Quantum initial condition sampling for linearized density matrix dynamics: Vibrational pure dephasing of iodine in krypton matrices

This paper reviews the linearized path integral approach for computing time dependent properties of systems that can be approximated using a mixed quantum-classical description. This approach is applied to studying vibrational pure dephasing of ground state molecular iodine in a rare gas matrix. The Feynman-Kleinert optimized harmonic approximation for the full system density operator is used to sample initial conditions for the bath degrees of freedom. This extremely efficient approach is compared with alternative initial condition sampling techniques at low temperatures where classical initial condition sampling yields dephasing rates that are nearly an order of magnitude too slow compared with quantum initial condition sampling and experimental results.Comment: 20 pages and 8 figure

Predicting and verifying transition strengths from weakly bound molecules

We investigated transition strengths from ultracold weakly bound 41K87Rb molecules produced via the photoassociation of laser-cooled atoms. An accurate potential energy curve of the excited state (3)1Sigma+ was constructed by carrying out direct potential fit analysis of rotational spectra obtained via depletion spectroscopy. Vibrational energies and rotational constants extracted from the depletion spectra of v'=41-50 levels were combined with the results of the previous spectroscopic study, and they were used for modifying an ab initio potential. An accuracy of 0.14% in vibrational level spacing and 0.3% in rotational constants was sufficient to predict the large observed variation in transition strengths among the vibrational levels. Our results show that transition strengths from weakly bound molecules are a good measure of the accuracy of an excited state potential.Comment: 7 pages, 7 figure

Experimental evidence of thermal fluctuations on the X-ray absorption near-edge structure at the aluminum K-edge

After a review of temperature-dependent experimental x-ray absorption near-edge structure (XANES) and related theoretical developments, we present the Al K-edge XANES spectra of corundum and beryl for temperature ranging from 300K to 930K. These experimental results provide a first evidence of the role of thermal fluctuation in XANES at the Al K-edge especially in the pre-edge region. The study is carried out by polarized XANES measurements of single crystals. For any orientation of the sample with respect to the x-ray beam, the pre-edge peak grows and shifts to lower energy with temperature. In addition temperature induces modifications in the position and intensities of the main XANES features. First-principles DFT calculations are performed for both compounds. They show that the pre-edge peak originates from forbidden 1s to 3s transitions induced by vibrations. Three existing theoretical models are used to take vibrations into account in the absorption cross section calculations: i) an average of the XANES spectra over the thermal displacements of the absorbing atom around its equilibrium position, ii) a method based on the crude Born-Oppenheimer approximation where only the initial state is averaged over thermal displacements, iii) a convolution of the spectra obtained for the atoms at the equilibrium positions with an approximate phonon spectral function. The theoretical spectra so obtained permit to qualitatively understand the origin of the spectral modifications induced by temperature. However the correct treatment of thermal fluctuation in XANES spectroscopy requires more sophisticated theoretical tools

Ab initio Molecular Dynamics in Adaptive Coordinates

We present a new formulation of ab initio molecular dynamics which exploits the efficiency of plane waves in adaptive curvilinear coordinates, and thus provides an accurate treatment of first-row elements. The method is used to perform a molecular dynamics simulation of the CO_2 molecule, and allows to reproduce detailed features of its vibrational spectrum such as the splitting of the Raman sigma+_g mode caused by Fermi resonance. This new approach opens the way to highly accurate ab initio simulations of organic compounds.Comment: 11 pages, 3 PostScript figure

On the Prospects for Laser Cooling of TlF

We measure the upper state lifetime and two ratios of vibrational branching fractions f_{v'v} on the B^{3}\Pi_{1}(v') - X^{1}\Sigma^{+}(v) transition of TlF. We find the B state lifetime to be 99(9) ns. We also determine that the off-diagonal vibrational decays are highly suppressed: f_{01}/f_{00} < 2x10^{-4} and f_{02}/f_{00} = 1.10(6)%, in excellent agreement with their predicted values of f_{01}/f_{00} < 8x10^{-4} and f_{02}/f_{00} = 1.0(2)% based on Franck-Condon factors calculated using Morse and RKR potentials. The implications of these results for the possible laser cooling of TlF and fundamental symmetries experiments are discussed.Comment: 5 pages, 2 figure

