了晶格振动，拉曼的电子声子耦合系数降低。
(2)研究了β胡萝卜素在极性溶剂1，2-二氯乙烷和非极性溶剂环己烷不同温度范围的电子吸收光谱和拉曼光谱，通过分析实验的光谱变化规律及理论计算，得出不同极性溶剂对β胡萝卜素分子结构有序性、π-电子离域、黄昆因子、电子声子耦合等有很大影响，在非极性溶剂环己烷中,分子间相互作用力及其种类少,分子结构有序性好,有效共轭长度大,π电子离域扩展容易, R. Tubino提出的带量纲电子声子耦合常数V小，相干弱阻尼电子-晶格振动强，拉曼活性好。在极性溶剂1,2-二氯乙烷中,存在着静电诱导能等多种作用使β胡萝卜素分子结构有序性差，有效共轭长度小，π电子离域范围小，有量纲的电子-声子耦合大，拉曼活性差。实现了电子能隙对碳碳键振动的调制作用。
(3)测量了β胡萝卜素溶于CS_2溶液中0.04-0.6Gpa下的高压紫外—可见吸收光谱和高压拉曼光谱，实验结果表明，随着压强的增加，溶液的密度和折射率的增大。分子被压缩并有序性下降，π电子能隙减小，使紫外-可见吸收光谱红移；由于压强增大，使溶质溶剂之间的相互作用增大，S1态的振动弛豫时间缩短，00带吸收光谱变宽。黄昆因子随着压强的增大而增加。随着压强的增大，由于电子能隙对碳碳键振动的调制作用变大，使得拉曼光谱中CC键的散射截面减小；根据吸收和拉曼光谱的各参数，我们计算了R. Tubino提出的带量纲电子声子耦合常数V，随着压强的增大，电子声子耦合常数增加。
综上所述，本论文通过改变温度、溶剂极性、压强等外界环境来研究电子声子耦合参数随外场（环境）变化规律，掌握其产生光学现象的机理，深入了解分子结构和分子内、分子间相互作用。明确线性多烯分子各种光电特性及光谱学机理，既能丰富多烯分子光谱学内容，也为研制高性能光电材料提供依据和参考。
π-Conjugated linear polymers are highly interesting subjects due to theiroptoelectronic applications, such as in light-emitting diodes, solar cells, andfield-effect transistors. Carotenoids have multiple roles in the photosynthetic process.They harvest incoming photons at wavelengths that chlorophyll molecules do notabsorb and are capable of accepting the energy of chlorophyll triplet states, which caninduce the formation of harmful singlet oxygen species. Its electro-optical propertiesare closely related to the structure ordered, that is π-electron delocalization extent.The researches on electron-phonon coupling of all-trans-β-carotene in resonantRaman scattering contain the important regularity between the electron and atomvibration. At the same time, it has theoretical value and bright application prospect forenriching molecule spectroscopy content and developing the high-quality polyenephotoelectric material. We need have deeper research on electron-phonon coupling,we need develop some practical application on it.
We use the resonance Raman and visible absorption spectroscopy technology toresearch following work according to the theory of quantum mechanics and molecularspectrum. We got resonance Raman spectra of the all-trans-β-carotene dissolved in1,2-dichloroethane in the83K to323K temperature range. The fundamental,combination and harmonic modes and width of CC bonds vary with temperature. Wemeasure the Raman and absorption spectra of all-trans-β-carotene in dimethylsulfoxide (DMSO) at the temperature range from25to81oCand analysis the effectof temperature on electron-phonon coupling. The absorption and resonance Ramanspectra of all-trans-β-carotene in nonpolar cyclohexane and polar1,2-dicholoroethaneat the temperature range from20to60oChave been measured to analysis the effectof solvent’s polar on electron-phonon coupling. The effect of pressure onelectron-phonon coupling of all-trans-β-carotene in CS2has been discussed. We gotthe following innovative achievements.
1. We got resonance Raman spectra of the all-trans-β-carotene dissolved in1,2-dichloroethane through varying temperature and obtain the temperature effect onfundamental, combination and harmonic modes and width of CC bonds. The innovateresearch describes that during the solid-liquid phase transition, the Raman ScatteringCross Section(RSCS) of the fundamental CC bonds rapidly decreases but the rate ofrelative intensities increases sharply as the temperature decreases. The observed highRaman activity in segment s can be attributed to the greater electron-phonon couplingthat can rapidly arise in all-trans-β-carotene.
