0000000000009761
AUTHOR
Manuel Vogel
Laser Investigations of Stored Metal Cluster Ions
The combination of ion storage in a Penning trap and photoexcitation by pulsed lasers has proven to be a versatile instrument in metal cluster research. Recent experiments which make use of both components allow a detailed study of the clusters' properties. In particular, a new method to measure dissociation energies is reviewed and preliminary results on the competition between electron emission and neutral monomer evaporation from dianionic metal clusters are presented.
Electron impact ionization/dissociation of size selected gold cluster cations
Abstract Singly charged gold clusters, Au n + in the size range n =12 to 72 have been captured and stored in a Penning trap, size selected and subjected to an electron beam. This interaction leads to further ionization as well as dissociation. The resulting abundance spectra of doubly and triply charged clusters show (a) a lower size limit for the production of multiply charged clusters from an ensemble of hot precursors, which can be understood in terms of the respective decay pathways, (b) an odd/even alternation of singly and doubly charged clusters in the size range below n =30, which inverses sign with change of charge state, and (c) magic numbers, i.e. prominent signals for particular…
Decay pathways of small gold clusters
The decay pathway competition between monomer and dimer evaporation of photoexcited cluster ions Au + n, n = 2-27, has been investigated by photodissociation of size-selected gold clusters stored in a Penning trap. For n > 6 the two decay pathways are distinguished by their experimental signature in time-resolved measurements of the dissociation. For the smaller clusters, simple fragment spectra were used. As in the case of the other copper-group elements, even-numbered gold cluster ions decay exclusively by monomer evaporation, irrespective of their size. For small odd-size gold clusters, dimer evaporation is a competitive alternative, and the smaller the odd-sized clusters, the more likel…
Determination of the g-Factor of Single Hydrogen-Like Ions by Mode Coupling in a Penning Trap
A method has been developed and applied for the determination of the electronic g-factor of single hydrogen-like ions stored in a Penning trap. The method is based on mode coupling of the ion trapping motions and is conceptionally advantageous as compared to previously used methods. It has been applied to hydrogen-like oxygen 16O7+ and yields a value for the gJ-factor which is in agreement with previously determined values. Experimental requirements and possibilities of the new method are discussed.
Model-free determination of dissociation energies of polyatomic systems.
We describe and apply a new procedure that allows a direct determination of dissociation energies of polyatomic systems (clusters, fullerenes, polymers, and other molecules) without any modeling of the systems under investigation. As an example, we have determined the dissociation energies of a series of gold clusters Au(+)n. A comparison with values obtained from statistical models of unimolecular dissociation shows that these models significantly fail to describe the data. In contrast, the new method yields values which are an order of magnitude more accurate, thus allowing one to experimentally set benchmarks for any theory which attempts to describe activated processes.
Electronic effects in the production of smali dianionic gold clusters by electron attachment on to stored Au-n, n = 12-28
Abstract Single charged gold clusters Au n -, 12 n 28, are stored in a Penning trap, size selected and transformed into dianions, Au2- n by the application of an electron beam. At the onset of dianion production, that is that range of cluster sizes n where the smallest doubly charged clusters are observed, the measured intensity ratio of the dianions to their precursors is not a continuous function of cluster size. Instead, there is a strong odd-even effect and a comparatively intense signal of Au2-18 The observed structures are very reminiscent of similar phenomena in the abundance spectra of metal clusters as observed by Knight et al. (1984, Phys. Rev. Lett., 52, 2141), which gave ris…
Multisequential photofragmentation of size-selected gold cluster ions
Time-resolved fragmentation measurements have been performed on stored, size-selected gold cluster ions ${\mathrm{Au}}_{n}^{+}$ $(n=17--21)$ that have been excited up to 15 eV by multiphoton absorption. These excitation energies are far above the clusters' dissociation thresholds and initiate multistep sequential unimolecular dissociation by evaporation of neutral monomers. The measurements allow for the determination of a combination of kinetic-energy release and radiative cooling of the excited clusters. Also, previously determined model-independent values of the cluster dissociation energies are confirmed by the present measurements. The data are consistent with thermal values of the kin…
New approaches to stored cluster ions
Ion traps are “wall-less containers” which allow the extended storage of selected species. During the storage various interaction steps may be repeatedly applied. To this end no further hardware has to be added - in contrast to beam experiments. In this progress report two examples of recent developments are presented: the experiments have been performed with metal clusters stored in a Penning (ion cyclotron resonance) trap. A new experimental scheme has been developed which allows precision measurements of the dissociation energies of polyatomic species. It has been triggered by investigations on the delayed photodissociation of stored metal clusters. However, the technique is also readily…
Non-destructive single-pass low-noise detection of ions in a beamline.
