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Final Report

Intense Pulse Phenomena.

Joseph H. Eberly

Published May 1, 1976• 0 citations
OpenAlex

Abstract

Theoretical and experimental studies were undertaken to better understand aspects of the interaction of intense light pulses with atomic and molecular matter. These studies fell into three categories: Theories of the light-matter interaction, Experimental studies in large organic molecules and Studies of realistic model systems of light emitters.

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Nonlinear optical pulse propagation in molecular media

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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.

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Reports on Subfields of Physics: Atomic, Molecular and Optical Physics

Bruce M. Schechter

Atomic, molecular and optical physics encompasses a broad range of theoretical and experimental research on matter at the atomic and molecular level and on light. In the United States it is pursued by over 300 small groups in university, national and industrial laboratories. Advances in this branch of physics not only add to our understanding of the basic laws of physics but lead to new instruments and techniques vital to other areas of science, to industry and to national programs. In their report the Panel on Atomic, Molecular and Optical physics has proposed a program of research initiatives intended to support scientific innovation and to provide an environment for rapid scientific advance. But the panel is quick to point out that in attempting to predict the most promising avenues for scientific advancement one is likely to miss whole new boulevards. The panel admits that had it met ten years ago it would have failed to mention or would have seriously underestimated many important developments: laser cooling of atoms and ions, low-energy highly charged ions, transient molecular states, Rydberg atoms, molecular clusters, four-wave mixing, phase conjugation, ultrasensitive detection. “Nevertheless,” writes the panel, “we believe that the program of research initiatives represents a realistic basis for scientific advance in the near future.” The research initiatives include:

Physics Today•Apr 1, 1986•2 citations
Theoretical and experimental studies were undertaken to better understand aspects of the interaction of intense light pulses with atomic and molecular matter. These studies fell into three categories: Theories of the light-matter interaction, Experimental studies in large organic molecules and Studies of realistic model systems of light emitters.
Intense light-matter interaction largely relies on the use of high-power light sources, creating fields comparable to, or even stronger than, the field keeping the electrons bound in atoms. Under such conditions, the interaction induces highly nonlinear processes such as high harmonic generation, in which the low-frequency photons of a driving laser field are upconverted into higher-frequency photons. These processes have enabled numerous groundbreaking advances in atomic, molecular, and optical physics, and they form the foundation of attosecond science. Until recently, however, such processes were typically described using semi-classical approximations, since the quantum properties of the light field were not required to explain the observables. This has changed in the recent past. Ongoing theoretical and experimental advances show that fully quantized descriptions of intense light-matter interactions, which explicitly incorporate the quantum nature of the light field, open new avenues for both fundamental research and technological applications at the fully quantized level. These advances emerge from the convergence of quantum optics with strong-field physics and ultrafast science. Together, they have given rise to the field of quantum optics and quantum electrodynamics of strong-field processes.
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.
Understanding collisions between ultracold molecules is crucial for making stable molecular quantum gases and harnessing their rich internal degrees of freedom for quantum engineering. Transient complexes can strongly influence collisional physics, but in the ultracold regime, key aspects of their behavior have remained unknown. To explain experimentally observed loss of ground-state molecules from optical dipole traps, it was recently proposed that molecular complexes can be lost due to photoexcitation. By trapping molecules in a repulsive box potential using laser light near a narrow molecular transition, we are able to test this hypothesis with light intensities three orders of magnitude lower than what is typical in red-detuned dipole traps. This allows us to investigate light-induced collisional loss in a gas of nonreactive fermionic 23Na40K^{23}\mathrm{Na}^{40}\mathrm{K}23Na40K molecules. Even for the lowest intensities available in our experiment, our results are consistent with universal loss, meaning unit loss probability inside the short-range interaction potential. Our findings disagree by at least two orders of magnitude with latest theoretical predictions, showing that crucial aspects of molecular collisions are not yet understood and provide a benchmark for the development of new theories.
Atomic, molecular and optical physics encompasses a broad range of theoretical and experimental research on matter at the atomic and molecular level and on light. In the United States it is pursued by over 300 small groups in university, national and industrial laboratories. Advances in this branch of physics not only add to our understanding of the basic laws of physics but lead to new instruments and techniques vital to other areas of science, to industry and to national programs. In their report the Panel on Atomic, Molecular and Optical physics has proposed a program of research initiatives intended to support scientific innovation and to provide an environment for rapid scientific advance. But the panel is quick to point out that in attempting to predict the most promising avenues for scientific advancement one is likely to miss whole new boulevards. The panel admits that had it met ten years ago it would have failed to mention or would have seriously underestimated many important developments: laser cooling of atoms and ions, low-energy highly charged ions, transient molecular states, Rydberg atoms, molecular clusters, four-wave mixing, phase conjugation, ultrasensitive detection. “Nevertheless,” writes the panel, “we believe that the program of research initiatives represents a realistic basis for scientific advance in the near future.” The research initiatives include: