Файл: Antsiferov V.V., Smirnov G.I. Physics of solid-state lasers (ISBN 1898326177) (CISP, 2005)(179s).pdf

Physics of Solid-State Lasers

5.2 INCREASING THE CONCENTRATION OF IMPURITY ACTIVE IONS

The concentration of active ions in the majority of solid-state media does not exceed 3 × 10 20 cm–3. An increase of the concentration of the impurity ions leads to both widening of the absorption bands and increase of the intensity, and also to the concentration quenching of luminescence for the majority of active media.

However, in trivalent Er ions in an yttrium–erbium crystal of the aluminium garnet the concentration decay of luminescence at the

4I11/12→ 4I12/2 transition is not present up to the Er ion concentration of 4 ×10 21 cm–3 and the efficiency of lasing rapidly increases [18].

The effect of concentration decay of luminescence is quite strong in Nd3+ ions as a result of the multipole-resonance interaction of absorption

(4I9/12→ 4I13/2, 4I15/2) and emission (4F3/2→ 4I15/2, 4I13/2) transitions of the adjacent ions. This results in a large decrease of the lifetime of

the upper working level 4F3/2 (Fig. 5.1).

The harmful effect of concentration decay of luminescence is prevented as a result of detuning these transitions by displacing the energy levels and by a corresponding relative shift of the frequency of the transitions, or as a result of increasing the width of the transitions by selecting the chemical composition of the active medium. The probability of the multipole-resonance interaction, which in dipole–dipole interaction changes as 1/r6, rapidly decreases when increasing the distance r > 0.45 nm between the interacting ions. When this condition is fulfilled, the interaction between the Nd ions, situated in the sites of the crystal

Fig. 5.1 Dependence of the lifetime τ (ms) of the upper working level 4F3/2 of Nd3+ on the concentration n (%) in different active media: 1) Nd:KGW, 2) Nd:YAG; 3) Nd:CNPhS (KNFS), 4) Nd:BLN, 5) Nd:LNA.

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lattice, is greatly weakened, irrespective of the high resonance of the electronic transitions.

The concentration of the active Nd ions of up to 4 × 10 21 cm–3 without any significant luminescence decay was obtained in neodymium pentaphosphates NdP5O14 [19] and neodymium tetraphosphates LiNdP4O12 [20]. However, these media are highly unstable and dissociate during heating. In addition, it is quite difficult to grow large single crystals. Therefore, these media are used mainly for the development of minilasers.

In Ref. 21 the authors reported lasing on Li–Nd–La phosphate glass (KNFS) with the Nd ion concentration of 3 × 10 21 cm–3, without any significant luminescence decay. KNFS glass is characterised by a small width of the lasing line, a lower threshold and higher lasing efficiency than silicate and phosphate glass. However, the KNFS glasses are not used widely because of the low heat conductivity coefficient, hardness and high hygroscopicity.

The crystals of potassium–gadolinium tungstate (KGd(WO4)2, KGW) with the Nd ion concentration more than 5 × 10 20 cm–3 are also characterised by a low concentration luminescence decay and higher lasing efficiency [22]. The efficiency factor of the Nd:KGW laser in the free lasing regime is twice as high and the energy of the giant pulse is four times higher in comparison with the Nd:YAG laser.

The high concentration of active ions can be obtained using disordered crystals in the form of mixed compounds (solid solutions) [23]. In these crystals, the active ions are situated in different positions differing in the force and symmetry of the crystal field. These structural variants of the crystal field are of statistical nature and result in detuning of the resonance between the ions situated in different positions. Consequently, the resonance bond between the adjacent activator ions weakens. These crystals have wide and non-uniform luminescence bands which change slowly with temperature. The absorption bands in these crystals are also wider and more intensive, and concentration luminescence decay is less marked. Consequently, the efficiency of application of the radiation of pumping lamps increases several times and the lasers with these matrices have a lower threshold and higher efficiency than the lasers on simple crystals.

5.3 SENSITISING OF LASER SOLID-STATE MEDIA

Lasing efficiency can be increased by developing matrices with double or even triple activation. Consequently, the functions of absorption of pumping energy by a certain type of activator and the emission functions by another type are separated. This method is referred to as sensitising. A sensitizer should efficiently absorb the pumping energy and also transfer efficiently excitation to the lasing activator. This

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condition is satisfied by fulfilling a large number of requirements [24] on the sensitizer: efficient widening of the excitation spectrum of the active medium; the presence of the metastable level above the upper working level of the activator; absence of other levels capable of trapping the excitation of the activator; the absence of the main or induced absorption on the lasing wavelength. Since it is difficult to satisfy all the requirements simultaneously, only a limited number of the effective sensitising active media have been produced so far.

