| 1. |
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| 2. |
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| 3. |
- Ademuyiwa, Adesoji O., et al.
(författare)
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Determinants of morbidity and mortality following emergency abdominal surgery in children in low-income and middle-income countries
- 2016
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Ingår i: BMJ Global Health. - : BMJ Publishing Group Ltd. - 2059-7908. ; 1:4
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Tidskriftsartikel (refereegranskat)abstract
- Background: Child health is a key priority on the global health agenda, yet the provision of essential and emergency surgery in children is patchy in resource-poor regions. This study was aimed to determine the mortality risk for emergency abdominal paediatric surgery in low-income countries globally.Methods: Multicentre, international, prospective, cohort study. Self-selected surgical units performing emergency abdominal surgery submitted prespecified data for consecutive children aged <16 years during a 2-week period between July and December 2014. The United Nation's Human Development Index (HDI) was used to stratify countries. The main outcome measure was 30-day postoperative mortality, analysed by multilevel logistic regression.Results: This study included 1409 patients from 253 centres in 43 countries; 282 children were under 2 years of age. Among them, 265 (18.8%) were from low-HDI, 450 (31.9%) from middle-HDI and 694 (49.3%) from high-HDI countries. The most common operations performed were appendectomy, small bowel resection, pyloromyotomy and correction of intussusception. After adjustment for patient and hospital risk factors, child mortality at 30 days was significantly higher in low-HDI (adjusted OR 7.14 (95% CI 2.52 to 20.23), p<0.001) and middle-HDI (4.42 (1.44 to 13.56), p=0.009) countries compared with high-HDI countries, translating to 40 excess deaths per 1000 procedures performed.Conclusions: Adjusted mortality in children following emergency abdominal surgery may be as high as 7 times greater in low-HDI and middle-HDI countries compared with high-HDI countries. Effective provision of emergency essential surgery should be a key priority for global child health agendas.
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| 4. |
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| 5. |
- AbdulWahab, Atqah, et al.
(författare)
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The emergence of multidrug-resistant Pseudomonas aeruginosa in cystic fibrosis patients on inhaled antibiotics
- 2017
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Ingår i: Lung India. - : Medknow Publications. - 0970-2113 .- 0974-598X. ; 34:6, s. 527-531
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Tidskriftsartikel (refereegranskat)abstract
- Introduction: Multidrug-resistant Pseudomonas aeruginosa (MDR-PA) is an important and growing issue in the care of patients with cystic fibrosis (CF), and a major cause of morbidity and mortality.Objective: The objective of the study was to describe the frequency of MDR-PA recovered from the lower respiratory samples of pediatric and adult CF patients, and its antibiotic resistance pattern to commonly used antimicrobial agents including beta-lactams, aminoglycosides, and fluoroquinolones.Materials and Methods: The lower respiratory isolates of P. aeruginosa were obtained from inpatients and outpatients CF clinics from a tertiary care teaching hospital for the period from October 2014 to September 2015. The identification and antimicrobial susceptibility for all the isolates were performed by using the BD Phoenix (TM) and E-test in compliance with Clinical and Laboratory Standards Institute (CLSI) guidelines.Results: A total of 61 P. aeruginosa samples were isolated from thirty CF patients from twenty families. Twelve sputum samples were positive for MDR-PA (seven nonmucoid and five mucoid isolates) from five CF patients (five families) with moderate-to-very severe lung disease given MDR-PA frequency of 19.7%. The median age of the study group was 20 (range 10-30) years. Three CF patients were on chronic inhaled tobramycin and two on nebulized colistin. The antimicrobial patterns of isolates MDR-PA showed the highest rate of resistance toward each gentamycin, amikacin, and cefepime (100%), followed by 91.7% to ciprofloxacin, 75% to tobramycin, 58.3% to meropenem, and 50% to piperacillin-tazobactam. None of the isolates were resistant to colistin during the study period.Conclusion: The study results emphasize that the emergence of a significant problem in the clinical isolates of P. aeruginosa in CF patients that dictate appropriate attention to the antibiotic management after proper surveillance.
