This article discusses various aspects of coherent control of the medium using a preparatory laser radiation that provides favorable conditions for the propagation of useful radiation. We discussed the possibility of decrease molecular scattering full section in channels of propagation of laser signals, formation of clarified channel in the inhomogeneous medium of propagation and we analyze the molecular dissociation resulting from an increase in rotational energy induced by two successive laser pulses with orthogonal polarizations. Based on the results of calculations, a constant dipole moment of the molecule is shown to play an insignificant role in its orientation in a laser field.
This article discusses various aspects of coherent control of the medium using a preparatory laser radiation that provides favorable conditions for the propagation of useful radiation. We discussed the possibility of decrease molecular scattering full section in channels of propagation of laser signals, formation of clarified channel in the inhomogeneous medium of propagation and we analyze the molecular dissociation resulting from an increase in rotational energy induced by two successive laser pulses with orthogonal polarizations. Based on the results of calculations, a constant dipole moment of the molecule is shown to play an insignificant role in its orientation in a laser field.
We consider deflection of polarizable molecules by inhomogeneous optical fields and analyze the role of molecular orientation and rotation in the scattering process. It is shown that molecular rotation induces spectacular rainbowlike features in the distribution of the scattering angle. Moreover, by preshaping molecular angular distribution with the help of short and strong femtosecond laser pulses, one may efficiently control the scattering process, manipulate the average deflection angle and its distribution, and reduce substantially the angular dispersion of the deflected molecules. We study the problem both classically and quantum mechanically and arrive at the same conclusions in both treatments. The effects of strong deflecting field on the scattering of rotating molecules are considered by the means of the adiabatic invariants formalism. The suggested control scheme opens new ways for many applications involving molecular focusing, guiding, and trapping by optical and static fields.
Coherent, optically dressed media composed of two-level molecular systems without inversion symmetry are considered as all-optically tunable sources of coherent radiation in the microwave domain. A theoretical model and a numerical toolbox are developed to confirm the main finding: the generation of low-frequency radiation, and the buildup and propagation dynamics of such low-frequency signals in a medium of polar molecules in a gas phase. The physical mechanism of the signal generation relies on the permanent dipole moment characterizing systems without inversion symmetry. The molecules are polarized with a DC electric field yielding a permanent electric dipole moment in the laboratory frame; the direction and magnitude of the moment depend on the molecular state. As the system is resonantly driven, the dipole moment oscillates at the Rabi frequency and, hence, generates microwave radiation. We demonstrate the tuning capability of the output signal frequency with the drive amplitude and detuning. We find that even though decoherence mechanisms such as spontaneous emission may damp the output field, a scenario based on pulsed illumination yields a coherent, pulsed output of tunable temporal width. Finally, we discuss experimental scenarios exploiting rotational levels of gaseous ensembles of heteronuclear diatomic molecules.
Various characteristics of molecules have been clarified by spectroscopic methods in which the interactions of molecules with the radiation field were investigated. A stationary response of a molecule excited by a radiation field appears as a spectral line. Information on molecules may be obtained from position (resonance frequency), intensity, and shape and width of the spectral line. So far the interaction of molecules with the radiation field has been studied primarily in a “frequency domain.” Although molecular spectroscopy is one of the research fields in modern science which has the longest history, a variety of important aspects have been demonstrated very recently in this field as radiation sources have been improved. When the radiation field is “weak,” the photon nature of the radiation field is dominant in the interaction with a molecule, such as in the cases of emission, absorption, and scattering of photons. When the radiation field is “strong,” in the sense that many photons exist in a proper mode of the radiation field, the wave nature of the field plays an important role in the interaction. In this case the radiation may be described in the form of the classical field, say, a sinusoidal function of the time and spatial coordinates, coherently interacting with the molecule, which is described quantum mechanically. Here nonlinear properties would appear in the interactions: saturation in absorption, induced scattering, multiphoton processes, coherent transients, etc.
The interaction of intense laser fields with matter is accompanied by a multitude of phenomena, ranging from the generation of coherent radiation across various spectral ranges (from terahertz to soft X-rays) to the creation of beams of accelerated charged particles and micromodification of the volume and surface of various samples.To describe this diversity of phenomena, several theoretical approaches have been developed to date.These approaches utilize different approximations to address this complex nonlinear problem, allowing for the explanation of specific aspects of such interactions.The developed theoretical frameworks consider the interaction at both microscopic and macroscopic levels; at the microscopic level, they investigate the characteristics of single atoms interacting with laser fields, while at the macroscopic level, they analyze nonlinear susceptibilities that describe the nonlinear polarization of the medium during the propagation of laser radiation through it.This work presents an overview of methods describing some of the most commonly employed theoretical approaches to model the response of a medium at a microscopic (quantum-mechanical) level, as well as various methods for controlling the properties of generated coherent radiation.A model for the gas medium is described that accounts for both the response characteristics of individual atoms and allows for consideration of phase and quasiphase matching effects during radiation generation.The influence of medium parameters on the efficiency of generation and polarization properties of generated radiation is analyzed under both phase and quasi-phase matching conditions.A detailed description of an analytical method for calculating the nonlinear susceptibility of a gas medium is provided.The obtained values of nonlinear susceptibility for arbitrary orders may be useful in numerical calculations concerning the propagation of laser radiation in matter.Various channels for radiation generation are analyzed as parameters of the laser field are varied.
We consider deflection of polarizable molecules by inhomogeneous optical fields, and analyze the role of molecular orientation and rotation in the scattering process. We show that by preshaping molecular angular distribution with the help of short and strong femtosecond laser pulses, one may efficiently control the scattering process, manipulate the average deflection angle and its distribution, and reduce substantially the angular dispersion of the deflected molecules. This opens new ways for many applications involving molecular focusing, guiding, and trapping by optical and static fields.
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.