Optimal control techniques combined with femtosecond laser pulse shaping are applied to steer and enhance the strong-field induced emission of highly charged atomic ions from silver clusters embedded in helium nanodroplets. With light fields shaped in amplitude and phase we observe a substantial increase of the Ag$^{q+}$ yield for $q>10$ when compared to bandwidth-limited and optimally stretched pulses. A remarkably simple double-pulse structure, containing a low-intensity prepulse and a stronger main pulse, turns out to produce the highest atomic charge states up to Ag$^{20+}$. A negative chirp during the main pulse hints at dynamic frequency locking to the cluster plasmon. A numerical optimal control study on pure silver clusters with a nanoplasma model converges to a similar pulse structure and corroborates, that the optimal light field adapts to the resonant excitation of cluster surface plasmons for efficient ionization.
Pulsed (30 - 100 microseconds) nozzle beams have been used to generate helium droplets (<N> = 10^4-10^5). The dependence of the beam intensity and the mean droplet size on the source stagnation pressure and temperature are studied via mass spectroscopy and laser induced fluorescence of embedded phthalocyanine molecules. In comparison to a cw beam the pulsed source for the same pressure and temperature has a factor of 100 higher flux and the droplet sizes are an order of a magnitude larger.
The mechanism of ionization of helium droplets has been investigated in numerous reports but one observation has not found a satisfactory explanation: How are $He^+$ ions formed and ejected from undoped droplets at electron energies below the ionization threshold of the free atom? Does this path exist at all? A measurement of the ion yields of $He^+$ and $He_2^+$ as a function of electron energy, electron emission current, and droplet size reveals that metastable $He^{*-}$ anions play a crucial role in the formation of free $He^+$ at subthreshold energies. The proposed model is testable.
Besides the use as cold matrix for spectroscopic studies, superfluid helium droplets have served as a cold environment for the synthesis of molecules and clusters. Since vibrational frequencies of molecules in helium droplets exhibit almost no shift compared to the free molecule values, one could assume the solvated particles move frictionless and undergo a reaction as soon as their paths cross. There have been a few unexplained observations that seemed to indicate cases of two species on one droplet not forming bonds but remaining isolated. In this work, we performed a systematic study of hel…
Electron ionization of helium droplets doped with cesium or potassium results in doubly and, for cesium, triply charged cluster ions. The smallest observable doubly charged clusters are $Cs_{9}^{2+}$ and $K_{11}^{2+}$; they are a factor two smaller than reported previously. The size of potassium dications approaches the Rayleigh limit nRay for which the fission barrier is calculated to vanish, i.e. their fissilities are close to 1. Cesium dications are even smaller than nRay, implying that their fissilities have been significantly overestimated. Triply charged cesium clusters as small as $Cs_{…
We use a novel technique to solvate silver cations in small clusters of noble gases. The technique involves formation of large, superfluid helium nanodroplets that are subsequently electron ionized, mass-selected by deflection in an electric field, and doped with silver atoms and noble gases (Ng) in pickup cells. Excess helium is then stripped from the doped nanodroplets by multiple collisions with helium gas at room temperature, producing cluster ions that contain no more than a few dozen noble gas atoms and just a few (or no) silver atoms. Under gentle stripping conditions helium atoms remai…
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…
Doping a helium nanodroplet with a tiny xenon cluster of a few atoms only, sparks complete ionization of the droplet at laser intensities below the ionization threshold of helium atoms. As a result, the intrinsically inert and transparent droplet turns into a fast and strong absorber of infrared light. Microscopic calculations reveal a two-step mechanism to be responsible for the dramatic change: Avalanche-like ionization of the helium atoms on a femtosecond time scale, driven by field ionization due to the quickly charged xenon core is followed by resonant absorption enabled by an unusual cig…
We report the first observation of cations, dications and trications of large clusters of adamantane. Cluster formation was initiated near 0 K in helium droplets and ionization was achieved with one or more collisions with energetic He species (He$^{\star}$, He$^{+}$ or He$^{\star}$$^{-}$). The occurrence of Coulomb explosion appeared to discriminate against the formation of small multiply charged clusters. High resolution mass spectrometry revealed the presence of "magic number" m/z peaks that can be attributed to the packing of adamantane molecules into cluster structures of special stabilit…
Within the diffusion Monte Carlo approach, we have determined the structure of isotopically pure and mixed helium droplets doped with one magnesium atom. For pure 4He clusters, our results confirm those of M. Mella et al. [J. Chem. Phys. 123, 054328 (2005)] that the impurity experiences a transition from a surface to a bulk location as the number of helium atoms in the droplet increases. Contrarily, for pure 3He clusters Mg resides in the bulk of the droplet due to the smaller surface tension of this isotope. Results for mixed droplets are presented. We have also obtained the absorption spectr…
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 …
Accurate analytical expressions for the state densities of liquid He-4 droplets are derived, incorporating the ripplon and phonon degrees of freedom. The microcanonical temperature and the ripplon angular momentum level density are also evaluated. The approach is based on inversions and systematic expansions of canonical thermodynamic properties.