The most efficient co-activator in crystals and glasses with trivalent rare-earth elements is the ion of trivalent chromium. The chromium ions Cr3+ prefer (because of special features of electron configuration) to occupy sites in the crystals with the octahedral co-ordination sphere.

The chromium ions have wide high-intensity absorption bands overlapping almost the entire visible spectral range. Gently absorbing pumping radiation, the ions of trivalent chromium transfer the excitation by the multipoleresonance mechanism to the upper working level of the activator. In addition, the energy of some levels of the chromium ions depends strongly on the force of the crystal field Dq [25] (Fig. 5.2). The main role in the process of exchange by interaction is played by the energy gap ∆ E between the levels 2E and 4T2 of the chromium ions [26].

With increasing force of the crystal field the energy gap between the levels 2E and 4T2 increases. The force of the crystal field in the ruby crystal (Cr3+:Al2O3) is such that the size of the energy gap is

∆ E = 2300 cm–1, in yttrium–aluminium garnet (Y3Al5O12) it is 1300 cm–1, consequently, the excitation relaxes from the long-life level

2E to the ground level 4A2, bypassing level 4T2. The energy gap in the GSGG crystals ∆ E is only 80 cm–1 [18] (Fig. 5.3).

At room temperature, the electrons with the energy of thermal excitation are transferred from the metastable level 2E to the short-life level

Fig. 5.2 Dependence of the energy E × 10 3 (cm–1) of several levels of Cr3+ ions on the strength of the crystal field Dq × 10 3 (cm–1).

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Fig. 5.3 Values of the energy ∆ E × 10 3 (cm–1) between the levels 2E and 4T2 of Cr3+ ions on the strength of the crystal field Dq × 10 3 (cm–1)for different crystal with Cr3+ ions: 1) GSGG, 2) GGG, 3) YGG, 4) YAG, 5) YSGG, 6) emerald, 7) aleksandrite.

4T2 which relaxes through the 4T2→ 4A2 strong transition in the form of a wide spectral luminescence band. This transition reaches resonance with absorption transitions of the ions of neodymium, erbium and ytterbium, and some other ions. If the chromium concentration and the concentration of the activator ions are correctly selected, the quantum yield of transfer is close to unity.

The transfer of excitation energy from Cr3+ to Nd3+ ions does not take place from the metastable state 2E but from the 4T2 state. The low value of the energy gap between them results in the rapid population of the 4T2 level. The spectrum of the wide-band luminescence from this level is efficiently overlapped by the spectrum of absorption of the Nd ions. This results in a high rate of emissionless transport of energy. Fast transfer of excitation energy from Cr3+ to Nd3+ ions (in comparison with the rate of deactivation of the upper working level 4T2 of the Nd ions) is possible on the condition when ∆ E < kT.

The crystal of yttrium–scandium–gallium garnet, activated with the Cr and Nd ions (Nd:Cr:YSGG) resulted in the efficiency of laser lasing of 7.8%, and in the Nd:Cr:GSGG laser the efficiency in the same conditions was 7.1% [26].

5.4 CROSS RELAXATION AND STEPPED SYSTEMS OF PUMPING LASER TRANSITIONS

An important role in threeand four-level lasing systems is played by emissionless transitions resulting in the conversion of energy to the upper working level and the scattering of the lower working level (in the four-level system). The same transitions represent the basis of heat generation and determine the efficiency of the medium. Heat generation produces a number of physical factors complicating lasing

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[24]. This is especially important in the case of infra-red lasers with the lasing wavelength greater than or close to 2 µm in which the mean pumping quantum is 5–10 times higher than the lasing quantum. The development of excitation systems, increasing lasing efficiency as a result of decreasing heat generation in wide-band pumping, is one of the significant achievements of the physics of solid-state lasers [28].

The application of cascade excitation of laser transition between a pair of excited levels may result in the inversion of the populations on the underlying levels. Intermediate laser heating in the presence of the laser cascade to three, four or more steps improves the efficiency of operation of the previous lasing channel, lowering it to the lower working level.

