These Proceedings are also a blueprint for development of electron paramagnetic resonance (EPR) / electron spin resonance (ESR) in the Asia-Pacific region in the 21st century. The Symposium reflected a variety of research fields developed over half a century and focuses especially on the most recent developments, such as high-field and high-frequency EPR, which are envisaged to be further developed and applied to various fields in the 21st century.
All sessions consisted of Plenary, Invited and Contributed presentations. The Plenary presentations aimed at summarizing the overall developments. Invited presentations, reviewing the most recent developments, and Contributed ones, dealing with original research recently carried out in the EPR/ESR area, were given in one of three parallel sessions. The unique research works presented cover various fields and reflect the existing diversity of applications of the EPR/ESR techniques.
The Proceedings in this volume are a refereed selection of presentations from The Third Asia-Pacific EPR/ESR Symposium (APES'01), held in Kobe, Japan from October 29 to November 1, 2001. Participants from 20 countries from Asia, Australia, Europe, North and South America presented 210 papers, of which 132 are included here.These Proceedings are also a blueprint for development of electron paramagnetic resonance (EPR) / electron spin resonance (ESR) in the Asia-Pacific region in the 21st century. The Symposium reflected a variety of research fields developed over half a century and focuses especially on the most recent developments, such as high-field and high-frequency EPR, which are envisaged to be further developed and applied to various fields in the 21st century.All sessions consisted of Plenary, Invited and Contributed presentations. The Plenary presentations aimed at summarizing the overall developments. Invited presentations, reviewing the most recent developments, and Contributed ones, dealing with original research recently carried out in the EPR/ESR area, were given in one of three parallel sessions. The unique research works presented cover various fields and reflect the existing diversity of applications of the EPR/ESR techniques.
Front Cover 1
EPR IN THE 21st CENTURY: BASICS AND APPLICATIONS TO MATERIAL, LIFE AND EARTH SCIENCES 4
Copyright Page 5
Contents 10
Editorial Note 6
President's Message 7
Contributors 8
Committees 9
Section 1: Physics and Magnetism 24
Chapter 1. Electron magnetic resonance (EMR) of the spin S> 1 systems: an overview of major intricacies awaiting unwary spectroscopists
Chapter 2. Recent developments in low-temperature ESR in quantum antiferromagnetic chains 38
Chapter 3. Direct numerical study on ESR line shape 50
Chapter 4. g Tensor of Er3+ centers in axial symmetry 56
Chapter 5. Continuous wave and pulsed EPR spectroscopy of paramagnetic ions in some fluoride, silicate and metaphosphate glasses 62
Chapter 6. Frequency dependence of resonance in one-dimensional antiferromagnetic Heisenberg chain 71
Chapter 7. ESR selection rules for direct transition of spin gap 77
Chapter 8. Spin solitons in the alternate charge polarization background of MMX chains 82
Chapter 9. Full Monte Carlo and Fourier transformed Monte Carlo EPR spectral simulations of 8s state ions 86
Chapter 10. X-Band ESR measurements of spin ladder system BIP-TEN0 92
Chapter 11.ESR Studies of a spin1 / 2 ferromagnetic-ferromagnetic-antiferromagnetic- antiferromagnetic tetramer chain 96
Chapter 12.ESR Studies of quasi-one-dimensional halogen-bridged mixed-metal complexes 102
Chapter 13. Microwave radiation from magnetostatic mode in high power FMR 108
Chapter 14. Parametrically excited magnetoelastic waves in FeB03 112
Chapter 15. Slow dynamics in chaotic magnon system 116
Chapter 16. ESR studies of spin-polarized atomic hydrogen adsorbed on 3He-4He mixture film 120
Section 2: Materiais Sciences 126
Chapter 17. Electron spin resonance studies of molecular photoionization in Cr-AlMCM-4 1 mesoporous oxide materials 128
Chapter 18. ESR and ENDOR spectroscopy of solitons and polarons in conjugated polymers 136
Chapter 19. ESR study of deoxygenated high-temperature superconductors and their constituents 148
Chapter 20. Magnetic phase separation in Lal,Ca,MnO3 near half-doped composition observed by EMR 150
Chapter 21. Temperature rises by microwave absorptions in superconducting materials and liquid nitrogen bubbling 156
Chapter 22. Comparison of near-Tc behaviors of microwave absorption and resistance in bulk YBCO superconductors 162
Chapter 23. Estimation of fluxon response-delay from magnetic field variations in superconductors using ESR system 168
Chapter 24. Coexistence of ferromagnetism with superconductivity in RuSr2GdCu208 from ESR measurements 174
Chapter 25. Ferromagnetic resonance and intragrai/intergrain crystallinity in La-Ba-Mn-0 thin films 180
Chapter 26. Temperature dependence of paramagnetic resonance in pure and doped ferrihydrite nanoparticles 185
Chapter 27. ESR study of Fe-SiOz granular films 191
Chapter 28. Oxygen dependent evolution of C60+ EPR signal in fullerene thin films 197
Chapter 29. Molecular orientations in Langmuir-Blodgett and vacuum-deposited films of VO-phthalocyanine 203
Chapter 30. Structural elucidation of vacuum deposited films of titanyl phthalocyanine by EPR 209
Chapter 31. ESR investigation of organic conductor with itinerant and local spins, (CHTM-TTP)zTCNQ 215
Chapter 32. X-band ESR measurements of Et2Me2P[Pd(dmit)2]2 220
Chapter 33. The role of Li+ and Na+ charge compensators in Sm3+-doped CaF2 and SrF2 224
Chapter 34. The HF and SHF interactions of V02+ ions in KZnClS04.3H20 single crystals 230
Chapter 35. EPR study of several Cr3+ centers in K2MgCl4 single crystal 236
Chapter 36. EPR study of Cr3+ centers in T12MgF4 and T12ZnF4 crystals 242
Chapter 37. Single crystal EPR study of Cr(II1)-doped magnesium potassium Tutton's salt 248
Chapter 38. ESEEM study of 14N nuclear quadrupole resonances in S=3/2 chromium(II1) complex 254
Chapter 39. EPR investigation of inhomogeneous phases in improper ferroelastic MgTiF6.6H20:Mn2+ 259
Chapter 40. EPR investigations on Fe3+ ions in alkali borotellurite glasses 265
Chapter 41. EPR study of X-ray and UV irradiated GeO2 glasses prepared by the sol-gel method 270
Chapter 42. Structural studies of the fresh water (Apple) snail, Pila globosa shells 276
Chapter 43. ESR study of iron-sites on Fe-ZSM5 zeolite 282
Chapter 44. CW/pulsed ESR studies of Euz+-doped SrA1204 phosphor 287
Chapter 45. Thermoluminescent mechanism of tridymite SiO2 phosphors 293
Chapter 46. ESR and luminescence spectral properties of europium compounds with trifluoroacetic acid 299
Chapter 47. ESR and luminescence studies on formation of Si ions through photochemical reactions in potassium halide crystals doped with sulfur and manganese 305
Chapter 48. Hyperfine structure ofNd3+ and Er3+ ions in LiNbO3 crystals 311
Chapter 49. The nature of coduction ESR linewidth temperature dependence in graphite 316
Chapter 50. ESR measurement of heavily doped Si:Fe 321
Chapter 51. ESR study of heavily doped GaAs:Er grown by organometallic vapor phase epitaxy 325
Chapter 52. Location of dangling bonds in ELA poly-Si 329
Chapter 53. ESR studies of BEDT-TTF organic conductors containing supramolecular assemblies 335
Chapter 54. EPR spectral study of gadolinium (111) cryptate 339
Chapter 55. Ground-recognition ability of b- and y-cyclodextrins as studied by the high-pressure EPR 345
Chapter 56. ESR Studies on a new phenyl t-butyl nitroxide biradical based on calix[4]arene 349
Section 3: Chemical Reactions 354
Chapter 57. Time-resolved EPR studies of excited states: some old and some new stories 356
Chapter 58. Time-resolved EPR studies of the excited triplet states of p-methylcinnamic acid and its deprotonated anion 367
Chapter 59. Quenching of singlet molecular oxygen (1Deltag) by vitamins and polyphenols studied by time-resolved ESR 372
Chapter 60. A time-resolved EPR study of weakly coupled triplet-doublet pairs of copper(II)-free base porphyrin dimers 378
Chapter 61. Pulsed-ESR investigations of the photo-excited triplet state of naphthalene 384
