We studied the recollision dynamics between the electrons and D$_2^+$ ions following the tunneling ionization of D$_2$ molecules in an intense short pulse laser field. The returning electron collisionally excites the D$_2^+$ ion to excited electronic states from there D$_2^+$ can dissociate or be further ionized by the laser field, resulting in D$^+$ + D or D$^+$ + D$^+$, respectively. We modeled the fragmentation dynamics and calculated the resulting kinetic energy spectrum of D$^+$ to compare with recent experiments. Since the recollision time is locked to the tunneling ionization time which occurs only within fraction of an optical cycle, the peaks in the D$^+$ kinetic energy spectra provides a measure of the time when the recollision occurs. This collision dynamics forms the basis of the molecular clock where the clock can be read with attosecond precision, as first proposed by Corkum and coworkers. By analyzing each of the elementary processes leading to the fragmentation quantitatively, we identified how the molecular clock is to be read from the measured kinetic energy spectra of D$^+$ and what laser parameters be used in order to measure the clock more accurately.
We report on the fragmentation dynamics of triply charged, diatomic, molecular ions of NO and CO. Dissociative fragmentation after multiple ionization of NO and CO is studied under the impact of 200 keV proton beam using recoil-ion momentum spectrometer. Kinetic Energy Release distributions (KERDs) for various fragmentation channels were obtained. We have also calculated the potential energy curves (PECs) for ground and several excited states of NO^{3+} and CO^{3+} molecular ion. The obtained KERDs are discussed in the background of the calculated PECs as well as the simple Coulomb excitation …
We study the fragmentation of very large dimers into two singly charged ions caused by absorption of a photon. In this process a photo electron emitted from one atom of the dimer has certain chances to hit the other atom knocking out one of its electrons. This results in the production of two singly charged ions and the consequent Coulomb explosion of the residual doubly charged system. We develop a theory of this process and apply it to calculate the fragmentation of $^4$He$_2$, $^7$Li - $^4$He and $^6$Li - $^4$He dimers. Our results for the helium dimer are in good agreement with available e…
Fragmentation of highly charged molecular ions or clusters consisting of more than two atoms can proceed in an onestep synchronous manner where all bonds break simultaneously or sequentially by emitting one ion after the other. We separated these decay channels for the fragmentation of CO23+ ions by measuring the momenta of the ionic fragments. We show that the total energy deposited in the molecular ion is a control parameter which switches between three distinct fragmentation pathways: the sequential fragmentation in which the emission of an O+ ion leaves a rotating CO2+ ion behind that frag…
We study the electron-impact induced ionization of O$_{2}$ from threshold to 120 eV using the electron spectroscopy method. Our approach is simple in concept and embodies the ion source with a collision chamber and a mass spectrometer with a quadruple filter as a selector for the product ions. The combination of these two devices makes it possible to unequivocally collect all energetic fragment ions formed in ionization and dissociative processes and to detect them with known efficiency. The ion source allows to vary and tune the electron-impact ionization energy and the target-gas pressure. W…
We study theoretically the fragmentation of the helium dimer, $^4$He$_2$, into singly charged ions in collisions with relativistic highly-charged projectiles. We discuss the main mechanisms driving this process with the focus on the fragmentation caused by direct ionization of both atomic sites of the dimer in a single collision with the projectile. This direct mechanism dominates the He$_2$ $\to $ He$^+$ + He$^+$ breakup events with the kinetic energies of the emerging ionic fragments below $4$--$5$ eV. We explore the energy and angular distributions of the He$^+$ ions produced in collisions …
We report an experimental and numerical study of the propagation of free-electron laser pulses (wavelength 24.3 nm) through helium gas. Ionisation and excitation populates the He$^{+}$ 4$p$ state. Strong, directional emission was observed at wavelengths of 469 nm, 164 nm, 30.4 nm, and 24.5 nm. We interpret the emissions at 469 nm and 164 nm as 4$p$-3$s$-2$p$ cascade superfluorescence, that at 30.4 nm as yoked superfluorescence on the 2$p$-1$s$ transition, and that at 25.6 nm as free-induction decay of the 3$p$ state.
