Luc jacquet - Academia.edu (original) (raw)
Papers by Luc jacquet
Journal of Inclusion Phenomena and Macrocyclic Chemistry, 1993
A new series of tetrapyrazolic macrocycles with a functionalized sidearm has been prepared. Their... more A new series of tetrapyrazolic macrocycles with a functionalized sidearm has been prepared. Their capability to transport Li+ salts of carboxylic acids has been examined and is shown to be strongly dependent on the functionality of the macrocycle sidearm. In the case of the Li+ (D, L.)-mandelate, chiral recognition has been observed.
Inorganic Chemistry, 1990
Page 1. Inorg. Chem. 1990, 29, 855-860 855 Contribution from the Service de Chimie Organique, CP ... more Page 1. Inorg. Chem. 1990, 29, 855-860 855 Contribution from the Service de Chimie Organique, CP 160, Universitd Libre de Bruxelles, 50 Av. F.-D. Roosevelt, B-1050 Brussels, Belgium ... Chem. Reo. 1988, 84, 85. Cook, M. J.; Thomson, AJ Chem. Br. 1984, 914. ...
Laser Chemistry, 1999
Transient resonance Raman (TR2) spectroscopy has been used to investigate the metalligand charge-... more Transient resonance Raman (TR2) spectroscopy has been used to investigate the metalligand charge-transfer (MLCT) excited states ofRu(II) polypyridyl complexes in DNA and in homogeneous solution. In DNA, complexes of the type [Ru(L)2(L')] 2+ were studied, where L 2, 2'-bipyridyl (bpy), 1,4, 5, 8-tetraazaphenanthrene (tap), and L' dipyrido [3,2:a-U,3:c]-phenazine (dppz) or 1,4,5,8,9,12-hexaazatriphenylene (HAT). For [Ru(bpy)2(HAT)]+, the enhancement pattern of vibrational modes in the TR spectra attributable to reduced HAT-in the triplet MLCT state suggest perturbations to the intraligand transition of HATin the presence of DNA. Transient RR spectra for [Ru(tap)2(dppz)] 2+ are indicative of formation of the species Run(tap-)(tap)(dppz) by electron transfer from DNA to the triplet MLCT state of the complex.
Journal of Molecular Structure, 2001
Nanosecond transient resonance Raman and picosecond transient absorption spectroscopic investigat... more Nanosecond transient resonance Raman and picosecond transient absorption spectroscopic investigations of the two structurally analogous Ru-polypyridyl complexes, Ruphen 2 dppz 21 (1) and Rutap 2 dppz 21 (2), are presented (phen 1,10phenanthroline, dppz dipyrido [3,2-a:2 0 ,3 0 -c] phenazine; tap 1,4,5,8 tetraazaphenanthrene). The ®ndings offer insight into the differing nature of the lowest excited states of the two complexes, and describe the role of these states within the very distinct photophysical behaviour of each, both in relation to solvent response and their interaction with DNA (facilitated in each case through the intercalating dppz ligand). The active, solvent-sensitive, dppz-based 3 MLCT states involved in the`lightswitch' behaviour of (1) are probed, alongside evidence of a progression through a precursor transient state when the complex is in non-aqueous environment. Evidence has been provided of a photophysical pathway for (2), involving formation of a tapbased lowest 3 MLCT state. When (2) is bound to DNA through the dppz ligand, a photo-driven electron transfer process ensues between the guanine base of DNA and the lowest 3 MLCT state. q
Journal of The Chemical Society, Chemical Communications, 1995
ABSTRACT
Chemical Communications, 1996
Resonance Raman (RR) spectroscopy has been used to probe the interaction between dipyridophenazin... more Resonance Raman (RR) spectroscopy has been used to probe the interaction between dipyridophenazine (dppz) complexes of ruthenium(II), [Ru(L) 2 (dppz)] 2+ (L = 1,10-phenanthroline (1) and 2,2-bipyridyl (2)), and calf-thymus DNA. Ground ...
Journal of The American Chemical Society, 1997
... Luc Jacquet, R. Jeremy H. Davies,* Andrée Kirsch-De Mesmaeker, and John M. Kelly* . Co... more ... Luc Jacquet, R. Jeremy H. Davies,* Andrée Kirsch-De Mesmaeker, and John M. Kelly* . Contribution fromthe School ... Kirsch-De Mesmaeker, A.; Lecomte, J.-P.; Kelly, JM Top. Curr. Chem. 1996, 177, 25−76. (11) Norden, B ...
