Total Excitation Energy Research Articles

Cluster perturbation theory. II. Excitation energies for a coupled cluster target state.

In cluster perturbation (CP) theory, we consider a target excitation space relative to a Hartree-Fock state and partition the target excitation space into a parent excitation space and an auxiliary excitation space. The zeroth-order state is in CP theory a coupled cluster (CC) state in the parent excitation space, and the target state is a CC state in the target excitation space. In this paper, we derive CP series for excitation energies in orders of the CC parent-state similarity-transformed fluctuation potential where the zeroth-order term in the series is an excitation energy for the CC parent state response eigenvalue equation and where the series formally converge to an excitation energy for the CC target state response eigenvalue equation. We give explicit expressions for the lowest-order excitation energy corrections. We also report calculations for CP excitation energy series for various parent and target excitation spaces and examine how well the lower-order corrections can reproduce the total excitation energies. Considering the fast local convergence we have observed for the CP excitation energy series, it becomes computationally attractive to use low-order corrections in CP series to obtain excitation energies of CC target state quality. For the CPS(D-n) series, the first-order correction vanishes, the second-order correction becomes the CIS(D) model, and for the CPS(D-3) model, our calculations suggest that excitation energies of CCSD quality are obtained. The numerical results also suggest that a similar behavior can be seen for the low-order excitation energy corrections for CP series where the parent state contains more than a singles excitation space, e.g., for the CPSD(T) model. We therefore expect the low-order excitation energy corrections in CP series soon to become state-of-the-art models for determining excitation energies of CC target state quality.

Energy Dependence of Fission-fragment Neutron Multiplicity in $^{235}$U$(n,f)$

A consistent framework for treating the energy dependence of fission-fragment neutron multiplicities is presented. The shape evolution of the compound nucleus towards scission is treated in the strong damping limit using the Metropolis walk method. The available excitation energy at scission is then divided statistically between the two fragments using microscopic level densities. Deformation energies, which contribute to the excitation energy when the fragments relax to their ground-state shapes, are also computed. From the total fragment excitation energies, the number of emitted neutrons is obtained and illustrated for neutron-induced fission of $^{235}\textrm{U}$.

Electronic stopping cross section for protons incident on biological and biomedical materials within a FSGO quantum chemistry description

Radiotherapy and dosimetry are techniques used for the treatment of cancer cells and require the proper description of the energy deposition of swift heavy ions when penetrating a biological material. In this work, we report the electronic stopping cross section, by proton radiation, of several complex organic molecules of biological interest that contain, in particular, F and Ar atoms. Our work implements the Harmonic Oscillator approach for the bound electrons through a Floating Spherical Gaussian Orbital description of the molecule in the intermediate to high collision energy within the first Born approximation. In particular, we study the stopping cross section for the following molecules: DNA, guanine, adenine, alanine, glycine, trimethylamine, tissue equivalent gas based on methane and propane, A-150 plastic equivalent material, tissue equivalent liquid, nylon, and air. For complex compounds, where the structure is given in percent by weight (or volume) of molecular fragments, we use a Bragg's-like rule within our model, to determine the electronic stopping cross section. We calculate the orbital and total mean excitation energies for these molecules, finding that it is the orbital mean excitation energy the principal parameter that characterizes the stopping cross section instead of the total molecular mean excitation energy. Our results are in good to excellent agreement to available experimental and theoretical data reported in the literature for these molecules and have an even better agreement than semi-empirical results from approaches like SRIM and PSTAR with the advantage of being analytically simple to implement as well as having a predicting capability for its region of validity.

Revisiting the sodium and calcium matrix effects in inductively coupled plasma optical emission spectrometry. Excitation mechanisms by inelastic collisions

The dependence of calcium and sodium matrix effects on the total excitation energy of analyte emission signals was used as a tool for the study of excitation mechanisms in radial view mode inductively coupled plasma optical emission spectroscopy. A total of 95 atomic and 66 ionic emission signals of aluminum, cobalt, chromium, iron, magnesium, manganese, nickel, and silicon in the 3.0–17.59 eV energy range were measured at the non-robust plasma operating conditions to facilitate the matrix effect study. Different matrix effects versus total excitation energy relationships were observed regarding the energy interval. The change of sign from negative to positive of the both matrix effect versus total excitation energy relationship observed around 14 eV, in the 12.06–17.59 eV energy range, is interpreted as experimental evidence of the action of two non-thermic excitation mechanisms: Penning ionization from approximately 12 to 14 eV and charge transfer from 14 to 17 eV. Based on the energy resonance principle and total spin conservation Wigner’s Theorem, possible reactions between excited ionic argon and ground state analyte ions were proposed.

Cable vibration caused by wind

The paper briefly presents selected basic kinds of excitation of cable vibration caused by dynamic effect of wind. It describes the aerodynamic phenomena such as vortex excitation, wind-rain excitation, galloping and buffeting. Cables are structures which are characterised by low internal damping, low rigidity and low weight, so they are not capable of total excitation energy dissipation, hence they can reach large amplitudes of vibration. Large amplitude of vibration causes excessive stress, thereby lowering the safety of the structure.

Impact of FIFRELIN input parameters on fission observables

Evaluated nuclear data are essential for nuclear reactor studies. In order to significantly improve the precision of nuclear data, more and more fundamental fission models are used in the evaluation processing. Therefore, tests of fission models become a central issue. In this framework, FIFRELIN (FIssion Fragments Evaporation Leading to an Investigation of Nuclear data) is a Monte Carlo code developed in order to modelize fission fragments de-excitation through the emission of neutrons, γ and conversion e-. To be performed, a FIFRELIN calculation relies on several models such as gamma strength function and nuclear level density and of more empirical hypothesis such as total excitation energy repartition or angular momentum given by the fission reaction. Moreover, pre-emission mass yield and kinetic energy distribution per mass are necessary to process the simulation. A set of five free parameters are chosen to reproduce a target observable. Often this observable corresponds to the mean neutron multiplicity for heavy and light fragment. In this work, the impact of the set of parameters on different output observables (neutron emission probability, neutron multiplicity as function of the fission fragment mass) is investigated.

Many-Body Subradiant Excitations in Metamaterial Arrays: Experiment and Theory.

Subradiant excitations, originally predicted by Dicke, have posed a long-standing challenge in physics owing to their weak radiative coupling to environment. Here we engineer massive coherently driven classical subradiance in planar metamaterial arrays as a spatially extended eigenmode comprising over 1000 metamolecules. By comparing the near- and far-field response in large-scale numerical simulations with those in experimental observations we identify strong evidence for classically correlated multimetamolecule subradiant states that dominate the total excitation energy. We show that similar spatially extended many-body subradiance can also exist in plasmonic metamaterial arrays at optical frequencies.

Dissipation and energy balance in electronic dynamics of Na clusters

We investigate the impact of dissipation on the energy balance in the electron dynamics of metal clusters excited by strong electro-magnetic pulses. The dynamics is described theoretically by Time-Dependent Density-Functional Theory (TDDFT) at the level of Local Density Approximation (LDA) augmented by a self interaction correction term and a quantum collision term in Relaxation-Time Approximation (RTA). We evaluate the separate contributions to the total excitation energy, namely energy exported by electron emission, potential energy due to changing charge state, intrinsic kinetic and potential energy, and collective flow energy. The balance of these energies is studied as function of the laser parameters (frequency, intensity, pulse length) and as function of system size and charge. We also look at collisions with a highly charged ion and here at the dependence on the impact parameter (close versus distant collisions). Dissipation turns out to be small where direct electron emission prevails namely for laser frequencies above any ionization threshold and for slow electron extraction in distant collisions. Dissipation is large for fast collisions and at low laser frequencies, particularly at resonances.

Energy balance and deformation at scission in 240Pu fission

The experimental determination of the total excitation energy, the total kinetic energy, and the evaporation neutron multiplicity of fully identified fragments produced in transfer-induced fission of 240Pu, combined with reasonable assumptions, permits to extract the intrinsic and collective excitation energy of the fragments as a function of their atomic number, along with their quadrupole deformation and their distance at scission. The results show that the deformation increases with the atomic number, Z, except for a local maximum around Z=44 and a minimum around Z=50, associated with the effect of deformed shells at Z∼44, N∼64, and spherical shells in 132Sn, respectively. The distance between the fragments also shows a minimum around Z1=44, Z2=50, suggesting a mechanism that links the effect of structure with the length of the neck at scission.

