1

Basic Physics of Lasers

1.1. SPONTANEOUS AND STIMULATED TRANSITIONS. EINSTEIN COEFFICIENTS. PROPERTIES OF STIMULATED RADIATION To understand the principle of lasers and their applications, it is essential to understand the interaction of radiation with matter. Quantum properties dominate the field of molecular physics and molecular spectroscopy. Both radiation and matter are quantized. Radiation corresponds to the electromagnetic spectrum presented in Fig. 1.1 that covers the range from long wavelengths of meters to short wavelengths of a fraction of angstroms. Visible light is only a narrow part of the electromagnetic spectrum. For a given frequency of radiation !, the photons of that radiation have quantized energy E with only one value given by the famous Planck relationship E h! 1:1

The energy of atoms or molecules is also quantized, which means the energy levels can have only certain quantized values. In the molecular system we can distinguish electronic, vibrational, rotational or additional levels attributed to the interaction with an external magnetic field. Electrons or molecules can jump between the quantized energy levels. These transitions are stimulated by the photons of radiation. During the transitions the atoms or the molecules absorb or emit radiation. These processes can be classified as stimulated absorption, stimulated emission and spontaneous emission (Fig. 1.2). Stimulated absorption denotes a process in which an atomic or a molecular system subjected to an electromagnetic field of frequency ! absorbs an energy of h! from the photon. As a result of the absorption the atom or the molecule is raised from the state n to the upper state m of higher energy. Stimulated absorption occurs only when the energy of the photon precisely matches the energy separation of the participating pair of quantum energy states Em En h!; 1:2

where En and Em are the energies of the initial state n and the final state m, ! is the circular frequency of the incident radiation, and h is Plancks constant (h h/2 ).
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104 Short wave radio 102 Television FM radio Microwaves radar 1 102 Millimeter waves, telemetry 104

1.
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Basic Physics of Lasers

108 cm

3 106

3 108

3 1010

3 1012

3 1014

3 1016

Low frequency Long wavelength Low quantum energy

High frequency Short wavelength High quantum energy

Fig. 1.1

Electromagnetic spectrum.

If the condition (1.2) is fulfilled, we say that the radiation is in resonance with the molecular transition. Almost immediately (usually after nano- or picoseconds) most excited molecules return from the upper state, m, to the lower state, n, through the emission of a photon. This process is known as spontaneous emission. Spontaneous emission is obviously a quantum effect, because in classical physics the system can stay in a definite energy state infinitely long, when no external field is applied. Spontaneous emission in the visible spectral range is called luminescence or fluorescence, when the transition occurs between states of the same multiplicity, or phosphorescence, when the initial and final state have different multiplicity. Spontaneous emission is

Em En h Stimulated absorption Em En Spontaneous emission Em En Stimulated emission

Em En

Em En h Em En 2h

Fig. 1.2 Scheme of a two-level system illustrating stimulated absorption, spontaneous emission and stimulated emission phenomena.

X-rays Gamma rays 3 1018 Hz

Visible light

Ultraviolet

AM radio

Infrared

1.1.

Spontaneous and Stimulated Transitions

not connected with the incident radiation in any way. The incident radiation does not affect the lifetime of a molecule in the excited state m from which the spontaneous emission is emitted. Moreover, spontaneous emission is not coherent, i.e., the emitted photons have no definite phase relation to each other. The emission comes from independent atoms or molecules, which are not related to one another in phase. When the external electromagnetic field is strong, emission can take place not only spontaneously but also under stimulation by the field. This kind of emission is called stimulated emission, which like stimulated absorption, is induced by the external radiation. In stimulated emission a photon of the incident radiation interacts with a molecule that is in the higher energy state m. The interaction results in giving the energy quantum back to the radiation field by a molecule, followed by a simultaneous emission and dropping back from the upper level m to the lower level n. In another words, if a molecule is already in an excited state, then an incoming photon, for which the quantum energy is equal to the energy difference between its present level and the lower level, can stimulate a transition to that lower state, producing a second photon of the same energy. In contrast to spontaneous emission, stimulated emission exhibits phase coherence with the external radiation field. It indicates that the phases of the incident electric field E E0 cos(!t k r ) and the emitted stimulated radiation are the same. Since the emitted photons have definite time and phase relations with the external field, they also have a definite time and phase relation to each other. Therefore the emitted light has a high degree of coherence. The coherence is a quantum effect and requires a quantum mechanical treatment of the interaction between the radiation and matter, which is beyond the scope of this book. However, the concept of coherence can also be understood by using a classical description of radiation. In the classical description the external electromagnetic field induces in a medium a polarization by forcing the dipole moments to oscillate in a phase consistent with the phase of the incident radiation. The oscillating dipole moments emit in turn radiation coherent with their own oscillations. A detailed description of the classical interactions between the field and the induced oscillators can be found in [1]. Stimulated transitions have several important properties: a) the probability of a stimulated transition between the states m and n is different from zero only for the external radiation field that is in resonance with the transition, for which the photon energy h! of the incident radiation is equal to the energy difference between these states, Em En h!, b) the incident electromagnetic radiation and the radiation generated by stimulated transitions have the same frequencies, phases, plane of polarization and direction of propagation. Thus, stimulated emission is, in fact, completely indistinguishable from the stimulating external radiation field, c) the probability of a stimulated transition per time unit is proportional to the energy density of the external field ! , that is the energy per unit of the circular frequency from the range between ! and ! d ! in the volume unit.

