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We present a method for the reconstruction of ion kinetic energy distributions from ion time-of-flight mass spectra through ion trajectory simulations. In particular, this method is applicable to complicated spectrometer geometries with largely anisotropic ion collection efficiencies. A calibration procedure using a single ion mass peak allows the accurate determination of parameters related to the spectrometer calibration, experimental alignment and instrument response function, which improves the agreement between simulations and experiment. The calibrated simulation is used to generate a set of basis functions for the time-of-flight spectra, which are then used to transform from time-of-flight to kinetic-energy spectra. We demonstrate this reconstruction method on a recent pump-probe experiment by Asmussen et al. (J. D. Asmussen et al., Phys. Chem. Chem. Phys., 23, 15138, (2021)) on helium nanodroplets and retrieve time-resolved kinetic-energy-release spectra for the ions from ion time-of-flight spectra.

Tailored light-matter interactions in the strong coupling regime enable the manipulation and control of quantum systems with up to unit efficiency, with applications ranging from quantum information to photochemistry. While strong light-matter interactions are readily induced at the valence electron level using long-wavelength radiation, comparable phenomena have been only recently observed with short wavelengths, accessing highly-excited multi-electron and inner-shell electron states. However, the quantum control of strong-field processes at short wavelengths has not been possible, so far, due to the lack of pulse shaping technologies in the extreme ultraviolet (XUV) and X-ray domain. Here, exploiting pulse shaping of the seeded free-electron laser (FEL) FERMI, we demonstrate the strong-field quantum control of ultrafast Rabi dynamics in helium atoms with high fidelity. Our approach unravels a strong dressing of the ionization continuum, otherwise elusive to experimental observables. The latter is exploited to achieve control of the total ionization rate, with prospective applications in many XUV and soft X-ray experiments. Leveraging recent advances in intense few-femtosecond to attosecond XUV to soft X-ray light sources, our results open an avenue to the efficient manipulation and selective control of core electron processes and electron correlation phenomena in real time.

Radiation damage in biological systems by ionizing radiation is predominantly caused by secondary processes such as charge and energy transfer leading to the breaking of bonds in DNA. Here, we study the fragmentation of cytosine (Cyt) and thymine (Thy) molecules, clusters and microhydrated derivatives induced by direct and indirect ionization initiated by extreme-ultraviolet (XUV) irradiation. Photofragmentation mass spectra and photoelectron spectra of free Cyt and Thy molecules are compared with mass and electron spectra of Cyt/Thy clusters and microhydrated Cyt/Thy molecules formed by aggregation in superfluid helium (He) nanodroplets. Penning ionization after resonant excitation of the He droplets is generally found to cause less fragmentation compared to direct photoionization and charge-transfer ionization after photoionization of the He droplets. When Cyt/Thy molecules and oligomers are complexed with water molecules, their fragmentation is efficiently suppressed. However, a similar suppression of fragmentation is observed when homogeneous Cyt/Thy clusters are formed in He nanodroplets, indicating a general trend. Penning ionization electron spectra (PIES) of Cyt/Thy are broad and nearly featureless but PIES of their microhydrated derivatives point at a sequential ionization process ending in unfragmented microsolvated Cyt/Thy cations., Comment: 9 pages, 8 figures

Photoionization spectroscopy and mass spectrometry of doped helium (He) nanodroplets rely on the ability to efficiently detect ions and/or electrons. Using a commercial quadrupole mass spectrometer and a photoelectron-photoion coincidence (PEPICO) spectrometer, we systematically measure yields of ions and electrons created in pure and doped He nanodroplets in a wide size range and in two ionization regimes -- direct ionization and secondary ionization after resonant photoexcitation of the droplets. For two different types of dopants (oxygen molecules, O$_2$, and lithium atoms, Li), we infer the optimal droplet size to maximize the yield of ejected ions. When dopants are ionized by charge-transfer to photoionized He nanodroplets, the highest yield of O$_2$ and Li ions is detected for a mean size of $\sim5\times10^4$ He atoms per nanodroplet. When dopants are Penning ionized via photoexcitation of the He droplets, the highest yield of O$_2$ and Li ions is detected for $\sim10^3$ and $\sim10^5$ He atoms per droplet, respectively. At optimum droplet sizes, the detection efficiency of dopant ions in proportion to the number of primary photoabsorption events is up to 20\,\% for charge-transfer ionization of O$_2$ and 2\,\% for Li, whereas for Penning ionization it is 1\,\% for O$_2$ and 4\,\% for Li. Our results are instrumental in determining optimal conditions for mass spectrometric studies and photoionization spectroscopy of molecules and complexes isolated in He nanodroplets.

