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1.
We have tailored some interesting mono- and diporphyrins, viz., 5, 10, 15, 20-tetrakis(octadecyloxyphenyl)-21 H,23 H-porphyrin (TP), 5, 15-bis(3, 5-dioctylphenyl)-2, 8, 12, 18-tetramethyl-3, 7, 13, 17-tetradodecyl-21 H,23 H-porphyrin (AP) and 1, 3-bis(10′,20′-diundecyl-21′ H,23′ H-porphyrin-5′-yl)benzene (DP) as host molecules to study their complexation behavior with C 60 and C 70. Fluorescence spectroscopic measurements showed that emission of TP, AP and DP in toluene was quenched in the presence of C 60 or C 70. Large binding constants ( K) in the magnitude of 1.5 × 10 4 dm 3 mol −1 have been obtained for the 1:1 complexes of C 70 with TP, AP and DP. However, the C 60 complexes have exhibited 8.5 times smaller K compared to C 70 complexes. Ab initio theoretical calculations give a good support in favor of strong complexation between C 70 and porphyrins. 相似文献
2.
In the present theoretical work we have explored mechanisms of dissociation reactions of the vinyl radical in the A 2A″ state (C 2H 3 (A 2A″)) and examined possible pathways for nonadiabatic dissociation of C 2H 3 (A 2A″) into C 2H 2 (X 1Σ g+). In the calculations we used the complete active space self-consistent field (CASSCF) and multiconfiguration second-order perturbation theory (CASPT2) methods in conjunction with the cc-pVDZ and cc-pVTZ basis sets. Mechanisms for the following three dissociation channels of C 2H 3 in the A 2A″ state were explored: (1) C 2H 3 (A 2A″) → C 2H 2 ( trans, 3A u) + H, (2) C 2H 3 (A 2A″) → C 2H 2 ( cis, 3A 2) + H, and (3) C 2H 3 (A 2A″) → H 2CC ( 3A 2) + H. The CASSCF and CASPT2 potential energy curve calculations for the C 2H 3 (A 2A″) dissociation channels (1)–(3) indicate that there is neither transition state nor intermediate for each of the channels. At the CASPT2//CASSCF/cc-pVTZ level, the dissociation energies for channels (1)–(3) are predicted to be 84.3, 91.1, and 86.9 kcal/mol, respectively. For a recently observed nonadiabatic dissociation of C 2H 3 (A 2A″) into C 2H 2 (X 1Σ g+) + H [J. Chem. Phys. 111 (1999) 3783], two previously suggested internal conversion (IC) pathways were examined based on our CASSCF and CASPT2 calculations. Our preliminary CASSCF and CASPT2 calculations indicate that the assumed IC pathway via the twisted C 2H 3 (A 2A ′) structure might be feasible. The CASSCF/cc-pVTZ geometry optimization and frequency analysis calculations were performed for the four C 2v bridge structures in the 2B 2, 2A 2, 2B 1, and 2A 1 states along the pathways of the 1 2A ′ (X 2A ′), 1 2A″ (A 2A″), 2 2A″, and 2 2A ′ states of C 2H 3, respectively, and the CASPT2//CASSCF/cc-pVTZ energetic results indicate that the assumed IC pathway, via a C 2v ( 2A 2) structure and then 2A 2/ 2A 1 surface crossing, be not feasible since at their excitation wavelengths (327.4 and 366.2 nm) the C 2v ( 2A 2) structure could not be accessed. 相似文献
3.
The photoabsorption spectrum of ozone in the UV range (5–9 eV) is calculated from a short-time wave packet propagation using six potential energy surfaces obtained from ab initio electronic structure calculations. It is shown that the (unnamed) band around 7 eV, which is immediately adjacent to the intense Hartley band, is primarily due to excitation of three electronic states: 5 1A′ (3 1A 1), 6 1A′ (4 1A 1), and 4 1A″ (2 1B 1). Excitation of the state 8 1A′ ( 1B 2) leads to a broad and intense band starting around 8 eV with a maximum near 9.1 eV. In full accord with the recent experimental study of Brouard et al. [M. Brouard, R. Cireasa, A.P. Clark, G.C. Groenenboom, G. Hancock, S.J. Horrocks, F. Quadrini, G.A.D. Ritchie, C. Vallance, J. Chem. Phys. 125 (2006) 133308], the excitation at 193 nm (6.42 eV) involves at least two states (5 1A′ and 4 1A″) different from the state excited in the Hartley band (3 1A′). The dynamics along the dissociation path is discussed in terms of one-dimensional potential curves. Several avoided crossings among the excited 1A′ as well as the 1A″ states point to a complicated fragmentation process. Although a quantitative analysis of branching ratios is not possible on the basis of the present calculations, we surmise, that in addition to and O( 1D) + O 2( 1Δ g), the next higher spin-allowed channel, , also is likely to be a major product channel, in agreement with experimental observations. 相似文献
4.
