4.8 Article

Origin of Low Temperature Trion Emission in CdSe Nanoplatelets

Journal

NANO LETTERS
Volume 21, Issue 23, Pages 10040-10046

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c03726

Keywords

nanocrystals; biexciton; charged exciton; transient absorption; hole transfer; colloidal quantum wells

Funding

  1. Air Force Office of Scientific Research [FA9550-20-1-0364]
  2. SHyNE Resource [NSF ECCS-2025633]
  3. IIN
  4. Northwestern's MRSEC program [NSF DMR-1720139]

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Colloidal semiconductor nanoplatelets are scalable materials for optoelectronic applications and can be used for spin-to-photon transduction in quantum information networks. Negative trions are appealing emitters, but more preparation knowledge is needed to use them as single photon-emitting states. Through power-dependent time-resolved transient absorptions, it was shown that trions form via biexciton decay and not through collisional mechanisms typical for 2D materials.
Colloidal semiconductor nanoplatelets (NPLs) are a scalable materials platform for optoelectronic applications requiring fast and narrow emission, including spin-to-photon transduction within quantum information networks. In particular, three-particle negative trions of NPLs are appealing emitters since, unlike excitons, they do not have an optically dark sublevel. In CdSe NPLs, trion emission dominates the photoluminescence (PL) spectrum at low temperature but using them as single photon-emitting states requires more knowledge about their preparation, since trions in these materials are not directly optically accessible from the ground state. This work demonstrates, using power-dependent time-resolved transient absorptions (TA) of CdSe NPLs, that trions form via biexciton decay in 1.6 ps. The scaling of the trion population and formation lifetime with excitation power indicates that they do not form through collisional mechanisms typical for 2D materials, but rather by a unimolecular hole transfer. This work is a step toward deterministic single photon emission from trions.

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