Journal of Physical Chemistry B, 1998
Resonance Raman (rR) spectroscopy was utilized to gain insight into the electronic structure of d... more Resonance Raman (rR) spectroscopy was utilized to gain insight into the electronic structure of dppz (dppz ) dipyrido[3,2-a:2′,3′-c]phenazine) complexes of Ru(II) and Os(II). The time-resolved resonance Raman (TR 3 ) spectrum of Ru(phen) 2 (dppz) 2+ (phen ) 1,10-phenanthroline) collected under 355 nm (fwhm ≈ 10 ns) excitation is consistent with the population of a ligand-centered (LC) 3 ππ* state of the dppz ligand. Since emission from the Ru(II) f (dppz) metal-to-ligand charge transfer (MLCT) excited state is observed, both states must possess similar energies. Lowering of the MLCT state energy in Ru(phen) 2 (F 2 -dppz) 2+ and Os(phen) 2 (dppz) 2+ with respect to that of the 3 ππ* state results in the disappearance of the LC 3 ππ* excitedstate peaks in the rR spectrum, indicative of its fast deactivation to the lower MLCT state in these complexes. Addition of DNA to the samples containing Ru(phen) 2 (dppz) 2+ and Ru(phen) 2 (F 2 -dppz) 2+ leads to a decrease in intensity of the peaks associated with the intercalating phenazine part of the dppz ligand. Further increase in the DNA:Ru ratio causes broadening of the spectrum. This broadening has been interpreted in terms of strong ππ interaction between the intercalated dppz ligand and the DNA bases.
Inorganic Chemistry, 1992
FAB (fast atom bombardment) mass spectrometry is shown to be a valuable technique for characteriz... more FAB (fast atom bombardment) mass spectrometry is shown to be a valuable technique for characterizing polymetallic complexes, when other methods, such as NMR spectroscopy, are not helpful due to the complexity of the NMR spectra. The studied complexes are based on the bridging ligand 1,4,5,8,9,12-hexaazatriphenylene which presents three symmetrically arranged chelating sites and allows the preparation of polymetallic homo-and heteronuclear complexes of Ru(1I) and Rh(II1). The major ionization mechanism under FAB conditions is shown to be a first loss of one negatively charged counterion, followed by the successive losses of other counterions, either as uncharged radicals or as negatively charged ions accompanied, in the latter case, by a one-electron reduction from the matrix; both ionization mechanisms lead to singly charged ions. Minor doubly and triply charged species are also observed, corresponding to the loss of a second and third negatively charged counterion without subsequent reduction by the matrix. Finally fragmentations of the complexes occur as demonstrated by the detection of metal-ligand moieties.
Journal of Photochemistry and Photobiology A-chemistry, 1996
Pure and Applied Chemistry, 1997
The quenching of the luminescence of Ru(TAP)++, Ru(HAT)z(bpyp+ (TAP = 1,4,5$-tetraazaphenanthrene... more The quenching of the luminescence of Ru(TAP)++, Ru(HAT)z(bpyp+ (TAP = 1,4,5$-tetraazaphenanthrene; HAT = 1,4,5,8,9,12-hexaazatphenylene; bpy = 2,2'bipyridyl) and related oxidising complexes by DNA, polynucleotides, and purine nucleotides occurs by reductive electron transfer. Laser flash photolysis provides evidence for the formation of the reduced metal complex and the deprotonated nucleotide radical cation. This photo-oxidation leads to DNA strand-breaks and to the formation of covalent adducts with GMP or DNA. The adducts with RU(TAP)~~+ or Ru(HAT),(bpy)2+ are formed via a covalent bond between the C atom p to the coordinating N in the TAP or HAT ligand and the N2 of guanine.
Inorganic Chemistry, 1989
... In Figure 7, the observed rate constants log kobs of electron transfer from various ferrocene... more ... In Figure 7, the observed rate constants log kobs of electron transfer from various ferrocene derivatives to CO(TIM)~+ in the presence of O2 ... A. Kirsch-De Mesmaeker,*,t*t L. Jacquet,+ A. Masschelein,ts F. Vanhecke," and K. Heremad Received December 6, 1988 The resonance ...
