Intermediate Excitation Research Articles

State-to-State Spectroscopy and Dynamics of Ions and Neutrals by Photoionization and Photoelectron Methods

Recent advances in high-resolution photoionization, photoelectron, and photodissociation studies based on single-photon vacuum ultraviolet (VUV) and two-color infrared (IR)-VUV, visible (Vis)-ultraviolet (UV), and VUV-VUV laser excitations are illustrated with selected examples. VUV laser photoionization coupled with velocity-map-imaging threshold photoelectron (VMI-TPE) detection can achieve comparable energy resolution but has higher-detection sensitivities than those observed in VUV laser pulsed field ionization photoelectron (PFI-PE) measurements. For molecules with known intermediate states, IR-VUV and Vis-UV excitation schemes are highly sensitive for rovibronically selected and resolved PFI-PE studies. The successful applications of the VUV-PFI-PE, VUV-VMI-TPE, and Vis-UV-PFI-PE methods to state-resolved and state-to-state photoelectron studies of transient radicals and transitional metal-containing molecules are highlighted. The most recently established VUV-VUV pump-probe time-slice VMI photoion method is shown to be promising for state-to-state photodissociation studies of small molecules relevant to planetary atmospheres and for the fundamental understanding of photodissociation dynamics.

Sequential multiple ionization and fragmentation of SF6 induced by an intense free electron laser pulse

We investigate the multiphoton ionization and the subsequent fragmentation of SF6 molecules with intense x-ray-free electron laser pulses at different photon energies. We observe highly charged molecular and atomic ions which were absent in previous experiments with conventional x-ray sources. The observation of fully stripped fluorine ions suggests sequential multiphoton ionization processes with intermediate 1s electron excitation. We measure the average momentum and kinetic energy of each fragment, the comparison of which implies many-body fragmentation pathways of the molecular ions. The observed non-monotonic dependence of the kinetic energy on the charge states of fluorine indicates the multiphoton ionization of ‘isolated’ atomic neutral fluorine or fluorine ions resultant from bond cleavages and also implies the fragmentation of highly charged molecular ions that are produced at a later time during a single pulse.

Chiral three-nucleon force at N4LO. II. Intermediate-range contributions

We derive the subleading contributions to the two-pion-one-pion exchange and ring three-nucleon force topologies emerging at next-to-next-to-next-to-next-to-leading order in chiral effective field theory. The resulting expressions do not involve any unknown parameters. To study convergence of the chiral expansion we work out the most general operator structure of a local isospin-invariant three-nucleon force. Using the resulting operator basis with 22 independent structures, we compare the strength of the corresponding potentials in configuration space for individual topologies at various orders in the chiral expansion. As expected, the subleading contributions from the two-pion-one-pion-exchange and ring diagrams are large which can be understood in terms of intermediate excitation of the Delta(1232) isobar.

Increased Redox-Sensitive Green Fluorescent Protein Reduction Potential in the Endoplasmic Reticulum following Glutathione-Mediated Dimerization

As the endoplasmic reticulum (ER) is the compartment where disulfide bridges in secreted and cell surface proteins are formed, the disturbance of its redox state has profound consequences, yet regulation of ER redox potential remains poorly understood. To monitor the ER redox state in live cells, several fluorescence-based sensors have been developed. However, these sensors have yielded results that are inconsistent with each other and with earlier non-fluorescence-based studies. One particular green fluorescent protein (GFP)-based redox sensor, roGFP1-iL, could detect oxidizing changes in the ER despite having a reduction potential significantly lower than that previously reported for the ER. We have confirmed these observations and determined the mechanisms by which roGFP1-iL detects oxidizing changes. First, glutathione mediates the formation of disulfide-bonded roGFP1-iL dimers with an intermediate excitation fluorescence spectrum resembling a mixture of oxidized and reduced monomers. Second, glutathione facilitates dimerization of roGFP1-iL, which shifted the equilibrium from oxidized monomers to dimers, thereby increasing the molecule's reduction potential compared with that of a dithiol redox buffer. We conclude that the glutathione redox couple in the ER significantly increased the reduction potential of roGFP1-iL in vivo by facilitating its dimerization while preserving its ratiometric nature, which makes it suitable for monitoring oxidizing and reducing changes in the ER with a high degree of reliability in real time. The ability of roGFP1-iL to detect both oxidizing and reducing changes in ER and its dynamic response in glutathione redox buffer between approximately -190 and -130 mV in vitro suggests a range of ER redox potentials consistent with those determined by earlier approaches that did not involve fluorescent sensors.

