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arXiv:quant-ph/0302021

Theory of four-wave mixing and accompanying dissociation and population transfer controlled with laser-induced continuum structures

Victor Kimberg, A. K. Popov, Thomas F. George

Published Feb 3, 2003• 0 citations
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Abstract

A theory is developed and applied to the study of opportunities and specific features of coherent control of four-wave mixing as well as of the accompanying processes in the continuous-wave regime, which involve transitions between bound and free quantum states. Such opportunities become feasible through constructive and destructive interference of quantum pathways. Two coupling schemes of practical importance are investigated. In the first, a ladder energy level scheme, fully-resonant sum-frequency nonlinear-optical generation of short-wavelength radiation driven by several strong fields is investigated. The relaxation processes as well as absorption of the fundamental and generated radiations, which play an important role, are taken into consideration. It is shown that the generation output can be considerably increased through the appropriate adjustment of several laser-induced continuum structures. In the second, a folded scheme, a possible control of two-photon dissociation (Lambda-scheme) using auxiliary laser radiation applied to the adjacent bound-free transition (V-configuration) is investigated. Besides dissociation, the proposed method enables one to control population transfer between two upper discreet levels via the lower-energy dissociation continuum, while direct transition between these states is not allowed. The opportunities of manipulating these processes as well as of four-wave-mixing-based spectroscopy are explored both analytically and through a numerical simulation for Na_2 dimers.

DOI
10.48550/arxiv.quant-ph/0302021

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A theory is developed and applied to the study of opportunities and specific features of coherent control of four-wave mixing as well as of the accompanying processes in the continuous-wave regime, which involve transitions between bound and free quantum states. Such opportunities become feasible through constructive and destructive interference of quantum pathways. Two coupling schemes of practical importance are investigated. In the first, a ladder energy level scheme, fully-resonant sum-frequency nonlinear-optical generation of short-wavelength radiation driven by several strong fields is investigated. The relaxation processes as well as absorption of the fundamental and generated radiations, which play an important role, are taken into consideration. It is shown that the generation output can be considerably increased through the appropriate adjustment of several laser-induced continuum structures. In the second, a folded scheme, a possible control of two-photon dissociation (Lambda-scheme) using auxiliary laser radiation applied to the adjacent bound-free transition (V-configuration) is investigated. Besides dissociation, the proposed method enables one to control population transfer between two upper discreet levels via the lower-energy dissociation continuum, while direct transition between these states is not allowed. The opportunities of manipulating these processes as well as of four-wave-mixing-based spectroscopy are explored both analytically and through a numerical simulation for Na_2 dimers.
A theory of quantum control of short-wavelength sum-frequency generation, which employs the continuum states, is developed. The proposed scheme employs all-resonant coupling and trade-off optimization of the accompanying constructive and destructive quantum interference effects in the lower-order and higher-order polarizations controlled by the overlap of two autoionizinglike laser-induced continuum structures. The scheme does not rely on adiabatic passage, coherent population trapping or maximum atomic coherence as a means to facilitate maximum output. The opportunities for manipulating transparency of the medium and refractive index for the fundamental and generated radiations, as well as nonlinear polarization in the multiple-resonant medium, are shown. This opens the feasibility of creating frequency-tunable narrowband filters, polarization rotators, and dispersive elements for vacuum ultraviolet radiation. The features specific for quantum interference in Doppler-broadened media are investigated. The feasibility of almost complete conversion of long-wavelength fundamental radiation into generated short-wavelength radiation, and of a dramatic decrease in the intensity of required fundamental radiations, is shown.
Summary form only given. Atomic coherence and interference of quantum pathways provides the means to manipulate the spectral features of absorption-gain and refractive indexes as well as the nonlinear-optical response of a medium. These open opportunities for lasing without inversion, forming laser-induced transparency, for manipulating by phase matching, and for increase in output of frequency-mixing generation. Theory and first experimental evidence of laser-induced continuum structures (LICS) have been reported. In this paper we develop the theory of LICS on the case of two strong fields coupled to bound-free transitions.
We have developed a theory of three-pulse coherent control of photochemical processes. It is based on adiabatic passage and quantum coherence and interference attributed to the lower-lying dissociation continuum and excited upper discrete states, which are otherwise not connected to the ground state by one-photon transitions. Opportunities offered by the proposed scheme are demonstrated through extensive numerical simulations with the aid of a model relevant to typical experiments. The opportunities for manipulating the distribution of the population among discrete and continuous states with any necessary ratio by the end of the pulses are demonstrated.
An influence of nonlinear interference processes at quantum transitions in strong resonance electromagnetic fields on absorption, amplification and refractive indices as well as on four-wave mixing processes is investigated. Doppler broadening of the coupled transitions, incoherent excitation, relaxation processes, as well as power saturation processes associated with the coupled levels are taken into account. Both closed (ground state is involved) and open (only excited states are involved) energy level configurations are considered. Common expressions are obtained which allow to analyze the optical characteristics (including gain without inversion and enhanced refractive index at vanishing absorption) for various V, (Lambda) and H configurations of interfering transitions by a simple substitution of parameters. Similar expressions for resonant four-wave mixing (FWM) in Raman configurations are derived too. Crucial role of Doppler broadening is shown. Theory is applied for numerical analysis of some recent and potential experiments.
A scheme is analyzed for effcient generation of vacuum ultraviolet radiation through four-wave mixing processes assisted by the technique of Stark-chirped rapid adiabatic passage. These opportunities are associated with pulse excitation of laddertype short-wavelength two-photon atomic or molecular transitions so that relaxation processes can be neglected. In this three-laser technique, a delayed-pulse of strong oR-resonant infrared radiation sweeps the laser-induced Stark-shift of a two-photon transition in a such way that facilitates robust maximum two-photon coherence induced by the first ultraviolet laser. A judiciously delayed third pulse scatters at this coherence and generates short-wavelength radiation. A theoretical analysis of these problems based on the density matrix is performed. A numerical model is developed to carry out simulations of a typical experiment. The results illustrate a behavior of populations, coherence and generated radiation along the medium as well as opportunities of effcient generation of deep (vacuum) ultraviolet radiation.