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2-甲基烯丙基的紫外光解离
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作者 Lucas Michael 覃院 +2 位作者 陈旻 孙格 张劲松 《Chinese Journal of Chemical Physics》 SCIE EI CAS CSCD 2024年第2期255-263,I0102,共10页
本文利用高里德堡态氢原子飞行时间探测技术,研究了2-甲基烯丙基自由基的3p里德堡态在解离光波长范围226~244 nm下的光解离动力学过程.2-甲基烯丙基自由基由3-氯-2-甲基-1-丙烯前体在193nm光解作用下产生.在226~244nm区间内,氢原子光解... 本文利用高里德堡态氢原子飞行时间探测技术,研究了2-甲基烯丙基自由基的3p里德堡态在解离光波长范围226~244 nm下的光解离动力学过程.2-甲基烯丙基自由基由3-氯-2-甲基-1-丙烯前体在193nm光解作用下产生.在226~244nm区间内,氢原子光解碎片谱随着波长的减小而信号强度增加。氢原子产物的飞行时间谱呈现双模结构.主要产物通道(占比~98%)的平动能峰值在~7kcal/mol,在226~244nm范围内氢原子和对应解离碎片平动能平均值为总过剩能量的(fT)~0.18,并且解离产物角分布呈各向同性.这些低平动能,角分布各向同性的产物来自经由电子激发态内转换形成的高度振动激发的热2-甲基烯丙基的统计单分子分解过程,其形成亚甲基环丙烷+氢原子,次要产物通道(占~2%)具有较大的平动能,峰值约为50kcal/mol,(fT)≈0.63且产物呈各向异性角分布(β≈-0.2).这些高平动能、各向异性的产物是非统计性的,推测是通过3p里德堡态或基态的排斥势能面部分直接失去一个氢原子生成1,3-丁二烯十氢原子. 展开更多
关键词 紫外光解离 甲基烯丙基 自由基
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Field Measurement of NO2 and RNO2 by Two-Channel Thermal Dissociation Cavity Ring Down Spectrometer 被引量:2
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作者 陈剑 吴昊 +2 位作者 刘安雯 胡水明 张劲松 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2017年第5期493-498,I0001,共7页
A two-channel thermal dissociation cavity ring down spectroscopy (CRDS) instrument has been built for in situ, real-time measurement of NO2 and total RNO2 (peroxy nitrates and alkyl nitrates) in ambient air, with ... A two-channel thermal dissociation cavity ring down spectroscopy (CRDS) instrument has been built for in situ, real-time measurement of NO2 and total RNO2 (peroxy nitrates and alkyl nitrates) in ambient air, with a NO2 detection limit of 0.10 ppbv at 1 s. A 6-day long measurement was conducted at urban site of Hefei by using the CRDS instrument with a time resolution of 3 s. A commercial molybdenum converted chemiluminescence (Mo-CL) instrument was also used for comparison. The average RNO2 concentration in the 6 days was measured to be 1.94 ppbv. The Mo-CL instrument overestimated the NO2 concentration by a bias of +1.69 ppbv in average, for the reason that it cannot distinguish RNO2 from NO2. The relative bias could be over 100% during the afternoon hours when NO2 was low but RNO2 was high. 展开更多
关键词 Cavity ring-down spectroscopy Molybdenum converted chemiluminescence Thermal dissociation Organic nitrates
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Resonance-Enhanced Photon Excitation Spectroscopy of the Even-Parity 3p^5(2P1/2)nl′ [K′]J (l′=1, 3) Autoionizing Rydberg States of Ar
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作者 李春燕 何志巍 +3 位作者 王婷婷 甄军锋 陈旸 张劲松 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2013年第3期259-264,I0003,共7页
Metastable 40Ar* atoms are produced in the two metastable states 3p54s [3/2]2 and 3p5 4s′ [1/2]0 in a pulsed DC discharge in a beam, and are subsequently excited to the even-parity autoionizing resonance series 3pSn... Metastable 40Ar* atoms are produced in the two metastable states 3p54s [3/2]2 and 3p5 4s′ [1/2]0 in a pulsed DC discharge in a beam, and are subsequently excited to the even-parity autoionizing resonance series 3pSnp′[3/2]1,2, 3p5 np′ [1/2]1, and 3p5nf′[5/2]3 using single photon excitation with a pulsed dye laser. The excitation spectra of the even-parity autoion- izing resonance series from the metastable 40Ar* are obtained by recording the autoionized Ar+ ions with time-of-flight ion detection in the photon energy range of 32500-35600 cm-1 with an experimental bandwidth of 〈0.1 cm-1. A wealth of autoionizing resonances are newly observed, from which more precise and systematic spectroscopic data of the level energies and quantum defects are derived. 展开更多
