| 1. |
- Amann, Peter, et al.
(författare)
-
A dedicated photoelectron spectroscopy instrument for studies of catalytic reactions at pressures exceeding 1 bar
-
Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- Here, we present a new high-pressure x-ray photoelectron spectroscopy system dedicated to probing catalytic reactions under realistic conditions at pressures exceeding 1 bar. The instrument builds around the concept of a “virtual cell” in which a gasflow is directed onto the sample surface creating a local high pressure on top of the sample. This allows the instrument to maintain a low pressure of a few mbars in the main chamber, while simultaneously keeping a local pressure of around 1 bar. Synchrotron radiation based grazing incidence photoemission within ± 5° is used to enhance the surface sensitivity in the experiment. The aperture, separating the high-pressure region from the differential pumping of the electron spectrometer, consists of multiple, evenly spaced, mm sized holes matching the footprint of the x-ray beam on the sample surface. As the photo-emitted electrons are subject to strong scattering in the gas phase and the resulting signal is therefore highly dependent on the sample to aperture distance, the latter is controlled with high precision using a fully integrated manipulator that allows for sample movement with step sizes of 10 nm between 0 and –5 mm with very low vibrational amplitude. The instrumental features allows acquisition of metallic bulk spectra at He pressures up to 2.5 bar and also allows for following C1s spectra under realistic gas mixtures of CO + H2with various temperatures up to 500°C. This capability opens for studies of catalytic reactions in operandi.
|
|
| 2. |
- Amann, Peter, et al.
(författare)
-
A high-pressure x-ray photoelectron spectroscopy instrument for studies of industrially relevant catalytic reactions at pressures of several bars
- 2019
-
Ingår i: Review of Scientific Instruments. - : American Institute of Physics (AIP). - 0034-6748 .- 1089-7623. ; 90:10
-
Tidskriftsartikel (refereegranskat)abstract
- We present a new high-pressure x-ray photoelectron spectroscopy system dedicated to probing catalytic reactions under realistic conditions at pressures of multiple bars. The instrument builds around the novel concept of a "virtual cell" in which a gas flow onto the sample surface creates a localized high-pressure pillow. This allows the instrument to be operated with a low pressure of a few millibar in the main chamber, while simultaneously a local pressure exceeding 1 bar can be supplied at the sample surface. Synchrotron based hard x-ray excitation is used to increase the electron mean free path in the gas region between sample and analyzer while grazing incidence <5 degrees close to total external refection conditions enhances surface sensitivity. The aperture separating the high-pressure region from the differential pumping of the electron spectrometer consists of multiple, evenly spaced, micrometer sized holes matching the footprint of the x-ray beam on the sample. The resulting signal is highly dependent on the sample-to-aperture distance because photoemitted electrons are subject to strong scattering in the gas phase. Therefore, high precision control of the sample-to-aperture distance is crucial. A fully integrated manipulator allows for sample movement with step sizes of 10 nm between 0 and -5 mm with very low vibrational amplitude and also for sample heating up to 500 degrees C under reaction conditions. We demonstrate the performance of this novel instrument with bulk 2p spectra of a copper single crystal at He pressures of up to 2.5 bars and C1s spectra measured in gas mixtures of CO + H-2 at pressures of up to 790 mbar. The capability to detect emitted photoelectrons at several bars opens the prospect for studies of catalytic reactions under industrially relevant operando conditions.
|
|
| 3. |
- Bäckström, Erik, 1983-, et al.
(författare)
-
Storing keV negative ions for an hour : The lifetime of the metastable 2P1/2 level in 32S−
- 2015
-
Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 114:14
-
Tidskriftsartikel (refereegranskat)abstract
- We use a novel electrostatic ion storage ring to measure the radiative lifetime of the upper level in the 3p 5 P 2 o 1/2 →3p 5 P 2 o 3/2 spontaneous radiative decay in S − 32 to be 503±54 sec . This is by orders of magnitude the longest lifetime ever measured in a negatively charged ion. Cryogenic cooling of the storage ring gives a residual-gas pressure of a few times 10 −14 mbar at 13 K and storage of 10 keV sulfur anions for more than an hour. Our experimental results differ by 1.3σ from the only available theoretical prediction.
|
|
| 4. |
- Chartkunchand, Kiattichart C., et al.
