Velocity Map Imaging Spectrometer Research Articles

A Versatile Velocity Map Ion-Electron Covariance Imaging Spectrometer for High-Intensity XUV Experiments

We report on the design and performance of a velocity map imaging (VMI) spectrometer optimized for experiments using high-intensity extreme ultraviolet (XUV) sources such as laser-driven high-order harmonic generation (HHG) sources and free-electron lasers (FELs). Typically exhibiting low repetition rates and high single-shot count rates, such experiments do not easily lend themselves to coincident detection of photo-electrons and -ions. In order to obtain molecular frame or reaction channel-specific information, one has to rely on other correlation techniques, such as covariant detection schemes. Our device allows for combining different photo-electron and -ion detection modes for covariance analysis. We present the expected performance in the different detection modes and present the first results using an intense high-order harmonic generation (HHG) source.

Time-resolved and spectrally resolved ionization with a single ultrashort XUV-IR beamline

We present a simple upgrade of a time-resolved attosecond extreme ultraviolet and infrared (XUV-IR) setup designed to perform time-resolved or spectrally resolved studies of a target under similar experimental conditions. A flat XUV grating inserted in the path of an attosecond pulse train obtained via high order harmonic generation in gases is used either in the zeroth order of diffraction to follow attosecond dynamics or in the first order of diffraction to study the target spectral response with a temporally stretched single harmonic. Electron momentum measurement is performed with a velocity map imaging spectrometer, and the 10 W femtosecond laser system operating at 5 kHz provides an XUV photon flux compatible with rapid acquisition in both the monochromatic and broadband configurations. The change of experimental configuration between broadband and monochromatic sources is rapid and performed in situ. We present the experimental implementation applied to krypton atoms and detail the capabilities and limits of this approach when an XUV grating with constant groove density is used with a converging XUV beam.

Fragmentation of endohedral fullerene Ho3N@C80 in an intense femtosecond near-infrared laser field

The fragmentation of gas phase endohedral fullerene, $\mathrm{H}{\mathrm{o}}_{3}\mathrm{N}@{\mathrm{C}}_{80}$, was investigated using femtosecond near-infrared laser pulses with an ion velocity map imaging spectrometer. We observed that $\mathrm{H}{\mathrm{o}}^{+}$ abundance associated with carbon cage opening dominates at an intensity of $1.1\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.16em}{0ex}}\mathrm{W}/\mathrm{c}{\mathrm{m}}^{2}$. As the intensity increases, the $\mathrm{H}{\mathrm{o}}^{+}$ yield associated with multifragmentation of the carbon cage exceeds the prominence of $\mathrm{H}{\mathrm{o}}^{+}$ associated with the gentler carbon cage opening. Moreover, the power law dependence of $\mathrm{H}{\mathrm{o}}^{+}$ on laser intensity indicates that the transition of the most likely fragmentation mechanisms occurs around $2.0\ifmmode\times\else\texttimes\fi{}{10}^{14}\phantom{\rule{0.16em}{0ex}}\mathrm{W}/\mathrm{c}{\mathrm{m}}^{2}$.

A New kHz Velocity Map Ion/Electron Imaging Spectrometer for Femtosecond Time-Resolved Molecular Reaction Dynamics Studies

A new velocity map imaging spectrometer is constructed for molecular reaction dynamics studies using time-resolved photoelectron/ion spectroscopy method. By combining a kHz pulsed valve and an ICCD camera, this velocity map imaging spectrometer can be run at a repetition rate of 1 kHz, totally compatible with the fs Ti:Sapphire laser system, facilitating time-resolved studies in gas phase which are usually time-consuming. Time-resolved velocity map imaging study of NH3 photodissociation at 200 nm was performed and the time-resolved total kinetic energy release spectrum of H+NH2 products provides rich information about the dissociation dynamics of NH3. These results show that this new apparatus is a powerful tool for investigating the molecular reaction dynamics using time-resolved methods.

A compact design for velocity-map imaging of energetic electrons and ions.

We present a compact design for a velocity-map imaging spectrometer for energetic electrons and ions. The standard geometry by Eppink and Parker [Rev. Sci. Instrum. 68, 3477 (1997)] is augmented by just two extended electrodes so as to realize an additional einzel lens. In this way, for a maximum electrode voltage of 7 kV, we experimentally demonstrate imaging of electrons with energies up to 65 eV. Simulations show that energy acceptances ≲270 and ≲1200 eV with an energy resolution ΔE∕E≲5% are achievable for electrode voltages ≤20 kV when using diameters of the position-sensitive detector of 42 and 78 mm, respectively.

