The absolute positions of the energy levels of colloidal quantum dots of Hg(S, Se, Te), which are of interest as mid-infrared materials, are determined by electrochemistry. The bulk valence bands are at -5.85, -5.50, and -4.77 eV (±0.05 eV) for zinc-blend HgS, HgSe, HgTe, respectively, in the same order as the anions p-orbital energies. The conduction bands are conversely at -5.20, -5.50, and -4.77 eV. The stable ambient n-doping of Hg(S, Se) quantum dots compared to HgTe arises because the conduction band is sufficiently lower than the measured environment Fermi level of ∼ -4.7 eV to allow for n-doping for HgS and HgSe quantum dots even with significant electron confinement. The position of the Fermi level and the quantum dots states are reported for a specific surface treatment with ethanedithiol and electrolyte environment. The positions are however sensitive to different surface treatments, providing an avenue to control doping. Electrochemical gating is further used to determine the carrier mobility in the films of the three different systems as a function of CQD size. HgSe and HgS show increasing mobility with increasing particle sizes while HgTe shows a nonmonotonous behavior, which is attributed to some degree of aggregation of HgTe QDs.
Nonaggregating HgTe colloidal quantum dots are synthesized without thiols as stabilizing ligands. The dots are spherical with a size tunability from 4.8 to 11.5 nm. When the results from optical and electrochemical measurement are combined, air-stable n-doping is observed in large sizes of HgTe quantum dots, which is attributed to the Hg-rich surface.
Improved mid-infrared photoconductors based on colloidal HgTe quantum dots are realized using a hybrid ligand exchange and polar phase transfer. The doping can also be controlled n and p by adjusting the HgCl 2 concentration in the ligand exchange process. We compare the photoconductive properties with the prior "solid-state ligand exchange" using ethanedithiol, and we find that the new process affords a ∼100-fold increase of the electron and hole mobility, a ∼100-fold increase in responsivity, and a ∼10-fold increase in detectivity. These photodetector improvements are primarily attributed to the increase in mobility (μ) because the optical properties are mostly unchanged. We show that the specific detectivity (D*) of a photoconductive device is expected to scale as μ . The application potential is further verified by long-term device stability.
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