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The relaxation of photoexcited nanosystems is a fundamental process of light–matter interaction. Depending on the couplings of the internal degrees of freedom, relaxation can be ultrafast, converting electronic energy in a few fs, or slow, if the energy is trapped in a metastable state that decouples from its environment. Here, we study helium nanodroplets excited resonantly by femtosecond extreme-ultraviolet (XUV) pulses from a seeded free-electron laser. Despite their superfluid nature, we find that helium nanodroplets in the lowest electronically excited states undergo ultrafast relaxation. By comparing experimental photoelectron spectra with time-dependent density functional theory simulations, we unravel the full relaxation pathway: Following an ultrafast interband transition, a void nanometer-sized bubble forms around the localized excitation (He∗) within 1 ps. Subsequently, the bubble collapses and releases metastable He∗ at the droplet surface. This study highlights the high level of detail achievable in probing the photodynamics of nanosystems using tunable XUV pulses., Funding from the Deutsche Forschungsgemeinschaft (MU 2347/8-1, STI 125/19-1, and the priority program 1840 QUTIF, the Carlsberg Foundation, National Science Foundation (DMR-1828019), Carl-Zeiss-Stiftung, Grant No. FIS2017-87801-P (AEI/FEDER, UE), and Swiss National Science Foundation (200020_162434) is gratefully acknowledged. O.G., D.M.N., and M.P.Z. were supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division, through Contract No. DE-AC02-05CH11231.

Clusters and nanodroplets hold the promise of enhancing high-order nonlinear optical effects due to their high local density. However, only moderate enhancement has been demonstrated to date. Here, we report the observation of energetic electrons generated by above-threshold ionization (ATI) of helium (He) nanodroplets which are resonantly excited by ultrashort extreme ultraviolet (XUV) free-electron laser pulses and subsequently ionized by near-infrared (NIR) or near-ultraviolet (UV) pulses. The electron emission due to high-order ATI is enhanced by several orders of magnitude compared with He atoms. The crucial dependence of the ATI intensities with the number of excitations in the droplets suggests a local collective enhancement effect.

We report on the observation of time-resolved quantum beats in the helium fluorescence from the transition 1s3p -> 1s2s, where the initial state is excited by XUV free-electron laser radiation. The quantum beats originate from the Zeeman splitting of the magnetic substates due to an external magnetic field. We perform a systematic study of this effect and discuss the possibilities of studying this phenomenon in the XUV and x-ray regime., 7 pages, 4 figures

We present the first measurements of photoelectron spectra of atomic clusters embedded in superfluid helium (He) nanodroplets. Owing to the large absorption cross section of xenon (Xe) around 100 eV photon energy (4d inner-shell ionization), direct dopant photoionization exceeds charge transfer ionization via the ionized He droplets. Despite the predominant creation of Xe^2+ and Xe^3+ by subsequent Auger decay of free Xe atoms, for Xe embedded in He droplets only singly charged Xe_k^+, k=1,2,3 fragments are observed. Broad Xe^+ ion kinetic-energy distributions indicate Coulomb explosion of the ions due to electron transfer to the primary Auger ions from surrounding neutral atoms. The electron spectra correlated with Xe ions emitted from the He nanodroplets contain a low-energy feature and nearly unshifted Xe photolines. These results pave the way to extreme ultraviolet (XUV) and x-ray photoelectron spectroscopy of clusters and molecular complexes embedded in He nanodroplets.

We present the first measurement of a one-photon extreme-ultraviolet photoelectron spectrum (PES) of molecules embedded in superfluid helium nanodroplets. The PES of coronene is compared to gas phase and the solid phase PES, and to electron spectra of embedded coronene generated by charge transfer and Penning ionization through ionized or excited helium. The resemblence of the He-droplet PES to the one of the solid phase indicates that mostly Cor clusters are photoionized. In contrast, the He-droplet Penning-ionization electron spectrum is nearly structureless, indicating strong perturbation of the ionization process by the He droplet. These results pave the way to extreme ultraviolet photoelectron spectroscopy (UPS) of clusters and molecular complexes embedded in helium nanodroplets. We present the first measurement of a one-photon extreme-ultraviolet photoelectron spectrum (PES) of molecules embedded in superfluid helium nanodroplets. The PES of coronene is compared to gas phase and the solid phase PES, and to electron spectra of embedded coronene generated by charge transfer and Penning ionization through ionized or excited helium. The resemblence of the He-droplet PES to the one of the solid phase indicates that mostly Cor clusters are photoionized. In contrast, the He-droplet Penning-ionization electron spectrum is nearly structureless, indicating strong perturbation of the ionization process by the He droplet. These results pave the way to extreme ultraviolet photoelectron spectroscopy (UPS) of clusters and molecular complexes embedded in helium nanodroplets