Chapter 62. Light-induced ESR studies of regioregular poly(3-alkylthiophene)-C6o composites 390
Chapter 63. ESR study of photodecomposition mechanism of a long-lived radical perfluoro-2,4-dimethyl-3-ethylpentyl-3. ESR spectrum of trifluoromethyl radical formed during solid-phase photodecomposition at 77K in glassy matrix 396
Chapter 64. ESR study and quantum-chemical calculations of alkyl radicals in the matrix of polycrystalline n-alkane irradiated at 77 K. Effects of intermolecular interactions and carbon chain length on the radical formation 401
Chapter 65. ESR/ENDOR study for new radical dianion species of 6-oxophenalenoxyl derivative 407
Chapter 66. Spin labeling study of polymer chain motion in PEGPVP blend 412
Chapter 67. EPR and UV-VIS studies on the influence of solute-solvent interactions on the self-redox reaction of bis (dithiophosphate) copper(II) 418
Section 4: Environmental Sciences 424
Chapter 68. In vivo and ex vivo EPR spectroscopy and imaging of endogenously produced nitric oxide under physiological and pathophysiological conditions 426
Chapter 69. Molecular-electronic mechanism of the toxicity of Dioxin and ability of some natural structures to concurrently interact to inhibit its activity 435
Section 5: Biology and Life Sciences 442
Chapter 70. Kinetic EPR study on reactions of vitamin E radicals 444
Chapter 72. ESR investigation on ROS initiated by visible light in PSI1 particles of high plants 452
Chapter 73. EPR and theoretical investigations of NiFe] hydrogenase: Insight into the mechanism of biological hydrogen conversion 460
Chapter 74. EPR studies on free radical generation by the reaction of methylglyoxal with amino acids and protein 469
Chapter 75. EPR monitoring on the quality of life 479
Chapter 76. EPR studies of manganese spin centers in the even-number oxidation states of water oxidizing complex in photosystem I1 489
Chapter 77. Magnetic resonance studies on ascorbate binding to albumin 494
Chapter 78. Electron magnetic resonance study on the effect of radioactive radiation on the photosynthesis of chlorophyll in lipid bilayers 500
Chapter 79. Effects of tannin compounds on metal ion-hydrogen peroxide systems 506
Chapter 80. The [2Fe-2S] cluster in sulredoxin from the thermoacidophilic archaeon sulfolobus tokodaii strain 7, a novel water-soluble Rieske protein 511
Chapter 81. EPR and saturation recovery investigations of spin probes in dispersions of hydrogenated castor oil 517
Section 6: Medical Sciences 524
Chapter 82. Advances in the spin labeling method 526
Chapter 83. Recent progress and future prospects of free radical imaging by PEDRI 538
Chapter 84. Electron paramagnetic resonance in medicine 548
Chapter 85. Development of in vivo ESW/spin probe technique for oxidative injuries 556
Chapter 86. In vivo ESR studies on spin-clearance in GPxl -transgenic mice 565
Chapter 87. Non-invasive analysis of stress-induced gastric ulcer in rats 571
Chapter 88. Nitric oxide production and inducible nitric oxide synthase induction in iron-loaded rats 575
Chapter 89. Collapse of redox state by glutamate transporter inhibition in the rat’s hippocampus 579
Chapter 90. Non-invasive assessment of oxidative stress in the brain of small animal models by using in vivo electron spin resonance (ESR) imaging system 585
Chapter 91. Possible production of hydroxyl free radical in the gastric legion of nitroso carcinogen-administrated rats 590
Section 7: Geology 596
Chapter 92. EPR and optical absorption spectroscopy on minerals 598
Chapter 93. Thermoluminescence and ESR centers of fluorapatite crystal from Brazil 608
Chapter 94. Spectral studies of divalent copper in antlerite mineral 612
Chapter 95. Paramagnetic criterions of prognosis for oil and gas rocks content 618
Section 8: Dosimetry 624
Chapter 96. EPR dose reconstruction in teeth: Fundamentals, applications, problems and perspectives 626
Chapter 97. ESR dating applications in archaeology and earth sciences 636
Chapter 98. ESR and NMR dosimetry 637
Chapter 99. K-band ESR spectra of irradiated tooth enamel 647
Chapter 100. Assessment of contribution of confounding factors to cumulative dose determined by EPR of enamel 651
