English

All-optical fluorescence blinking control in quantum dots with ultrafast mid-infrared pulses

Mesoscale and Nanoscale Physics 2023-02-22 v1 Materials Science Chemical Physics Optics

Abstract

Photoluminescence (PL) intermittency is a ubiquitous phenomenon detrimentally reducing the temporal emission intensity stability of single colloidal quantum dots (CQDs) and the emission quantum yield of their ensembles. Despite efforts for blinking reduction via chemical engineering of the QD architecture and its environment, blinking still poses barriers to the application of QDs, particularly in single-particle tracking in biology or in single-photon sources. Here, we demonstrate the first deterministic all-optical suppression of quantum dot blinking using a compound technique of visible and mid-infrared (MIR) excitation. We show that moderate-field ultrafast MIR pulses (5.5 μ\mum, 150 fs) can switch the emission from a charged, low quantum yield 'grey' trion state to the 'bright' exciton state in CdSe/CdS core-shell quantum dots resulting in a significant reduction of the QD intensity flicker. Quantum-tunneling simulations suggest that the MIR fields remove the excess charge from trions with reduced emission quantum yield to restore higher brightness exciton emission. Our approach can be integrated with existing single-particle tracking or super-resolution microscopy techniques without any modification to the sample and translates to other emitters presenting charging-induced PL intermittencies, such as single-photon emissive defects in diamond and two-dimensional materials.

Keywords

Cite

@article{arxiv.2105.01190,
  title  = {All-optical fluorescence blinking control in quantum dots with ultrafast mid-infrared pulses},
  author = {Jiaojian Shi and Weiwei Sun and Hendrik Utzat and Ardavan Farahvash and Frank Y. Gao and Zhuquan Zhang and Ulugbek Barotov and Adam P. Willard and Keith A. Nelson and Moungi G. Bawendi},
  journal= {arXiv preprint arXiv:2105.01190},
  year   = {2023}
}

Comments

35 pages, 5 figures