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Physical Review A

Quantum-mechanical interference between optical transitions and the effect of laser phase noise

James C. Camparo, P. Lambropoulos

Published Jan 1, 1997• 13 citations
Publisher

Abstract

We consider three-photon--one-photon phase control of resonance-enhanced photonioization with a phase-diffusion field. As is well known, control is achieved because excitation via the fundamental field interferes with excitation via the third harmonic field, and the form of the interference (i.e., constructive or destructive) depends on the relative phase difference between the two fields. In the problem, the stochastic nature of the field influences control because the propagation constant of a dispersive medium depends on the field's fluctuating frequency. Here, we approach the influence of laser phase noise on control via (i) a physically intuitive zeroth-order approximation, (ii) first-order perturbation theory, and (iii) numerical simulation. Our results show that first-order perturbation theory is not attractive for the study of this problem, since it requires the evaluation of very high order correlation functions associated with the fundamental field"s fluctuating frequency. More importantly, however, numerical simulation demonstrates that highly efficient control can be attained even in the presence of very large linewidth fields.

DOI
10.1103/physreva.55.552

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Quantum-mechanical interference between optical transitions: The effect of laser intensity noise

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In a previous publication [Phys. Rev. A 55, 552 (1997)] we considered the effect of laser phase fluctuations on three-photon--one-photon phase control of resonance-enhanced photoionization. Here we extend those studies by considering the role of laser intensity noise in addition to laser phase noise. While our results indicate that relative intensity fluctuations between the fundamental field and its third harmonic have a significant effect on control, the contrast between constructive and destructive interference is nonetheless two orders of magnitude, even under (reasonable) worst case situations. Consequently, neither laser intensity nor phase fluctuations appear to pose a serious impediment to the efficient phase control of atomic and molecular processes.

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Summary form only given. The destructive quantum interference of resonantly excited transitions within a lambda-system in case of two photon resonance leads to a medium, which is coherently prepared in a superpositional dark state. The corresponding distinct enhancement of radiation transmission is well known as electromagnetically induced transparency. Interaction of quantized fields with such a medium yields a correlation of quantum phase fluctuations of the fields even for independent cw lasers. The experiments are done on the Na D/sub 1/ line by means of a temperature stabilized sodium vapor cell. One frequency component is modulated by a broad spectrum of phase fluctuations of about 50 MHz width by means of an electrooptical phase modulator driven by a noise generator. A transfer of noise to the other frequency components within a lambda- or a closed double-lambda transition scheme during transmission through the dark state medium is observed using the heterodyne spectroscopy. The verified exponential decay of the width of the beat signal in dependence on the medium optical density proofs the noise transfer and hence the correlation of phase fluctuations between the corresponding frequency components. This behaviour as well as the different limits of decay for lambda- (towards the transparency linewidth) and closed double-lambda (towards zero) scheme is in good qualitative agreement with the theory.

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We consider effects which occur when four-wave sum frequency generation and multiphoton ionization are induced by lasers tuned near a three-photon resonance and simultaneously near or at a dipole allowed four-photon resonance. In studies with unfocused laser beams, if the phase mismatch of the generated four-wave-mixing field is large and the related two-photon resonance for the absorption of a four-wave-mixing photon and a laser photon results in strong absorption of the four-wave-mixing field, a coherent cancellation occurs between the pumping of the resonance by two- and four-photon processes. This interference effect occurs when the first laser is tuned on either side of the three-photon resonance and \ensuremath{\Vert}\ensuremath{\Delta}${\mathit{k}}_{\mathit{r}}$L\ensuremath{\Vert}\ensuremath{\gg}1, where \ensuremath{\Delta}${\mathit{k}}_{\mathit{r}}$ is the mismatch and L is the length of the path of the laser beams in the gas. With focused laser beams large differences occur between ionization with unidirectional beams and with counterpropagating laser beams when \ensuremath{\Vert}\ensuremath{\Delta}${\mathit{k}}_{\mathit{r}}$b\ensuremath{\Vert}\ensuremath{\gg}1, where b is the confocal parameter of the focused laser beams. Strong absorption of the four-wave-mixing field is shown not to be necessary for strong destructive interference with focused laser beams when the phase mismatch is large. This work also suggests an explanation for earlier experiments where the presence of a four-photon resonance enabled the generation of third-harmonic light in a positively dispersive wavelength region. We argue that this process can occur when the laser used to achieve the four-photon resonance is focused on the small z (z is the coordinate in the direction of propagation) side of the focal point of the laser responsible for the third-harmonic generation. In this way the absorption of the third-harmonic light on one side of the focal point is made much stronger than on the other side. Correspondingly, contributions to the third-harmonic field from the two sides of the focal point are unequal and cannot undergo complete destructive interference as would otherwise occur in a positively dispersive region.