Chapter 101. Retrospective EPR-dosimetry in Semipalatinsk nuclear test site region 657
Chapter 102. Determination of total ionizing radiation dose on animals from west Kazakhstan by EPR method 663
Section 9: Cross-Disciplinary and Methodology 668
Chapter 103. Pulsed ESR double resonance (PELDOR) spectroscopy: Application to spin-labeled peptides 670
Chapter 104. The carotenoid triplet state in Rhodobacter sphaeroides reaction centers. An EPR magnetophotoselection study 682
Chapter 105. Electron dipole-dipole interaction in ESEEM of biradicals 692
Chapter 106. The influence of label spins on EPR spectra of charge separated states in photosynthetic reaction center 701
Chapter 107. The structural analysis of photosystem I1 by PELDOR of three spin system 702
Chapter 108. Application of pulsed ELDOR detected NMR measurements on the studies of photosystem I1 707
Chapter 109. Pulsed-ENDOR cavities modified from the CW-ENDOR TM-mode and pulsed-ESR TE-mode cavities 711
Chapter 110. Ferroelectric resonators for EPR spectrometers at 35, 65 and 125 GHz 717
Chapter 111. Fourier-transform ESR spectroscopy and observation of ultrafast spin-lattice relaxation by optical means 723
Chapter 112. Subnanosecond relaxation of optically-induced magnetization in aqueous solutions of transition-metal ions 729
Chapter 113. Detection of the internal electric field and relaxational magnetoelectric effect in chromium mesogen 733
Section 10: High Frequency and High Field EPR 740
Chapter 114. Modern ESR methods in studies of the dynamic structure of proteins and membranes 742
Chapter 115. High-frequency single-crystal EPR application to multifrequency approach: Study of metalloproteins 754
Chapter 116. EPR evidence of onset of the quantum critical point in CuGe03:Fe 764
Chapter 117. Millimeter and submillimeter wave ESR measurements of spin ladder system Sr(Cul.,ZnX)2O3 770
Chapter 118. High frequency ESR on quantum spin systems by using single shot and repeating pulsed fields 774
Chapter 119. ESR study on magnetic ordering of spin-frustrated antiferromagnet ZnCr204 single crystal 778
Chapter 120. ESR study of frustrated spin chain [Cu(bpy)HzO] [Cu(bpy)(mal)H2O](C104)2 782
Chapter 121. Millimeter wave ESR measurement of diamond chain substance azurite 786
Chapter 122. High field ESR of(Ca1-ySry)1-x CuO2 with edge-sharing Cu02 chain 790
Chapter 123. High field ESR measurements of(V0)2P207 794
Chapter 124. ESR measurements on triangular antiferromagnets CsCu~.,Co,Cl~ 798
Chapter 125. Gyrotron ESR in CsFeC13 up to 40 T 802
Chapter 126. Magnetic properties of Fe12 ring: ESR and magnetization measurements 807
Chapter 127. High magnetic field ESR measurements of ACu2(P04)2 (A=Ba, Sr) 811
Chapter 128. ESR transmission experiments on b’-(ET)2SF5CF2SO3 and (ET)2SF5NN02, investigations of spin-Peierls systems 816
Chapter 129. High field ESR measurements on molecular oxygen 822
Chapter 130. High field ESR measurements ofCuZ(CsH12N2)2C14 under high pressure 826
Chapter 131. ESR at ultra-low temperatures and observation of new mode in Cu-Benzoate 830
Chapter 132. ESR spectrometer using frequency tunable gyrotrons as a radiation source 836
Chapter 133. High-frequency (W-band) EPR studies of biological samples 841
Author Index 848
Electron magnetic resonance (EMR) of the spin S≥1 systems: an overview of major intricacies awaiting unwary spectroscopists
C. Rudowicz Department of Physics and Materials Science, City University of Hong Kong, Kowloon Tong, Hong Kong SAR, China
The aim of this paper is to bring about a better understanding of the intricacies of the spin Hamiltonian (SH) theory. A number of theoretical aspects underpinning the experimental EMR (encompassing EPR, ESR and related techniques) studies of paramagnetic species with the spin S≥1, especially transition ions, which require a thorough clarification, are critically reviewed. Examples of the intricacies awaiting unwary spectroscopists, drawn from recent EMR literature, are discussed in a nutshell in order to illustrate the potential pitfalls and their consequences.