Abstract: We have studied the dynamic evolution of a Cs atom photo-excited from 6s to 6p and 7s states on a helium droplet using time-dependent 4 He-DFT simulations. Depending on the excited electronic state, the Cs impurity remains on the droplet surface or it is ejected. Upon subsequent photo-ionization of the excited Cs atom the resulting Cs + cation may either be ejected or come back to the droplet, depending on the time delay between photo-excitation and photo-ionization. We have calculated the critical time delay separating these two different behaviors, as well as final ion velocities. These observables will be used for future comparison with planned pump-probe experiments. Graphical abstract: [Figure not available: see fulltext.].

Helium nanodroplets are a unique system of quantum fluid clusters possessing several intriguing properties. From the perspective of atomic systems, they have been predominantly viewed as a spectroscopic matrix hosting other molecules and systems of interest. In this report, we draw particular attention to select electronic processes in He aggregates hosting other atoms, in particular, Rb. From this perspective, we present the details of single- and multi-electron processes occurring in this alkali-He system interacting with single extreme ultraviolet and soft X-ray photons. The features brought out in this study are generic and pertinent to systems with similar design on the atomic scale.

The desorption dynamics of rubidium dimers (Rb_2) off the surface of helium nanodroplets induced by laser excitation is studied employing both nanosecond and femtosecond ion imaging spectroscopy. Similarly to alkali metal atoms, we find that the Rb_2 desorption process resembles the dissociation of a diatomic molecule. However, both angular and energy distributions of detected Rb_2^+ ions appear to be most crucially determined by the Rb_2 intramolecular degrees of freedom rather than by those of the Rb_2He_N complex. The pump-probe dynamics of Rb_2^+ is found to be slower than that of Rb^+ pointing at a weaker effective guest-host repulsion for excited molecules than for single atoms., accepted by J. Phys. Chem. A (2016)

Acene molecules (anthracene, tetracene, pentacene) and fullerene (C$_{60}$) are embedded in He nanodroplets (He$_N$) and probed by EUV synchrotron radiation. When resonantly exciting the He nanodroplets, the embedded molecules M are efficiently ionized by the Penning reaction $\mathrm{He}_N^*+\mathrm{M}\rightarrow\mathrm{He}_N + \mathrm{M}^+ + e^-$. However, the Penning electron spectra are broad and structureless -- showing no resemblance neither with those measured by binary Penning collisions, nor with those measured for dopants bound to the He droplet surface. The similarity of all four spectra indicates that electron spectra of embedded species are substantially altered by electron-He scattering. Simulations based on elastic binary electron-He collisions qualitatively reproduce the measured spectra, but require the assumption of unexpectedly large He droplets.

The desorption of excited rubidium (Rb) atoms off the surface of helium (He) nanodroplets is studied in detail using femtosecond time-resolved photoion and photoelectron imaging spectroscopy in combination with quantum wave packet simulations. The good agreement of the measured time-dependent velocity distributions with the simulation when exciting the Rb dopant atoms into the 6p-state supports the pseudo-diatomic model (PDM) for the Rb-He droplet interaction, even on the level of quantum wave packet dynamics. Time-resolved photoelectron spectra reveal the partitioning of excitation energy into the dopant and the droplet degrees of freedom.

Phase-modulated wave-packet interferometry is combined with mass-resolved photoion detection to investigate rubidium atoms attached to helium nanodroplets in a molecular beam experiment. The spectra of atomic Rb electronic states show a vastly enhanced sensitivity and spectral resolution when compared to conventional pump-probe wave-packet interferometry. Furthermore, the formation of Rb*He exciplex molecules is probed and for the first time a fully resolved vibrational spectrum for transitions between the lowest excited $5\Pi_{3/2}$ and the high-lying electronic states $2^2\Pi$, $4^2\Delta$, $6^2\Sigma$ is obtained and compared to theory. The feasibility of applying coherent multidimensional spectroscopy to dilute cold gas phase samples is demonstrated in these experiments.

