Measuring Picosecond Electronic Dynamics in a Single Nanocrystal
Darius Hashemi Kalibar a, Sarah Linder a, Lorenz Moehrle a, Alfred Leitenstorfer a, Ron Tenne a b
a Department of Physics, University of Konstanz, 78464 Konstanz, Germany,
b Schulich Faculty of Chemistry, Technion – Israel Institute of Technology, Haifa, Israel, 32000
Proceedings of MATSUS Fall 2025 Conference (MATSUSFall25)
E4 (Ultrafast) Spectroscopy for Energy Materials - #SpEM
València, Spain, 2025 October 20th - 24th
Organizers: Jaco Geuchies and Freddy Rabouw
Invited Speaker, Ron Tenne, presentation 337
Publication date: 21st July 2025

Individual quantum dots (QDs) serve as inherent sources for quantum states of light such as single photons and entangled photon pairs. Ideally, under cryogenic conditions, their radiation is fully coherent – maintaining a constat phase relation throughout the emission lifetime. Often, however, the interaction of excited electrons with the lattice limits the coherence lifetime to the picosecond timescale. Experimentally, such a timescale necessitates the use of pump-probe measurements with ultrashort laser pulses. While the generation of short pulses is hardly a novelty, applying them to the sensitive spectroscopy of single nano objects is a highly challenging task. Here, we present the first transient-transmission experiments directly measuring the coherent dynamics of excitons in an individual epitaxial CdSe QD.

Using a highly stable femtosecond Er:fiber laser source, we generate the pump and probe beams that are focused through a high-numerical-aperture objective within an optical cryostat (T=1.6 K). Exciting well above the lowest-energy transition (ΔE=105 meV) temporal oscillations of the spectral lines are a fingerprint of coherence, occurring due to an evolving superposition of two nearly degenerate exciton. To explore higher-energy excitonic state, we tune our pump laser to a narrow absorption line (ΔE=21 meV). This reveals a quasi-stable excitonic state which also maintains coherence for hundreds of picoseconds. This result is especially surprising considering the frequent scattering of phonons by states with excess energy and is indicative of a robust phonon bottleneck.

The unprecedented capability of our setup to expose the full energy landscape of a single confined exciton and its dynamics following excitation promises to bring to light new physics in the realm of nano and quantum optics.

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