Journal of The Chemical Society, Faraday Transactions, 1992
Journal of Inclusion Phenomena and Macrocyclic Chemistry, 1993
A new series of tetrapyrazolic macrocycles with a functionalized sidearm has been prepared. Their... more A new series of tetrapyrazolic macrocycles with a functionalized sidearm has been prepared. Their capability to transport Li+ salts of carboxylic acids has been examined and is shown to be strongly dependent on the functionality of the macrocycle sidearm. In the case of the Li+ (D, L.)-mandelate, chiral recognition has been observed.
Inorganic Chemistry, 1990
Page 1. Inorg. Chem. 1990, 29, 855-860 855 Contribution from the Service de Chimie Organique, CP ... more Page 1. Inorg. Chem. 1990, 29, 855-860 855 Contribution from the Service de Chimie Organique, CP 160, Universitd Libre de Bruxelles, 50 Av. F.-D. Roosevelt, B-1050 Brussels, Belgium ... Chem. Reo. 1988, 84, 85. Cook, M. J.; Thomson, AJ Chem. Br. 1984, 914. ...
Laser Chemistry, 1999
Transient resonance Raman (TR2) spectroscopy has been used to investigate the metalligand charge-... more Transient resonance Raman (TR2) spectroscopy has been used to investigate the metalligand charge-transfer (MLCT) excited states ofRu(II) polypyridyl complexes in DNA and in homogeneous solution. In DNA, complexes of the type [Ru(L)2(L')] 2+ were studied, where L 2, 2'-bipyridyl (bpy), 1,4, 5, 8-tetraazaphenanthrene (tap), and L' dipyrido [3,2:a-U,3:c]-phenazine (dppz) or 1,4,5,8,9,12-hexaazatriphenylene (HAT). For [Ru(bpy)2(HAT)]+, the enhancement pattern of vibrational modes in the TR spectra attributable to reduced HAT-in the triplet MLCT state suggest perturbations to the intraligand transition of HATin the presence of DNA. Transient RR spectra for [Ru(tap)2(dppz)] 2+ are indicative of formation of the species Run(tap-)(tap)(dppz) by electron transfer from DNA to the triplet MLCT state of the complex.
Journal of Molecular Structure, 2001
Nanosecond transient resonance Raman and picosecond transient absorption spectroscopic investigat... more Nanosecond transient resonance Raman and picosecond transient absorption spectroscopic investigations of the two structurally analogous Ru-polypyridyl complexes, Ruphen 2 dppz 21 (1) and Rutap 2 dppz 21 (2), are presented (phen 1,10phenanthroline, dppz dipyrido [3,2-a:2 0 ,3 0 -c] phenazine; tap 1,4,5,8 tetraazaphenanthrene). The ®ndings offer insight into the differing nature of the lowest excited states of the two complexes, and describe the role of these states within the very distinct photophysical behaviour of each, both in relation to solvent response and their interaction with DNA (facilitated in each case through the intercalating dppz ligand). The active, solvent-sensitive, dppz-based 3 MLCT states involved in the`lightswitch' behaviour of (1) are probed, alongside evidence of a progression through a precursor transient state when the complex is in non-aqueous environment. Evidence has been provided of a photophysical pathway for (2), involving formation of a tapbased lowest 3 MLCT state. When (2) is bound to DNA through the dppz ligand, a photo-driven electron transfer process ensues between the guanine base of DNA and the lowest 3 MLCT state. q
Journal of The Chemical Society, Chemical Communications, 1995
ABSTRACT
Chemical Communications, 1996
Resonance Raman (RR) spectroscopy has been used to probe the interaction between dipyridophenazin... more Resonance Raman (RR) spectroscopy has been used to probe the interaction between dipyridophenazine (dppz) complexes of ruthenium(II), [Ru(L) 2 (dppz)] 2+ (L = 1,10-phenanthroline (1) and 2,2-bipyridyl (2)), and calf-thymus DNA. Ground ...
Journal of The American Chemical Society, 1997
... Luc Jacquet, R. Jeremy H. Davies,* Andrée Kirsch-De Mesmaeker, and John M. Kelly* . Co... more ... Luc Jacquet, R. Jeremy H. Davies,* Andrée Kirsch-De Mesmaeker, and John M. Kelly* . Contribution fromthe School ... Kirsch-De Mesmaeker, A.; Lecomte, J.-P.; Kelly, JM Top. Curr. Chem. 1996, 177, 25−76. (11) Norden, B ...
