Single-hole States Research Articles

Detailed structure of Sn131 populated in the β decay of isomerically purified In131 states

The excited structure of the single-hole nucleus Sn131 populated by the β− decay of In131 was investigated in detail at the ISOLDE facility at CERN. This new experiment took advantage of isomeric purification capabilities provided by resonant ionization, making it possible to independently study the decay of each isomer for the first time. The position of the first-excited νh11/2 neutron-hole state was confirmed via an independent mass spectroscopy experiment performed at the Ion Guide Isotope Separator On-Line facility at the University of Jyväskylä. The level scheme of Sn131 was notably expanded with the addition of 31 new γ-ray transitions and 22 new excited levels. The γ-emitting excited levels above the neutron separation energy in Sn131 were investigated, revealing a large number of states, which in some cases decay by transitions to other neutron-unbound states. Our analysis showed the dependence between the population of these states in Sn131 and the β-decaying In131 state feeding them. Profiting from the isomer selectivity, it was possible to estimate the direct β feeding to the 3/2+ ground and 11/2− isomeric states, disentangling the contributions from the three indium parent states. This made possible to resolve the discrepancies in logft for first-forbidden transitions observed in previous studies, and to determine the β-delayed neutron decay probability (Pn) values of each indium isomers independently. The first measurement of subnanosecond lifetimes in Sn131 was performed in this work. A short T1/2=18(4)−ps value was measured for the 1/2+ neutron single-hole 332-keV state, which indicates an enhanced l-forbidden M1 behavior for the ν3s1/2−1→ν3d3/2−1 transition. The measured half-lives of high-energy states populated in the β decay of the (21/2+) second isomeric state (In131m2) provided valuable information on transition rates, supporting the interpretation of these levels as core-excited states analogous to those observed in the doubly-magic Sn132. Published by the American Physical Society 2024

Resonant Auger decay of iodobenzene below the I 4d edge.

New data are presented on the resonant Auger decay of iodobenzene (C6H5I) in the region of the I 4d-1 ionization threshold. The excited molecules decay by participator and spectator processes to populate single-hole valence states and two-hole, one-particle excited states of the cation, providing new information on the structure of C6H5I+. Excitation of dissociative C6H5I (I 4d5/2,3/2-1)σ* resonances can, in principle, result in ultrafast dissociation to C6H5 + I** and the subsequent autoionization of I**, but no evidence for this process is observed. The results are compared with our recent study of the resonant Auger decay of methyl iodide (CH3I).

Unraveling the variational breakdown of core valence separation calculations: Diagnostic and cure to the over relaxation error of double core hole states.

The core valence separation (CVS) approximation is the most employed strategy to prevent the variational collapse of standard wave function optimization when attempting to compute electronic states bearing one or more electronic vacancies in core orbitals. Here, we explore the spurious consequences of this approximation on the properties of the computed core hole states. We especially focus on the less studied case of double core hole (DCH) states, whose spectroscopic interest has recently been rapidly growing. We show that the CVS error leads to a systematic underestimation of DCH energies, a property in stark contrast with the case of single core hole states. We highlight that the CVS error can then be interpreted as an over relaxation effect and design a new correction strategy adapted to these specificities.

Electron scattering with ethane adsorbed on rare gas multilayers: Hole transfer, coulomb decay, and ion dissociation.

Positive ion desorption following electron impact dissociative ionization of ethane adsorbed on Ar, Kr, and Xe multilayers has been studied as a function of incident electron energy from threshold to 100eV. Based on the dependence of ion yields on the identity of the rare gas, it is likely that the majority of ethane molecules undergo indirect ionization following hole transfer from the ionized underlying rare gas. This has also been corroborated by density of states calculations showing the energetic alignment of the outer valence states of ethane and the condensed rare gas ionization energies. Due to the near-resonant nature of charge transfer for single-hole states, the ethane molecular ion is excited to different final ionic states on different rare gases, which leads to differences in ion desorption yields and branching ratios. The quantitative yields increase with increasing ionization energy gap between the rare gas and ethane, in the order Ar > Kr > Xe. The large increase in yields from 25eV onwards for all rare gases is likely due to the formation and decay of two-hole states on neighboring rare gas and ethane molecules due to interatomic and intermolecular Coulomb decay (ICD) and not electron transfer mediated decay (ETMD). The ICD and ETMD pathways become accessible when the incoming electron has sufficient energy to excite the inner valence ns level of the rare gas to a Rydberg state or ionize it. The experimental findings are supported by calculations of thresholds, density of states for the final configurations of these processes, and coupling strengths for hole transfer between ethane and rare gases. The fragment ion branching ratios vary with energy from threshold to about 35eV, showing the fragmentation pattern changes with the mode of hole transfer and availability of excess energy. Sigma C-C bonds are more likely to break than C-H bonds in the mid-20eV range, and this effect is most pronounced for Xe, followed by Kr, and then Ar.

Contributions of exciton fine structure and hole trapping on the hole state filling effect in the transient absorption spectra of CdSe quantum dots.

The optoelectronic properties of quantum confined semiconductor nanocrystals depend critically on the band edge electron and hole levels and their exciton fine structures. Transient absorption (TA) spectroscopy has been widely used to probe the dynamics of photogenerated electrons, holes, and excitons in these materials through their state filling induced bleach of the band edge exciton transition. Such effects, in principle, reflect the band edge fine structures and are well understood for the conduction band electrons. However, the valence band hole state filling signals remain poorly understood due to the complexity of the valence band level structure and the presence of fast hole trapping in many materials. Herein, we report a study of the valence band hole state filling effect by comparing the TA spectra of CdSe quantum dots (QDs) with different degrees of hole trapping and by selective removal of the conduction band electrons to adsorbed methyl viologen molecules. We observe that in CdSe/CdS core/shell QDs with a high photoluminescence quantum yield of 81%, the valence band hole contributes to 22% ± 1% of the exciton bleach, while a negligible hole state filling signal is observed in CdSe core only QDs with a photoluminescence quantum yield of 17%. This hole state filling effect can be explained by a simplified valence band edge hole model that contains two sets of twofold degenerate hole levels that are responsible for the higher energy bright exciton and lower energy dark exciton states, respectively. Our result clarifies the TA spectral features of the valence band holes and provides insights into the nature of single hole states in CdSe-based QDs.

Effective shell-model interaction for nuclei “southeast” of Sn100

We construct an effective shell-model interaction for the valence space spanned by single-particle neutron and single-hole proton states in $^{100}$Sn. Starting from chiral nucleon-nucleon and three-nucleon forces and single-reference coupled-cluster theory for $^{100}$Sn we apply a second similarity transformation that decouples the valence space. The particle-particle components of the resulting effective interaction can be used in shell model calculations for neutron deficient tin isotopes. The hole-hole interaction can be used to calculate the $N = 50$ isotones south of $^{100}$Sn, and the full particle-hole interaction describes nuclei in the region southeast of $^{100}$Sn. We compute low-lying excited states in selected nuclei southeast of $^{100}$Sn, and find reasonable agreement with data. The presented techniques can also be applied to construct effective shell-model interactions for other regions of the nuclear chart.

Cluster structure of 21Ne and 21Na

We study the cluster structure of 21Ne and 21Na within the framework of the cluster shell model (CSM) and show that they have a complex cluster structure with the coexistence of a 20Ne+n, 20Ne+p structure and a 19Ne+2n, 19F+2p structure. Seven rotational bands are identified in 21Ne and four in 21Na and assigned to single-particle cluster states, single-hole cluster states and vibrational states. The single-particle states are associated with the 20Ne+n and 20Ne+p cluster structure, while the single-hole states are associated with the 19Ne+2n and 19F+2p structure.

How Exciton and Single Carriers Block the Excitonic Transition in Two-Dimensional Cadmium Chalcogenide Nanoplatelets.

Cadmium chalcogenide nanoplatelets (NPLs) possess unique properties and have shown great potential in lasing, light-emitting diodes, and photocatalytic applications. However, the exact natures of the band-edge exciton and single carrier (electron and hole) states remain unclear, even though they affect the key properties and applications of these materials. Herein, we study the contribution of a single carrier (electron or hole) state to phase space filling of single exciton states of cadmium chalcogenide NPLs. With pump fluence dependent TA study and selective electron removal, we determine that a single electron and hole states contribute 85% and 12%, respectively, to the blocking of the excitonic transition in CdSe/ZnS core/shell NPLs. These observations can be rationalized by a model of band-edge exciton and single carrier states of 2D NPLs that differs significantly from that of quantum dots.

Quantum entanglement in the t−J chain: From charge-spin separation to recombination

In contrast to the conventional von Neumann bipartite entanglement entropy (bEE), we show that a more appropriate description of the one-dimensional doped Mott insulator is a new kind of mutual entanglement entropy (mEE) between the charge and spin degrees of freedom. Such a charge-spin mEE can clearly distinguish the important and distinct features between the $t$-$J$ model and the so-called $\sigma\cdot{t}$-$J$ model. In the latter, the phase string sign structure is switched off such that a single doped hole always behaves like a Bloch wave in the whole regime of $J/t$, whereas in the former it exhibits a series of level crossing with the total momentum jumps in the single-hole ground state from spin-charge separation at $J/t\rightarrow{0}$ to spin-charge recombination at large $J/t$, which are failed to be detected by bEE. We further show that the distinctions between the two models persist to finite energy density, which can be similarly well characterized by mEE but not by bEE. By studying the dynamic time evolution of the states set out of equilibrium at the beginning, we show that mEE indeed always increases with the time, satisfying the common characteristic of entropy.

Fragmentation of Single-Particle Strength around the Doubly Magic Nucleus ^{132}Sn and the Position of the 0f_{5/2} Proton-Hole State in ^{131}In.

Spectroscopic factors of neutron-hole and proton-hole states in ^{131}Sn and ^{131}In, respectively, were measured using one-nucleon removal reactions from doubly magic ^{132}Sn at relativistic energies. For ^{131}In, a 2910(50)-keV γ ray was observed for the first time and tentatively assigned to a decay from a 5/2^{-} state at 3275(50)keV to the known 1/2^{-} level at 365keV. The spectroscopic factors determined for this new excited state and three other single-hole states provide first evidence for a strong fragmentation of single-hole strength in ^{131}Sn and ^{131}In. The experimental results are compared to theoretical calculations based on the relativistic particle-vibration coupling model and to experimental information for single-hole states in the stable doubly magic nucleus ^{208}Pb.

Doublon-holon excitations split by Hund's rule coupling within the orbital-selective Mott phase

Multiorbital interactions have the capacity to produce an interesting kind of doublon-holon bound state that consists of a single-hole state in one band and a doubly-occupied state in another band. Interband doublon-holon pair excitations in the two-orbital Hubbard model are studied by using dynamical mean-field theory with the Lanczos method as the impurity solver. We find that the interband bound states may provide several in-gap quasiparticle peaks in the density of states of the narrow band in the orbital-selective Mott phase with a small Hund's rule coupling ($J$). There exists a corresponding energy relation between the in-gap states of the narrow band and the peaks in the excitation spectrum of the doublon for the wide band. We also find that the spin flip and pair-hopping Hund interactions can divide one quasiparticle peak into two peaks, where the splitting energy increases linearly with increasing $J$. Strong Hund's rule coupling can move the interband doublon-holon pair excitations outside the Mott gap and restrict the bound states by suppressing the orbital selectivity of the doubly-occupied and single-hole states.

An experimental and theoretical study of the C 1s ionization satellites in CH3I.

The C 1s ionization spectrum of CH3I has been studied both experimentally and theoretically. Synchrotron radiation has been employed to record polarization dependent photoelectron spectra at a photon energy of 614 eV. These spectra encompass the main-line due to the C 1s single-hole state and the peaks associated with the shake-up satellites. Vertical ionization energies and relative photoelectron intensities have been computed using the fourth-order algebraic-diagrammatic construction approximation scheme for the one-particle Green's function and the 6-311++G** basis set. The theoretical spectrum derived from these calculations agrees qualitatively with the experimental results, thereby allowing the principal spectral features to be assigned. According to our calculations, two 2A1 shake-up states of the C 1s-1 σCI → σCI * type with singlet and triplet intermediate coupling of the electron spins (S' = 0, 1) play an important role in the spectrum and contribute significantly to the overall intensity. Both of these states are expected to have dissociative diabatic potential energy surfaces with respect to the C-I separation. Whereas the upper of these states perturbs the manifold of Rydberg states, the lower state forms a band which is characterized by a strongly increased width. Our results indicate that the lowest shake-up peak with significant spectral intensity is due to the pair (S' = 0, 1) of 2E (C 1s-1 I 5p → σCI *) states. We predict that these 2E states acquire photoelectron intensity due to spin-orbit interaction. Such interactions play an important role here due to the involvement of the I 5p orbitals.

