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1.
Rev Sci Instrum ; 95(2)2024 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-38341722

RESUMO

The Greifswald multi-reflection time-of-flight setup has been extended with a magnetron sputtering gas aggregation source for the production of atomic cluster ions with sizes ranging from a single to thousands of atoms. This source, combined with a newly added quadrupole mass filter and a linear Paul trap, opens up the possibility of many new atomic-cluster studies not feasible with the setup before. The new components and their interfacing with the previous setup are described, and benchmarking as well as the first experimental results are presented. The capability of the system to handle singly charged ions with masses of several ten thousand atomic mass units is demonstrated.

2.
Phys Chem Chem Phys ; 26(2): 1105-1112, 2024 Jan 03.
Artigo em Inglês | MEDLINE | ID: mdl-38098439

RESUMO

Millisecond-delayed photodissociation of gas-phase Sn22- clusters stored in a Penning trap is investigated as a function of excitation energy. Sn15- is the only significant charged fragment, indicative of the break-off of neutral heptamers. Fits of the time-resolved fragmentation require a distribution of decay constants, caused by the finite width of the internal energy distribution of the cluster ensemble prior to photoexcitation. A lower limit for the dissociation energy for the loss of Sn7 is determined to be 2.1(1) eV, a factor of two above literature quantum chemical calculations.

3.
Anal Bioanal Chem ; 415(18): 4209-4220, 2023 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-37014373

RESUMO

MS SPIDOC is a novel sample delivery system designed for single (isolated) particle imaging at X-ray Free-Electron Lasers that is adaptable towards most large-scale facility beamlines. Biological samples can range from small proteins to MDa particles. Following nano-electrospray ionization, ionic samples can be m/z-filtered and structurally separated before being oriented at the interaction zone. Here, we present the simulation package developed alongside this prototype. The first part describes how the front-to-end ion trajectory simulations have been conducted. Highlighted is a quadrant lens; a simple but efficient device that steers the ion beam within the vicinity of the strong DC orientation field in the interaction zone to ensure spatial overlap with the X-rays. The second part focuses on protein orientation and discusses its potential with respect to diffractive imaging methods. Last, coherent diffractive imaging of prototypical T = 1 and T = 3 norovirus capsids is shown. We use realistic experimental parameters from the SPB/SFX instrument at the European XFEL to demonstrate that low-resolution diffractive imaging data (q < 0.3 nm-1) can be collected with only a few X-ray pulses. Such low-resolution data are sufficient to distinguish between both symmetries of the capsids, allowing to probe low abundant species in a beam if MS SPIDOC is used as sample delivery.


Assuntos
Capsídeo , Elétrons , Simulação por Computador , Síncrotrons , Raios X
4.
Rev Sci Instrum ; 92(6): 063203, 2021 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-34243583

RESUMO

The performance of a multi-reflection time-of-flight (MR-ToF) mass spectrometer is evaluated under the use of four voltage feedback loops to actively regulate its mirror potentials. Different electronic hardware is characterized to find the most useful configuration for parallel regulation of all of the MR-ToF analyzer's reflecting potentials. The gain in mass resolving power for low-abundance ion species is demonstrated by measuring pairs of molecular isobars of zinc clusters and analyzed in the context of expected flight-time fluctuations. For higher-abundance species, the resolving powers reached in short- and long-term measurements are probed with bismuth-cluster ions, resulting in values up to 500 000 and 200 000, respectively, in the absence of offline corrections. Additionally, feedback-loop regulation is found to be advantageous for changes of experiment cycles in which voltages are switched for, e.g., ion ejection.

5.
Rev Sci Instrum ; 91(2): 023201, 2020 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-32113431

RESUMO

Repeated switching of electric potentials within a single experimental cycle is introduced for a multi-reflection time-of-flight mass spectrometer (also known as an electrostatic ion beam trap) in order to eject different ion species after different storage times. The method is demonstrated with two cluster ions with considerably different mass-to-charge ratios (the A = 624 and 832 isotopologues of Pb3 + and Pb4 +, respectively) for the specific case where the sequential ejections result in an identical number of revolution periods. Thus, the ions' flight lengths are identical, and the resulting time-of-flight values allow single-reference mass determination. The requirements for the switching time window are studied in detail. For the present system and ion pair, the relative mass uncertainty is found to be 3 · 10-7 for short measurements (≈10 min) and 6 · 10-8 for longer ones (≈2 h).