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Phase-dependent atomic coherence and interference in multi-level atomic systems

Jiepeng Zhang, Yifu Zhu

Atomic coherence and interference manifested by electromagentically induced transparency (EIT) and coherent population trapping (CPT) plays an important role in the current studies of atom-photon interactions and has found numerous applications in optical physics. EIT is created in a three-level atomic system by a coupling field and results in destructive interference between two excitation paths of a weak probe laser interacting with the atomic medium. This leads to suppressed linear absorption and rapidly varying atomic dispersion for the probe laser near the atomic resonance, which provides the platform for a variety of applications such as nonlinear optics at low light levels, slow light manipulation, and quantum state engineering for photons and atoms. Here we extend the simple three-level EIT system to more complicated and versatile configurations in a multi-level atomic system coupled by multiple laser fields. We show that with multiple excitation paths provided by different laser fields, phase-dependent quantum interference is induced: either constructive or destructive interference can be realized by varying the relative phases among the laser fields. Two specific examples are discussed. One is a three-level system coupled by bichromatic coupling and probe fields, in which the phase dependent interference between the resonant two-photon Raman transitions can be initiated and controlled. Another is a four-level system coupled by two coupling fields and two probe fields, in which a double-EIT configuration is created by the phase-dependent interference between three-photon and one-photon excitation processes. We analyze the coherently coupled multi-level atomic system and discuss the control parameters for the onset of constructive or destructive quantum interference. We describe two experiments performed with cold Rb atoms that can be approximately treated as the coherently coupled three-level and four-level atomic systems respectively. The experimental results show the phase-dependent quantum coherence and interference in the multi-level Rb atomic system, and agree with the theoretical calculations based on the coherently coupled three-level or four-level model system.