Interatomic Coulombic decay (ICD) is induced in helium nanodroplets by photoexciting the $n=2$ excited state of ${\mathrm{He}}^{+}$ using XUV synchrotron radiation. By recording multiple-coincidence electron and ion images we find that ICD occurs in various locations at the droplet surface, inside the surface region, or in the droplet interior. ICD at the surface gives rise to energetic ${\mathrm{He}}^{+}$ ions as previously observed for free He dimers. ICD deeper inside leads to the ejection of slow ${\mathrm{He}}^{+}$ ions due to Coulomb explosion delayed by elastic collisions with neighboring He atoms, and to the formation of ${\mathrm{He}}_{k}{}^{+}$ complexes.

We describe an experimental setup comprised of a discharge source for supersonic beams of metastable helium atoms and a magneto-optical trap (MOT) for ultracold lithium atoms that makes it possible to study Penning ionization and associative ionization processes at high ion count rates. The cationic reaction products are analyzed using a novel ion detection scheme which allows for mass selection, a high ion extraction efficiency and a good collision-energy resolution. The influence of elastic He-Li collisions on the steady-state Li atom number in the MOT is described, and the collision data are used to estimate the excitation efficiency of the discharge source. We also show that Penning collisions can be directly used to probe the temperature of the Li cloud without the need for an additional time-resolved absorption or fluorescence detection system., accepted by J. Chem. Phys. (Dec. 2018)

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.

We present a combined experimental and theoretical study of the charging dynamics of helium nanodroplets doped with atoms of different species and irradiated by intense near-infrared (NIR) laser pulses (

Here, we report the observation of electron transfer mediated decay (ETMD) involving Mg clusters embedded in helium nanodroplets which is initiated by the ionization of helium followed by removal of two electrons from the Mg clusters of which one is transferred to the He environment neutralizing it while the other electron is emitted into the continuum. The process is shown to be the dominant ionization mechanism for embedded clusters for photon energies above the ionization potential of He. The photoelectron spectrum reveals a low energy ETMD peak. For Mg clusters larger than 5 atoms we observe stable doubly-ionized clusters. We argue that ETMD provides a new pathway to the formation of doubly-ionized cold species., 5 pages submitted to Phys. Rev. Lett

Femtosecond pump–probe spectroscopy has been used to study vibrational dynamics of potassium dimers attached to superfluid helium nanodroplets. Comparing the measured data with theoretical results based on dissipative quantum dynamics we propose that the most important effect of the helium environment is a general damping of the vibrational dynamics. The calculations allow us to explain crucial experimental findings that are unobserved in gas phase measurements. Remarkably, wave packet velocities of such alkali dimer vibrations are just about in the range of the Landau critical velocity of superfluid helium. We therefore also discuss a possible influence of superfluidity on the induced wave packet dynamics.

The stability of two-component clusters consisting of light (Na or K) and heavy (Rb or Cs) alkali atoms formed on helium nanodroplets is studied by femtosecond laser ionization in combination with mass spectrometry. Characteristic stability patterns reflecting electron shell-closures are observed in dependence of the total number of atoms contained in the mixed clusters. Faster decay of the stability of mixed clusters compared to the pure light ones as a function of size indicates a destabilizing effect of heavy alkali atoms on light alkali clusters, presumably due to second order spin-orbit interaction.

Helium nanodroplets are widely used as a cold, weakly interacting matrix for spectroscopy of embedded species. In this work, we excite or ionize doped He droplets using synchrotron radiation and study the effect onto the dopant atoms depending on their location inside the droplets (rare gases) or outside at the droplet surface (alkali metals). Using photoelectron-photoion coincidence imaging spectroscopy at variable photon energies (20-25 eV), we compare the rates of charge-transfer to Penning ionization of the dopants in the two cases. The surprising finding is that alkali metals, in contrast to the rare gases, are efficiently Penning ionized upon excitation of the (n = 2)-bands of the host droplets. This indicates rapid migration of the excitation to the droplet surface, followed by relaxation, and eventually energy transfer to the alkali dopants.

Ionization dynamics of resonantly excited helium nanodroplets have been studied by intense XUV light. By doping the nanodroplets with atoms that either attach to the surface or submerge into the center of the droplet, one can study the dynamics of excitation and ionization through the droplet. When resonantly exciting the droplet, we observe a strong ionization enhancement for atoms attached to the surface. On the other hand, atoms embedded inside the nanodroplet are less efficiently ionized. We attribute this effect to an ultrafast energy transfer to the surface of the droplet and subsequent Penning ionization of the surface-bound dopant.

