# Essay on the Gamma Ray Laser September 197911footnote 1Typed in 1999 after the original September 1979 manuscript

The coherent, high-intensity sources of light, known as lasers, represented a great progress in modern optics. Whenever a sufficiently high population can be stored in a higher state of a quantal system which also has a lower, relatively unpopulated, energy level, the process of stimulated emission confers to that source the character of a laser. We say ”character”, because strictly speaking, an essential component of a laser is the resonant cavity. But if the particles in higher state are so dense and the cross section of the process so big as to give rise to large gains, the upper state is depopulated by a travelling wave: we have to do in this case not with a true laser, but rather with a superradiant source. There is a property of the laser radiation which is conserved, even with superradiant sources: the high intensity of the radiation; to a certain extent, it is also conserved the directionality of the radiation.

Usually the optical cavity consists of two mirrors with good reflectivity at the operating frequency of the laser. The property of reflection is related at optical frequencies to the interaction of the electromagnetic field with the free electrons characteristic to the internal structure of the mirror. Reflective materials can be found which cover the whole range of optical frequencies.

The basic concepts related to the optical laser, like discrete energy levels, populating of the higher states, stimulated emission, inversion and gain, are in principle applicable to any quantal system. Practically, it is not always easy to accomodate the requirements for inversion and gain.

Lasers are built which make use of atomic and molecular transitions, which are operating in the infrared, in the visible, in the ultraviolet. The upper limit of the photon energy attained with the excimer lasers is of about 10 eV, or 10 nm. Attempts to obtain laser radiation in the X-ray region from atomic transitions to the inner electronic shells have failed because of the extremely short life-times of the corresponding excited states.

The level of structure of the matter, next to the molecular and atomic one, is represented by the atomic nucleus. A given nucleus can exist in the ground state, or in one of its excited states. The transitions between these states are accompanied by the emission or absorption of electromagnetic radiation. The radiations characteristic to nuclear transitions are called gamma rays and their energy ranges from keV’s to tens of MeV.

The life-time of the nuclear excited states cover an extraordinarily wide range of values: states with a life-time of $`10^{18}`$ sec, and excited states with life-time of years are known; a frequent life-time of a nuclear level in the 1 MeV region is 1 nsec.

Because the nucleus is relatively isolated of the other surrounding nuclei by the electronic shell, the width of the levels is not affected by collisional processes. Therefore, the cross section for many resonant transitions is the Breit-Wigner one, which is proportional to the square of the wavelength of the electromagnetic radiation, and lower energy gamma rays have so large cross sections as $`10^{18}`$ cm<sup>2</sup>. Another consequence of the screening between the nuclei, mediated by the electron cloud, is the existence of long-lived excited states, called isomeric states, which correspond to highly forbidden gamma ray transitions.

A nucleus may be found in its excited state as a result of the decay of another unstable nucleus and a sample of such unstable nuclei represents the common gamma ray source. The unstable nuclei are obtained from other, stable nuclei by irradiation with fluxes of particles, which are most conveniently neutrons. Sometimes, the absorption by a nucleus of another particle, like a neutron, leaves the resulting nucleus in one of its excited states, and represents a method in situ for having nuclei in excited states.

The thermal motion of the nuclei produces a Doppler broadening of the lines, and the energy shift known as the recoil shift, due to the momentum carried away by the nucleus in the process of transition, often puts off resonance the process of transition. These two effects, which are proportional to the energy, and to the square of the transition energy, become important with gamma ray transitions, and produce a diminishing of the transition cross section by many orders of magnitude. Yet for transition energy not higher than 100 keV, the binding of the nuclei in crystalline lattices eliminates both the Doppler effect and the recoil energy shift, through what is known as the Mössbauer effect.

Since a typical solid-state particle density is some $`10^{22}`$/cm<sup>3</sup>, since there are means of populating higher nuclear states, and since the cross section for the induced emission can be, under favorable conditions, some $`10^{18}`$ cm<sup>2</sup>, there are no principle constraints to the construction of a device operating as a laser at gamma-ray frequencies. Such a device would be a superradiating gamma ray source, rather than a laser, because there is not possible to construct the analogue of the optical cavity at gamma ray frequencies. The purpose of this paper is to investigate the conditions for the amplification of the gamma rays.

