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Title: Feasibility and advantages of off-resonance lasers in chemically reacting systems

Abstract

The problem of understanding the semiclassical description of the time evolution of an ensemble of two state systems under the influence of a coherent radiation field is of considerable importance. Previous attempts to deal with these problems have dealt with either broad pulses or ultrashort pulses which allow the use of the rate equations or finite phase memory to be incorporated into the description. In neither case, however, has the effect of incoherent feeding and off-resonance effects in a coherently driven two-level system been analyzed. A closed form solution that includes the effects of relaxation and spontaneous emission between the two levels has been obtained for the general case when the ensemble is being incoherently fed from a population reservoir, as would be the case, for example, in a chemical laser. In addition to providing a basis for understanding the modifications which occur for such a system, the mathematical formulation predicts that an important effect may be observed. This effect, which is termed ''kinetic coherence,'' is the production of a long-term coherent component that results directly from the kinetic feeding. The magnitude of the component is related to the rate of creating excited states, relaxation pathways and the off-resonance frequency.more » It is shown how, in principle, it is possible to utilize these off-resonance effects in any inhomogeneously broadened system to significantly overcome the losses from T$sub 2$ relaxation processes and to provide an experimental system capable of controlling the relative ratio of spontaneous and stimulated emission. Finally, the relationships between chemical kinetics, the off-resonance feature and sustained self-regulation in a system exhibiting gain are discussed. (auth)« less

Authors:
Publication Date:
Research Org.:
California Univ., Berkeley (USA). Lawrence Berkeley Lab.
OSTI Identifier:
4187457
Report Number(s):
LBL-3916; CONF-750683-1
NSA Number:
NSA-33-005406
DOE Contract Number:
W-7405-ENG-48
Resource Type:
Technical Report
Resource Relation:
Conference: 27. international meeting of the Societe de Chimie Physique, Paris, France, 17 Jun 1975; Other Information: Orig. Receipt Date: 30-JUN-76
Country of Publication:
United States
Language:
English
Subject:
N42210* -Engineering-Facilities & Equipment-Lasers; 420300* -Engineering-Lasers; *CHEMICAL LASERS; REACTION KINETICS; RESONANCE; TIME DEPENDENCE

Citation Formats

Harris, C.B. Feasibility and advantages of off-resonance lasers in chemically reacting systems. United States: N. p., 1975. Web. doi:10.2172/4187457.
Harris, C.B. Feasibility and advantages of off-resonance lasers in chemically reacting systems. United States. doi:10.2172/4187457.
Harris, C.B. Sun . "Feasibility and advantages of off-resonance lasers in chemically reacting systems". United States. doi:10.2172/4187457. https://www.osti.gov/servlets/purl/4187457.
@article{osti_4187457,
title = {Feasibility and advantages of off-resonance lasers in chemically reacting systems},
author = {Harris, C.B.},
abstractNote = {The problem of understanding the semiclassical description of the time evolution of an ensemble of two state systems under the influence of a coherent radiation field is of considerable importance. Previous attempts to deal with these problems have dealt with either broad pulses or ultrashort pulses which allow the use of the rate equations or finite phase memory to be incorporated into the description. In neither case, however, has the effect of incoherent feeding and off-resonance effects in a coherently driven two-level system been analyzed. A closed form solution that includes the effects of relaxation and spontaneous emission between the two levels has been obtained for the general case when the ensemble is being incoherently fed from a population reservoir, as would be the case, for example, in a chemical laser. In addition to providing a basis for understanding the modifications which occur for such a system, the mathematical formulation predicts that an important effect may be observed. This effect, which is termed ''kinetic coherence,'' is the production of a long-term coherent component that results directly from the kinetic feeding. The magnitude of the component is related to the rate of creating excited states, relaxation pathways and the off-resonance frequency. It is shown how, in principle, it is possible to utilize these off-resonance effects in any inhomogeneously broadened system to significantly overcome the losses from T$sub 2$ relaxation processes and to provide an experimental system capable of controlling the relative ratio of spontaneous and stimulated emission. Finally, the relationships between chemical kinetics, the off-resonance feature and sustained self-regulation in a system exhibiting gain are discussed. (auth)},
doi = {10.2172/4187457},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Sun Jun 01 00:00:00 EDT 1975},
month = {Sun Jun 01 00:00:00 EDT 1975}
}

Technical Report:

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  • This report presents the mathematical bases for measuring internal temperatures within batch and flowing systems using chemically reacting tracers. This approach can obtain temperature profiles of plug-flow systems and temperature histories within batch systems. The differential equations for reactant conversion can be converted into Fredholm integral equations of the first kind. The experimental variable is the tracer-reaction activation energy. When more than one tracer is used, the reactions must have different activation energies to gain information. In systems with temperature extrema, multiple solutions for the temperature profiles or histories can exist, When a single parameter in the temperature distribution ismore » needed, a single-tracer test may furnish this information. For multi-reaction tracer tests, three Fredholm equations are developed. Effects of tracer-reaction activation energy, number of tracers used, and error in the data are evaluated. The methods can determine temperature histories and profiles for many existing systems, and can be a basis for analysis of the more complicated dispersed-flow systems. An alternative to using the Fredholm-equation approach is the use of an assumed temperature- distribution function and incorporation of this function into the basic integral equation describing tracer behavior. The function contains adjustable parameters which are optimized to give the temperature distribution. The iterative Fredholm equation method is tested to see what is required to discriminate between two models of the temperature behavior of Hot Dry Rock (HDR) geothermal reservoirs. Experimentally, ester and amide hydrolyses are valid HDR tracer reactions for measuring temperatures in the range 75-100{degrees}C. Hydrolyses of bromobenzene derivatives are valid HDR tracer reactions for measuring temperatures in the range 150-275{degrees}C.« less
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