Experimental investigation of the detection mechanism in WSi nanowire superconducting single photon detectors

We use quantum detector tomography to investigate the detection mechanism in WSi nanowire superconducting single photon detectors. To this purpose, we fabricated a 250 nm wide and 250 nm long WSi nanowire and measured its response to impinging photons with wavelengths ranging from λ = 900 nm to λ = 1650 nm. Tomographic measurements show that the detector response depends on the total excitation energy only. Moreover, for total absorbed energies >0.8 eV the current–energy relation is linear, similar to what was observed in NbN nanowires, whereas the current–energy relation deviates from linear behavior for total energies below 0.8 eV.

Two-Photon Activation of p-Hydroxyphenacyl Phototriggers: Toward Spatially Controlled Release of Diethyl Phosphate and ATP.

Two-photon activation of the p-hydroxyphenacyl (pHP) photoactivated protecting group is demonstrated for the first time using visible light at 550 nm from a pulsed laser. Broadband two-photon absorption measurements reveal a strong two-photon transition (>10 GM) near 4.5 eV that closely resembles the lowest-energy band at the same total excitation energy in the one-photon absorption spectrum of the pHP chromophore. The polarization dependence of the two-photon absorption band is consistent with excitation to the same S3 ((1)ππ*) excited state for both one- and two-photon activation. Monitoring the progress of the uncaging reaction under nonresonant excitation at 550 nm confirms a quadratic intensity dependence and that two-photon activation of the uncaging reaction is possible using visible light in the range 500-620 nm. Deprotonation of the pHP chromophore under mildly basic conditions shifts the absorption band to lower energy (3.8 eV) in both the one- and two-photon absorption spectra, suggesting that two-photon activation of the pHP chromophore may be possible using light in the range 550-720 nm. The results of these measurements open the possibility of spatially and temporally selective release of biologically active compounds from the pHP protecting group using visible light from a pulsed laser.

QUANTUM-STATE DEPENDENCE OF PRODUCT BRANCHING RATIOS IN VACUUM ULTRAVIOLET PHOTODISSOCIATION OF N2

ABSTRACT The branching ratios for the N(4S) + N(2D), N(4S) + N(2P), and N(2D) + N(2D) channels are measured for the photodissociation of N 2 ( X 1 &Sgr; g + ; v ″ = 0 , J ″ ) ?> in the vacuum ultraviolet (VUV) region of 100,808–122,159 cm−1 using the VUV–VUV pump-probe approach combined with velocity-map-imaging-photoion detection. No evidence of forming the ground-state N(4S) + N(4S) products is found. No potential barrier is observed for the N(2D) + N(2D) channel, but the N(4S) + N(2P) channel has a small potential barrier of ≈740 cm−1. The branching ratios are found to depend on the symmetry of predissociative N2 states instead of the total VUV excitation energy, indicating that N2 photodissociation is nonstatistical. When the branching ratios for N(4S) + N(2D) and N(4S) + N(2P) products are plotted as a function of the VUV excitation energy for the valence N2 1Πu and 1 &Sgr; u + ?> states, oscillations in these ratios are observed demonstrating how these channels are competing with each other. These data can be used to select both the velocity and internal states of the atomic products by picking the quantum state that is excited. High-level ab initio potential energy curves of the excited N2 states are calculated to provide insight into the mechanisms for the observed branching ratios. The calculations predict that the formation of both N(4S) + N(2D) and N(4S) + N(2P) channels involves potential energy barriers, in agreement with experimental observations. A discussion of the application of the present results to astronomy, planetary sciences, and comets is given.

The scission point configuration of fissioning nuclei

We define the optimal shape which fissioning nuclei attain just before the scission and calculate the deformation energy as function of the mass asymmetry at the scission point. The calculated deformation energy is used in quasi-static approximation for the estimation of mass distribution, total kinetic and excitation energy of fission fragments, and the total number of prompt neutrons. The calculated results reproduce rather well the experimental data on the position of the peaks in the mass distribution of fission fragments, the total kinetic and excitation energy of fission fragments. The calculated value of neutron multiplicity is somewhat larger than experimental results. The saw-tooth structure of neutron multiplicity is qualitatively reproduced.

