Shell Excitation Research Articles

Quadrupole Coupling of Circular Rydberg Qubits to Inner Shell Excitations.

Divalent atoms provide excellent means for advancing control in Rydberg atom-based quantum simulation and computing due to the second optically active valence electron available. Particularly promising in this context are circular Rydberg atoms, for which long-lived ionic core excitations can be exploited without suffering from detrimental autoionization. Here, we report the implementation of electric quadrupole coupling between the metastable 4D_{3/2} level and a very high-n (n=79) circular Rydberg qubit, realized in doubly excited ^{88}Sr atoms prepared from an optical tweezer array. We measure the kHz-scale differential level shift on the circular Rydberg qubit via beat-node Ramsey interferometry comprising spin echo. Observing this coupling requires coherent interrogation of the Rydberg states for more than 100 μs, which is assisted by tweezer trapping and circular state lifetime enhancement in a black-body radiation suppressing capacitor. Further, we find no noticeable loss of qubit coherence under continuous photon scattering on the ion core, paving the way for laser cooling and imaging of Rydberg atoms. Our results demonstrate access to weak electron-electron interactions in Rydberg atoms and expand the quantum simulation toolbox for optical control of highly excited circular state qubits via ionic core manipulation.

Mass distributions in 12C + 232Th fission: role of shell effects and excitation energy

This article reports the measurement of cross sections of charge and mass identified fission products and the mass distributions in 232Th(12C,f) reaction at 62.5, 70.7 and 102.9 MeV beam energies to investigate the role of single particle effects. The study was carried out using the recoil catcher technique followed by off-line γ-ray spectrometry. Cross sections of 32, 54 and 64 fission products were measured for 62.5, 70.7 and 102.9 MeV beam energies, respectively. The mass distributions obtained at 62.5 and 70.7 MeV show a flat-top nature indicating significant asymmetric fission contribution (heavy mass peak corresponding to Z range of 54–56), whereas, a nearly Gaussian behaviour was observed at 102.9 MeV indicating dominant contribution from symmetric fission. The experimental mass distributions were in gross agreement with the “GEF, 2021/1.1” calculations which predicted significant asymmetric fission contribution dominated by Z ≈ 55 (‘Standard 2’ mode) at 62.5 and 70.7 MeV. The present study shows the significant role of charge polarization resulting in the deviation of the most probable charge (ZP) values from those obtained using UCD hypothesis. “GEF, 2023/2.1” calculations were unable to explain the observed mass distributions with significant asymmetric fission contribution due to comparatively lower contribution from higher chance fission resulting from the lower saddle point energies. An attempt has been made to estimate the mass distributions arising from the complete fusion fission and α-transfer induced fission. The trend shows an increase in the α-transfer induced fission contribution with increasing beam energy which is in qualitative agreement with the sum-rule model calculations.

Preparation and Characterization of Uniform and Controlled Silica Encapsulating on Lithium Yttrium Fluoride-Based Upconversion Nanoparticles.

In this work, we present an advancement in the encapsulation of lithium yttrium fluoride-based (YLiF4:Yb,Er) upconversion nanocrystals (UCNPs) with silica (SiO2) shells through a reverse microemulsion technique, achieving UCNPs@SiO2 core/shell structures. Key parameters of this approach were optimized to eliminate the occurrence of core-free silica particles and ensure a controlled silica shell thickness growth on the UCNPs. The optimal conditions for this method were using 6 mg of UCNPs, 1.5 mL of Igepal CO-520, 0.25 mL of ammonia, and 50 μL of tetraethyl orthosilicate (TEOS), resulting in a uniform silica shell around UCNPs with a thickness of 8 nm. The optical characteristics of the silica-encased UCNPs were examined, confirming the retention of their intrinsic upconversion luminescence (UC). Furthermore, we developed a reliable strategy to avoid the coencapsulation of multiple UCNPs within a single silica shell. This approach led to a tenfold increase in the UC luminescence of the annealed particles compared to their nonannealed counterparts, under identical silica shell thickness and excitation conditions. This significant improvement addresses a critical challenge and amplifies the applicability of the resulting UCNPs@SiO2 core/shell structures in various fields.

