David Leimbach, Julia Sundberg, Yangyang Guo, Rizwan Ahmed, Jochen Ballof, Lars Bengtsson, Ferran Boix Pamies, Anastasia Borschevsky, Katerina Chrysalidis, Ephr… 展开作者
David Leimbach, Julia Sundberg, Yangyang Guo, Rizwan Ahmed, Jochen Ballof, Lars Bengtsson, Ferran Boix Pamies, Anastasia Borschevsky, Katerina Chrysalidis, Ephraim Eliav, Dmitry Fedorov, Valentin Fedosseev, Oliver Forstner, Nicolas Galland, Ronald Fernando Garcia Ruiz, Camilo Granados, Reinhard Heinke, Karl Johnston, Agota Koszorus, Ulli Koester, Moa K. Kristiansson, Yuan Liu, Bruce Marsh, Pavel Molkanov, Lukas F. Pasteka, Joao Pedro Ramos, Eric Renault, Mikael Reponen, Annie Ringvall-Moberg, Ralf Erik Rossel, Dominik Studer, Adam Vernon, Jessica Warbinek, Jakob Welander, Klaus Wendt, Shane Wilkins, Dag Hanstorp, Sebastian Rothe
One of the most important properties influencing the chemical behavior of an element is the energy released with the addition of an extra electron to the neutral atom, referred to as the electron affinity (EA). Among the remaining elements with unknown EA is astatine, the purely radioactive element 85. Astatine is the heaviest naturally occurring halogen and its isotope $^{211}$At is remarkably well suited for targeted radionuclide therapy of cancer. With the At$^-$ anion being involved in many aspects of current astatine labelling protocols, the knowledge of the electron affinity of this element is of prime importance. In addition, the EA can be used to deduce other concepts such as the electronegativity, thereby further improving the understanding of astatine's chemistry. Here, we report the first measurement of the EA for astatine to be 2.41578(7)eV. This result is compared to state-of-the-art relativistic quantum mechanical calculations, which require incorporation of the electron-electron correlation effects on the highest possible level. The developed technique of laser-photodetachment spectroscopy of radioisotopes opens the path for future EA measurements of other radioelements such as polonium, and eventually super-heavy elements, which are produced at a one-atom-at-a-time rate.
The electron affinity of tellurium has been determined to 1.970 876(7) eV. The threshold for photodetachment of Te^-(^{2} P_{3/2}) forming neutral Te in the ground state was investigated by measuring the total photodetachment cross section using a collinear laser-ion beam geometry. The electron affinity was obtained from a fit to the Wigner law in the threshold region.
Today, the electron affinity is experimentally well known for most of the elements and is a useful guideline for developing ab initio computational methods. However, the measurements of isotope shifts on the electron affinity are limited by both resolution and sensitivity. In this context, theory eventually contributes to the knowledge and understanding of atomic structures, even though correlation plays a dominant role in negative ions properties and, particularly, in the calculation of the specific mass shift contribution. The present study solves the longstanding discrepancy between calcula…
We have investigated the threshold of photodetachment of Li^- leading to the formation of the residual Li atom in the $2p ^2P$ state. The excited residual atom was selectively photoionized via an intermediate Rydberg state and the resulting Li^+ ion was detected. A collinear laser-ion beam geometry enabled both high resolution and sensitivity to be attained. We have demonstrated the potential of this state selective photodetachment spectroscopic method by improving the accuracy of Li electron affinity measurements an order of magnitude. From a fit to the Wigner law in the threshold region, we …
The specific mass shift in the electron affinity between ^{35}Cl and ^{37}Cl has been determined by tunable laser photodetachment spectroscopy to be -0.51(14) GHz. The isotope shift was observed as a difference in the onset of the photodetachment process for the two isotopes. In addition, the electron affinity of Cl was found to be 29138.59(22) cm^{-1}, giving a factor of 2 improvement in the accuracy over earlier measurements. Many-body calculations including lowest-order correlation effects demonstrates the sensitivity of the specific mass shift and show that the inclusion of higher-order co…
The electron affinities eA(S) are measured for the two isotopes 32S and 34S (16752.9753(41) and 16752.9776(85) cm-1, respectively). The isotope shift in the electron affinity is found to be positive, eA(34S)-eA(32S) = +0.0023(70) cm-1, but the uncertainty allows for the possibility that it may be either "normal" (eA(34S) > eA(32S)) or "anomalous" (eA(34S) < eA(32S)). The isotope shift is estimated theoretically using elaborate correlation models, monitoring the electron affinity and the mass polarization term expectation value. The theoretical analysis predicts a very large specific mass shift…
Core-polarization interactions are investigated in low-energy electron elastic scattering from the atoms In,Sn,Eu,Au and At through the calculation of their electron affinities. The complex angular momentum method wherein is embedded the vital electron-electron correlations is used. The core-polarization effects are studied through the well investigated rational function approximation of the Thomas-Fermi potential,which can be analytically continued into the complex plane. The EAs are extracted from the large resonance peaks in the calculated low-energy electron atom scattering total cross sec…
Theoretical calculations based on the Dirac--Coulomb--Breit relativistic coupled cluster method have been carried out for the electron affinities and ionization potentials of the superheavy element nihonium (Nh) and its lighter homologues In and Tl. The In and Tl calculations are in agreement with measurement within uncertainties. For Nh, where experiment is yet unknown, we predict the ionization potential of 7.569(48) eV and electron affinity of 0.776(30) eV.
