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Heralded Spectroscopy Reveals Exciton-Exciton Correlations in Single Colloidal Quantum Dots

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2021

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Lubin, Gur
Ulku, Arin Can
Antolovic, Ivan Michel
Burri, Samuel
Karg, Sean
Yallapragada, Venkata Jayasurya
Bruschini, Claudio
Charbon, Edoardo
Oron, Dan

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Published

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Nano Letters. American Chemical Society (ACS). 2021, 21(16), pp. 6756-6763. ISSN 1530-6984. eISSN 1530-6992. Available under: doi: 10.1021/acs.nanolett.1c01291

Zusammenfassung

Multiply excited states in semiconductor quantum dots feature intriguing physics and play a crucial role in nanocrystal-based technologies. While photoluminescence provides a natural probe to investigate these states, room-temperature single-particle spectroscopy of their emission has proved elusive due to the temporal and spectral overlap with emission from the singly excited and charged states. Here, we introduce biexciton heralded spectroscopy enabled by a single-photon avalanche diode array based spectrometer. This allows us to directly observe biexciton-exciton emission cascades and measure the biexciton binding energy of single quantum dots at room temperature, even though it is well below the scale of thermal broadening and spectral diffusion. Furthermore, we uncover correlations hitherto masked in ensembles of the biexciton binding energy with both charge-carrier confinement and fluctuations of the local electrostatic potential. Heralded spectroscopy has the potential of greatly extending our understanding of charge-carrier dynamics in multielectron systems and of parallelization of quantum optics protocols.

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530 Physik

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quantum dots, multiexcitons, biexciton binding energy, single-particle spectroscopy, SPAD arrays

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ISO 690LUBIN, Gur, Ron TENNE, Arin Can ULKU, Ivan Michel ANTOLOVIC, Samuel BURRI, Sean KARG, Venkata Jayasurya YALLAPRAGADA, Claudio BRUSCHINI, Edoardo CHARBON, Dan ORON, 2021. Heralded Spectroscopy Reveals Exciton-Exciton Correlations in Single Colloidal Quantum Dots. In: Nano Letters. American Chemical Society (ACS). 2021, 21(16), pp. 6756-6763. ISSN 1530-6984. eISSN 1530-6992. Available under: doi: 10.1021/acs.nanolett.1c01291
BibTex
@article{Lubin2021-08-25Heral-55312,
  year={2021},
  doi={10.1021/acs.nanolett.1c01291},
  title={Heralded Spectroscopy Reveals Exciton-Exciton Correlations in Single Colloidal Quantum Dots},
  number={16},
  volume={21},
  issn={1530-6984},
  journal={Nano Letters},
  pages={6756--6763},
  author={Lubin, Gur and Tenne, Ron and Ulku, Arin Can and Antolovic, Ivan Michel and Burri, Samuel and Karg, Sean and Yallapragada, Venkata Jayasurya and Bruschini, Claudio and Charbon, Edoardo and Oron, Dan}
}
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