We study single dibenzoterrylene molecules in an anthracene single crystal at 1.4 K in two insertion sites at 785.1 and 794.3 nm. The single-molecule zero-phonon lines are narrow (about 30 MHz), intense (the detected fluorescence rates at saturation reach 100,000 counts s(-1)), and very photostable. The intersystem-crossing yield is extremely low (10(-7) or lower). All of these features are hallmarks of an excellent system for high-resolution spectroscopy and nanoscale probing at cryogenic temperatures.
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The fluorescence quantum yield of organic NIR-emitters is typically limited by internal conversion (IC), restricting their applications in imaging and quantum technology. Here, we study the impact of deuteration and temperature on the emission properties of dibenzoterrylene (DBT) by bulk and single molecule spectroscopy. Based on simple photophysical modelling, we first clarify how IC affects the single molecule emission rate.
View Article and Find Full Text PDFFluorescence-Detected Two-Dimensional Electronic Spectroscopy of a Single Molecule.
Nano Lett
October 2024
Experimental Physics III, University of Bayreuth, 95447 Bayreuth, Germany.
Single-molecule fluorescence spectroscopy is a powerful method that avoids ensemble averaging, but its temporal resolution is limited by the fluorescence lifetime to nanoseconds at most. At the ensemble level, two-dimensional spectroscopy provides insight into ultrafast femtosecond processes, such as energy transfer and line broadening, even beyond the Fourier limit, by correlating pump and probe spectra. Here, we combine these two techniques and demonstrate coherent 2D spectroscopy of individual dibenzoterrylene (DBT) molecules at room temperature.
View Article and Find Full Text PDFHigh-Resolution Cryogenic Spectroscopy of Single Molecules in Nanoprinted Crystals.
ACS Nano
August 2024
Max Planck Institute for the Science of Light, D-91058 Erlangen, Germany.
Article Synopsis
- Researchers use laser spectroscopy at very low temperatures (2 K) to study single dibenzoterrylene (DBT) molecules in tiny anthracene crystals made through a special printing technique.
- They find that the light emitted by these single molecules has very sharp transitions, almost as clear as those seen in bulk materials, indicating high-quality optical properties.
- By taking super-resolution images and changing the polarization of the light, they can measure the size and orientation of the crystals, which is important for future applications involving precisely placed quantum emitters.
2,3-Dichloroanthracene crystal, a new rigid matrix for single molecule optical investigations.
Chemphyschem
April 2024
Institute of Physics, Polish Academy of Sciences, Al. Lotników 32/46, 02-668, Warsaw, Poland.
Absorption and emission spectra of single crystals of 2,3-dichloroathracene (23DCA) and 23DCA dispersed in n-nonane matrix were studied at 5 K. Singlet and triplet excitonic bands in the crystal were estimated to be at about 415 nm and at wavelengths shorter than 700 nm, respectively. Thus, from the spectroscopic point of view, these crystals satisfy all criteria for a transparent and rigid matrix for low temperature optical studies of single molecules of dibenzoterrylene, which have their purely electronic S→S transition at around 785 nm.
View Article and Find Full Text PDFQuantum Efficiency of Single Dibenzoterrylene Molecules in -Dichlorobenzene at Cryogenic Temperatures.
J Phys Chem B
June 2023
Max Planck Institute for the Science of Light, D-91058 Erlangen, Germany.
We measure the quantum efficiency (QE) of individual dibenzoterrylene (DBT) molecules embedded in -dichlorobenzene at cryogenic temperatures. To achieve this, we combine two distinct methods based on the maximal photon emission and on the power required to saturate the zero-phonon line to compensate for uncertainties in some key system parameters. We find that the outcomes of the two approaches are in good agreement for reasonable values of the parameters involved, reporting a large fraction of molecules with QE values above 50%, with some exceeding 70%.
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