Picosecond spectroscopy and solvation clusters. The dynamics of localizing electrons in polar fluids

Kenney‐Wallace, Geraldine A.; Jonah, Charles D.

doi:10.1021/j100211a007

Cited by 163 publications

(122 citation statements)

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“…These are also important data for models of photoionization and electron transfer originating from high lying singlet states in pyrene in alcohols. The nature and lifetime of the ionizing state could well be important considerations in the interpretation of experiments which seek to measure the electron localization and solution time through the time-dependent appearance of e, absorption (32)(33)(34)(35). Clearly the pyrene photoionization step must be very efficient, and the lifetime of the ionizing state short, in order to complete effectively against ps vibronic relaxation.…”

Section: Organic Molecular Photophysics and Dynamicsmentioning

confidence: 99%

Subpicosecond laser spectroscopy: strong field effects on molecular photophysics and dynamics

Quitevis¹,

Kröger²,

Kalpouzos³

et al. 1983

Can. J. Chem.

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This prlper is cleciicateci to Professor-Harrj E. G~olrlirlg or1 the oc~cn.sior~ of his 65th birthcloy E. QUITEVIS, P. M. KROGER, C. KALPOUZOS, and G. A. KENNEY-WALLACE. Can. J . Chem. 61, 975 (1983).The possible role of strong field effects is discussed in the context of picosecond relaxation and reaction in polyatomic systems. The picosecond pulse diagnostics from an argon-ion synchronously pumped dye laser are then outlined in terms of cavity detuning and laser pumping parameters. A profile of auto-correlation data on ensemble-averaged pulses and streak camera data on single pulses is presented, from which the domain of stable, single pulse operation can be deduced. Finally data are presented on the photoionization and energy relaxation of pyrene in alcohols and micelles, and for the reorientational dynamics of liquid chlorobenzene, which illustrate different consequences of strong field phenomena in dense media.E. QUITEVIS, P. M. KROGER, C. KALPOUZOS et G. A. KENNEY-WALLACE. Can. J . Chem. 61, 975 (1983).On discute du r61e que pourrait jouer des effets de champ fort dans le contexte de relaxation et de reaction de I'ordre de la picoseconde dans des systitmes polyatomiques. On dCcrit une mCthode de diagnostique par impulsion de I'ordre de la picoseconde basCe sur un laser a colorant active d'une f a~o n synchrone par de l'argon, en fonction d'un dksajustement de la cavitC et des parametres de pompage du laser. On prCsente une courbe des donnees d7autocorrClation pour des impulsions ajustCes au niveau de l'ensemble des donnCes d'une camera "streak camera" relatives aux impulsions uniques; a partir de ces donnCes, on peut dCduire le domaine d'opiration stable d'un impulsion unique. Finalement on prtsente les donnCes sur la photoionisation et sur la relaxation d'Cnergie du pyrene dans des alcools et des micelles et sur la rkorientation dynamique du chlorobenzene liquide, qui illustrent les diffkrentes consCquences du phCnomkne de champ fort dans les milieux denses.[Traduit par le journal]

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Section: Organic Molecular Photophysics and Dynamicsmentioning

confidence: 99%

Subpicosecond laser spectroscopy: strong field effects on molecular photophysics and dynamics

Quitevis¹,

Kröger²,

Kalpouzos³

et al. 1983

Can. J. Chem.

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“…absorption spectra of such cluster-trapped electrons are almost identical to the spectra of "solvated electrons" in neat aliphatic alcohols [33].…”

Section: /12/04mentioning

confidence: 67%

Multimer Radical Ions and Electron/Hole Localization in Polyatomic Molecular Liquids: A Critical Review

Shkrob

Sauer

2004

ChemInform

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Abstract.While ionization of some polyatomic molecular liquids (such as water and aliphatic alcohols) yields so-called "solvated electrons" in which the excess electron density is localized in the interstices between the solvent molecules, most organic and inorganic liquids yield radical anions and cations in which the electron and spin densities reside on the solvent molecule or, more commonly, a group of such molecules. The resulting multimer ions have many unusual properties, such as high rates of diffusive hopping. The "solvated electron" can be regarded as a variant of a multimer radical anion in which the charge, while perturbing the solvent molecules, mainly resides in the space between these molecules. We give several examples of less known modes for electron localization in liquids that yield multimer radical anions (such as C 6 F 6 , benzene, acetonitrile, carbon disulfide and dioxide, etc.) and holes localization in liquids that yield multimer radical cations (such as cycloalkanes). Current understanding of the reaction properties for these high-mobility solvent radical anions and cations is discussed.