Mg +—Ar ion—molecule complexes are produced in a pulsed supersonic nozzle cluster source. The complexes are mass selected and studied with laser photodissociation spectroscopy in a reflectron time-of-flight mass spectrometer system. An electronic transition assigned as X 2Σ + → 2Π is observed with an origin at 31387 cm −1 (vac) for 24Mg +—Ar. The 24Mg +—Ar spectrum is characterized by a 15 member progression with a frequency (ω′ e) of 272 cm −1. An extrapolation of this progression fixes the excited state dissociation energy ( D′ o) at 5552 cm −1. The corresponding ground-state value ( D″ o) is 1270 cm −1 (3.6 kcal/mol). The 2Π
,
spin—orbit splitting is 76 cm −. 相似文献
5.
139La-NMR chemical shifts were measured for several anionic complexes of formulae Li(C 4H 8O 2) 3/2 [La(ν 3-C 3H 5) 4], [Li(C 4H 8O 2) 2][Cp′ nLa(ν 3-C 3]H 5) 4−n] (Cp′ = Cp(ν 5-C 5H 5); n = 1, 2 and Cp′ = Cp * (ν 5-C 5Me5); N = 1) and Li[R nLa(ν 3-C 3H 4) 4− n] (R = N(SiMe 3) 2; n = 1, 2 and R = CCsIMe 3; n = 4), as well as for neutral compounds for formulae La(ν 3-C 3H 5) 3L n (L = (C 4H 8O 2) 1.5, (HMPT) 2, TMED), Cp′ nLa(ν 3-C 3H 5) 3−n (Cp′= Cp(ν 5-Cp 5H 5), Cp *(ν 5-C 5Me 5); n = 1, 2) and La(ν 3-C 3H 2) 2X(THF) 2 X = Cl, Br, I). Typical ranges of the 139La-NMR chemical shifts were found for the different types of complex independent of number and kind of organyl groups directly bonded to lanthanum. Zusammenfassung139La-NMR-Spektroskopie wurde an einer Reihe anionischer Allyllanthanat(III)-Komplexe der Zusammensetzung
]- [La)ν3-C3H5)4, [Li(C4H8)2][Cp′nLa(ν3-C3H5)4−n(Cp′ = Cp(ν5-C5H5); n = 1, 2 und Cp′ = Cp * (ν5-C5Me5); N = 1) und Li[RnLa(ν3-C3H5)4−n (R = B(SiMe3)2; n = 1, 2 und R = CCSiMe3; n = 4 sowie neutraler Allyllanthan(III)-Komplexe der Zusammensetzung La(ν3-C3H5)3Ln (Ln = (C4H8O2)1.5, (HMPT)2, TMED), Cp′n, La(ν3-C3H5)3−n (Cp′ = Cp(ν5-C5H5), Cp * (ν5- Cp5Me5); n = 1, 2) und La(ν3-Cp3H5)2X(THF)2 (X = Cl, Br, I) durchgefürt. In Abhängikeit von der Anzahl und der Art der am Lanthan gebundenen Gruppen wurden für die verschieden Komplextypen charakteristische Resonanzbereiche ermittelt. 相似文献
6.