Study of the neutron rich sulfure isotope 43S through intermediate energy Coulomb excitation

The reduced transition probability B(E2: 3/2− 7/2−2) has been measured in 43S using Coulomb excitation at intermediate energy. The nucleus of interest was produced by fragmentation of a 48Ca beam at GANIL. The reaction products were separated in the LISE spectrometer. After Coulomb-excitation of 43S in a 208Pb target, the γ rays emitted inflight were detected by 64 BaF2 detectors of the Chǎteau de Cristal array. The preliminary value deduced for the reduced transition probability B(E2: 3/2−7/2−2) is in agreement with the predictions of the shell model calculations and supports a prolate-spherical shape coexistence in the 43S nucleus.

Effects of Thermodynamic Pairing on Nuclear Level Density

Thermodynamic properties of some selected even-even nuclei such as $^{56}$Fe, $^{60}$Ni, $^{98}$Mo, and $^{116}$Sn are studied within the Bardeen-Cooper-Schrieffer theory at finite temperature (FTBCS) taking into account pairing correlations. The theory also incorporates the particle-number projection within the Lipkin-Nogami method (FTLN). The level densities are derived based on the statistical theory of the grand-canonical ensemble (GCE). The results obtained are compared with the recent experimental data by Oslo (Norway) group. It is found that pairing correlations have significant effects on nuclear level density, especially at low and intermediate excitation energies.

Flow past a normal flat plate undergoing inline oscillations

The flow past an inline oscillating normal flat plate has been considered with the view to explore the variety of wake phenomena which arise even at the low Reynolds number (Re) equal to 100 based on the free stream velocity and the width of the plate. The three-dimensional Navier-Stokes equations were integrated in time over a wide range of excitation frequencies and amplitudes. A wake flow regime map was produced on the basis of the 24 computer simulations. For a certain excitation amplitude, the wake vortex shedding is first antisymmetric at low excitation frequencies fe. When fe is increased the wake first becomes chaotic and thereafter turns into a symmetric shedding mode, for instance the S-II mode with a binary vortex pair on each side of the wake. If fe is increased even further, more complex symmetric wake patterns may occur before the wake ultimately turns into chaos. Symmetric wakes are thus only observed in a band of intermediate excitation frequencies and then with the dominating flow frequency locked-on to fe. In one particular case, the S-II mode in the very near wake turned into what might be considered as a new S-IV mode which comprised four different vortex pairs per shedding cycle. In spite of the low Re considered, several cases exhibited distinct three-dimensionalities whereas some other cases remained strictly 2D. In some of the cases, at least, the transition from 2D to 3D wake flow was ascribed to a “mode competition.” Finally, for one of the two-dimensional cases the Reynolds number was first increased to 300 and then to 500 and a complex three-dimensional wake flow was observed. However, even at Re = 100, two-dimensional computer simulations are unable to reproduce the three-dimensional wake flow characteristics reported from the present study.

Vibrational Excitation Can Control Tropospheric Chemistry

Which products form during the oxidation of acetylene by hydroxyl radicals and oxygen depends on the internal excitation of a radical intermediate.