Sensitivity of Prompt Neutron Multiplicity to Fission Fragment Characteristics

The Point-by-Point (PbP) model as well as the related computer code is a useful tool to provide different prompt emission data [as a function of fragment mass A, fragment charge Z, total kinetic energy (TKE), and total average ones]. The present work focuses on the sensitivity of prompt neutron multiplicity to different properties of the fission fragments. In the construction of the fragmentation range of the PbP treatment, the use of different Z prescriptions affects the multiparametric matrices of different fragment and prompt emission quantities q(A,Z,TKE). The nonnegligible influence of how the most probable charge is considered (as unchanged charge distribution without or with the charge deviations ΔZ as a function of A or an average ΔZ value), as well as the number of Z taken at each A, is discussed. The calculated average prompt emission quantities as a function of A, as a function of TKE, and total average ones depend on the accuracy of experimental Y(A,TKE) distributions. The prompt neutron multiplicity of complementary fragments vpair (A) has a weak dependence on the total excitation energy (TXE) partition between complementary fully accelerated fragments. This assures a good prediction of the average prompt neutron multiplicity as a function of TKE and of the total average one even in the case of a rough or inappropriate TXE partition. The systematic behavior revealed by the experimental ratio vH/vpair as a function of AH together with the weak dependence of vpair(A) on the TXE partition can be exploited—in the absence of experimental v(A) information—for an indirect verification of predicted v(A).

Characterization of the scission point from fission-fragment velocities

The isotopic-yield distributions and kinematic properties of fragments produced in transfer-induced fission of 240Pu and fusion-induced fission of 250Cf, with 9 MeV and 45 MeV of excitation energy respectively, were measured in inverse kinematics with the spectrometer VAMOS. The kinematic properties of identified fission fragments allow to derive properties of the scission configuration such as the distance between fragments, the total kinetic energy, the neutron multiplicity, the total excitation energy, and, for the first time, the proton- and neutron-number sharing during the emergence of the fragments. These properties of the scission point are studied as functions of the fragment atomic number. The correlation between these observables, gathered in one single experiment and for two different fissioning systems at different excitation energies, give valuable information for the understanding and modeling of the fission process.

Trajectory and Model Studies of Collisions of Highly Excited Methane with Water Using an ab Initio Potential.

Quasi-classical trajectory studies have been performed for the collision of internally excited methane with water using an accurate methane-water potential based on a full-dimensional, permutationally invariant analytical representation of energies calculated at a high level of theory. The results suggest that most energy transfer takes place at impact parameters smaller than about 8 Bohr; collisions at higher impact parameters are mostly elastic. Overall, energy transfer is fairly facile, with values for ⟨ΔEdown⟩ and ⟨ΔEup⟩ approaching almost 2% of the total excitation energy. A classical model previously developed for the collision of internally excited molecules with atoms (Houston, P. L.; Conte, R.; Bowman, J. M. J. Phys. Chem. A 2015, 119, 4695-4710) has been extended to cover collisions of internally excited molecules with other molecules. For high initial rotational levels, the agreement with the trajectory results is quite good (R(2) ≈ 0.9), whereas for low initial rotational levels it is only fair (R(2) ≈ 0.7). Both the model and the trajectories can be characterized by a four-dimensional joint probability distribution, P(J1,f,ΔE1,J2,f,ΔE2), where J1,f and J2,f are the final rotational levels of molecules 1 and 2 and ΔE1 and ΔE2 are the respective changes in internal energy. A strong anticorrelation between ΔE1 and ΔE2 is observed in both the model and trajectory results and can be explained by the model. There is evidence in the trajectory results for a small amount of V ↔ V energy transfer from the water, which has low internal energy, to the methane, which has substantial internal energy. This observation suggests that V ↔ V energy transfer in the other direction also occurs.

