Thermal broadening of optical homogeneous linewidths in organic glasses and polymers studied via photochemical hole-burning

Thijssen, H.P.H.; Berg, R. van den; Völker, S.

doi:10.1016/0009-2614(83)80011-6

Cited by 103 publications

(21 citation statements)

References 30 publications

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“…93, 95,102 In order to resolve this discrepancy, one phenomenologically introduces an ad hoc distribution of A that goes such as A µ , with µ a small fraction, typically around 0.3. 15,95,96,[124][125][126][127][128][129][130] This yields hole widths whose temperature dependence is dominated by a T 1+µ power law, in accord with experiment. Although the behavior of this distribution function at A f 0, where it goes to zero, is surely unrealistic, the main effect of this modification is to make the distribution rise slowly, rather than being a constant throughout most of the range of values of A.…”

Section: Two-level System and Sudden Jump Modelsmentioning

confidence: 53%

Theory of Single-Molecule Optical Line-Shape Distributions in Low-Temperature Glasses

1997

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We present a theoretical framework for analyzing the distribution of optical line shapes in low-temperature glasses, as measured by single-molecule spectroscopy. The theory is based on the standard tunneling twolevel system model of low-temperature glasses and on the stochastic sudden jump model for the two-level system dynamics. Within this framework we present an explicit formula for the line shape of a single molecule and employ Monte Carlo simulation techniques to calculate the distribution of single-molecule line shapes. We compare our calculated line-width distributions to those measured experimentally. We find that the twolevel system model captures the features of the experimental line-width distributions very well, although there are discrepancies for small line widths. We also discuss the relation of single-molecule line-shape distributions to more traditional "line shapes", as measured by hole-burning and photon echo spectroscopies. Using the results from our analysis of the single-molecule line-width distributions, with no adjustable parameters we can compare theoretical predictions with experiment for photon echo decay times and hole widths. In general, the agreement is good, providing further evidence that the standard tunneling model in glasses is basically correct. For two systems, however, theory and experiment do not agree quantitatively.

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Section: Two-level System and Sudden Jump Modelsmentioning

confidence: 53%

Theory of Single-Molecule Optical Line-Shape Distributions in Low-Temperature Glasses

1997

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“…Intramolecular photochemistry may be reversible [e.g. photoautomerism in free-base por phyrins (14,IS,(36)(37)(38)(39)(40)], or irreversible [e.g. photodissociation of dimethyl s-tetrazine (13) and s-tetrazine (35)].…”

Section: Mechanismsmentioning

confidence: 99%

“…The most common probing schemes are transmission spectroscopy (11,42,47,50,(59)(60)(61)(62)(63)(64)(65) and excitation spectroscopy (10,(13)(14)(15)40,48,56,58). In the latter, the spectrum is generally scanned with the same laser as used for burning, but at 10 -3_10 -1 of its original intensity.…”

Section: Techniquesmentioning

confidence: 99%

“…The fi rst molecule /' "" " :9 � investigated was free-base porphin (H2P), because of its well-known behavior in crystalline hosts. Hole-burning experiments between 1.2 and 4.2K (39,40,66), and later down to 0.3K (43,76,77) and up to 20K (76), were performed on the S I <-So 0-0 transition in a large variety of glasses and polymers. In strong contrast to the data reported by other groups, the following results were found: (a) narrow holes of about hundreds of MHz to a few GHz at T � 2K; (b) the value ofrhom = �rhole (at very low burning fl uences) did extrapolate to the fluorescence lifetime-limited value, ro � 10 MHz of H2P, when T � 0; (c) rhom -rO followed a TJ.3-temperature law, independent of the organic amorphous host used.…”

Section: Organic Molecules In Organic Glassesmentioning

confidence: 99%

“…In fact, many organic amorphous systems subsequently showed that rhomr 0 oc rJ.3, at least between 0.3 and 20K (76), independent of their hole burning mechanism (40,43,52,76). [See Figure 7 for an example for ionic dyes (43,76).]…”

Section: Organic Molecules In Organic Glassesmentioning

confidence: 99%

See 2 more Smart Citations

Hole-Burning Spectroscopy

Völker¹

1989

Annu. Rev. Phys. Chem.

225

103

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Photochemisches Lochbrennen und optische Relaxationsspektroskopie in Polymeren und Gläsern

1984

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Photochemisches Lochbrennen ist eine spezielle Art der Siittigungsspektroskopie im optischen Bereich, die vie1 Xhnlichkeit rnit NMR-Methoden zur Bestimmung von Relaxationszeiten hat. Die Lochergenauer gesagt Einkerbungenbrennt man (mit Laserlicht) in Absorptionsbanden von Farbstoffmolekiilen, die in einem Polymer oder Glas in Spuren enthalten sind. Aufgrund ihrer Linienscharfe sind photochemisch erzeugte Lacher hochempfindliche Sensoren. Sie reagieren auf geringfiigige Storungen des Systems durch auDere Parameter mit meDbaren Verschiebungen oder Verbreiterungen. Anwendungen des photochemischen Lochbrennens in der Spektroskopie von Biomolekiilen und im Bereich der Datenspeicherung zeigen in mogliche Richtungen fur zukiinftige Entwicklungen.

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Thermal broadening of optical homogeneous linewidths in organic glasses and polymers studied via photochemical hole-burning

Cited by 103 publications

References 30 publications

Theory of Single-Molecule Optical Line-Shape Distributions in Low-Temperature Glasses

Theory of Single-Molecule Optical Line-Shape Distributions in Low-Temperature Glasses

Hole-Burning Spectroscopy

Photochemisches Lochbrennen und optische Relaxationsspektroskopie in Polymeren und Gläsern

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