Journal of Physical Chemistry B, 1998
Resonance Raman (rR) spectroscopy was utilized to gain insight into the electronic structure of d... more Resonance Raman (rR) spectroscopy was utilized to gain insight into the electronic structure of dppz (dppz ) dipyrido[3,2-a:2′,3′-c]phenazine) complexes of Ru(II) and Os(II). The time-resolved resonance Raman (TR 3 ) spectrum of Ru(phen) 2 (dppz) 2+ (phen ) 1,10-phenanthroline) collected under 355 nm (fwhm ≈ 10 ns) excitation is consistent with the population of a ligand-centered (LC) 3 ππ* state of the dppz ligand. Since emission from the Ru(II) f (dppz) metal-to-ligand charge transfer (MLCT) excited state is observed, both states must possess similar energies. Lowering of the MLCT state energy in Ru(phen) 2 (F 2 -dppz) 2+ and Os(phen) 2 (dppz) 2+ with respect to that of the 3 ππ* state results in the disappearance of the LC 3 ππ* excitedstate peaks in the rR spectrum, indicative of its fast deactivation to the lower MLCT state in these complexes. Addition of DNA to the samples containing Ru(phen) 2 (dppz) 2+ and Ru(phen) 2 (F 2 -dppz) 2+ leads to a decrease in intensity of the peaks associated with the intercalating phenazine part of the dppz ligand. Further increase in the DNA:Ru ratio causes broadening of the spectrum. This broadening has been interpreted in terms of strong ππ interaction between the intercalated dppz ligand and the DNA bases.
Inorganic Chemistry, 1992
FAB (fast atom bombardment) mass spectrometry is shown to be a valuable technique for characteriz... more FAB (fast atom bombardment) mass spectrometry is shown to be a valuable technique for characterizing polymetallic complexes, when other methods, such as NMR spectroscopy, are not helpful due to the complexity of the NMR spectra. The studied complexes are based on the bridging ligand 1,4,5,8,9,12-hexaazatriphenylene which presents three symmetrically arranged chelating sites and allows the preparation of polymetallic homo-and heteronuclear complexes of Ru(1I) and Rh(II1). The major ionization mechanism under FAB conditions is shown to be a first loss of one negatively charged counterion, followed by the successive losses of other counterions, either as uncharged radicals or as negatively charged ions accompanied, in the latter case, by a one-electron reduction from the matrix; both ionization mechanisms lead to singly charged ions. Minor doubly and triply charged species are also observed, corresponding to the loss of a second and third negatively charged counterion without subsequent reduction by the matrix. Finally fragmentations of the complexes occur as demonstrated by the detection of metal-ligand moieties.
Journal of Photochemistry and Photobiology A-chemistry, 1996
Pure and Applied Chemistry, 1997
The quenching of the luminescence of Ru(TAP)++, Ru(HAT)z(bpyp+ (TAP = 1,4,5$-tetraazaphenanthrene... more The quenching of the luminescence of Ru(TAP)++, Ru(HAT)z(bpyp+ (TAP = 1,4,5$-tetraazaphenanthrene; HAT = 1,4,5,8,9,12-hexaazatphenylene; bpy = 2,2'bipyridyl) and related oxidising complexes by DNA, polynucleotides, and purine nucleotides occurs by reductive electron transfer. Laser flash photolysis provides evidence for the formation of the reduced metal complex and the deprotonated nucleotide radical cation. This photo-oxidation leads to DNA strand-breaks and to the formation of covalent adducts with GMP or DNA. The adducts with RU(TAP)~~+ or Ru(HAT),(bpy)2+ are formed via a covalent bond between the C atom p to the coordinating N in the TAP or HAT ligand and the N2 of guanine.
Inorganic Chemistry, 1989
... In Figure 7, the observed rate constants log kobs of electron transfer from various ferrocene... more ... In Figure 7, the observed rate constants log kobs of electron transfer from various ferrocene derivatives to CO(TIM)~+ in the presence of O2 ... A. Kirsch-De Mesmaeker,*,t*t L. Jacquet,+ A. Masschelein,ts F. Vanhecke," and K. Heremad Received December 6, 1988 The resonance ...
Journal of The Chemical Society, Faraday Transactions, 1992