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| 6. |
- Atak, Kaan, et al.
(författare)
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The Chemical Bond in Carbonyl and Sulfinyl Groups Studied by Soft X-ray Spectroscopy and ab Initio Calculations
- 2012
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Ingår i: ChemPhysChem. - : Wiley. - 1439-4235 .- 1439-7641. ; 13:13, s. 3106-3111
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Tidskriftsartikel (refereegranskat)abstract
- The polar character of the sulfinyl bond, which determines many of the properties of dimethyl sulfoxide (DMSO), is a result of charge transfer in low-lying π-type orbitals. This characteristic—together with the wide energy gap between the highest occupied and the lowest unoccupied molecular orbitals of this substance—makes DMSO a relatively inert aprotic solvent with strong nucleophilicity and electrophilicity.
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| 7. |
- Aziz, Emad F., et al.
(författare)
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Cation-specific interactions with carboxylate in amino acid and acetate aqueous solutions : X-ray absorption and ab initio calculations
- 2008
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Ingår i: Journal of Physical Chemistry B. - : American Chemical Society (ACS). - 1520-6106 .- 1520-5207. ; 112:40, s. 12567-12570
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Tidskriftsartikel (refereegranskat)abstract
- Relative interaction strengths between cations (X = Li+, Na+, K+, NH4+) and anionic carboxylate groups of acetate and glycine in aqueous solution are determined. These model systems mimic ion pairing of biologically relevant cations with negatively charged groups at protein surfaces. With oxygen ls X-ray absorption spectroscopy, we can distinguish between spectral contributions from H2O and carboxylate, which allows us to probe the electronic structure changes of the atomic site of the carboxylate group being closest to the countercation. From the intensity variations of the COOaq- ls X-ray absorption peak, which quantitatively correlate with the change in the local partial density of states from the carboxylic site, interactions are found to decrease in the sequence Na+ > Li+ > K+ > NH4+. This ordering, as well as the observed bidental nature of the -COOaq- and X-aq(+) interaction, is supported by combined ab initio and molecular dynamics calculations.
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| 8. |
- Aziz, Emad F., et al.
(författare)
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Interaction between liquid water and hydroxide revealed by core-hole de-excitation
- 2008
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 455:7209, s. 89-91
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Tidskriftsartikel (refereegranskat)abstract
- The hydroxide ion plays an important role in many chemical and biochemical processes in aqueous solution(1). But ourmolecular- level understanding of its unusual and fast transport in water, and of the solvation patterns that allow fast transport, is far from complete. One proposal seeks to explain the properties and behaviour of the hydroxide ion by essentially regarding it as a water molecule that is missing a proton(2), and by inferring transport mechanisms and hydration structures from those of the excess proton. A competing proposal invokes instead unique and interchanging hydroxide hydration complexes, particularly the hypercoordinated OH-(H2O)(4) species and tri- coordinated OH-(H2O)(3) that can form a transient hydrogen bond between the H atom of the OH- and a neighbouring water molecule(3-5). Here we report measurements of core- level photoelectron emission and intermolecular Coulombic decay(6-8) for an aqueous hydroxide solution, which show that the hydrated hydroxide ion is capable of transiently donating a hydrogen bond to surrounding watermolecules. In agreement with recent experimental studies of hydroxide solutions(9-12), our finding thus supports the notion that the hydration structure of the hydroxide ion cannot be inferred from that of the hydrated excess proton.
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| 9. |
- Aziz, Emad F., et al.