We used cold helium droplets as nano-scale reactors to form and ionize, by electron bombardment and charge transfer, aromatic amino acid heterodimers of histidine with tryptophan, methyl-tryptophan, and indole. The molecular interaction occurring through an N-H...N hydrogen bond leads to a proton transfer from the indole group of tryptophan to the imidazole group of histidine in a radical cationic environment.
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 o…
An experimental approach is presented that allows for the incorporation of large mass/charge selected ions in liquid helium droplets. It is demonstrated that droplets can be efficiently doped with a mass/charge selected amino acid as well as with the much bigger m$\approx$12 000 amu protein Cytochrome C in selected charge states. The sizes of the ion-doped droplets are determined via electrostatic deflection. Under the experimental conditions employed, the observed droplet sizes are very large and range, dependent on the incorporated ion, from 10$^{10}$ helium atoms for protonated Phenylalanin…
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 ap…
We report on the production and study of stable, highly charged droplets of superfluid helium. Using a novel experimental setup we produce neutral beams of liquid helium nanodroplets containing millions of atoms or more that can be ionized by electron impact, mass-per-charge selected, and ionized a second time before being analyzed. Droplets containing up to 55 net positive charges are identified and the appearance sizes of multiply charge droplets are determined as a function of charge state. We show that the droplets are stable on the millisecond time scale of the experiment and decay throug…
The spectroscopy of free radicals and radical containing entrance-channel complexes embedded in superfluid helium nano-droplets is reviewed. The collection of dopants inside individual droplets in the beam represents a micro-canonical ensemble, and as such each droplet may be considered an isolated cryo-reactor. The unique properties of the droplets, namely their low temperature (0.4 K) and fast cooling rates ($\sim10^{16}$ K s$^{-1}$) provides novel opportunities for the formation and high-resolution studies of molecular complexes containing one or more free radicals. The production methods o…
High-resolution mass spectra of helium droplets doped with C$_{60}$ and formic acid (FA) are ionized by electrons. Positive ion mass spectra reveal cluster ions [(C$_{60}$)$_p$FA$_n$]$^+$ together with their hydrogenated and dehydrogenated counterparts. Also observed are ions containing one or more water (W) molecules. The abundance distributions of these ions reveal several interesting features: i) [(C$_{60}$)$_p$FA$_n$]$^+$ ions are more abundant than hydrogenated [(C$_{60}$)$_p$FA$_n$H]$^+$ ions even though the opposite is true in the absence of C$_{60}$ (i.e. if $p$ = 0); ii) although [C$_…
We present a quantum Monte Carlo study of the structure and energetics of silver doped helium clusters AgHe$_n$ for $n$ up to 100. Our simulations show the first solvation shell of the Ag atom to be composed by roughly 20 He atoms, and to possess a structured angular distribution. Moreover, the electronic $^2$P$_{1/2}\leftarrow ^2$S$_{1/2}$ and $^2$P$_{3/2}\leftarrow ^2$S$_{1/2}$ electronic transitions of the embedded silver impurity have been studied as a function of the number ofhelium atoms. The computed spectra show a redshift for $n\leq 15$ and an increasing blueshift for larger clusters,…
Interatomic Coulombic decay (ICD) is induced in helium (He) nanodroplets by photoexciting the n=2 excited state of 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 He^+ ions as previously observed for free He dimers. ICD deeper inside leads to the ejection of slow He^+ ions due to Coulomb explosion delayed by elastic collisions with neighboring He atoms, and to the formation of He_k^…
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 …
A significant fraction of superfluid helium nanodroplets produced in a free-jet expansion have been observed to gain high angular momentum resulting in large centrifugal deformation. We measured single-shot diffraction patterns of individual rotating helium nanodroplets up to large scattering angles using intense extreme ultraviolet light pulses from the FERMI free-electron laser. Distinct asymmetric features in the wide-angle diffraction patterns enable the unique and systematic identification of the three-dimensional droplet shapes. The analysis of a large dataset allows us to follow the evo…
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 Coulom…
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.
