The way conduction electrons respond to ultrafast external perturbations in low dimensional materials is at the core of the design of future devices for (opto)electronics, photodetection and spintronics. Highly charged ions provide a tool for probing the electronic response of solids to extremely strong electric fields localized down to nanometre-sized areas. With ion transmission times in the order of femtoseconds, we can directly probe the local electronic dynamics of an ultrathin foil on this timescale. Here we report on the ability of freestanding single layer graphene to provide tens of electrons for charge neutralization of a slow highly charged ion within a few femtoseconds. With values higher than 1012 A cm−2, the resulting local current density in graphene exceeds previously measured breakdown currents by three orders of magnitude. Surprisingly, the passing ion does not tear nanometre-sized holes into the single layer graphene. We use time-dependent density functional theory to gain insight into the multielectron dynamics.

The impact of a highly charged ion onto a solid gives rise to charge exchange between the ion and target atoms, so that a slow ion gets neutralized in the vicinity of the surface. Using highly charged Ar and Xe ions and the surface-only material graphene as a target, we show that the neutralization and deexcitation of the ions proceeds on a sub-10 fs time scale. We further demonstrate that a multiple Interatomic Coulombic Decay (ICD) model can describe the observed ultrafast deexcitation. Other deexcitation mechanisms involving nonradiative decay and quasimolecular orbital formation during the impact are not important, as follows from the comparison of our experimental data with the results of first-principles calculations. Our method also enables the estimation of ICD rates directly.

Experimental charge exchange and energy loss data for the transmission of slow highly charged Xe ions through ultra-thin polymeric carbon membranes are presented. Surprisingly, two distinct exit charge state distributions accompanied by charge exchange dependent energy losses are observed. The energy loss for ions exhibiting large charge loss shows a quadratic dependency on the incident charge state indicating that equilibrium stopping force values do not apply in this case. Additional angle resolved transmission measurements point on a significant contribution of elastic energy loss. The observations show that regimes of different impact parameters can be separated and thus a particle's energy deposition in an ultra-thin solid target may not be described in terms of an averaged energy loss per unit length. Modern approaches in ion and electron irradiation of solids such as nano-structuring of thin films or even structuring of free-standing monolayers such as graphene [1][2][3] or MoS 2 [4, 5] rely on models for structural and electronic defect formation. Most important for processes during ion-solid interaction is the amount of deposited energy and its dissipation channels [6]. We show that the energy loss and charge exchange of ions in very thin films, such as 2D-materials, show significant differences to solids with reduced thickness. The understanding of these differences is not only of importance for ion beam analysis of 2D-materials but in particular for manipulating and tailoring their properties. [7]. To probe interaction processes in very thin target materials slow highly charged ions (HCI) are ideal tools due to their energy deposition confinement to shallow surface regions. Besides the well known near-surface potential energy deposition [8,9] also an expected increased pre-equilibrium kinetic energy loss (stopping force) [10] is confined to a few nm at the surface. In the conventional description of both contributions to the stopping force, i.e. nuclear and electronic stopping, the charge state of an ion is identified with its equilibrium charge state by Bohr's stripping criterion [11,12]. The equilibrium charge state by Bohr is given as Q eq = Z 1/3 v/v 0 and describes the (average) charge state of an ion passing through a solid at a given velocity v (v 0 : Bohr's velocity, Z: nuclear charge of the ion). The charge state Q of slow highly charged ions is much higher than the equilibrium charge state Q eq (Q eq Q < ∼ Z). Therefore, the interaction of HCI with surfaces may not be described in terms of an equilibrium charge state dependent stopping force. Furthermore, due to the localization of the energy deposition slow HCI can be used as an efficient tool for surface nano-structuring [13][14][15][16][17][18][19][20][21][22][23][24] and tuning of the electrical properties of materials [25], as well as a probe for surface energy deposition processes [26,27]. Recently, it has been shown that slow HCI can create pores in 1 nm thick carbon nanomembranes (CNM) [28,29] mainly by deposition of their potential ...

