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arXiv:0711.4037 · Physical Review A

Nonlinear effects in pulse propagation through Doppler-broadened closed-loop atomic media

Robert Fleischhaker, Jörg Evers

Published Apr 3, 2008• 28 citations
arXivHTMLPDF

Abstract

Nonlinear effects in pulse propagation through a medium consisting of four-level double-$\ensuremath{\Lambda}$-type systems are studied theoretically. We apply three continuous-wave driving fields and a pulsed probe field such that they form a closed interaction loop. Due to the closed loop and the finite frequency width of the probe pulses, the multiphoton resonance condition cannot be fulfilled, such that a time-dependent analysis is required. By identifying the different underlying physical processes we determine the parts of the solution relevant to calculate the linear and nonlinear response of the system. We find that the system can exhibit a strong intensity-dependent refractive index with small absorption over a range of several natural linewidths. For a realistic example we include Doppler and pressure broadening and calculate the nonlinear self-phase modulation in a gas cell with sodium vapor and argon buffer gas. We find that a self-phase modulation of $\ensuremath{\pi}$ is achieved after the propagation of a few centimeters through the medium while the absorption and pulse shape distortion in the corresponding spectral range is small.

DOI
10.1103/physreva.77.043805

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The present thesis is devoted to theoretical studies of pulse propagation of light through linear and nonlinear media, and of light-induced nuclear dynamics. The first part of the thesis addresses propagation of light pulses in linear periodical media - photonic crystals. The main accent was put on studies of the angular properties of two qualitatively different types of photonic crystals: holographic photonic crystals, and impurity band based photonic crystals. The anisotropy of band structure, group velocity and pulse delay with respect to the light polarization are analyzed. In the second part of the thesis a strict theory of nonlinear propagation of a few strong interacting light beams is presented. The key idea of this approach is a self-consistent solution of the nonlinear wave equation and the density matrix equations of the material. This technique is applied to studies of dynamics of cavityless lasing generated by ultra-fast multi-photon excitation. It is shown that interaction of co- and counter-propagating pulses of amplified spontaneous emission (ASE) affects the dynamics and efficiency of nonlinear conversion. Our dynamical theory allows to explain the asymmetric spectral properties of the forward and backward ASE pulses, which were observed in recent experiment with different dye molecules. It is shown that the ASE spectral profile changes drastically when the pump intensity approaches the threshold level. The effect of the temporal self-pulsation of ASE is studied in detail. The third part of the thesis is devoted to light-induced nuclear dynamics. Time- and frequency-resolved X-ray spectroscopy of molecules driven by strong and coherent infrared (IR) pulses shows that the phase of the IR field strongly influences the trajectory of the nuclear wave packet, and hence, the X-ray spectrum. Such a dependence arises due to the interference of one (X-ray) and two-photon (X-ray + IR) excitation channels. The phase of the light influences the dynamics also when the Rabi frequency approaches the vibrational frequency, breaking down the rotating-wave approximation. The probe X-ray spectra are also sensitive to the delay time, the duration, and the shape of the pulses. The evolution of the nuclear wave packets in the dissociative core-excited state affects the dynamics of resonant Auger scattering from fixed-in-space molecules. One of the important dynamical effects is the atomic-like resonance which experiences electronic Doppler shift. We predict that the scattering of the Auger electrons by nearby atoms leads to new Doppler shifted resonances. These extra resonances show sharp maxima in the bond directions, which makes them very promising as probes for local molecular structure using energy and angular resolved electron-ion coincidence techniques. Our theory provides prediction of several new effects, but also results that are in good agreement with the available experimental data.

