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Physics of the Solid State

Problems in searching for new solid-state UV-and VUV-active media: The role of photodynamic processes

Vadim Vladimirovich Semashko

Published Aug 1, 2005• 24 citations
Publisher

Abstract

The impact of photodynamic processes induced by pump radiation in crystals doped with rare-earth (RE) ions on the possibility of generating stimulated radiation in the UV and VUV spectral ranges is analyzed. It is shown that, in addition to objective factors, one of the main causes preventing the lasing effect from being obtained using the interconfigurational 4ƒ n−15d-4ƒ n transitions of RE ions is insufficient consideration of the photodynamic processes involved in experiments. It is proposed to correct laser test techniques and “pumpprobe” experiments aimed at investigating active media appropriate for lasing in the UV and VUV ranges. Extended criteria oriented to search for new solid-state UV and VUV active media are formulated.

DOI
10.1134/1.2014502

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The impact of photodynamic processes induced by pump radiation in crystals doped with rare-earth (RE) ions on the possibility of generating stimulated radiation in the UV and VUV spectral ranges is analyzed. It is shown that, in addition to objective factors, one of the main causes preventing the lasing effect from being obtained using the interconfigurational 4ƒ n−15d-4ƒ n transitions of RE ions is insufficient consideration of the photodynamic processes involved in experiments. It is proposed to correct laser test techniques and “pumpprobe” experiments aimed at investigating active media appropriate for lasing in the UV and VUV ranges. Extended criteria oriented to search for new solid-state UV and VUV active media are formulated.
A method of suppression of losses due to excited-state absorption (ESA) in laser crystals is proposed, based on the well-known phenomenon of electromagnetically induced transparency. Typical situations in which ESA prevents lasing are considered. Theoretical analysis shows that by using an additional driving laser field one can inhibit ESA and make lasing possible. On the basis of available spectroscopic information estimates for rare-earth-ion-doped laser materials are presented. They show the feasibility of obtaining optical gain at parity-allowed $4{f}^{n}\ensuremath{\leftrightarrow}4{f}^{n\ensuremath{-}1}5d$ transitions of rare-earth ions in the ultraviolet spectral region after suppression of ESA at an emission wavelength into the conduction band of a host material.
Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,
Summary form only given: Amplification in rare-earth doped solid state planar optical structures has attracted a lot of interest in recent years due to the fact that the rare earth ions show sharp absorption and emission bands and relatively long luminescence lifetimes. In particular the erbium (Er) ion is very attractive because of its intra 4f-transition from the first excited state to the ground state around 1.53 mum (4I13/2-4I15/2). The main problem of the erbium doped waveguide amplifiers (EDWAs) is that high values of the Er3+concentration are required to reach high gain figures in a compact length, but in this way the concentration quenching effects become very considerable and detrimental to the optical gain, since they reduce the population in the first excited state. A good solution to overcome this dramatic drawback is to consider erbium doped photonic crystal amplifier (EDPCA). In fact the small group velocity of electromagnetic eigenmodes brings about the enhancement of stimulated emission if the photonic crystals are doped by active media as the rare earth ions E3+r or Yt3+. This phenomenon originates from the long interaction time between radiation field and the matter caused by the small group velocity near the edge of the photonic band gap. The efficient confinement of light is achievable not only by tuning the input signal at the band edge of the gap of the photonic crystal but it is also obtainable by introducing local defects inside photonic crystals. The density of electromagnetic states inside a cavity is significantly modified and the spontaneous emission of atoms in a cavity can be either enhanced or inhibited. Erbium doped silica-titania one-dimensional photonic crystal microcavities have been analyzed by solving the erbium rate equations and the Maxwell equations by means of an auxiliary differential equation finite difference time domain technique. Since the performance of optical amplifiers depends on the populations of the energy levels participating in radiative transitions, determined principally by the distribution and concentration of the rare-earth ions and by the pumping conditions, the relations between these parameters and the transmittance of the EDPCMA have been studied
The recent achievements devoted to cooling of solids with a laser are presented in this paper. We discuss the latest results of traditional laser cooling of solids based on rare earth ions and new techniques based on colloidal lead-salt quantum dots doped in a glass host, laser cooling in Tm3+-doped oxy-fluoride glass ceramic. Relatively short (microsecond) lifetime of the excited level of the PbSe QDs compared to the millisecond lifetime of the excited level of RE ions allows an acceleration of the cooling process and provides an opportunity to use new materials with higher phonon energy as hosts, which are normally considered unsuitable for cooling with RE ions. Another new approach to the laser cooling problem based on super-radiance has been considered in this paper. The advantages of optical refrigeration with rare earth doped semiconductors, in which not only optically active electrons of the 4f shell but the valence and conduction bands of the host material are involved in cooling cycle is discussed. It is shown that involving the valence and conduction bands of the host in the cooling cycle allows the pump wavelength to be shorter than mean fluorescence wavelength. Raman laser cooling of solids as well as observation of spontaneous Brillouin cooling have been presented.
New ways are proposed of increasing broadband-lamp pumping effectiveness of laser crystals with trivalent lanthanides. The method is based on the broadening of lasing-ion absorption spectrum by the remove (excitation) of their considerable part from the ground state into one (some) of the upper states with the help of additional resonant bleaching laser add-pumping Advantages of the new pumping schemes are illustrated by the results, obtained during quantitative analysis of the necessary conditions of stimulated-emission excitation for four laser crystals (LaF3, LiYF4, BaY2F8, and YA103) with Pr3+ ions, which can lase at 3Po → 3F4,3,2, 3H6,5 channels at 300 K with lamp pumping. The method proposed is also suitable for laser effectiveness increase in crystals with other lanthanides activators.