The predissociation dynamics of lithium iodide (LiI) in the first excited A-state is investigated for molecules in the gas phase and embedded in helium nanodroplets, using femtosecond pump-probe photoionization spectroscopy. In the gas phase, the transient Li(+) and LiI(+) ion signals feature damped oscillations due to the excitation and decay of a vibrational wave packet. Based on high-level ab initio calculations of the electronic structure of LiI and simulations of the wave packet dynamics, the exponential signal decay is found to result from predissociation predominantly at the lowest avoided X-A potential curve crossing, for which we infer a coupling constant VXA = 650(20) cm(-1). The lack of a pump-probe delay dependence for the case of LiI embedded in helium nanodroplets indicates fast droplet-induced relaxation of the vibrational excitation.

We present a comprehensive analysis of autoionization processes in Ne clusters (similar to 5000 atoms) after multiple valence excitations by free electron laser radiation. The evolution from 2-body interatomic Coulombic decay (ICD) to 3-body ICD is demonstrated when changing from surface to bulk Frenkel exciton excitation. Super Coster-Kronig type 2-body ICD is observed at Wannier exciton which quenches the main ICD channel.

The dynamics of vibrational wave packets excited in K$_2$ dimers attached to superfluid helium nanodroplets is investigated by means of femtosecond pump-probe spectroscopy. The employed resonant three-photon-ionization scheme is studied in a wide wavelength range and different pathways leading to K$^+_2$-formation are identified. While the wave packet dynamics of the electronic ground state is not influenced by the helium environment, perturbations of the electronically excited states are observed. The latter reveal a strong time dependence on the timescale 3-8 ps which directly reflects the dynamics of desorption of K$_2$ off the helium droplets.

Cold alkali diatomic molecules (LiCs, NaCs) in the lowest vibrational state of the electronic triplet ground state are formed on superfluid helium nanodroplets. Using photoionization detection the excitation spectra of the $2^3\Pi \leftarrow 1^3\Sigma^ + $ transitions are recorded. The splitting of the vibrational structure in the LiCs spectrum, not observed in the NaCs spectrum, is interpreted in terms of molecular fine structure. The spectra are well reproduced by a model based on quantum chemistry potential curves including spin-orbit coupling, in combination with an asymmetric line shape function to account for cluster-induced broadening. Our refined potential curves provide important input data for the photoassociation of ultracold dipolar alkali molecules from atomic quantum gases.

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)

Free electron lasers (FELs) offer the unprecedented capability to study reaction dynamics and image the structure of complex systems. When multiple photons are absorbed in complex systems, a plasma-like state is formed where many atoms are ionized on a femtosecond timescale. If multiphoton absorption is resonantly-enhanced, the system becomes electronically-excited prior to plasma formation, with subsequent decay paths which have been scarcely investigated to date. Here, we show using helium nanodroplets as an example that these systems can decay by a new type of process, named collective autoionization. In addition, we show that this process is surprisingly efficient, leading to ion abundances much greater than that of direct single-photon ionization. This novel collective ionization process is expected to be important in many other complex systems, e.g. macromolecules and nanoparticles, exposed to high intensity radiation fields.

Elastic scattering cross sections are measured for lithium atoms colliding with rare-gas atoms and SF${}_{6}$ molecules at tunable relative velocities down to $\ensuremath{\sim}$50 m/s. Our scattering apparatus combines a velocity-tunable molecular beam with a magneto-optic trap which provides an ultracold cloud of lithium atoms as a scattering target. Comparison with theory reveals the quantum nature of the collision dynamics in the studied regime, including rainbows as well as orbiting resonances.

The ultra-fast dynamics of He nanodroplets (103–105 atoms) in intense (1…7 ×1014 W/cm2), few-cycle (∼10 fs), infrared (∼790 nm) laser pulses has been investigated as a function of the number of dopant rare-gas atoms, the laser intensity and the rare-gas species. We find the “ignition” behaviour predicted by theory for 20 fs resulting in the complete ionisation and disintegration of the droplet, otherwise entirely transparent, initiated by just a few, less than 5 dopant atoms.

The vibrational wave-packet dynamics of diatomic rubidium molecules (Rb2) in triplet states formed on the surface of superfluid helium nanodroplets is investigated both experimentally and theoretically. Detailed comparison of experimental femtosecond pump–probe spectra with dissipative quantum dynamics simulations reveals that vibrational relaxation is the main source of dephasing. The rate constant for vibrational relaxation in the first excited triplet state 13Σ+g is found to be constant γ ≈ 0.5 ns−1 for the lowest vibrational levels v [less, similar] 15 and to increase sharply when exciting to higher energies. Dieser Beitrag ist mit Zustimmung des Rechteinhabers aufgrund einer (DFG-geförderten) Allianz- bzw. Nationallizenz frei zugänglich.