Despite this apparently favorable situation, the attempts to obtain stimulated gamma radiation failed. If one tries to populate the excited states by the conventional method of the decay of unstable nuclei, the particle density in the excited state is some $`10^{22}`$/cm<sup>3</sup>, corresponding to a sample consisting only of the unstable species, times the ratio of the life-time of the level to the half-life of the unstable nucleus. Even in the very favorable situation of a level of 10 $`\mu `$sec and a half-life of $`10^3`$ seconds, the particle density in the excited state cannot exceed $`10^{15}`$/cm<sup>3</sup>, and the resulting gain, $`10^3`$/cm is not sufficient for amplification. Levels with longer life-time cannot be used, because they are broadened by imperfect sample preparation and that diminishes the cross section, and unstable nuclei with halflives lower than $`10^3`$ sec are difficult to concentrate up to $`10^{22}`$/cm<sup>3</sup>.

Or one could try to populate the upper level by irradiating the sample with neutrons. The fraction of the nuclei in the excited state is the number of neutrons per cm<sup>2</sup> sec times the neutron capture cross section times the life-time of the level. <sup>2</sup><sup>2</sup>2It is implicit that the excitation by absorption of neutrons creates a chemically different nucleus which is in the excited state, and the same at the decay of an unstable nucleus. The highest today-available neutron flux is some $`10^{15}`$/cm<sup>2</sup> sec, and assuming $`10^{22}`$ cm <sup>2</sup> (100 barns) for the neutron capture cross section and $`10^5`$ sec for the life-time of the level, the fraction becomes $`10^{12}`$, which corresponds to an upper-state particle density not exceeding $`10^{11}`$/cm<sup>3</sup>, and a gain of $`10^7`$.

The case of a neutron pulse appears more favorable: the fraction of the nuclei in the upper, excited state is the product of the number of neutrons per cm<sup>2</sup> times the neutron capture cross section. For a neutron capture cross section of 100 barns, the neutron density resulting in a gain of 1/cm is $`10^{18}`$/cm<sup>2</sup>, or at least $`10^{20}`$ neutrons per $`10^5`$ sec pulse duration, and that is not a laboratory experiment.

A gain of $`10^3`$/cm is not, strictly speaking, without significance, but the samples appropriate for the assumed very narrow lines are probably sensitive to the high irradiation level required to obtain the population of the upper state.

The previous estimations show that states with life-times below 10 $`\mu `$sec do not allow enough populating to obtain relevant gains. High particle concentrations could be obtained in the isomeric states. For long-lived states, one can think, in principle, of samples consisting only of isomeric nuclei, that is of densities of some $`10^{22}`$/cm<sup>3</sup>. The difficulty here is that the cross section of the transition to a lower state is the Breit-Wigner, $`10^{18}`$ cm<sup>2</sup>, cross section, reduced by the ratio of the life-time of the lower level to the half-life of the isomeric state, and, as before, imperfect sample preparation and the concentration make that this ratio be something like $`10^5/10^3`$, and that results in a gain not exceeding $`10^3`$/cm, under most favorable conditions. One could think of using the transition between the upper, isomeric state, and the lower, ground state, but the imperfect sample preparation reduces the Breit-Wigner cross section in the ratio of the effective to the natural life-time of the isomeric state. We are confrunted here with the puzzling problem of having a large concentration of nuclei in the upper, isomeric state, which seemingly cannot be transferred to the lower state.

We have sometimes thought that a two photon transition could provide a way to avoid the small matrix elements connecting the isomeric state with the lower states. The two-photon nuclear transitions mediated by the magnetic sublevels, which generally have cross sections up to $`10^{20}`$ cm<sup>2</sup>, are not appropriate to this situation because their cross section contains the same small matrix element, which in fact defines the existence of the isomeric state. Other types of multiphoton processes are clearly not useful, because their cross section is definitely lower than $`10^{23}`$ cm<sup>2</sup>.

But one possibility remains: the existence of states nearly degenerate with the nuclear isomeric state. Roughly speaking, if the nuclei in the sample are initially in the isomeric state, an electromagnetic field irradiating the sample, of frequency resonant to the transition energy between the isomeric and the nearly degenerate state, will populate the nearly degenerate state; the larger the cross section for single-photon, resonant transition from the isomeric to the nearly degenerate, states, and the larger the power density in the electromagnetic field, the higher the particle concentration in the state degenerate with the isomeric state. The transition from the level nearly degenerate with the isomeric state, which level will be called the normal upper level, to a lower state has a Breit-Wigner cross section, provided the life-times of the normal and of the lower levels are not too long. This will be also a Mössbauer transition, because it is the energy transferred between the nucleus and the field which determines the Mössbauer character of the process, and not the absolute location of the levels. Now, if the gain resulting from the particle concentration in the normal upper state is large enough, a wave travelling in the active sample will be amplified and the upper level will be depleted in the creation of a gamma ray pulse.