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Basic Physics of Lasers

The properties of stimulated absorption, stimulated emission and spontaneous emission discussed so far can be described using the following relations:
A Bnm Wnm SE B mn Wmn ! !

for stimulated absorption; for stimulated emission; for spontaneous emission;

1:3 1:4 1:5

SPE A mn Wmn

A , W SE and W SPE denote the probabilities of the transitions for stimuwhere Wnm mn mn lated absorption, stimulated emission and spontaneous emission per time unit. The constants of proportionality Bnm, Bmn and Amn are called the Einstein coefficients. Let us establish the relations between Bnm, Bmn and Amn. For this purpose let us consider an ensemble of quantum molecules in equilibrium with the field of their own radiation (absorbed and emitted photons), which is called thermal radiation. This type of equilibrium is often considered in physics, and a spectacular example of its application is Plancks formula for blackbody radiation. Let us assume that the quantum molecules are represented by two-level quantum states that are non-degenerated. Since the system is in equilibrium with the radiation field, the number of the transitions per unit time from the upper state m ! n has to be equal to the number of the transitions from the lower state n ! m

Nm!n Nn!m :

1:6

The number of the transitions, N, depends on the transition probabilities per time unit W, and on the number of molecules in the initial state. Eq. (1.6) can be written as Wm!n nm Wn!m nn : 1:7

For the system in equilibrium the quantum levels population is described by the Boltzmann distribution n Em n nn exp Em kT ; 1:8

where k is Boltzmanns constant, and T is temperature in Kelvins. Moreover, the total probability of the emission m ! n is the sum of spontaneous emission W SPE mn SE and stimulated emission W mn
SPE SE Wm!n Wmn W mn ;

1:9

therefore using eqs. (1.41.5) one gets, Wm!n Amn Bmn

!:

1:10

The total probability of the absorption Wn!m is equal to the probability of stimuA given by eq. (1.3) lated absorption W nm
A Wn!m Wnm Bnm !:

1:11

1.1.

Spontaneous and Stimulated Transitions

Inserting (1.10) and (1.11) into equation (1.7) one can write Amn Bmn
! nm

Bnm

! nn :

1:12

Inserting eq. (1.8) into eq. (1.12) one obtains the radiation density ! :
!

A mn B B mn nm

1 exp
E
m

En

: 1

1:13

Bmn

kT

Because the density of the thermal radiation energy ! , is described by Plancks equation for blackbody radiation
!

! 2 h! h! c3 exp kT

1:14

one can compare (1.13) and (1.14). From the comparison we obtain the following relations for the Einstein coefficients Bnm Bmn and Amn !3 h Bmn : c3 1:16 1:15

Readers who are interested in the derivation of Plancks equation are referred to textbooks describing this issue, e.g., [2]. When the levels m and n are degenerated, and their degeneration degrees are gm and gn, the relation (1.15) is modified to the form gn Bnm gm Bmn : 1:17

Thus, we have obtained the relations between the Einstein coefficients. First, equation (1.15) indicates that the probability of stimulated emission is equal to the probability of stimulated absorption. A practical hint from this relation is that materials characterized by strong absorption are expected to exhibit also a large stimulated emission. The relation (1.16) indicates that a material in which spontaneous emission does not take place, does not exhibit stimulated emission either. These simple relations determine the principal conditions which should be taken into account when looking for materials to be employed as the active medium in lasers (see section 1.2). To gain a better insight into the interplay between these three processes let us calculate the coefficient !3 h/ c3 in equation (1.16) determining the connection between spontaneous emission Amn and stimulated emission Bmn. For a wavelength 514 nm characteristic for an ion argon laser Ar corresponding to ! 36:64 1014 rad s 1 the coefficient !3 h/ c3 is 6 10 14. This indicates that the coefficient of stimulated emission, Bmn, is much larger than the coefficient of spontaneous emission, Amn. However, it does not indicate that the intensity of spontaneous