Multistep emission extraction of energy, supplied to the medium, and the resultant suppression of emissionless relaxation of the levels of the laser cascade result in a large decrease of the extent of heat generation in the medium and increases total lasing efficiency. In addition, the systems make it possible to widen the range of lasing wavelength [29].

A large number of variants of the cascade systems with the application of fluorideand oxygen-containing crystals, activated with rare-earth ions, have already been developed. The spectral range of lasing has been extended to 5.15 µm. Lasing on the ions of praseodymium, neodymium, holmium, erbium and thullium has been achieved [30,31].

There is another physical process capable of competing with emissionless transitions, i.e. the so-called cross relaxation which is the transfer of excitation energy in which the donor transfers to the acceptor only part of its excitation energy. This increases the intensity of excitation by a factor 2 or sometimes 3, and in some media the quantum efficiency of the process may exceed unity. In transport of a group of electronic excitations, formed during cross relaxation to the upper laser level with the quantum efficiency close to unity, these excitations are efficiently transformed to lasing [32]. Cross relaxation is activated with increasing concentration of the activators and, consequently, many highly concentrated systems contain cross relaxation stages in their working stages.

In a crystal of yttrium–erbium–aluminium garnet at the transition

of the erbium ions 4I11/2→ 4I13/2 with the chromium concentration higher than 1021 cm–3, lasing was obtained at the radiation wavelength of

2.9 µm, with a mean output power higher than 20 W. During cross relaxation, excitation is transferred from the long-life lower level (τ = 6 ms) to the relatively rapidly relaxing upper level (τ = 100 µs). This takes place at exciting pumping rates higher than some critical value. The probability of interaction of the excited ions depends on

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the population of the upper laser level. In this case, the laser transition ceases to be self-restricted and stationary inversion may take place. In stationary lasing in absorption of a single quantum in the visible end of the spectrum three quanta can be emitted in the 3 µm range [28].

Examination of the mechanisms of cross relaxation in the crystals of potassium–niobium–gallium garnet with the ions of trivalent thullium resulted in continuous lasing of radiation with a wavelength of 2.02 µm in pumping with laser radiation on an Nd-doped aluminium– yttrium garnet [33].

The efficiency of pumping radiation is also increased by stepped sensitising or the processes of summation of excitation. The physical nature of these processes is similar to the cross relaxation processes and they represent the emissionless transfer of excitation from one active centre to another. Above all, being an additional relaxation channel of excitation, they are capable of improving the operation of laser transitions ending on the metastable levels. Secondly, the stepped processes may ensure efficient utilisation of the energy absorbed in the bands, associated with the levels situated below the upper working level of the laser transition which in the conventional systems is assumed to be irreversibly lost. Finally, the efficient inclusion of electronic excitations stored on the storage levels in the course of prior cross relaxation conversion of absorption energy is possible during the process of pumping of laser transition. The quantum efficiency of excitation of the storage levels in the pumping bands of the medium is automatically transferred to the working level of the lasing transition [24].

The direction of investigations in this area is associated with the detection of the mechanisms and special features of the population of the main and intermediate levels of transfer of pumping energy [34,35] in order to obtain effective radiation parameters and optimise the lasing conditions [36].

5.5 LOW-THRESHOLD SOLID-STATE MEDIA

In addition to efficiency, another important characteristic of the solidstate laser is the lasing threshold, i.e. the minimum value of the pumping energy at which lasing starts. The main criterion of the low-threshold medium is the high value of the cross-section of the laser transition.

The widely used Nd:YAG crystal has the laser transition crosssection of σ = 3.3 × 10 –19 cm2 at a radiation wavelength of 1064 nm [37]. Active solid-state media with a larger laser transition cross-section are known, i.e. germanates of rare-earths, the transition cross-section of the NAYGeO4 crystal with Nd at a wavelength of 1.06 µm is σ 1.06 = 4.1 × 10 –19 cm2 [38]. The same large laser transition cross-

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section σ 1.06= 6 × 10 –19 cm2 and a low lasing threshold are shown by crystals of cadmium vanadate with Nd (Nd:CdVO4) [39]. Recently,

experiments were carried out with lasing on new low-threshold and efficient active media: lanthanum scandoborate, activated with ions of Nd and Cr (Nd3:Cr3+:LaSc3(BO3)4) [40], Nd3+: LaBGeO5 [41] and lithium–yttrium tetrafluoride (LiYF4) with praseodymium [22]. The high values of the laser transition cross-section and the low duration threshold are also typical of the crystal of potassium–gadolinium tungstenate with Nd (Nd:KGW) [22]. Investigations of these crystals make it possible to increase greatly the lasing efficiency of solid-state lasers.

