Control and femtosecond time-resolved imaging of torsion in a chiral molecule

We study how the combination of long and short laser pulses can be used to induce torsion in an axially chiral biphenyl derivative (3,5-difluoro-3 ,5 -dibromo-4 -cyanobiphenyl). A long, with respect to the molecular rotational periods, elliptically polarized laser pulse produces 3D alignment of the molecules, and a linearly polarized short pulse initiates torsion about the stereogenic axis. The torsional motion is monitored in real-time by measuring the dihedral angle using femtosecond time-resolved Coulomb explosion imaging. Within the first 4 picoseconds (ps), torsion occurs with a period of 1.25 ps and an amplitude of 3◦ in excellent agreement with theoretical calculations. At larger times, the quantum states of the molecules describing the torsional motion dephase and an almost isotropic distribution of the dihedral angle is measured.We demonstrate an original application of covariance analysis of two-dimensional ion images to reveal strong correlations between specific ejected ionic fragments from Coulomb explosion. This technique strengthens our interpretation of the experimental data

Deformation of Gabor systems

We introduce a new notion for the deformation of Gabor systems. Such deformations are in general nonlinear and, in particular, include the standard jitter error and linear deformations of phase space. With this new notion we prove a strong deformation result for Gabor frames and Gabor Riesz sequences that covers the known perturbation and deformation results. Our proof of the deformation theorem requires a new characterization of Gabor frames and Gabor Riesz sequences. It is in the style of Beurling's characterization of sets of sampling for bandlimited functions and extends significantly the known characterization of Gabor frames 'without inequalities' from lattices to non-uniform sets.

Probing quantum gravity using photons from a flare of the active galactic nucleus Markarian 501 observed by the MAGIC telescope

We analyze the timing of photons observed by the MAGIC telescope during a flare of the active galactic nucleus Mkn 501 for a possible correlation with energy, as suggested by some models of quantum gravity (QG), which predict a vacuum refractive index similar or equal to 1 + (E/M-QGn)(n), n = 1, 2. Parametrizing the delay between gamma-rays of different energies as Delta t = +/-tau E-1 or Delta t = +/-tau E-q(2), we find tau(1) = (0.030 +/- 0.012) s/GeV at the 2.5-sigma level, and tau(q) = (3.71 +/- 2.57) x 10(-6) s/GeV2, respectively. We use these results to establish lower limits M-QG1 > 0.21 X 10(18) GeV and M-QG2 > 0.26 x 10(11) GeV at the 95% C.L. Monte Carlo studies confirm the MAGIC sensitivity to propagation effects at these levels. Thermal plasma effects in the source are negligible, but we cannot exclude the importance of some other source effect.

Quantum magnetic deflagration in Mn12 acetate

We report controlled ignition of magnetization reversal avalanches by surface acoustic waves in a single crystal of Mn12 acetate. Our data show that the speed of the avalanche exhibits maxima on the magnetic field at the tunneling resonances of Mn12. Combined with the evidence of magnetic deflagration in Mn12 acetate [Y. Suzuki et al., Phys. Rev. Lett. 95, 147201 (2005)], this suggests a novel physical phenomenon: deflagration assisted by quantum tunneling.

Characterization and quantification of polyradical character

The decomposition of 〈͈Ŝ²〉 into atomic and diatomic contributions (local spin analysis) is used to detect and quantify the polyradical character of molecular systems. A model triradical system is studied in detail, and the local spin analysis is used to distinguish several patterns of local spin distributions and spin-spin interactions that can be found for different electronic states. How close a real molecular system is to an ideal system of k perfectly localized spin centers is utilized to define a measure of its k-radical character. The spin properties and triradical character of the lowest-lying electronic states of a number of all σ, all π, and σ-π organic triradicals are discussed in detail. The local spin contributions exhibit good correlation with experimental triradical stabilization energies

New approximation to the third-order density : application to the calculation of correlated multicenter indices

In this work we present the formulas for the calculation of exact three-center electron sharing indices (3c-ESI) and introduce two new approximate expressions for correlated wave functions. The 3c-ESI uses the third-order density, the diagonal of the third-order reduced density matrix, but the approximations suggested in this work only involve natural orbitals and occupancies. In addition, the first calculations of 3c-ESI using Valdemoro's, Nakatsuji's and Mazziotti's approximation for the third-order reduced density matrix are also presented for comparison. Our results on a test set of molecules, including 32 3c-ESI values, prove that the new approximation based on the cubic root of natural occupancies performs the best, yielding absolute errors below 0.07 and an average absolute error of 0.015. Furthemore, this approximation seems to be rather insensitive to the amount of electron correlation present in the system. This newly developed methodology provides a computational inexpensive method to calculate 3c-ESI from correlated wave functions and opens new avenues to approximate high-order reduced density matrices in other contexts, such as the contracted Schrödinger equation and the anti-Hermitian contracted Schrödinger equation

Finite-temperature T matrix in a real-time formalism

A generalized off-shell unitarity relation for the two-body scattering T matrix in a many-body medium at finite temperature is derived, through a consistent real-time perturbation expansion by means of Feynman diagrams. We comment on perturbation schemes at finite temperature in connection with an erroneous formulation of the Dyson equation in a paper recently published.

Minimum-uncertaity states and pseudoclassical dynamics. II

The set of initial conditions for which the pseudoclassical evolution algorithm (and minimality conservation) is verified for Hamiltonians of degrees N (N>2) is explicitly determined through a class of restrictions for the corresponding classical trajectories, and it is proved to be at most denumerable. Thus these algorithms are verified if and only if the system is quadratic except for a set of measure zero. The possibility of time-dependent a-equivalence classes is studied and its physical interpretation is presented. The implied equivalence of the pseudoclassical and Ehrenfest algorithms and their relationship with minimality conservation is discussed in detail. Also, the explicit derivation of the general unitary operator which linearly transforms minimum-uncertainty states leads to the derivation, among others, of operators with a general geometrical interpretation in phase space, such as rotations (parity, Fourier).

Excitation modes of vortices in submicron magnetic disks

Classical and quantum theory of spin waves in the vortex state of a mesoscopic submicron magnetic disk have been developed with account of the finite mass density of the vortex. Oscillations of the vortex core resemble oscillations of a charged string in a potential well in the presence of the magnetic field. A conventional gyrotropic frequency appears as a gap in the spectrum of spin waves of the vortex. The mass of the vortex has been computed, and the result agrees with experimental findings. The finite vortex mass generates a high-frequency branch of spin waves. The effects of an external magnetic field and dissipation have been addressed.