The size of the sample is limited by its absolute radioactivity. A 1 Ci sample consisting of nuclei in the isomeric state of half-life $`10^6`$ sec ($`10`$ days) would contain about $`3\times 10^{16}`$ isomeric nuclei. Assuming complete conversion of the isomeric nuclei to the lower state, the gamma-ray pulse would carry an energy of about 50 Joules. We also note that a global recoil momentum becomes important due to the high concentrations in the sample.

The many intersections which occur in the Nilsson diagrams suggest that nearly degenerate states have a real existence. The fact that one of the states has to be isomeric, and the selection rule requirements, represent, of course, additional constraints. In any case, two nearly degenerate states with an energy separation corresponding to optical frequencies are beyond the resolving power of the existing gamma-ray spectroscopy. Spontaneous transitions between such states are also imperceptible because that probability is proportional to the third power of the frequency of transition.

The cross section of a single photon radiative exchange between the states $`n,n_0`$ of a quantal system and the mode of frequency $`\omega `$ and width $`\gamma `$ of the electromagnetic field is, apart from numerical coefficients,

$$\sigma \frac{e^2}{\mathrm{}c}\frac{\omega }{\gamma }|v_{nn_0}|^2,$$
(1)   
where $`ev`$ is the reduced matric element $`v_\alpha `$ defined in Eq. 44 of the Third Gamma Optical Paper.<sup>3</sup><sup>3</sup>3Note added in May 1999: the referenced work is S. Olariu et al., Phys. Rev. C 23, 50 (1981); it was submitted for publication on 30 November 1979. Since the natural width of a level is proportional to $`\frac{e^2}{\mathrm{}c^3}\omega ^3|v_{nn_0}|^2,`$ and if the width of the mode is the same as the width of the level, then substituting the above expression in the expression, Eq. 1, for $`\sigma `$ gives the $`\lambda ^2`$ dependence of the Breit-Wigner cross section.

In our case, the width $`\gamma `$ of the normal upper state is determined by the transition to the lower state (see Figure). The width is roughly

$$\gamma \frac{e^2}{\mathrm{}c^3}\omega _{nl}^3|v_{nl}|^2.$$
(2)   
The cross section for a single photon transition between the isomeric and the normal upper state is, according to Eq. 1,

$$\sigma _{ni}\frac{e^2}{\mathrm{}c}\frac{\omega _{ni}}{\gamma }|v_{ni}|^2.$$
(3)   
Substituting in Eq. 3 the expression of the width of the normal upper state, Eq. 2, gives for the cross section $`\sigma _{ni}`$,

$$\sigma _{ni}\left(\frac{c}{\omega _{nl}}\right)^2\frac{\omega _{ni}}{\omega _{nl}}\frac{|v_{ni}|^2}{|v_{nl}|^2}.$$
(4)   
The first factor represents the Breit-Wigner cross section between the states $`n`$ and $`l`$ and Eq. 4 states that the cross section for a single photon transition between the nearly degenerate states, $`n`$ and $`i`$, is the typical $`10^{18}`$ cm<sup>2</sup>, Breit-Wigner cross section, reduced in the ratio of the energy separation to the energy of transition and by a factor depending on he type of transitions between the states $`ni`$ and $`nl`$. For example, the transition $`il`$ could be E3 and the transitions $`ni,nl`$ be E1 and E2; depending on which of them is the E1, the ratio of the matrix elements is larger or smaller than 1. It is, therefore, not possible to obtain an a priori estimate of the cross section $`\sigma _{ni}`$.

If the sample consisting of nuclei in the isomeric state $`i`$ is illuminated by a pulse of optical radiation, the probability of having the nucleus in the normal upper state $`n`$ is the number, $`N_{/cm^2}`$, of optical photons per cm<sup>2</sup> which crosses the sample multiplied by the transition cross section $`\sigma _{ni}`$, provided the duration of the pulse is shorter or comparable to the width of the state $`n`$. In order to obtain the significant gamma ray gain of 1/cm with a gamma-ray cross section of $`10^{18}`$ cm<sup>2</sup> we have to have a particle density in the state $`n`$ of $`10^{18}`$ nuclei/cm<sup>3</sup>. That means that the product $`N_{/cm^2}\sigma _{ni}`$ has to be about $`10^4`$. We have explained previously that the radioactivity from the isomeric state limits the number of the nuclei in the sample to about $`10^{18}`$ nuclei. If the length of the sample is 1 cm, its transverse area will be about $`10^3`$ cm<sup>2</sup>.

