| 1. |
- Redekop, Evgeniy A., et al.
(författare)
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Synchronizing gas injections and time-resolved data acquisition for perturbation-enhanced APXPS experiments
- 2021
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Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 92:4
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Tidskriftsartikel (refereegranskat)abstract
- An experimental approach is described in which well-defined perturbations of the gas feed into an Ambient Pressure X-ray Photoelectron Spectroscopy (APXPS) cell are fully synchronized with the time-resolved x-ray photoelectron spectroscopy data acquisition. These experiments unlock new possibilities for investigating the properties of materials and chemical reactions mediated by their surfaces, such as those in heterogeneous catalysis, surface science, and coating/deposition applications. Implementation of this approach, which is termed perturbation-enhanced APXPS, at the SPECIES beamline of MAX IV Laboratory is discussed along with several experimental examples including individual pulses of N2 gas over a Au foil, a multi-pulse titration of oxygen vacancies in a pre-reduced TiO2 single crystal with O2 gas, and a sequence of alternating precursor pulses for atomic layer deposition of TiO2 on a silicon wafer substrate.
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| 2. |
- Kinnunen, Jussi, et al.
(författare)
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Nondestructive fluorescence-based quantification of threose-induced collagen cross-linking in bovine articular cartilage
- 2012
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Ingår i: Journal of Biomedical Optics. - : SPIE - International Society for Optical Engineering. - 1083-3668 .- 1560-2281. ; 17:9, s. 97003-
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Tidskriftsartikel (refereegranskat)abstract
- Extensive collagen cross-linking affects the mechanical competence of articular cartilage: it can make the cartilage stiffer and more brittle. The concentrations of the best known cross-links, pyridinoline and pentosidine, can be accurately determined by destructive high-performance liquid chromatography (HPLC). We explore a nondestructive evaluation of cross-linking by using the intrinsic fluorescence of the intact cartilage. Articular cartilage samples from bovine knee joints were incubated in threose solution for 40 and 100 h to increase the collagen cross-linking. Control samples without threose were also prepared. Excitation-emission matrices at wavelengths of 220 to 950 nm were acquired from the samples, and the pentosidine and pyridinoline cross-links and the collagen concentrations were determined using HPLC. After the threose treatment, pentosidine and lysyl pyridinole (LP) concentrations increased. The intrinsic fluorescence, excited below 350 nm, decreased and was related to pentosidine [r=−0.90, 240/325nm (excitation/emission)] or LP (r=−0.85, 235/285nm) concentrations. Due to overlapping, the changes in emission could not be linked specifically to the recorded cross-links. However, the fluorescence signal enabled a nondestructive optical estimate of changes in the pentosidine and LP cross-linking of intact articular cartilage.
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| 3. |
- Kokkonen, E., et al.
(författare)
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Ambient pressure x-ray photoelectron spectroscopy setup for synchrotron-based in situ and operando atomic layer deposition research
- 2022
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Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 1089-7623 .- 0034-6748. ; 93:1
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Tidskriftsartikel (refereegranskat)abstract
- An ambient pressure cell is described for conducting synchrotron-based x-ray photoelectron spectroscopy (XPS) measurements during atomic layer deposition (ALD) processes. The instrument is capable of true in situ and operando experiments in which it is possible to directly obtain elemental and chemical information from the sample surface using XPS as the deposition process is ongoing. The setup is based on the ambient pressure XPS technique, in which sample environments with high pressure (several mbar) can be created without compromising the ultrahigh vacuum requirements needed for the operation of the spectrometer and the synchrotron beamline. The setup is intended for chemical characterization of the surface intermediates during the initial stages of the deposition processes. The SPECIES beamline and the ALD cell provide a unique experimental platform for obtaining new information on the surface chemistry during ALD half-cycles at high temporal resolution. Such information is valuable for understanding the ALD reaction mechanisms and crucial in further developing and improving ALD processes. We demonstrate the capabilities of the setup by studying the deposition of TiO2 on a SiO2 surface by using titanium(IV) tetraisopropoxide and water as precursors. Multiple core levels and the valence band of the substrate surface were followed during the film deposition using ambient pressure XPS.
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| 4. |
- Kokkonen, Esko, et al.