Helium nanodroplets are ideal model systems to unravel the complex interaction of condensed matter with ionizing radiation. Here we study the effect of purely elastic electron scattering on angular and energy distributions of photoelectrons emitted from He nanodroplets of variable size ($10$-$10^9$ atoms per droplets). For large droplets, photoelectrons develop a pronounced anisotropy along the incident light beam due to a shadowing effect within the droplets. In contrast, the detected photoelectron spectra are only weakly perturbed. This opens up possibilities for photoelectron spectroscopy of dopants embedded in droplets provided they are smaller than the penetration depth of the light and the trapping range of emitted electrons.

Ultrafast electron dynamics drive phenomena such as photochemical reactions, catalysis, and light harvesting. To capture such dynamics in real-time, femtosecond to attosecond light sources are extensively used. However, an exact match between the excitation photon energy and a characteristic resonance is crucial. High-harmonic generation sources are exceptional in terms of pulse duration but limited in spectral tunability in the VUV range. Here, we present a monochromatic femtosecond source continuously tunable around 21 eV photon energy utilizing the second harmonic of an OPCPA laser system to drive high-harmonic generation. The unique tunability of the source is verified in an experiment probing the interatomic Coulombic decay in doped He nanodroplets across the He absorption bands. Moreover, we achieved intensities sufficient for driving non-linear processes using a tight focusing of the VUV beam. We demonstrated it on the observation of collective autoionization of multiply excited pure He nanodroplets., Comment: 12 pages, 5 figures, submitted to Nat. Commun

Femtosecond extreme ultraviolet wave packet interferometry (XUV-WPI) was applied to study resonant inter-atomic Coulombic decay (ICD) in the HeNe dimer. The high demands on phase stability and sensitivity for vibronic XUV-WPI of molecular-beam targets are met using an XUV phase-cycling scheme. The detected quantum interferences exhibit vibronic dephasing and rephasing signatures along with an ultrafast decoherence assigned to the ICD process. A Fourier analysis reveals the molecular absorption spectrum with high resolution. The demonstrated experiment shows a promising route for the real-time analysis of ultrafast ICD processes with both high temporal and spectral resolution., Comment: 7 pages, 4 figures

We present a new endstation for the AMOLine of the ASTRID2 synchrotron at Aarhus University, which combines a cluster and nanodroplet beam source with a velocity map imaging and time-of-flight spectrometer for coincidence imaging spectroscopy. Extreme-ultraviolet spectroscopy of free nanoparticles is a powerful tool for studying the photophysics and photochemistry of resonantly excited or ionized nanometer-sized condensed-phase systems. Here we demonstrate this capability by performing photoelectron-photoion coincidence (PEPICO) experiments with pure and doped superfluid helium nanodroplets. Different doping options and beam sources provide a versatile platform to generate various van der Waals clusters as well as He nanodroplets. We present a detailed characterization of the new setup and present examples of its use for measuring high-resolution yield spectra of charged particles, time-of-flight ion mass spectra, anion-cation coincidence spectra, multi-coincidence electron spectra and angular distributions. A particular focus of the research with this new endstation is on intermolecular charge and energy-transfer processes in heterogeneous nanosystems induced by valence-shell excitation and ionization., Comment: 28 pages, 17 figures, submitted to Review of Scientific Instruments