1 INTRODUCTION
Electron magnetic resonance (EMR), which nowadays encompasses electron paramagnetic resonance (EPR ‐ the term dominating applications in physics) and electron spin resonance (ESR ‐ the term dominating applications in chemistry) as well as related techniques, is a mature area with applications ranging from biology to materials sciences [1–8]. However, various theoretical aspects underpinning the interpretation of experimental EMR data, which are often confused in the EMR literature, can be identified. In this paper the major points concerning EMR studies of paramagnetic species with the spin S≥1, especially transition ions, which have recently been clarified, are reviewed. Examples of the intricacies awaiting unwary spectroscopists, drawn from recent EMR literature, are presented in a nutshell in order to illustrate the potential pitfalls, e.g. usage of erroneous relations and misinterpretation of experimental EMR data. Thus we hope to bring about a better understanding of the intricacies of the spin Hamiltonian (SH) theory [9–14], especially the zero‐field splitting (ZFS) Hamiltonian, ZFS, and the crystal‐field (CF) Hamiltonian, CF, which are fundamental to EMR studies [1–8]. Ramifications include the magnetic susceptibility, magnetic anisotropy, Mössbauer spectroscopy, which rely on SH, as well as the optical absorption spectroscopy, inelastic neutron scattering, and infrared spectroscopy, which rely on CF Hamiltonian.
First we outline briefly the reference notations for ZFS [1, 2] to provide background for the discussion in Sections 2 to 7. In terms of the extended Stevens (ES) operators [9] the compact form of ZFS (as defined in [10]; to be distinguished from the expanded form using explicitly the pairs of the tensor operators with ±q in ZFS) is given as:
ZFS=∑kqBkqOkq(Sx,Sy,Sz)=∑kqfkbkqOkq(Sx,Sy,Sz).
(1)
The uniform ‘scaling’ of ZFS parameters kq requires the factors fk to be taken as [1,2,10, 14]:
2=1/3,f4=1/60,f6=1/1260
(2)
For numerical convenience, the second form of ZFS Equation (1) has been more often used in EMR studies of transition ions.
The conventional form of ZFS most widely used in the literature, which is suitable for paramagnetic species with the spin S≥ 1 at sites with triclinic symmetry, is given by [1–7, 10]:
ZFS=S.D.S,
(3)
whereas for the spin S≥2 the higher‐order ZFS terms are required. For orthorhombic symmetry as well as for monoclinic and triclinic symmetry with ZFS expressed in the principal axis system, the conventional form of ZFS is given by [1–3, 10, 14]:
ZFS=D[Sz2−13S(S+1)]+E[Sx2−Sy2]
(4)
where the axes (x, y, z) may be chosen in different ways for orthorhombic symmetry [10, 11] (see Section 5), whereas for monoclinic and triclinic symmetry the orientation of the principal axes (x, y, z) with respect to the crystallographic axis system (X, Y, Z) must be provided [10].
In Sections 2 to 6 various categories of the intricacies of the SH theory are briefly outlined; for details and references the reader shall refer to the respective original papers. In Section 7 possible remedies to some of the problems encountered by experimentalists in interpretation of EMR data are presented.
