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AIP conference proceedings

Coherent Control of Extreme Nonlinear Optical Properties of Quantum System via Ultrashort Laser Pulses

Shangqing Gong, Keyu Xia, Yueping Niu, Theodore E. Simos, George Maroulis

Published Jan 1, 2007• 0 citations
Publisher

Abstract

We investigate the extreme nonlinear optical properties of quantum system driven by ultrashort laser pulses by solving the one and two dimensional, full‐wave Maxwell‐Bloch coupled equations. We find that the near‐dipole‐dipole (NDD) interactions have a crucial influence on the absolute phase of few‐cycle laser pulses. The difference of the absolute phase between the cases with and without NDD effects can go up to π. Moreover, a novel ultrafast transient population grating induced by a two‐dimensional, ultrashort dipole soliton is demonstrated. The number of lines and the period of the grating can be controlled by the beam waist and the area of the pulse.

DOI
10.1063/1.2836203

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We investigate the extreme nonlinear optical properties of quantum system driven by ultrashort laser pulses by solving the one and two dimensional, full‐wave Maxwell‐Bloch coupled equations. We find that the near‐dipole‐dipole (NDD) interactions have a crucial influence on the absolute phase of few‐cycle laser pulses. The difference of the absolute phase between the cases with and without NDD effects can go up to π. Moreover, a novel ultrafast transient population grating induced by a two‐dimensional, ultrashort dipole soliton is demonstrated. The number of lines and the period of the grating can be controlled by the beam waist and the area of the pulse.
An ultrafast transient population grating induced by a (1+1)(1+1)(1+1)-dimensional, ultrashort dipole soliton is demonstrated by solving the full-wave Maxwell-Bloch equations. The number of lines and the period of the grating can be controlled by the beam waist and the area of the pulse. Of interest is that a polarization grating is produced. A coherent control scheme based on these phenomena can be contemplated as ultrafast transient grating techniques.
The four-wave mixing produced with two ultrashort phase-locked !-3! laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5! anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques. Phenomena arising from the coherent control of nonlinear interactions are of importance in fields as diverse as optoelectronics and materials research, in high harmonic generation, in photoionization or molecular dissociation, and in biological applications such as spectroscopy and imaging, among others [1, 2, 3, 4, 5, 6, 7]. Optical quantum coherent control is based on the fact that the phases of interfering transition amplitudes in light-matter interactions can be controlled through the optical phase of coherent light sources that drive the interaction, in such a way that the transition rates to final states and the dynamics at various stages of the process can be modified [1]. In a recent paper [8], a theoretical investigation on the quantum coherent control of the optical transient four-wave mixing of two intense phase-locked femtosecond laser pulses of central angular frequencies ω and 3ω propagating in a two-level atom (TLA) was reported. It was shown how the nonlinear (χ (3) ) coupling to the antiStokes Raman field at frequency 5ω depends critically on the initial relative phase φ of the propagating pulses. In Ref. [8], the study was centered to intense pulses in the visible and ultraviolet spectral regions, with frequencies at resonance or lower than the atomic transition. The phenomena observed in [8], however, can be scaled to various laser and material parameters. In the infrared spectral range, for instance, experiments on ultrafast molecular dynamics are frequently performed by help of twocolor pump probe nonlinear spectroscopy techniques. In this type of studies, due to the high intensities inherent to ultrashort (subpicosecond) pulses, nonlinear effects such as stimulated Raman processes may become important and are often utilized as a complementary tool to gain information [9]. In this Letter, we address the conditions for quantum coherent control of transient four-wave mixing interactions with two phase-locked ω-3ω femtosecond laser pulses in the mid-IR spectral region. Our purpose is to reveal the basic physics for a strict two-level medium and to this end the Maxwell-Bloch TLA will be considered. We will study pulses with a duration of 300 fs (with a w 5w
Creation, erasing and ultrafast control of population density gratings using few-cycle optical pulses coherently interacting with resonant medium is discussed. In contrast to the commonly used schemes, here the pulses do not need to overlap in the medium, interaction between the pulses is mediated by excitation of polarization waves. We investigate the details of the dynamics arising in such ultrashort pulse scheme and develop an analytical theory demonstrating the importance of the phase memory effects in the dynamics.
A theoretical investigation on the coherent control of optical transient four-wave mixing interactions in two-level systems with two intense few-cycle propagating laser pulses of central angular frequencies $\ensuremath{\omega}$ and $3\ensuremath{\omega}$ is reported. By numerically solving the full Maxwell-Bloch equations beyond the slowly varying envelope and rotating-wave approximations in the time domain, the nonlinear coupling to the optical field at frequency $5\ensuremath{\omega}$ is found to depend critically on the initial relative phase $\ensuremath{\phi}$ of the propagating pulses: the coupling is enhanced when the pulses interfere constructively in the center $(\ensuremath{\phi}=0)$, while it is nearly suppressed when they are out of phase $(\ensuremath{\phi}=\ensuremath{\pi})$.
The four-wave mixing produced with two ultrashort phase-locked w-3w laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5w anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques.