Inelastic Excitation Research Articles

Nickelocene SPM tip as a molecular spin sensor.

Functionalization of a scanning microscopy probe with a single nickelocene allows reproducible
spin-sensitive measurements of magnetic systems on surfaces. The triplet ground state of the nicke-
locene tip gives rise to a characteristic inelastic electron spin-flip excitation, which can change upon
interaction with spin systems on the surface. These changes, together with theoretical simulations,
enable us to determine the local spin moment on the surface. In this paper, we discuss the exper-
imental and theoretical aspects of nickelocene-tip measurements. We rationalize the interactions
between the nickelocene spin and the magnetic centers using a spin Heisenberg and dipole model,
complemented by cotunneling theory, and compare the simulated dI/dV with selected experimental
results. We developed a Python script to simulate this magnetic interaction, which is available on
GitHub.

N-changing population of Rydberg states by low-energy electron-Rydberg collisions.

Inelastic n-changing collisions play an important role in the evolution of Rydberg atoms into ultracold plasmas. However, for the initially intermediate n (n ∼ 40) Rydberg states, these collisions can hardly be observed due to the low electron temperature in ultracold plasmas. In this work, we designed an experimental scheme to facilitate collisions between free electrons at 1.5eV and intermediate n Rydberg atoms. Using the field ionization technique, we measured the state distributions resulting from the evolution of initially cold rubidium atoms in the 45P3/2 Rydberg state. The experimentally obtained probability of inelastic collisions excitation agrees well with the Monte Carlo simulation results. In addition, our experimental results indicate that the n-changing population induced by hot electrons is significant for lower nP Rydberg states. Our work plays a significant role in calculating the rates of electron-ion three-body recombination in ultracold plasmas.

Strong Electron-Vibration Signals in Weakly Coupled Molecular Junctions: Activation of Spin-Crossover.

Manipulating individual molecular spin states with electronic current has the potential to revolutionize quantum information devices. However, it is still unclear how a current can cause a spin transition in single-molecule devices. Here, we propose a spin-crossover (SCO) mechanism induced by electron-phonon coupling in an iron(II) phthalocyanine molecule situated on a graphene-decoupled Ir(111) substrate. We performed simulations of both elastic and inelastic electron tunneling spectroscopy (IETS), which reveal current-induced Fe-N vibrations and an underestimation of established electron-vibration signals. Going beyond standard perturbation theory, we examined molecules in various charge and spin states using the Franck-Condon framework. The increased probability of spin switching suggests that notable IETS signals indicate SCO triggered by the inelastic vibrational excitation associated with Fe-N stretching.

Recent advances in relativistic excitation of atomic hydrogen

Within the framework of the relativistic regime ( E k > 2700 eV) and the first Born approximation, we investigate the inelastic excitation of atomic hydrogen by electron impact from 1 s to 2 p state. The incoming and outgoing electrons are described by free Dirac spinors, while the hydrogen atom target is described by the exact solutions of Dirac equation with a central potential. A detailed study has been devoted to the non-relativistic regime as well as the relativistic regime of the process, and the results obtained show the differences between the two regimes. These differences have revealed that the differential cross section (DCS) is influenced by the parameters of the 1 s and 2 p states, along with significant effects on diffusion during small pulse transfers. The relativistic effects are responsible for the significant changes in the DCS as a function of diffusion angles which depend on the chosen geometry.

Electronic structure and resonant inelastic x-ray scattering in Ca3Ru2O7

We have investigated the electronic structure of the transition metal oxide Ca3Ru2O7 within density-functional theory using the generalized gradient approximation while considering strong Coulomb correlations in the framework of the fully relativistic spin-polarized Dirac linear muffin-tin orbital band structure method. Ca3Ru2O7 can be classified as a Mott insulator since it was expected to be metallic from band structure calculations. We found that the magnetic ground state of Ca3Ru2O7 possesses an AFM−b magnetic structure with the Ru spin moments ordered antiferromagnetically along the b axis. We have investigated the resonant inelastic x-ray scattering (RIXS) spectra at the Ru and Ca K, L3, and M3 edges as well as at the OK edge. The experimentally measured RIXS spectrum of Ca3Ru2O7 at the Ru L3 edge possesses a sharp feature ≤2eV corresponding to transitions within the Ru t2g levels. The excitation located from 2 to 4 eV is due to t2g→ eg transitions. The third wide structure situated at 4.5−11eV appears due to transitions between the Ru 4dO states derived from the tails of oxygen 2p states and eg and t2g states. The RIXS spectra at the Ru L3 and M3 edges are quite similar. However, the corresponding RIXS spectra at the Ca site are quite different from each other due to the significant difference in the widths of core levels. The RIXS spectrum at the OK edge consists of three major inelastic excitations. We found that the first two low energy features ≤2.5eV are due to interband transitions between occupied and empty Ot2g states which appear due to the strong hybridization between oxygen 2p and Ru t2g states in close vicinity to the Fermi level. The next major peak between 2.5 and 8 eV reflects interband transitions from occupied O2p to empty Ot2g states. A wide energy interval between 4 and 11 eV is occupied by rather weak O2p→Oeg transitions. Published by the American Physical Society 2024

Shear wave propagation in a liquid crystal: An inelastic X-ray scattering study.

We investigated the spectrum of density fluctuations of a liquid crystal, CB7CB, in two different orientations by using high-resolution inelastic x-ray scattering. Our analysis, based on Bayesian principles, revealed that high-frequency collective excitations propagate through this mesoscale-ordered sample in a peculiar manner that lies somewhere between those observed in liquids and crystalline systems. Interestingly, when we probed longer length scales, a more pronounced solid-like response emerged. This was mainly characterized by anomalously sharp inelastic excitations and the onset of shear mode propagation. Comparison with previous x-ray diffraction results suggests a correlation between the observed behavior and the mesogen arrangement.

The slopes of sub-barrier heavy-ion fusion excitation functions shed light on the dynamics of quantum tunnelling

Quantum tunnelling plays a crucial role in heavy-ion fusion reactions at sub-barrier energies, especially in the context of nuclear physics and astrophysics. The nuclear structure of the colliding nuclei and nucleon transfer processes represent intrinsic degrees of freedom. They are coupled to the relative ion motion and, in general, increase the probability of tunnelling. The influence of couplings to nucleon transfer channels relatively to inelastic excitations, on heavy-ion fusion cross sections, is one of the still open problems in this field. We present a new analysis of several systems, based on the combined observation of the energy-weighted excitation functions Eσ\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$E\\sigma $$\\end{document} in relation to their first energy derivatives d(Eσ)/dE\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$d(E\\sigma )/dE$$\\end{document}. The relation between d(Eσ)/dE\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$d(E\\sigma )/dE$$\\end{document} and Eσ\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$E\\sigma $$\\end{document} removes the basic differences due to the varying Coulomb barrier when comparing different systems. We show that, depending on the nuclear structure and/or the presence of strong transfer channels, this representation reveals characteristic features below the barrier. The possible presence of cross section oscillations makes this analysis less clear for light- or medium-light systems.

The 50th anniversary of the coupled channels Born approximation (CCBA) and the coupled reaction channels (CRC) theories of nucleon transfer reactions (a unique interplay between theory, experiment and computer technology, conducted during the most tumultuous period in modern American society)

Nucleon transfer reactions have played a fundamental role in understanding the single-particle components, shell structure and collective properties of atomic nuclei. The conventional distorted wave Born approximation (DWBA) envisioned the nucleon transfer reaction as a one-step process, which proceeds directly from the ground state of the target nucleus to a state of the residual nucleus. The coupled channels Born approximation (CCBA) and coupled reaction channels (CRC) theories evolved because a number of nucleon transfer reaction cross sections could not be reconciled within the DWBA. These coupled channels models revealed that, in addition to the “one-step” process of the DWBA, “multi-step” nucleon transfer processes involving accessary pathways can participate in populating the final nuclear state. In the CCBA, the auxiliary pathways involved inelastic excitations of the target and/or residual nucleus, whereas, in the CRC, the pathways included sequential nucleon transfer passing through nuclear states of an intermediate partition. Coherent addition of contributions from one-step and multi-step nucleon transfer processes resulted in dramatic alterations in reaction cross sections, which were experimentally confirmed. The CCBA and CRC linked the structure of the nuclei participating in a reaction to modalities of nucleon transfer arising during the relative motion between the interacting ions. These complementary theories inexorably changed physicists’ interpretations of nucleon transfer reactions and, in doing so, heralded in the new field of direct heavy-ion reactions.

Role of multi-neutron transfer channels on fusion enhancement

Fusion reactions 40Ar + 116Sn, 40Ar + 122Sn and 40Ca + 124Sn have been examined by employing coupled channel (CC) approach using code-CCFULL. Here we aim to investigate the influence of multi-neutron transfer channels in addition to coupling of collective excitations on sub-barrier fusion enhancement. Incorporation of inelastic excitations alone reproduced the experimental results for 40Ar + 116Sn system while for 40Ar + 122Sn contribution of 2n transfer channel is required to explain the experimental data. However, CC calculations with 2n transfer could not explain the enhancement at sub-barrier energies for 40Ca + 124Sn system. Therefore, the empirical coupled channel (ECC) calculations have been carried out to include the effect of multi-neutron transfer channels and it is found that the incorporation of sequential 4n transfer channel reproduced the experimental results in entire energy region. Nevertheless, it is observed that multi-neutron transfer coupling significantly contributed in raising the sub-barrier fusion cross sections particularly for the reactions where colliding partners are spherical. Importantly, it is also found that transfer of even number of neutrons play dominating role in sub-barrier fusion enhancement.

Inelastic scattering of Li＋ with CO: New ab initio potential energy surface and quantum dynamics

The interaction potential between Li＋ and CO has been investigated using quantum dynamical calculations. The ab initio ground electronic potential energy surface has been computed using the aug-cc-pVQZ basis set at MRCI level of accuracy. Quantum dynamics results within the VCC-RIOSA framework have been presented at collision energy Ec.m. = 3.64 eV. The computed differential cross sections (DCS) for the inelastic vibrational excitations have been found to be in qualitative agreement with those obtained in the experiments of Böttner et al. (1976). Other attributes like rotationally-summed state-to-state DCS, and integral cross sections, are also calculated. The rotational excitations are studied using rigid-rotor coupled-states methodology at Ec.m. = 4.23 eV showing excitations up to j′ = 40. Rotational excitations rates at very low collision energy range (Ec.m. = 0–300 cm−1) using rigid-rotor full close-coupling method have also been calculated in view of their astrophysical significance.

Collision integrals of electronically excited atoms in air plasmas. I. N–N and O–O interactions

The current work presents the collision integral data for N(4 S)–N(4 S, 2 D, 2 P) and O(3 P, 1 D, 1 S)–O(3 P, 1 D, 1 S) interactions in the temperature range of 500–50 000 K. The collision integrals are calculated based on high-quality potential energy curves (PECs) obtained from fitting the high-level calculation data in a wide energy range to the neural network (NN) functions. In the construction of PECs, the diabatic PECs are adopted when avoided crossings exist because the diabatic paths are much more likely to be followed for such situations. Moreover, the nonadiabatic transition effects are estimated to be negligible for PECs crossings. The accuracy of traditional analytical formulas to fit PECs are also examined. It is found that the collision integral calculations are sensitive to the accuracy of PECs and the NN based PECs overwhelm the others. The contribution of inelastic excitation exchange processes to the diffusion collision integrals are also computed by using an accurate evaluation of the differences of PECs for gerade and ungerade pairs of excited atoms. Finally, based on the new collision integral data, we calibrate the collision model parameters suitable for the widely used particle simulation methods. The collision integrals and collision models developed in this work can be used to support high-confidence simulations of weakly ionized air plasma problems.

Influence of neutron transfer channels on fusion dynamics near the Coulomb barrier for 28Si + 116,120,124Sn systems

The phenomenon of enhanced fusion cross-section as compared to the theoretical predictions of 1-D BPM has been extensively studied over the past few decades. However, the unambiguous role of neutron transfer channels on the sub-barrier fusion enhancement is still elusive in most cases. Fusion cross-section measurements ≈ 15% below and above the Coulomb barrier were performed to elucidate the mechanisms responsible for the experimentally observed sub-barrier fusion enhancement. Coupled-channels calculations using CCFULL were used to decipher the reaction dynamics. CC calculations explained the fusion excitation function for 28Si + 116,120Sn systems after the inclusion of inelastic excitations along with a pair transfer. However, the observed behavior for the 28Si + 124Sn system could not be explained. The fusion barrier distribution has been extracted from the experimental data to unveil the various channels coupled in the concerned rection. A single uncoupled barrier was transformed into a distribution of barriers depicting the presence of different channels coupled in the reaction. The results indicate a significant effect from multi-neutron transfer channels on the fusion dynamics.

(Invited) Interplay Between π–Conjugation and Exchange Magnetism in One-Dimensional Porphyrinoid Polymers

The field of carbon magnetism has gained an increased attention in view of the recent progress made in the synthesis and characterization of open-shell polycyclic aromatic hydrocarbons following a bottom-up synthetic approach[1,2]. Under this scenario, the comprehensive fabrication of magnetic porphyrinoid-based polymers emerges as a highly appealing field of research. However, the vast majority of the porphyrinoid species and polymers studied to date exhibit a closed-shell ground state[3].In this work, we introduce an exemplary approach toward the bottom-up fabrication of unprecedented magnetic porphyrinoid-based polymers homocoupled via surface-catalyzed [3 + 3] cycloaromatization of isopropyl substituents studied on Au(111) under ultra-high vacuum (UHV) conditions. The chemical structure of the polymer, formed by thermal-activated intra- and intermolecular oxidative ring closure reactions followed by controlled tip-induced hydrogen dissociation from the porphyrinoid units, have been clearly elucidated by scanning tunneling microscopy (STM) and non-contact atomic force microscopy (nc-AFM). Scanning tunneling spectroscopy (STS), complemented by computational investigations reveals the open-shell character, i.e. antiferromagnetic singlet ground state (S=0) of the formed polymers, which display singlet−triplet inelastic excitations observed between spins of adjacent porphyrinoid units only along a specific π-conjugation pathway, thus revealing the interplay between π-conjugation and magnetic exchange. We envision that our approach can be a highly relevant step towards the on-surface synthesis of covalently linked 1D magnetic organic polymers with prospects in nanoscale spintronic devices.

A deformed global spherical optical potential to describe proton scattering off statically deformed heavy nuclei

We examine the applicability of the adiabatic approximation in the case of proton scattering off statically deformed actinide and rare-earth nuclei. This is achieved by deforming a global spherical potential to allow coupling of the elastic channel to inelastic rotational excitation states. Only the radius of volume term of the spherical potential is deformed. The rest of the potential parameters are used unaltered. The model reproduced the scattering observables well. The results are congruent to those of a global model in the literature that determines the potential parameters by fitting the experimental data within a channel coupling formalism. A necessary requirement for the adiabatic approximation to hold is that the speed of the proton should be much larger than the angular speed of the deformed target nucleus. The fact that our calculated angular distributions and total cross sections agree well with experiment indicates that this condition is still valid despite the possibility of the proton being decelerated by the coulomb force as it approaches the deformed nucleus.

Exploring the possibilities of sub barrier fusion enhancement in fusion reactions induced by 28Si on 64Ni, 96Zr, 100Mo and 154Sm at energies around Coulomb barrier

The fusion excitation functions of reactions induced by 28Si on 64Ni, 96Zr, 100Mo and 154Sm targets at around Coulomb barrier energies have been analysed theoretically within coupled channel approach. Here we have examined the sensitivity of fusion cross section at sub-barrier energies towards coupling of inelastic excitations of fusing partners and positive Q-value neutron transfer (PQNT) channels. Along with the transfer channel, the influence of variation in deformation of fusing nuclei after transfer and of nuclear structure of fusing nuclei has also been considered. With a view to investigate the influence of nuclear structure here we have taken targets with different structural properties. It is found that coupling of neutron transfer channels produced a significant enhancement in sub-barrier fusion for the systems where one of the interacting nuclei is spherical or less deformed and no influence of transfer coupling has been observed for the system where both the participating nuclei are deformed.

Light Emission from Single Oxygen Vacancies in Cu2O Films Probed with Scanning Tunneling Microscopy.

Global photoluminescence (PL) and spatially resolved scanning tunneling microscopy (STM) luminescence are compared for thick Cu2O films grown on Au(111). While the PL data reveal two peaks at 750 and 850 nm, assigned to radiative electron decays via localized gap states induced by O vacancies, a wide-band emission between 700 and 950 nm is observed in STM luminescence. The latter is compatible with cavity plasmons stimulated by inelastic electron tunneling and contains no spectral signature of the Cu2O defects. The STM luminescence is nonetheless controlled by O vacancies that provide inelastic excitation channels for the cavity plasmons. In fact, the emission yield sharply peaks at 2.2 V sample bias, when tip electrons are resonantly injected into O defect states and recombine with holes at the valence-band top via plasmon stimulation. The spatially confined emission centers detected in photon maps of the Cu2O films are therefore assigned to excitation channels mediated by single or few O vacancies in the oxide matrix.

