No Arabic abstract
We demonstrate detection of NaRb Feshbach molecules at high magnetic field by combining molecular photodissociation and absorption imaging of the photofragments. The photodissociation process is carried out via a spectroscopically selected hyperfine Zeeman level correlated with the Na ($3P_{3/2}$) + Rb ($5S_{1/2}$) asymptote which, following spontaneous emission and optical pumping, leads to ground-state atoms in a single level with near unity probability. Subsequent to the dissociation, the number of molecules is obtained by detecting the resultant $^{23}$Na and $^{87}$Rb atoms. We have also studied the heating effect caused by the photodissociation process and optimized the detection protocol for extracting the temperature of the molecular cloud. This method enables the $in~situ$ detection of fast time scale collision dynamics between NaRb Feshbach molecules and will be a valuable capability in studying few-body physics involving molecules.
The toolbox for imaging molecules is well-equipped today. Some techniques visualize the geometrical structure, others the electron density or electron orbitals. Molecules are many-body systems for which the correlation between the constituents is decisive and the spatial and the momentum distribution of one electron depends on those of the other electrons and the nuclei. Such correlations have escaped direct observation by imaging techniques so far. Here, we implement an imaging scheme which visualizes correlations between electrons by coincident detection of the reaction fragments after high energy photofragmentation. With this technique, we examine the H2 two-electron wave function in which electron-electron correlation beyond the mean-field level is prominent. We visualize the dependence of the wave function on the internuclear distance. High energy photoelectrons are shown to be a powerful tool for molecular imaging. Our study paves the way for future time resolved correlation imaging at FELs and laser based X-ray sources.
We demonstrate rather interesting manifestations of co-existence of resonance features in characteristics of the photoionization of 3d-electrons in Xe@C60. It is shown that the reflection of photoelectrons produced by the 3d Xe photoionization affects greatly partial photoionization cross-sections of and levels and respective angular anisotropy parameters, both dipole and non-dipole adding to all of them additional maximums and minimums. The calculations are performed treating the 3/2 and 5/2 electrons as electrons of different kinds with their spins up and down. The effect of C60 shell is accounted for in the frame of the orange skin potential model.
We use (1+1$$) resonance-enhanced multiphoton photodissociation (REMPD) to detect the population in individual rovibronic states of trapped HfF$^+$ with a single-shot absolute efficiency of 18%, which is over 200 times better than that obtained with fluorescence detection. The first photon excites a specific rotational level to an intermediate vibronic band at 35,000-36,500 cm$^{-1}$, and the second photon, at 37,594 cm$^{-1}$ (266 nm), dissociates HfF$^+$ into Hf$^+$ and F. Mass-resolved time-of-flight ion detection then yields the number of state-selectively dissociated ions. Using this method, we observe rotational-state heating of trapped HfF$^+$ ions from collisions with neutral Ar atoms. Furthermore, we measure the lifetime of the $^3Delta_1$ $v=0,, J=1$ state to be 2.1(2) s. This state will be used for a search for a permanent electric dipole moment of the electron.
We discuss the complicated resonance structure of the endohedral atom photoionization cross section. Very strong enhancement and interference patterns in the photoionization cross-section of the valent and subvalent subshells of noble gas endohedral atoms A@C60 are demonstrated. It is shown also that the atomic Giant resonance can be either completely destroyed or remains almost untouched depending on the velocity of photoelectrons that are emitted in the resonances decay process. These effects are results of dynamic modification of the incoming beam of radiation due to polarization of the fullerenes electron shell and reflection of photoelectrons be the fullerenes shell static potential. We have considered the outer np- and subvalent ns-subshells for Ne, Ar, Kr and Xe noble gas atoms. The modification of the Giant resonances is considered for a whole sequence of endohedrals with atoms and ions Xe, Ba, La, Ce+, Ce+4, Eu. The polarization of the fullerene shell is expressed via the total photoabsorption cross section. The photoelectron reflection from the static potential is taken into account in the frame of the so-called bubble potential that is a spherical -type potential.
The reversible control of a single spin of an atom or a molecule is of great interest in Kondo physics and a potential application in spin based electronics.Here we demonstrate that the Kondo resonance of manganese phthalocyanine molecules on an Au(111) substrate have been reversibly switched off and on via a robust route through attachment and detachment of single hydrogen atom to the magnetic core of the molecule. As further revealed by density functional theory calculations, even though the total number of electrons of the Mn ion remains almost the same in the process, gaining one single hydrogen atom leads to redistribution of charges within 3d orbitals with a reduction of the molecular spin state from S = 3/2 to S = 1 that directly contributes to the Kondo resonance disappearance. This process is reversed by a local voltage pulse or thermal annealing to desorb the hydrogen atom.