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Time Resolved Photochemistry in Ionic Clusters 离子团簇中的时间分辨光化学
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.sthb1
W. C. Lineberger
{"title":"Time Resolved Photochemistry in Ionic Clusters","authors":"W. C. Lineberger","doi":"10.1364/msslg.1995.sthb1","DOIUrl":"https://doi.org/10.1364/msslg.1995.sthb1","url":null,"abstract":"Ultrafast pump-probe studies of photodissociation and the subsequent recombination or photochemistry in size-selected ionic clusters (ICI-(CO2)n, I-2(CO2)n, (O2)-n) will be discussed. The experiments provide direct measurements of the effect of partial solvation on the electronic structure of the solute.","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"9 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"121204692","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Vibrational Dynamics of CO Bound to Myoglobin and Metallo-porphyrins CO与肌红蛋白和金属卟啉结合的振动动力学
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.stha3
K. Peterson, J. R. Hill, Dana D. Diott, M. Fayer
{"title":"Vibrational Dynamics of CO Bound to Myoglobin and Metallo-porphyrins","authors":"K. Peterson, J. R. Hill, Dana D. Diott, M. Fayer","doi":"10.1364/msslg.1995.stha3","DOIUrl":"https://doi.org/10.1364/msslg.1995.stha3","url":null,"abstract":"We have made direct measurements of the vibrational lifetimes of carbonmonoxide (CO) bound at the active site of wildtype myoglobin [1] and myoglobin with single residue mutations in the binding pocket. Measurements were also made for CO bound to water soluble metalloporphyrins with differing metals and peripheral substituents. A pump-probe technique using tunable microjoule pulses from an infrared free-electron laser was used to monitor the loss of vibrational energy from the CO ligand with 2 picosecond time resolution. Recovery to the CO vibrational ground state in both the protein and soluble porphyrin systems occurs in the range from 10 to 30 picoseconds. The vibrational lifetime of CO bound to myoglobin is essentially independent of temperature from 20 to 300 K.","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"36 3 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"124383297","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Degenerate Four Wave Mixing Spectroscopy of Free Radicals in Low-Pressure Plasmas 低压等离子体中自由基的简并四波混频光谱
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.ssab2
J. W. Hudgens, David S. Green
{"title":"Degenerate Four Wave Mixing Spectroscopy of Free Radicals in Low-Pressure Plasmas","authors":"J. W. Hudgens, David S. Green","doi":"10.1364/msslg.1995.ssab2","DOIUrl":"https://doi.org/10.1364/msslg.1995.ssab2","url":null,"abstract":"Four wave mixing spectroscopies offer new ways to measure chemical species in extremely hostile environments. Among the most demanding of these applications is the measurement of radical chemistry within plasmas. Most plasmas are highly luminous and are characterized by steep gradients in temperature and concentration. These hostile properties thwart fluorescence and absorption diagnostics. In addition, in many useful plasma reactors the electrodes and associated electronics impose cumbersome optical geometries. We are using degenerate four-wave mixing (DFWM) spectroscopy to sidestep these impediments and to provide sensitive and spatially resolved measurements of concentration and temperature. In conjunction with computer simulations this data will lead to a better understanding of fundamental chemistry within plasma environments. In this paper we describe proof-of-principal experiments that use NH radical spectra to profile the evolution of gas mixtures containing ammonia, hydrogen (or fluorine) and argon passed through a microwave discharge. We will also present data from similar experiments in which hydrocarbon radicals are the important reaction intermediates produced by the plasma chemistry.","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"20 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"122029449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Quantum Theory of Vibrational Relaxation in Liquids 液体振动弛豫的量子理论
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.sfb2
V. M. Kenkre
{"title":"Quantum Theory of Vibrational Relaxation in Liquids","authors":"V. M. Kenkre","doi":"10.1364/msslg.1995.sfb2","DOIUrl":"https://doi.org/10.1364/msslg.1995.sfb2","url":null,"abstract":"We present a theory of vibrational relaxation of polyatomic molecules in polyatomic solvents, which is also applicable to solid solutions, with Fermi's Golden Rule as the point of departure. We avoid rotating wave or random phase approximations, and treat both the internal degrees of freedom of the relaxing molecule and the bath degrees of freedom in a fully quantum mechanical manner. The results allow one to go beyond earlier analyses which treated only cascade processes and to consider all participating bosons. We construct the theory in a manner which facilitates the use of recent developments in the analysis of instantaneous