Kinetics of Aging of Large Colloidal Quantum Dots of Lead Selenide

Volume 7, Issue 3, June 2022     |     PP. 42-61      |     PDF (992 K)    |     Pub. Date: June 24, 2022
DOI: 10.54647/chemistry15265    101 Downloads     102968 Views  

Author(s)

Witold Palosz, Brimrose Corporation of America, Sparks, MD
Sudhir Trivedi, Brimrose Corporation of America, Sparks, MD
Janet L. Jensen, Edgewood Chemical Biological Center, Aberdeen Proving Ground, MD

Abstract
Effectiveness of passivation of large PbSe colloidal quantum dots (CQD) (first excitonic peak position 2 - 2.8 μm) using commonly used passivants is studied. The kinetics of oxidation over a period of up to more than one year is investigated. The effect of in-situ passivation with CdCl2, NH4Cl, Tetrabutylammonium Iodide (TBAI), and 3-Chloro-1-propanethiol (ClPTh), and of Solid-State Ligand Exchange (SSLE) using 3-Mercaptopriopionic Acid (MPA), TBAI, and 1,2-Ethanedithiol (EDT) is studied. Oxidation under different oxygen concentrations and aging of solutions is investigated. It is found that non-passivated CQDs oxidize, in the first two hours in air, at the initial rate of 2-5 layers a day. Passivation with CdCl2 or NH4Cl may reduce that initial rate by more than two orders of magnitude. Solid State Ligand Exchange process with TBAI as substituting ligand reduces the initial oxidation rate for non-passivated grains by an order of magnitude. For passivated materials SSLE process may add further protection, particularly when TBAI is used as substituting agent. EDT used as substituting agent apparently de-passivates grains. Under low concentration of Oxygen (<50 PPM) the oxidation rate can be reduced to about one oxidized Pb atom per grain over 10-day period for passivated and then SSLE'd films. TBAI was found to be the most effective both as in-situ passivant and as exchange ligand in SSLE process. The specific results of our investigation show, that meeting conditions of acceptable (negligent) oxidation (for some specific applications) may be feasible with moderately stringent technical requirements. Long term stability of devices, using typical passivation and SSLE methods, would require encapsulation.

Keywords
PbSe; colloidal quantum dots; aging; passivation

Cite this paper
Witold Palosz, Sudhir Trivedi, Janet L. Jensen, Kinetics of Aging of Large Colloidal Quantum Dots of Lead Selenide , SCIREA Journal of Chemistry. Volume 7, Issue 3, June 2022 | PP. 42-61. 10.54647/chemistry15265

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