Neutron-hole states in 131Sn and spin-orbit splitting in neutron-rich nuclei

In atomic nuclei, the spin-orbit interaction originates from the coupling of the orbital motion of a nucleon with its intrinsic spin. Recent experimental and theoretical works have suggested a weakening of the spin-orbit interaction in neutron-rich nuclei far from stability. To study this phenomenon, we have investigated the spin-orbit energy splittings of single-hole and single-particle valence neutron orbits of 132Sn. The spectroscopic strength of single-hole states in 131Sn was determined from the measured differential cross sections of the tritons from the neutron-removing 132Sn(d, t)131Sn reaction, which was studied in inverse kinematics at the Holifield Radioactive Ion Beam Facility at Oak Ridge National Laboratory. The spectroscopic factors of the lowest 3/2+, 1/2+ and 5/2+ states were found to be consistent with their maximal values of (2j+1), confirming the robust N=82 shell closure at 132Sn. We compared the spin-orbit splitting of neutron single-hole states in 131Sn to those of single-particle states in 133Sn determined in a recent measurement of the 132Sn(d, p)133Sn reaction. We found a significant reduction of the energy splitting of the weakly bound 3p orbits compared to the well-bound 2d orbits, and that all the observed energy splittings can be reproduced remarkably well by calculations using a one-body spin-orbit interaction and a Woods–Saxon potential of standard radius and diffuseness. The observed reduction of spin-orbit splitting can be explained by the extended radial wavefunctions of the weakly bound orbits, without invoking a weakening of the spin-orbit strength.

Auger decay and natural lifetime widths of single and double K-shell vacancy states of Al4+–Al11+ ions

The Auger decay of single and double K-shell hole and hollow states of Al4+–Al11+ was theoretically investigated in the framework of perturbation theory implemented by the distorted wave approximation. The natural lifetime widths of the hollow states x + are found to be 1.3–1.9 times larger than those of corresponding hole states x + . The maximal ratio is found originating from the hollow states of , which is ∼2.9 times as large as the hole states of . The calculated energy levels and natural lifetime widths are compared with the experimental and other theoretical results wherever available in the literature. The Auger decay rates and natural lifetime widths presented in this work are useful in the modeling of ultra-intensive x-ray laser interaction with aluminum.

Intrinsic translational symmetry breaking in a doped Mott insulator

Whether a doped hole propagates as a Bloch wave or not is an important issue of doped Mott physics. Here we examine this problem based on the quasiparticle spectral weight $Z$ distribution, calculated by density matrix renormalization group (DMRG). By tuning the anisotropy of a two-leg $t$-$J$ ladder without closing the background spin gap, the $Z$ distribution unambiguously reveals a transition of the single hole state from a Bloch wave to a novel one with spontaneous translational symmetry breaking. We further establish a direct connection of such a transition with a nonlocal phase string entanglement between the hole and quantum spins, which explains numerical observations.

Ionization potential depression in an atomic-solid-plasma picture

Exotic solid density matter such as heated hollow crystals allow extended material studies while their physical properties and models such as the famous ionization potential depression are presently under renewed controversial discussion. Here we develop an atomic-solid-plasma (ASP) model that permits ionization potential depression studies also for single and multiple core hole states. Numerical calculations show very good agreement with recently available data not only in absolute values but also for Z-scaled properties while currently employed methods fail. For much above solid density compression, the ASP model predicts increased K-edge energies that are related to a Fermi surface rising. This is in good agreement with recent quantum molecular dynamics simulations. For hot dense matter a quantum number dependent optical electron finite temperature ion sphere model is developed that fits well with line shift and line disappearance data from dense laser produced plasma experiments. Finally, the physical transparency of the ASP picture allows a critical discussion of current methods.