(författare)
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Upgrade of the SPECIES beamline at the MAX IV Laboratory
- 2021
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Ingår i: Journal of Synchrotron Radiation. - 1600-5775. ; 28, s. 588-601
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Tidskriftsartikel (refereegranskat)abstract
- The SPECIES beamline has been transferred to the new 1.5 GeV storage ring at the MAX IV Laboratory. Several improvements have been made to the beamline and its endstations during the transfer. Together the Ambient Pressure X-ray Photoelectron Spectroscopy and Resonant Inelastic X-ray Scattering endstations are capable of conducting photoelectron spectroscopy in elevated pressure regimes with enhanced time-resolution and flux and X-ray scattering experiments with improved resolution and flux. Both endstations offer a unique capability for experiments at low photon energies in the vacuum ultraviolet and soft X-ray range. In this paper, the upgrades on the endstations and current performance of the beamline are reported.
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| 5. |
- Kokkonen, Mikko, et al.
(författare)
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Advanced research trends in dye-sensitized solar cells
- 2021
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Ingår i: Journal of Materials Chemistry A. - : Royal Society of Chemistry. - 2050-7488 .- 2050-7496. ; 9:17, s. 10527-10545
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Forskningsöversikt (refereegranskat)abstract
- Dye-sensitized solar cells (DSSCs) are an efficient photovoltaic technology for powering electronic applications such as wireless sensors with indoor light. Their low cost and abundant materials, as well as their capability to be manufactured as thin and light-weight flexible solar modules highlight their potential for economic indoor photovoltaics. However, their fabrication methods must be scaled to industrial manufacturing with high photovoltaic efficiency and performance stability under typical indoor conditions. This paper reviews the recent progress in DSSC research towards this goal through the development of new device structures, alternative redox shuttles, solid-state hole conductors, TiO2 photoelectrodes, catalyst materials, and sealing techniques. We discuss how each functional component of a DSSC has been improved with these new materials and fabrication techniques. In addition, we propose a scalable cell fabrication process that integrates these developments to a new monolithic cell design based on several features including inkjet and screen printing of the dye, a solid state hole conductor, PEDOT contact, compact TiO2, mesoporous TiO2, carbon nanotubes counter electrode, epoxy encapsulation layers and silver conductors. Finally, we discuss the need to design new stability testing protocols to assess the probable deployment of DSSCs in portable electronics and internet-of-things devices.
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| 6. |
- Kulmala, Katariina, et al.
(författare)
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Diffusion of ionic and non-ionic contrast agents in articular cartilage with increased cross-linking : contribution of steric and electrostatic effects
- 2013
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Ingår i: Medical Engineering and Physics. - : Elsevier. - 1350-4533 .- 1873-4030. ; 35:10, s. 1415-20
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Tidskriftsartikel (refereegranskat)abstract
- OBJECTIVE: To investigate the effect of threose-induced collagen cross-linking on diffusion of ionic and non-ionic contrast agents in articular cartilage.DESIGN: Osteochondral plugs (Ø=6mm) were prepared from bovine patellae and divided into two groups according to the contrast agent to be used in contrast enhanced computed tomography (CECT) imaging: (I) anionic ioxaglate and (II) non-ionic iodixanol. The groups I and II contained 7 and 6 sample pairs, respectively. One of the paired samples served as a reference while the other was treated with threose to induce collagen cross-linking. The equilibrium partitioning of the contrast agents was imaged after 24h of immersion. Fixed charge density (FCD), water content, contents of proteoglycans, total collagen, hydroxylysyl pyridinoline (HP), lysyl pyridinoline (LP) and pentosidine (Pent) cross-links were determined as a reference.RESULTS: The equilibrium partitioning of ioxaglate (group I) was significantly (p=0.018) lower (-23.4%) in threose-treated than control samples while the equilibrium partitioning of iodixanol (group II) was unaffected by the threose-treatment. FCD in the middle and deep zones of the cartilage (p<0.05) and contents of Pent and LP (p=0.001) increased significantly due to the treatment. However, the proteoglycan concentration was not systematically altered after the treatment. Water content was significantly (-3.5%, p=0.007) lower after the treatment.CONCLUSIONS: Since non-ionic iodixanol showed no changes in partition after cross-linking, in contrast to anionic ioxaglate, we conclude that the cross-linking induced changes in charge distribution have greater effect on diffusion compared to the cross-linking induced changes in steric hindrance.
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| 7. |
- Lin, Jack J., et al.