The autoionization dynamics of superexcited superfluid He nanodroplets doped with Na atoms is studied by extreme-ultraviolet (XUV) time-resolved electron spectroscopy. Following excitation into the higher-lying droplet absorption band, the droplet relaxes into the lowest metastable atomic $1s2s$ $^{1,\,3}$S states from which Interatomic Coulombic Decay (ICD) takes places either between two excited He atoms or between an excited He atom and a Na atom attached to the droplet surface. Four main ICD channels are identified and their time constants are determined by varying the delay between the XUV pulse and a UV pulse that ionizes the initial excited state and thereby quenches ICD. The time constants for the different channels all fall in the range $\sim$1~ps indicating that the ICD dynamics are mainly determined by the droplet environment. A periodic modulation of the transient ICD signals is tentatively attributed to the oscillation of the bubble forming around the localized He excitation. The ICD efficiency depends on the total number of excited states in a droplet rather than the density of excited states pointing to a collective enhancement of ICD.

Interferometric pump-probe experiments in the extreme ultraviolet (XUV) domain are experimentally very challenging due to the high phase stability required between the XUV pulses. Recently, an efficient phase stabilization scheme was introduced for seeded XUV free electron lasers (FELs) combining shot-to-shot phase modulation with lock-in detection. This method stabilized the seed laser beampath on the fundamental ultraviolet wavelength to a high degree. Here, we extend this scheme including the stabilization of the XUV beampath, incorporating phase fluctuations from the FEL high gain harmonic generation process. Our analysis reveals a clear signal improvement with the new method compared to the previous stabilization scheme.

Rubidium dimers residing on the surface of He nanodroplets are doubly ionized by an intense fs laser pulse leading to fragmentation into a pair of $\mathrm{Rb^+}$ ions. We show that the kinetic energy of the $\mathrm{Rb^+}$ fragment ions can be used to identify dimers formed in either the X $^1\Sigma_{\mathrm{g}}^+$ ground state or in the lowest-lying triplet state, a $^3\Sigma_{\mathrm{u}}^+$. From the experiment, we estimate the abundance ratio of dimers in the a and X states as a function of the mean droplet size and find values between 4:1 and 5:1. Our technique applies generally to dimers and trimers of alkali atoms, here also demonstrated for $\mathrm{Li_2}$, $\mathrm{Na_2}$, and $\mathrm{K_2}$, and will enable fs time-resolved measurements of their rotational and vibrational dynamics, possibly with atomic structural resolution., Comment: 5 pages, 4 figures

The relaxation dynamics of superexcited superfluid He nanodroplets is thoroughly investigated by means of extreme-ultraviolet (XUV) femtosecond electron and ion spectroscopy complemented by time-dependent density functional theory (TDDFT). Three main paths leading to the emission of electrons and ions are identified: Droplet autoionization, pump-probe photoionization, and autoionization induced by re-excitation of droplets relaxing into levels below the droplet ionization threshold. The most abundant product of both droplet autoionization and photoionization is He$_2^+$, whereas the delayed appearance of He$^+$ is indicative of the ejection of excited He atoms from the droplets. The state-resolved time-dependent photoelectron spectra reveal that intermediate excited states of the droplets are populated in the course of the relaxation, terminating in the lowest-lying metastable singlet and triplet He atomic states. The slightly faster relaxation of the triplet state compared to the singlet state is in agreement with the simulation showing faster formation of a bubble around a He atom in the triplet state.

The acetylene-vinylidene system serves as a benchmark for investigations of ultrafast dynamical processes where the coupling of the electronic and nuclear degrees of freedom provides a fertile playground to explore the femto- and sub-femto-second physics with coherent extreme-ultraviolet (EUV) photon sources both on the table-top as well as free-electron lasers. We focus on detailed investigations of this molecular system in the photon energy range $19...40$ eV where EUV pulses can probe the dynamics effectively. We employ photoelectron-photoion coincidence (PEPICO) spectroscopy to uncover hitherto unrevealed aspects of this system. In this work, the role of excited states of the $C_{2}H_{2}^{+}$ cation, the primary photoion, is specifically addressed. From photoelectron energy spectra and angular distributions, the nature of the dissociation and isomerization channels is discerned. Exploiting the $4\pi$-collection geometry of velocity map imaging spectrometer, we not only probe pathways where the efficiency of photoionization is inherently high but also perform PEPICO spectroscopy on relatively weak channels., Comment: 12 pages, 7 figures, 5 tables