(författare)
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Photoinduced formation of N-2 molecules in ammonium compounds
- 2007
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Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 111:39, s. 9662-9669
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Tidskriftsartikel (refereegranskat)abstract
- Via fluorescence yield (FY) and resonant inelastic scattering spectroscopy in the soft X-ray range we find that soft X-rays induce formation of N-2 molecules in solid NH4Cl and in related compounds. The nitrogen molecules form weak bonds in NH4Cl, so that a substantial fraction of the molecules remains in the sample. From measurements of the FY as a function of exposure and temperature, the rates for the photochemical processes are estimated. At elevated temperatures (363 K), several nitrogen atoms are removed from the sample per incoming photon. At lower temperatures (233 K), the rate is reduced to around 0.02 nitrogen atoms for each incoming photon. Virtually all these atoms form N-2 molecules which are bound in the sample. The generality and implications of these results are briefly discussed.
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| 10. |
- Aziz, Emad F, et al.
(författare)
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Probing the electronic structure of the hemoglobin active center in physiological solutions.
- 2009
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 102:6, s. 068103-
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Tidskriftsartikel (refereegranskat)abstract
- Soft-x-ray absorption spectroscopy at the L_{2,3} edge of the iron center in bovine hemoglobin and hemin under physiological conditions is reported for the first time. Spectra of the same compounds in solid form are presented for comparison. Striking differences in the electronic structure of the metalloporphyrin are observed between the liquid and solid compounds. We unambiguously show that hemoglobin and hemin are in a high-spin ferric state in solution, and that the 2p spin-orbit coupling decreases for hemin compared to the hemoglobin, while this is not the case in solids. The spectra were simulated using ligand field multiplet theory, in good agreement with the experiment, allowing quantification of the amount of charge transfer between the porphyrin and Fe3+ ion in hemoglobin and in hemin.
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| 11. |
- Borgström, Magnus, et al.
(författare)
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Sensitized hole injection of phosphorus porphyrin into NiO : Toward new photovoltaic devices
- 2005
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Ingår i: Journal of Physical Chemistry B. - : American Chemical Society (ACS). - 1520-6106 .- 1520-5207. ; 109:48, s. 22928-22934
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Tidskriftsartikel (refereegranskat)abstract
- This paper describes the preparation and the characterization of a photovoltaic cell based on the sensitization of a wide band gap p-type semiconductor (NiO) with a phosphorus porphyrin. A photophysical study with femtosecond transient absorption spectroscopy showed that light excitation of the phosphorus porphyrin chemisorbed on NiO particles induces a very rapid interfacial hole injection into the valence band of NiO, occurring mainly on the 2-20 ps time scale. This is followed by a recombination in which ca. 80% of the ground-state reactants are regenerated within 1 ns. A photoelectrochernical device, prepared with a nanocrystalline NiO electrode coated with the phosphorus porphyrin, yields a cathodic photocurrent indicating that electrons indeed flow from the NiO electrode toward the solution. The low incident-to-photocurrent efficiency (IPCE) can be rationalized by the rapid back recombination reaction between the reduced sensitizer and the injected hole which prevents an efficient regeneration of the sensitizer ground state from the iodide/triiodide redox mediator. To the best of our knowledge, this work represents the first example of a photovoltaic cell in which a mechanism of hole photoinjection has been characterized.
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| 12. |
- El Bairi, Khalid, et al.
(författare)
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The tale of TILs in breast cancer: A report from The International Immuno-Oncology Biomarker Working Group
- 2021
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Ingår i: npj Breast Cancer. - : Springer Science and Business Media LLC. - 2374-4677. ; 7:1
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Forskningsöversikt (refereegranskat)abstract
- The advent of immune-checkpoint inhibitors (ICI) in modern oncology has significantly improved survival in several cancer settings. A subgroup of women with breast cancer (BC) has immunogenic infiltration of lymphocytes with expression of programmed death-ligand 1 (PD-L1). These patients may potentially benefit from ICI targeting the programmed death 1 (PD-1)/PD-L1 signaling axis. The use of tumor-infiltrating lymphocytes (TILs) as predictive and prognostic biomarkers has been under intense examination. Emerging data suggest that TILs are associated with response to both cytotoxic treatments and immunotherapy, particularly for patients with triple-negative BC. In this review from The International Immuno-Oncology Biomarker Working Group, we discuss (a) the biological understanding of TILs, (b) their analytical and clinical validity and efforts toward the clinical utility in BC, and (c) the current status of PD-L1 and TIL testing across different continents, including experiences from low-to-middle-income countries, incorporating also the view of a patient advocate. This information will help set the stage for future approaches to optimize the understanding and clinical utilization of TIL analysis in patients with BC.
