2005
DOI: 10.1002/cphc.200400579
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Vibronic Excitation of Single Molecules: A New Technique for Studing Low‐Temperature Dynamics

Abstract: 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, whic… Show more

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Cited by 9 publications
(10 citation statements)
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References 21 publications
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“…This interpretation is consistent with low-temperature single-molecule studies on a low molecular weight dye (terrylenediimide) [71] as well as MEH-PPV, [43] both embedded in poly(methyl-methacrylate), where a broadening of their emission lines as a function of the integration time was demonstrated.…”
supporting
confidence: 84%
“…This interpretation is consistent with low-temperature single-molecule studies on a low molecular weight dye (terrylenediimide) [71] as well as MEH-PPV, [43] both embedded in poly(methyl-methacrylate), where a broadening of their emission lines as a function of the integration time was demonstrated.…”
supporting
confidence: 84%
“…In the subsequent discussion, much of the focus will be on spectrally dispersed luminescence detection following excitation by a single laser wavelength. This approach is only of limited applicability to single molecules in crystalline matrices as these materials tend to exhibit very narrow absorption lines and may randomly drift in and out of resonance with a narrow exciting‐laser line 72, 73. The elementary transitions in conjugated polymers appear to be broader, not least due to the presence of multiple coupled chromophores, so that reasonably constant molecular‐excitation densities and emission intensities can be reached as a function of time.…”
Section: Experimental Approachmentioning
confidence: 99%
“…A first analysis demonstrated that the magnitude of spectral jitter scales exponentially with polarization anisotropy, underlining how a small change in shape can have a large impact on the emission 59. Although this correlation between molecular rigidity and linewidth is known from studies of single dye molecules in different matrices,72, 73 it appears to be much more pronounced in conjugated polymers, where the polymer backbone effectively constitutes the matrix for the emissive chromophore 116…”
Section: Structure–property Relations From the Bottom Upmentioning
confidence: 99%
“…The spectrally narrow zero‐phonon line (ZPL) emission arising from the purely electronic radiative transition S 1, v =0 → S 0, v =0 of single dye molecules can be observed at liquid helium temperatures by exciting higher vibronic levels of the electronically excited molecular state using optical microscopy and spectroscopy (see, for example, refs. 16, 17). Even though the intensity and the spectral position of the ZPL emission were found to fluctuate on a timescale of seconds, this emission has been proven to be a proper source of indistinguishable photons having ultra‐long coherence times in the nanosecond regime 18.…”
Section: Resultsmentioning
confidence: 99%