6.
Phys Rev Lett ; 120(25): 253001, 2018 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-29979073

RESUMO

A method is presented to monitor the internal energy distribution of cluster anions via delayed electron detachment by pulsed photoexcitation and demonstrated on Co_{4}^{-} in an electrostatic ion beam trap. In a cryogenic operation, we calibrate the detachment delay to internal energy. By laser frequency scans, at room temperature, we reconstruct the time-dependent internal energy distribution of the clusters. The mean energies of ensembles from a cold and a hot ion source both approach thermal equilibrium. Our data yield a radiative emission law and the absorptivity of the cluster for thermal radiation.

7.
Rev Sci Instrum ; 89(1): 015114, 2018 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-29390654

RESUMO

The recently introduced method of ion separation by transversal ejection of unwanted species in electrostatic ion-beam traps and multi-reflection time-of-flight devices has been further studied in detail. As this separation is performed during the ion storage itself, there is no need for additional external devices such as ion gates or traps for either pre- or postselection of the ions of interest. The ejection of unwanted contaminant ions is performed by appropriate pulses of the potentials of deflector electrodes. These segmented ring electrodes are located off-center in the trap, i.e., between one of the two ion mirrors and the central drift tube, which also serves as a potential lift for capturing incoming ions and axially ejecting ions of interest after their selection. The various parameters affecting the selection effectivity and resolving power are illustrated with tin-cluster measurements, where isotopologue ion species provide mass differences down to a single atomic mass unit at ion masses of several hundred. Symmetric deflection voltages of only 10 V were found sufficient for the transversal ejection of ion species with as few as three deflection pulses. The duty cycle, i.e., the pulse duration with respect to the period of ion revolution, has been varied, resulting in resolving powers of up to several tens of thousands for this selection technique.

8.
Eur J Mass Spectrom (Chichester) ; 15(2): 283-91, 2009.
Artigo em Inglês | MEDLINE | ID: mdl-19423913

RESUMO

Azimuthal quadrupolar excitation is a commonly used technique in the field of ion cyclotron resonance mass spectrometry, in particular in combination with buffer-gas collisions to achieve axialization of the stored ions. If the quadrupolar excitation is applied with only one phase to a set of two opposing ring segments (rather than the "regular" method where two sets of electrodes are addressed with opposite polarities), parametric resonance effects at the frequencies 2nu(z) and nu(p) = nu(+) - nu(-) can lead to unintended ejection of ions from the trap. These parametric resonances have been revisited both theoretically and experimentally: multipole components of different azimuthal excitation schemes are derived by a simple vector representation of the excitation signal applied to the ring segments. Thus, parametric contributions can be easily identified, as demonstrated for the two-electrode and the four-electrode quadrupolar excitation schemes as well as further examples. In addition, the effect of the single-phase two-electrode quadrupolar excitation is demonstrated for storage and axialization of cluster ions.

9.
Eur J Mass Spectrom (Chichester) ; 11(5): 457-68, 2005.
Artigo em Inglês | MEDLINE | ID: mdl-16322651

RESUMO

Clusters consisting of a few atoms build the bridge between individual atoms and the condensed phase of matter and they are, thus, of high general interest. Over the last two decades, considerable progress has been made in the study of their properties, and ion storage techniques, in particular the use of ion cyclotron resonance (Penning) traps, are important tools for advanced investigations. Vice versa, cluster ions can serve as probes for the evaluation of ion-trap properties. Furthermore, they are ideally suited for the calibration of mass spectrometers and for consistency checks in high-accuracy mass determinations. Examples from the research areas mentioned, i.e. the investigation of cluster properties and the application of cluster ions for Penning-trap studies and mass calibration, are reported.

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