•Jan 1, 2006•1 citation
Nonlinear effects in pulse propagation through a medium consisting of four-level double-\ensuremathΛ\ensuremath{\Lambda}\ensuremathΛ-type systems are studied theoretically. We apply three continuous-wave driving fields and a pulsed probe field such that they form a closed interaction loop. Due to the closed loop and the finite frequency width of the probe pulses, the multiphoton resonance condition cannot be fulfilled, such that a time-dependent analysis is required. By identifying the different underlying physical processes we determine the parts of the solution relevant to calculate the linear and nonlinear response of the system. We find that the system can exhibit a strong intensity-dependent refractive index with small absorption over a range of several natural linewidths. For a realistic example we include Doppler and pressure broadening and calculate the nonlinear self-phase modulation in a gas cell with sodium vapor and argon buffer gas. We find that a self-phase modulation of \ensuremathπ\ensuremath{\pi}\ensuremathπ is achieved after the propagation of a few centimeters through the medium while the absorption and pulse shape distortion in the corresponding spectral range is small.
The light propagation of a probe field pulse in a four-level double-lambda type system driven by laser fields that form a closed interaction loop is studied. The finite frequency width of the probe pulse requires a time-dependent analysis beyond the multiphoton resonance assumption. We apply a Floquet decomposition to the equations of motion to solve this time-dependent problem and to identify the different scattering processes contributing to the medium response. We find that the response oscillating in phase with the probe field is phase-independent. The phase dependence arises from a scattering of the coupling fields into the probe field mode at a frequency which in general differs from the probe field frequency. In particular for short pulses with a large frequency width, inducing a closed loop interaction contour may lead to a distortion of the pulse shape via this phase-sensitive scattering. Finally, we demonstrate that both the closed loop and the nonclosed loop configuration allow for sub- and superluminal light propagation with small absorption or even gain, where one of the coupling field Rabi frequencies acts as a control parameter that enables one to switch between sub- and superluminal light propagation.
The third-order susceptibility is investigated in a five-level atomic system in which the laser beams couple the ground state to a four-level closed-loop system. It is found that under the condition of the multiphoton resonance, one can enhance the Kerr nonlinearity of such a medium by properly adjusting the amplitudes and phases of the applied fields. In this case, the linear and nonlinear absorption reduce considerably in a region with a positive group velocity. It is demonstrated that the third-order susceptibility is very sensitive to the relative phase of the applied fields. An analytical model is presented to elucidate such phase control of the Kerr nonlinearity. A comparison is also made between the Kerr-nonlinear indices for the five-, four-, and three-level systems. It is realized that the magnitude of the Kerr nonlinearity for the five-level system is larger than that of the three- and four-level counterparts. Finally, it is shown that effect of Doppler broadening can lead to an enhanced Kerr nonlinearity while maintaining linear and nonlinear absorption.
Using semiclassical radiation theory, a formalism similar to that used by Lamb in his Theory of an Optical Maser is developed for studying the amplification of vector traveling waves in a laser-type medium. The effect of the medium on the waves is given in terms of space (or time) dependent field amplitudes and phases and a nonlinear index of refraction. With particular emphasis on typical gaseous media, the effects of Doppler broadening are treated in detail for arbitrary ratios of natural to Doppler linewidths. Polarization and propagation vectors in various directions are considered, and the nonlinear effects are found to make an isotropic medium effectively anisotropic. Lowest order nonlinear effects (due to a polarization cubic in the field amplitudes) are studied extensively, and the frequency dependence of several of these processes is presented in graphical form. In particular, the introduction of fields at new frequencies and polarization effects are considered. The characteristics of these nonlinear processes peculiar to Doppler broadened lines are discussed, and the processes are interpreted in terms of saturation and coherent modulation of the population inversion density. Strong nonlinear effects are considered in a more approximate way and are found to consist of saturation of the various linear and nonlinear processes previously considered. These strong nonlinear effects should occur at low enough intensities to be easily observed in practice on a CW basis. With the present formalism, the analytical results of Gordon, White and Rigden regarding gain saturation in laser amplifiers are obtained, and the extension is made to include frequencies away from line center and the effects of multiple spectral components. Again, the introduction of fields at new frequencies is considered in detail. These results are also discussed in terms of saturation and coherent modulation of the populations and hole burning.
