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Coherent Radiative Control of Chemical Reactions

Paul W. Brumer

Published Jan 1, 1992• 0 citations
OpenAlex

Abstract

Abstract : We continue research on our approach to the coherent radiative control of molecular processes. Our focus remains, as in the past, on extending the general theory and on theoretically designing laboratory scenarios for displaying control. The latter also entails a significant effort to minimize effects which tend to diminish dephasing, thermal population distributions and partial laser coherence. We have, during the course of this grant period, done several seminal pieces of research which both extend the theory and provide the basis for considerably greater advances in the near future. jg p.8

Related papers

Laser control of chemical reactions in a thermal environment

Zhidang Chen, Moshe Shapiro, Paul W. Brumer

Coherent radiative control is a quantum-interference based approach to controlling molecular processes by the use of coherent radiation. A method of carrying out such control in the presence of thermal broadening effects and laser jitter is described and applied to the photodissociation of Na2.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Jan 5, 1994•0 citations

Coherent effects in laser chemistry

Moshe Shapiro, Paul W. Brumer

We describe the current status of coherent radiative control, a quantum-interference based approach to controlling molecular processes by the use of coherent radiation. In addition to providing an overview of proposed laboratory scenarios, ongoing experimental studies and recent theoretical developments, we call attention to recent theoretical results on symmetry breaking in achiral systems.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Apr 1, 1992•0 citations

Experimental investigations of coherent control

Daniel S. Elliott, Ce Chen, Yi-Yian Yin +3 more

The potential of using interferences between transition amplitudes for the coherent control of photoionization rates and of asymmetric photoelectron angular distributions has been demonstrated previously. Current efforts in our laboratories are directed toward control of photoionization of NO, and on control of photoionization channels in atomic barium. This latter system is, of course, much simpler than a molecular system, and thus may provide better insight into the mechanisms involved. We will discuss our investigations of the effects of nonlinear coupling, absorption, and dispersion of the laser beams on their propagation through dense media, as observed via interference effects. Laser band structure effects and the effect of Doppler broadening will also be discussed.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Jun 17, 1994•0 citations

Coherent control and geometric phase

Xuan Li

We present the ability to coherently control triatomic chemical reactions with pulsed-laser techniques. We show that one can control the final state probability distribution of triatomic chemical reactions with nearly 100% selectivity. We develop the population transfer by adiabatic passage theory to coherently control the chemical reaction with the ability of choosing the translational energies of the final reaction products. We also show a new way to achieve the creation of both homonuclear and heteronuclear diatomic molecules at an ultracold temperature using laser catalysis.

•Jan 1, 2008•2 citations

Introduction

Bruce W. Shore

The quantum world within an atom or molecule that once attracted explorations only by academic physicists now provides fertile sustenance for chemists seeking control of chemical reactions and for engineers developing ever smaller electronic devices or tools for processing information with greater security. Whereas the first pioneers could only discover the most elementary properties – the discrete energy levels that characterize the internal structures of atoms and the radiative transitions that link these structures to our external world – it is now possible to alter that structure at will, albeit briefly. Objective This monograph presents the physical principles that describe such deliberately crafted changes, namely how single atoms or molecules (or other simple quantum systems) are affected by coherent interactions, primarily laser light – a subject that has been regarded first as a part of quantum electronics and then quantum optics but is most generally described as coherent atomic excitation [Sho90]. This physics has relevance to such basic concerns as the detection and quantitative analysis of trace amounts of chemicals, the catalysis or control of chemical reactions, the alignment of molecules, and the processing of quantum information. The physics necessarily involves elementary quantum mechanics, but it has many associations to the classical dynamics that governs macroscopic objects – waves and particles. The mathematics that quantifies the changes is that of differential equations, specifically coupled ordinary differential equations (ODEs), whose parameters incorporate the controls of experimenters and whose solutions, appropriately interpreted, quantify the resulting changes.