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| 13. |
- Engel, Nicholas, et al.
(författare)
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DMSO-Water Clustering in Solution Observed in Soft X-ray Spectra
- 2012
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Ingår i: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 3:24, s. 3697-3701
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Tidskriftsartikel (refereegranskat)abstract
- The significant deviation from the ideality of dimethyl sulfoxide (DMSO)/water mixtures can be addressed based on the change of the local molecular orbitals of each solvent upon mixing. Oxygen K-edge absorption and emission spectra of DMSO/water solutions were measured using the liquid microjet technique. The spectra demonstrate that the hydrogen bond network in liquid water is already influenced at small DMSO concentrations, and at the molar fraction x(DMSO) = 0.43 we find strong evidence of DMSO-water clustering reflected by the influence on the occupied molecular orbitals.
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| 14. |
- Gråsjö, Johan, et al.
(författare)
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Electronic structure of water molecules confined in a micelle lattice
- 2009
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Ingår i: Journal of Physical Chemistry B. - : American Chemical Society (ACS). - 1520-6106 .- 1520-5207. ; 113:24, s. 8201-8205
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Tidskriftsartikel (refereegranskat)abstract
- Oxygen K absorption and emission spectra of water molecules confined in dodecyltrimethyl ammonium chloride micelle structures are presented. The local electronic structure of the water molecules is found to be dramatically different from the electronic structure of water molecules in the gas-phase as well as in liquid water. Hybridization with states of the ions in the surrounding ions is directly observed, and evidence for stabilization of the water molecules relative to molecules in bulk water is found.
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| 15. |
- Hans, Andreas, et al.
(författare)
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Optical Fluorescence Detected from X-ray Irradiated Liquid Water
- 2017
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Ingår i: Journal of Physical Chemistry B. - : American Chemical Society (ACS). - 1520-6106 .- 1520-5207. ; 121:10, s. 2326-2330
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Tidskriftsartikel (refereegranskat)abstract
- Despite its importance, the structure and dynamics of liquid water are still poorly understood in many apsects. Here, we report on the observation of optical fluorescence upon soft X-ray irradiation of liquid water. Detection of spectrally resolved fluorescence was achieved by a combination of the liquid microjet technique and fluorescence spectroscopy. We observe a genuine liquid-phase fluorescence manifested by a broad emission band in the 170-340 nm (4-7 eV) photon wavelength range. In addition, another narrower emission near 300 nm can be assigned to the fluorescence of OH (A state) in the gas phase, the emitting species being formed by Auger electrons escaping from liquid water. We argue that the newly observed broad-band emission of liquid water is relevant in search of extraterrestrial life, and we also envision the observed electron-ejection mechanism to find application for exploring solutes at liquid vapor interfaces.
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| 16. |
- Hans, Andreas, et al.
(författare)
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Soft X-ray induced ultraviolet fluorescence emission from bulk and interface of a liquid water microjet
- 2017
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Ingår i: Journal of Physics, Conference Series. - : Institute of Physics Publishing (IOPP). - 1742-6588 .- 1742-6596. ; 875
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Tidskriftsartikel (refereegranskat)abstract
- Tremendous progress has been made in the research on the structure and dynamics of liquids due to the development of advanced experimental techniques such as liquid microjets, enabling investigations on volatile samples in ultrahigh vacuum environments. The spectroscopy of charged particles, e.g. photoelectron or Auger electron spectroscopy on liquids, is an established field by now. Here, we report on the successful application of a fluorescence spectrometer to measure optical emission spectra from liquids irradiated with soft X-ray synchrotron radiation.