This thesis deals with the study of propagation effects experienced by weak light pulses as they propagate in atomic media driven by strong pulses. We explore both the ultra-short and long pulse regime and investigate the phenomena that arise at these different time scales. In the short pulse regime, a strongly driven two level atomic system presents transient light shifts, and non-adiabatic transitions occur between these adiabatic levels. We have studied a method to probe these light shifts in real time by propagating a weak probe through the medium. The light shifts enrich the spectrum of the probe and the probe gets shaped as a result. In this way a strongly driven two-level system can act as an active pulse shaper, and can introduce oscillations in the temporal profile of an ultra-short pulse at a time scale shorter than the pulse duration. We also show that by driving the system with two time delayed non-resonant strong fields, the non-adiabatic effects can be rendered phase dependent. This gives very sensitive phase control of the excited state population and can be used to formulate new techniques in interferometry. In the long pulse regime we present a new method of slowing light that can be realized in a double two-level system interacting with two orthogonally polarized light pulses that propagate along different axis. Spatio-temporal dependence of the total polarization induces a grating in the ground Zeeman coherence. The stronger of the two fields (the control field) is diffracted from this grating into the direction of the weak probe field compensating for the absorption of this latter field. A transparency window is thus created in the absorption spectrum of the probe leading to the slowing down of light. The transparency window exhibits characteristics similar to the one obtained by EIT (electromagnetic induced transparency) method. However, the important difference between our method and the traditional EIT method, is that ours doesn't rely on realizing dark state in the system. This may open the possibility of slowing down light in more complex atomic media. Moreover, when the linear absorptive response of the medium is cancelled in this manner, the nonlinear response becomes more important. In the situation where fields propagate in the same direction and have same frequency, two regimes have been investigated. For small optical depths, the effective susceptibility behaves as chi_lin exp[2 i phi] (with phi the phase difference between two fields). This renders phase control of the medium response, and the medium can be changed from an absorber to an amplifier, with normal or anomalous dispersion, by adjusting the relative phase phi.  In the regime of large optical thickness, phase saturation takes place and the effective susceptibility turns into chi_lin*, changing an absorber into an amplifier without effecting the dispersive response (chi_lin is linear susceptibility).
Nonlinear effects of sublevel coherence on resonant backward-degenerate four-wave mixing are analyzed in the saturation regime of an inhomogeneously broadened and optically thin gas medium, composed of \ensuremath{\Lambda}-type three-level atoms. No limitations are set to the pump-field intensities, and an analytical approach is presented in the Doppler limit and efficient transverse-optical-pumping regime. It is shown that coherent population trapping due to strong pump-field coupling has a negligible incidence in phase conjugation, while interference of two imbalanced coherent-population-injection channels determines the mixing process. Level-crossing emission resonances are found to exhibit particular line-shape characteristics: (1) an insensitivity to power shifts, (2) strong power-broadening accompanied by incomplete line splitting, or (3) field-induced line-broadening inhibition. The conditions under which these effects should be observable are identified, and their dependence on pump imbalance is remarked.
The present thesis is devoted to theoretical studies of pulse propagation of light through linear and nonlinear media, and of light-induced nuclear dynamics. The first part of the thesis addresses propagation of light pulses in linear periodical media - photonic crystals. The main accent was put on studies of the angular properties of two qualitatively different types of photonic crystals: holographic photonic crystals, and impurity band based photonic crystals. The anisotropy of band structure, group velocity and pulse delay with respect to the light polarization are analyzed. In the second part of the thesis a strict theory of nonlinear propagation of a few strong interacting light beams is presented. The key idea of this approach is a self-consistent solution of the nonlinear wave equation and the density matrix equations of the material. This technique is applied to studies of dynamics of cavityless lasing generated by ultra-fast multi-photon excitation. It is shown that interaction of co- and counter-propagating pulses of amplified spontaneous emission (ASE) affects the dynamics and efficiency of nonlinear conversion. Our dynamical theory allows to explain the asymmetric spectral properties of the forward and backward ASE pulses, which were observed in recent experiment with different dye molecules. It is shown that the ASE spectral profile changes drastically when the pump intensity approaches the threshold level. The effect of the temporal self-pulsation of ASE is studied in detail. The third part of the thesis is devoted to light-induced nuclear dynamics. Time- and frequency-resolved X-ray spectroscopy of molecules driven by strong and coherent infrared (IR) pulses shows that the phase of the IR field strongly influences the trajectory of the nuclear wave packet, and hence, the X-ray spectrum. Such a dependence arises due to the interference of one (X-ray) and two-photon (X-ray + IR) excitation channels. The phase of the light influences the dynamics also when the Rabi frequency approaches the vibrational frequency, breaking down the rotating-wave approximation. The probe X-ray spectra are also sensitive to the delay time, the duration, and the shape of the pulses. The evolution of the nuclear wave packets in the dissociative core-excited state affects the dynamics of resonant Auger scattering from fixed-in-space molecules. One of the important dynamical effects is the atomic-like resonance which experiences electronic Doppler shift. We predict that the scattering of the Auger electrons by nearby atoms leads to new Doppler shifted resonances. These extra resonances show sharp maxima in the bond directions, which makes them very promising as probes for local molecular structure using energy and angular resolved electron-ion coincidence techniques. Our theory provides prediction of several new effects, but also results that are in good agreement with the available experimental data.