Alignment, orientation, and Coulomb explosion of difluoroiodobenzene studied with the pixel imaging mass spectrometry (PImMS) camera.

Laser-induced adiabatic alignment and mixed-field orientation of 2,6-difluoroiodobenzene (C6H3F2I) molecules are probed by Coulomb explosion imaging following either near-infrared strong-field ionization or extreme-ultraviolet multi-photon inner-shell ionization using free-electron laser pulses. The resulting photoelectrons and fragment ions are captured by a double-sided velocity map imaging spectrometer and projected onto two position-sensitive detectors. The ion side of the spectrometer is equipped with a pixel imaging mass spectrometry camera, a time-stamping pixelated detector that can record the hit positions and arrival times of up to four ions per pixel per acquisition cycle. Thus, the time-of-flight trace and ion momentum distributions for all fragments can be recorded simultaneously. We show that we can obtain a high degree of one-and three-dimensional alignment and mixed-field orientation and compare the Coulomb explosion process induced at both wavelengths.

Soft X-ray spectroscopy of nanoparticles by velocity map imaging.

Velocity map imaging (VMI), a technique traditionally used to study chemical dynamics in the gas phase, is applied here to study X-ray photoemission from aerosol nanoparticles. Soft X-rays from the Advanced Light Source synchrotron, probe a beam of nanoparticles, and the resulting photoelectrons are velocity mapped to obtain their kinetic energy distributions. A new design of the VMI spectrometer is described. The spectrometer is benchmarked by measuring vacuum ultraviolet photoemission from gas phase xenon and squalene nanoparticles followed by measurements using soft X-rays. It is demonstrated that the photoelectron distribution from X-ray irradiated squalene nanoparticles is dominated by secondary electrons. By scanning the photon energies and measuring the intensities of these secondary electrons, a near edge X-ray absorption fine structure (NEXAFS) spectrum is obtained. The NEXAFS technique is used to obtain spectra of aqueous nanoparticles at the oxygen K edge. By varying the position of the aqueous nanoparticle beam relative to the incident X-ray beam, evidence is presented such that the VMI technique allows for NEXAFS spectroscopy of water in different physical states. Finally, we discuss the possibility of applying VMI methods to probe liquids and solids via X-ray spectroscopy.

An experimental setup to study delayed electron emission upon photoexcitation of trapped polyatomic anions.

A Velocity Map Imaging (VMI) spectrometer has been designed and integrated with an electrostatic ion beam trap to study delayed electron emission from trapped polyatomic anions upon photodetachment. The VMI spectrometer is small in size and can record a wide range of photoelectron energies, with variable magnification. Delayed electron emission can be recorded in our experimental setup for any time duration after the photoexcitation of the polyatomic anions. Experiments were carried out with trapped O- and C5- ions to demonstrate the capability of the spectrometer. Delayed electron emissions from C5- as well as prompt photoelectrons from O- were detected by the VMI spectrometer upon photoexcitation. The design and performance of the spectrometer are presented in detail.

Photofragmentation dynamics and dissociation energies of MoO and CrO.

Neutral metal-containing molecules and clusters present a particular challenge to velocity map imaging techniques. Common methods of choice for producing such species-such as laser ablation or magnetron sputtering-typically generate a wide variety of metal-containing species and, without the possibility of mass-selection, even determining the identity of the dissociating moiety can be challenging. In recent years, we have developed a velocity map imaging spectrometer equipped with a laser ablation source explicitly for studying neutral metal-containing species. Here, we report the results of velocity map imaging photofragmentation studies of MoO and CrO. In both cases, dissociation at the two- and three-photon level leads to fragmentation into a range of product channels, some of which can be confidently assigned to particular Mo* (Cr*) and O atom quantum states. Analysis of the kinetic energy release spectra as a function of photon energy allows precise determination of the ground state dissociation energies of MoO (=44 064 ± 133 cm-1) and CrO (=37 197 ± 78 cm-1), respectively.

Ion-ion coincidence imaging at high event rate using an in-vacuum pixel detector.