(författare)
-
Dianion diagnostics in DESIREE : High-sensitivity detection of C-n(2-) from a sputter ion source
- 2018
-
Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 89:3
-
Tidskriftsartikel (refereegranskat)abstract
- A sputter ion source with a solid graphite target has been used to produce dianions with a focus on carbon cluster dianions, C-n(2-), with n = 7-24. Singly and doubly charged anions from the source were accelerated together to kinetic energies of 10 keV per atomic unit of charge and injected into one of the cryogenic (13 K) ion-beam storage rings of the Double ElectroStatic Ion Ring Experiment facility at Stockholm University. Spontaneous decay of internally hot C-n(2-) dianions injected into the ring yielded C-n(2-) anions with kinetic energies of 20 keV, which were counted with a microchannel plate detector. Mass spectra produced by scanning the magnetic field of a 90 degrees analyzing magnet on the ion injection line reflect the production of internally hot C-7(2-) - C-24(2-) dianions with lifetimes in the range of tens of microseconds to milliseconds. In spite of the high sensitivity of this method, no conclusive evidence of C-6(2-) was found while there was a clear C-7(2-) signal with the expected isotopic distribution. This is consistent with earlier experimental studies and with theoretical predictions. An upper limit is deduced for a C-6(2-) signal that is two orders-of-magnitude smaller than that for C-7(2-). In addition, CnO2- and CnCu2- dianions were detected.
|
|
| 5. |
- Chartkunchand, Kiattichart C., et al.
(författare)
-
Radiative lifetimes of the bound excited states of Pt-
- 2016
-
Ingår i: Physical Review A - Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 94:3
-
Tidskriftsartikel (refereegranskat)abstract
- © 2016 American Physical Society.The intrinsic radiative lifetimes of the 5d106sS1/22 and 5d96s2 D3/22 bound excited states in the platinum anion Pt- have been studied at cryogenic temperatures at the Double ElectroStatic Ion Ring Experiment (DESIREE) facility at Stockholm University. The intrinsic lifetime of the higher-lying 5d106s S1/22 state was measured to be 2.54±0.10s, while only a lifetime in the range of 50-200 ms could be estimated for the 5d96s2 D3/22 fine-structure level. The storage lifetime of the Pt- ion beam was measured to be a little over 15 min at a ring temperature of 13K. The present study reports the lifetime of an atomic negative ion in an excited bound state with an electron configuration different from that of the ground state.
|
|
| 6. |
- Eklund, Gustav, et al.
(författare)
-
Cryogenic merged-ion-beam experiments in DESIREE : Final-state-resolved mutual neutralization of Li+ and D-
- 2020
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society (APS). - 2469-9926 .- 2469-9934. ; 102:1
-
Tidskriftsartikel (refereegranskat)abstract
- We have developed an experimental technique to study charge-and energy-flow processes in sub-eV collisions between oppositely charged, internally cold, ions of atoms, molecules, and clusters. Two ion beams are stored in separate rings of the cryogenic ion-beam storage facility DESIREE, and merged in a common straight section where a set of biased drift tubes is used to control the center-of-mass collision energy locally in fine steps. Here, we present measurements on mutual neutralization between Li+ and D- where a time-sensitive imaging-detector system is used to measure the three-dimensional distance between the neutral Li and D atoms as they reach the detector. This scheme allows for direct measurements of kinetic-energy releases, and here it reveals separate populations of the 3s state and the (3p + 3d) states in neutral Li while the D atom is left in its ground state 1s. The branching fraction of the 3s final state is measured to be 57.8 +/- 0.7% at a center-of-mass collision energy of 78 +/- 13 meV. The technique paves the way for studies of charge-, energy-, and mass-transfer reactions in single collisions involving molecular and cluster ions in well-defined quantum states.
|
|
| 7. |
- Gatchell, Michael, et al.