Carrier envelope phase (CEP) stabilized pulses of intense 800 nm light of 5 fs duration are used to probe the dissociation dynamics of dications of isotopically-substituted water, HOD. HOD$^{2+}$ dissociates into either H$^+$ + OD$^+$ or D$^+$ + OH$^+$. The branching ratio for these two channels is CEP-dependent; the OD$^+$/OH$^+$ ratio (relative to that measured with CEP-unstabilized pulses) varies from 150% to over 300% at different CEP values, opening prospects of isotope-dependent control over molecular bond breakage. The kinetic energy released as HOD$^{2+}$ Coulomb explodes is also CEP-d…
Atomic ions confined in multi-electrode traps have been proposed as a basis for scalable quantum information processing. This scheme involves transporting ions between spatially distinct locations by use of time-varying electric potentials combined with laser or microwave pulses for quantum logic in specific locations. We report the development of a fast multi-channel arbitrary waveform generator for applying the time-varying electric potentials used for transport and for shaping quantum logic pulses. The generator is based on a field-programmable gate array controlled ensemble of 16-bit digit…
The description of threshold fragmentation under long range repulsive forces is presented. The dominant energy dependence near threshold is isolated by decomposing the cross section into a product of a back ground part and a barrier penetration probability resulting from the repulsive Coulomb interaction. This tunneling probability contains the dominant energy variation and it can be calculated analytically based on the same principles as Wannier's description for threshold ionization under attractive forces. Good agreement is found with the available experimental cross sections on detachment …
We image spatial distributions of Xe$^{q+}$ ions in the focus of a laser beam of ultrashort, intense pulses in all three dimensions, with a resolution of $\sim$3 $μ$m and $\sim$12 $μ$m in the two transverse directions. This allows for studying ionization processes without spatially averaging ion yields. Our \emph{in situ} ion imaging is also useful to analyze focal intensity profiles and to investigate the transverse modal purity of tightly focused beams of complex light. As an example, the intensity profile of a Hermite-Gaussian beam mode HG$_{1,0}$ recorded with ions is found to be in good a…
Singly ionized nitrogen molecules in ambient air pumped by near-infrared femtosecond laser give rise to superradiant emission. Here we demonstrate coherent control of this superradiance by injecting a pair of resonant seeding pulses inside the nitrogen gas plasma. Strong modulation of the 391.4 nm superradiance with a period of 1.3 fs is observed when the delay between the two seeding pulses are finely tuned, pinpointing the essential role of macroscopic coherence in this lasing process. Based on this time-resolved method, the complex temporal evolution of the macroscopic coherence between two…
We report the analysis of paired photon pulses arising from two cascading transitions in continuously pumped Erbium-doped YLiF$_4$ 1% and 0.01% crystals at 1.6 K. The dependence of the pulse peak intensity on the squared number of involved Erbium ions, between 10$^{11}$ and 10$^{13}$, definitely identifies the cooperative nature of the two pulsed emissions, that are generated by the subsequent, spontaneous formation of coherent states. The observed fluctuations of the time interval between the paired pulses and, most importantly, its correlation with the second pulse duration, demonstrate that…
We use a pulsed nitrogen laser to produce atomic ions by laser ablation, measuring the relative ion yield for several elements, including some that have only recently been proposed for use in cold trapped ion experiments. For barium, we monitor the ion yield as a function of the number of applied ablation pulses for different substrates. We also investigate the ion production as a function of the pulse energy, and the efficiency of loading an ion trap as a function of radiofrequency voltage.
A simple model for sequential multiphoton ionization by ultra-intense x-rays is presented. The derived scaling of the ion yield with pulse energy quantitatively reproduces the experimental data, which shows that the ion yield increases according to the "power law" behavior typical of multiphoton ionization, followed by saturation at high pulse energies. The calculated average time interval between ionizations for producing ions at a certain charge state is found to be proportional to the pulse duration and independent of all other x-ray pulse parameters. This agrees with previous studies where…
We have investigated the all-optical generation of ions by photo-ionisation of atoms generated by pulsed laser ablation. A direct comparison between a resistively heated oven source and pulsed laser ablation is reported. Pulsed laser ablation with 10 ns Nd:YAG laser pulses is shown to produce large calcium flux, corresponding to atomic beams produced with oven temperatures greater than 650 K. For an equivalent atomic flux, pulsed laser ablation is shown to produce a thermal load more than one order of magnitude smaller than the oven source. The atomic beam distributions obey Maxwell-Boltzmann …
We study a hybrid quantum system composed of an ion and an electric dipole. We show how a trapped ion can be used to measure the small electric field generated by a classical dipole. We discuss the application of this scheme to measure the electric dipole moment of cold polar molecules, whose internal state can be controlled with ultrafast laser pulses, by trapping them in the vicinity of a trapped ion.