Collinear double-pulse seeding of the High-Gain Harmonic Generation (HGHG) process in a free-electron laser (FEL) is a promising approach to facilitate various coherent nonlinear spectroscopy schemes in the extreme ultraviolet (XUV) spectral range. However, in collinear arrangements using a single nonlinear medium, temporally overlapping seed pulses may introduce nonlinear mixing signals that compromise the experiment at short time delays. Here, we investigate these effects in detail by extending the analysis described in a recent publication (Wituschek et al., Nat. Commun., 11, 883, 2020). High-order fringe-resolved autocorrelation and wave-packet interferometry experiments at photon energies > $23\,$eV are performed, accompanied by numerical simulations. It turns out that both the autocorrelation and the wave-packet interferometry data are very sensitive to saturation effects and can thus be used to characterize saturation in the HGHG process. Our results further imply that time-resolved spectroscopy experiments are feasible even for time delays smaller than the seed pulse duration., Comment: This is accepted version of the article. The Version of Record is available online at https://doi.org/10.1364/OE.401249

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.

Making quantum mechanical equations and concepts come to life through interactive simulation and visualization are commonplace for augmenting learning and teaching. However, graphical visualizations nearly always exhibit a set of hard-coded functionalities while corresponding text-based codes offer a higher degree of flexibility at the expense of steep learning curves or time investments. We introduce Quantum Composer, which allows the user to build, expand, or explore quantum mechanical simulations by interacting with graphically connectable nodes, each corresponding to a physical concept, mathematical operation, visualization, etc. Abstracting away numerical and programming details while at the same time retaining accessibility, emphasis on understanding, and rapid feedback mechanisms, we illustrate through a series of examples its open-ended applicability in both introductory and advanced quantum mechanics courses, student projects, and for visual exploration within research environments., Comment: 29 pages, 12 figures

Alkali metal dimers attached to the surface of helium nanodroplets are found to be efficiently doubly ionized by electron transfer-mediated decay (ETMD) when photoionizing the helium droplets. This process is evidenced by detecting in coincidence two energetic ions created by Coulomb explosion and one low-kinetic energy electron. The kinetic energy spectra of ions and electrons are reproduced by simple model calculations based on diatomic potential energy curves, and are in agreement with ab initio calculations for the He-Na_2 and He-KRb systems. This work demonstrates that ETMD is an important decay channel in heterogeneous nanosystems exposed to ionizing radiation.

The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within a XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths., Comment: This is the accepted version of the article. The Version of Record is available online at 10.1038/s41467-020-14721-2

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., Comment: accepted by J. Chem. Phys. (Dec. 2018)

We present a comparison of two technically distinct methods for the generation of rotationally cold, pulsed supersonic beams of methyl radicals (CH3): a plate discharge source operating in the glow regime, and a dielectric barrier discharge source (DBD). The results imply that the efficiency of both sources is comparable, and that molecular beams with similar translational and rotational temperatures are formed. Methane (CH4) proved to be the most suitable radical precursor species.

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.

Helium (He) nanodroplets irradiated by intense near-infrared laser pulses form a nanoplasma by avalanche-like electron impact ionizations even at lower laser intensities where He is not directly field ionized, provided that the droplets contain a few dopant atoms which provide seed electrons for the electron impact ionization avalanche. In this theoretical paper on calcium and xenon doped He droplets we elucidate the mechanism which induces ionization avalanches, termed ignition. We find that the partial loss of seed electrons from the activated droplets starkly assists ignition, as the Coulomb barrier for ionization of helium is lowered by the electric field of the dopant cations, and this deshielding of the cation charges enhances their electric field. In addition, the dopant ions assist the acceleration of the seed electrons (slingshot effect) by the laser field, supporting electron impact ionizations of He and also causing electron loss by catapulting electrons away. The dopants' ability to lower the Coulomb barriers at He as well as the slingshot effect decrease with the spatial expansion of the dopant, causing a dependence of the dopants' ignition capability on the dopant mass. Here, we develop criteria (impact count functions) to assess the ignition capability of dopants, based on (i) the spatial overlap of the seed electron cloud with the He atoms and (ii) the overlap of their kinetic energy distribution with the distribution of Coulomb barrier heights at He. The relatively long time delays between the instants of dopant ionization and ignition (incubation times) for calcium doped droplets are determined to a large extent by the time it takes to deshield the dopant ions.