We demonstrate ultrafast resonant energy absorption of rare-gas doped He nanodroplets from intense few-cycle (~10 fs) laser pulses. We find that less than 10 dopant atoms "ignite" the droplet to generate a non-spherical electronic nanoplasma resulting ultimately in complete ionization and disintegration of all atoms, although the pristine He droplet is transparent for the laser intensities applied. Our calculations at those intensities reveal that the minimal pulse length required for ignition is about 9 fs.

The dynamics of vibrational wave packets in triplet states of rubidium dimers $({\text{Rb}}_{2})$ formed on helium nanodroplets are studied using femtosecond pump-probe photoionization spectroscopy. Due to fast desorption of the excited ${\text{Rb}}_{2}$ molecules off the droplets and due to their low internal temperature, wave-packet oscillations can be followed up to very long pump-probe delay times $\ensuremath{\gtrsim}1.5\text{ }\text{ns}$. In the first-excited triplet state $(1){^{3}\ensuremath{\Sigma}}_{g}^{+}$, full and fractional revivals are observed with high contrast. Fourier analysis provides high-resolution vibrational spectra which are in excellent agreement with ab initio calculations.

We systematically investigate the formation and stability of snowballs formed by femtosecond photoionization of small alkali clusters bound to helium nanodroplets. For all studied alkali species Ak = (Na,K,Rb,Cs) we observe the formation of snowballs Ak(+)He(N) when multiply doping the droplets. Fragmentation of clusters Ak(N) upon ionization appears to enhance snowball formation. In the case of Na and Cs we also detect snowballs Ak(2) (+)He(N) formed around Ak dimer ions. While the snowball progression for Na and K is limited to less than 11 helium atoms, the heavier atoms Rb and Cs feature wide distributions at least up to Ak(+)He(41). Characteristic steps in the mass spectra of Cs-doped helium droplets are found at positions consistent with predictions on the closure of the first shell of helium atoms around the Ak(+) ion based on variational Monte Carlo simulations.

The reaction of alkali-metal (Na, Cs) clusters with water clusters embedded in helium nanodroplets is studied using femtosecond photoionization as well as electron-impact ionization. Unlike Na clusters, Cs clusters are found to completely react with water in spite of the ultracold helium droplet environment. Mass spectra of the ${\mathrm{Cs}}_{n}+({\mathrm{H}}_{2}\mathrm{O}{)}_{m}$ reaction products are interpreted in terms of stability with respect to fragmentation using high-level molecular structure calculations.

Femtosecond multiphoton pump-probe photoionization is applied to helium nanodroplets doped with rubidium (Rb). The yield of Rb+ ions features pronounced quantum interference (QI) fringes demonstrating the coherence of a superposition of electronic states on a time scale of tens of picoseconds. Furthermore, we observe QI in the yield of formed RbHe exciplex molecules. The quantum interferogram allows us to determine the vibrational structure of these unstable molecules. From a sliced Fourier analysis one cannot only extract the population dynamics of vibrational states but also follow their energetic evolution during the RbHe formation.

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.

The dynamics of vibrational wave packets excited in Na2 dimers in the triplet ground and excited states is investigated by means of helium nanodroplet isolation (HENDI) combined with femtosecond pump-probe spectroscopy. Different pathways in the employed resonant multi-photon ionization scheme are identified. Within the precision of the method, the wave packet dynamics appears to be unperturbed by the helium droplet environment.

The ultrafast dynamics of pure and doped helium nanodroplets is studied using VIS and XUV femto-second pump-probe spectroscopy in combination with ion and electron imaging detection.

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$^{-1}$.

Summary form only given. A quasi-electrostatic trap (QUEST) realized with a CO/sub 2/ laser relies on the electrostatic polarizability of the trapped particles and therefore represents a universal storage device for ultracold particles. All intriguing application of the QUEST is the simultaneous storage of different atomic species. Elastic and inelastic ground-state interactions can be investigated, one species may act as an agent to sympathetically cool the other species, and the formation and storage of cold ground-state molecules becomes possible in the same trapping volume. Our experiments start with a two-species magneto-optical trap for lithium and cesium.

