Theory of time-resolved resonance scattering

Berg, Jacqueline O.; Langhoff, C. A.; Robinson, G. W.

doi:10.1016/0009-2614(74)85112-2

Cited by 83 publications

(9 citation statements)

References 8 publications

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“…A more general relationship between line shape and 'lifetime' has recently been discussed by a number of authors (Friedman and Hochstrasser 1974a;Mukamel and Jortner 1975;Nitzan, A., 1974, private communication;Berg et al 1974) where o is the angular frequency, i.e. a reduced energy variable in units of h, and where the lifetime is determined by the time dependence of Pl(t), the probability that at time t the system is in the state 1 prepared by a light source whose output characteristics are defined by the amplitude function When the amplitude functions S(t) and S(o) conform to [3], the output of the excitation source will be said to be transform limited APE -LIFETIME RELATIONSHIP 2069 (Bradley and New 19742 ;von der Linde 19723) with intensity functions I(t) = IS(t)12 and f(o) = IS(o)12 in the time and frequency domains re~pectively.~ It is easily established that it is immaterial whether total energy is obtained by integration over the entire intensity function in the time domain or in the frequency d~m a i n .~ 111.…”

Section: The Line Shape -Lifetime Relationshipmentioning

confidence: 95%

Line Shape – Lifetime Relationship and Emission and Scattering of Light by Polyatomic Molecules

Robinson¹,

Berg²

1975

Can. J. Phys.

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A unified theory of ordinary Rayleigh scattering, Raman scattering, and the absorption and reemission of light is presented and discussed from an experimental spectroscopist's point of view. Application to polyatomic molecules presents unique problems which are discussed. The theory should be able to account for experimental results off, near, and on resonance, using weak exciting light sources of various band shapes. The evolution of the Franck-Condon envelope on nearing the resonance region is described, and time dependent aspects of the interaction are treated in a general way. The theory in its present form cannot be used when the light source is so intense that population inversion, multiphoton effects, and stimulated processes take place.Une thkorie unifiee de ladiffusion Rayleigh ordinaire, de la diffusion Raman, et de l'absorption et reemission de lurnikre est presentke et discutke d'un point de vue de spectroscopie expkrimentale. L'application aux molCcules polyatomiques presente des problemes specifiques qui sont discutks. La theorie doit itre capable de rendre compte des resultats expkrimentaux loin de, prks de, et a la resonance, en utilisant des sources lumineuses excitatrices faibles de diverses distributions spectrales. L'tvolution de I'enveloppe de Franck-Condon en approchant de la regionde resonance est dCcrite, et les aspects des interactions, dependant du temps sont trait& de maniere genkrale. La thkorie presente ne peut pas Stre utilisee quand la source lumineuse est d'une intensite telle que surviennent: I'inversion de population, les effets a plusieurs photons, et des processus stimulks.[Traduit par le journal]Can. J. Phys., 53,2068 (1975)

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Section: The Line Shape -Lifetime Relationshipmentioning

confidence: 95%

Line Shape – Lifetime Relationship and Emission and Scattering of Light by Polyatomic Molecules

Robinson¹,

Berg²

1975

Can. J. Phys.

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“…При удалении от резонанса появляется НРС с малой длительностью ~τ имп амплитуда которого падает с увеличением отстройки, но «эффективность» (т. е. специально определенный квантовый выход) возрастает, и кинетика свечения в целом может выглядеть биэкспоненциальной. Численные расчеты [84][85][86] показывают, что при больших отстрой-ках и Δω ког амплитуда НРС достаточно велика для выделения быстрой компоненты на фоне медленной.…”

Section: 4unclassified

Nonexponential fluorescence decay of polyatomic molecules

Medvedev¹

1991

Usp. Fiz. Nauk

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“…Time It is well known that there exists a time delay between the time at which a laser pulse reaches its maximum intensity and the time at which the fluorescence intensity induced by the laser pulse has maximum intensity, which is related to such properties as the lifetime r of the excited state from which the fluorescence transition originates and the cross section of the absorption transition from ground to excited state (18,19). Thus, for equal absorption cross sections, one finds that the build up of fluorescence of a short-lived excited state occurs more rapidly than that of a longer-lived fluorescence process.…”

Section: Chl a In Benzene Solutionmentioning

confidence: 99%

Detection limitations of photomultiplier tubes in pulsed-laser emission spectroscopy: time-resolved fluorescence spectra of chlorophyll solutions

Wilton¹,

Haley²,

Koningstein³

1982

Can. J. Chem.

