氟溴苯分子和甲基苯甲醚分子的激发态和离子态光谱研究
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摘要
芳香族化合物的激发态和离子态光谱研究在大气化学、燃烧化学、环境监测以及天体化学等领域有着重要的应用。通过对分子激发态和离子态光谱进行实验研究和理论计算,可以获得分子在激发态和离子态的几何结构、振动频率、激发能、电离能、分子轨道和对称性等多方面的信息,为深入研究分子的化学反应机制提供帮助。本文利用共振增强多光子电离(REMPI)技术和质量分辨阂值电离(MATI)光谱技术对芳香族化合物氟溴苯分子和甲基苯甲醚分子的激发态和离子态光谱进行了研究,得到以下主要结果：
1.使用单光共振双光子电离(1C-R2PI)技术测量了三种同分异构体邻、间、对氟溴苯分子基态到第一电子激发态(S1←S0)的光谱,得到邻、间、对氟溴苯分子第一电子激发态(S1态)的激发能E1)分别为36987、36961和36223cm-1。结合理论计算,对邻、间、对氟溴苯分子S1态的谱峰进行了标识。研究表明氟溴苯分子S1态的激发能和振动能级结构由其受到的共振效应和诱导效应共同决定。此外,通过比较对氟溴苯分子的REMPI谱和由对氟溴苯分子解离生成的Br原子的REMPI谱,得到对氟溴苯分子在S1态的解离势垒(S1束缚态和排斥态交叉点相对S1态带源的能量差)约为2815cm-1(0.35eV)。
2.使用1C-R2PI技术和MATI技术测量了间甲基苯甲醚分子顺反异构体的S1←S0的光谱和阈值电离光谱。得到顺式、反式间甲基苯甲醚分子的E1分别为36049±2和36117±2cm-1,绝热电离能(IE)分别为64859±5和65110±5cm-1。结合理论计算,解释了顺式、反式间甲基苯甲醚分子E1和IE存在差异的原因,并对S1态和离子基态D0态的谱峰进行了标识。研究表明间甲基苯甲醚分子顺反异构体在S1态和Do态的活性振动主要是甲基转动、面内环的运动和与取代基相关的弯曲振动。间甲基苯甲醚分子的S1态振动光谱、D0态离子光谱以及理论计算均表明这两个转动异构体在D0态的几何构型与S1态的中性几何构型相比有较大改变,取代基与取代基、取代基与苯环间的相互作用强度高低次序为：S0 3.使用1C-R2PI技术和MATI技术研究了反式邻甲基苯甲醚分子的S1←S0的光谱和阈值电离光谱。得到反式邻甲基苯甲醚分子的E1为36364±2cm-1,绝热IE为64755±5cm-1。结合理论计算对S1态和D0态的谱峰进行了标识。反式邻甲基苯甲醚分子的S1和IE相对苯甲醚分子和甲苯分子的S1和IE有相对红移,表明甲基和甲氧基与苯环的相互作用在S1和D0态时比在基态时强。反式邻甲基苯甲醚分子的S1态和D0态光谱以及理论计算均表明其在D0态的几何构型与S1态的几何构型相比有较大改变。
The research on vibronic and cation spectra of aromatic compounds has very important significance in the field of atmospheric environmental chemistry, combustion chemistry, environment monitoring and astrochemistry. The experimental results and theoretical calculations on the first electronically excited S1state and the cation ground Do state will help us to obtain the information about the geometry structure, vibrational frequency, excited energy, ionization energy, molecular orbital and symmetry of the molecules in the S1state and the Do state, and provide experimental basis for further research on the chemical reaction mechanism. In the present paper, the resonance-enhanced mutiphoton ionization (REMPI) and the mass-analyzed threshold ionization (MATI) techniques have been used to study the excited and ionic spectra of bromofluorobenzene and methylanisole. The following are the main results:
1. The S1←S0electronic transition of o-, m-, and p-bromofluorobenzene were investigated by using one-color resonant two-photon ionization (1C-R2PI) technique. The first electronic excitation energies of o-, m-, and p-bromofluorobenzene were measured to be36987,36961, and36223cm-1, respectively. The vibrational bands observed in the REMPI spectra were assigned with the help of ab initio and density functional theory (DFT) calculations. The excitation energies and the vibrational bands of these molecules were determined by the combined action of resonant effect and inductive effect. In addition, comparing the REMPI spectrum of p-bromofluorobenzene and the REMPI spectrum of Br atom which come from the photodissociation of p-bromofluorobenzene, the potential barrier height (the energy of the crossing points between the bound S1state and a repulsive state relative to the S1minimum) of p-bromofluorobenzene in the S1state was determined to be lower than2815cm-1(0.35eV).
