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The Journal of Chemical Physics

Coherent propagation of intense ultrashort laser pulses in a molecular multilevel medium

Szczepan Chelkowski, André D. Bandrauk

Published Sep 15, 1988• 30 citations
Publisher

Abstract

The Maxwell–Schrödinger equations describing the ultrashort laser pulse propagation in multilevel molecular media are shown to be analytically solvable and to reduce to nonlinear multisine-Gordon equations for certain models of the field–molecule system. Special cases of level schemes are shown to lead to soliton propagation. A numerical study is presented in order to examine the effect of nonresonant (virtual) transitions on pulse propagation and amplification in a three-level molecular system as a function of intensity and detuning.

DOI
10.1063/1.454882

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The Maxwell–Schrödinger equations describing the ultrashort laser pulse propagation in multilevel molecular media are shown to be analytically solvable and to reduce to nonlinear multisine-Gordon equations for certain models of the field–molecule system. Special cases of level schemes are shown to lead to soliton propagation. A numerical study is presented in order to examine the effect of nonresonant (virtual) transitions on pulse propagation and amplification in a three-level molecular system as a function of intensity and detuning.
We model the response of a molecular medium to an intense pulse of light. We begin by reducing the Maxwell-Bloch equations for a multilevel molecular model system to a set of simplified propagation equations. We thereby obtain expressions for the frequency, temperature, and field intensity dependence of the ground and excited electronic state absorption cross sections, and the emission cross section, as well as the temperature dependence of the decay rate of the excited state. The phenomena of saturation, excited-state absorption, optically induced dichroism and birefringence, vibronic energy transfer, induced molecular alignment, decay of the matter-field interaction energy, and rotational diffusion are considered within the general formalism for describing the propagation of an intense pulse of light in the molecular medium. We find that the cross section for absorption (emission) of a photon is not identical to the cross section for molecular excitation (deexcitation) via the matter-field interaction. This is explained in terms of an energy balance between the matter, radiation, the matter-radiation interaction, and the bath responsible for the broadening of the molecular transitions. The inequality of these cross sections determines whether the system supplies or draws energy from the thermal bath. The rise in the vibrational temperature of molecules subjected to an intense short pulse is shown to significantly affect propagation of the pulse. The alignment of the molecular system resulting from saturation of the ground-state transition by a polarized laser pulse and the effects of the orientational dependence of the matter-field interaction including effects of rotational diffusion are determined. As an example of the formalism we consider pulse propagation in a Rhodamine 6G solution. We fit the parameters of the model to determine the frequency dependence of the ground- and excited-state absorption cross sections and the emission cross section and compare with experimentally determined cross sections. We describe the propagation of a pulse whose temporal width is comparable to the rotational diffusion time of the molecules in the dye solution and calculate polarization pulse probe signals.
Propagation and amplification of an ultrashort laser pulse in a two-level medium is numerically investigated with the use of the finite-difference time-domain (FDTD) procedure simultaneously solving Maxwell and Schrodinger equations with no assumptions characteristic of slowly varying envelope approximation. Comparison of the results of FDTD numerical simulations with the predictions of the pulse area theorem has demonstrated that the developed numerical procedure provides an adequate description of pulse evolution in a two-level medium. Amplification of ultrashort light pulses in a two-level medium is analyzed. Two methods of improving the gain of ultrashort pulses in a two-level medium by modulating the spatial distribution of dipole moments of resonant transitions and using initially chirped frequency-detuned pulses are explored.
We consider the propagation of ultrashort optical solitons in media described by a general Hamiltonian of multilevel atoms. Assuming that all transition frequencies of the medium are well below the typical wave frequency, i.e., only the contribution of infrared transitions is taken into account, we use a short-wave approximation and a rigorous application of the reductive perturbation formalism to derive a cumbersome coupled system of nonlinear partial differential equations describing ultrashort soliton evolution in such systems. The rather complicated set of coupled equations can be simplified to a generic double-sine-Gordon equation for a special case of identical three-level atoms, whereas for a special case of identical four-level atoms the system of coupled equations can be reduced to a generalized double-sine-Gordon equation. Numerical simulations showing the formation of robust breather-type solutions of both the standard double-sine-Gordon and of the generalized double-sine-Gordon equations from sinusoidal inputs with Gaussian envelopes are also presented.
We theoretically analyze linear and nonlinear coherent propagation of linearly polarized, plane-wave, resonant single-cycle terahertz pulses through spatially extended rigid-rotor molecular media. Our model incorporates mixed state medium preparation, nonperturbative nonlinearities, saturation, coherence, memory effects, and propagation, but ignores the effects of damping. Explicit solutions are reported in the linear propagation regime. These solutions are the multilevel superposition of linear, single-cycle $0\ensuremath{\pi}$ pulses, and appear as temporal beats in the time domain. For media initially in thermal equilibrium, the pulse and molecular beats are dispersive and broaden temporally with increased propagation distance. In the simplified limit of equal rotational line strength (an idealized situation), the emitted impulses are exact temporal copies of the input pulse. An efficient, scalable computational method for solving the reduced multilevel Maxwell-Bloch equations for molecular media is reported. This method is based on a standard differential method for the propagation equation together with an operator splitting method for the Bloch equations. It invokes neither the slowly varying envelope (SVEA) or rotating wave approximations (RWA), and incorporates a large number of possible energy eigenstates (we solve for 7744 levels). Case studies of nonlinear single-cycle pulse propagation are then provided by means of computer solutions. In the nonlinear regime, we observe strong molecular orientations and suppression of the pulse and orientational revivals predicted by linear theory. For sufficiently strong pulses, coherent bleaching effects lead to increased transmission of the driving pulse, which also bears signs of self-modulation and carrier-shock formation.
Coherent amplification of short-pulse XeCl lasers is studied theoretically by using multilevel Maxwell–Bloch equations in which the vibrational–rotational structures of a XeCl gain spectrum are included. The model used considers 100 transitions each in the P and R branches for six different vibrational transitions of XeCl(B, υ = 0) → XeCl(X, υ′ = 0–5). Coherence components between sublevels in the B and X states are also properly calculated. The model can successfully predict coherent effects such as a quantum beat caused by the spectrum overlap of the several vibrational–rotational transitions involved in a short-pulse laser spectrum. During amplification, laser pulses experience some nonlinear effects caused by the complex gain spectrum structure and by the coherent interactions; thus a considerable change in the laser pulse shape and a substantial reduction in the duration of the amplified laser pulse are predicted. The Frantz–Nodvik equation in the rate-equation limit and even single-level Maxwell–Bloch equations are not applicable for short-pulse propagation analyses in inhomogeneously broadened gain media.