A new ion-ion coincidence imaging spectrometer based on a pixelated complementary metal-oxide-semiconductor detector has been developed for the investigation of molecular ionization and fragmentation processes in strong laser fields. Used as a part of a velocity map imaging spectrometer, the detection system is comprised of a set of microchannel plates and a Timepix detector. A fast time-to-digital converter (TDC) is used to enhance the ion time-of-flight resolution by correlating timestamps registered separately by the Timepix detector and the TDC. In addition, sub-pixel spatial resolution (<6 μm) is achieved by the use of a center-of-mass centroiding algorithm. This performance is achieved while retaining a high event rate (104 per s). The spectrometer was characterized and used in a proof-of-principle experiment on strong field dissociative double ionization of carbon dioxide molecules (CO2), using a 400 kHz repetition rate laser system. The experimental results demonstrate that the spectrometer can detect multiple ions in coincidence, making it a valuable tool for studying the fragmentation dynamics of molecules in strong laser fields.

The coincident measurement in the experimental atomic molecular research

The targets of atomic molecular physics are atoms or molecules consist of a few atoms. Due to their simple geometrical structure, in order to obtain unrevealed properties, the advanced experimental techniques are often required to view the target from multi view-points and follow the history of the relevant states if possible. This scientific desire drives us to promote the technical specification and flexibility of instruments. Here, we reviewed several coincident setup, they are based on: field free electron time of flight spectrometer, electron energy-dispersive analyzer, magnetic bottle spectrometer, reaction microscope and velocity map imaging spectrometer. They are widely used in the experiments based on ultrafast laser, free electron laser and synchrotron radiation. We give not only the description of the working principles and the technical differences among them, but also put emphasize on the recent scientific desires and possible breakthroughs.

Low energy electron attenuation lengths in core-shell nanoparticles.

A velocity map imaging spectrometer is used to measure photoemission from free core-shell nanoparticles, where a salt core is coated with a liquid hydrocarbon shell (i.e. squalane). By varying the radial thickness of the hydrocarbon shell, electron attenuation lengths (EALs) are determined by measuring the decay in photoemission intensity from the salt core. In squalane, electrons with kinetic energy (KE) above 2 eV are found to have EALs of 3-5 nm, whereas electrons with smaller KE (<2 eV) have significantly larger EALs of >15 nm. These results (in the context of other energy-resolved EAL measurements) suggest that the energy dependent behavior of low energy electrons is similar in dielectrics when KE > 2 eV. At this energy the EALs do not appear to exhibit strong energy dependence. However, at very low KE (<2 eV), the EALs diverge and appear to be extremely material dependent.

Probing the Heterogeneous Ozonolysis of Squalene Nanoparticles by Photoemission.

The heterogeneous reaction of ozone (O3) with 200 nm squalene nanoparticles is studied using near-edge X-ray absorption fine structure (NEXAFS) and ultraviolet (UPS) and X-ray photoelectron spectroscopy (XPS). Photoelectrons are detected from free nanoparticle beams using a velocity map imaging (VMI) spectrometer capable of detecting photoelectrons with up to 40 eV of kinetic energy. Heterogeneous kinetics are quantified using changes in the UPS, XPS, and NEXAFS spectrum, yielding uptake coefficients for the decay of the double bonds in squalene of (3.1 ± 0.7) × 10-4, (2.6 ± 0.6) × 10-4, and (2.9 ± 0.7) × 10-4, respectively. When comparing these values with the uptake coefficient, (1.0 ± 0.2) × 10-3, determined by the molecular decay of squalene measured with aerosol mass spectrometry, it is found that on average 1.6 ± 0.2 double bonds are removed for each ozone-squalene reactive collision, suggesting the importance of evaporation of small molecular weight reaction products from the aerosol. From further analysis of the nanoparticle XPS spectrum, it is found that ozonolysis increases the oxygen-to-carbon (O:C) ratio of the aerosol to 0.43 ± 0.03 and produces 16 ± 4% and 84 ± 4% secondary ozonides and carbonyls, respectively. The methods developed here show how aerosol photoemission can be used to quantify heterogeneous reaction on free nanoparticles.

Adiabatic Mixed-Field Orientation of Ground-State-Selected Carbonyl Sulfide Molecules.

A strong adiabatic mixed-field orientation (Nup /Ntot =0.882) of carbonyl sulfide (OCS) molecules in their absolute ground state is experimentally demonstrated. OCS is oriented in a combination of nonresonant laser and static electric fields inside a two-plate velocity map imaging spectrometer. The transition from nonadiabatic to adiabatic orientation for the rotational ground state is studied by varying the applied laser intensity and static electric field. Above static electric field strengths of 10 kV cm-1 and laser intensities of 1011 W cm-2 the observed degree of orientation reaches a plateau. These results are in good agreement with computational solutions of the time-dependent Schrödinger equation.

