Robust control over the carrier type is fundamental for the fabrication of nanocrystal‐based optoelectronic devices, such as the p–n homojunction, but effective incorporation of impurities in semiconductor nanocrystals and its characterization is highly challenging due to their small size. Herein, InAs nanocrystals (NCs), post‐synthetically doped with Cd, serve as a model system for successful p‐type doping of originally n‐type InAs nanocrystals, as demonstrated in field effect transistors (FETs). Advanced structural analysis, using atomic resolution electron microscopy and synchrotron X‐ray absorption fine structure spectroscopy reveal that Cd impurities reside near and on the nanocrystal surface acting as substitutional p‐dopants replacing Indium. Commensurately, Cd‐doped InAs FETs exhibit remarkable stability of their hole conduction, mobility, and hysteretic behavior over time when exposed to air, while intrinsic InAs NCs FETs are easily oxidized and their performance quickly declines. Therefore, Cd plays a dual role acting as a p‐type dopant, and also protects the nanocrystals from oxidation, as evidenced directly by X‐ray photoelectron spectroscopy measurements of air exposed samples of intrinsic and Cd‐doped InAs NCs films. This study demonstrates robust p‐type doping of InAs nanocrystals, setting the stage for implementation of such doped nanocrystal systems in printed electronic devices.
Indium phosphide (InP) nanocrystals are emerging as an alternative to heavy metal containing nanocrystals for optoelectronic applications but lag behind in terms of synthetic control. Herein, luminescent wurtzite InP nanocrystals with narrow size distribution were synthesized via a cation exchange reaction from hexagonal Cu3P nanocrystals. A comprehensive surface treatment with NOBF4 was performed, which removes excess copper while generating stoichiometric In/P nanocrystals with fluoride surface passivation. The attained InP nanocrystals manifest a highly resolved absorption spectrum with a narrow emission line of 80 meV, and photoluminescence quantum yield of up to 40%. Optical anisotropy measurements on ensemble and single particle bases show the occurrence of polarized transitions directly mirroring the anisotropic wurtzite lattice, as also manifested from modeling of the quantum confined electronic levels. This shows a green synthesis path for achieving wurtzite InP nanocrystals with desired optoelectronic properties including color purity and light polarization with potential for diverse optoelectronic applications.
The electrical functionality of an array of semiconductor nanocrystals depends critically on the free carriers that may arise from impurity or surface doping. Herein, we used InAs nanocrystals thin films as a model system to address the relative contributions of these doping mechanisms by comparative analysis of as-synthesized and Cu-doped nanocrystal based field effect transistor (FET) characteristics. By applying FET simulation methods used in conventional semiconductor FETs, we elucidate surface and impurity-doping contributions to the overall performance of InAs NCs based FETs. As-synthesized InAs nanocrystal based FETs show n-type characteristics assigned to the contribution of surface electrons accumulation layer that can be considered as an actual electron donating doping level with specific doping density and is energetically located just below the conduction band. The Cu-doped InAs NCs FETs show enhanced n-type conduction as expected from the Cu impurities location as an interstitial n-dopant in InAs nanocrystals. The simulated curves reveal the additional contribution from electrons within an impurity sub band close to the conduction band onset of the InAs NCs. The work therefore demonstrates the utility of the bulk FET simulation methodology also to NC based FETs. It provides guidelines for control of doping of nanocrystal arrays separately from surface contributions and impurity doping in colloidal semiconductor NCs towards their future utilization as building blocks in bottom-up prepared optoelectronic devices.
FET Characterization: Electrical characterization of the devices was performed under vacuum using a sealed probe station, in the dark. Measurements were taken using two Keithley 2400 source meters for source -gate, and source -drain bias, respectively.Details on the optical and spectroscopic characterizations are provided in the Supporting Information.
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