We have conceived, built, and operated a device for the non-destructive single-pass detection of charged particles in a beamline. The detector is based on the non-resonant pick-up and subsequent low-noise amplification of the image charges induced in a cylindrical electrode surrounding the particles' beam path. The first stage of the amplification electronics is designed to be operated from room temperature down to liquid helium temperature. The device represents a non-destructive charge counter as well as a sensitive timing circuit. We present the concept and design details of the device. We have characterized its performance and show measurements with low-energy highly charged ions (such …
HITRAP – a facility for experiments on heavy highly charged ions and on antiprotons
HITRAP is a facility for very slow highly-charged heavy ions at GSI. HITRAP uses the GSI relativistic ion beams, the Experimental Storage Ring ESR for electron cooling and deceleration to 4 MeV/u, and consists of a combination of an interdigital H-mode (IH) structure with a radiofrequency quadrupole structure for further deceleration to 6 keV/u, and a Penning trap for accumulation and cooling to low temperatures. Finally, ion beams with low emittance will be delivered to a large variety of atomic and nuclear physics experiments. Presently, HITRAP is in the commissioning phase. The deceleration of heavy-ion beam from the ESR storage ring to an energy of 500 keV/u with the IH structure has be…
SpecTrap: precision spectroscopy of highly charged ions—status and prospects
We present the status of the SpecTrap experiment currently being commissioned in the framework of the HITRAP project at GSI, Darmstadt, Germany. SpecTrap is a cryogenic Penning trap experiment dedicated to high-accuracy laser spectroscopy of highly charged ions (HCI) near rest. Determination of fine structure and hyperfine structure splittings in HCI with an expected relative spectral resolution of 10−7 will offer the possibility to test quantum electrodynamics in strong fields with unprecedented accuracy. Recently, we have demonstrated trapping and laser Doppler cooling of singly charged magnesium ions in SpecTrap. We report on the status of the experimental apparatus, measurements and pre…
Model-independent determination of dissociation energies: method and applications
A number of methods are available for the purpose of extracting dissociation energies of polyatomic particles. Many of these techniques relate the rate of disintegration at a known excitation energy to the value of the dissociation energy. However, such a determination is susceptible to systematic uncertainties, mainly due to the unknown thermal properties of the particles and the potential existence of 'dark' channels, such as radiative cooling. These problems can be avoided with a recently developed procedure, which applies energy-dependent reactions of the decay products as an uncalibrated thermometer. Thus, it allows a direct measurement of dissociation energies, without any assumption …
The magnetic moment anomaly of the electron bound in hydrogen-like oxygen16O7
The measurement of the g-factor of the electron bound in a hydrogen-like ion is a high-accuracy test of the theory of quantum electrodynamics (QED) in strong fields. Here we report on the measurement of the g-factor of the bound electron in hydrogen-like oxygen (16O7+). In our experiment a single highly charged ion is stored in a Penning trap. The electronic spin state of the ion is monitored via the continuous Stern?Gerlach effect in a quantum non-demolition measurement. Quantum jumps between the two spin states (spin up and spin down) are induced by a microwave field at the spin precession frequency of the bound electron. The g-factor of the bound electron is obtained by varying the micro…
Phase-sensitive measurement of trapped particle motions
We have developed and applied a novel method for the precise determination of small frequency differences of particle motions inside a Penning trap. In the present case, the frequency differences on the order of 100 mHz at motional frequencies on the order of 1 MHz are used to determine the spin state of an electron bound in a hydrogen-like ion. This novel technique measures the integrated phase difference of the particles' motions relative to an excitation with a well-defined phase. Thereby, the Fourier-limit for frequency measurements based on Fourier-analyses of detection signals can be overcome.
Absolute cross-sections for the nonresonant multi-photon ionization of toluene and xylene in the gas phase
Abstract The absolute multi-photon ionization cross-section of the phenyl ring was determined by laser-ionization of toluene and xylene molecules in the gas phase. Excitation was achieved using nonresonant four-photon absorption of the frequency doubled light of a 10 ns pulsed Nd:YAG laser (532 nm). The resulting ions were stored in a Penning trap and detected by time-of-flight mass spectrometry. The values of the cross-sections are 1.4(3)×10 −42 cm 8 W −4 s −1 and 1.3(3)×10 −42 cm 8 W −4 s −1 for toluene and xylene, respectively.
