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Semiconductor Physics Quantum Electronics & Optoelectronics

Effect of non-linear absorption on characteristics of laser-induced luminescence

Serge E. Zelensky, E-mail: zele@univ.kiev.ua

Published Jun 30, 2008• 0 citations
Publisher

Abstract

This paper deals with the methodology of laser-induced luminescence at high excitation levels.For a case when a photodetector collects integral (over the volume) luminescence power, a method is proposed for processing the experimentally-measured luminescence power and optical transmittance as some functions of the incident laser power.The method is based on the analysis of relative increments of luminescence and transmitted laser power.Considered are two examples of mechanisms of non-linear laserinduced luminescence, namely: saturated molecular luminescence and luminescence excited via two-photon absorption.

DOI
10.15407/spqeo8.02.051

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This paper deals with the methodology of laser-induced luminescence at high excitation levels.For a case when a photodetector collects integral (over the volume) luminescence power, a method is proposed for processing the experimentally-measured luminescence power and optical transmittance as some functions of the incident laser power.The method is based on the analysis of relative increments of luminescence and transmitted laser power.Considered are two examples of mechanisms of non-linear laserinduced luminescence, namely: saturated molecular luminescence and luminescence excited via two-photon absorption.
The main achievements in our research on the physical phenomena of the excited-state nonlinear absorption in a molecular system and its applications in photonic technology are described. In the first part of this paper, some energy-level models and rate-equations are used to explain various mechanisms of the excited-state nonlinear absorption under different conditions, such as reverse saturable absorption caused by the triplet and/or the singlet excited-state absorption; saturable absorption due to the first and/or the second singlet excited-state absorption; and the excited-state nonlinear absorption induced by two-photon absorption. The experimental results for metal-organic and C 60 materials irradiated by ps and ns laser pulses are consistent with the simulated curves of the transmittance versus fluences. In the second part, the applications of excited-state nonlinear absorption in photonic techniques including optical bistability, optical switching, optical limiting, optical modulation, optical logic and optical storage are introduced. The working principles of the photonic devices based on the excited-state nonlinear absorption are presented. The experimental characteristic curves are found in good agreement with the theoretical simulations for these devices.
The time behavior of a two- and a three-level molecular system under narrowband pulsed-laser excitation is discussed, and relations are presented for the temporal variation of the concentrations of the levels involved. It is shown that if saturation is approached, the response time of the molecular system is strictly related to the pumping time, which is given by the reciprocal of the product of the laser spectral density and the Einstein coefficient of stimulated absorption. Typical calculations of the fractional number densities of the levels are presented as a function of the value of the laser spectral density required to achieve saturation for a few typical molecules such as benzophenone, fluorene, and rhodamine 6G.
A new theoretical model describing the emission and absorption dynamics in an ensemble of molecules under intense coherent pulsed pumping is developed on the basis of the concepts of cooperative light-induced luminescence (CLIL). The CLIL development is described within the framework of formalism of the system density matrix in the space of photon wave functions. It is shown that the fast growth of CLIL relates to the development of coherent states of the quantum field in the area of efficient cooperative interactions of molecules (coherence volume). A system of equations for the calculation of CLIL energy, population of excited states, and optical absorption of the system in dependence on the laser pump energy density is solved. The theoretical results obtained are in good agreement with the experimental data.
By applying a sufficiently intense beam of off-resonant light, simultaneously with a conventional excitation source beam, the efficiencies of one- and two-photon absorption processes may be significantly modified. The nonlinear mechanism that is responsible, known as laser modified absorption, is fully described by a quantum electrodynamical analysis. The origin of the process, which involves stimulated forward Rayleigh-scattering of the auxiliary beam, relates to higher order terms which are secured by a time-dependent perturbation treatment. These terms, usually inconsequential when a single beam of light is present, become prominent under the secondary optical stimulus – even with levels of intensity that are moderate by today’s standards. Distinctive kinds of behaviour may be observed for chromophores fixed in a static arrangement, or for solution- or gas-phase molecules whose response is tempered by a rotational average of orientations. In each case the results exhibit an interplay of factors involving the beam polarisations and the molecular electronic response. Special attention is given to interesting metastable states that are symmetry forbidden by one- or two-photon absorption. Such states may be accessible, and thus become populated, on input of the auxiliary beam. For example, in the one-photon absorption case, terms arise that are more usually associated with three-photon processes, corresponding to very different selection rules. Other kinds of metastable state also arise in the two-photon process, and measuring the effect of applying the stimulus beam to absorbances of such character adds a new dimension to the information content of the associated spectroscopy. Finally, based on these novel forms of optical nonlinearity, there may be new possibilities for quantum non-demolition measurements.
Abstract The book so far is almost entirely concerned with linear optical processes, where the response of a material to incident light is described by its linear susceptibility and the rates of optical processes are proportional to the incident intensity. However, examples of nonlinear behaviour occur in the saturation of atomic transitions, discussed in §1.7, and in the power-broadened susceptibility, derived in eqn (2.8.6). Atomic saturation is also an important component in the laser theory of§§t.10 and 7.3. The expressions derived in these examples contain the electromagnetic energy density or photon number in denominators whose expansions include terms proportional to all positive powers of the optical energy. The higherorder, or nonlinear, terms are normally much smaller than the linear term for conventional light sources but their influence is often significant in experiments that use laser sources. The present chapter treats the effects of the nonlinear terms in modifying the properties of incident light beams.