We present quantitative measurements of the photoassociation of cesium molecules inside a far-detuned optical dipole trap. A model of the trap depletion dynamics is derived which allows to extract absolute photoassociation rate coefficients for the initial single-photon photoassociation step from measured trap-loss spectra. The sensitivity of this approach is demonstrated by measuring the Franck-Condon modulation of the weak photoassociation transitions into the low vibrational levels of the outer well of the 0g- state that correlates to the 6s+6p3/2 asymptote. The measurements are compared to theoretical predictions. In a magneto-optical trap these transitions have previously only been observed indirectly through ionization of ground state molecules.

We present studies of strong coupling in single-photon photoassociation of cesium dimers using an optical dipole trap. A thermodynamic model of the trap depletion dynamics is employed to extract absolute rate coefficents. From the dependence of the rate coefficient on the photoassociation laser intensity, we observe saturation of the photoassociation scattering probability at the unitarity limit in quantitative agreement with the theoretical model by Bohn and Julienne [Phys. Rev. A 60, 414 (1999)]. Also the corresponding power broadening of the resonance width is measured. We could not observe an intensity-dependent light shift in contrast to findings for lithium and rubidium, which is attributed to the absence of a $p$- or $d$-wave shape resonance in cesium.

We present measurements of the rate of hyperfine-state-changing collisions of unpolarized cesium $(^{133}\mathrm{Cs})$ and lithium $(^{7}\mathrm{Li})$ atoms confined in an optical dipole trap in the temperature range between 30 and $130\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{K}$. To infer rate coefficients from trap-loss data, we derive a simple thermodynamic model describing relaxation heating as a consequence of atom loss in a conservative potential. For hyperfine-changing $\mathrm{Cs}\text{\ensuremath{-}}\mathrm{Cs}$ collisions, the experimental results are compared with theoretical predictions and excellent agreement is found. Hyperfine-state-changing collisions in a mixture of lithium and cesium atoms are observed and rate coefficients are inferred for all combinations of hyperfine ground-state asymptotes.

The thermodynamics in a mixture of two different atomic gases at ultralow temperatures are explored. An intrinsically loss-free approach is presented which can be generalized to a vast range of atomic species and even molecules. The model system is a mixture of cesium and lithium in an extremely far-detuned optical dipole trap. Cesium is an excellent cooling agent, since it can be optically cooled to very low temperatures, mainly due to its high mass. Lithium, on the other side, is difficult to cool optically. In addition, it is nearly an ideal gas due the very small cross-section for elastic Li-Li collisions. Thermalization of Li thus occurs purely through collisions with the Cs atoms. From the time scale of thermalization one can deduce the a priori unknown interspecies scattering cross-section. Currently, the formation of ultracold Cs/sub 2/ molecules through photoassociation in the dipole trap is being investigated. The production of molecules in the lowest vibrational states of the outer well of the O/sub g//sup -/ potential is possible to observe by investigating the trap loss signals. Phenomena like saturation effects can be studied.

We simultaneously trap ultracold lithium and cesium atoms in an optical dipole trap formed by the focus of a CO$_2$ laser and study the exchange of thermal energy between the gases. The cesium gas, which is optically cooled to $20 \mu$K, efficiently decreases the temperature of the lithium gas through sympathetic cooling. The measured cross section for thermalizing $^{133}$Cs-$^7$Li collisions is $8 \times 10^{-12}$ cm$^2$, for both species in their lowest hyperfine ground state. Besides thermalization, we observe evaporation of lithium purely through elastic cesium-lithium collisions (sympathetic evaporation)., Comment: 4 pages 3 figs

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 2001

We have trapped cesium atoms over many minutes in the focus of a CO$_2$-laser beam employing an extremely simple laser system. Collisional properties of the unpolarized atoms in their electronic ground state are investigated. Inelastic binary collisions changing the hyperfine state lead to trap loss which is quantitatively analyzed. Elastic collisions result in evaporative cooling of the trapped gas from 25 $\mu$K to 10 $\mu$K over a time scale of about 150 s., Comment: 5 pages, 3 figures

Highly excited states of rubidium (Rb) atoms attached to helium (He) nanodroplets are studied by two-photon ionization spectroscopy in combination with electron and ion imaging. We find high yields of RbHe and RbHe(2) exciplexes when exciting to the 4D and 6P bands but not at the 6S band, in accord with a direct formation of exciplexes in binding RbHe pair potentials. Photoion spectra and angular distributions are in good agreement with a pseudodiatomic model for the RbHe(N) complex. Repulsive interactions in the excited states entail fast dissociation followed by ionization of free Rb atoms as well as of RbHe and RbHe(2) exciplexes.