Physics

We study frustrated double ionization in a strongly-driven heteronuclear molecule HeH + and compare with H 2 . We compute the probability distribution of the sum of the final kinetic energies of the nuclei for strongly-driven HeH + . We find that this distribution has more than one peak for strongly-driven HeH + , a feature we do not find to be present for strongly-driven H 2 . Moreover, we compute the probability distribution of the n quantum number of frustrated double ionization. We find that this distribution has several peaks for strongly-driven HeH + , while the respective distribution has one main peak and a "shoulder" at lower n quantum numbers for strongly-driven H 2 . Surprisingly, we find this feature to be a clear signature of the intertwined electron-nuclear motion.

We present experimental results on the sub-Doppler Rydberg spectroscopy of potassium in a hot cell and cold atoms, performed with two counter-propagating laser beams of 405 nm and 980 nm in the inverted ladder-type system (4S1/2-5P3/2-nS1/2 and nD3/2;5/2). Such an inverted ladder-type scheme is predicted to be without sub-Doppler electromagnetically induced transparency (EIT) feature in a thermal ensemble under the weak-probe approximation. Instead, we utilized a strong probe field and successfully observed a transparency window with a width narrower than 50~MHz. Our all-order numerical simulation is in satisfactory agreement with the experimental results. This narrow linewidth allows us to measure the energy levels of the Rydberg levels from n =20-70 with improved accuracy. The deduced ionization energy agrees with the previous measurements. Furthermore, the two-photon Rydberg excitation scheme was applied to the cold ensembles to study the ground-state atoms population decrease in the MOT for various Rydberg states. Our experimental observations suggested two distinct regimes of the trap losses under different probe detuning conditions. While the far off-resonance case (\delta p>>0) can be described by the picture of dressed atom, the on-resonance case (\delta p~0) reveals more interesting results. The higher Rydberg states suffer larger trap loss. Besides, even with similar level energies, the excitation to nD states result in faster escape of the ground-state atom from trap than nearby nS states.

Versatile quantum modes emerge for plasmon describing the collective oscillations of free electrons in metallic nanoparticles when the particle sizes are greatly reduced. Rather than traditional nanoscale study, the understanding of quantum plasmon desires extremal atomic control of the nanoparticles, calling for size dependent plasmon measurement over a series of nanoparticles with atomically adjustable atom number over several orders of magnitude. Here we report the N dependent plasmonic evolution of atomically size selected gold particles with N= 100 70000 using electron energy loss (EEL) spectroscopy in a scanning transmission electron microscope. The EEL mapping assigns a feature at 2.7 eV as the bulk plasmon and another at 2.4 eV as surface plasmon, which evolution reveals three regimes. When N decreases from 70000 to 887, the bulk plasmon stays unchanged while the surface plasmon exhibits a slight red shift from 2.4 to 2.3 eV. It can be understood by the dominance of classical plasmon physics and electron boundary scattering induced retardation. When N further decreases from 887 to 300, the bulk plasmon disappears totally and the surface plasmon shows a steady blueshift, which indicates that the quantum confinement emerges and modifies the intraband transition. When N 100 300, the plasmon is split to three fine features, which is attributed to superimposed single electron transitions between the quantized molecular like energy level by the time dependent density functional theory calculations. The surface plasmon's excitation ratio has a scaling law with an exponential dependence on N ( N^0.669), essentially the square of the radius. A unified evolution picture from the classical to quantum, molecular plasmon is thus demonstrated.

We investigate the contribution of Interatomic Coulombic Decay induced by ion impact in neon and argon dimers (Ne 2 and Ar 2 ) to the production of low energy electrons. Our experiments cover a broad range of perturbation strengths and reaction channels. We use 11.37 MeV/u S 14+ , 0.125 MeV/u He 1+ , 0.1625 MeV/u He 1+ and 0.150 MeV/u He 2+ as projectiles and study ionization, single and double electron transfer to the projectile as well as projectile electron loss processes. The application of a COLTRIMS reaction microscope enables us to retrieve the three-dimensional momentum vectors of the ion pairs of the fragmenting dimer into Ne q+ /Ne 1+ and Ar q+ /Ar 1+ (q = 1, 2, 3) in coincidence with at least one emitted electron.

The fragmentation times corresponding to the loss of the chromophore (C α -- C β bond dissociation channel) after photoexcitation at 263 nm have been investigated for several small peptides containing tryptophan or tyrosine. For tryptophan-containing peptides, the aromatic chromophore is lost as an ionic fragment (m/z 130), and the fragmentation time increases with the mass of the neutral fragment. In contrast, for tyrosine-containing peptides the aromatic chromophore is always lost as a neutral fragment (mass = 107 amu) and the fragmentation time is found to be fast (\textless{}20 ns). These different behaviors are explained by the role of the postfragmentation interaction in the complex formed after the C α --C β bond cleavage.

