Direct and secondary nuclear excitation with x-ray free-electron lasers

The direct and secondary nuclear excitation produced by an x-ray free electron laser when interacting with a solid-state nuclear target is investigated theoretically. When driven at the resonance energy, the x-ray free electron laser can produce direct photoexcitation. However, the dominant process in that interaction is the photoelectric effect producing a cold and very dense plasma in which also secondary processes such as nuclear excitation by electron capture may occur. We develop a realistic theoretical model to quantify the temporal dynamics of the plasma and the magnitude of the secondary excitation therein. Numerical results show that depending on the nuclear transition energy and the temperature and charge states reached in the plasma, secondary nuclear excitation by electron capture may dominate the direct photoexcitation by several orders of magnitude, as it is the case for the 4.8 keV transition from the isomeric state of $^{93}$Mo, or it can be negligible, as it is the case for the 14.4 keV M\"ossbauer transition in $^{57}\mathrm{Fe}$. These findings are most relevant for future nuclear quantum optics experiments at x-ray free electron laser facilities.Comment: 17 pages, 7 figures; minor corrections made; accepted by Physics of Plasma

Diffractive imaging of dissociation and ground state dynamics in a complex molecule

We have investigated the structural dynamics in photoexcited 1,2-diiodotetrafluoroethane molecules (C2F4I2) in the gas phase experimentally using ultrafast electron diffraction and theoretically using FOMO-CASCI excited state dynamics simulations. The molecules are excited by an ultra-violet femtosecond laser pulse to a state characterized by a transition from the iodine 5p orbital to a mixed 5p|| hole and CF2 antibonding orbital, which results in the cleavage of one of the carbon-iodine bonds. We have observed, with sub-Angstrom resolution, the motion of the nuclear wavepacket of the dissociating iodine atom followed by coherent vibrations in the electronic ground state of the C2F4I radical. The radical reaches a stable classical (non-bridged) structure in less than 200 fs.Comment: 13 pages, 11 figure

Nuclear Anapole Moments

Nuclear anapole moments are parity-odd, time-reversal-even E1 moments of the electromagnetic current operator. Although the existence of this moment was recognized theoretically soon after the discovery of parity nonconservation (PNC), its experimental isolation was achieved only recently, when a new level of precision was reached in a measurement of the hyperfine dependence of atomic PNC in 133Cs. An important anapole moment bound in 205Tl also exists. In this paper, we present the details of the first calculation of these anapole moments in the framework commonly used in other studies of hadronic PNC, a meson exchange potential that includes long-range pion exchange and enough degrees of freedom to describe the five independent $S-P$ amplitudes induced by short-range interactions. The resulting contributions of pi-, rho-, and omega-exchange to the single-nucleon anapole moment, to parity admixtures in the nuclear ground state, and to PNC exchange currents are evaluated, using configuration-mixed shell-model wave functions. The experimental anapole moment constraints on the PNC meson-nucleon coupling constants are derived and compared with those from other tests of the hadronic weak interaction. While the bounds obtained from the anapole moment results are consistent with the broad ``reasonable ranges'' defined by theory, they are not in good agreement with the constraints from the other experiments. We explore possible explanations for the discrepancy and comment on the potential importance of new experiments.Comment: 53 pages; 10 figures; revtex; submitted to Phys Rev

Beyond Vibrationally Mediated Electron Transfer: Coherent Phenomena Induced by Ultrafast Charge Separation

Wave packet propagation succeeding electron transfer (ET) from alizarin dye molecules into the nanocrystalline TiO2 semiconductor has been studied by ultrafast transient absorption spectroscopy. Due to the ultrafast time scale of the ET reaction of about 6 fs the system shows substantial differences to molecular ET systems. We show that the ET process is not mediated by molecular vibrations and therefore classical ET theories lose their applicability. Here the ET reaction itself prepares a vibrational wave packet and not the electromagnetic excitation by the laser pulse. Furthermore, the generation of phonons during polaron formation in the TiO2 lattice is observed in real time for this system. The presented investigations enable an unambiguous assignment of the involved photoinduced mechanisms and can contribute to a corresponding extension of molecular ET theories to ultrafast ET systems like alizarin/TiO2.Comment: This work was supported by the German Research Foundation (DFG) (Hu 1006/6-1, WA 1850/6-1) and European Union projects FDML-Raman (FP7 ERC StG, contract no. 259158) and ENCOMOLE-2i (Horizon 2020, ERC CoG no. 646669

Computation of atomic astrophysical opacities

The revision of the standard Los Alamos opacities in the 1980-1990s by a group from the Lawrence Livermore National Laboratory (OPAL) and the Opacity Project (OP) consortium was an early example of collaborative big-data science, leading to reliable data deliverables (atomic databases, monochromatic opacities, mean opacities, and radiative accelerations) widely used since then to solve a variety of important astrophysical problems. Nowadays the precision of the OPAL and OP opacities, and even of new tables (OPLIB) by Los Alamos, is a recurrent topic in a hot debate involving stringent comparisons between theory, laboratory experiments, and solar and stellar observations in sophisticated research fields: the standard solar model (SSM), helio and asteroseismology, non-LTE 3D hydrodynamic photospheric modeling, nuclear reaction rates, solar neutrino observations, computational atomic physics, and plasma experiments. In this context, an unexpected downward revision of the solar photospheric metal abundances in 2005 spoiled a very precise agreement between the helioseismic indicators (the radius of the convection zone boundary, the sound-speed profile, and helium surface abundance) and SSM benchmarks, which could be somehow reestablished with a substantial opacity increase. Recent laboratory measurements of the iron opacity in physical conditions similar to the boundary of the solar convection zone have indeed predicted significant increases (30-400%), although new systematic improvements and comparisons of the computed tables have not yet been able to reproduce them. We give an overview of this controversy, and within the OP approach, discuss some of the theoretical shortcomings that could be impairing a more complete and accurate opacity accountingComment: 31 pages, 10 figures. This review is originally based on a talk given at the 12th International Colloquium on Atomic Spectra and Oscillator Strengths for Astrophysical and Laboratory Plasmas, Sao Paulo, Brazil, July 2016. It has been published in the Atoms online journa