Saddle point geometries and barrier heights have been calculated for the H abstraction reaction HO 2( 2A″)+H( 2S) → H 2( 1Σ +g)+O 2( 3Σ −g) and the concerted H approach-O removing reaction HO 2 ( 2A″)+H( 2S) → H 2O( 1A 1)+O( 3P) by using SDCI wavefunctions with a valence double-zeta plus polarization basis set. The saddle points are found to be of C s symmetry and the barrier heights are respectively 5.3 and 19.8 kcal by including size consistent correction. Moreoever kinetic parameters have been evaluated within the framework of the TST theory. So activation energies and the rate constants are estimated to be respectively 2.3 kcal and 0.4×10 9 ℓ mol −1 s −1 for the first reaction, 20.0 kcal and 5.4.10 −5 ℓ mol −1 s −1 for the second. Comparison of these results with experimental determinations shows that hydrogen abstraction on HO 2 is an efficient mechanism for the formation of H 2 + O 2, while the concerted mechanism envisaged for the formation of H 2O + O is highly unlikely. 相似文献
7.
The DANTE technique and NOESY two-dimensional method have been employed to observe the isomerization of the chiral cationic complex [Pd(η 3-CH 2CMeCH 2(P-P′)] + (1a), where P-P′ = the chiral chelating ligand ( S)( N-diphenylphosphino)(2-diphenylphosphinoxymethyl)pyrrolidine. The rate constant was found to be 0.5 s −1 in CHCl 3 at 295 K and 1.50 s −1 in the presence of added free ligand. In the latter case the epimerization proceeds by a π-σ-π mechanism via the intermediacy of a primary η 1-allylpalladium complex. Although the intermediate was not detected, the NMR findings reveal that it has the allylic terminus η 1-bonded to palladium. The structure of 1a in its PF 6− salt has been determined. The compound crystallizes in the orthorhombic space group P2 12 12 1 with a 10.029(4) b 19.203(8) c 36.115(6) Å, Z = 8, R = 0.0572 and Rw = 0.0712 for 3716 observed reflections with I > 3σ( I). 相似文献
8.
Nest-shaped cluster [MoOICu 3S 3(2,2′-bipy) 2] (1) was synthesized by the treatment of (NH 4) 2MoS 4, CuI, ( n-Bu) 4NI, and 2,2′-bipyridine (2,2′-bipy) through a solid-state reaction. It crystallizes in monoclinic space group P2 1/ n, a=9.591(2) Å, b=14.820(3) Å, c=17.951(4) Å, β=91.98(2)°, V=2549.9(10) Å 3, and Z=4. The nest-shaped cluster was obtained for the first time with a neutral skeleton containing 2,2′-bipy ligand. The non-linear optical (NLO) property of [MoOICu 3S 3(2,2′-bipy) 2] in DMF solution was measured by using a Z-scan technique with 15 ns and 532 nm laser pulses. The cluster has large third-order NLO absorption and the third-order NLO refraction, its 2 and n2 values were calculated as 6.2×10 −10 and −3.8×10 −17 m 2 W −1 in a 3.7×10 −4 M DMF solution. 相似文献
9.
Three spiro[pyrrolidine-2,3′-oxindoles], 1,1′,2,2′,5′,6′,7′,7′a-octahydro-2-oxo-1′-phenyl-spiro[3 H-indole-3,3′-[3 H]-pyrrolizine]-2′-carboxylic acid methyl ester (1), 1,1′,2,2′,5′,6′,7′,7′a-octahydro-2-oxo-1′-nitro-2′-phenyl-spiro[3 H-indole-3, 3′-[3 H]-pyrrolizine] (2) and 1,1′,2,2′,5′,6′,7′,7′a-octahydro-2-oxo-1′-nitro-2′-(4″-chlorophenyl)-spiro[3 H-indole-3,3′-[3H]-pyrrolizine] (3) have been synthesized and their 1H, 13C and 15N spectra assigned. The chemical shift assignments are based on Pulsed Field Gradient (PFG) Double Quantum Filter (DQF) 1H, 1H correlation spectroscopy (COSY), PFG 1H, 13C Heteronuclear Multiple Quantum Coherence (HMQC) and PFG 1H,X (X = 13C and 15N) Heteronuclear Multiple Bond Correlation (HMBC) experiments. The single crystal X-ray structures of 1–3 have been determined. Compounds 1 and 2 crystallized in monoclinic space group C2/ c and compound 3 in monoclinic space group P2 1/ c, respectively. Also the ESI-TOF MS data of 1–3 are given. 相似文献
10.