5.6 EXPANDING THE SPECTRAL RANGE OF LASING

Expansion of the spectral range of lasing of the solid-state lasers is of considerable scientific and practical importance. Investigations in this direction can be divided conventionally into two large groups: the development of laser sources generating radiation in new areas of the spectrum; the development of solid-state active media with wide amplification bands. The first group includes the previously mentioned laser sources of the short-range infra-red lasing region (1.5–5 µm), based on emitting transitions in rare-earth ions. The application of the methods of non-linear optics also makes it possible to expand greatly the spectral range of coherent radiation by means of the lasing of harmonics, the displacement of frequencies and parametric frequency transformation. Recently, extensive investigations were carried out into the development of active media with wide gain bands. This type of active media is attractive because of two aspects: the fact that lasing is easily modified in a wide spectral range, and the lasing of extremely short light pulses by the methods of mode synchronisation.

Of the wide-band solid-state media it is important to mention the crystals activated by ions of the group of transition metals. One of these ion crystals is the alexandrite crystal which was used for the first time to produce lasing on the electronic–vibrational transition of chromium ions 4T2→ 4A2 [43]. The authors of Ref. 6,7,44,45 examined in detail the energy and, for the first time, the spectral–time parameters of the free lasing of an alexandrite laser and obtained tunable lasing in the range 700–800 nm. This stimulated the development of new active media with chromium ions. The lasing of Cr3+ ions on the electronicvibrational transition was realised and examined on crystals: emerald (Cr3+:Be3Al2Si6O18) [45, 46], perovskite (KZNF3), beryllium hexa-aluminate (BeAl6O10), ZnWO4, SrAlF5, ScBO3, Al2(WO4)3. KSc(WO4)2, and others. Quite detailed investigations have been carried out on the crystals of rare-earth–gallium garnet with chromium, lasing in the 4T2→ 4A2 electronic–vibrational; transition, which showed tunable lasing in the

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spectral ranges: 740–830 nm (Nd:GSGG), 710–790 nm (Nd:YSGG) and 760–810 nm (Nd:GSAG) [7,45].

A unique active medium in the group of the examined active media is the sapphire crystal with titanium ions (Ti3+:Al2O3), characterised by the widest amplification line of all active media, i.e. 680–1100 nm. In a spectrometer based on a titanium–sapphire laser, it was possible to realise continuously tunable lasing in the range 202–3180 nm. This crystal was used for producing record light pulses with a duration of 10 fs.

5.7 INCREASING THE BEAM STRENGTH OF SOLID-STATE MEDIA

The problem of the beam strength of solid-state active media is associated with the problem of laser failure of transparent materials. The mechanisms of laser failure can be divided into two groups [48]: determined by heating of absorbing defects in the medium; associated with impact and instantaneous ionisation, leading to optical breakdown in the medium.

Of the greatest importance with respect to the threshold of failure of the medium are metallic and nonmetallic inclusions. In glasses, the volume beam strength after radiation pulses with a duration of 30 ns is: in the presence of metallic inclusions 15 J/cm2, at a content of ceramic inclusions 150 J/cm2, and in the absence of inclusions 400500 J/cm2 [49]. In this case, thermal breakdown or explosion takes place as a result of rapid local heating in the areas of inclusions absorbing radiation. The inclusions usually appear during the growth of crystals or boiling of glass taking place at high temperatures, as microparticles of the crucible material. The improvement or modification of the technology of growth of laser active media and the purification of initial materials may minimise the number of microinclusions and suppress this failure mechanism.

Breakdown is usually associated with the formation of a subthreshold avalanche or multiphoton ionisation of defects or natural states of the matrix under the effect of the field of the light wave increasing the efficiency of absorption as a result of the appearance of excited carriers and dye centres [49].

A significant role in the failure of the active medium may be played by non-linear processes accompanying the propagation of radiation in the medium (in particular, self-focusing). In this case, the failure threshold is determined by the self-focusing threshold and not by the natural beam resistance of the material [48].

The build-up effect also plays a significant role in the processes of laser failure. In this effect, the micro-failure of the optical material takes place as a result of the effect of a series of laser radiation

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