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Relativistic Prediction of the Ground State of Atomic Lawrencium J.-P Relativistic prediction of the ground state of atomic Lawrencium J.-P. Desclaux, B. Fricke To cite this version: J.-P. Desclaux, B. Fricke. Relativistic prediction of the ground state of atomic Lawrencium. Journal de Physique, 1980, 41 (9), pp.943-946. 10.1051/jphys:01980004109094300. jpa-00208925 HAL Id: jpa-00208925 https://hal.archives-ouvertes.fr/jpa-00208925 Submitted on 1 Jan 1980 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. J. Physique 41 (1980) 943-946 SEPTEMBRE 1980, 943 Classification Physics Abstracts 31.20 Relativistic prediction of the ground state of atomic Lawrencium J.-P. Desclaux and B. Fricke (*) Centre d’Etudes Nucléaires de Grenoble, DRF-LIH, 85X, 38041 Grenoble Cedex, France (Reçu le 4 février 1980, accepté le 28 avril 1980) Résumé. 2014 Contrairement à la systématique du tableau périodique, mais en accord avec les suggestions antérieures de Brewer et de Mann, la configuration de l’état fondamental de l’atome de Lawrencium (Z = 103) n’est pas 7s2 6d 2D3/2 mais 7s2 7p 2P1/2. Cet écart à l’évolution normale à travers le tableau périodique est dû à l’importance des effets relativistes sur la couche la plus exteme 7p1/2. On donne les résultats obtenus par la méthode multi- configurationnelle Dirac-Fock pour l’atome de Lawrencium et certains atomes similaires plus légers. Ces calculs incluent les contributions magnétiques et de retard ainsi qu’une estimation des corrections dues à l’électrodyna- mique quantique. Abstract. 2014 In contradiction to the prediction of the Periodic Table but in agreement with earlier suggestions by Brewer and Mann, the ground state configuration of atomic Lawrencium (Z = 103) will not be 7s2 6d 2D3/2 but 7s2 7p 2P1/2. The reason for this deviation from normal trends across the Periodic Table are strong relativistic effects on the outermost 7p1/2 orbital. Multiconfiguration Dirac-Fock calculations are reported for Lawrencium and analogous lighter atoms. These calculations include contributions from magnetic and retardation interactions and an estimation of quantum electrodynamic corrections. Introduction. - It is well-known that relativistic différence between the two possible ground states effects play an important role in the interpretation was found to be very small. A good theoretical of inner shell phenomena [1]. During the last years, prediction is very important, not only as a guide to one also became more and more aware of the rela- the complicated experiment, but also as an excellent tivistic influences on outer shell problems like atomic check for relativistic influences on outer shells and radii [2], oscillator strength [3], photo-electron spec- of the quality of the calculations. troscopy [4] etc. From the interpretation of relativistic Because the splitting between the two configurations SCF calculations of heavy atoms [5] it became obvious is expected to be small, single configuration Dirac- that chemistry is also partly affected by relativistic Fock calculations may give the wrong ordering of the effects, even in the known region of elements like the levels if correlation effects, neglected in such calcu- main valency two of lead. lations, have rather different contributions to the Up to now, no element is known whose ground energy of the two states under consideration. To take state is different compared to the normal continuation the influence of these correlation effects partially into of the Periodic Table [6], due to direct relativistic account, we have used the multiconfiguration Dirac- influences. One possible candidate for such a deviation Fock (MCDF) method [13], which we briefly summa- is element Lawrencium (Z = 103). Every Periodic rize in the first section. Table shows 5f 14 7s2 6d’ as the ground state confi- guration. It was Mann [7] who first pointed out that 1. Method of calculation. - It is well known that single configuration Dirac-Fock calculations give the multiconfiguration method [14] is an efficient one Sf 14 7s2 7p’ as the ground state. Independently Brewer to take into account most of the correlation effects [8] came to the same conclusion using a semi-empirical while a of confi- extrapolation. Subsequent detailed investigations retaining only reasonable number gurations. In its relativistic version it has the further came to different conclusions [9-12], because the advantage of working ab initio in the intermediate coupling scheme and thus to allow convergence to a (*) Permanent address : Physics Department, University of well specified state. Besides the introduction of many Kassel, D-3500 