Contribution of molecular orbital promotion to the electronic stopping cross section at slow atom solid collisions

The autoionization states formation due to MO promotion during collisions of keV-energy ions with solids produces a dominant contribution to inelastic energy losses and, accordingly, to the electronic stopping powers dE/dx. The correlations of emitted electron numbers δ with the values of inelastic energy losses Q are shown. When corresponding distances of closest approach are reached, the MO orbital promotion produces a stepwise increase in values of Q and δ. Based on the measured ionization cross-sections and Q values, electronic stopping powers can be calculated. For the case when such measurements are not available, the scaling for the ionization cross section in the case of K, L and M shell excitation can be used.We have proposed a new model for calculating electronic stopping power in which the formation of autoionization states in atomic collisions makes a dominant contribution to the inelastic energy loss and ionization of colliding atoms. Using data on the values of energy losses and ionization cross sections, it is possible to calculate the values of electronic stopping. The model predicts the threshold character of the dE/dx dependence versus the collision velocity and an increase in inelastic energy losses at the collision energies at which the threshold for the corresponding MO promotion occurs.

Contribution of molecular orbital promotion to the electronic stopping cross section at slow atom solid collisions

The autoionization states formation due to MO promotion during collisions of keV-energy ions with solids produces a dominant contribution to inelastic energy losses and, accordingly, to the electronic stopping powers dE/dx. The correlations of emitted electron numbers δ with the values of inelastic energy losses Q are shown. When corresponding distances of closest approach are reached, the MO orbital promotion produces a stepwise increase in values of Q and δ. Based on the measured ionization cross-sections and Q values, electronic stopping powers can be calculated. For the case when such measurements are not available, the scaling for the ionization cross section in the case of K, L and M shell excitation can be used.We have proposed a new model for calculating electronic stopping power in which the formation of autoionization states in atomic collisions makes a dominant contribution to the inelastic energy loss and ionization of colliding atoms. Using data on the values of energy losses and ionization cross sections, it is possible to calculate the values of electronic stopping. The model predicts the threshold character of the dE/dx dependence versus the collision velocity and an increase in inelastic energy losses at the collision energies at which the threshold for the corresponding MO promotion occurs.

Atomic Electron Shell Excitations in Double-β Decay

The problem of the transition of electron shells of atoms to excited states in the process of neutrinoless double-βdecay is investigated. This subject is crucial for modeling the energy spectrum ofβ-electrons, which is sensitive to the mass and Majorana nature of neutrinos. The dependence of the obtained results on the atomic number indicates an important role of the Feinberg–Migdal effect in the electron shell excitations. We report the overlap amplitudes of the electron shells of the parent atom and the daughter ion for eleven atoms, the two-neutrino double-βdecay of which was observed experimentally. In around one-fourth of the cases where the structure of the electron shells is inherited from the parent atom, there is a transition to the ground state or the excited state with the lowest energy. The de-excitation of the daughter ion in the latter scenario is accompanied by the emission of photons in the ultraviolet range, which can serve as an auxiliary signature of double-βdecay. The average excitation energy of the electron shells ranges between 300 and 800 eV, with the variance ranging from (1.7 keV)2in calcium to (14 keV)2in uranium.

Atomic Electron Shell Excitations in Double-β Decay

The problem of the transition of electron shells of atoms to excited states in the process of neutrinoless double-beta decay is investigated. This subject is crucial for modeling the energy spectrum of beta -electrons, which is sensitive to the mass and Majorana nature of neutrinos. The dependence of the obtained results on the atomic number indicates an important role of the Feinberg–Migdal effect in the electron shell excitations. We report the overlap amplitudes of the electron shells of the parent atom and the daughter ion for eleven atoms, the two-neutrino double-beta decay of which was observed experimentally. In around one-fourth of the cases where the structure of the electron shells is inherited from the parent atom, there is a transition to the ground state or the excited state with the lowest energy. The de-excitation of the daughter ion in the latter scenario is accompanied by the emission of photons in the ultraviolet range, which can serve as an auxiliary signature of double-beta decay. The average excitation energy of the electron shells ranges between 300 and 800 eV, with the variance ranging from (1.7 keV)2 in calcium to (14 keV)2 in uranium.