Collective excitations in a melt of fast phase change material GeCu2Te3

Inelastic x-ray scattering measurements have been carried out to investigate atomic dynamics in a melt of fast phase change material GeCu2Te3. The dynamic structure factor was analysed using the model function with three damped harmonic oscillator components. By investigating the correlation between the excitation energy and the linewidth, and that between the excitation energy and the intensity on contour maps of a relative approximate probability distribution function proportional to , we could judge the reliability of each inelastic excitation in the dynamic structure factor. The results indicate that there are two inelastic excitation modes besides the longitudinal acoustic one in the liquid. The lower energy excitation could be assigned to the transverse acoustic one whereas the higher energy one disperses like fast sound. The latter result may imply that the liquid ternary alloy exhibits a microscopic phase separation tendency.

Analysis of nucleon-nucleus scattering data using a density-dependent semi-microscopic optical model with channel coupling

Background: The neutron scattering data was previously analyzed using a semi-microscopic optical model with channel coupling to inelastic excited states [Phys. Rev. C 100, 014603 (2019)]. The real part of the potential was constructed by single folding the density-independent M3Y-Paris bare nucleon-nucleon ($NN$) interaction, with zero-range knock-on exchange term, over the density of the target nucleus. The model reproduced the overall features of the inelastic angular distributions and polarization data. The elastic angular distributions were well reproduced.Purpose: In this work we test the effectiveness of the semi-microscopic optical model with channel coupling, but we employ a density-dependent BDM3Y1-Paris bare ($NN$) interaction, with the finite-range form of the knock-on exchange term, in describing the scattering observables, particularly, the inelastic distributions and polarization data.Method: The real volume term of the semi-microscopic model is constructed by single folding the density-dependent BDM3Y1-Paris bare ($NN$) interaction, over the matter distribution of the target nucleus. The ground state is coupled to low-lying inelastic excitation levels. The potential parameters are determined by fitting the elastic, inelastic, and polarization data corresponding to nucleon scattering off a wide range of mass numbers in the range $7\ensuremath{\le}A\ensuremath{\le}208$ for various energies from 10--95 MeV.Results: The density-dependent model resulted in significant improvements in the description of the inelastic angular distributions and analyzing power. In addition, the potential depths showed systematic linear dependence on incident energy, and one set of geometrical parameters is obtained for each nuclear target. We used our best-fit potential parameters to calculate the total cross sections corresponding to nucleon scattering off the considered nuclei. The calculated cross sections are in good agreement with the measured data.Conclusions: In a semi-microscopic optical model, construction of the real volume term by single folding the density-dependent BDM3Y1-Paris bare ($NN$) interaction, with finite form of the knock-on exchange term, results in significant improvements in reproducing the inelastic angular distributions and polarization data as compared to the case of using the density-independent M3Y-Paris bare nucleon-nucleon ($NN$) interaction, with either zero-range or finite-range exchange term.

Spin gap in the weakly interacting quantum spin chain antiferromagnet KCuPO4·H2O

The $S=1/2$ Heisenberg linear chain antiferromagnet is the simplest spin model; nevertheless it serves as a platform for various quantum many-body phenomena. Here, we report the magnetic behavior of a quasi-one-dimensional antiferromagnet ${\mathrm{KCuPO}}_{4}\ifmmode\cdot\else\textperiodcentered\fi{}{\mathrm{H}}_{2}\mathrm{O}$. A long-range commensurate antiferromagnetic order with ordered moment 0.31(1) ${\ensuremath{\mu}}_{\mathrm{B}}$ per spin occurs at ${T}_{\mathrm{N}}=11.7(1)$ K. Above ${T}_{\mathrm{N}}$, the inelastic neutron excitation is characterized by a two spinon continuum. The intrachain interaction $J$ and interchain interaction $|{J}^{\ensuremath{'}}|$ are estimated to be 172 and 4.25(4) K, respectively; thus the ratio of $|{J}^{\ensuremath{'}}|/J=0.0247(3)$. At lower energies, below ${T}_{\mathrm{N}}$, a spin gap is observed in the dispersive excitations. These results are consistent with characteristics observed in a weakly interacting $S=1/2$ Heisenberg chain system.

A Nanocar and Rotor in One Molecule.

Depending on its adsorption conformation on the Au(111) surface, a zwitterionic single-molecule machine works in two different ways under bias voltage pulses. It is a unidirectional rotor while anchored on the surface. It is a fast-drivable molecule vehicle (nanocar) while physisorbed. By tuning the surface coverage, the conformation of the molecule can be selected to be either rotor or nanocar. The inelastic tunneling excitation producing the movement is investigated in the same experimental conditions for both the unidirectional rotation of the rotor and the directed movement of the nanocar.