When weakly-bound complexes are multiply excited by intense electromagnetic radiation, energy can be exchanged between neighboring atoms through a type of resonant interatomic Coulombic decay (ICD). This decay mechanism due to multiple excitations has been predicted to be relatively slow, typically lasting tens to hundreds of picoseconds. Here, we directly measure the ICD timescale in resonantly excited helium droplets using a high resolution, tunable, extreme ultraviolet free electron laser. Over an extensive range of droplet sizes and laser intensities, we discover the decay to be surprising…
Alignment of OCS, CS$_2$ and I$_2$ molecules embedded in helium nanodroplets is measured as a function of time following rotational excitation by a non-resonant, comparatively weak ps laser pulse. The distinct peaks in the power spectra, obtained by Fourier analysis, are used to determine the rotational, B, and centrifugal distortion, D, constants. For OCS, B and D match the values known from IR spectroscopy. For CS$_2$ and I$_2$, they are the first experimental results reported. The alignment dynamics calculated from the gas-phase rotational Schrödinger equation, using the experimental in-dro…
Helium nanodroplets doped with polar molecules are studied by electrostatic deflection. This broadly applicable method allows even polyatomic molecules to attain sub-Kelvin temperatures and nearly full orientation in the field. The resulting intense force from the field gradient strongly deflects even droplets with tens of thousands of atoms, the most massive neutral systems studied by beam "deflectometry." We use the deflections to extract droplet size distributions. Moreover, since each host droplet deflects according to its mass, spatial filtering of the deflected beam translates into size …
Dimers of carbon disulfide (CS$_2$) molecules embedded in helium nanodroplets are aligned using a moderately intense, 160ps, non-resonant, circularly polarized laser pulse. It is shown that the intermolecular carbon-carbon (C-C) axis aligns along the axis perpendicular to the polarization plane of the alignment laser pulse. The degree of alignment, quantified by $\langle \cos^2(θ_\text{2D}) \rangle$, is determined from the emission directions of recoiling CS$_2$$^+$ fragment ions, created when an intense 40fs probe laser pulse doubly ionizes the dimers. Here, $θ_\text{2D}$ is the projection of…
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…
We systematically investigate the formation and stability of snowballs formed by femtosecond photo-ionization of small alkali clusters bound to helium nanodroplets. For all studied alkali species Ak=(Na, K, Rb, Cs) we observe the formation of snowballs (AkHe_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_2He_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 wi…
In several settings of physics and chemistry one has to deal with molecules interacting with some kind of an external environment, be it a gas, a solution, or a crystal surface. Understanding molecular processes in the presence of such a many-particle bath is inherently challenging, and usually requires large-scale numerical computations. Here, we present an alternative approach to the problem - that based on the notion of the angulon quasiparticle. We show that molecules rotating inside superfluid helium nanodroplets and Bose-Einstein Condensates form angulons, and therefore can be described …
Iodine (I$_2$) molecules embedded in He nanodroplets are aligned by a 160 ps long laser pulse. The highest degree of alignment, occurring at the peak of the pulse and quantified by $\langle \cos^2 θ_{2D} \rangle$, is measured as a function of the laser intensity. The results are well described by $\langle \cos^2 θ_{2D} \rangle$ calculated for a gas of isolated molecules each with an effective rotational constant of 0.6 times the gas-phase value, and at a temperature of 0.4 K. Theoretical analysis using the angulon quasiparticle to describe rotating molecules in superfluid helium rationalizes w…
Rotationally resolved infrared spectra are reported for the X-HCN (X = Cl, Br, I) binary complexes solvated in helium nanodroplets. These results are directly compared with that obtained previously for the corresponding X-HF complexes [J. M. Merritt, J. Küpper, and R. E. Miller, PCCP, 7, 67 (2005)]. For bromine and iodine atoms complexed with HCN, two linear structures are observed and assigned to the $^{2}Σ_{1/2}$ and $^{2}Π_{3/2}$ ground electronic states of the nitrogen and hydrogen bound geometries, respectively. Experiments for HCN + chlorine atoms give rise to only a single band which is…
