Low-temperature spectroscopic studies of single molecules in 3-D and on 2-D hosts

Smit, R. (2024)

Doctoral Thesis

Spectroscopic studies on fluorescent single molecules in organic condensed matter does not only provide information about the molecule itself, but also its near environment. By suppression of phonon-induced broadening of spectral lines through cooling to low temperatures, small changes in the spectral lines’ position can be observed in response to weak variations in local fields. These variations can for instance be caused by rearrangements of charges or minute changes in the crystal lattice around the molecule. Therefore, molecules are sensitive sensors to what happens at the nanoscale. This is exemplified by coupling to an external electric field, inducing a Stark shift of the molecule’s spectral lines, as shown in Chapter 4. Other dynamics, related to the crystal around the molecule, are resolved in the fluorescence of molecules on the surface of two-dimensional hexagonal boron nitride, shown in Chapter 5. In Chapter 2, 3 and 6, perylene molecules are studied in a new host crystal with the aim of detecting a ‘forbidden’ transition to the triplet state from the ground state, a transition required for building a single-molecule optical switch.

• Single-molecule spectroscopy
• Stark effect
• Triplet states
• Fluorescence
• 2D materials
• Quantum optics

• All authors: Smit, R.
• Supervisor: Orrit, M.A.G.J.
• Co-supervisor: Zant, H.S.J. van der
• Committee: Sandoghdar, V.; Toninelli, C.; Aarts, J.; Exter, M. van; Ruitenbeek, J.M. van
• Qualification: Doctor (dr.)
• Awarding Institution: Leiden Institute of Physics (LION), Faculty of Science, Leiden University
• Date: 2024-06-12