The chiral ligands, 4,4′-bis{(1 S,2 R,4 S)-(−)-bornyloxy}-2,2′-bipyridine, (1 S,2 R,4 S)-1, and 4,4′-bis{(1 R,2 S,4 R)-(+)-bornyloxy}-2,2′-bipyridine, (1 R,2 S,4 R)-1, have been prepared and characterized by spectroscopic techniques and, for (1 S,2 R,4 S)-1, by single crystal X-ray diffraction. Despite the use of enantiomerically pure ligands, the formation of the complexes [Fe((1 S,2 R,4 S)-1) 3] 2+, [Ru((1 S,2 R,4 S)-1) 3] 2+, [Ru((1 S,2 R,4 S)-1)(bpy) 2] 2+ and [Ru((1 R,2 S,4 R)-1)(bpy) 2] 2+ proceeds without preference for either the Δ or Λ-diastereoisomers. 相似文献
11.
本文研究了缺电子敏化剂9,10-二氰基蒽(DCA)对苄醇类化合物(二苯甲醇、苯甲醇)及甲苯类化合物(甲苯、对-二甲苯)的光敏化夺氢反应,证明上述两类反应是经由两种不同机制进行的。 相似文献
12.
The novel compounds [(η 6-p-cymene)RuCl(μ-RR-DTO N,N′Ru S,S′-Pt)Pt(RR-DTO)(P-N)Cl] (P-N = 2-diphenylphosphino-pyridine, RR-DTO = N,N′-dialkyl-dithioxamidato, R = benzyl, 1; R = (R)-(−)-2-hydroxypropyl (coming from (R)-(−)-2-hydroxypropyl-amine), 2;) exhibit a Pt---Ru chiral axis which is a new example of stereoisomerism in inorganic chemistry. The crystal structure of 2 is also reported. 相似文献
13.
The Schiff base compound, N- N′-bis(4-methoxybenzylidene)ethylenediamine (C 18H 20N 2O 2) has been synthesized and its crystal structure has been investigated by X-ray analysis and PM3 method. The compound crystallizes in monoclinic space group P2 1/ n with a=10.190(1), b=7.954(1), c=10.636(1) Å, β=111.68(1)°, V=801.1(1) Å 3, Z=2 and Dcal=1.229 Mgm −3. The title structure was solved by direct methods and refined to R=0.056 for 2414 reflections [ I>3.0σ( I)] by full-matrix anisotropic least-squares methods. The energy profile of the compound was calculated by PM3 method as a function of θ[N1′–C9′–C9–N1]. The most stable molecular structure of the title compound is the anti conformation, which is different in energy by 5.0 and 1.0 kcal mol −1 from the eclipsed conformation I and gauche conformations, (III and V), respectively. 相似文献
14.
The photophysics of three complexes of the form Ru(bpy) 3−(pypm) 2+ (where bpy2,2′-bipyridine, pypm 2-(2′-pyridyl)pyrimidine and P=1, 2 or 3) was examined in H 2O, propylene carbonate, CH 3CN and 4:1 (v/v) C 2H 5OH---CH 3OH; comparison was made with the well-known photophysical behavior of Ru(bpy) 32+. The lifetimes of the luminescent metal-to-ligand charge transfer (MLCT) excited states were determined as a function of temperature (between −103 and 90 °C, depending on the solvent), from which were extracted the rate constants for radiative and non-radiative decay and Δ E, the energy gap between the MLCT and metal-centered (MC) excited states. The results indicate that *Ru(bpy) 2(pypm) 2+ decays via a higher lying MLCT state, whereas *Ru(pypm) 32+ and *Ru(pypm) 2(bpy) 2+ decay predominantly via the MC state. 相似文献
15.