Dissociation energies of silver clusters Agn+, n=14, 15, 16, 18
A recently developed method to determine dissociation energies has been applied to positively charged silver clusters of size n=14, 15, 16 and 18. The method uses a combination of sequential and single step decays. It requires an uncalibrated thermometer which here is provided by the evaporation rate constants of the product clusters. For this purpose, earlier measurements [J. Chem. Phys. 57 (1998) 2786] are reanalyzed with the new method. The resulting dissociation energies are compared with the liquid drop values and the measured decay rate constants with expected rate constants from detailed balance theory.
Photodissociation of small group-11 metal cluster ions: Fragmentation pathways and photoabsorption cross sections
Noble metal cluster ions Cu(n)(+), Ag(n)(+) and Au(n)(+) (n = 3-21) have been stored in a Penning trap and photodissociated by low intensity laser pulses of 10 ns at photon energies of 3.49 eV and 4.66 eV. The fragmentation pathways, neutral monomer and dimer evaporation, have been monitored as a function of cluster size, excitation energy and element. It is found that the behavior of the branching ratio between monomer and dimer evaporation as a function of excitation energy depends on the metal under investigation. In particular, the slope of the energy dependence is positive for silver but negative for gold and copper cluster ions. Furthermore, photoabsorption cross sections are determin…
Highly charged ions, quantum-electrodynamics, and the electron mass
Abstract High precision experiments on the magnetic moment of hydrogen-like ions confined in a Penning trap have provided the most stringent test of bound-state quantum-electrodynamic calculations. Experiments have been performed on single C 5+ and O 7+ ions. These experiments are briefly reviewed and prospects for future improvements and extension to other systems are discussed.
The influence of internal degrees of freedom on the unimolecular decay of the molecule–cluster compound Au8+CH3OH
Time-resolved photodissociation measurements of the sequential reaction Au8+CH3OH→Au8+→Au7+ and the direct reaction Au8+→Au7+ have been performed for several excitation energies. The production rates and yields of the final state Au7+ in the sequential process are strongly influenced by the excitation energy deposited into the evaporated methanol molecule during the initial fragmentation step. Both the rate constants and yields can be fitted with a single parameter, the cluster–methanol binding energy.
Observation of multiply charged silver-cluster anions
Singly charged silver-cluster anions are produced in a laser vaporization source and transferred into a Penning trap. After size selection the clusters are subjected to an electron bath in the trap, which results in the attachment of further electrons. The relative abundance of dianions or trianions as a function of the clusters' size is analyzed by time-of-flight mass spectrometry. Silver-cluster dianions are observed for sizes n≥ 24 and trianions for n > 100. In addition, a detailed study of the cluster sizes 24 ?n? 60 shows a pronounced resistance to electron attachment for singly charged anions Agn- with a closed electronic shell, in particular Ag29-, Ag33-, and Ag39-. Both the threshol…
Continuous Stern–Gerlach effect and the magnetic moment of the antiproton
Abstract The measurement of the magnetic moment (or g-factor ) of the antiproton and of the proton is a sensitive test of CPT invariance. We discuss the possibility of applying the continuous Stern–Gerlach effect to detect quantum jumps between the two spin states (spin up and spin down) of the antiproton. The measurement will be performed on a single antiproton stored in a Penning trap. The g -factor of the antiproton is determined by measuring its cyclotron frequency and its spin precession frequency in the magnetic field of the trap. With the double Penning trap method the g -factor of the antiproton can be determined with an accuracy of 1 ppb.