Multi-photon-pumped stimulated emission from ZnO nanowires: A time-resolved study

In this work, we study temporal evolution of multi-photon-pumped stimulated emission from ZnO nanowires. In addition to second harmonic generation, ultraviolet stimulated emission is observed in ZnO nanowires under femtosecond pulse excitation at 800 nm. Sharp emission peaks appear when excitation flux reaches a threshold of 80 mJ/cm2, which can be interpreted as lasing action in self-formed nanowire microcavities. Temporal evolution of the emission captured by Kerr shutter technique shows strong excitation-power dependence. The dynamic trace of stimulated emission exhibits a fast decay with a lifetime about 4.5 ps at intermediate excitation (∼100 mJ/cm2) and a lifetime about 2 ps at high excitation (>160 mJ/cm2). The difference in the lifetime can be attributed to different gain mechanisms related to excitonic interaction and electron-hole plasma, respectively.

Maximal Variability of Phase Synchrony in Cortical Networks with Neuronal Avalanches

Ongoing interactions among cortical neurons often manifest as network-level synchrony. Understanding the spatiotemporal dynamics of such spontaneous synchrony is important because it may (1) influence network response to input, (2) shape activity-dependent microcircuit structure, and (3) reveal fundamental network properties, such as an imbalance of excitation (E) and inhibition (I). Here we delineate the spatiotemporal character of spontaneous synchrony in rat cortex slice cultures and a computational model over a range of different E-I conditions including disfacilitated (antagonized AMPA, NMDA receptors), unperturbed, and disinhibited (antagonized GABA(A) receptors). Local field potential was recorded with multielectrode arrays during spontaneous burst activity. Synchrony among neuronal groups was quantified based on phase-locking among recording sites. As network excitability was increased from low to high, we discovered three phenomena at an intermediate excitability level: (1) onset of synchrony, (2) maximized variability of synchrony, and (3) neuronal avalanches. Our computational model predicted that these three features occur when the network operates near a unique balanced E-I condition called "criticality." These results were invariant to changes in the measurement spatial extent, spatial resolution, and frequency bands. Our findings indicate that moderate average synchrony, which is required to avoid pathology, occurs over a limited range of E-I conditions and emerges together with maximally variable synchrony. If variable synchrony is detrimental to cortical function, this is a cost paid for moderate average synchrony. However, if variable synchrony is beneficial, then by operating near criticality the cortex may doubly benefit from moderate mean and maximized variability of synchrony.

Use of stochastic optimization techniques for damage detection in complex nonlinear systems

In this study, the performance of stochastic optimization techniques in the finite element model updating approach was investigated for damage detection in a quarter-scale two-span reinforced concrete bridge system which was tested experimentally at the University of Nevada, Reno. The damage sequence in the structure was induced by a range of progressively increasing excitations in the transverse direction of the specimen. Intermediate non-destructive white noise excitations and response measurements were used for system identification and damage detection purposes. It is shown that, when evaluated together with the strain gauge measurements and visual inspection results, the applied finite element model updating algorithm on this complex nonlinear system could accurately detect, localize, and quantify the damage in the tested bridge columns throughout the different phases of the experiment.

Nonlinear phononics as an ultrafast route to lattice control

To date, two types of coupling between electromagnetic radiation and a crystal lattice have been identified experimentally. One is direct, for infrared (IR)-active vibrations that carry an electric dipole. The second is indirect, it occurs through intermediate excitation of the electronic system via electron-phonon coupling, as in stimulated Raman scattering. Nearly 40 years ago, proposals were made of a third path, referred to as ionic Raman scattering (IRS). It was posited that excitation of an IR-active phonon could serve as the intermediate state for a Raman scattering process relying on lattice anharmonicity as opposed to electron phonon interaction. In this paper, we report an experimental demonstration of ionic Raman scattering and show that this mechanism is relevant to optical control in solids. The key insight is that a rectified phonon field can exert a directional force onto the crystal, inducing an abrupt displacement of the atoms from the equilibrium positions that could not be achieved through excitation of an IR-active vibration alone, for which the force is oscillatory. IRS opens up a new direction for the coherent control of solids in their electronic ground state, different from approaches that rely on electronic excitations.