BENTHAM SCIENCE PUBLISHERS eBooks•Jan 1, 2009•0 citations
We consider three-photon--one-photon phase control of resonance-enhanced photonioization with a phase-diffusion field. As is well known, control is achieved because excitation via the fundamental field interferes with excitation via the third harmonic field, and the form of the interference (i.e., constructive or destructive) depends on the relative phase difference between the two fields. In the problem, the stochastic nature of the field influences control because the propagation constant of a dispersive medium depends on the field's fluctuating frequency. Here, we approach the influence of laser phase noise on control via (i) a physically intuitive zeroth-order approximation, (ii) first-order perturbation theory, and (iii) numerical simulation. Our results show that first-order perturbation theory is not attractive for the study of this problem, since it requires the evaluation of very high order correlation functions associated with the fundamental field"s fluctuating frequency. More importantly, however, numerical simulation demonstrates that highly efficient control can be attained even in the presence of very large linewidth fields.
In a previous publication [Phys. Rev. A 55, 552 (1997)] we considered the effect of laser phase fluctuations on three-photon--one-photon phase control of resonance-enhanced photoionization. Here we extend those studies by considering the role of laser intensity noise in addition to laser phase noise. While our results indicate that relative intensity fluctuations between the fundamental field and its third harmonic have a significant effect on control, the contrast between constructive and destructive interference is nonetheless two orders of magnitude, even under (reasonable) worst case situations. Consequently, neither laser intensity nor phase fluctuations appear to pose a serious impediment to the efficient phase control of atomic and molecular processes.
Summary form only given. The destructive quantum interference of resonantly excited transitions within a lambda-system in case of two photon resonance leads to a medium, which is coherently prepared in a superpositional dark state. The corresponding distinct enhancement of radiation transmission is well known as electromagnetically induced transparency. Interaction of quantized fields with such a medium yields a correlation of quantum phase fluctuations of the fields even for independent cw lasers. The experiments are done on the Na D/sub 1/ line by means of a temperature stabilized sodium vapor cell. One frequency component is modulated by a broad spectrum of phase fluctuations of about 50 MHz width by means of an electrooptical phase modulator driven by a noise generator. A transfer of noise to the other frequency components within a lambda- or a closed double-lambda transition scheme during transmission through the dark state medium is observed using the heterodyne spectroscopy. The verified exponential decay of the width of the beat signal in dependence on the medium optical density proofs the noise transfer and hence the correlation of phase fluctuations between the corresponding frequency components. This behaviour as well as the different limits of decay for lambda- (towards the transparency linewidth) and closed double-lambda (towards zero) scheme is in good qualitative agreement with the theory.
Summary form only given. The destructive quantum interference of resonantly excited transitions within a lambda-system in case of two photon resonance leads to a medium, which is coherently prepared in a superpositional dark state. The corresponding distinct enhancement of radiation transmission is well known as electromagnetically induced transparency. Interaction of quantized fields with such a medium yields a correlation of quantum phase fluctuations of the fields even for independent cw lasers. The experiments are done on the Na D/sub 1/ line by means of a temperature stabilized sodium vapor cell. One frequency component is modulated by a broad spectrum of phase fluctuations of about 50 MHz width by means of an electrooptical phase modulator driven by a noise generator. A transfer of noise to the other frequency components within a lambda- or a closed double-lambda transition scheme during transmission through the dark state medium is observed using the heterodyne spectroscopy. The verified exponential decay of the width of the beat signal in dependence on the medium optical density proofs the noise transfer and hence the correlation of phase fluctuations between the corresponding frequency components. This behaviour as well as the different limits of decay for lambda- (towards the transparency linewidth) and closed double-lambda (towards zero) scheme is in good qualitative agreement with the theory.
A time-dependent approach to study phase control over molecular photoabsorption, provided by intense laser pulses, is elaborate. The method allows for the decay linewidth of molecular states and frequency bandwidth of the controlling laser field, and can be applied in weak and strong laser fields where the perturbation theory is invalid. It is shown that a frequency mismatch between the fundamental laser wave and its third harmonic can destroy control. For the example of the one-photon versus three-photon control a simple picture of interference from two monochromatic absorption pathways is not enough to explain phase control and one needs to consider a nonlinear temporal interference of multiquantum transitions. In the perturbation-theory limit an elegant generalization of the famous Shapiro-Hepburn-Brumer equation for the one-photon versus three-photon control is derived. Various numerical calculations illustrate the dependence of phase control on molecular linewidth, fundamental laser wavelength, pulse duration, and peak intensity. It is obtained, that the one-photon versus three-photon control is productive if the molecular state populations, individually produced by each laser wave, have beats of approximately the same frequency. The calculations demonstrate that an enough intense optical pulse can suppress molecular decay and may be used in order to keep stable the state population of a decaying molecule for a long time. The available experimental results for the one-photon versus three-photon control over simple and large polyatomic molecules are analyzed and recommendations for the experimental improvement of control are formulated.
We consider effects which occur when four-wave sum frequency generation and multiphoton ionization are induced by lasers tuned near a three-photon resonance and simultaneously near or at a dipole allowed four-photon resonance. In studies with unfocused laser beams, if the phase mismatch of the generated four-wave-mixing field is large and the related two-photon resonance for the absorption of a four-wave-mixing photon and a laser photon results in strong absorption of the four-wave-mixing field, a coherent cancellation occurs between the pumping of the resonance by two- and four-photon processes. This interference effect occurs when the first laser is tuned on either side of the three-photon resonance and \ensuremath{\Vert}\ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​L\ensuremath{\Vert}\ensuremath{\gg}1, where \ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​ is the mismatch and L is the length of the path of the laser beams in the gas. With focused laser beams large differences occur between ionization with unidirectional beams and with counterpropagating laser beams when \ensuremath{\Vert}\ensuremath{\Delta}kr{\mathit{k}}_{\mathit{r}}kr​b\ensuremath{\Vert}\ensuremath{\gg}1, where b is the confocal parameter of the focused laser beams. Strong absorption of the four-wave-mixing field is shown not to be necessary for strong destructive interference with focused laser beams when the phase mismatch is large. This work also suggests an explanation for earlier experiments where the presence of a four-photon resonance enabled the generation of third-harmonic light in a positively dispersive wavelength region. We argue that this process can occur when the laser used to achieve the four-photon resonance is focused on the small z (z is the coordinate in the direction of propagation) side of the focal point of the laser responsible for the third-harmonic generation. In this way the absorption of the third-harmonic light on one side of the focal point is made much stronger than on the other side. Correspondingly, contributions to the third-harmonic field from the two sides of the focal point are unequal and cannot undergo complete destructive interference as would otherwise occur in a positively dispersive region.
Atomic coherence and interference manifested by electromagentically induced transparency (EIT) and coherent population trapping (CPT) plays an important role in the current studies of atom-photon interactions and has found numerous applications in optical physics. EIT is created in a three-level atomic system by a coupling field and results in destructive interference between two excitation paths of a weak probe laser interacting with the atomic medium. This leads to suppressed linear absorption and rapidly varying atomic dispersion for the probe laser near the atomic resonance, which provides the platform for a variety of applications such as nonlinear optics at low light levels, slow light manipulation, and quantum state engineering for photons and atoms. Here we extend the simple three-level EIT system to more complicated and versatile configurations in a multi-level atomic system coupled by multiple laser fields. We show that with multiple excitation paths provided by different laser fields, phase-dependent quantum interference is induced: either constructive or destructive interference can be realized by varying the relative phases among the laser fields. Two specific examples are discussed. One is a three-level system coupled by bichromatic coupling and probe fields, in which the phase dependent interference between the resonant two-photon Raman transitions can be initiated and controlled. Another is a four-level system coupled by two coupling fields and two probe fields, in which a double-EIT configuration is created by the phase-dependent interference between three-photon and one-photon excitation processes. We analyze the coherently coupled multi-level atomic system and discuss the control parameters for the onset of constructive or destructive quantum interference. We describe two experiments performed with cold Rb atoms that can be approximately treated as the coherently coupled three-level and four-level atomic systems respectively. The experimental results show the phase-dependent quantum coherence and interference in the multi-level Rb atomic system, and agree with the theoretical calculations based on the coherently coupled three-level or four-level model system.