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“…Soulignons qu'une Cvolution similaire du spectre de e-,,, a aussi MC enregistree dans le cas du propanol-1 vitreux 2 77 Des etudes dans le domaine picoseconde par radiolyse pulsCe (22)(23)(24) et impulsions laser (24,25) ont ensuite Clargi le domaine de temperature et port6 sur une skrie d'alcools aliphatiques de C , h C,,. Ces expCriences ont pleinement confirm6 l'existence de e-,, precurseur de e-,,,,.…”

Section: B Dynamique Et Mkcanisme(s) De Solvatationunclassified

“…Ces expCriences ont pleinement confirm6 l'existence de e-,, precurseur de e-,,,,. Kenney-Wallace et Jonah (23,24) ont observt que 1'Cvolution cinCtique de l'absorbance h une longueur d'onde donnCe (entre 450 et 750 nm) montre en effet un signal rapide qui apparait dans le temps de rCsolution de l'appareil (<lo ps) et un signal lent (10-300 ps), indkpendant de la longueur d'onde, dCcrit par une exponentielle (figure 2).…”

Section: B Dynamique Et Mkcanisme(s) De Solvatationunclassified

Électrons en excès dans les milieux polaires homogènes et hétérogènes

Bernas¹,

Ferradini²,

Jay‐Gerin³

1996

Can. J. Chem.

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RCsumC : Une synthkse des connaissances actuelles concernant la solvatation des Clectrons en excks (e,,, + e-s,l,) produits par photoionisation ou par radiolyse dans les milieux polaires a Ct C tentee. Sont successivement envisagees les diverses propriCtCs de l'espece alors forrnCe : les rnCcanisrnes proposCs pour sa solvatation, sa structure, ses caractCristiques physico-chimiques. En dCpit de certaines analogies entre les anions halogenure solvatCs et e-,,,, celui-ci ne parait pas pouvoir en constituer le prototype. Le cornporternent de e; , , dans des systkmes hCtCrogknes modeles, tels que solutions micellaires et agrCgats molCculaires, est tgalement abordC et corrC1C aux rCsultats relatifs aux solutions homogenes.Mots c l b : electrons en excks, milieux polaires homogknes et hCtCrogenes, photoionisation, radiolyse, solvatation, transfert de charge au solvant, propriCtCs de I'Clectron solvatC, solutions micellaires, agrCgats moleculaires, comparaison avec la solvatation des anions.Abstract: A review of our present knowledge concerning the solvation of excess electrons (e-,,, + e-,,lv) produced by photoionization or radiolysis in polar media has been attempted. Various properties of the solvated electron (proposed solvation mechanisms, structure, physicochemical characteristics) are considered. In spite of some similarities, e-,,,, does not seem to be a good prototype for solvated halide anions. The behavior of e-,,, in heterogeneous model systems, such as micellar solutions and molecular clusters, is described and correlated with that observed in homogeneous media.

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Picosecond spectroscopy and solvation clusters. The dynamics of localizing electrons in polar fluids

Cited by 163 publications

References 8 publications

Subpicosecond laser spectroscopy: strong field effects on molecular photophysics and dynamics

Subpicosecond laser spectroscopy: strong field effects on molecular photophysics and dynamics

Multimer Radical Ions and Electron/Hole Localization in Polyatomic Molecular Liquids: A Critical Review

Électrons en excès dans les milieux polaires homogènes et hétérogènes

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