High-Precision Measurements of the Bound Electron’s Magnetic Moment
Highly charged ions represent environments that allow to study precisely one or more bound electrons subjected to unsurpassed electromagnetic fields. Under such conditions, the magnetic moment (g-factor) of a bound electron changes significantly, to a large extent due to contributions from quantum electrodynamics. We present three Penning-trap experiments, which allow to measure magnetic moments with ppb precision and better, serving as stringent tests of corresponding calculations, and also yielding access to fundamental quantities like the fine structure constant α and the atomic mass of the electron. Additionally, the bound electrons can be used as sensitive probes for properties of the …
Trapped Ion Oscillation Frequencies as Sensors for Spectroscopy
The oscillation frequencies of charged particles in a Penning trap can serve as sensors for spectroscopy when additional field components are introduced to the magnetic and electric fields used for confinement. The presence of so-called "magnetic bottles" and specific electric anharmonicities creates calculable energy-dependences of the oscillation frequencies in the radiofrequency domain which may be used to detect the absorption or emission of photons both in the microwave and optical frequency domains. The precise electronic measurement of these oscillation frequencies therefore represents an optical sensor for spectroscopy. We discuss possible applications for precision laser and microw…
Electron and positron cooling of highly charged ions in a cooler Penning trap
Abstract Electron cooling is a well-established technique to increase the phase space density of particle beams in storage rings. In this paper, we discuss the feasibility of electron and positron cooling of ions in a Penning trap. We calculate the cooling times for the cases of trapped bare ions with nuclear charge Z =1 (protons), Z =36 (krypton) and Z =92 (uranium) with the Spitzer formula. Our calculations show that for typical experimental conditions the time for cooling from initial energies of 10 keV per charge down to rest is in the order of a second. We investigate the dependence of the cooling time on the number of ions and electrons, and their charge and mass.
Determination of dissociation energies by use of energy-dependent decay pathway branching ratios
Abstract We present a method for the determination of dissociation energies of polyatomic systems that undergo sequential fragmentation with energy-dependent decay pathway branching. It allows to experimentally determine the dissociation energy of any polyatomic system that shows such fragmentation behaviour without the need for a specific modelling of the system or of its fragmentation process, thus eliminating several systematic errors of traditional methods. The new method has been applied to the sequential fragmentation of Au+14 and Au+16. The resulting dissociation energies are highly accurate and in good agreement with model-free values based on rates of sequential decays.
Signature of cluster isomers in time-resolved photodissociation experiments
Abstract The unrecognized presence of structure isomers in mass-selected cluster ensembles may obstruct investigations of the systems’ intrinsic properties, since isomers differ not only in geometry, but also in other important properties. By the same token isomers are very interesting objects in the detailed study of atomic clusters. In the present work, different scenarios of isomeric coexistence are presented. They vary in the relative values of the interconversion barrier and the dissociation energies. For some idealized cases the possibility of a distinction of isomers by photodissociation experiments is discussed. In favorable situations isomeric structures may even be selected.
Precision studies in traps: Measurement of fundamental constants and tests of fundamental theories
Experiments on single atomic particles confined in Penning ion traps have contributed significantly to the improvements of fundamental constants and to tests of the theory of Quantum Electrodynamics for free and bound electrons. The most precise value of the fine structure constant as well as the electron mass have been derived from trap experiments. Numerous atomic masses of interest for fundamental questions have been determined with precisions of 10 � 9 or below. Further progress is envisaged in the near future.
Towards electronic g-factor measurements in medium-heavy hydrogen-like and lithium-like ions
Abstract Measurements of the anomalous magnetic moment of the electron bound in hydrogen-like ions with spinless nuclei have proven to be highly sensitive tests of corresponding calculations based on bound-state quantum electrodynamics. Measurements performed on H-like carbon 12C5+ and oxygen 16O7+ together with bound-state QED calculations on the same level of accuracy have achieved sensitivities around 0.25% of the QED bound state contributions to the calculated electronic g-factors of these ions. Currently, a similar experiment on hydrogen-like calcium 40Ca19+, lithium-like calcium 40Ca17+ and other medium-heavy ions is being prepared, which is capable of increasing this sensitivity on t…
ElectronicgFactor of Hydrogenlike OxygenO7+16
We present an experimental value for the $g$ factor of the electron bound in hydrogenlike oxygen, which is found to be ${g}_{\mathrm{e}\mathrm{x}\mathrm{p}\mathrm{t}}=2.000\text{ }047\text{ }025\text{ }4\text{ }(15)(44)$. The experiment was performed on a single $^{16}\mathrm{O}^{7+}$ ion stored in a Penning trap. For the first time, the expected line shape of the $g$-factor resonance is calculated which is essential for minimizing the systematic uncertainties. The measurement agrees within $1.1\text{ }\ensuremath{\sigma}$ with the predicted theoretical value ${g}_{\mathrm{t}\mathrm{h}\mathrm{e}\mathrm{o}\mathrm{r}\mathrm{y}}=2.000\text{ }047\text{ }020\text{ }2\text{ }(6)$. It represents a…
Cluster isobars for high-precision mass spectrometry
Doublet mass measurements of the isobars28Si3 and12C7 are performed by use of a Penning trap mass spectrometer and the Fourier transform ion cyclotron resonance (FT-ICR). The carbon and silicon cluster ions are produced by laser ablation. Results of these preliminary measurements are presented.