Comparing different energy partitions at scission used in prompt emission model codes GEF and Point-by-Point

Different methods to partition the total excitation energy (TXE) of fully accelerated fragments, presently used in prompt emission calculations include different assumptions about what is happening at scission. In fact the energy partition takes place at scission or even before scission, depending on the physical assumptions supporting the models used in different methods of TXE partition.The paper discusses two TXE partition methods in which the amount of energy to be shared (at scission and before scission, respectively) is very different. These methods (based on different principles and physical considerations) are: A. The method used in the Point-by-Point (PbP) treatment of prompt emission in which the available excitation energy at scission is shared between complementary nascent fragments. The amount of energy to be shared is sufficiently high to consider the nascent fragments in the Fermi-gas regime of the level density. B. The method used in the GEF code, in which the intrinsic energy before scission is shared between pre-nascent fragments according to the “energy sorting mechanism”. This sorting mechanism is based on the assumption of level densities in the constant temperature regime, only. This is supported by the low amount of the shared intrinsic energy in the case of thermal and low energy neutron induced fission.Taking into account that the principles and physical considerations of any TXE partition method are independent on the way to treat the prompt emission (i.e. deterministically as in the PbP model or probabilistically by Monte-Carlo as in the code GEF) the methods A and B are applied to the same fission fragment range (built as in the PbP treatment). Extreme hypotheses are made for the fragment level densities on which the partitions are based (only in the Fermi-gas regime or only in the constant temperature regime). The results are compared with the energy partition obtained with fragment level densities described by the composite Gilbert–Cameron formula. Different assumptions for the deformation energies of fragments (absolute deformation at scission, or extra-deformation at scission with respect to the full acceleration) impacting the sawtooth-like shape of the excitation energy E⁎(A) at full acceleration are discussed, too. Limitations and advantages of these methods are also mentioned. Both TXE partition methods applied in the PbP model lead to prompt emission results (e.g. ν(A) and Eγ(A)) describing well the experimental data.

The Scission Point Configuration and the Multiplicity of Prompt Neutrons

We defined the optimal shape which fissioning nuclei attain just before the scission and calculated the deformation energy as function of the mass asymmetry and elongation at the scission point. The calculated deformation energy is used in quasi-static approximation for estimation of the mass distribution of fission fragments, total kinetic and excitation energy of fission fragments, and the total number of prompt neutrons. The calculated results reproduce rather well the experimental data on the position of the peaks in the mass distribution of fission fragments, the total kinetic and excitation energy of fission fragments. The calculated value of neutron multiplicitiy is somewhat larger than experimental results.

Influence of the density of states on the odd-even staggering in the charge distribution of the emitted fragments in nuclear heavy-ion collisions

The fragmentation of thermalized sources is studied using a version of the Statistical Multifragmentation Model which employs state densities that take the pairing gap in the nuclear levels into account. Attention is focused on the properties of the charge distributions observed in the breakup of the source. Since the microcanonical version of the model used in this study provides the primary fragment excitation energy distribution, one may correlate the reduction of the odd-even staggering in the charge distribution with the increasing occupation of high-energy states. Thus, in the framework of this model, such staggering tends to disappear as a function of the total excitation energy of the source, although the energy per particle may be small for large systems. We also find that, although the deexcitation of the primary fragments should, in principle, blur these odd-even effects as the fragments follow their decay chains, the consistent treatment of pairing may significantly enhance these staggering effects on the final yields. In the framework of this model, we find that odd-even effects in the charge distributions should be observed in the fragmentation of relatively light systems at very low excitation energies. Our results also suggest that the odd-even staggering may provide useful information on the nuclear state density.

Scission-point configuration within the two-center shell model shape parameterization

Within the two-center shell model parameterization we defined the optimal shape that fissioning nuclei attain just before the scission and calculated the total deformation energy (liquid-drop part plus the shell correction) as a function of the mass asymmetry and elongation at the scission point. The three minima corresponding to one mass-symmetric and two mass-asymmetric peaks in the mass distribution of fission fragments are found in the deformation energy at the scission point. The calculated deformation energy is used in a quasistatic approximation for the estimation of the total kinetic and excitation energies of fission fragments and the total number of emitted prompt neutrons. The calculated results reproduce rather well the experimental data on the position of the peaks in the mass distribution of fission fragments, and the total kinetic and excitation energies of fission fragments. The calculated value of neutron multiplicity is somewhat larger than experimental results.