Treatment of [Ru 2(CO) 4(MeCN) 6][BF 4] 2 or [Ru 2(CO) 4(μ-O 2CMe) 2(MeCN) 2] with uni-negative 1,1-dithiolate anions via potassium dimethyldithiocarbamate, sodium diethyldithiocarbamate, potassium tert-butylthioxanthate, and ammonium O, O′-diethylthiophosphate gives both monomeric and dimeric products of cis-[Ru(CO) 2(η 2-(SS)) 2] ((SS) −=Me 2NCS 2− (1), Et 2NCS 2− (2), tBuSCS 2− (3), (EtO) 2PS 2− (4)) and [Ru(CO)(η 2-(Me 2NCS 2))(μ,η 2-Me 2NCS 2)] 2 (5). The lightly stabilized MeCN ligands of [Ru 2(CO) 4(MeCN) 6][BF 4] 2 are replaced more readily than the bound acetate ligands of [Ru 2(CO) 4(μ-O 2CMe) 2(MeCN) 2] by thiolates to produce cis-[Ru(CO) 2(η 2-(SS)) 2] with less selectivity. Structures 1 and 5 were determined by X-ray crystallography. Although the two chelating dithiolates are cis to each other in 1, the dithiolates are trans to each other in each of the {Ru(CO)(η 2-Me 2NCS 2) 2} fragment of 5. The dimeric product 5 can be prepared alternatively from the decarbonylation reaction of 1 with a suitable amount of Me 3NO in MeCN. However, the dimer [Ru(CO)(η 2-Et 2NCS 2)(μ,η 2-Et 2NCS 2)] 2 (6), prepared from the reaction of 2 with Me 3NO, has a structure different from 5. The spectral data of 6 probably indicate that the two chelating dithiolates are cis to each other in one {Ru(CO)(η 2-Et 2NCS 2) 2}fragment but trans in the other. Both 5 and 6 react readily at ambient temperature with benzyl isocyanide to yield cis-[Ru(CO)(CNCH 2Ph)(η 2-(SS)) 2] ((SS)=Me 2NCS 2− (7) and Et 2NCS 2− (8)). A dimerization pathway for cis-[Ru(CO) 2(η 2-(SS)) 2] via decabonylation and isomerization is proposed. 相似文献
16.
在水热体系中合成了3个中心金属为镍离子, 以六配位扭曲八面体构型形成的具有螺旋结构的配位聚合物{[Ni 2L 2(bib) 2·2H 2O]·5H 2O} n(1), [Ni 2L 2(bpy)] n(2)和{[Ni 2L 2(bibpip) 2·2H 2O]·6H 2O} n(3)[H 2L=4,4'-三苯胺二甲酸; bib=1,3-二(咪唑基)苯; bpy=4,4-联吡啶; bibpip=1,4-二(4-咪唑苄基)哌嗪]. 通过单晶及粉末X射线衍射、 红外光谱、 元素分析和热重分析对这3种化合物进行了表征. 结果表明, 化合物1属于单斜晶系, C2 /c空间群, 其骨架为具有{4 2·6 5·8}拓扑结构的二维层结构; 化合物2属于斜方晶系, Fdd2空间群, 其骨架为具有{4 8·5 4·6 3}拓扑结构的三维超分子网络; 化合物3属于三斜晶系, P空间群, 为1个五重穿插的三维超分子网络, 其骨架具有{4 4·6 2}拓扑结构. 相似文献
17.
The neutral nitrogen-bidentate ligand, diphenylbis(3,5-dimethylpyrazol-1-yl)methane, Ph 2CPz′ 2, can readily be obtained by the reaction of Ph 2CCl 2 with excess HPz′ in a mixed-solvent system of toluene and triethylamine. It reacts with [Mo(CO) 6] in 1,2-dimethoxyethane to give the η 2-arene complex, [Mo(Ph 2CPz′ 2)(CO) 3] (1). This η 2-ligation appears to stabilize the coordination of Ph 2CPz′ 2 in forming [Mo(Ph 2CPz′ 2)(CO) 2(N 2C 6H 4NO 2- p)][BPh 4] (2) and [Mo(Ph 2CPz′ 2)(CO) 2(N 2Ph)] [BF 4] (3) from the reaction of 1 with the appropriate diazonium salt but the stabilization seems not strong enough when [Mo{P(OMe) 3} 3(CO) 3] is formed from the reaction of 1 with P(OMe) 3. The solid-state structures of 1 and 3 have been determined by X-ray crystallography: 1-CH 2Cl 2, monoclinic, P2 1/ n, a = 11.814(3), b = 11.7929(12), c = 19.46 0(6) Å, β = 95.605(24)°, V = 2698.2(11) Å 3, Z = 4, Dcalc = 1.530 g/cm 3 , R = 0.044, Rw = 0.036 based on 3218 reflections with I > 2σ( I); 2 (3)-1/2 hexane-1/2 CH 3OH-1/2 H 2O-1 CH 2Cl 2, monoclinic, C2/ c, a = 41.766(10), b = 20.518(4), c = 16.784(3) Å, β = 101.871(18)°, V = 14076(5) Å 3, Z = 8, Dcalc = 1.457 g/cm 3, R = 0.064, Rw = 0.059 based on 5865 reflections with I > 2σ( I). Two independent cations were found in the asymmetric unit of the crystals of 3. The average distance between the Mo and the two η 2-ligated carbon atoms is 2.574 Å in 1 and 2.581 and 2.608 Å in 3. The unfavourable disposition of the η 2-phenyl group with respect to the metal centre in 3 and the rigidity of the η 2-arene ligation excludes the possibility of any appreciable agostic C---H → Mo interaction. 相似文献
18.