Coexistence of single-particle and collective excitation in Ni61

The high spin states in 61 Ni have been studied using the fusion evaporation reaction, Ti( $^{14}$C,3n) $^{61}$Ni at an incident beam energy of 40 MeV. A Compton suppressed multi-HPGe detector setup, consisting of six Clover detectors and three single crystal HPGe detectors was used to detect the de-exciting $\gamma$ rays from the excited states. The level scheme has been extended up to an excitation energy of 12.8 MeV and a tentative J$_{\pi}$ = 35/2$^+$ . The low-lying negative parity levels are found to be generated by single particle excitation within the f p shell and also excitations to the g$_{9/2}$ orbitals as explained well with shell model calculations using the GXPF1Br+V M U (modified) interaction. Two rotational structure of regular E2 sequences with small to moderate axial deformation have been established at higher excitation energy. Most interestingly, two sequences of M1 transitions are reported for the first time and described as magnetic rotational bands. The shears mechanism for both the bands can be described satisfactorily by the geometrical model. The shell model calculation involving the cross shell excitation beyond the fp shell well reproduce the M1 and E2 sequences. The shell model predicted B(M1) values for the magnetic rotational band B1 show the decreasing trend with spin as expected with closing of the shears.

Anomalous power-dependent color tuning of Er upconverting luminescence via 1530 nm excitation

The upconversion color tuning of Lanthanide ions usually requires complex core–shell structures and excitation configurations. This work presents simple Er3+ doped Yttria phosphors capable of color change through the manipulation of 1530 nm excitation intensity. Compared to the reported results of Er3+ color change from green to red with the increase in excitation intensity, the formed color-tunable phosphors show an inverse change of red to green. The color tuning mechanisms are attributed to the competition between the upward absorption and the downward decay at the Er3+ intermediate state. Finally, the potential applications of the formed color-tunable phosphors are demonstrated. This work provides a simple solution for high-performance upconversion color tuning and thus shows wide application prospects.

Theoretical Study of Valence Shell Excitation by Electron Impact in CCl4

This paper reports a theoretical study of valence shell excitation in CCl4 by high-energy electron impact. Generalized oscillator strengths are calculated for the molecule at the equation-of-motion coupled-cluster singles and doubles level. To elucidate the influence of nuclear dynamics on electron excitation cross-sections, the effects of molecular vibration are included in the calculation. Based on a comparison with recent experimental data, several reassignments of spectral features are made, and it is found that excitations from the Cl 3p nonbonding orbitals to σ* antibonding orbitals, 7a1 and 8t2, play dominant roles below the excitation energy of ∼9 eV. Furthermore, the calculations reveal that distortion of the molecular structure due to the asymmetric stretching vibration significantly affects the valence excitations at small momentum transfers, where contributions from dipole transitions are dominant. It indicates that vibrational effects have a considerable influence on Cl formation in the photolysis of CCl4.

Excitation-energy dependence of the fission-fragment neutron-excess ratio

Within the improved scission-point fission model, it is shown that the average neutron number per proton is not the same in fission fragments and is not equal to that in a fissioning nucleus. For the induced fission of $^{238}\mathrm{U}$, $^{240}\mathrm{Pu}$, $^{244}\mathrm{Cm}$, and $^{250}\mathrm{Cf}$, the dependencies of the fission-fragment neutron-excess ratio on the shell structure and excitation energy of fragment are studied.

Electron and ion spectroscopy of azobenzene in the valence and core shells.

Azobenzene is a prototype and a building block of a class of molecules of extreme technological interest as molecular photo-switches. We present a joint experimental and theoretical study of its response to irradiation with light across the UV to x-ray spectrum. The study of valence and inner shell photo-ionization and excitation processes combined with measurement of valence photoelectron-photoion coincidence and mass spectra across the core thresholds provides a detailed insight into the site- and state-selected photo-induced processes. Photo-ionization and excitation measurements are interpreted via the multi-configurational restricted active space self-consistent field method corrected by second order perturbation theory. Using static modeling, we demonstrate that the carbon and nitrogen K edges of azobenzene are suitable candidates for exploring its photoinduced dynamics thanks to the transient signals appearing in background-free regions of the NEXAFS and XPS.

Oscillator strengths and cross sections of the valence shell excitations in nitrous oxide studied by high-energy electron scattering

Generalized oscillator strengths (GOSs) of the valence shell excitations to the A1Σ−+B1Δ, C1Π, D1Σ+ and 21Π states in nitrous oxide have been determined by employing an angle-resolved electron energy loss spectrometer operated at an incident energy of 1500 eV and an energy resolution of about 80 meV. Detailed comparisons with the previous data indicate that the higher-order Born terms play a significant role in the GOSs of C1Π and D1Σ+ states at either low impact energies or large momentum transfers, and the GOSs of A1Σ−+B1Δ and C1Π states measured with the gas cell may suffer from the pressure effect. The measured GOS data are fitted with the Lassettre formula to determine the corresponding optical oscillator strengths (OOSs) and calculate the integral cross sections (ICSs) based on the BE-scaling method. The oscillator strengths and cross sections in this work provide a cross check on the previous data and can serve as a benchmark for testing the developed theoretical models and computational codes.