Calculations on the dynamics of ions and electrons in near-infrared laser fields at intensities up to $3 \times 10^{23}$ W/cm$^2$ are presented. We explore the acceleration of ions in a laser focus by conservation of canonical momentum during ionization events and by the ponderomotive force in the f/1 focal geometry required to reach such intensity. At intensity exceeding 10$^{23}$ W/cm$^2$, highly charged ions are expelled from the laser focus before they can interact with the laser pulse at peak intensity, decreasing the predicted ionization yields of deeply-bound states. We consider the int…
High harmonic generation in benzene is studied using a mixed quantum-classical approach in which the electrons are described using time-dependent density functional theory while the ions move classically. The interaction with both circularly and linearly polarised infra-red ($λ= 800$ nm) laser pulses of duration 10 cycles (26.7 fs) is considered. The effect of allowing the ions to move is investigated as is the effect of including self-interaction corrections to the exchange-correlation functional. Our results for circularly polarised pulses are compared with previous calculations in which the…
We report on coherent control of excitation processes of translationally ultracold rubidium dimers in a magneto-optical trap by using shaped femtosecond laser pulses. Evolution strategies are applied in a feedback loop in order to optimize the photoexcitation of the Rb2 molecules, which subsequently undergo ionization or fragmentation. A superior performance of the resulting pulses compared to unshaped pulses of the same pulse energy is obtained by distributing the energy among specific spectral components. The demonstration of coherent control to ultracold ensembles opens a path to actively i…
An apparatus for production of various atomic and molecular ions inside a linear Paul trap has been set up. The system applies a custom-made, low energy, pulsed electron gun to produce ions in electron impact process. Such ionization method can find some interesting possible applications such as derivation of ions inaccessible other-ways, which can be used in molecular ion experiments. The technique allows also for determination of cross sections for various collisional processes. As a feasibility study, the apparatus was used for determination of ionization integral cross section of calcium i…
A scheme to infer the temporal coherence of EUV frequency combs generated from intra-cavity high-order harmonic generation is put forward. The excitation dynamics of highly charged Mg-like ions, interacting with EUV pulse trains featuring different carrier-envelope-phase fluctuations, are simulated. While demonstrating the microscopic origin of the macroscopic equivalence between excitations induced by pulse trains and continuous-wave lasers, we show that the coherence time of the pulse train can be determined from the spectrum of the excitations. The scheme will provide a verification of the …
We demonstrate the efficient generation of Be$^+$ ions with a 60 ns and 150 nJ laser pulse near 235 nm for two-step photo-ionization, proven by subsequent counting the number of ions loaded into a linear Paul trap. The bandwidth and power of the laser pulse are chosen in such a way that a first, resonant step fully saturates the entire velocity distribution of beryllium atoms effusing from a thermal oven. The second excitation step is driven by the same light field causing efficient non-resonant ionization. Our ion-loading scheme is more than 15 times more efficient as compared to former pathw…
A model based on the strong-field and Born-Oppenheimer approximations qualitatively describes the distribution over vibrational states formed in a diatomic molecular ion following ionization of the neutral molecule by intense laser pulses. Good agreement is found with a recent experiment [X. Urbain et al., Phys. Rev. Lett. 92, 163004 (2004)]. In particular, the observed deviation from a Franck-Condon-like distribution is reproduced. Additionally, we demonstrate control of the vibrational distribution by a variation of the peak intensity or a change of frequency of the laser pulse.