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| 17. |
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| 18. |
- Huang, Hongyun, et al.
(författare)
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Clinical Cell Therapy Guidelines for Neurorestoration (IANR/CANR 2017)
- 2018
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Ingår i: Cell Transplantation. - : SAGE Publications. - 0963-6897 .- 1555-3892. ; 27:2, s. 310-324
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Forskningsöversikt (refereegranskat)abstract
- Cell therapy has been shown to be a key clinical therapeutic option for central nervous system diseases or damage. Standardization of clinical cell therapy procedures is an important task for professional associations devoted to cell therapy. The Chinese Branch of the International Association of Neurorestoratology (IANR) completed the first set of guidelines governing the clinical application of neurorestoration in 2011. The IANR and the Chinese Association of Neurorestoratology (CANR) collaborated to propose the current version "Clinical Cell Therapy Guidelines for Neurorestoration (IANR/CANR 2017)". The IANR council board members and CANR committee members approved this proposal on September 1, 2016, and recommend it to clinical practitioners of cellular therapy. These guidelines include items of cell type nomenclature, cell quality control, minimal suggested cell doses, patient-informed consent, indications for undergoing cell therapy, contraindications for undergoing cell therapy, documentation of procedure and therapy, safety evaluation, efficacy evaluation, policy of repeated treatments, do not charge patients for unproven therapies, basic principles of cell therapy, and publishing responsibility.
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| 19. |
- Lange, Kathrin M., et al.
(författare)
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On the Origin of the Hydrogen-Bond-Network Nature of Water : X-Ray Absorption and Emission Spectra of Water-Acetonitrile Mixtures
- 2011
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Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 50:45, s. 10621-10625
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Tidskriftsartikel (refereegranskat)abstract
- A liquid microjet was used to obtain oxygen K-edge X-ray absorption and emission spectra of water–acetonitrile mixtures of various compositions. The observed spectral changes are unambiguously related to the increasing number of broken hydrogen bonds with decreasing water concentration, and the hydrogen-bond network of liquid water can thus be addressed on purely experimental grounds without the need for theoretical modeling.
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| 20. |
- Lange, Kathrin M., et al.
(författare)
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X-ray emission from pure and dilute H2O and D2O in a liquid microjet : Hydrogen bonds and nuclear dynamics
- 2012
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Ingår i: Physical Review B. Condensed Matter and Materials Physics. - 1098-0121 .- 1550-235X. ; 85:15, s. 155104-
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Tidskriftsartikel (refereegranskat)abstract
- Knowledge about the hydrogen bond network of water is essential for understanding its anomalies as well as its special role for biochemical systems. Different types of x-ray spectroscopy allow probing of the molecular orbitals of water, revealing the electronic structure which reflects the hydrogen bond conformations. In this work a recently developed high-resolution x-ray emission spectrometer was used in combination with the microjet technique for recording spectra of liquid H2O and D2O and their mixtures with acetonitrile. Variation of the nuclear dynamics via isotope substitution and variation of the hydrogen bond conformation via dissolution in acetonitrile was investigated. These two effects have two clearly distinguishable spectral fingerprints.
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| 21. |
- Metzler, Veronika M., et al.