A new experimental approach and signal processing scheme for the detection and quantitation of 31P brain neurochemicals from in vivo MRS studies using dual tuned (1H/31P) head coil

Brain 31P-neurometabolites play an important role in energy and membrane metabolism. Unambiguous identification and quantification of these neurochemicals in different brain regions would be a great aid in advancing the understanding of metabolic processes in the nervous system. Phosphomonoester (PME), consisting of phosphoethanolamine (PE) and phosphocholine (PC), is the “building block” for membranes, while phosphodiesters (PDE), consisting of glycerophosphocholine (GPC) and glycerophosphoethanolamine (GPE) metabolites are involved in the membrane breakdown process. In the clinical setting, generating well-resolved spectra for PC, PE, GPC, and GPE could be crucial phospholipids in providing information regarding membrane metabolism. We present here a new experimental approach for generating well-resolved 31P spectra for PC and PE as well as for GPC, GPE, and other 31P metabolites. Our results (based on uni-dimensional (1D) and multi-voxel 31P studies) indicate that an intermediate excitation pulse angle (35°) is best suited to obtain well-resolved PC/PE and GPC/GPE resonance peaks. Our novel signal processing scheme allows generating metabolite maps of different phospholipids include PC/PE and GPC/GPE using the ‘time-domain–frequency-domain’ method as referred to in the MATLAB programming language.

A fully simultaneously optimizing genetic approach to the highly excited coupled-cluster factorization problem

In this article we report on the coupled-cluster factorization problem. We describe the first implementation that optimizes (i) the contraction order for each term, (ii) the identification of reusable intermediates, (iii) the selection and factoring out of common factors simultaneously, considering all projection levels in a single step. The optimization is achieved by means of a genetic algorithm. Taking a one-term-at-a-time strategy as reference our factorization yields speedups of up to 4 (for intermediate excitation levels, smaller basis sets). We derive a theoretical lower bound for the highest order scaling cost and show that it is met by our implementation. Additionally, we report on the performance of the resulting highly excited coupled-cluster algorithms and find significant improvements with respect to the implementation of Kállay and Surján [J. Chem. Phys. 115, 2945 (2001)] and comparable performance with respect to MOLPRO's handwritten and dedicated open shell coupled cluster with singles and doubles substitutions implementation [P. J. Knowles, C. Hampel, and H.-J. Werner, J. Chem. Phys. 99, 5219 (1993)].

Controlling inelastic light scattering quantum pathways in graphene

Inelastic light scattering spectroscopy has, since its first discovery, been an indispensable tool in physical science for probing elementary excitations, such as phonons, magnons and plasmons in both bulk and nanoscale materials. In the quantum mechanical picture of inelastic light scattering, incident photons first excite a set of intermediate electronic states, which then generate crystal elementary excitations and radiate energy-shifted photons. The intermediate electronic excitations therefore have a crucial role as quantum pathways in inelastic light scattering, and this is exemplified by resonant Raman scattering and Raman interference. The ability to control these excitation pathways can open up new opportunities to probe, manipulate and utilize inelastic light scattering. Here we achieve excitation pathway control in graphene with electrostatic doping. Our study reveals quantum interference between different Raman pathways in graphene: when some of the pathways are blocked, the one-phonon Raman intensity does not diminish, as commonly expected, but increases dramatically. This discovery sheds new light on the understanding of resonance Raman scattering in graphene. In addition, we demonstrate hot-electron luminescence in graphene as the Fermi energy approaches half the laser excitation energy. This hot luminescence, which is another form of inelastic light scattering, results from excited-state relaxation channels that become available only in heavily doped graphene.

