Epifluorescence, confocal and total internal reflection microscopy for single‐molecule experiments: a quantitative comparison

We employ low-temperature single-molecule spectroscopy combined with pattern recognition techniques for data analysis on a methyl-substituted ladder-type poly(para-phenylene) (MeLPPP) to investigate the electron-phonon coupling to low-energy vibrational modes as well as the origin of the strong spectral diffusion processes observed for this conjugated polymer. The results indicate weak electron-phonon coupling to low-frequency vibrations of the surrounding matrix of the chromophores, and that low-energy intrachain vibrations of the conjugated backbone do not couple to the electronic transitions of MeLPPP at low temperatures. Furthermore, these findings suggest that the main line-broadening mechanism of the zero-phonon lines of MeLPPP is fast, unresolved spectral diffusion, which arises from conformational fluctuations of the side groups attached to the MeLPPP backbone as well as of the surrounding host material.

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“…A similar experimental setup as the one used in this study has been described in ref. [32] in more detail.…”

Section: Methodsmentioning

confidence: 98%

Single‐Molecule Spectroscopy on a Ladder‐Type Conjugated Polymer: Electron–Phonon Coupling and Spectral Diffusion

Hildner¹,

Winterling²,

Lemmer³

et al. 2009

ChemPhysChem

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“…Both setups have already been described in detail. [12,20] The first setup [20] is equipped with a CCD camera Andor DV887DCS-BV and a tunable singlemode ring dye laser (Coherent CR 699-21 Autoscan system) which allowed for recording the fluorescence excitation spectra of SMs across the whole absorption band (570 to 600 nm) with high-precision measurement (~5 MHz) of the absolute wavelength. The sample was kept at a temperature of 1.5 K. The second setup [12] has a tunable single-mode dye laser (Coherent CR599-21) operating with Rhodamine 6G in the spectral region between 565 and 585 nm (spectral bandwidth about 2 MHz including jitter).…”

Section: Methodsmentioning

confidence: 99%

Ortho‐Dichlorobenzene Doped with Terrylene—a Highly Photo‐Stable Single‐Molecule System Promising for Photonics Applications

et al. 2010

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The study of a new dye-matrix system-quickly frozen ortho-dichlorobenzene weakly doped with terrylene--via single-molecule (SM) spectroscopy is presented. The spectral and photo-physical properties, dynamics, and temperature broadening of SM spectra at low temperatures are discussed. The data reveal a broad inhomogeneous distribution, which indicates a high degree of matrix inhomogeneities, but at the same time, huge fluorescence emission rates and extraordinary SM spectral and photochemical stability with almost complete absence of blinking and bleaching. These unusual properties render the new system a promising candidate for applications in photonics, for example, for delivering single photons on demand.

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“…[58,59] The latter provides the most efficient suppression of the background as has been demonstrated by comparing the above mentioned techniques for exactly the same single molecule. [60] The intriguing feature of single-molecule spectroscopy is that it enables one to elucidate information that is commonly washed out by ensemble averaging. For example, it allows one to map out the (static) energetic disorder ΔE n .…”

Section: Unmasking Static Disorder By Single-molecule Spectrosopymentioning

confidence: 99%

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Brixner

Hildner

Köhler

et al. 2017

Advanced Energy Materials

302

301

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The transport of excitation energy in molecular aggregates is of crucial importance for the function of organic optoelectronic devices and next‐generation solar cells. First, this review summarizes the theoretical background of the nature of the electronically excited states of molecular aggregates. For these systems, the electronic interaction between the monomers leads to the formation of exciton states. This goes along with a shift of the excitation energies and a redistribution of the oscillator strength with respect to the monomers. Next, a brief overview is provided over experimental techniques that allow to study the properties of excitons in molecular aggregates. This includes single‐molecule spectroscopy, coherent two‐dimensional (2D) spectroscopy, and single‐molecule coherent spectroscopy. Finally, examples of molecular aggregates spanning the range from natural systems that act in photosynthesis as light‐harvesting antennas to artificial aggregates built from synthetic chromophores are illustrated.

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Epifluorescence, confocal and total internal reflection microscopy for single‐molecule experiments: a quantitative comparison

Cited by 34 publications

References 40 publications

Single‐Molecule Spectroscopy on a Ladder‐Type Conjugated Polymer: Electron–Phonon Coupling and Spectral Diffusion

Single‐Molecule Spectroscopy on a Ladder‐Type Conjugated Polymer: Electron–Phonon Coupling and Spectral Diffusion

Ortho‐Dichlorobenzene Doped with Terrylene—a Highly Photo‐Stable Single‐Molecule System Promising for Photonics Applications

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

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