2. The S1←S0electronic transition and threshold ionization of the cis and trans rotamers of m-methylanisole were investigated by using1C-R2PI and MATI techniques. The first electronic excitation energies were measured to be36049±2and36117±2cm-1, and the adiabatic ionization energies were determined to be64859±5and65110±5cm-1for cis-and trans-m-methylanisole, respectively. Results from the ab initio and DFT calculations provide satisfactory interpretation for our experimental findings on the difference of the transitional energies of the cis and trans rotamers and help us assign the vibronic and cation spectra obtained in the present experiments. The observed active vibrations of both rotamers of m-methylanisole in the electronically excited S1and cationic ground Do states mainly involve the methyl torsion, in-plane ring deformation, and substituent-sensitive bending vibrations. The present experimental and theoretical results show that the geometry of the cation in the Do state is somewhat different from that of the neutral in the S1state for cis-and trans-m-methylanisole. In addition, the strengths of the through-space substituent-substituent and substituent-ring interactions are found to follow the order:S0 3. The S1←S0electronic transition and threshold ionization of trans-o-methylanisole were investigated by using1C-R2PI and MATI techniques. The excitation energy of the S1←S0transition and the adiabatic ionization energy of this molecule were measured to be36364±2and64755±5cm-1, respectively. The vibronic and cation spectra of trans-o-methylanisole were assigned with the help of ab initio and DFT calculations. The red-shift of excitation energy and ionization energy with respect to those of anisole and toluene indicates that the interaction of the CH3and OCH3group with the ring is stronger in S1and Do states than that in the So state. Results from the calculations and the observed vibronic and cation spectra implies that the molecular geometry, symmetry, and vibrational coordinates of the cation changed too much during the D0←S1ionization process.
1.使用单光共振双光子电离(1C-R2PI)技术测量了三种同分异构体邻、间、对氟溴苯分子基态到第一电子激发态(S1←S0)的光谱,得到邻、间、对氟溴苯分子第一电子激发态(S1态)的激发能E1)分别为36987、36961和36223cm-1。结合理论计算,对邻、间、对氟溴苯分子S1态的谱峰进行了标识。研究表明氟溴苯分子S1态的激发能和振动能级结构由其受到的共振效应和诱导效应共同决定。此外,通过比较对氟溴苯分子的REMPI谱和由对氟溴苯分子解离生成的Br原子的REMPI谱,得到对氟溴苯分子在S1态的解离势垒(S1束缚态和排斥态交叉点相对S1态带源的能量差)约为2815cm-1(0.35eV)。
2.使用1C-R2PI技术和MATI技术测量了间甲基苯甲醚分子顺反异构体的S1←S0的光谱和阈值电离光谱。得到顺式、反式间甲基苯甲醚分子的E1分别为36049±2和36117±2cm-1,绝热电离能(IE)分别为64859±5和65110±5cm-1。结合理论计算,解释了顺式、反式间甲基苯甲醚分子E1和IE存在差异的原因,并对S1态和离子基态D0态的谱峰进行了标识。研究表明间甲基苯甲醚分子顺反异构体在S1态和Do态的活性振动主要是甲基转动、面内环的运动和与取代基相关的弯曲振动。间甲基苯甲醚分子的S1态振动光谱、D0态离子光谱以及理论计算均表明这两个转动异构体在D0态的几何构型与S1态的中性几何构型相比有较大改变,取代基与取代基、取代基与苯环间的相互作用强度高低次序为：S0
The research on vibronic and cation spectra of aromatic compounds has very important significance in the field of atmospheric environmental chemistry, combustion chemistry, environment monitoring and astrochemistry. The experimental results and theoretical calculations on the first electronically excited S1state and the cation ground Do state will help us to obtain the information about the geometry structure, vibrational frequency, excited energy, ionization energy, molecular orbital and symmetry of the molecules in the S1state and the Do state, and provide experimental basis for further research on the chemical reaction mechanism. In the present paper, the resonance-enhanced mutiphoton ionization (REMPI) and the mass-analyzed threshold ionization (MATI) techniques have been used to study the excited and ionic spectra of bromofluorobenzene and methylanisole. The following are the main results:
1. The S1←S0electronic transition of o-, m-, and p-bromofluorobenzene were investigated by using one-color resonant two-photon ionization (1C-R2PI) technique. The first electronic excitation energies of o-, m-, and p-bromofluorobenzene were measured to be36987,36961, and36223cm-1, respectively. The vibrational bands observed in the REMPI spectra were assigned with the help of ab initio and density functional theory (DFT) calculations. The excitation energies and the vibrational bands of these molecules were determined by the combined action of resonant effect and inductive effect. In addition, comparing the REMPI spectrum of p-bromofluorobenzene and the REMPI spectrum of Br atom which come from the photodissociation of p-bromofluorobenzene, the potential barrier height (the energy of the crossing points between the bound S1state and a repulsive state relative to the S1minimum) of p-bromofluorobenzene in the S1state was determined to be lower than2815cm-1(0.35eV).
2. The S1←S0electronic transition and threshold ionization of the cis and trans rotamers of m-methylanisole were investigated by using1C-R2PI and MATI techniques. The first electronic excitation energies were measured to be36049±2and36117±2cm-1, and the adiabatic ionization energies were determined to be64859±5and65110±5cm-1for cis-and trans-m-methylanisole, respectively. Results from the ab initio and DFT calculations provide satisfactory interpretation for our experimental findings on the difference of the transitional energies of the cis and trans rotamers and help us assign the vibronic and cation spectra obtained in the present experiments. The observed active vibrations of both rotamers of m-methylanisole in the electronically excited S1and cationic ground Do states mainly involve the methyl torsion, in-plane ring deformation, and substituent-sensitive bending vibrations. The present experimental and theoretical results show that the geometry of the cation in the Do state is somewhat different from that of the neutral in the S1state for cis-and trans-m-methylanisole. In addition, the strengths of the through-space substituent-substituent and substituent-ring interactions are found to follow the order:S0
引文
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