Spectral Diffusion of Single Dibenzoterrylene Molecules in 2,3‐Dimethylanthracene

Abstract

We study single dibenzoterrylene molecules embedded in the dipolar disordered crystal 2,3-dimethylanthracene at 1.25 K. Broad linewidths (about 1 GHz, ∼30 times broader than in the anthracene crystal), high saturation excitation intensities (∼1000 times larger than in anthracene), as well as strong spectral diffusions are observed. Additionally, spectral jumping is studied by varying the excitation intensity and the temperature. We propose that the spectral diffusion and dynamic disorder in this system arise from the combination of a static disorder with slight reorientations of the methyl groups of the host molecules.

Spectroscopy of Single Dibenzoterrylene Molecules in para‐Dichlorobenzene

“…In the near‐infrared region, 7,8:15,16‐dibenzoterrylene (C 38 H 20 , DBT, see Figure ) was found to be a suitable fluorophore for low‐temperature single‐molecule spectroscopy . At low temperatures, single DBT molecules have been investigated in matrices of naphthalene, anthracene, and 2,3‐dimethylanthracene so far. These host–guest systems are typically prepared either by co‐sublimation of DBT and the respective matrix material or they are grown from a solution of DBT in the molten host‐matrix.…”

“…In the near-infrared region, 7,8:15,16-dibenzoterrylene (C 38 H 20 ,D BT,s ee Figure 1) was found to be as uitable fluoro-phore for low-temperature single-molecule spectroscopy. [9][10][11][12][13][14] At low temperatures,s ingle DBT moleculesh ave been investigated in matriceso fn aphthalene, [11] anthracene, [9,12,14] and 2,3dimethylanthracene [13] so far.T hese host-guest systems are typicallyp repared either by co-sublimation of DBT and the respectivem atrix material or they are grown from as olution of DBT in the molten host-matrix. In the case of co-sublimation the dimensions and shape of the resulting crystals are hardly controllable and the combination of these crystals with other nano-objects such as nanoparticles or opticalw aveguidesc an be ac hallenging task.…”

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

“…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.…”

“…[1] The spatial isolation of the molecule is achieved with an optical microscope by placing the probe molecule (guest) inside a solid (host) at a sufficiently low concentration (nm-mm). Long observation times of the line of a single molecule are possible only if the host dynamics and the associated spectral diffusion [2] of the single-molecule line are negligible in the experiments. For many interesting photonic applications [3][4][5][6][7][8] the stability of the molecule is critical, and fluctuations in local interactions between the dye and its nanoenvironment (host) should be avoided.…”

Single Molecule as a Local Acoustic Detector for Mechanical Oscillators

“…Such dynamics lead to spectral diffusion or to spectral jumps of the ZPL [20][21][22], and should therefore be eliminated or minimized for sensing applications. For example, the ZPL is very sensitive to librations of any methyl groups present in the host matrix [23]. Static hydrostatic pressure is also a well-known factor which shifts the ZPLs of single molecules [24][25][26][27].…”