Molecular Dipolar Crystals as High Fidelity Quantum Memory for Hybrid Quantum Computing

We study collective excitations of rotational and spin states of an ensemble of polar molecules, which are prepared in a dipolar crystalline phase, as a candidate for a high fidelity quantum memory. While dipolar crystals are formed in the high density limit of cold clouds of polar molecules under 1D and 2D trapping conditions, the crystalline structure protects the molecular qubits from detrimental effects of short range collisions. We calculate the lifetime of the quantum memory by identifying the dominant decoherence mechanisms, and estimate their effects on gate operations, when a molecular ensemble qubit is transferred to a superconducting strip line cavity (circuit QED). In the case rotational excitations coupled by dipole-dipole interactions we identify phonons as the main limitation of the life time of qubits. We study specific setups and conditions, where the coupling to the phonon modes is minimized. Detailed results are presented for a 1D dipolar chain

High-resolution Fourier-transform XUV photoabsorption spectroscopy of 14N15N

The first comprehensive high-resolution photoabsorption spectrum of 14N15N has been recorded using the Fourier-transform spectrometer attached to the Desirs beamline at the Soleil synchrotron. Observations are made in the extreme ultraviolet (XUV) and span 100,000-109,000 cm-1 (100-91.7 nm). The observed absorption lines have been assigned to 25 bands and reduced to a set of transition energies, f values, and linewidths. This analysis has verified the predictions of a theoretical model of N2 that simulates its photoabsorption and photodissociation cross section by solution of an isotopomer independent formulation of the coupled-channel Schroedinger equation. The mass dependence of predissociation linewidths and oscillator strengths is clearly evident and many local perturbations of transition energies, strengths, and widths within individual rotational series have been observed.Comment: 14 pages, 8 figures, one data archiv

Dynamics of Bulk vs. Nanoscale WS_2: Local Strain and Charging Effects

We measured the infrared vibrational properties of bulk and nanoparticle WS$_2$ in order to investigate the structure-property relations in these novel materials. In addition to the symmetry-breaking effects of local strain, nanoparticle curvature modifies the local charging environment of the bulk material. Performing a charge analysis on the \emph{xy}-polarized E$_{1u}$ vibrational mode, we find an approximate 1.5:1 intralayer charge difference between the layered 2H material and inorganic fullerene-like (IF) nanoparticles. This effective charge difference may impact the solid-state lubrication properties of nanoscale metal dichalcogenides.Comment: 6 pages, 5 figure

Strong fragmentation of low-energy electromagnetic excitation strength in 117^{117}Sn

Results of nuclear resonance fluorescence experiments on $^{117}$Sn are reported. More than 50 $\gamma$ transitions with $E_{\gamma} < 4$ MeV were detected indicating a strong fragmentation of the electromagnetic excitation strength. For the first time microscopic calculations making use of a complete configuration space for low-lying states are performed in heavy odd-mass spherical nuclei. The theoretical predictions are in good agreement with the data. It is concluded that although the E1 transitions are the strongest ones also M1 and E2 decays contribute substantially to the observed spectra. In contrast to the neighboring even $^{116-124}$Sn, in $^{117}$Sn the $1^-$ component of the two-phonon $[2^+_1 \otimes 3^-_1]$ quintuplet built on top of the 1/2$^+$ ground state is proved to be strongly fragmented.Comment: 4 pages, 3 figure

A new technique for elucidating β\beta-decay schemes which involve daughter nuclei with very low energy excited states

A new technique of elucidating $\beta$-decay schemes of isotopes with large density of states at low excitation energies has been developed, in which a Broad Energy Germanium (BEGe) detector is used in conjunction with coaxial hyper-pure germanium detectors. The power of this technique has been demonstrated on the example of 183Hg decay. Mass-separated samples of 183Hg were produced by a deposition of the low-energy radioactive-ion beam delivered by the ISOLDE facility at CERN. The excellent energy resolution of the BEGe detector allowed $\gamma$ rays energies to be determined with a precision of a few tens of electronvolts, which was sufficient for the analysis of the Rydberg-Ritz combinations in the level scheme. The timestamped structure of the data was used for unambiguous separation of $\gamma$ rays arising from the decay of 183Hg from those due to the daughter decays