Nuclear excitation by electron transition

Abstract A consistent relativistic energy approach to the calculation of probabilities of cooperative electron-gamma-nuclear processes is developed. The nuclear excitation by electron transition (NEET) effect is studied. The NEET process probability and cross section are determined within the S-matrix Gell-Mann and Low formalism (energy approach) combined with the relativistic many-body perturbation theory (PT). Summary of the experimental and theoretical works on the NEET effect is presented. The calculation results of the NEET probabilities for the y Os, yy Ir, and yg Au atoms are presented and compared with available experimental and alternative theoretical data. The theoretical and experimental study of the cooperative electron-gamma-nuclear process such as the NEET effect is expected to allow the determination of nuclear transition energies and the study of atomic vacancy effects on nuclear lifetime and population mechanisms of excited nuclear levels. 

Relativistic Energy Approach to the Process of Nuclear Excitation by Electron Transition... 

The fundamental parameter of the cooperative NEET process is a probability NEET (cross section) of the nuclear excitation by electron transition. In fact, it can be defined as the probability that the decay of the initial excited atomic state will result to the excitation of and subsequent decay from the corresponding nuclear state. Within the energy approach, the decay probability is connected with an imaginary part of energy shift for the system (nuclear subsystem plus electron subsystem) excited state. An imaginary part of the excited state / energy shift in the lowest PT order can be in general form written as [18,26]... 

One aspect of the decay rate of "mTc has been suggested by Hinneburg et al. [35]. Its low-lying level structure is shown in Fig. 6. The energy difference of 2.17 keV between the 142.7 and 140.5 keV nuclear levels is similar to that between the M5 and L3 atomic levels (2.42 keV), but this degree of similarity is not enough to cause an inverse NEET (nuclear transition by electronic transition) [36], However, de-excitation is possible by an electron-bridge (EB) mechanism [35] which involves a third order correction to the internal conversion (IC). Emission of a photon and the simultaneous ejection of an orbital... 

It is obvious that more sophisticated relativistic many-body methods should be used for correct treating the NEET effect. Really, the nuclear wave functions have the many-body character (usually, the nuclear matrix elements are parameterized according to the empirical data). The correct treating of the electron subsystem processes requires an account of the relativistic, exchange-correlation, and nuclear effects. Really, the nuclear excitation occurs by electron transition from the M shell to the K shell. So, there is the electron-hole interaction, and it is of a great importance a correct account for the many-body correlation effects, including the intershell correlations, the post-act interaction of removing electron and hole. 

In spectroscopy we may distinguish two types of process, adiabatic and vertical. Adiabatic excitation energies are by definition thermodynamic ones, and they are usually further defined to refer to at 0° K. In practice, at least for electronic spectroscopy, one is more likely to observe vertical processes, because of the Franck-Condon principle. The simplest principle for understandings solvation effects on vertical electronic transitions is the two-response-time model in which the solvent is assumed to have a fast response time associated with electronic polarization and a slow response time associated with translational, librational, and vibrational motions of the nuclei.92 One assumes that electronic excitation is slow compared with electronic response but fast compared with nuclear response. The latter assumption is quite reasonable, but the former is questionable since the time scale of electronic excitation is quite comparable to solvent electronic polarization (consider, e.g., the excitation of a 4.5 eV n — n carbonyl transition in a solvent whose frequency response is centered at 10 eV the corresponding time scales are 10 15 s and 2 x 10 15 s respectively). A theory that takes account of the similarity of these time scales would be very difficult, involving explicit electron correlation between the solute and the macroscopic solvent. One can, however, treat the limit where the solvent electronic response is fast compared to solute electronic transitions this is called the direct reaction field (DRF). 49,93 The accurate answer must lie somewhere between the SCRF and DRF limits 94 nevertheless one can obtain very useful results with a two-time-scale version of the more manageable SCRF limit, as illustrated by a very successful recent treatment... 

In the case of direct vibrational excitation, the vibrational transition probability is given by p, where are the intermediate and ground vibrational states, respectively, and is the vibrational transition moment. The electronic transition probability out of the intermediate state is < n < e ng e > n>, where are the excited and ground electronic states, respectively, and is the electronic dipole moment operator and vibrational state in the upper electronic state. Applying the Born-Oppenheimer approximation, where the nuclear electronic motion are separated, S can be presented as... 

The acetylene A <- X electronic transition is a bent <- linear transition that would be electronically forbidden ( - ) at the linear structure. The usual approximation is to ignore the possibility that the electronic part of the transition moment depends on nuclear configuration and to calculate the relative strengths of vibrational bands as the square of the vibrational overlap between the initial and final vibrational states (Franck-Condon factor). A slightly more accurate picture would be to express the electronic transition moment as a linear function of Q l (the fra/w-bending normal coordinate on the linear X1 state) in such a treatment, the transition moment would be zero at the linear structure and the vibrational overlap factors would be replaced by matrix elements of Qfl- Nevertheless, as long as one makes use of low vibrational levels of the A state, neglect of the nuclear coordinate dependence of the electronic excitation function is unlikely to affect the predicted dynamics or to complicate any proposed control scheme. 

Nuclear decay processes that are often used to populate Mossbauer isotope excited states are (30) electron capture (electron + proton neutron), / decay (neutron - proton + electron), and isomeric transition (a long half-life nuclear excited state decays to the Mossbauer excited state). In addition, several of the parent nuclides of the heavy isotopes can be populated by a-particle emission. 

According to the Franck-Condon principle, the photoexcitation triggers a vertical transition to the excited state, which is followed by a rapid nuclear equilibration. Without donor excitation, the electron transfer process would be highly endothermic. However, after exciting the donor, electron transfer occurs at the crossing of the equilibrated excited state surface and the product state. 

The wavepacket /(t), on the other hand, is constructed in a completely different way. In view of (4.4), the initial state multiplied by the transition dipole function is instantaneously promoted to the excited electronic state. It can be regarded as the state created by an infinitely short light pulse. This picture is essentially classical (Franck principle) the electronic excitation induced by the external field does not change the coordinate and the momentum distributions of the parent molecule. As a consequence of the instantaneous excitation process, the wavepacket /(t) contains the stationary wavefunctions for all energies Ef, weighted by the amplitudes t(Ef,n) [see Equations (4.3) and (4.5)]. When the wavepacket attains the excited state, it immediately begins to move under the influence of the intramolecular forces. The time dependence of the excitation of the molecule due to the external perturbation and the evolution of the nuclear wavepacket /(t) on the excited-state PES must not be confused (Rama Krishna and Coalson 1988 Williams and Imre 1988a,b)... 

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