An aplanatic-lens velocity map imaging spectrometer with improved kinetic energy resolution for photoions

We propose a new method to improve the energy resolution of photoions with an aplanatic velocity map imaging spectrometer. Building on the traditional VMI spectrometer with three aperture electrodes, we apply a stepped voltage on the extractor electrode of the spectrometer to reduce the spherical aberration effect of the electrostatic lens. This stepped voltage acts as a diverging electrostatic lens in ion optics. A combination of the converging electrostatic lens and the subsequent diverging electrostatic lens constitutes an aplanatic electrostatic lens. With precisely controlling the moment of the voltage, we suppress the spherical aberration effect induced by the converging electrostatic lens in the traditional VMI spectrometer. Both simulated and experimental results demonstrate that the energy resolution is significantly improved using this aplanatic-lens VMI spectrometer.

An instrument combining an electrospray ionization source and a velocity-map imaging spectrometer for studying delayed electron emission of polyanions.

An instrument combining an electrospray ionization source and a velocity-map imaging (VMI) spectrometer has been developed in order to study the delayed electron emission of molecular anions and especially of polyanions. It operates at a high repetition rate (kHz) in order to increase the acquisition speed. The VMI spectrometer has been upgraded for nanosecond time resolution by gating the voltages applied on the position-sensitive detector. Kinetic energy release distribution of thermionic emission (without any contribution from direct detachment) can be recorded for well-defined delays after the nanosecond laser excitation. The capability of the instrument is demonstrated by recording photodetachment spectra of the benchmark C60(-) anion and C84(2-) dianion.

Angular distribution and circular dichroism in the two-colour XUV+NIR above-threshold ionization of helium

The photoelectron angular distribution and the circular dichroism in two-colour XUV+NIR above-threshold ionization of helium atoms have been investigated both experimentally and theoretically. Circularly polarized XUV pulses from the free electron laser FERMI have been spatially and temporally overlapped with circularly polarized optical pulses in the interaction region with an atomic helium jet. The emitted electrons were energy and angle analyzed by means of a velocity map imaging spectrometer. Asymmetry parameters of the angular distribution were determined and compared to theoretical predictions based on the strong field approximation and perturbation theory, respectively. For low NIR intensities, the ratio of the partial waves in the two-photon ionization process and their relative phase could be deduced. For high NIR intensities, the influence of multi-photon processes is discussed. Circular dichroism was revealed in both cases and is in good agreement with the results of the strong field approximation.

Influence of the interaction volume on the kinetic energy resolution of a velocity map imaging spectrometer**Project supported by the National Natural Science Foundation of China (Grant Nos. 11234004 and 61275126).

We investigate the influence of the interaction volume on the energy resolution of a velocity map imaging spectrometer. The simulation results show that the axial interaction size has a significant influence on the resolution. This influence is increased for a higher kinetic energy. We further show that the radial interaction size has a minor influence on the energy resolution for the electron or ion with medium energy, but it is crucial for the resolution of the electron or ion with low kinetic energy. By tracing the flight trajectories we show how the electron or ion energy resolution is influenced by the interaction size.

Electron spectroscopy of rare-gas clusters irradiated by x-ray free-electron laser pulses from SACLA

We have measured electron energy spectra and asymmetry parameters of Ar clusters and Xe clusters illuminated by intense x-rays at 5 and 5.5 keV. A velocity map imaging spectrometer was developed for this purpose and employed at an x-ray free-electron laser facility, SACLA in Japan. The cluster size dependence and the peak fluence dependence of the electron spectra and asymmetry parameters are discussed.

Interference stabilization of autoionizing states in molecular N2 studied by time- and angular-resolved photoelectron spectroscopy.

An autoionizing resonance in molecular N2 is excited by an ultrashort XUV pulse and probed by a subsequent weak IR pulse, which ionizes the contributing Rydberg states. Time- and angular-resolved photoelectron spectra recorded with a velocity map imaging spectrometer reveal two electronic contributions with different angular distributions. One of them has an exponential decay rate of 20 ± 5 fs, while the other one is shorter than 10 fs. This observation is interpreted as a manifestation of interference stabilization involving the two overlapping discrete Rydberg states. A formalism of interference stabilization for molecular ionization is developed and applied to describe the autoionizing resonance. The results of calculations suggest, that the effect of the interference stabilization is facilitated by rotationally-induced couplings of electronic states with different symmetry.