Isotope effect in the linewidth distribution of single-molecule spectra in doped toluene at 2K

Vainer, Yuri G.; Naumov, Andrei V.; Bauer, Markus; Kador, Lothar

doi:10.1016/j.jlumin.2007.02.026

Cited by 24 publications

(17 citation statements)

References 22 publications

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“…[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). It allows for continuous scanning of the light frequency over 30 GHz.…”

Section: Methodsmentioning

confidence: 99%

“…The internal heterogeneities in such solids often give rise to tunneling systems (two-level systems; TLSs) or quasi-localized low-frequency vibrational modes (LFMs), the coupling of which to single chromophores causes frequency jumps and/or thermal broadening of the absorption lines of the latter. [9,12,13] Light-induced spectral jumps or photo-bleaching at higher excitation intensities can also occur when the chromophores are not tightly embedded in a well-ordered crystal. As a consequence, only few polycrystalline systems have been reported to date which fulfill the requirements for applications in photonics, such as light sources providing single photons on demand.…”

Section: Introductionmentioning

confidence: 99%

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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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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

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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“…These observations have been related to the structural and/or dynamic disorder of the bulk host properties. [2,[25][26][27][28] In these studies, the sensitivity of the narrow zero-phonon line (ZPL) of the single fluorophore was used to probe the local nature of phonon-like and tunneling excitations in disordered solids. However, the physical nature of TLSs has not yet been totally clarified, and the complex dynamics cannot always be described properly with the TLS model.…”

Section: Introductionmentioning

confidence: 99%

Stable Single‐Molecule Lines of Terrylene in Polycrystalline para‐Dichlorobenzene at 1.5 K

et al. 2014

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The spectroscopic properties of single terrylene (Tr) molecules are studied in a polycrystalline matrix of para-dichlorobenzene (p-DCB) at 1.5 K. Samples grown in a glass capillary show a very strong site at 597 nm, which is redshifted by more than 700 cm(-1) from the observed transition energy for Tr in p-DCB prepared as a film on a coverslip (572 nm). Each of these two sites is characterized by measuring their single-molecule spectroscopic parameters at 1.5 K. Lifetime-limited linewidths of 45±5 MHz are found for both sites. Fluorescence detection rates reach 8×10(4) count s(-1) at saturation. The spectral trails of the majority of single molecules show no spectral jumps, indicating an absence of interacting two-level systems; however, the small distribution of linewidths may indicate weak interactions with low-frequency modes. Frequency jumps are observed for 10 % of the molecules. The complete emission spectra from two different single molecules at the center of each of the two sites is presented. Debye-Waller factors of αDW=0.33±0.05 for the normal site (572 nm) and αDW=0.30±0.05 for the red site (597 nm) are reported. This new host-guest system provides a quick and easy way to obtain lifetime-limited single-molecule lines.

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“…11 The excitation light source was a tunable single-mode dye laser COHERENT CR 599-21 operating with Rhodamine 6G in the spectral range 565 -625 nm. The actual diffusion depths may be 1 -2 nm larger, since the diffusion coefficient in the first 1 -2 nm below a polymer surface is known to be higher than in the bulk, at least at the glass transition temperature (see, e.g., 7 ).…”

Section: Methodsmentioning

confidence: 99%

Fluorescence microscopy and spectroscopy of subsurface layer dynamics of polymers with nanometer resolution in the axial direction

et al. 2015

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We studied the dynamics in ultrathin subsurface layers of an amorphous polymer by the spectra of single fluorescent molecules embedded into the layer by vapor deposition and subsequent controlled diffusion to the desired depth in ≈0.5 nm steps. The spectral trails of single molecules were recorded at 4.5 K as a function of diffusion depth. In depths shallower than 20 nm, the spectral dynamics deviate from those deep in the bulk. Less than 5 nm deep, the linewidths increase rapidly, whereas the number of detected molecules decreases. No zero-phonon lines were observed closer than 0.5 nm to the polymer surface. Possible physical reasons of the observed phenomena are discussed.

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Isotope effect in the linewidth distribution of single-molecule spectra in doped toluene at 2K

Cited by 24 publications

References 22 publications

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

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

Stable Single‐Molecule Lines of Terrylene in Polycrystalline para‐Dichlorobenzene at 1.5 K

Fluorescence microscopy and spectroscopy of subsurface layer dynamics of polymers with nanometer resolution in the axial direction

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