Large-scale shell-model study for excitations across the neutron N=82 shell gap in Sb131–133

The cross-shell excitations in the mass-130 region are determined by the behavior of the single-particle (or single-hole) states around the doubly magic nucleus $^{132}\mathrm{Sn}$ and the size of the energy gaps at $N=82$ and/or $Z=50$. The present work reports on the results from large-scale shell-model calculations with the extended paring plus quadrupole-quadrupole force, usually with additions of monopole corrections (the EPQQM model). This paper applies the EPQQM model to the northwestern quadrant of $^{132}\mathrm{Sn}$. The model space includes the orbits of $(0{g}_{7/2},1{d}_{5/2},1{d}_{3/2},2{s}_{1/2},0{h}_{11/2})$ for both protons and neutrons, with two additional neutron orbits $(1{f}_{7/2},2{p}_{3/2})$ above the $N=82$ shell gap, allowing cross-shell excitations. It is found that the experimentally known low-lying levels for $^{133}\mathrm{Sb}, ^{132}\mathrm{Sb}$, and $^{131}\mathrm{Sb}$ can be well described. The highly excited states above 4.0 MeV are clearly explained as excitations across the neutron $N=82$ shell gap. The monopole effects in these nuclei are carefully examined. In contrast to the already studied northeastern and southwestern quadrants around $^{132}\mathrm{Sn}$ by the EPQQM model, the description of the current Sb data does not request particular monopole corrections. Experiments to further explore the cross-shell excitations in the Sb isotopes are called for.

Non-Abelian ν=12 quantum Hall state in Γ8 valence band hole liquid

In search of states with non-Abelian statistics, we explore the fractional quantum Hall effect in a system of two-dimensional charge carrier holes. We propose a new method of mapping states of holes confined to a finite width quantum well in a perpendicular magnetic field to states in a spherical shell geometry. This method provides single-particle hole states used in exact diagonalization of systems with a small number of holes in the presence of Coulomb interactions. An incompressible fractional quantum Hall state emerges in a hole liquid at the half-filling of the ground state in a magnetic field in the range of fields where single-hole states cross. This state has a negligible overlap with the Halperin 331 state, but a significant overlap with the Moore-Read Pfaffian state. Excited fractional quantum Hall states for small systems have sizable overlap with non-Abelian excitations of the Moore-Read Pfaffian state.

Contribution from optically excited many-electron states to the superexchange interaction in Mott-Hubbard insulators

We propose a multielectron approach to calculate superexchange interaction in magnetic Mott- Hubbard insulator La2CuO4(further La214) that allows to obtain the effect of optical pumping on the superexchange interaction. We use the cell perturbation theory with exact diagonalization of the multiband pd Hamiltonian inside each CuO6 unit cell and treating the intercell hopping as perturbation. To incorporate effect of optical pumping we include in this work the excited singlehole local states as well as all two-hole singlets and triplets. By projecting out the interband intercell electron hopping we have obtained the effective Heisenberg-like Hamiltonian with the local spin at site Ri being a superposition of the ground and excited single-hole states. We found that antiferromagnetic contribution to the exchange energy in La214 will increase in accordance to ~ 4*10_{-3} eV /(%) at the resonance light occupation of the excited single hole in-gap state.

Auger decay rates of core hole states using equation of motion coupled cluster method

The recent development of Linac coherent light source high intense X-ray laser makes it possible to create double core ionization in the molecule. The generation of double core hole state and its decay is identified by Auger spectroscopy. The decay of this double core hole (DCH) states can be used as a powerful spectroscopic tool in chemical analysis. In the present work, we have implemented a promising approach, known as CAP-EOMCC method, which is a combination of complex absorbing potential (CAP) and equation-of-motion coupled cluster (EOMCC) approach to calculate the lifetime of single and double core hole states. We have applied this method to calculate the lifetime of the single core hole (K-LL) and double core hole (KK-KLL) states of CH4, NH3 and HF molecules. The predicted lifetime is found to be extremely short.