We thoroughly investigate vibrational quantum dynamics of dimers attached to He droplets motivated by recent measurements with K-2 [1]. For those femtosecond pump-probe experiments, crucial observed features are not reproduced by gas phase calculations but agreement is found using a description based on dissipative quantum dynamics, as briefly shown in [2]. Here we present a detailed study of the influence of possible effects induced by the droplet. The helium droplet causes electronic decoherence, shifts of potential surfaces, and relaxation of wave packets in attached dimers. Moreover, a rea…
Two-component nanoplasmas generated by strong-field ionization of doped helium nanodroplets are studied in a pump-probe experiment using few-cycle laser pulses in combination with molecular dynamics simulations. High yields of helium ions and a pronounced, droplet size-dependent resonance structure in the pump-probe transients reveal the evolution of the dopant-induced helium nanoplasma. The pump-probe dynamics is interpreted in terms of strong inner ionization by the pump pulse and resonant heating by the probe pulse which controls the final charge states detected via the frustration of elect…
Rotationally resolved infrared spectra are reported for halogen atom - HF free radical complexes formed in helium nanodroplets. An effusive pyrolysis source is used to dope helium droplets with Cl, Br and I atoms, formed by thermal dissociation of Cl$_2$, Br$_2$ and I$_2$. A single hydrogen fluoride molecule is then added to the droplets, resulting in the formation of the X-HF complexes of interest. Analysis of the resulting spectra confirms that the observed species have $^2Π_{3/2}$ ground electronic states, consistent with the linear hydrogen bound structures predicted from theory. Stark spe…
An effusive pyrolysis source is described for generating a continuous beam of radicals under conditions appropriate for the helium droplet pick-up method. Rotationally resolved spectra are reported for the $ν_1$ vibrational mode of the propargyl radical in helium droplets at 3322.15 cm$^{-1}$. Stark spectra are also recorded that allow for the first experimental determination of the permanent electric dipole moment of propargyl, namely -0.150 D and -0.148 D for ground and excited state, respectively, in good agreement with previously reported ab initio results of -0.14 D [1]. The infrared spec…
We present a microscopic analysis of the quantum solvation structures of para-H$_2$ around the OCS molecule when embedded in low temperature $^4$He droplets. The structures of clusters containing M=5 and 6 para-H$_2$ molecules are compared with corresponding structures for M=1 (OCS-H$_2$ complex) and M=17 (a full solvation shell), as well as with the clusters in the absence of helium. We find that the helium has negligible effect on the structures for the small and large OCS(H$_2$)$_M$ clusters, but that it modifies the cluster structure for M=6. We discuss implications of these results for th…
We have explored the light induced dynamics in superfluid helium nanodroplets with wide-angle scattering in a pump-probe measurement scheme. The droplets are doped with xenon atoms to facilitate the ignition of a nanoplasma through irradiation with near-infrared laser pulses. After a variable time delay of up to 800 ps, we image the subsequent dynamics using intense extreme ultraviolet pulses from the FERMI free-electron laser. The recorded scattering images exhibit complex intensity fluctuations that are categorized based on their characteristic features. Systematic simulations of wide-angle …
Doubly-excited Rydberg states of helium (He) nanodroplets have been studied using synchrotron radiation. We observed Fano resonances related to the atomic N = 2,0 series as a function of droplet size. Although similar qualitatively to their atomic counterparts, the resonance lines are broader and exhibit a shift in energy which increases for the higher excited states. Furthermore, additional resonances are observed which are not seen in atomic systems. We discuss these features in terms of delocalized atomic states perturbed by the surrounding He atoms and compare to singly excited droplets.
