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14 1. Basic Physics of Lasers: Radiationless Transition

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14

n1 E1 n2 Pumping

1.

Basic Physics of Lasers

Radiationless transition E2 Laser action E3

n0

E0

Radiationless transition

Fig. 1.9

Energy diagram of a four-level laser.

a small fraction of the Al3 ions are replaced with chromium Cr3 ions. The crystal is pumped by a flash lamp exciting the Cr3 ions from the ground electronic level E0 to the excited level E1, which is actually made up of sublevel series resulting from interaction between an electron and vibrations of the crystal lattice. The fast radiationless transition from the E1 state, characterized by a lifetime of about 50 ns causes the population of the metastable level E2 of the Cr3 ion, which has a lifetime of about 5 ms. If the flash lamp emits sufficiently intense pumping light, it is possible to produce population inversion that creates a laser action between the E2 and E0 levels (Fig. 1.8). The population inversion can be achieved either by increasing the metastable upper state population or by decreasing the lower state population. The latter cannot be used in the three-level lasers because the laser transition takes place between the metastable excited state E2 and the lowest energy level the ground state E0. It indicates that there is a competition between depletion and population of the E0 state, which leads to much lower efficiency of the population inversion than can be achieved in the four-level lasers illustrated in Fig. 1.9. In this case the level E3 populated as a result of the laser transition E2 ! E3 is depleted quickly in a radiationless transition E3 ! E0 . The four-level system permits a considerable increase in the efficiency of population inversion without delivering additional pumping energy. The most typical example of the four-level laser is a neodymium laser Nd:YAG (the solid active medium of the yttrium aluminum garnet (YAG) crystal doped with neodymium Nd3 ions) and a dye laser (liquid active medium). The ion argon Ar laser often used in molecular spectroscopy laboratories is not the four-level laser. However, it may be treated as a special case of the four-level laser, with a preliminary pumping causing the ionization of argon atoms (Fig. 1.10).
Radiationless transition Proper pumping 3p5 Radiationless transition Ionization pumping 3p6 Ar Ar+

4p Laser action 4s

Fig. 1.10

Energy diagram for one of the laser transitions of an argon laser Ar.

1.4.

Amplification and Saturation

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1.4. AMPLIFICATION AND SATURATION In thermodynamic equilibrium the population of energy states is described by the Boltzmann distribution. This indicates that at any temperature the majority of molecules usually stays in lower energy states. This statement is not always true for rotational levels exhibiting a high degree of degeneracy. Since the probabilities of stimulated transitions from the lower energy state to the higher energy state (absorption) and from the higher energy state to the lower energy state (stimulated emission) are equal, the total number of upward transitions is larger than the number of downward transitions, and the system absorbs the radiation energy @! < 0; @t 1:26

where ! is the energy density of the external field, that is the energy per unit circular frequency from the range between ! and ! d ! in volume units. @ In order to amplify the incident radiation ( @t! > 0), the population inversion has to be achieved n m n > n ; gm g n 1:27

where nm and nn are the number of molecules at m and n energy levels, gm and gn are the degeneracy numbers of the energy levels. When the population inversion is achieved, the traditional Lambert-Beer equation I I0 e l loses its sense. It was derived for the assumption that the absorption coefficient is constant, which is valid only in linear optics, when the incident radiation intensity is small and deviation from thermodynamic equilibrium is negligible. When larger intensity radiation is employed more and more molecules become transferred to a higher energy level and the state of saturation is achieved n n m n : gm gn 1:28

This indicates that the system is bleached, neither absorption nor emission of energy dominates. The LambertBeer equation I I0 e l can be maintained formally if we assume that 0. With further growth of the incident radiation intensity the system achieves the state called the population inversion, that is n m > n n and the system begins gn gm to emit more energy than it absorbs (formally the absorption coefficient becomes negative < 0). Fig. 1.11 illustrates these three situations.

m Absorbing system n Transparent system

m Emitting system n

m n

>0

=0

<0

Fig. 1.11

Dependence of absorption coefficient on incident radiation intensity in nonlinear optics range.

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