Photoionizaton of Pure and Doped Helium Nanodroplets

Helium nanodroplets, commonly regarded as the "nearly ideal spectroscopic matrix", are being actively studied for more than two decades now. While they mostly serve as cold, weakly perturbing and transparent medium for high-resolution spectroscopy of embedded molecules, their intrinsic quantum properties such as microscopic superfluidity still are subject-matter of current research. This article reviews recent work on pure and doped He nanodroplets using PI spectroscopy, an approach which has greatly advanced in the past years. While the notion of the ideal spectroscopic matrix mostly no longer holds in this context, photoionization techniques provide detailed insights into the photo-physical properties of pure and doped He nanodroplets and their relaxation dynamics following electronic excitation. Exploiting nowadays available high laser fields, even highly ionized states of matter on the nanoscale can be formed. Our particular focus lies on recent experimental progress including fs time-resolved spectroscopy, photoion and electron imaging, and novel sources of highly energetic radiation.Comment: accepted by International Reviews in Physical Chemistr

Dynamics of solvation and desolvation of rubidium attached to He nanodroplets

The real-time dynamics of photoexcited and photoionized rubidium (Rb) atoms attached to helium (He) nanodroplets is studied by femtosecond pump-probe mass spectrometry. While excited Rb atoms in the perturbed 6p-state (Rb*) desorb off the He droplets, Rb^+ photoions tend to sink into the droplet interior when created near the droplet surface. The transition from Rb^+ solvation to full Rb* desorption is found to occur at a delay time t~600 fs for Rb* in the 6pSigma-state and t~1200 fs for the 6pPi-state. Rb^+He ions are found to be created by directly exciting bound Rb*He exciplex states as well as by populating bound Rb^+He-states in an photoassociative ionization process.Comment: accepted by J. Chem. Phy

A compact design for velocity-map imaging energetic electrons and ions

We present a compact design for a velocity-map imaging spectrometer for energetic electrons and ions. The standard geometry by Eppink and Parker [A. T. J. B. Eppink and D. H. Parker, Rev. Sci. Instrum. 68, 3477 (1997)] is augmented by just two extended electrodes so as to realize an additional einzel lens. In this way, for a maximum electrode voltage of 7 kV we experimentally demonstrate imaging of electrons with energies up to 65 eV. Simulations show that energy acceptances of <270 and <1,200 eV with an energy resolution of dE / E <5% are achievable for electrode voltages of <20 kV when using diameters of the position-sensitive detector of 42 and 78 mm, respectively

Formation and relaxation of RbHe exciplexes on He nanodroplets studied by femtosecond pump and picosecond probe spectroscopy

Vibrationally resolved photoionization spectra of RbHe exciplexes forming on He nanodroplets are recorded using femtosecond pump-probe spectroscopy with amplitude-shaped probe pulses. The time-evolution of the spectra reveals an exciplex formation time ~10ps followed by vibrational relaxation extending up to >1ns. This points to an indirect, time-delayed desorption process of RbHe off the He surface

Efficiency of Dopant-Induced Ignition of Helium Nanoplasmas

Helium nanodroplets irradiated by intense near-infrared laser pulses ignite and form highly ionized nanoplasmas even at laser intensities where helium is not directly ionized by the optical field, provided the droplets contain a few dopant atoms. We present a combined theoretical and experimental study of the He nanoplasma ignition dynamics for various dopant species. We find that the efficiency of dopants to ignite a nanoplasma in helium droplets strongly varies and mostly depends on (i) the pick-up process, (ii) the number of free electrons each dopant donates upon ionization, and remarkably, (iii) by the hitherto unexplored effect of the dopant location in or on the droplet

Atom-molecule collisions in an optically trapped gas

Cold inelastic collisions between confined cesium (Cs) atoms and Cs$\_2$ molecules are investigated inside a CO$\_2$ laser dipole trap. Inelastic atom-molecule collisions can be observed and measured with a rate coefficient of $\sim 2.5 \times 10^{-11}$cm$^3$ s$^{-1}$, mainly independent of the molecular ro-vibrational state populated. Lifetimes of purely atomic and molecular samples are essentially limited by rest gas collisions. The pure molecular trap lifetime ranges 0,3-1 s, four times smaller than the atomic one, as is also observed in a pure magnetic trap. We give an estimation of the inelastic molecule-molecule collision rate to be $\sim 10^{-11}$ cm$^{3}$ s$^{-1}$

Kilohertz laser ablation for doping helium nanodroplets

A new setup for doping helium nanodroplets by means of laser ablation at kilohertz repetition rate is presented. The doping process is characterized and two distinct regimes of laser ablation are identified. The setup is shown to be efficient and stable enough to be used for spectroscopy, as demonstrated on beam-depletion spectra of lithium atoms attached to helium nanodroplets. For the first time, helium droplets are doped with high temperature refractory materials such as titanium and tantalum. Doping with the non-volatile DNA basis Guanine is found to be efficient and a number of oligomers are detected

Mixture of ultracold lithium and cesium atoms in an optical dipole trap

We present the first simultaneous trapping of two different ultracold atomic species in a conservative trap. Lithium and cesium atoms are stored in an optical dipole trap formed by the focus of a CO$_2$ laser. Techniques for loading both species of atoms are discussed and observations of elastic and inelastic collisions between the two species are presented. A model for sympathetic cooling of two species with strongly different mass in the presence of slow evaporation is developed. From the observed Cs-induced evaporation of Li atoms we estimate a cross section for cold elastic Li-Cs collisions.Comment: 10 pages 9 figures, submitted to Appl. Phys. B; v2: Corrected evaporation formulas and some postscript problem

Sympathetic Cooling of Lithium by Laser-cooled Cesium

We present first indications of sympathetic cooling between two neutral, optically trapped atomic species. Lithium and cesium atoms are simultaneously stored in an optical dipole trap formed by the focus of a CO$_2$ laser, and allowed to interact for a given period of time. The temperature of the lithium gas is found to decrease when in thermal contact with cold cesium. The timescale of thermalization yields an estimate for the Li-Cs cross-section.Comment: 4 pages, proceedings of ICOLS 200

Desorption Dynamics of Heavy Alkali Metal Atoms (Rb, Cs) off the Surface of Helium Nanodroplets

We present a combined ion imaging and density functional theory study of the dynamics of the desorption process of rubidium and cesium atoms off the surface of helium nanodroplets upon excitation of the perturbed $6s$ and $7s$ states, respectively. Both experimental and theoretical results are well represented by the pseudodiatomic model for effective masses of the helium droplet in the desorption reaction of m_eff/m_He~10 (Rb) and 13 (Cs). Deviations from this model are found for Rb excited to the 6p state. Photoelectron spectra indicate that the dopant-droplet interaction induces relaxation into low-lying electronic states of the desorbed atoms in the course of the ejection process.Comment: in press, J. Phys. Chem. A (2014