Single molecule lines and spectral hole burning of terrylene in different matrices

Kozankiewicz, Β.; Bernard, J.; Orrit, Michel

doi:10.1063/1.467968

Cited by 131 publications

(117 citation statements)

References 33 publications

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“…In general, the spectral properties of each individual molecule vary from molecule to molecule due to differences in the local environments with which each SM is interacting [6,7,8,9,10,11,12,13,14,15,16]. With its unique ability to detect dynamical phenomena occurring at the level of an individual molecule surrounded by its local environment, SMS has uncovered the statistical distributions of microscopic quantities of the environment that are hidden in traditional ensemble averaged spectroscopy.…”

Section: Introductionmentioning

confidence: 99%

A Stochastic Theory of Single Molecule Spectroscopy

Jung

Barkai

Silbey

2002

Advances in Chemical Physics

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A theory is formulated for time dependent fluctuations of the spectrum of a single molecule in a dynamic environment. In particular, we investigate the photon counting statistics of a single molecule undergoing a spectral diffusion process. Based on the stochastic optical Bloch equation, fluctuations are characterized by Mandel's Q parameter yielding the variance of number of emitted photons and the second order intensity correlation function, g (2) (t). Using a semi-classical approach and linear response theory, we show that the Q parameter can be described by a three-time dipole correlation function. This approach generalizes the Wiener-Khintchine formula that gives the average number of fluorescent photons in terms of a one-time dipole correlation function. We classify the time ordering properties of the three-time dipole correlation function, and show that it can be represented by three different pulse shape functions similar to those used in the context of nonlinear spectroscopy. An exact solution is found for a single molecule whose absorption frequency undergoes a two state random telegraph process (i.e., the Kubo-Anderson sudden jump process.) Simple expressions are obtained from the exact solution in the slow and fast modulation regimes based on appropriate approximations for each case. In the slow modulation regime Q can be large even in the long time limit, while in the fast modulation regime it becomes small.

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Section: Introductionmentioning

confidence: 99%

A Stochastic Theory of Single Molecule Spectroscopy

Jung

Barkai

Silbey

2002

Advances in Chemical Physics

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“…Application of SMS has been found mostly in line-shape measurements. 7,8,[49][50][51] For example, line-width distributions of guest molecules embedded in a solid matrix (such as terrylene in polyethylene) have been measured at low temperatures. Nonlinear optical measurements, which are usually performed in bulk solids, are adopted for SMS.…”

Section: Introductionmentioning

confidence: 99%

Spin versus Boson Baths in Nonlinear Spectroscopy

1998

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The third-order optical response function of a chromophore coupled to a bath consisting of noninteracting two-level systems (TLSs) undergoing stochastic jumps is calculated. The results can be applied to a broad class of nonlinear optical techniques in single-molecule spectroscopy and bulk measurements in glasses, polymers, and mixed crystals. In the limit of many TLSs weakly coupled to the chromophore, the response can be obtained using the second-order cumulant expansion and resembles that of the Brownian oscillator model. Quantum corrections to the spectral density which accounts for the Stokes shift can be included in this limit using the fluctuation-dissipation theorem. However, the temperature dependence predicted by the two models is very different. Corrections to the cumulant expansion to fourth order in coupling strength are derived.

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“…For instance, the fluorescence excitation line widths of a large number of chromophores are distributed over an interval of up to 3 orders of magnitude. 78,79 The average fluorescence excitation line width is always larger than can be expected from 2PE experiments on the same samples. 7,8,80 The typical time scale of a single-molecule experiment is often taken to be the time it takes to scan the line width of a molecule, typically tens of seconds.…”

Section: Resultsmentioning

confidence: 80%

Ethanol Glass Dynamics: Logarithmic Line Broadening and Optically Induced Dephasing

Lazonder¹,

Duppen

Wiersma

2000

J. Phys. Chem. B

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The time and fluence dependence of the homogeneous line width of Zn-porphin in deuterated ethanol glass at 1.8 K is remeasured by stimulated photon echo. The observed spectral dynamics is interpreted in terms of the standard two-level system model and by using a commonly used modified version of it. It is shown, as was suggested recently (Phys. ReV. B 1997, 56, 11571), that time-dependent local heating is the cause of the plateau found in earlier echo experiments on this system. The anomalous intensity loss of the photon echo in the population dimension, however, is confirmed, as well as the existence of excess optical dephasing on a short time scale. The former effect is attributed to spontaneous frequency jumps outside the laser bandwidth, the latter to spectral diffusion induced by the change of electronic state of the chromophore. This phenomenon is not captured in existing theoretical models, which assume the probe molecule to be just a spectator of glass dynamics.

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Single molecule lines and spectral hole burning of terrylene in different matrices

Cited by 131 publications

References 33 publications

A Stochastic Theory of Single Molecule Spectroscopy

A Stochastic Theory of Single Molecule Spectroscopy

Spin versus Boson Baths in Nonlinear Spectroscopy

Ethanol Glass Dynamics: Logarithmic Line Broadening and Optically Induced Dephasing

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