关键词 AR Pulsed DC discharge Resonance-enhanced photon excitation spectroscopy Autoionizing Rydberg resonance
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正丙醇和异丙醇的紫外光解动力学(英文) 被引量:3
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作者 周卫东 张劲松 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 北大核心 2002年第3期233-236,共4页
利用高里德堡态氢原子飞行时间 (HRTOF)探测技术 ,研究了正丙醇和异丙醇的紫外光解动力学过程 .在 193.3nm光辐射下 ,O -H键快速断裂过程构成主要的氢原子生成通道 .伴随O -H键的碎裂 ,相当大的一部分能量转换成氢原子及其相应碎片的平... 利用高里德堡态氢原子飞行时间 (HRTOF)探测技术 ,研究了正丙醇和异丙醇的紫外光解动力学过程 .在 193.3nm光辐射下 ,O -H键快速断裂过程构成主要的氢原子生成通道 .伴随O -H键的碎裂 ,相当大的一部分能量转换成氢原子及其相应碎片的平动能 (正丙醇〈fv〉 =0 .76 ;异丙醇〈fv〉 =0 .78) .氢原子碎片具有各向异性的角度分布 ;其角分布异向因子 β分别为 - 0 .79(正丙醇 )和 - 0 .77(异丙醇 ) .研究结果表明 ,吸收 1个 193.3nm光子后 ,丙醇分子跃迁到一个寿命很短的电子激发态 ;沿着O -H反应坐标 ,该激发态势能面是排斥的 ,因而O -H键快速断裂 .此外 ,还得到了丙醇的O -H键离解能 :(432± 2 )kJ/mol(正丙醇 )和 (433± 2 )kJ/mol(异丙醇 ) . 展开更多
关键词 紫外光 光解动力学 正丙醇 异丙醇 高里德堡态 氢原子飞行时间探测技术
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利用激光腔内共振衰减技术研究CH_2CHO自由基的近紫外吸收光谱(英文)
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作者 王黎明 张劲松 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 北大核心 2004年第3期357-361,共5页
利用激光腔内共振衰减技术 (CRDS) ,获取了CH2 CHO自由基的近紫外吸收光谱 .在此吸收光谱中 ,有一从 2 8786cm-1起始的振动 电子带 ,和一随能量而增加的宽吸收背景 .此CRDS吸收光谱和以前的低分辨吸收光谱相一致 ;其振动 电子吸收峰位... 利用激光腔内共振衰减技术 (CRDS) ,获取了CH2 CHO自由基的近紫外吸收光谱 .在此吸收光谱中 ,有一从 2 8786cm-1起始的振动 电子带 ,和一随能量而增加的宽吸收背景 .此CRDS吸收光谱和以前的低分辨吸收光谱相一致 ;其振动 电子吸收峰位置和在激光诱导荧光光谱及光解产物谱中的峰位置相吻合 . 展开更多
关键词 利用激光腔内共振衰减技术 CH2CHO自由基 近紫外吸收光谱
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基于刻蚀反应的纳米结构空心化 被引量:1
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作者 叶祖洋 殷亚东 《高等学校化学学报》 SCIE EI CAS CSCD 北大核心 2023年第1期1-12,共12页
中空纳米材料的可控合成使其在催化、能量转换与储存、生物医药等领域具有广阔的应用前景.本专论旨在揭示刻蚀反应对纳米结构空心过程的关键影响.讨论了通过增强纳米粒子表面在刻蚀液中的相对稳定性来精确操纵中空化过程的策略,主要关注... 中空纳米材料的可控合成使其在催化、能量转换与储存、生物医药等领域具有广阔的应用前景.本专论旨在揭示刻蚀反应对纳米结构空心过程的关键影响.讨论了通过增强纳米粒子表面在刻蚀液中的相对稳定性来精确操纵中空化过程的策略,主要关注3种刻蚀策略,包括硬模板法、氧化还原辅助中空法和表面钝化自模板法.最后,对基于刻蚀反应的纳米结构空心化可控合成未来的发展方向进行了展望. 展开更多
关键词 中空结构 刻蚀 模板 自模板法 纳米合成 表面钝化
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H-atom Dissociation Channels in Ultraviolet Photochemistry of m-Pyridyl Radical
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作者 Michael Lucas Jasmine Minor +1 位作者 张劲松 Christopher Brazier 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2014年第6期621-627,I0003,共8页
The H atom production channels in the ultraviolet (UV) photochemistry of m-pyridyl radical (m-C5H4N) were investigated at excitation wavelengths from 224 nm to 248 nm by high-n Rydberg atom time-of-flight (HRTOF... The H atom production channels in the ultraviolet (UV) photochemistry of m-pyridyl radical (m-C5H4N) were investigated at excitation wavelengths from 224 nm to 248 nm by high-n Rydberg atom time-of-flight (HRTOF) technique. The photofragment yield (PFY) spectrum of the H atoms indicates a broad UV absorption feature near 234 nm. The product kinetic energy release is small; the average product kinetic energy at the wavelengths from 224 nm to 248 nm is 0.12 to 0.19 of the maximum excess energy (assuming the lowest energy product channel, H+cyanovinylacetylene). The product kinetic energy distributions are consistent with the H cyanovinylacetylene, H 3,4-pyridyne, and H 2,3-pyridyne product channels, with H cyanovinylacetylene as the main H-loss channel. The angular distributions of the H-atom products are isotropic. After the UV electronic excitation, the m-pyridyl radical undergoes internal conversion to the ground electronic state and then unimolecular dissoci-ation to the H cyanovinylacetylene, H 3,4-pyridyne, and H 2,3-pyridyne products. The dissociation mechanism of the m-pyridyl radical is similar to that of the o-pyridyl radical reported in the early study. 展开更多