Guiding of highly charged ions through tilted capillaries promises to develop into a tool to efficiently collimate and focus low-energy ion beams to sub-micrometer spot size. One control parameter to optimize guiding is the residual electrical conductivity of the insulating material. Its strong, nearly exponential temperature dependence is the key to transmission control and can be used to suppress transmission instabilities arising from flux fluctuations of incident ions which otherwise would lead to Coulomb blocking of the capillary. We demonstrate the strong dependence of transmission of Ar 7+ ions through a single macroscopic glass capillary on temperature and ion flux. Results in the regime of dynamical equilibrium can be described by balance equations in the linear-response regime.

The retinal protonated Schiff-base (RPSB) in its all-trans form is found in bacterial rhodopsins, whereas visual rhodopsin proteins host 11-cis RPSB. In both cases, photoexcitation initiates fast isomerization of the retinal chromophore, leading to proton transport, storage of chemical energy or signaling. It is an unsolved problem, to which degree this is due to protein interactions or intrinsic RPSB quantum properties. Here, we report on time-resolved action-spectroscopy studies, which show, that upon photoexcitation, cis isomers of RPSB have an almost barrierless fast 400 fs decay, whereas all-trans isomers exhibit a barrier-controlled slow 3 ps decay. Moreover, formation of the 11-cis isomer is greatly favored for all-trans RPSB when isolated. The very fast photoresponse of visual photoreceptors is thus directly related to intrinsic retinal properties, whereas bacterial rhodopsins tune the excited state potential-energy surface to lower the barrier for particular double-bond isomerization, thus changing both the timescale and specificity of the photoisomerization.

This roadmap article highlights recent advances, challenges and future prospects in studies of the dynamics of molecules and clusters in the gas phase. It comprises nineteen contributions by scientists with leading expertise in complementary experimental and theoretical techniques to probe the dynamics on timescales spanning twenty order of magnitudes, from attoseconds to minutes and beyond, and for systems ranging in complexity from the smallest (diatomic) molecules to clusters and nanoparticles. Combining some of these techniques opens up new avenues to unravel hitherto unexplored reaction pathways and mechanisms, and to establish their significance in, e.g.  radiotherapy and radiation damage on the nanoscale, astrophysics, astrochemistry and atmospheric science. Graphic abstract

Modification of surface and bulk properties of solids by irradiation with ion beams is a widely used technique with many applications in material science. In this study, we show that nano-hillocks on CaF2 crystal surfaces can be formed by individual impact of medium energy (3 and 5 MeV) highly charged ions (Xe22+ to Xe30+) as well as swift (kinetic energies between 12 and 58 MeV) heavy xenon ions. For very slow highly charged ions the appearance of hillocks is known to be linked to a threshold in potential energy (Ep) while for swift heavy ions a minimum electronic energy loss per unit length (Se) is necessary. With our results we bridge the gap between these two extreme cases and demonstrate, that with increasing energy deposition via Se the Ep-threshold for hillock production can be lowered substantially. Surprisingly, both mechanisms of energy deposition in the target surface seem to contribute in an additive way, which can be visualized in a phase diagram. We show that the inelastic thermal spike model, originally developed to describe such material modifications for swift heavy ions, can be extended to the case where both kinetic and potential energies are deposited into the surface.

Cross-linking of a self-assembled monolayer of 1,1'-biphenyl-4-thiol by low energy electron irradiation leads to the formation of a carbon nanomembrane, which is only 1 nm thick. Here we study the perforation of these freestanding membranes by slow highly charged ion irradiation with respect to the pore formation yield. It is found that a threshold in potential energy of the highly charged ions of about 10 keV must be exceeded in order to form round pores with tunable diameters in the range of 5-15 nm. Above this energy threshold the efficiency for a single ion to form a pore increases from 70% to nearly 100% with increasing charge state. These findings are verified by two independent methods, namely the analysis of individual membranes stacked together during irradiation and the detailed analysis of exit charge state spectra utilizing an electrostatic analyzer.