2 MAJOR INTRICACIES CONCERNING NOTATIONS AND NOMENCLATURE
2.1 Multitude of notations for the operators and the ZFS parameters
There exist in the EMR (as well as CF) literature a multitude of notations for the operators and the associated ZFS (CF) parameters. Such an abundance hampers comparisons of data from various sources. All notations appearing in the EMR‐related literature up to late 1986 were comprehensively surveyed in [10], whereas recent literature will be summarized in [12]. A general pitfall concerning all SH notations consists in the misleading or often inconsistent nomenclature for various terms appearing in ZFS. Historical developments have led to the existence of various SH notations classified briefly into three groups as follows [10,14].
A Conventional SH notations
Any notation using explicitly the ‘spin’ operators Sx, Sy, Sz or Sz, S± =Sx ± iSy, like Equations (3) and (4), belongs to the conventional notations [10]. In fact, the ‘spin’ may mean the physical spin S, or the effective spin, ˜, or the fictitious spin, S′ (see Section 3). The conventional notations are particularly inconvenient for low‐symmetry, e.g. monoclinic and triclinic, which require a large number of ZFS terms [10]. Hence, these notations have been mostly used for higher‐symmetry and low‐spin cases [1–8, 10]. In spite of the widespread usage of the tensor‐operator notations in the literature, some recent books still adopt only the conventional notation with the former notations receiving only scant remarks, see, e.g. [4–7]. The major pitfall concerning the conventional SH notation is the existence of a number of conventions for operator combinations and symbols for ZFS parameters as reviewed in [10]. One must be cautious when comparing SH parameter values from different original sources and reviews.
B Tensor‐operator notations
Tensor‐operator notations may be collectively denoted by the generic symbols: χlm for operators and Alm for the associated parameters [10, 14]. Apart from the most common product form: Almχlm, alternate tensor forms of the ZFS Hamiltonian are sporadically used in the literature [10, 14]. The advantages of the tensor operators [10, 14] have led to the development of several notations, which can be subdivided into two subgroups, each consisting of several different types of tensor operators interrelated by conversion coefficients. The general classification briefly outlined below may serve as a quick reference guide for practitioners. The most representative symbols originally introduced for the operators and their coefficients, defining the ZFS parameters, are given for each tensor‐operator notation. A full review of the present status and a detailed survey of operator and parameter notations currently in usage in the EMR area, including a list of specific intricacies, will be provided in [12]. A general pitfall concerning the tensor‐operator notations is the fact that several symbols have been used for the same quantity and conversely, the same symbols have been used to denote different quantities.
B1 Tesseral‐tensor operators (TTO)
Historically [9, 14] Stevens [15] introduced an incomplete set of tesseral‐tensor operators (TTO), kq(L), being “operator equivalents” of real tesseral harmonics with the components q limited to k ≥ q ≥ 0, which latter become known as the Stevens operators [1, 3, 9, 10]. Some misleading statements concerning the ‘operator equivalents’ in [4] are discussed in [14]. The Stevens operators, kq(S), with L replaced by S (in fact ˜ or S′ ‐ see Section 3) have been widely used in the EMR area. However, the lack of the negative q components hampered application of the Stevens operators for low‐symmetry cases [10]. The extended Stevens (ES) operators kq(S) including all components: −k ≤ q ≤ +k were introduced and their transformation properties were worked out in [9]. These are now the most widely used operators in the EMR area. Thus we adopt the ES operators as the...
| Erscheint lt. Verlag | 1.7.2002 |
|---|---|
| Sprache | englisch |
| Themenwelt | Schulbuch / Wörterbuch ► Lexikon / Chroniken |
| Naturwissenschaften ► Chemie ► Analytische Chemie | |
| Naturwissenschaften ► Chemie ► Physikalische Chemie | |
| Naturwissenschaften ► Physik / Astronomie ► Elektrodynamik | |
| Technik | |
| ISBN-10 | 0-08-053972-6 / 0080539726 |
| ISBN-13 | 978-0-08-053972-0 / 9780080539720 |
| Haben Sie eine Frage zum Produkt? |
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