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 (<10^15 Wcm-2). In particular, we elucidate the interplay of dopant ionization inducing the ignition of a helium nanoplasma, and the charging of the dopant atoms driven by the ionized helium host. Most efficient nanoplasma ignition and charging is found when doping helium droplets with xenon atoms, in which case high charge states both of helium (He2+) and of xenon (Xe^21+) are detected. In contrast, only low charge states of helium and dopants are measured when doping with potassium and calcium atoms. Classical molecular dynamics simulations which include focal averaging generally reproduce the experimental results and provide detailed insights into the correlated charging dynamics of guest and host clusters.

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.

We have measured the dependence of the relative integral cross section of the reaction Li+HF-->LiF+H on the collision energy using crossed molecular beams. By varying the intersection angle of the beams from 37{\deg} to 90{\deg} we covered the energy range 25 meV < E_tr < 131 meV. We observe a monotonous rise of the cross section with decreasing energy over the entire energy range indicating that a possible translational energy threshold to the reaction is significantly smaller than 25 meV. The steep rise is quantitatively recovered by a Langevin-type excitation function based on a vanishing threshold and a mean interaction potential energy ~R^-2.5 where R is the distance between the reactants. To date all threshold energies deduced from ab-initio potentials and zero-point vibrational energies are at variance with our results, however, our findings support recent quantum scattering calculations that predict significant product formation at collision energies far below these theoretical thresholds., Comment: 8 pages, 7 figures

Homo- and heteronuclear alkali quartet trimers of the type K_{3-n}Rb_{n} (n=0,1,2,3) formed on helium nanodroplets are probed by one-color femtosecond photoionization spectroscopy. The obtained requencies are assigned to vibrations in different electronic states by comparison to high level ab initio calculations of the involved potentials including pronounced Jahn-Teller and spin-orbit couplings. Despite the fact that the resulting complex vibronic structure of the heavy alkali molecules complicates the comparison of experiment and theory we find good agreement for many of the observed lines for all species.

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 is found to be constant ~0.5ns^-1 for the lowest vibrational levels v< 15 and to increase sharply when exciting to higher energies.

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 as a result of the interaction between dimer and collective degrees of freedom of the helium droplet. The calculations allow us to explain crucial experimental findings that are unobserved in gas-phase measurements. Remarkably, best agreement with experiment is found for a model where we neglect damping once a wave packet moves below a critical velocity. In this way the results provide first direct evidence for the Landau critical velocity in superfluid nanodroplets., Comment: 4.1 pages, 5 figures

We show that the quantum reflection coefficient of ultracold heavy atoms scattering off a dielectric surface can be tuned in a wide range by suitable choice of surface and environment temperatures. This effect results from a temperature dependent long-range repulsive part of the van der Waals-Casimir-Polder-Lifshitz atom-surface interaction potential.

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.

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$^{-1}$.

Coupling by the resonant dipole-dipole energy transfer between cold cesium Rydberg atoms is investigated using time-resolved narrow-band de-excitation spectroscopy. This technique combines the advantage of efficient Rydberg excitation with high-resolution spectroscopy at variable interaction times. The coherent character of the process is studied by back and forth transfer in the np+np <--> ns+(n+1)s reaction. Decoherence in the ensemble has two different origins: the atom motion induced by dipole-dipole interaction and the migration of the s-Rydberg excitation in the environment of p-Rydberg atoms., Comment: 4 pages, 5 figures