The electron affinity (EA) of superheavy element Og is calculated by the use of the relativistic Fock-space coupled cluster (FSCC) and configuration interaction methods. The FSCC cluster operator expansion included single, double, and triple excitations treated in a non-perturbative manner. The Gaunt and retardation electron-electron interactions are taken into account. Both methods yield the results that are in agreement with each other. The quantum electrodynamics correction to EA is evaluated using the model Lamb-shift operator approach. The electron affinity of Og is obtained to be 0.076(4…
We investigate the (0001) surface of single crystal quartz with a submonolayer of Rb adsorbates. Using Rydberg atom electromagnetically induced transparency, we investigate the electric fields resulting from Rb adsorbed on the quartz surface, and measure the activation energy of the Rb adsorbates. We show that the adsorbed Rb induces a negative electron affinity (NEA) on the quartz surface. The NEA surface allows low energy electrons to bind to the surface and cancel the electric field from the Rb adsorbates. Our results are important for integrating Rydberg atoms into hybrid quantum systems a…
The multiconfiguration Dirac-Hartree-Fock method is applied to study the electron affinities of At and its homologous elements Cl, Br, and I. Our method of calculation is validated through the comparison with the available experimental electron affinities of Cl, Br, I, and other theoretical values. The agreement between our predicted electron affinities and the available experimental values for Cl, Br, and I is within 0.2%, which is an improvement of more than a factor of 10 over previous theoretical studies. Applying the same method to At, the electron affinity of At is predicted to be 2.3729…
The complex angular momentum (CAM) calculated low-energy 0 < E < 5 eV electron elastic total cross section (TCS) for In is benchmarked through its recently measured electron affinity (Walter et al, Phys. Rev. A 82, 032507 (2010)). The TCSs for Tl and Ga atoms are then calculated using the CAM method. From the dramatically sharp resonances in the TCSs binding energies for Tl^{-} and Ga^{-} negative ions formed during the collisions are extracted and compared with existing values. Three stable bound negative ions of Tl are predicted.
We present the results of experimental studies of photon-negative ion interactions involving the dynamics of two electrons. Resonances associated with doubly excited states of Li^- and He^- have been observed using laser photodetachment spectroscopy. Total and partial photodetachment cross sections have been investigated. In the former case, the residual atoms are detected irrespective of their excitation state, while in the latter case only those atoms in specific states are detected. This was achieved by the use of a state selective detection scheme based on the resonant ionization of the re…
Using recently developed version of the configuration interaction method for atoms with open shells we calculate electron structure and spectroscopic properties of the mendelevium atom (Md, $Z=101$). These include energy levels, first and second ionisation potentials, electron affinity, hyperfine structure and electric dipole transition amplitudes between ground and low lying states of opposite parity. The accuracy of the calculations is controlled by performing similar calculations for lighter analog of mendelevium, thulium atom and comparing the results with experiment and other calculations…
The Regge-pole calculated low-energy electron elastic total cross sections (TCSs) for Cm and No, characterized generally by negative-ion formation, shape resonances and Ramsauer-Townsend(R-T) minima, exhibit atomic and fullerene molecular behavior near threshold. Also, a polarization-induced metastable cross section with a deep R-T minimum near threshold is identified in the Cm TCSs, which flips over to a shape resonance appearing very close to threshold in the TCSs for No. We attribute these novel manifestations to size effects and orbital collapse impacting significantly the polarization int…
We study atoms with N electrons, and nuclear charge Z. It is well known that the cationic regime, Z > N is qualitatively described by Thomas-Fermi theory. The anionic regime, Z < N, on the other hand, is characterized by an instability threshold at Z_c <~ N-1, below which the atom spontaneously emits an electron. We compute the slope of the energy curve at Z=N-1 by means of a simple model that depends on the electron affinity and the covalent radius of the neutral atom with N-1 electrons. This slope is used in order to estimate Z_c, which is compared with previous numerical results. Extrapolat…
Investigations of low-energy electron-scattering of the lanthanide atoms Eu, Nd, Tb, Tm demonstrate that electron-correlation effects and core polarization are the dominant fundamental many-body effects responsible for the formation of metastable states of negative ions. Ramsauer Townsend minima, shape resonances and binding energies of the resultant anions are identified and extracted from the elastic total cross sections calculated using the complex angular momentum method. The large discrepancy between the recently measured electron affinity of 0.116 and the previously measured value of 1.0…
A new relativistic method for calculation of positron binding to atoms is presented. The method combines a configuration interaction treatment of the valence electron and the positron with a many-body perturbation theory description of their interaction with the atomic core. We apply this method to positron binding by the copper atom and obtain the binding energy of 170 meV (+ - 10%). To check the accuracy of the method we use a similar approach to calculate the negative copper ion. The calculated electron affinity is 1.218 eV, in good agreement with the experimental value of 1.236 eV. The pro…
We study $N$-electron atoms with nuclear charge $Z$. It is well known that, in the cationic ($Z > N$) high-$Z$ region, the atom behaves as a weakly interacting system. The anionic ($Z < N$) regime, on the other hand, is characterized by an instability threshold at $Z_c \lesssim N-1$, below which the atom spontaneously emits an electron. We construct a regularized perturbative series (RPS) for the ionization potential of ions in an isoelectronic sequence that exactly reproduces both, the large $Z$ and the $Z$ near $Z_c$ limits. The large-$Z$ expansion coefficients are analytically computed from…
Here we investigate ground and metastable negative ion formation in low-energy electron collisions with the actinide atoms Th, Pa, U, Np and Pu through the elastic total cross sections (TCSs) calculations. For these atoms, the presence of two or more open d- and f- subshell electrons presents a formidable computational task for conventional theoretical methods, making it difficult to interpret the calculated results. Our robust Regge pole methodology which embeds the crucial electron correlations and the vital core-polarization interaction is used for the calculations. These are the major phys…