The new chloro(cyclopentadienyl)silanes Cp′SiH yCl 3−y (Cp′=Me 4EtC 5, y=1: 1; Cp′=Me 4C 5H, y=1: 2; y=0: 3; Cp′=Me 3C 5H 2, y=1: 4 and pentachloro(cyclopentadienyl)disilanes Cp′Si 2Cl 5 (Cp′=Me 5C 5 5, Me 4EtC 5 6, Me 4C 5H 7, Me 3C 5H 2 8, Me 3SiC 5H 4 9) are synthesized in good yields via metathesis reactions. Treatment of 1–9 with LiAlH 4 leads under Cl–H exchange to the hydridosilyl compounds Cp′SiH 3 (Cp′=Me 4EtC 5 10, Me 4C 5H 11, Me 3C 5H 2 12) and to the hydridodisilanyl compounds Cp′Si 2H 5 (Cp′=Me 5C 5 13, Me 4EtC 5 14, Me 4C 5H 15, Me 3C 5H 2 16, Me 3SiC 5H 4 17). Complexes 1–17 are characterized by 1H, 13C, and 29Si-NMR spectroscopy, IR spectroscopy, mass spectrometry and CH-analysis. The structures of 6, 7 and 9 are determined by single-crystal X-ray diffraction analysis. Pyrolysis studies of the cyclopentadienylsilanes 10–12 and disilanes 13–17 show their suitability as precursors in the MOCVD process. 相似文献
19.
A series of Cu(II) complexes of disubstituted 2,2′-bipyridine bearing ammonium groups [Cu(L 1−4) 2Br] 5+ (1–4, L 1 = [5,5′-(Me 2NHCH 2) 2-bpy] 2+, L 2 = [5,5′-(Me 3NCH 2) 2-bpy] 2+, L 3 = [4,4′-(Me 2NHCH 2) 2-bpy] 2+, L 4 = [4,4′-(Me 3NCH 2) 2-bpy] 2+ and bpy = 2,2′-bipyridyl) were synthesized, of which complexes 1 and 4 were structurally characterized. Both coordination configurations of Cu(II) ions can be described as distorted trigonal bipyramid. The interaction between all complexes and CT-DNA was evaluated by thermal-denaturation experiments and CD spectroscopy. Results show that the complexes interact with CT-DNA via outside electrostatic interactions and their binding ability follows the order: 1 > 2 > 3 > 4. In the absence of any reducing agents, the cleavage of plasmid pBR322 DNA by these complexes was investigated and the hydrolysis kinetics of DNA was studied in Tris buffer (pH 7.5) at 37 °C. Obtained pseudo-Michaelis–Menten kinetic parameters: 15.0, 13.6, 2.01 and 1.69 h −1 for 1, 2, 3 and 4, respectively, indicate that complexes 1 and 2 exhibit very high DNA cleavage activities. According to their crystal data, the high nuclease activity may be attributed to the strong interaction of the metal moiety and two ammonium groups with phosphate groups of DNA. 相似文献
20.
Polarized absorption spectra of Ba(MnO 4) 2·3H 2O/Ba(ClO 4) 2·3H 2O mixed single crystals are reported at 4.2°K. Previous 1T 2 → 1A 1 assignments for the 5200 Å and 3000 Å absorption bands of MnO 4− are substantiated; further support is provided for the 1T 1 → 1A 1 assignment of the 3600 Å absorption band of MnO 4−. The site-splitting of the 5200 Å 1T 2 state is E( 1E)− E( 1A) ≈ −150 cm −1; that of the 3000 Å 1T 2 state is E( 1E)− E( 1A) ≈ 300 cm −1. A significant e vibronic intensity component is observed in the 5200 Å 1T 2 state. 相似文献
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