We measure high resolution photoelectron angular distributions (PADs) for above-threshold ionization of xenon atoms in infrared laser fields. Based on the Ammosov-Delone-Krainov theory, we develop an intuitive quantum-trajectory Monte Carlo model encoded with Feynman's path-integral approach, in which the Coulomb effect on electron trajectories and interference patterns are fully considered. We achieve a good agreement with the measured PADs of atoms for above-threshold ionization. The quantum-trajectory Monte Carlo theory sheds light on the role of ionic potential on PADs along the longitudinal and transverse direction with respect to the laser polarization, allowing us to unravel the classical coordinates (i.e., tunneling phase and initial momentum) at the tunnel exit for all of the photoelectrons of the PADs. We study the classical-quantum correspondence and build a bridge between the above-threshold ionization and the tunneling theory.
In search of functional molecular materials and the study of their formation mechanism, we report the elucidation of a hierarchical step-by-step formation from monomer (Mn) to heptamer (Mn 7 ) to nonadecamer (Mn 19 ) satisfying the relation 1 + Σ n 6n, where n is the ring number of the Brucite structure using high-resolution electrospray ionization mass spectrometry (HRESI-MS). Three intermediate clusters, Mn 10 , Mn 12 , and Mn 14 , were identified. Furthermore, the Mn 19 disc remains intact when dissolved in acetonitrile with a well-resolved general formula of [Mn 19 (L) x (OH) y -(N 3 ) 36−x−y ] 2+ (x = 18, 17, 16; y = 8, 7, 6; HL = 1-(hydroxymethyl)-3,5-dimethylpyrazole) indicating progressive exchange of N 3 − for OH − . The high symmetry (R-3) Mn 19 crystal structure consists of a well-ordered discotic motif where the peripheral organic ligands form a double calix housing the anions and solvent molecules. From the formula and valence bond sums, the charge state is mixed-valent, [Mn II 15 Mn III 4 ]. Its magnetic properties and electrochemistry have been studied. It behaves as a ferrimagnet below 40 K and has a coercive field of 2.7 kOe at 1.8 K, which can be possible by either weak exchange between clusters through the anions and solvents or through dipolar interaction through space as confirmed by the lack of ordering in frozen CH 3 CN. The moment of nearly 50 Nμ B suggests Mn II −Mn II and Mn III −Mn III are ferromagnetically coupled while Mn II −Mn III is antiferromagnetic which is likely if the Mn III are centrally placed in the cluster. This compound displays the rare occurrence of magnetic ordering from nonconnected high-spin molecules.
The long-persistent phosphorescent metal-organic framework (MOF) is a kind of highly desirable but rare material. Here, two new molecular MOF materials, {[Zn(tipa)Cl]⋅NO3⋅2 DMF}n (1) and {[Cd2(tipa)2Cl4]⋅6 DMF}n (2) (tipa = tri(4-imidazolylphenyl)amine), which have 3D twofold interpenetrated (utp) and 2D noninterpenetrated (kgd) topologies, respectively, are reported. They exhibit unexpected long-persistent emissions yet reported: At 77 K, they persist in glowing after stopping the UV irradiation on a timescale up to seconds at 77 K, which can be detected by the naked eye (ca. 2 s). Compounds 1 and 2 also undergo single-crystal-to-single-crystal (SC-SC) transformations through different routes; a simple anion-exchange route for 1 and a complicated replacement of μ1-Cl(-) ions by DMF molecules accompanying I3(-) captured in the void for 2.
We measure photoelectron angular distributions of single ionization of krypton and xenon atoms by laser pulses at 1320 nm, 0.2-1.0×10(14) W/cm(2), and observe that the yield of near-zero-momentum electrons in the strong-field tunneling ionization regime is significantly suppressed. Semiclassical simulations indicate that this local ionization suppression effect can be attributed to a fraction of the tunneled electrons that are released in a certain window of the initial field phase and transverse velocity are ejected into Rydberg elliptical orbits with a frequency much smaller than that of the laser; i.e., the corresponding atoms are stabilized. These electrons with high-lying atomic orbits are thus prevented from ionization, resulting in the substantially reduced near-zero-momentum electron yield. The refined transition between the Rydberg states of the stabilized atoms has implication on the THz radiation from gas targets in strong laser fields.
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