A pulse of 10 Joule of photon energy 1 eV corresponds to about $`10^{20}`$ photons, or $`10^{23}`$ photons/cm<sup>2</sup> crossing the sample per pulse. That means that a cross section $`\sigma _{ni}`$ of about $`10^{27}`$ cm<sup>2</sup> would result in the significant gain of 1/cm. From Eq. 4, we see that the ratio $`\omega _{ni}/\omega _{nl}`$ is about $`10^4`$, while the ratio of the matrix elements may be small as well as large. It is therefore not unreasonable to expect cross sections $`\sigma _{ni}`$ in the range $`10^{24}`$ cm<sup>2</sup>.

The fine investigation of the nuclear structure in the vicinity of a given state has, of course, a fundamental importance. We have argued here that, if a state nearly degenerate with long-lived isomeric states exists, which is related to this and to the lower states by appropriate selection rules, this occurrence will open a way toward the gamma ray laser.

The high-resolution investigation of the nuclear structure near an isomeric state is a surprisingly simple problem. The idea is that, if the sample consisting of isomeric nuclei is immersed in tunable optical radiation, the resonance of the optical radiation to the sought for nearly degenerate transition energy would result in the increase of the radioactivity of the sample.

That will happen whenever the product $`N_{/cm^2}\sigma _{ni}/\tau _n`$ which represents the probability of the emission of gamma rays through the process $`inl`$ is larger than the probability of spontaneous emission from the state $`i`$, $`1/\tau _i`$; $`\tau _n`$ and $`\tau _i`$ are the life-times of the states $`n`$ and $`i`$, respectively:

$$N_{/cm^2}\sigma _{ni}>\tau _n/\tau _i.$$
(5)   
Values of $`\tau _n`$ of practical interest are $`\tau _n<10\mu `$sec (because of the difficulties in the preparation of the samples) and for $`\tau _i`$ we assume $`10^6`$ seconds (10 days). Because we need radiation, tunable over a wide range of frequencies, it seems appropriate to take $`N_{/cm^2}10^{18}`$/cm<sup>2</sup> per pulse. Then the lower limit of measurable $`\sigma _{ni}`$ is of about $`10^{30}`$ cm<sup>2</sup>. Of course, this technique of measurement of $`\sigma _{ni}`$ requires the comparing of the signals obtained with the optical field on, and off. Weak gamma ray sources (1 mCi) and very small particle concentrations of isomeric nuclei can be used. This method is different from the radiofrequency resonance techniques, because it is not the absorption of the optical power which matters, but its effect on the large, gamma ray, transition. The nuclides with isomeric states of half-life longer than 10 days are listed further:

half-life $`>`$ 10 d   
Nb<sup>92</sup>, Nb<sup>93</sup>, Tc<sup>95</sup>, Tc<sup>97</sup>, Rh<sup>102</sup>, Ag<sup>108</sup>, Ag<sup>110</sup>, Cd<sup>115</sup>, Sn<sup>117</sup>, Sn<sup>119</sup>, Sn<sup>121</sup>, Te<sup>121</sup>, Te<sup>123</sup>, Te<sup>125</sup>, Te<sup>127</sup>, Te<sup>129</sup>, Xe<sup>131</sup>, Pm<sup>148</sup>, Ho<sup>166</sup>, Lu<sup>174</sup>, Lu<sup>177</sup>, Hf<sup>178</sup>, Hf<sup>179</sup>, Re<sup>184</sup>, Re<sup>186</sup>, Ir<sup>192</sup>, Ir<sup>193</sup>, Ir<sup>194</sup>, Bi<sup>210</sup>, Am<sup>242</sup>

Since the tunability range of the optical power, multiplied by the number of isomeric states and divided by the average separation between the nuclear levels represents the statistical probability of finding a convenient degenerate pair, there is a few percent chance for the existence of the pair. But, as very little is known about the fine actual nuclear structure, a search for degenerate states could demonstrate equally no structure as well as reveal surprising things.