关键词 PHOTOLYSIS Photofragment PYRIDYL PYRIDINE Decomposition Excited state
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Ultraviolet Photodissociation Dynamics of 1-Pentyl Radical
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作者 Ge Sun Yu Song Jingsong Zhang 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2018年第4期439-445,613,614,共9页
The ultraviolet (UV) photodissociation of jet-cooled 1-pentyl radical is investigated in the wavelength region of 236-254 nm using the high-n Rydberg-atom time-of-flight (HRTOF) technique. The H-atom photofragment... The ultraviolet (UV) photodissociation of jet-cooled 1-pentyl radical is investigated in the wavelength region of 236-254 nm using the high-n Rydberg-atom time-of-flight (HRTOF) technique. The H-atom photofragment yield spectrum of the 1-pentyl radical shows a broad UV absorption feature peaking near 245 nm, similar to the 2pz→3s absorption bands of ethyl and n-propyl. The center-of-mass translational energy distribution, P(ET), of the H+CsH10 product channel is bimodal, with a slow peak at -5 kcal/mol and a fast peak at -50 kcal/mol. The fraction of the average translational energy release in the total available energy, (fT), is 0.30, with those of the slow and fast components being 0.13 and 0.58, respectively. The slow component has an isotropic product angular distribution, while the fast component is anisotropic with an anisotropy parameter -0.4. The bimodal translational energy and angular distributions of the H+C5H10 products indicate two H-atom elimination channels in the photodissociation of 1-pentyl: (i) a direct, prompt dissociation from the electronic excited state and/or the repulsive part of the ground electronic state potential energy surface; and (ii) a unimolecular dissociation of internally hot radical in the ground electronic state after internal conversion from the electronic excited state. 展开更多
关键词 PHOTODISSOCIATION 1-Pentyl ALKYL Decomposition RYDBERG Excited state
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Two-Photon Dissociation Dynamics of Hydroxyl Radical
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作者 Ge Sun Xian-feng Zheng +4 位作者 Yuan Qin Yu Song Jingsong Zhang Jose Martin Amero Gabriel J.Vázquez 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2020年第2期129-134,I0002,共7页
Two-photon dissociation dynamics of the OH radical is studied using the high-n Rydberg atom time-of-flight(HRTOF) technique. The H(2 S)+O(1 D) and H(2 S)+O(1 S) product channels are observed in the dissociation of the... Two-photon dissociation dynamics of the OH radical is studied using the high-n Rydberg atom time-of-flight(HRTOF) technique. The H(2 S)+O(1 D) and H(2 S)+O(1 S) product channels are observed in the dissociation of the OH radical on the 22Π and B2Σ+repulsive states, respectively, from sequential two-photon excitation via the A2Σ+(v′=2, J′=0.5-2.5)state. Both H+O product channels have anisotropic angular distributions, with β=-0.97 for H(2 S)+O(1 D) and 1.97 for H(2 S)+O(1 S). The anisotropic angular distributions are consistent with a mechanism of OH direct dissociation on the repulsive potential energy curves(PECs) leading to the H+O products. The OH bond dissociation energy D0(O-H) is determined to be 35580±15 cm-1. 展开更多
关键词 PHOTODISSOCIATION Hydroxyl radical Excited state Potential energy curves
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