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. 60,2198 (1982). An experimental method is described for determination of the onset of saturation effects on the performance of photomultiplier tubes (PMTs) used in time-resolved pulsed-laser spectroscopy. Changes in the dark level response in time (on the 0-100 ns time scale) of the PMT were observed to indicate saturation of the tube. At low repetition rates conditions were found for which an RCA 8850 PMT and an RCA 7 102 PMT can be used to obtain reliable fluorescence decays on the 0-100 ns time scale while operating at high anode currents, without modification of interdynode voltages.Results for time-resolved fluorescence studies of Chl n in solution, in benzene and in pyridine, are discussed. The fluorescence decays at -680 nm indicate that several Chl a species are present in each solution. In pyridine, the main fluorescence process at 677 nm, characterised by a lifetime of -7 ns, is assigned as arising from ligated monomeric species of Chl n . A second longer-lived and weaker component (r = 75 ns) is assigned to the ligated monomeric species of Chl n '. A third, and even weaker process characterised by a lifetime r = 145 ns is also observed. The time-resolved fluorescence spectral band shape ofthis component has aunique narrow profile, and is assigned to a dimeric or more highly aggregated species of Chl n . The time-resolved measurements also indicate that another emission band occurs at 740 nm, and that this process has a lifetime 75 ns < r < 145 ns.A. DE WILTON, L. V. HALEY et J. A. KoNINGSTEIN. Can. J. Chem. 60, 2198Chem. 60, (1982. On dkcrit une m6thode experimentale pour determiner le debut des effets de saturation sur la performance des tubes photomultiplicateurs (TPM) utilises dans la spectroscopie laser a impulsion, a resolution en fonction du temps. On a observe des variations dans la reponse au niveau sombre dans le temps (dans 1'Cchelle de temps allant de 0 a 100 ns) du TMP indiquant ainsi la saturation du tube. A de faibles vitesses de repetition, on a trouve les conditions dans lesquelles on peut utiliser des tubes photomultiplicateurs RCA8850 et RCA7 102 pour obtenir des valeurs sures pour la desintegration de la fluorescence a des Cchelles de temps allant de 0 a 100 ns lorsqu'on opkre avec de forts courants anodiques sans modification des voltages interdynodes.On discute des resultats obtenus lors d'etudes de fluorescence, resolue en fonction du temps, du composi Chl n en solution dans le benzkne et dans la pyridine. Les desintegrations de la fluorescence ?I 680 nm indiquent que plusieurs espkces de Chl n sont presents dans chaque solution. Dans la pyridine, on attribue le mode principal de fluorescence a 677 nm, caractirise par un temps de vie d'environ 7 ns, a des espkces monomkres de Chl n reliees entre elles. On attribue une deuxikme composante plus faible et d'une duree de vie plus longue (r = 75 ns) 5 des espkces monomkres de Chl n ' reliees entre elles. On a Cgalement observe un troisieme processus qui est encore plus faible et qui est caracterisk par un temps de vie r = 145 ns. ...

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Theory of time-resolved resonance scattering

Cited by 83 publications

References 8 publications

Line Shape – Lifetime Relationship and Emission and Scattering of Light by Polyatomic Molecules

Line Shape – Lifetime Relationship and Emission and Scattering of Light by Polyatomic Molecules

Nonexponential fluorescence decay of polyatomic molecules

Detection limitations of photomultiplier tubes in pulsed-laser emission spectroscopy: time-resolved fluorescence spectra of chlorophyll solutions

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