Evolution of the ionic polarization in multiple sequential ionization: General equations and an illustrative example

Modern free-electron lasers generate a highly intense polarized radiation which initiates a sequence of ionization and decay events. Their probability depends on the polarization of each involved state as a function of time. Its complete account is limited by the fact that a state can be formed in various ways. Here we present an equivalent of rate equations for population that completely accounts for polarization of radiation formulated in terms of statistical tensors. To illustrate our approach we theoretically consider the sequential photoionization of krypton by an intense extreme ultraviolet femtosecond pulse for photon energies below the $3d$-shell excitation threshold. The calculations of the ion yields, photoelectron spectra, and ionic polarization for various photon fluences are presented and the role of the polarization is discussed.

Calculations of electron-impact excitation and dielectronic recombination rate coefficients of highly charged silicon ions

The rate coefficients for dielectronic recombination and electron-impact excitation processes with H-like to Be-like silicon ions (${\mathrm{Si}}^{13+}\text{\ensuremath{-}}{\mathrm{Si}}^{10+}$) are calculated using relativistic distorted-wave approach. The prominent $▵n=1$ and the weaker $▵n=2$ and 3 dielectronic recombination (DR) resonances with $K$-shell excitations are presented, and compared with the existing DR experimental rate coefficients of ${\mathrm{Si}}^{13+}, {\mathrm{Si}}^{12+}$, and ${\mathrm{Si}}^{11+}$ ions, it is found that the theoretical DR rate coefficients are in very good agreement with the experimental results. With the same approach, the direct and resonant electron-impact excitation (EIE) cross sections associated with $1s\ensuremath{-}{n}^{\ensuremath{'}}{l}^{\ensuremath{'}}$ core excitations are calculated for the ground states of ${\mathrm{Si}}^{13+}\text{\ensuremath{-}}{\mathrm{Si}}^{10+}$ ions and found in excellent agreement with the available experiment. Finally, we present the synthesized DR and EIE rate coefficients for the sum of all detected $(13+\ensuremath{\sim}10+)$ charge states of Si and these agree well with the experimental results.

Generalized Oscillator Strengths for the Valence Shell Excitations in Carbon Tetrachloride Studied by Fast Electron Impact.

A joint experimental and theoretical investigation of the valence shell excitations of carbon tetrachloride has been performed by fast electron scattering and time dependent density functional theory calculations. At a collision energy of 1.5 keV and an energy resolution of about 70 meV, the dipole-forbidden transition of a1σ* ← 2t1 has been clearly observed at large momentum transfers, and its excitation energy of 6.15 eV and line width of 0.72 eV have been determined. Two new features are also recognized at 9.97 and 10.26 eV. The generalized oscillator strengths of the excited states at 5-11.3 eV have been determined from the measured spectra. The calculated generalized oscillator strength of the a1σ* ← 2t1 transition with the vibronic effect shows better agreement with the experiment, and the vibronic effect also accounts for its nonzero intensity at zero squared momentum transfer. The optical oscillator strengths of the valence shell excitations have also been obtained by extrapolating the generalized oscillator strengths to the limit of zero squared momentum transfer. The integral cross sections have been systematically determined from the threshold to 5000 eV by means of the BE-scaling method. The present oscillator strengths and cross sections provide the fundamental data of carbon tetrachloride and have important applications in photochemical modeling for atmospheric physics.

Frontier orbital stability of nitroxyl organic radicals probed by means of inner shell resonantly enhanced valence band photoelectron spectroscopy.

We have investigated the frontier orbitals of persistent organic radicals known as nitroxyls by resonant photoelectron spectroscopy (ResPES) under inner shell excitation. By means of this site-specific technique, we were able to disentangle the different atomic contributions to the outer valence molecular orbitals and examine several core-hole relaxation pathways involving the singly occupied molecular orbital (SOMO) localized on the nitroxyl group. To interpret the ResPES intensity trends, especially the strong enhancement of the SOMO ionized state at the N K-edge, we computed the Dyson spin orbitals (DSOs) pertaining to the transitions between the core-excited initial states and several of the singly ionized valence final states. We found that the computed vertical valence ionization potentials and norms of the DSOs are reasonably reliable when based on the long-range corrected CAM-B3LYP density functional. Thanks to their unpaired electrons, nitroxyls have recently found application in technological fields implying a spin control, such as spintronics and quantum computing. The present findings on the electronic structure of nitroxyl persistent radicals furnish important hints for their implementation in technological devices and, more in general, for the synthesis of new and stable organic radicals with tailored properties.