normal modes of liquids. We address the problem of the inverted temperature dependence of the relaxation rate observed recently by Tokmakoff, Sauter and Fayer (J. Chem. Phys. 100, 9035 (1994)) and provide three different possible explanations of the phenomenon. The first is based on the temperature dependence of the density of states of the instantaneous normal modes as suggested by the authors of the experimental paper. The second stems from an energy mismatch mechanism which gives rise to dressing effects. The third arises naturally from the representation of the dynamics of the liquid in terms of anharmonic oscillators.","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"32 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"131171338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Collisional Relaxation of Highly Vibrationally Excited O2 and a Bimodal Vibrational Distribution of O2 from O3 Photolysis: A Possible Explanation of the "Ozone Deficit Problem" 高振动激发O2的碰撞弛豫和O3光解O2的双峰振动分布:“臭氧赤字问题”的一种可能解释
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.ssab3
A. Wodtke, J. M. Price, C. A. Rogaski, J. A. Mack
{"title":"Collisional Relaxation of Highly Vibrationally Excited O2 and a Bimodal Vibrational Distribution of O2 from O3 Photolysis: A Possible Explanation of the \"Ozone Deficit Problem\"","authors":"A. Wodtke, J. M. Price, C. A. Rogaski, J. A. Mack","doi":"10.1364/msslg.1995.ssab3","DOIUrl":"https://doi.org/10.1364/msslg.1995.ssab3","url":null,"abstract":"Stimulated emission pumping was used to investigate the collisional relaxation of vibrationally state selected \u0000 \u0000 \u0000 \u0000 O\u0000 2\u0000 \u0000 \u0000 (\u0000 \u0000 \u0000 X\u0000 3\u0000 \u0000 \u0000 Σ\u0000 g\u0000 −\u0000 \u0000 ,\u0000 19\u0000 ≤\u0000 v\u0000 ≤\u0000 28\u0000 \u0000 )\u0000 \u0000 \u0000 \u0000 . Strong evidence was obtained suggesting that \u0000 \u0000 \u0000 \u0000 O\u0000 2\u0000 \u0000 \u0000 (\u0000 \u0000 \u0000 X\u0000 3\u0000 \u0000 \u0000 Σ\u0000 g\u0000 −\u0000 \u0000 ,\u0000 v\u0000 ≥\u0000 26\u0000 \u0000 )\u0000 \u0000 \u0000 \u0000 reacts with O2 to form O3 + O. Collisional relaxation at lower vibrational excitation appears to agree well with theoretical models which derive effective information about the interaction potential from ab initio calculations of the (O2)2 van der Waals molecule. This remarkable result shows how existing theories designed to explain vibrational energy transfer at low excitation may be extended to the \"chemical energy regime.\" Results of recent experiments on the photolysis of ozone at 226 nm show that the vibrational distribution of the \u0000 \u0000 \u0000 \u0000 O\u0000 2\u0000 \u0000 \u0000 (\u0000 \u0000 \u0000 X\u0000 3\u0000 \u0000 \u0000 Σ\u0000 g\u0000 −\u0000 \u0000 ,\u0000 v\u0000 \u0000 )\u0000 \u0000 \u0000 \u0000 is markedly bimodal, with one peak near v = 14 and another at v = 27. The explanation of this is, as yet, completely lacking and represents an interesting fundamental problem for ab initio theory. The production of highly vibrationally excited O2 by ozone photolysis together with the reactivity of highly vibrationally excited O2 may have significant atmospheric consequences. Initial modelling results suggest that the inclusion of highly vibrationally excited O2 may reconcile the long-standing discrepancy between the predicted and observed concentrations of stratospheric ozone.","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"217 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"124283990","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Vibrational Dynamics in Electron Transfer 电子传递中的振动动力学
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.stha2
K. Spears, X. Wen
{"title":"Vibrational Dynamics in Electron Transfer","authors":"K. Spears, X. Wen","doi":"10.1364/msslg.1995.stha2","DOIUrl":"https://doi.org/10.1364/msslg.1995.stha2","url":null,"abstract":"Electron transfer is a widely studied and important phenomena with an extensive literature. The measurement of electron transfer (ET) rates as a function of vibrational state has been a long sought goal for testing the vibrational reorganization component of electron transfer. Prior insight into vibrational effects has been indirect, initially through correlations of rate versus exothermicity for a variety of compounds, and more recently through Raman spectroscopic identification of important vibrational modes. A direct electron transfer rate measurement for two vibrational states and subsequent identification of the final vibrational quantum numbers following electron transfer have been measured in our recent work for the first time.1","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"33 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"125804174","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Spectroscopy of an Electron in Zeolites: Time Domain Theory and the Modeling of the Material’s Properties 沸石中电子的光谱学:时域理论和材料性质的建模
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.sfb1
H. Metiu, N. Blake
