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1.
H. P. Gunnlaugsson 《Hyperfine Interactions》2006,167(1-3):851-854
The general problem of finding a distribution in hyperfine interaction parameters from experimental Mössbauer spectra is outlined. Existing methods may lack flexibility to be easily applicable to simple problems. A line shape for hyperfine parameter distributions is given, which is based on linear segments in the probability function. This method is applied in the analysis of samples containing iron in a silicate glass. 相似文献
2.
Örn Helgason Haraldur P. Gunnlaugsson Siguröur Steinthorsson Steen Mørup 《Hyperfine Interactions》1992,70(1-4):981-984
Mössbauer spectroscopy of basalt lava samples, exhibiting reversible thermal magnetization (JS-T) curves with Curie temperatures of about 580°C, has revealed considerable amounts of maghemite (γ-Fe2O3) in many samples. In view of the expected instability, of maghemite at temperatures above 350°C, this reversibility is rather surprising. Here we report Mössbauer studies on heated lava samples, showing high content of maghemite. The samples were kept at 600°C in oxidizing, reducing, and inactive atmospheres, respectively, for different lengths of time, and then analyzed with Mössbauer spectroscopy at room temperature. The Mössbauer spectra showed that maghemite is stable in the oxidizing atmosphere for at least several hours. In the inactive atmosphere a considerable amount of maghemite still exists after two hours heating. In the reducing atmosphere maghemite had transformed to magnetite after only 30 minutes. 相似文献
3.
H. P. Gunnlaugsson K. Bharuth-Ram M. Dietrich M. Fanciulli H. O. U. Fynbo G. Weyer 《Hyperfine Interactions》2006,169(1-3):1315-1318
We report on the detection of Fe i –B pairs in heavily B doped silicon using 57Fe emission Mössbauer spectroscopy following implantation of radioactive 57Mn+ parent ions (T 1/2?=?1.5 min) at elevated temperatures >?850 K. The Fe i –B pairs are formed upon the dissociation of Fe i –V pairs during the lifetime of the Mössbauer state (T 1/2?=?100 ns). The resulting free interstitial Fei diffuses over sufficiently large distances during the lifetime of the Mössbauer state to encounter a substitutional B impurity atom, forming Fe i –B pairs, which are stable up to ~1,050 K on that time scale. 相似文献
4.
Praic M. Keane Kyra O'Sullivan Fergus E. Poynton Bjrn C. Poulsen Igor V. Sazanovich Michael Towrie Christine J. Cardin Xue-Zhong Sun Michael W. George Thorfinnur Gunnlaugsson Susan J. Quinn John M. Kelly 《Chemical science》2020,11(32):8600
Ruthenium polypyridyl complexes which can sensitise the photo-oxidation of nucleic acids and other biological molecules show potential for photo-therapeutic applications. In this article a combination of transient visible absorption (TrA) and time-resolved infra-red (TRIR) spectroscopy are used to compare the photo-oxidation of guanine by the enantiomers of [Ru(TAP)2(dppz)]2+ in both polymeric {poly(dG-dC), poly(dA-dT) and natural DNA} and small mixed-sequence duplex-forming oligodeoxynucleotides. The products of electron transfer are readily monitored by the appearance of a characteristic TRIR band centred at ca. 1700 cm−1 for the guanine radical cation and a band centered at ca. 515 nm in the TrA for the reduced ruthenium complex. It is found that efficient electron transfer requires that the complex be intercalated at a G-C base-pair containing site. Significantly, changes in the nucleobase vibrations of the TRIR spectra induced by the bound excited state before electron transfer takes place are used to identify preferred intercalation sites in mixed-sequence oligodeoxynucleotides and natural DNA. Interestingly, with natural DNA, while it is found that quenching is inefficient in the picosecond range, a slower electron transfer process occurs, which is not found with the mixed-sequence duplex-forming oligodeoxynucleotides studied.Efficient electron transfer requires the complex to be intercalated at a G-C base-pair. Identification of preferred intercalation sites is achieved by TRIR monitoring of the nucleobase vibrations before electron transfer. 相似文献
5.
Gunnlaugsson T Leonard JP Sénéchal K Harte AJ 《Chemical communications (Cambridge, England)》2004,(7):782-783
The cationic cyclen based Eu(III)-phen conjugated 1.Eu was synthesised as a chemosensor for Cu(II), where the recognition in water at pH 7.4 gave rise to quenching of the Eu(III) luminescence and the formation of tetranuclear polymetallic Cu(II)-Eu(III) macrocyclic complexes in solution where Cu(II) was bound by three 1.Eu conjugates. 相似文献
6.
The cyclen based aromatic diaza-15-crown-5 and 18-crown-6 ether conjugates 1Tb-4Tb were designed as luminescent switches for sodium and potassium where the delayed Tb(III) emission, occurring as line-like emission bands between 490-622 nm, was 'switched on' upon recognition of these ions in pH 7.4 buffered water solution. 相似文献
7.