Finite Element Model Updating Using Evolutionary Strategy for Damage Detection

Abstract: Structural health monitoring through the use of finite element model updating techniques for dispersed civil infrastructures usually deals with minimizing a complex, nonlinear, nonconvex, high-dimensional cost function with several local minima. Hence, stochastic optimization algorithms with promising performance in solving global optimization problems have received considerable attention for finite element model updating purposes in recent years. In this study, the performance of an evolutionary strategy in the finite element model updating approach was investigated for damage detection in a quarter-scale two-span reinforced concrete bridge system which was tested experimentally at the University of Nevada, Reno. The damage sequence in the structure was induced by a range of progressively increasing excitations in the transverse direction of the specimen. Intermediate nondestructive white noise excitations and response measurements were used for system identification and damage detection purposes. It is shown that, when evaluated together with the strain gauge measurements and visual inspection results, the applied finite element model updating algorithm of this article could accurately detect, localize, and quantify the damage in the tested bridge columns throughout the different phases of the experiment.

The ab initio No-Core Shell Model and Light Nuclei

The ab initio no-core shell model (NCSM) is a well-established theoretical framework aimed at an exact description of nuclear structure starting from high-precision interactions between the nucleons. In the NCSM we consider a system of A point-like, non-relativistic nucleons that interact by realistic inter-nucleon interactions. We consider two-nucleon interactions that reproduce nucleon-nucleon phase shifts with high precision, typically up to 350 MeV lab energy. We can also include three-nucleon interactions with terms, e.g., related to two-pion exchanges with an intermediate delta excitation. Both semi-phenomenological potentials, based on meson-exchange models, as well as modern chiral interactions can be considered. The performance of the NCSM within nuclear physics will be exemplified by showing results from studies of light nuclei. Major challenges in the future development of the method will be outlined.

Exchange and polarization effect in high-order harmonic imaging of molecular structures

We analyze the importance of exchange, polarization, and electron-electron correlation in high-order harmonic generation in molecules interacting with intense laser fields. We find that electron exchange can become particularly important for harmonic emission associated with intermediate excitations in the molecular ion. In particular, for orbitals associated with two-hole one-particle excitations, exchange effects can eliminate structure-related minima and maxima in the harmonic spectra. Laser-induced polarization of the neutral molecule may also have major effects on orbital structure-related minima and maxima in the harmonic spectra. Finally, we show how exchange terms in recombination can be viewed as a shakedownlike process induced by sudden electronic excitation in the ion.

Electrically controllable RKKY interaction in semiconductor quantum wires

We demonstrate in theory that it is possible to all-electrically manipulate the RKKY interaction in a quasi-one-dimensional electron gas embedded in a semiconductor heterostructure, in the presence of Rashba and Dresselhaus spin-orbit interaction. In an undoped semiconductor quantum wire where intermediate excitations are gapped, the interaction becomes the short-ranged Bloembergen-Rowland super-exchange interaction. Owing to the interplay of different types of spin-orbit interaction, the interaction can be controlled to realize various spin models, e.g., isotropic and anisotropic Heisenberg-like models, Ising-like models with additional Dzyaloshinsky-Moriya terms, by tuning the external electric field and designing the crystallographic directions. Such controllable interaction forms a basis for quantum computing with localized spins and quantum matters in spin lattices.

Intermediate Energy Coulomb Excitation of Neutron-Rich Nuclei

We reinvestigate the collective effects of the retardation as well as the bending on the Coulomb excitation cross sections and also on the B(E2) strengths of some neutron-rich isotopes using the intermediate energy Coulomb excitation theory. It is found that the B(E2) strengths extracted from the experimental Coulomb excitation cross section data get suppressed approximately by 6%. Furthermore, the obtained B(E2) strengths in the energy range 30–100 MeV/A are found to be in better agreement with the corresponding values known from other sources, than those obtained by using the recoil-corrected relativistic Coulomb excitation theory.