Search results for "Coupled"
showing 10 items of 742 documents
Simulataneous application of charge coupled device array-detected Raman spectroscopy and differential scanning calorimetry to in situ investigation o…
1992
The combination of differential scanning calorimetry (DSC) with charge coupled device (CCD) array-detected Raman spectroscopy for the in situ investigation of phase transition is illustrated using ammonium nitrate as an example. This method aids unambiguous characterization of different phases by providing a simultaneous probe of thermodynamic and vibrational data. The availability of real-time vibrational data, including both the internal and external mode regions, is unique to array-detected Raman spectroscopy. The intensity changes of the symmetric stretching mode ν1 of the nitrate ions and the lattice vibrations, that accompany the phase transition IV → II of ammonium nitrate, are ratio…
Trace element data covering 96-7 ka BP from stalagmite CM (Santo Tomas Cave, Cuba)
2020
We present a new speleothem trace element and stable isotope record, which extends previous paleoclimate evidence from Cuban speleothems to the last 96 ka. Stable isotope samples were micromilled at a resolution of 0.10-0.33mm, and measured using an IRMS equipped with a Gasbench. Line scans of Element/Calcium ratios of the speleothem were measured by laser ablation ICPMS and were reduced to the resolution of the stable isotope records.
Nonadiabatic orientation, toroidal current, and induced magnetic field in BeO molecules.
2008
It is predicted that oriented BeO molecules would give rise to unprecedentedly strong, unidirectional electric ring current and an associated magnetic field upon excitation by a right or left circularly polarized laser pulse into the first excited degenerate singlet state. The strong toroidal electric ring current of this state is dominated by the ring current of the 1π± orbital about the molecular axis. Our predictions are based on the analysis of the orbital composition of the states involved and are substantiated by high level electronic structure calculations and wavepacket simulations of the laser-driven orientation and excitation dynamics. Luis.Serrano@uv.es
Submicrometer in-plane integrated surface plasmon cavities.
2007
International audience; The optical properties of in-plane integrated surface plasmon polariton (SPP) cavities comprised of a thin film area sandwiched between two one-dimensional Bragg SPP mirrors are investigated numerically and experimentally. We discuss the resonance condition of these cavities, and we analyze in details the physical origin of the dispersion of this resonance. On the basis of numerical results, we show that in-plane SPP cavities can be used to achieve local SPP field enhancement and antireflecting SPP layers. The numerical results are compared to near-field optical images recorded by operating a photon scanning tunneling microscope. From the near-field images recorded o…
Communication: The pole structure of the dynamical polarizability tensor in equation-of-motion coupled-cluster theory.
2018
In this letter, we investigate the pole structure of dynamical polarizabilities computed within the equation-of-motion coupled-cluster (EOM-CC) theory. We show, both theoretically and numerically, that approximate EOM-CC schemes such as, for example, the EOM-CC singles and doubles model exhibit an incorrect pole structure in which the poles that reflect the excitations from the target state (i.e., the EOM-CC state) are supplemented by artificial poles due to excitations from the CC reference state. These artificial poles can be avoided by skipping the amplitude response and reverting to a sum-over-states formulation. While numerical results are generally in favor of such a solution, its maj…
Transition-Dipole Moments for Electronic Excitations in Strong Magnetic Fields Using Equation-of-Motion and Linear Response Coupled-Cluster Theory
2019
An implementation of transition-dipole moments at the equation-of-motion coupled-cluster singles-doubles (EOM-CCSD) and CCSD linear response (LR) levels of theory for the treatment of atoms and molecules in strong magnetic fields is presented. The presence of a finite magnetic field leads, in general, to a complex wave function and a gauge-origin dependence, necessitating a complex computer code together with the use of gauge-including atomic orbitals. As in the field-free case, for EOM-CC, the evaluation of transition-dipole moments consists of setting up the one-electron transition-density matrix (TDM) which is then contracted with dipole-moment integrals. In the case of CC-LR, the evalua…
Equation-of-motion coupled-cluster methods for atoms and molecules in strong magnetic fields.
2017
A program for the direct calculation of excitation energies of atoms and molecules in strong magnetic fields is presented. The implementation includes the equation-of-motion coupled-cluster singles-doubles (EOM-CCSD) method for electronically excited states as well as its spin-flip variant. Differences to regular EOM-CCSD implementations are due to the appearance of the canonical angular-momentum operator in the Hamiltonian causing the wave function to become complex. The gauge-origin problem is treated by the use of gauge-including atomic orbitals. Therefore, a modified Davidson method for diagonalizing complex non-Hermitian matrices is used. Excitation energies for selected atoms and mole…
A Lagrangian framework for deriving triples and quadruples corrections to the CCSD energy.
2014
Using the coupled cluster Lagrangian technique, we have determined perturbative corrections to the coupled cluster singles and doubles (CCSD) energy that converge towards the coupled cluster singles, doubles, and triples (CCSDT) and coupled cluster singles, doubles, triples, and quadruples (CCSDTQ) energies, considering the CCSD state as the unperturbed reference state and the fluctua- tion potential as the perturbation. Since the Lagrangian technique is utilized, the energy corrections satisfy Wigner’s 2n + 1 rule for the cluster amplitudes and the 2n + 2 rule for the Lagrange multi- pliers. The energy corrections define the CCSD perturbation series, CCSD(T–n) and CCSD(TQ–n), which are ter…
New Nuclear Magnetic Moment of Bi209 : Resolving the Bismuth Hyperfine Puzzle
2018
A recent measurement of the hyperfine splitting in the ground state of Li-like ${^{208}\mathrm{Bi}}^{80+}$ has established a ``hyperfine puzzle''---the experimental result exhibits a $7\ensuremath{\sigma}$ deviation from the theoretical prediction [J. Ullmann et al., Nat. Commun. 8, 15484 (2017); J. P. Karr, Nat. Phys. 13, 533 (2017)]. We provide evidence that the discrepancy is caused by an inaccurate value of the tabulated nuclear magnetic moment (${\ensuremath{\mu}}_{I}$) of $^{209}\mathrm{Bi}$. We perform relativistic density functional theory and relativistic coupled cluster calculations of the shielding constant that should be used to extract the value of ${\ensuremath{\mu}}_{I}(^{209…
Full Configuration-Interaction Study on the Tetrahedral Li4 Cluster
2008
International audience; The Li4 cluster low lying electronic states were studied. In particular we investigated the tetrahedral geometry at full CI and coupled cluster level, with basis sets of increasing quality. The 5A2 electronic state, characterized by having all the valence electrons unpaired, forming a quite stable no-pair bonding state, was studied in greater detail. In order to compare the energies we also studied the Li4 rhombus singlet ground state. The ability of coupled cluster with perturbative triples to correctly reproduce energy levels in a quasi-degenerate system was validated with respect to the full CI.