(författare)
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Androgen dependent mechanisms of pro-angiogenic networks in placental and tumor development
- 2017
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Ingår i: Placenta. - : W B SAUNDERS CO LTD. - 0143-4004 .- 1532-3102. ; 56, s. 79-85
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Tidskriftsartikel (refereegranskat)abstract
- The placenta and tumors share important characteristics, including a requirement to establish effective angiogenesis. In the case of the placenta, optimal angiogenesis is required to sustain the blood flow required to maintain a successful pregnancy, whereas in tumors establishing new blood supplies is considered a key step in supporting metastases. Therefore the development of novel angiogenesis inhibitors has been an area of active research in oncology. A subset of the molecular processes regulating angiogenesis are well understood in the context of both early placentation and tumorigenesis. In this review we focus on the well-established role of androgen regulation of angiogenesis in cancer and relate these mechanisms to placental angiogenesis. The physiological actions of androgens are mediated by the androgen receptor (AR), a ligand dependent transcription factor. Androgens and the AR are essential for normal male embryonic development, puberty and lifelong health. Defects in androgen signalling are associated with a diverse range of clinical disorders in men and women including disorders of sex development (DSD), polycystic ovary syndrome in women and many cancers. We summarize the diverse molecular mechanisms of androgen regulation of angiogenesis and infer the potential significance of these pathways to normal and pathogenic placental function. Finally, we offer potential research applications of androgen-targeting molecules developed to treat cancer as investigative tools to help further delineate the role of androgen signalling in placental function and maternal and offspring health in animal models.
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| 22. |
- Nolting, Dirk, et al.
(författare)
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pH-induced protonation of lysine in aqueous solution causes chemical shifts in X-ray photoelectron spectroscopy.
- 2007
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 129:45, s. 14068-73
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Tidskriftsartikel (refereegranskat)abstract
- We demonstrate the applicability of X-ray photoelectron spectroscopy to obtain charge- and site-specific electronic structural information of biomolecules in aqueous solution. Changing the pH of an aqueous solution of lysine from basic to acidic results in nitrogen 1s and carbon 1s chemical shifts to higher binding energies. These shifts are associated with the sequential protonation of the two amino groups, which affects both charge state and hydrogen bonding to the surrounding water molecules. The N1s chemical shift is 2.2 eV, and for carbon atoms directly neighboring a nitrogen the shift for C1s is approximately 0.4 eV. The experimental binding energies agree reasonably with our calculated energies of lysine(aq) for different pH values.
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| 23. |
- Ottosson, Niklas, et al.
(författare)
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Large variations in the propensity of aqueous oxychlorine anions for the solution/vapor interface
- 2009
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 131:12, s. 124706-
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Tidskriftsartikel (refereegranskat)abstract
- Core-level photoelectron spectroscopy measurements have been performed of aqueous solutions of NaCl codissolved with NaClOn (n=1-4). Each species has a distinct Cl 2p electron binding energy, which can be exploited for depth-profiling experiments to study the competition between Cl-and ClOn- anions for residing in the outermost layers of the solution/vapor interface. Strongest propensity for the surface is observed for n=4 (perchlorate), followed by n=3 (chlorate), n=2 (chlorite), n=0 (chloride), and n=1 (hypochlorite). Molecular dynamics simulations rationalize the greatest surface propensity of the most oxidized anions in terms of their larger size and polarizability. The anomalous behavior of hypochlorite, being less surface-active than chloride, although it is both larger and more polarizable, is suggested to arise from the charge asymmetry over the anion, increasing its efficiency for bulk solvation. (C) 2009 American Institute of Physics. [doi:10.1063/1.3236805]
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| 24. |
- Sabir, Emad F., et al.
