Publisher’s Note: “Low temperature single molecule spectroscopy using vibronic excitation and dispersed fluorescence detection” [J. Chem. Phys. <b>118</b>, 10821 (2003)]

Kiraz, Alper; Ehrl, M.; Bräuchle, Christoph; Zumbusch, Andreas

doi:10.1063/1.1982791

Cited by 27 publications

(48 citation statements)

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“…It is conceivable that the two states observed at 524 nm and 530 nm arise from one single chromophore, which undergoes reversible spectral switching as in the case of single dye molecules. [49,53] Alternatively, the two states could equally well correspond to two chromophore units, with almost equal properties, such as the PL linewidth and intensity. This case is conceivable if it is not the emitting unit that is di- rectly excited by the laser, but rather a higher energy state that leads to population of the emitting unit by rapid energy transfer.…”

Section: Spectral Diffusionmentioning

confidence: 98%

“…[15,20,[47][48][49][50][51][52] This is due to the fact that the nonresonant excitation required to observe the purely electronic transition in PL emission implies absorption within the vibronic progression, which for narrow band excitation turns out to be much weaker than absorption into the purely electronic state. [44,53] Additionally, narrow band excitation in emission spectroscopy dramatically enhances spectral diffusion, which leads to the molecule moving out of resonance with the exciting laser. This is in contrast to high-temperature measurements, where nonresonant excitation into the vibronic progression is much more efficient owing to an increased population of vibrational modes.…”

Section: Detecting Single Chromophores In Single Moleculesmentioning

confidence: 99%

“…Reports of nonresonant excitation of single molecules at low temperatures have only really started appearing over the past year, and are primarily founded on employing spectrally broader laser sources. [43,53,54] The MEH-PPV chromophore possesses a convoluted vibronic progression, and each feature is at least as wide as the purely electronic transition of~20 cm À1 . Although we cannot measure the absorption linewidth directly, this width can provide an upper estimate for the spectral width relevant to absorption.…”

Section: Detecting Single Chromophores In Single Moleculesmentioning

confidence: 99%

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Single Chromophore Spectroscopy of MEH‐PPV: Homing‐In on the Elementary Emissive Species in Conjugated Polymers

Schindler

Lupton

2005

ChemPhysChem

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Low-temperature, single-molecule spectroscopy can provide unparalleled access to the primary emissive species of conjugated polymers. We demonstrate this with the example of one of the most commonly studied polymers, poly(2-methoxy-5-(2'-ethylhexoxy)-1,4-phenylenevinylene), MEH-PPV, which is shown to exhibit sharp fluorescence signatures over one hundred times narrower than the ensemble. These unprecedented narrow emission features can be assigned to single chromophores on the polymer chain, which are selectively addressed by the narrow band excitation. As with organic dye systems, the emission from single chromophores is not static with time, but shows a substantial spectral fluctuation. We find that, for single chromophores, this spectral fluctuation always follows a universal Gaussian statistical distribution. High-resolution spectroscopy provides unique insight into low-energy vibrational modes in the polymer emission, which are generally inaccessible with conventional spectroscopic methods such as site-selective fluorescence or Raman spectroscopy. Interchromophoric coupling can also occur owing to the flexible nature of the polymer backbone. This leads to substantial spectral broadening and a loss of resolution in the vibronic progression. We observe reversible switching within one single molecule between narrow and broad emission, which directly correlates with a discrete switching in emission intensity. We conclude that one and the same single molecule can support aggregated and nonaggregated emission, that is, emission from isolated and aggregated chromophores in one single molecule, rather than the tendency for aggregate emission being intrinsic to the molecule.

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Section: Spectral Diffusionmentioning

confidence: 98%

Section: Detecting Single Chromophores In Single Moleculesmentioning

confidence: 99%

Section: Detecting Single Chromophores In Single Moleculesmentioning

confidence: 99%

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Single Chromophore Spectroscopy of MEH‐PPV: Homing‐In on the Elementary Emissive Species in Conjugated Polymers

Schindler

Lupton

2005

ChemPhysChem

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“…[14][15][16][17] Orientational dynamics, on the other hand, can be studied by modulating the excitation polarization [18][19][20] or by analyzing the emission polarization. [18,21] Furthermore, spectral dynamics of single molecules reflect the energetic interactions of the fluorophore with its direct environment and can be detected at cryogenic temperatures [22][23][24] as well as at room temperature. [25,26] Moreover, by simultaneously applying different SMS techniques, one can investigate different properties, like the position, orientation, and emission spectrum of an individual molecule in the host matrix.…”

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confidence: 99%

Single‐Molecule Traffic in Mesoporous Materials: Translational, Orientational, and Spectral Dynamics

et al. 2007

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“…We have previously shown in a separate experiment using vibronic excitation and a high-finesse Fabry-Perot interferometer that the ZPL emission linewidth of TDI in HD indeed reaches nearly lifetime-limited values of 65 MHz. [11,12] The common scanning of the excitation laser line is superior for the resolution of small spectral jumps in crystalline systems. However, only vibronic excitation can reveal wide spectral jumps of the ZPL in a crystalline sample as depicted in Figure 2 a.…”

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confidence: 99%

Vibronic Excitation of Single Molecules: A New Technique for Studing Low‐Temperature Dynamics

et al. 2005

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Herein, we present vibronic excitation and detection of purely electronic zero-phonon lines (ZPL) of single molecules as a new tool for investigating dynamics at cryogenic temperatures. Applications of this technique to study crystalline and amorphous matrix materials are presented. In the crystalline environment, spectrally stable ZPLs are observed at moderate excitation powers. By contrast, investigations at higher excitation intensities reveal the opening of local degrees of freedom and spectral jumps, which we interpret as the observation of elementary steps in the melting of a crystal. We compare these results to spectral single-molecule trajectories recorded in a polymer. The way in which much more complicated spectral features can be analysed is shown. Surprisingly, pronounced spectral shifts on a previously not accessible large energy scale are observed, which are hard to reconcile with the standard two-level model system used to describe low-temperature dynamics in disordered systems.

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Publisher’s Note: “Low temperature single molecule spectroscopy using vibronic excitation and dispersed fluorescence detection” [J. Chem. Phys. 118, 10821 (2003)]

Cited by 27 publications

References 0 publications

Single Chromophore Spectroscopy of MEH‐PPV: Homing‐In on the Elementary Emissive Species in Conjugated Polymers

Single Chromophore Spectroscopy of MEH‐PPV: Homing‐In on the Elementary Emissive Species in Conjugated Polymers

Single‐Molecule Traffic in Mesoporous Materials: Translational, Orientational, and Spectral Dynamics

Vibronic Excitation of Single Molecules: A New Technique for Studing Low‐Temperature Dynamics

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