This article highlights some of the recent developments in the use of responsive cyclen based lanthanide luminescent devices, focusing on Eu(III), Tb(III), Nd(III) and Yb(III) complexes, where the photophysical properties, such as the excited state lifetimes, quantum yield/intensity and emission polarisation are modulated by the local chemical environment, e.g. ions and molecules, or through self-assembly of either f-f or mixed f-d cyclen complexes. 相似文献
8.
T Gunnlaugsson D A Mac Dónaill D Parker 《Journal of the American Chemical Society》2001,123(51):12866-12876
The Eu(III) tetraazamacrocyclic complexes [Eu.1] and [Eu.2], and the Tb(III) and Yb(III) complexes [Tb.1] and [Yb.2], have been synthesized as luminescent molecular-level devices. The Eu complexes exhibit unique dual pH switching behavior in water under ambient conditions. The delayed Eu emission is reversibly switched on in acid, with an enhancement factor of several hundred for [Eu.1]. These observations are consistent with the protonation of the quinoline aryl nitrogen moiety (pK(a) approximately equal to 5.9 for [Eu.1]). The fluorescence emission spectra of these complexes are unaffected by acid, but pronounced changes occur in alkaline solution due to the deprotonation of the aryl amide nitrogen (pK(a) approximately 9.4 for [Eu.1]). [Tb.1] shows a more intriguing pH dependence; Tb emission is switched "on" only in the presence of H+ and in the absence of molecular oxygen, whereas the fluorescence emission properties are similar to those observed with [Eu.1]. This behavior can be conveniently described as a molecular-level logic gate, corresponding to a two-input INHIBIT function, A wedge B'. The analogous [Yb.2] complex shows no such pH or O(2) dependence. 相似文献
9.
Exploring the Effect of Ligand Structural Isomerism in Langmuir–Blodgett Films of Chiral Luminescent EuIII Self‐Assemblies 下载免费PDF全文
Agostino Galanti Dr. Oxana Kotova Dr. Salvador Blasco Chloe J. Johnson Dr. Robert D. Peacock Shaun Mills Prof. John J. Boland Prof. Martin Albrecht Prof. Thorfinnur Gunnlaugsson 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(28):9709-9723
Here we have investigated the influence of the antenna group position on both the formation of chiral amphiphilic EuIII‐based self‐assemblies in CH3CN solution and, on the ability to form monolayers on the surface of quartz substrates using the Langmuir–Blodgett technique, by changing from the 1‐naphthyl ( 2(R) , 2(S) ) to the 2‐naphthyl ( 1(R) , 1(S) ) position. The evaluation of binding constants of the self‐ assemblies in CH3CN solution was achieved using conventional techniques such as UV/Visible and luminescence spectroscopies along with more specific circular dichroism (CD) spectroscopy. The binding constants obtained for EuL , EuL2 and EuL3 species in the case of 2‐naphthyl derivatives were comparable to those obtained for 1‐naphthyl derivatives. The analysis of the changes in the CD spectra of 1(R) and 1(S) upon addition of EuIII not only allowed us to evaluate the values of the binding constants but the resulting recalculated spectra may also be used as fingerprints for assignment of the chiral self‐assembly species formed in solution. The obtained monolayers were predominantly formed from EuL3 (≈85 %) with the minor species present in ≈15 % EuL2 . 相似文献
10.
Thorfinnur Gunnlaugsson Andrew J. Harte Joseph P. Leonard Mark Nieuwenhuyzen 《Supramolecular chemistry》2013,25(7-8):505-519
The synthesis of four lanthanide ion complexes Eu?1, Eu?2, Tb?1 and Tb?2, from the heptadentate tri-arm cyclen (1,4,7,10-tetraazacyclododecane) ligands 1 and 2 that were made in one-pot syntheses is described. These coordinatively unsaturated complexes have two labile metal-bound water molecules, as demonstrated by X-ray crystallography. This was also confirmed by evaluating their hydration state (q~2) by measuring their lifetimes in D2O and H2O, respectively. The above complexes were all designed as being “photophysically silent” prior to the recognition of the anion, since they do not possess antenna that can participate in sensitisation of the Eu(III) or the Tb(III) excited state. However, the two water molecules can be displaced upon anion binding by the appropriate aromatic carboxylates to give ternary complexes in water, through either four- or six-member ring chelates (q~0), or possibly via a monodentate binding. In the case of Tb?1 and Tb?2, large luminescence enhancements were observed upon the formation of such ternary complexes with N,N-dimethylaminobenzoic acid at ambient pH. Such binding and luminescent enhancements were also observed for Tb?1 in the presence of salicylic acid. On all occasions, the anion recognition “switched” the emission “on” over two logarithmic units. At higher concentrations, the emission is reduced possibly due to quenching. In the case of aspirin, the binding was too weak to be measured, indicating that Tb?1 selectively detects salicylic acid, the active form of aspirin in water. In the case of Eu?1 and Eu?2, the affinity of these complexes towards such aromatic carboxylates was too weak for efficient ternary complex formation. 相似文献