Wind induced oscillation on a tall circular storage shell for various terrains

The wind is an important natural phenomenon, which adversely affects different structures, such as high-rise buildings, chimneys, tanks, silos, bridges etc. The effect of wind on tall circular storage shell structures becomes critical, especially when it is in empty condition. Wind induced radial, meridional and axial stresses can cause ovalling, buckling, rupture, overturning etc. on circular storage shells. Terrain, topography, surface roughness, wind velocity, etc. are some of the important factors which influences the wind pressure distribution on circular storage shells. Also, the wind-induced oscillation may lead to structural failure of such shells. Significantly, a small number of studies are there on the effect of these factors on the aerodynamic excitation of circular storage shells. These available scopes and the importance of the studies on circular shell under aerodynamic excitation draws the attention of the present authors to investigate in this field. In the present study the authors have conducted computational fluid dynamics analysis, fluid–structure interaction analysis and modal analysis on a tall circular storage shell with slenderness ratio 4.0 considering four different terrains as per IS 875, part 3, 2015. These terrains are open terrain (terrain 1), open terrain with well scattered low to mid-rise objects (terrain 2), terrain with numerous closely spaced low and mid-rise objects (terrain 3) and terrain with closely spaced tall objects (terrain 4). The atmospheric boundary for each terrain is simulated using power law. The effect of terrain variation is assessed through the variation in the mean, and fluctuating wind pressure coefficient distribution around the circumference of the tall shell. It is observed that the mean pressure coefficients decreases and the fluctuating pressure coefficients increases in the side region of the shell, with the change in terrain conditions from terrain 1 to terrain 4. The highest and lowest pressure fluctuations are observed in the side region and leeward region, respectively. The wind-induced oscillation of the tall shell in relation to the fluctuating pressure coefficients have been assessed and the deformation of the tall storage shell for six consecutive mode shapes have been highlighted for terrain 4, where the distribution of fluctuating pressure coefficients is highest in magnitude.

Core-shell excitation of isoxazole at the C, N, and O K-edges - an experimental NEXAFS and theoretical TD-DFT study.

The near-edge X-ray absorption fine structure (NEXAFS) spectra of the gas-phase isoxazole molecule have been measured by collecting total ion yields at the C, N, and O K-edges. The spectral structures have been interpreted using time-dependent density functional theory (TD-DFT) with the short-range corrected SRC2-BLYP exchange-correlation functional. Experimental and calculated energies of core excitations are generally in good agreement, and the nature of observed core-excitation transitions has been elucidated. The experimental C 1s, N 1s, and O 1s core electron binding energies (CEBEs) have additionally been estimated from another yield measurement where the neutral fragments in high-Rydberg (HR) states were ionized by the electric field. For comparison, theoretical CEBEs have been calculated at the ΔM06-2X//mixed basis set level. We have also calculated the vibrationally resolved spectra pertaining to the lowest C 1s and N 1s core-excited roots in the Franck-Condon-Herzberg-Teller (FCHT) approximation. These spectra correlate well with the observed spectral features and have proven useful in resolving certain ambiguities in the assignment of the low-lying C 1s NEXAFS bands.

Oscillator strength study of the excitations of valence-shell of C2H2 by high-resolution inelastic x-ray scattering

The oscillator strengths of the valence–shell excitations of C2H2 are extremely important for testing theoretical models and studying interstellar gases. In this study, the high-resolution inelastic x-ray scattering (IXS) method is adopted to determine the generalized oscillator strengths (GOSs) of the valence–shell excitations of C2H2 at a photon energy of 10 keV. The GOSs are extrapolated to their zero limit to obtain the corresponding optical oscillator strengths (OOSs). Through taking a completely different experimental method of the IXS, the present results offer the high energy limit for electron collision to satisfy the first Born approximation (FBA) and cross-check the previous experimental and theoretical results independently. The comparisons indicate that an electron collision energy of 1500 eV is not enough for C2H2 to satisfy the FBA for the large squared momentum transfer, and the line saturation effect limits the accuracy of the OOSs measured by the photoabsorption method.