ABSTRACT
We explore the unusual nature of chemical bonding of thorium atoms with a ring of six carbon atoms (hexagon) in novel carbon materials. Our ab initio calculations of Th-based metallofullerenes (Th@C60 and Th@C20) and Th bound to benzene or coronene at the Hartree-Fock level with the second order perturbation (MP2) correction accounting for the van der Waals interactions demonstrate that the optimal position of the thorium atom is where it faces the center of a hexagon and is located at a distance of 2.01-2.07 Å from the center. For Th encapsulated in C60 it is found at 2.01 Å, whereas the other local energy minima are shifted to larger energies (0.22 eV and higher). Inside C60 the highest local minimum at 1.17 eV is observed when Th faces the center of the five member carbon ring (pentagon). Based on our calculations for Th with benzene and coronene where the global minimum for Th corresponds to its position at 2.05 Å (benzene) or 2.02 Å (coronene) from the hexagon center, we conclude that a well pronounced minimum is likely to be present in graphene and in a single wall carbon nanotube. The ground state of Th is singlet, and other high spin states (triplet and quintet) lie higher in energy (>1.62 eV). We discuss a potential use of carbon nanomaterials with the 229Th isotope having its nuclear transition in the optical range, for metrological purposes.
ABSTRACT
Excitation of the anomalously low lying nuclear isomer ^{229m}Th(3/2^{+},8.28±0.17 eV) in the process of inelastic electron scattering is studied theoretically in the framework of the perturbation theory for the quantum electrodynamics. The calculated cross sections of ^{229m}Th by the extremely low energy electrons in the range 9-12 eV for the Th atom and Th^{1+,4+} ions lie in the range 10^{-25}-10^{-26} cm^{2}. Being so large, the cross section opens up new possibilities for the effective nonresonant excitation of ^{229m}Th in experiments with an electron beam or electron (electric) current. This can be crucial, since the energy of the isomeric state is currently known with an accuracy insufficient for the resonant excitation by photons. In addition, the cross section of the time reversed process is also large, and as a consequence, the probability of the nonradiative ^{229m}Th decay via the conduction electrons in metal is ≈10^{6} s^{-1}, that is, close to the internal conversion probability in the Th atom.
ABSTRACT
The main decay channels of the anomalous low-energy 3/2^{+}(7.8±0.5 eV) isomeric level of the ^{229}Th nucleus, namely the γ emission and internal conversion, inside a dielectric sphere, dielectric thin film, and conducting spherical microcavity are investigated theoretically, taking into account the effect of media interfaces. It is shown that (1) the γ decay rate of the nuclear isomer inside a dielectric thin film and dielectric microsphere placed in a vacuum or in a metal cavity can decrease (increase) in dozen of times, (2) the γ activity of the distributed source as a function of time can be nonexponential, and (3) the metal cavity, whose size is of the order of the radiation wavelength, does not affect the probability of the internal conversion in ^{229}Th, because the virtual photon attenuates at much shorter distances and the reflected wave is very weak.
ABSTRACT
A possibility of the amplification of the 7.6 eV γ radiation by the stimulated γ emission of the ensemble of the (229m)Th isomeric nuclei in a host dielectric crystal is proved theoretically. This amplification is a result of (1) the excitation of a large number of (229m)Th isomers by laser radiation, (2) the creation of the inverse population of nuclear levels in a cooled sample owing to the interaction of thorium nuclei with the crystal electric field or with an external magnetic field, (3) the emission or absorption of the optical photons by thorium nuclei in the crystal without recoil, and (4) the nuclear spin relaxation through the conduction electrons of the metallic covering.