In molecular photofragmentation processes by soft X-rays, a number of ionic fragments can be produced, each having a different abundance and correlation with the emitted electron kinetic energy. For investigating these fragmentation processes, electron-ion and electron-ion-ion coincidence experiments, in which the kinetic energy of electrons are analyzed using an electrostatic analyzer while the mass of the ions is analyzed using a pulsed electric field, are very powerful. For such measurements, however, the contribution of random coincidences is substantial and affects the data in a non-trivi…
We present experimental results on the ionization/dissociation of methane in femtosecond pulses of radiation. Angular and intensity dependent yields of singly and doubly charged species were measured using an imaging mass spectrometer. The measured data shows that all fragments yields exhibit some degree of anisotropy as a result of them being preferably ejected parallel to the polarization direction. Additionally, an anomalous perpendicular fragmentation pattern is found for CH\-(2)\+(2+). We find evidence of multiple dissociation mechanisms including statistical decay, field assisted dissoci…
We have probed the fragmentation dynamics in a bent triatomic molecule, water, a non-planar molecule, methanol, and a planar ring-structured molecule, benzene, using 100 fs duration pulses of linearly and circularly polarized, infrared, intensity-selected laser light. At laser intensities larger than 10$^{15}$ W cm$^{-2}$, the yield of singly and multiply charged atomic fragments from these molecules is suppressed when the light is circularly polarized. At lower intensities, the fragment ion yield is not significantly polarization dependent. This hitherto-unobserved intensity dependent effect …
We demonstrate parallel composite quantum logic gates with phases implemented locally through nanoscale movement of ions within a global laser beam of fixed pulse duration. We show that a simple four-pulse sequence suffices for constructing ideal arbitrary single-qubit rotations in the presence of large intensity inhomogeneities across the ion trap due to laser beam-pointing or beam-focusing. Using such sequences, we perform parallel arbitrary rotations on ions in two trapping zones separated by 700 $μ$m with fidelities comparable to those of our standard laser-controlled gates. Our scheme imp…
We experimentally observe the action of multiple light pulses on the transverse motion of a continuous beam of fullerenes. The light potential is generated by non-resonant ultra-short laser pulses in perpendicular spatial overlap with the molecule beam. We observe a small but clear enhancement of the number of molecules in the center fraction of the molecular beam. Relatively low light intensity and short laser pulse duration prevent the molecule from fragmentation and ionization. Experimental results are confirmed by Monte Carlo trajectory simulations.
We demonstrate that the formation of negative hydrogen ions (H-) occurs in a wide class of atomic and molecular collisions. In our experiments, H- emission from hydroxyl cations and acetone molecules was observed in keV-energy collisions. We show that hydride (H-) anions are formed via direct collisional fragmentation of molecules, followed by electron grabbing by fast hydrogen fragments. Such general mechanism in hydrogen-containing molecules may significantly influence reaction networks in planetary atmospheres and astrophysical media and new reaction pathways may have to be added in radioly…
We simulate the pump-probe experiments of lasing in molecular nitrogen ions with particular interest on the effects of rotational wave-packet dynamics. Our computations demonstrate that the coherent preparation of rotational wave packets in N$_2^+$ by an intense short non-resonant pulse results in a modulation of the subsequent emission from $B^2Σ_u^+ \rightarrow X^2Σ_g^+$ transitions induced by a resonant seed pulse. We model the dynamics of such pumping and emission using density matrix theory to describe the N$_2^+$ dynamics and the Maxwell wave equation to model the seed pulse propagation.…
A photofragmentation study of gas-phase indole (C$_8$H$_7$N) upon single-photon ionization at a photon energy of 420 eV is presented. Indole was primarily inner-shell ionized at its nitrogen and carbon $1s$ orbitals. Electrons and ions were measured in coincidence by means of velocity map imaging. The angular relationship between ionic fragments is discussed along with the possibility to use the angle-resolved coincidence detection to perform experiments on molecules that are strongly oriented in their recoil-frame. The coincident measurement of electrons and ions revealed fragmentation-pathwa…
Carrier envelope phase (CEP) stabilized 5 fs and 22 fs pulses of intense 800 nm light are used to probe the strong-field ionization dynamics of multielectron entities, xenon and carbon disulfide. We compare ion yields obtained with and without CEP-stabilization: with 8-cycle (22 fs) pulses, Xe$^{6+}$ yields are suppressed (relative to Xe$^+$ yields) by between 30% and 50%, depending on phase, reflecting the phase dependence of non-sequential ionization and its contribution to the formation of higher charge states. On the other hand, ion yields for Xe$^{q+}$ ($q$=2-4) with CEP-stablized pulses …