(författare)
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Pre-deliquescent water uptake in deposited nanoparticles observed with in situ ambient pressure X-ray photoelectron spectroscopy
- 2021
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:6, s. 4709-4727
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Tidskriftsartikel (refereegranskat)abstract
- We study the adsorption of water onto deposited inorganic sodium chloride and organic malonic acid and sucrose nanoparticles at ambient water pressures corresponding to relative humidities (RH) from 0 % to 16 %. To obtain information about water adsorption at conditions which are not accessible with typical aerosol instrumentation, we use surface-sensitive ambient pressure X-ray photoelectron spectroscopy (APXPS), which has a detection sensitivity starting at parts per thousand. Our results show that water is already adsorbed on sodium chloride particles at RH well below deliquescence and that the chemical environment on the particle surface is changing with increasing humidity. While the sucrose particles exhibit only very modest changes on the surface at these relative humidities, the chemical composition and environment of malonic acid particle surfaces is clearly affected. Our observations indicate that water uptake by inorganic and organic aerosol particles could already have an impact on atmospheric chemistry at low relative humidities. We also establish the APXPS technique as a viable tool for studying chemical changes on the surfaces of atmospherically relevant aerosol particles which are not detected with typical online mass-and volume-based methods.
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| 8. |
- Näslund, Lars-Åke, 1968-, et al.
(författare)
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Chemical bonding of termination species in 2D carbides investigated through valence band UPS/XPS of Ti3C2T xMXene
- 2021
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Ingår i: 2D Materials. - : IOP Publishing. - 2053-1583. ; 8:4
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Tidskriftsartikel (refereegranskat)abstract
- MXenes are technologically interesting 2D materials that show potential in numerous applications. The properties of the MXenes depend at large extent on the selection of elements that build the 2D MX-layer. Another key parameter for tuning the attractive material properties is the species that terminate the surfaces of the MX-layers. Although being an important parameter, experimental studies on the bonding between the MX-layers and the termination species are few and thus an interesting subject of investigation. Here we show that the termination species fluorine (F) bonds to the Ti3C2-surface mainly through Ti 3p - F 2p hybridization and that oxygen (O) bonds through Ti 3p - O 2p hybridization with a significant contribution of Ti 3d and Ti 4p. The study further shows that the Ti3C2-surface is not only terminated by F and O on the threefold hollow face-centered-cubic site. A significant amount of O sits on a bridge site bonded to two Ti surface atoms on the Ti3C2-surface. In addition, the results provide no support for hydroxide (OH) termination on the Ti3C2-surface. On the contrary, the comparison of the valence band intensity distribution obtained through ultraviolet- and x-ray photoelectron spectroscopy with computed spectra by density of states, weighed by matrix elements and sensitivity factors, reveals that OH cannot be considered as an inherent termination species in Ti3C2T x . The results from this study have implications for correct modeling of the structure of MXenes and the corresponding materials properties. Especially in applications where surface composition and charge are important, such as supercapacitors, Li-ion batteries, electrocatalysis, and fuel- and solar cells, where intercalation processes are essential.
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| 9. |
- Rieppo, Lassi, et al.
(författare)
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Infrared microspectroscopic determination of collagen cross-links in articular cartilage
- 2017
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Ingår i: Journal of Biomedical Optics. - : SPIE - International Society for Optical Engineering. - 1083-3668 .- 1560-2281. ; 22:3
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Tidskriftsartikel (refereegranskat)abstract
- Collagen forms an organized network in articular cartilage to give tensile stiffness to the tissue. Due to its long half-life, collagen is susceptible to cross-links caused by advanced glycation end-products. The current standard method for determination of cross-link concentrations in tissues is the destructive high-performance liquid chromatography (HPLC). The aim of this study was to analyze the cross-link concentrations nondestructively from standard unstained histological articular cartilage sections by using Fourier transform infrared (FTIR) microspectroscopy. Half of the bovine articular cartilage samples (n=27) were treated with threose to increase the collagen cross-linking while the other half (n=27) served as a control group. Partial least squares (PLS) regression with variable selection algorithms was used to predict the cross-link concentrations from the measured average FTIR spectra of the samples, and HPLC was used as the reference method for cross-link concentrations. The correlation coefficients between the PLS regression models and the biochemical reference values were r=0.84 (p<0.001), r=0.87 (p<0.001) and r=0.92 (p<0.001) for hydroxylysyl pyridinoline (HP), lysyl pyridinoline (LP), and pentosidine (Pent) cross-links, respectively. The study demonstrated that FTIR microspectroscopy is a feasible method for investigating cross-link concentrations in articular cartilage.
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