(författare)
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Impact of hospital volume on local recurrence and distant metastasis in bladder cancer patients treated with radical cystectomy in Sweden
- 2013
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Ingår i: Scandinavian Journal of Urology. - : Medical Journals Sweden AB. - 2168-1813 .- 2168-1805. ; 47:6, s. 483-490
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Tidskriftsartikel (refereegranskat)abstract
- Objective. This study evaluated the impact of hospital volume on local recurrence and distant metastasis in a population-based series of radical cystectomy patients in Sweden. Material and methods. All patients who underwent cystectomy for bladder cancer in 1997-2002 in Sweden and were reported to the National Bladder Cancer Registry were included. A high-volume hospital (HVH) was defined as one with >= 10 cystectomies/year and a low-volume hospital (LVH) as one with <10 cystectomies/year. Information on preoperative tumour, node, metastasis (TNM) classification, operative procedure, postoperative course and follow-up was obtained from medical records. Results. Of the 1126 patients, 827 (74%) were males. The mean age was 66 years and median follow-up 47 months. Of the 610 (54%) HVH patients, 68 (11%) were pT0, 123 (20%) pT2 and 69 (11%) were microscopic non-radical. Corresponding figures for the 516 (46%) LVH patients were 35 (7%), 68 (13%), 191 (37%), 222 (43%) and 96 (19%). Local recurrence was observed in 245 patients (22%): 113 (19%) at HVHs and 132 (26%) at LVHs. Distant metastasis was found in 363 (32%): 203 (33%) at HVHs and 160 (31%) at LVHs. Perioperative chemotherapy was given to 193 (17%). Multivariate Cox proportional hazards analysis showed that local recurrence was associated with LVHs and non-organ-confined disease, whereas distant metastasis was correlated with non-organ-confined disease and lymph-node metastases. Conclusions. In this retrospective analysis, local tumour recurrence after cystectomy was common, particularly in patients with non-organ-confined disease. Furthermore, local recurrence was more frequent at LVHs than HVHs, and overall survival was better at HVHs. These findings suggest that concentrating cystectomies in HVHs may improve outcomes such as local recurrence and overall survival.
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| 25. |
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| 26. |
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| 27. |
- Unger, Isaak, et al.
(författare)
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Observation of electron-transfer-mediated decay in aqueous solution
- 2017
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Ingår i: Nature Chemistry. - : NATURE PUBLISHING GROUP. - 1755-4330 .- 1755-4349. ; 9:7, s. 708-714
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Tidskriftsartikel (refereegranskat)abstract
- Photoionization is at the heart of X-ray photoelectron spectroscopy (XPS), which gives access to important information on a sample's local chemical environment. Local and non-local electronic decay after photoionization-in which the refilling of core holes results in electron emission from either the initially ionized species or a neighbour, respectively-have been well studied. However, electron-transfer-mediated decay (ETMD), which involves the refilling of a core hole by an electron from a neighbouring species, has not yet been observed in condensed phase. Here we report the experimental observation of ETMD in an aqueous LiCl solution by detecting characteristic secondary low-energy electrons using liquid-microjet soft XPS. Experimental results are interpreted using molecular dynamics and high-level ab initio calculations. We show that both solvent molecules and counterions participate in the ETMD processes, and different ion associations have distinctive spectral fingerprints. Furthermore, ETMD spectra are sensitive to coordination numbers, ion-solvent distances and solvent arrangement.
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| 28. |
- Winter, Bernd, et al.
(författare)
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Electron dynamics in charge-transfer-to-solvent states of aqueous chloride revealed by Cl- 2p resonant Auger-electron spectroscopy
- 2008
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 130:22, s. 7130-7138
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Tidskriftsartikel (refereegranskat)abstract
- Charge-transfer-to-solvent (CTTS) excited states of aqueous chloride are studied by a novel experimental approach based on resonant inner-shell photoexcitation, Cl-aq(-) 2p -> e(i), i = 1-4, which denotes a series of excitations to lowest and higher CTTS states. These states are clearly identified through the occurrence of characteristic spectator Auger decays to double Cl 3p valence-hole states, where the CTTS states can be more stabilized as compared to single Cl-aq(-) 2p core excitations and optical valence excitations. Furthermore, we have found for the first time that the CTTS electron e(i) bound by a single Cl 2p hole not only behaves as a spectator e(i) -> e'(i), bound by a double valence-hole state before relaxation of the excited electron (i) itself, but also shows electron dynamics to the relaxed lowest state, e(i) -> e'(1*). This interpretation is supported by ab initio calculations. The key to performing photoelectron and Augerelectron spectroscopy studies from aqueous solutions is the use of a liquid microjet in ultrahigh vacuum in conjunction with synchrotron radiation.
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| 29. |
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| 30. |
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