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NASA STI/Recon Technical Report N

Quantum Mechanics Applied to Dye Lasers.

Carol K. Pearce

Published Sep 1, 1981• 0 citations
OpenAlex

Abstract

Abstract : The application of quantum mechanics to dye laser theory is reviewed, based upon recent semiclassical and fully quantum mechanical studies. Both semiclassical and fully quantum mechanical approaches were included. Phenomena investigated in the dye laser medium included spectral hole burning, propagation of light pulses, and light absorption and emission. Some studies realistically included consideration of the triplet state. Mixtures of lasing dyes, or of lasing and saturable absorber dyes, were not treated, nor were vapor dye lasers. Theoretical limitations that might be inherent in dye lasers, such as gain and power output, are other important areas that deserve examination in future studies. (Author)

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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Oct 20, 2008•0 citations
Abstract : The application of quantum mechanics to dye laser theory is reviewed, based upon recent semiclassical and fully quantum mechanical studies. Both semiclassical and fully quantum mechanical approaches were included. Phenomena investigated in the dye laser medium included spectral hole burning, propagation of light pulses, and light absorption and emission. Some studies realistically included consideration of the triplet state. Mixtures of lasing dyes, or of lasing and saturable absorber dyes, were not treated, nor were vapor dye lasers. Theoretical limitations that might be inherent in dye lasers, such as gain and power output, are other important areas that deserve examination in future studies. (Author)
We have developed a self-consistent description, based on the semiclassical radiation theory of the propagation of a light pulse in a dye medium. The multilevel nature of the energy bands of a dye molecule and the solvent cage effect in a solution are taken into account. In the case of light pulses whose duration is much shorter than the solvent-solute relaxation time but much longer than the time of atomic phase memory, the latter being of the order of ${10}^{\ensuremath{-}12}$ sec for dyes, we solve the coupled system of equations for the field and the medium by the perturbation procedure. The hole-burning effect is incorporated into the solution in a natural manner. This is especially clear in the direct transition approximation where all the intermediate transitions are neglected. A recent idea of pulse superposition, consisting in storing the energy of a pulse in the form of population inversion followed by stimulated emission triggered by another pulse, is further discussed. Contrary to the orginal model developed by one of us (S.L.C.), we show that no cw pumping is required. The feasibility of the pulse superposition is supported by some experimental results obtained by sending a train of 10-psec pulses through a glycerine solution of oxazine 1 perchlorate.
We develop a fully quantum-mechanical theory for the organic-dye-solution laser, obtain density-matrix equations of motion for the single-mode radiation-density operator and the matter-density operator, and solve and investigate the steady-state case. We generalize the usual Born-Markoff approximation master equation for two matter states to include four matter states, each one of which interacts with the laser radiation field. This allows us to treat exactly the organic-dye molecular triplet-state levels which participate in the laser operation in an essential way. For experimentally realizable conditions the steady-state solution contains features which are qualitatively different from nondye lasers. These effects are directly attributable to intensity-dependent triplet-state radiation absorption losses. At threshold the diagonal matrix elements of the radiation photon distribution (Rn{R}_{n}Rn​) can be a decreasing function of the photon number nnn with an inflection point rather than the usual truncated Gaussian. This necessitates redefinition of threshold. For pumping just above threshold there may be both a maximum and a minimum in Rn{R}_{n}Rn​ rather than just a maximum as in usual laser theories. We also specify the effect of triplets on the narrowing of Rn{R}_{n}Rn​ for pumping above threshold and the subsequent widening of Rn{R}_{n}Rn​ for pumping well above threshold. Many of our results require photon-counting experiments for verification. Also, our equations are easily reducible to a semiclassical theory, where our treatment of the triplets variables is an improvement over the usual rate equations.
This paper reviews the basic theory of the mechanical action of light in resonant interaction with atoms. At present the main application is laser cooling, but the approach is applicable to a broader range of phenomena. It is based on an adiabatic elimination philosophy, which turns out to give the lowest-order quantum corrections to the behavior found when the photon momentum goes to zero. Hence it is called a semiclassical theory. In this manner a subjective but consistent approach can be presented; other treatments are incorporated or mentioned at the appropriate places. Both the classical and the quantum-mechanical approach are discussed. Those readers who wish to obtain only a heuristic overview of the phenomena can concentrate on Sec. III, which treats both the photon momentum effects and their connection with photon counting statistics. The detailed theoretical treatment utilizes Wigner functions and Fokker-Planck techniques. The ensuing theory is applied both to the cooling of free particles and trapped ones. The paper ends with an extensive bibliography, where the author lists most papers of interest for research into the mechanical manifestations of light. For completeness, many papers are included that are not explicitly mentioned in the text.
This dissertation presents experimental and theoretical studies of transient degenerate four wave mixing (DFWM) in organic dyes. Chapter 1 is an introduction to DFWM. Chapter 2 describes DFWM experiments that were performed in the gain medium of a dye laser. Chapter 3 presents the theory of DFWM of short pulses in three level saturable media. Chapter 4 presents DFWM experiments of femtosecond pulses in the saturable absorber of a passively modelocked ring dye laser. Chapter 5 presents the theory of DFWM of ultrashort pulses in resonant media.
This work explores the feasibility of inducing lasing action in a single dye molecule using an optical microcavity. A single-molecule light source is proposed, in which a microcavity-coupled dye molecule is pumped by multiple energy donors via an intermolecular resonance energy transfer mechanism. A quantitative model based on realistic parameters for microcavities and for organic dyes shows that stimulated emission may become dominant over spontaneous fluorescence under optimal yet technically reachable conditions, suggesting the likelihood of achieving a single-molecule lasing photon source with the proposed device. Lasing of a single dye molecule generates signals much brighter than spontaneous fluorescence, and may find applications in a wide range of fields from physics and chemistry to biology.
Motivated by the recent progresses in one-atom laser and single-molecule manipulation, this work presents the model and simulations of a single dye molecule laser device, which consists of a single dye molecule as an acceptor in a microcavity pumped by multiple donors via the intermolecular resonance energy transfer mechanism. The photon intensity is calculated at the emission peaks of donor and acceptor dyes for different pump rates and donor numbers. Finally, it is demonstrated that stimulated emission gains a distinct advantage over spontaneous emission under appropriate conditions. This work would have many important applications in a wide range of fields from physics and chemistry to nanotechnology in future.