Cambridge University Press eBooks•Sep 29, 2011•6 citations

Cold Controlled Chemistry

Roman V. Krems

Collisions of molecules in a thermal gas are difficult to control. Thermal motion randomizes molecular encounters and diminishes the effects of external radiation or static electromagnetic fields on intermolecular interactions. The effects of the thermal motion can be reduced by cooling molecular gases to low temperatures. At temperatures near or below 1 K, the collision energy of molecules becomes less significant than perturbations due to external fields. At the same time, inelastic scattering and chemical reactions may be very efficient in low-temperature molecular gases. The purpose of this article is to demonstrate that collisions of molecules at temperatures below 1 K can be manipulated by external electromagnetic fields and to discuss possible applications of cold controlled chemistry. The discussion focuses on molecular interactions at cold (0.001-2 K) and ultracold (<0.001 K) temperatures and is based on both recent theoretical and experimental work. The article concludes with a summary of current challenges for theory and experiment in the research of cold molecules and cold chemistry.

Bulletin of the American Physical Society•May 31, 2008•7 citations
Abstract : We continue research on our approach to the coherent radiative control of molecular processes. Our focus remains, as in the past, on extending the general theory and on theoretically designing laboratory scenarios for displaying control. The latter also entails a significant effort to minimize effects which tend to diminish dephasing, thermal population distributions and partial laser coherence. We have, during the course of this grant period, done several seminal pieces of research which both extend the theory and provide the basis for considerably greater advances in the near future. jg p.8
The potential of using interferences between transition amplitudes for the coherent control of photoionization rates and of asymmetric photoelectron angular distributions has been demonstrated previously. Current efforts in our laboratories are directed toward control of photoionization of NO, and on control of photoionization channels in atomic barium. This latter system is, of course, much simpler than a molecular system, and thus may provide better insight into the mechanisms involved. We will discuss our investigations of the effects of nonlinear coupling, absorption, and dispersion of the laser beams on their propagation through dense media, as observed via interference effects. Laser band structure effects and the effect of Doppler broadening will also be discussed.
We present the ability to coherently control triatomic chemical reactions with pulsed-laser techniques. We show that one can control the final state probability distribution of triatomic chemical reactions with nearly 100% selectivity. We develop the population transfer by adiabatic passage theory to coherently control the chemical reaction with the ability of choosing the translational energies of the final reaction products. We also show a new way to achieve the creation of both homonuclear and heteronuclear diatomic molecules at an ultracold temperature using laser catalysis.
The quantum world within an atom or molecule that once attracted explorations only by academic physicists now provides fertile sustenance for chemists seeking control of chemical reactions and for engineers developing ever smaller electronic devices or tools for processing information with greater security. Whereas the first pioneers could only discover the most elementary properties – the discrete energy levels that characterize the internal structures of atoms and the radiative transitions that link these structures to our external world – it is now possible to alter that structure at will, albeit briefly. Objective This monograph presents the physical principles that describe such deliberately crafted changes, namely how single atoms or molecules (or other simple quantum systems) are affected by coherent interactions, primarily laser light – a subject that has been regarded first as a part of quantum electronics and then quantum optics but is most generally described as coherent atomic excitation [Sho90]. This physics has relevance to such basic concerns as the detection and quantitative analysis of trace amounts of chemicals, the catalysis or control of chemical reactions, the alignment of molecules, and the processing of quantum information. The physics necessarily involves elementary quantum mechanics, but it has many associations to the classical dynamics that governs macroscopic objects – waves and particles. The mathematics that quantifies the changes is that of differential equations, specifically coupled ordinary differential equations (ODEs), whose parameters incorporate the controls of experimenters and whose solutions, appropriately interpreted, quantify the resulting changes.
Collisions of molecules in a thermal gas are difficult to control. Thermal motion randomizes molecular encounters and diminishes the effects of external radiation or static electromagnetic fields on intermolecular interactions. The effects of the thermal motion can be reduced by cooling molecular gases to low temperatures. At temperatures near or below 1 K, the collision energy of molecules becomes less significant than perturbations due to external fields. At the same time, inelastic scattering and chemical reactions may be very efficient in low-temperature molecular gases. The purpose of this article is to demonstrate that collisions of molecules at temperatures below 1 K can be manipulated by external electromagnetic fields and to discuss possible applications of cold controlled chemistry. The discussion focuses on molecular interactions at cold (0.001-2 K) and ultracold (<0.001 K) temperatures and is based on both recent theoretical and experimental work. The article concludes with a summary of current challenges for theory and experiment in the research of cold molecules and cold chemistry.