(författare)
-
Commissioning of the DESIREE storage rings - a new facility for cold ion-ion collisions
- 2014
-
Ingår i: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013). - : Institute of Physics (IOP). ; 488:1
-
Konferensbidrag (refereegranskat)abstract
- We report on the ongoing commissioning of the Double ElectroStatic Ion Ring ExpEriment, DESIREE, at Stockholm University. Beams of atomic carbon anions (C-) and smaller carbon anion molecules (C-2(-), C-3(-), C-4(-) etc.) have been produced in a sputter ion source, accelerated to 10 keV or 20 keV, and stored successfully in the two electrostatic rings. The rings are enclosed in a common vacuum chamber cooled to below 13 Kelvin. The DESIREE facility allows for studies of internally relaxed single isolated atomic, molecular and cluster ions and for collision experiments between cat-and anions down to very low center-of-mass collision energies (meV scale). The total thermal load of the vacuum chamber at this temperature is measured to be 32 W. The decay rates of stored ion beams have two components: a non-exponential component caused by the space charge of the beam itself which dominates at early times and an exponential term from the neutralization of the beam in collisions with residual gas at later times. The residual gas limited storage lifetime of carbon anions in the symmetric ring is over seven minutes while the 1/e lifetime in the asymmetric ring is measured to be about 30 seconds. Although we aim to improve the storage in the second ring, the number of stored ions are now sufficient for many merged beams experiments with positive and negative ions requiring milliseconds to seconds ion storage.
|
|
| 8. |
- Gatchell, Michael, et al.
(författare)
-
First results from the Double ElectroStatic Ion-Ring ExpEriment, DESIREE
- 2014
-
Ingår i: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013). - : Institute of Physics (IOP). ; 488
-
Konferensbidrag (refereegranskat)abstract
- We have stored the first beams in one of the rings of the double electrostatic ion-storage ring, DESIREE at cryogenic and at room temperature conditions. At cryogenic operations the following parameters are found. Temperature; T= 13K, pressure; p <10(-13) mbar, initial number of stored ions; N > 10(7) and storage lifetime of a C-2(-) beam; tau = 450 S.
|
|
| 9. |
- Hartman, Henrik, et al.
(författare)
-
First storage of ion beams in the Double Electrostatic Ion-Ring Experiment : DESIREE
- 2013
-
Ingår i: Review of Scientific Instruments. - : American Institute of Physics (AIP). - 0034-6748 .- 1089-7623. ; 84:5
-
Tidskriftsartikel (refereegranskat)abstract
- We report on the first storage of ion beams in the Double ElectroStatic Ion Ring ExpEriment, DESIREE, at Stockholm University. We have produced beams of atomic carbon anions and small carbon anion molecules (Cn-, n = 1, 2, 3, 4) in a sputter ion source. The ion beams were accelerated to 10 keV kinetic energy and stored in an electrostatic ion storage ring enclosed in a vacuum chamber at 13 K. For 10 keV C2- molecular anions we measure the residual-gas limited beam storage lifetime to be 448 s +/- 18 s with two independent detector systems. Using the measured storage lifetimes we estimate that the residual gas pressure is in the 10-14 mbar range. When high current ion beams are injected, the number of stored particles does not follow a single exponential decay law as would be expected for stored particles lost solely due to electron detachment in collision with the residual-gas. Instead, we observe a faster initial decay rate, which we ascribe to the effect of the space charge of the ion beam on the storage capacity.
|
|
| 10. |
- Kamińska, Magdalena, et al.
(författare)
-
Lifetime of the bound excited level in Ni
- 2016
-
Ingår i: Physical Review A. - 1050-2947 .- 1094-1622. ; 93:1
-
Tidskriftsartikel (refereegranskat)abstract
- The intrinsic lifetime of the upper level in the bound-bound 3d(9) 4s(2) D-2(3/2) -> 3d(9) 4s(2) D-2(5/2) radiative transition in Ni- was measured to be 15.1 +/- 0.4 s. The experiment was performed at cryogenic temperatures in one of the ion-beam storage rings of the Double ElectroStatic Ion Ring ExpEriment facility at Stockholm University. The storage lifetime of the Ni- ion beam was measured to be close to 5 min at a ring temperature of 13 K.
|
|