We report on studies of collisions between 3 keV Ar + projectile ions and neutral targets of isolated 1,3-butadiene (C 4 H 6 ) molecules and cold, loosely bound clusters of these molecules. We identify molecular growth processes within the molecular clusters that appears to be driven by knockout processes and that could result in the formation of (aromatic) ring structures. These types of reactions are not unique to specific projectile ions and target molecules, but will occur whenever atoms or ions with suitable masses and kinetic energies collide with aggregates of matter, such as carbonaceous grains in the interstellar medium or aerosol nanoparticles in the atmosphere.

We study the ionization dynamics of Ar clusters exposed to ultrashort near-infrared (NIR) laser pulses for intensities well below the threshold at which tunnel ionization ignites nanoplasma formation. We find that the emission of highly charged ions up to Ar 8+ can be switched on with unit contrast by generating only a few seed electrons with an ultrashort extreme ultraviolet (XUV) pulse prior to the NIR field. Molecular dynamics simulations can explain the experimental observations and predict a generic scenario where efficient heating via inverse bremsstrahlung and NIR avalanching are followed by resonant collective nanoplasma heating. The temporally and spatially well-controlled injection of the XUV seed electrons opens new routes for controlling avalanching and heating phenomena in nanostructures and solids, with implications for both fundamental and applied laser-matter science.

Large ammonia clusters represent a model system of ices which are omnipresent throughout the space. The interaction of ammonia ices with other hydrogen-boding molecules such as methanol or water and their behavior upon an ionization are thus relevant in the astrochemical context. In this study, ammonia clusters (NH3)N with the mean size N ~230 were prepared in molecular beams and passed through a pickup cell in which methanol molecules were adsorbed. At the highest exploited pickup pressures, the average composition of (NH3)N(CH3OH)M clusters was estimated to be N:M ~210:10. On the other hand, the electron ionization of these clusters yielded about 75% of methanol-containing fragments (NH3)n(CH3OH)mH+ compared to 25% contribution of pure ammonia (NH3)nH+ ions. Based on this substantial disproportion, we propose the following ionization mechanism: The prevailing ammonia is ionized in most cases, resulting in NH+4 core solvated most likely with four ammonia molecules, yielding the well-known "magic number" structure (NH3)4NH+4 . The methanol molecules exhibit strong propensity for sticking to the fragment ion. We have also considered mechanisms of intracluster reactions. In most cases, proton transfer between ammonia units take place. The theoretical calculations suggested the proton transfer either from the methyl group or from the hydroxyl group of the ionized methanol molecule to ammonia to be the energetically open channels. However, the experiments with selectively deuterated methanols did not show any evidence for the D+ transfer from the CD3 group. The proton transfer from the hydroxyl group could not be excluded entirely nor confirmed unambiguously by the experiment.

In the present work, we investigate the ionization of molecules of biological interest by the impact of multicharged ions in the intermediate to high energy range. We performed full non-perturbative distorted-wave calculations (CDW) for thirty-six collisional systems composed by six atomic targets: H, C, N, O, F, and S -which are the constituents of most of the DNA and biological molecules- and six charged projectiles (antiprotons, H, He, B, C, and O). On account of the radiation damage caused by secondary electrons, we inspect the energy and angular distributions of the emitted electrons from the atomic targets. We examine seventeen molecules: DNA and RNA bases, DNA backbone, pyrimidines, tetrahydrofuran (THF), and C n H n compounds. We show that the simple stoichiometric model (SSM), which approximates the molecular ionization cross sections as a linear combination of the atomic ones, gives reasonably good results for complex molecules. We also inspect the extensively used Toburen scaling of the total ionization cross sections of molecules with the number of weakly bound electrons. Based on the atomic CDW results, we propose new active electron numbers, which leads to a better universal scaling for all the targets and ions studied here in the intermediate to the high energy region. The new scaling describes well the available experimental data for proton impact, including small molecules. We perform full molecular calculations for five nucleobases and test a modified stoichiometric formula based on the Mulliken charge of the composite atoms. The difference introduced by the new stoichiometric formula is less than 3%, which indicates the reliability of the SSM to deal with this type of molecules. The results of the extensive ion-target examination included in the present study allow us to assert that the SSM and the CDW-based scaling will be useful tools in this area.

In processes when particles such as nanodroplets, clusters, or molecules move through a dilute background gas and undergo capture collisions, it is often important to know how much translational kinetic energy is deposited into the particles by these pick-up events. For sticking collisions with a Maxwell-Boltzmann gas, an exact expression is derived which is valid for arbitrary relative magnitudes of the particle and thermal gas speeds.