Recent gold cluster studies in a Penning trap
Abstract A progress report is given on the investigation of metal clusters with an ion cyclotron resonance (Penning) trap. The examples are taken from the recent studies on gold clusters. In particular, the monomer and dimer evaporation is monitored as a function of cluster size. For the particular case of Au 7 + this study is expanded to include the energy dependence of the branching ratio. In connection with the sequential decay of Au 8 + the information can be used for a model-free determination of the dissociation energy of Au 8 + . A second line of studies concerns the production, properties and storage behavior of polyanionic gold clusters. Such species have recently been produced by …
Photoinduced dissociation of anionic and electron detachment of dianionic gold clusters by use of a laser pointer
Abstract Size-selected anionic and dianionic gold clusters have been stored in a Penning trap and irradiated with the green light of a laser pointer. As examples of special interest, the systems Au 7 − and Au 29 2− have been chosen. In particular, Au 7 − , a small gold cluster with closed electron shell, is observed to decay into Au 6 − and Au 5 − with a decay pathway branching ratio similar to that of Au 9 + . The dianionic cluster Au 29 2− shows electron detachment upon photoexcitation. This observation is in agreement with independent experiments [Stoermer et al., Int. J. Mass Spectrom. 201 (2001) 63], where Au 29 2− is found to be the smallest dianion produced by neutral monomer evapora…
Decay pathways of stored metal-cluster anions after collisional activation
Size-selected gold clusters, Open image in new window (n ≤ 21), and tungsten clusters, Open image in new window , and Open image in new window (n = 4 – 8 and 12), stored in a Penning trap have been collisionally activated. Neutral monomer and dimer evaporation are observed in the case of gold. While no fragment products have been observed for tungsten clusters, there is evidence of electron emission from the anions.
First Observation of Doubly Charged Negative Gold Cluster Ions
Singly charged gold cluster anions in the size range n = 16–30 have been captured, stored and size selected in a Penning trap. After application of an electron beam doubly charged gold cluster anions have been observed for 20 ≤ n ≤ 30. To our knowledge this is the first observation of metal cluster dianions. The threshold appearance size is in good agreement with a simple charged sphere model. The application of argon gas pulses simultaneously with the electron beam is found to increase the production rate by an order of magnitude.
Energy dependence of the decay pathways of optically excited small gold clusters
The pathway competition between neutral monomer and neutral dimer evaporation from optically excited odd-size gold cluster ions Au+ n, n=7–15, has been investigated as a function of cluster size and excitation energy. Gold cluster ions of these sizes are the only ones to show observable pathway competition while all other sizes exclusively evaporate either neutral monomers or neutral dimers. The investigation has been performed by photoexcitation of stored size-selected gold cluster ions with a single 10-ns laser pulse. Subsequent time-resolved observation of the delayed dissociation allows us to quantitatively determine the relative fragment yields of the respective decay channels as a fun…
Dimer dissociation energies of small odd-size clusters
The dimer dissociation energies of gold cluster ions Au + n , n = 9, 11, 13, 15 have been determined with an extension of a recently developed model-independent method. Monomer-dimer decay pathway branching ratios provide the energy dependent process which is needed in this method. The measured values are D 2 ( Au + 9 ) = 3.66(8)(9) eV, D 2 ( Au + 11 ) = 4.27(11)(8) eV, D 2 ( Au + 13 ) = 4.50(9)(7) eV and D 2 ( Au + 15 ) = 4.29(10)(6) eV.
Beamline for low-energy transport of highly charged ions at HITRAP
Abstract A beamline for transport of highly charged ions with energies as low as a few keV/charge has been constructed and commissioned at GSI. Complementary to the existing infrastructure of the HITRAP facility for deceleration of highly charged ions from the GSI accelerator, the new beamline connects the HITRAP ion decelerator and an EBIT with the associated experimental setups. Therefore, the facility can now transport the decelerated heavy highly charged ions to the experiments or supply them offline with medium-heavy highly charged ions from the EBIT, both at energies as low as a few keV/charge. Here we present the design of the 20 m long beamline with the corresponding beam instrument…