Kassel, West Germany. body effects this is an important improvement over Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:01980004109094300 944 calculations the relativistic single configuration which state (s2 p 1, 2 2p 1, 2 state) we have to deal with 35 confi- are restricted to single j configurations or to the gurations. This rather large number of configurations average energy, i.e. the centre of gravity of all the is due to the fact that in the relativistic case the only levels. Neither of these two restrictions is satisfactory good quantum number is the total angular momen- for high quality predictions. The method works as tum and not the orbital and spin total angular follows, the total wavefunction is expressed as : momenta separately. Being interested in the two S2 p 1/2 and s2 d3/2 configurations of Lr, the only two candidates for the ground state, we carried out the calculations by converging to the states for which these have where ai stands for all quantum numbers necessary configurations the largest weight. We to completely describe the i-th configuration of total found that, except for Sc, this state was the ground angular momentum J and projection M. Restricting state. For Sc it is known [17] that the lowest J = 1/2 is almost character the total Hamiltonian of the system to a sum of one- levels of pure dsp and that the lowest electron Dirac operators plus the classical Coulomb odd level has a total angular momentum J = 3/2. repulsion between the electrons, the variational prin- These two results are well reproduce by the MCDF ciple is used to determine both the radial functions method which gives for each of these levels a weight = - 99 for the with the J and the mixing coefficients ai we will use weights of % dsp configuration 3/2 = for their square a2 - of the various configurations. state 410 cm -1 below the J 1 /2 one (to be compared with value of 337 For After self-consistency, the total energy is corrected by the experimental cm -1 ). La, first order perturbation theory for magnetic interaction our result is in disagreement with the accepted ground and retardation in the Coulomb repulsion. Both of state configuration [18] of the J = 1/2 level. If single these contributions have been evaluated exactly for configuration calculations, in intermediate coupling, that the is lower than the each state considered, with the method we developed predict dsp configuration recently [15-16], and not within the average confi- s2 p one, multiconfiguration calculations give a ground guration approximation. state with a predominant s2 p character (66 %) and an contribution This Furthermore we include an estimation of QED important dsp (24 %). suggests studies of La are needed as we will corrections based on hydrogenic results for the self- that further but, see later in the this will not our energy and on the expectation value of the Uehling discussion, change Lr. potential for the vacuum polarization. Our method conclusion for of handling these corrections is described elsewhere Before discussing our results more in detail let us the [16]. In the present use of the MCDF method we first consider the mixing coefficients between include all the electronic configurations arising from various configurations included in the calculation. For the J = even state of all the atoms the distribution of 3 electrons in the ns, npi/2, np3/2, 3/2 considered, the S2 is far the most (n - 1) d3/2, (n - 1) d5/2 as well as the nearest f5/2 d3/2 configuration by important and f7/2 orbitals, where n is the principal quantum one and contributes between 0.9 to 0.95 to the coef- number of the outermost occupied orbital. This set ficients ai of equation (1), whereas all other confi- of configurations was being chosen to include the gurations contribute to 0.2 or less each (which means most important contributions to correlation effects a weight a2 less than 4 %). The J = 1/2 odd parity in the valence shells due to both intra-shell correlation state shows a much more complicated behaviour as results I. For La we (i.e. mixing between configuratidns with the same illustrated by the given in table found contributions 0.25 and 0.17 principal quantum number n) and inter-shell cor- very strong of 0.38, relation between the valence electrons and the nearest core electrons. We have to point out, nevertheless, Table I. - Coefficients ai (according to eq. 1) of the that we are restricted to either double excitations or main configurations contributing to the lowest J = 1/2’ the elements single excitations with a change in the orbital quantum state for Sc, Y, La, Lu, Ac and Lr.
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