The temperature dependence (25-81oC) of the visible absorption and Ramanspectra of all-trans-β-carotene extremely diluted in dimethyl sulfoxide (DMSO) isinvestigated to clarify the effects of temperature on the absorption wavelength,characteristic energy, Huang-Rhys (HR) factor and electron-phonon coupling. Aprominent feature of the temperature evolution of all-trans-β-carotene is theacceleration of molecular movement, which results in a decrease in entropy andcauses the solution to become unstable. Weakening of the coherent weakly dampedCC stretching vibrations of all-trans-β-carotene caused by a decrease in thestructurally ordered properties of the molecules leads to decreases in the RSCS. Wemeasure the absorption spectra of all-trans-β-carotene at different temperatures. Aprominent feature of the all-trans-β-carotene absorption spectrum is the blueshift withincreases in temperature. We interpret the phenomenon with Lorentz-Lorenz function.Therefore, with increasing temperature, the blueshift of the all-trans-β-caroteneabsorption spectrum in the visible region could be interpreted as arising fromconcomitant decreases in the liquid density and refractive index by theLorentz-Lorenz function. The decrease in effective conjugation length (ECL) withincreasing temperature can lead to the blueshift of absorption spectra. Inaddition, we also calculated an important parameter: Huang-Rhys (HR) factor, itdescribes the degree of electron-phonon coupling. The HR factor trend in theabsorption indicates that excitons have strengthened coupling with the primaryphonon with energy of E_p when temperature is increased. The full width at half maximum (FWHM) of the Raman peak increases monotonically with increasingtemperature. We calculate electron–phonon coupling parameter combine the Ramanand absorption spectra. With increasing temperature, the degree of effectiveconjugation length, modifying the lattice configuration, electron–phonon couplingdecreases.
(2) We measure the absorption and resonance Raman spectra ofall-trans-β-carotene in nonpolar cyclohexane and polar1,2-dicholoroethane at thetemperature range from20to60oC. We get the effect of solvent polar on structureordered, πelectron delocalization, HR factor and electron–phonon coupling ofall-trans-β-carotene. The few species of interaction force between the molecules makethe structure ordered better in a non-polar solvent cyclohexane. The ECL increases,πelectron delocalization extended and coherent weakly electron-lattice vibrationenhanced lead to the high Raman activity. The electron-phonon coupling constant ofall-trans-β-carotene in non-polar solvent cyclohexane is smaller than that in polarsolvent1,2-dicholoroethane. However, the electrostatic induction ofall-trans-β-carotene in decreases the structural ordered, shorten the ECL, diminishedπelectron delocalization. All-trans-β-carotene has low Raman activity in polar solvent1,2-dicholoroethane.
(3) Visible absorption and Raman spectra of all-trans-β-carotene are measured inCS2at pressure range from0.04-0.6Gpa. The results indicated that the visibleabsorption spectra are red-shifted, FWHM increases, the RSCS decreases,Huang-Rhys factor increases, the electron-phonon coupling constants of CC bondvibration modes increases. The reasons for these phenomena are the molecularstructural order of β-carotene decreased and π electron energy gap diminished withthe pressure increased. The visible absorption spectra are red-shifted. Otherwise, thedensity and refractive index increase with the increasing pressure. It makescontribution on the red shift. The FWHM of the0-0peak increases monotonicallywith increasing pressure. The intermolecular electrostatic interactions enhanced withthe increasing pressure. The broader bandwidth of this band in S1relative to its width in S_0is ascribed to the shorter vibrational relaxation time in the S1state. Thevibrational relaxation is due to the intermolecular electrostatic interactions betweenthe transition dipoles of the solute molecules. Weakening of the coherent weaklydamped CC stretching vibrations of all-trans-β-carotene caused by a decrease in thestructurally ordered properties of the molecules leads to decreases in the Ramanscattering cross section. We combine the absorption spectra with the Raman spectra tocalculate the electron-phonon coupling constants. The electron-phonon couplingconstant of CC bond vibration modes which is proposed by R. Tubino increases withincreasing pressure.
In summary, we analyse the effect of external field such as temperature, solventpolarity, pressure on electron-phonon coupling parameter. The mechanism ofgenerating optical phenomenon and the interactions between intramolecular andintermolecular have been grasped. It has theoretical value and bright applicationprospect for enriching molecule spectroscopy content and developing the high-qualitypolyene photoelectric material.
引文
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