{"title":"Spectroscopy of an Electron in Zeolites: Time Domain Theory and the Modeling of the Material’s Properties","authors":"H. Metiu, N. Blake","doi":"10.1364/msslg.1995.sfb1","DOIUrl":"https://doi.org/10.1364/msslg.1995.sfb1","url":null,"abstract":"We have developed a realistic model for the interaction of an electron or an ion with a zeolite frame and used a newly developed time dependent theory to calculate the spectroscopic properties of an electron absorbed in various zeolites.","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"45 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"125889996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Energy flow in molecular solids 分子固体中的能量流动
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.stha4
D. Dlott
{"title":"Energy flow in molecular solids","authors":"D. Dlott","doi":"10.1364/msslg.1995.stha4","DOIUrl":"https://doi.org/10.1364/msslg.1995.stha4","url":null,"abstract":"The heating and cooling of a condensed phase molecule is of considerable interest in many areas of chemistry. Owing to the short distance scale (nanometers) and time scale (picoseconds) of these processes, the conventional concepts of thermal conduction do not apply. Instead the more complicated approach of molecular mechanical energy transfer needs to be considered.","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"5 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"114138382","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
New near infrared spectra of the CH2 radical CH2自由基的新近红外光谱
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.ssaa3
Bor-Chen Chang, Ming T. Wu, G. Hall, T. Sears
{"title":"New near infrared spectra of the CH2 radical","authors":"Bor-Chen Chang, Ming T. Wu, G. Hall, T. Sears","doi":"10.1364/msslg.1995.ssaa3","DOIUrl":"https://doi.org/10.1364/msslg.1995.ssaa3","url":null,"abstract":"An analysis of the \u0000 \u0000 \u0000 \u0000 \u0000 \u0000 b\u0000 ˜\u0000 \u0000 \u0000 1\u0000 \u0000  \u0000 \u0000 B\u0000 1\u0000 \u0000 −\u0000 \u0000 \u0000 \u0000 a\u0000 ˜\u0000 \u0000 \u0000 1\u0000 \u0000  \u0000 \u0000 A\u0000 1\u0000 \u0000 \u0000 \u0000 electronic spectrum of methylene was first reported in 1966 by Herzberg and Johns.1 Since that time, numerous experimental and theoretical investigations have been carried out on this chemically important species. The two lowest singlet states in CH2 lie approximately 3000 and 12000 cm-1 above the ground \u0000 \u0000 \u0000 \u0000 \u0000 \u0000 X\u0000 ˜\u0000 \u0000 \u0000 3\u0000 \u0000  \u0000 \u0000 B\u0000 1\u0000 \u0000 \u0000 \u0000 state and correlate with a degenerate \u0000 \u0000 \u0000 \u0000 \u0000 1\u0000 \u0000 \u0000 Δ\u0000 g\u0000 \u0000 \u0000 \u0000 state at the linear configuration of the molecule. This degeneracy leads to extreme complexity in the spectrum. The \u0000 \u0000 \u0000 \u0000 a\u0000 ˜\u0000 \u0000 \u0000 \u0000 and \u0000 \u0000 \u0000 \u0000 b\u0000 ˜\u0000 \u0000 \u0000 \u0000 states may be regarded as derived from a severe Renner-Teller effect in a linear singlet CH2 molecule and the resulting vibronic structure leads to a highly irregular band system, especially at energies near to that of the degenerate linear configuration, recently2 calculated to lie some 8800 cm-1 above the zero point level of the \u0000 \u0000 \u0000 \u0000 a\u0000 ˜\u0000 \u0000 \u0000 \u0000 state. Although the visible region of the \u0000 \u0000 \u0000 \u0000 b\u0000 ˜\u0000 \u0000 −\u0000 \u0000 a\u0000 ˜\u0000 \u0000 \u0000 \u0000 spectrum has been extensively studied3,4 since the original work of Herzberg and Johns, there have been no experiments reported in the near infrared region due to less efficient dye laser operation at these wavelengths.","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"41 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"117234914","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Raman Echo Studies of Vibrational Dephasing 振动减相的拉曼回波研究
Modern Spectroscopy of Solids, Liquids, and Gases Pub Date : 1900-01-01 DOI: 10.1364/msslg.1995.stha5
M. Berg, D. V. Bout
{"title":"Raman Echo Studies of Vibrational Dephasing","authors":"M. Berg, D. V. Bout","doi":"10.1364/msslg.1995.stha5","DOIUrl":"https://doi.org/10.1364/msslg.1995.stha5","url":null,"abstract":"In the condensed phase, interaction with the environment causes vibrational dephasirtg and broadening of isotropic Raman lines. However, measurements of the Raman line width provide only a limited probe of these interactions. They cannot directly determine the lifetime of the interactions. In different language, the line width could be due to either inhomogeneous broadening (long lifetimes) or homogeneous broadening (short lifetimes).","PeriodicalId":266792,"journal":{"name":"Modern Spectroscopy of Solids, Liquids, and Gases","volume":"43 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"1900-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"132855694","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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