The ionization dynamics of helium droplets in a wide size range from 220 to 10^6 He atoms irradiated with intense femtosecond extreme ultraviolet (XUV) pulses of 10^9 ÷ 10^{12} W/cm2 power density is investigated in detail by photoelectron spectroscopy. Helium droplets are resonantly excited in the photon energy range from ~ 21 eV (corresponding to the atomic 1s2s state) up to the atomic ionization potential (IP) at ~ 25 eV. A complex evolution of the electron spectra as a function of droplet size and XUV intensity is observed, ranging from atomic-like narrow peaks due to binary autoionization…
The reaction of alkali (Na, Cs) clusters with water clusters embedded in helium nanodroplets is studied using femtosecond photo-ionization 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 Cs$_n$+(H$_2$O)$_m$ reaction products are interpreted in terms of stability with respect to fragmentation using high-level molecular structure calculations.
Rotational dynamics of D$_2$ molecules inside helium nanodroplets is induced by a moderately intense femtosecond (fs) pump pulse and measured as a function of time by recording the yield of HeD$^+$ ions, created through strong-field dissociative ionization with a delayed fs probe pulse. The yield oscillates with a period of 185 fs, reflecting field-free rotational wave packet dynamics, and the oscillation persists for more than 500 periods. Within the experimental uncertainty, the rotational constant BHe of the in-droplet D$_2$ molecule, determined by Fourier analysis, is the same as Bgas for …
Relaxation processes following inner-valence ionization of a system can be modified dramatically by embedding this system in a suitable environment. Surprisingly, such an environment can be even composed of helium atoms, the most inert species available. As demonstrated by the examples of Ne and Ca atoms embedded in He droplets, a fast relaxation process [Interatomic Coulombic Decay (ICD)] takes place merely due to the presence of the He surroundings. We have computed ICD widths for both 4He_N and 3He_N droplets doped with Ne and Ca and discuss the findings in some detail. In the case of Ne, I…
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 to He …
The dynamics of an x-ray-ionized two-component core-shell nanosystem is probed using doped helium (He) nanodroplets. First, a soft x-ray pump pulse selectively inner-shell ionizes the core cluster formed of heavier rare-gas atoms, causing electron migration from the He shell to the highly charged core. This ignites a He nanoplasma which is then driven by an intense near-infrared probe pulse. The ultrafast charge redistribution, evidenced by the rise of He$^+$ and He$^{2+}$ ion yields from the nanoplasma within $<70$ fs, leads to strong damping of the core cluster expansion. Thus, He droplets a…
This much revised and shortened PhD thesis contains many ideas that I could not follow up on, like self destructing beams in scattering cells, the depletion enhancing Wittig tube, ionic seeding via beta-decay foil or Langmuir-Taylor filaments, analysis of the popular <N> ~ Delta(N) relation in droplet size distributions, etc. Avoiding pasting again the usual that is found in many a thesis in the He-droplet field, we focus instead on what is presented insufficiently rigorous elsewhere, like chopper selection, ionization yield curves, or certain widely employed yet wrong derivations. It is not t…
High-resolution mass spectra of helium droplets doped with gold and ionized by electrons reveal He$_n$Au$^+$ cluster ions. Additional doping with heavy noble gases results in NenAu+, Ar$_n$Au$^+$, Kr$_n$Au$^+$, and Xe$_n$Au$^+$ cluster ions. The high stability predicted for covalently bonded Ar$_2$Au$^+$, Kr$_2$Au$^+$, and Xe$_2$Au$^+$ is reflected in their relatively high abundance. Surprisingly, the abundance of Ne$_2$Au$^+$ which is predicted to have zero covalent bonding character and no enhanced stability features a local maximum, too. The predicted size and structure of complete solvatio…
Coherent diffractive imaging of individual free nanoparticles has opened novel routes for the in-situ analysis of their transient structural, optical, and electronic properties. So far, single-shot single-particle diffraction was assumed to be feasible only at extreme ultraviolet (XUV) and X-ray free-electron lasers, restricting this research field to large-scale facilities. Here we demonstrate single-shot imaging of isolated helium nanodroplets using XUV pulses from a femtosecond-laser driven high harmonic source. We obtain bright wide-angle scattering patterns, that allow us to uniquely iden…
