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Register a new userFrom Impurity Doping to Metallic Growth in Diffusion Doping: Properties and Structure of Ag Doped InAs Nanocrystals
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Tuning of the electronic properties of pre-synthesized colloidal semiconductor nanocrystals (NCs) by doping plays a key role in the prospect of implementing them in printed electronics devices such as transistors, and photodetectors. While such impurity doping reactions have already been introduced, the understanding of the doping process, the nature of interaction between the impurity and host atoms, and the conditions affecting the solubility limit of impurities in nanocrystals are still unclear. Here, we used a post-synthesis diffusion based doping reaction to introduce Ag impurities into InAs NCs. Optical absorption spectroscopy along with analytical inductively coupled plasma mass-spectroscopy (ICP-MS) were used to present a two stage doping model consisting of a doping region and a growth region, depending on the concentration of the impurities in the reaction vessel. X-ray absorption fine-structure (XAFS) spectroscopy was employed to determine the impurity location and correlate between the structural and electronic properties for different sizes of InAs NCs and dopant concentrations. The resulting structural model describes a heterogeneous system where the impurities initially dope the NC, by substituting for In atoms near the surface of the NC, until the solubility limit is reached, after which the rapid growth and formation of metallic structures are identified.
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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, 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 exhibited remarkable stability of their hole conduction, mobility, and hysteretic behavior over time when exposed to air, while intrinsic InAs NCs FETs were easily oxidized and their performance quickly declined. Therefore, Cd plays a dual role acting as a p-type dopant, and also protects the nanocrystals from oxidation, as evidenced directly by Xray 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.
Sn$_{0.97-y}$Co$_{0.03}$Ni$_{y}$O$_{2}$ (0 $leq y leq$ 0.04) nanocrystals, with average crystallite size in the range of 7.3 nm ($y$=0.00) to 5.6 nm ($y$=0.04), have been synthesized using pH-controlled chemical co-precipitation technique. The non-stoichiometric Sn related defects and the O related stoichiometric Frenkel defects arising in the nanocrystals because of co-doping have been identified and their effect on the structural and optical properties of the nanocrystals have been extensively studied. It has been observed, using XPS that on increasing the Ni co-doping concentration ($y$), the non-stoichiometric Sn defect Sn$_{text{Sn}}^{}$ increases in compensation of existing defect Sn$_{i}^{....}$ for $y$ = 0.00 nanocrystals. High resolution transmission electron microscopy (HR-TEM) also confirms the existence of Sn$_{text{Sn}}^{}$. Regarding the Frenkel defect, XPS results indicate that the concentration of $V_{text{O}}$ and O$_{i}$, manifested in the form of dangling bond related surface defect states,increases with increase in $y$. Temperature dependent magnetisation measurement of the nanocrystals confirm the charge state of $V_{text{O}}$. The point defects have been found to affect the structural properties in a way that distortion in octahedral geometry of complete Sn-O octahderon effectively reduces whereas distortion in the trigonal planar coordination geometry of O increases. The investigation of Urbach edge indicates an enhancement in the disorder in the nanocrystals on co-doping. The optical band gap of the nanocrystals has been found to be red shifted upto $y$=0.02 and then a gradual blue shift has been observed. A direct effect of the O related defect has been observed on the blue luminescence of the nanocrystals such that the spectral contribution of blue luminescence in the total emission intensity increases by 72% for $y$=0.04 as compared to $y$=0.00.
By means of first-principles density functional theory calculations, we find that hydrogen-passivated ultrathin silicon nanowires (SiNWs) along [100] direction with symmetrical multiple surface dangling bonds (SDBs) and boron doping can have a half-metallic ground state with 100% spin polarization, where the half-metallicity is shown quite robust against external electric fields. Under the circumstances with various SDBs, the H-passivated SiNWs can also be ferromagnetic or antiferromagnetic semiconductors. The present study not only offers a possible route to engineer half-metallic SiNWs without containing magnetic atoms but also sheds light on manipulating spin-dependent properties of nanowires through surface passivation.
In order to study the metallic ferromagnetism induced by electron doping in the narrow-gab semiconductor FeSb$_2$, single crystals of FeSb$_2$, Fe$_{1-x}$Co$_x$Sb$_2$ ($0 le x le 0.5$) and FeSb$_{2-y}$Te$_y$ ($0 le y le 0.4$), were grown by a simplified self-flux method. From powder x-ray diffraction (XRD) patterns, wavelength-dispersive x-ray spectroscopy (WDX) and x-ray Laue diffraction, pure and doped high-quality single crystals, within the selected solubility range, show only the orthorhombic $Pnnm$ structure of FeSb$_2$ with a monotonic change in lattice parameters with increasing the doping level. In consistence with the model of nearly ferromagnetic small-gap semiconductor, the energy gap of FeSb$_2$ Pauli paramagnet gradually collapses by electron doping before it closes at about $x$ or $y$ = 0.15 and subsequent itinerant electron anisotropic ferromagnetic states are observed with higher doping levels. A magnetic phase diagram is established and discussed in view of proposed theoretical scenarios.
During the past years there has been renewed interest in the wide-bandgap II-VI semiconductor ZnO, triggered by promising prospects for spintronic applications. First, ferromagnetism was predicted for dilute magnetic doping. In comprehensive investigation of ZnO:Co thin films based on the combined measurement of macroscopic and microscopic properties, we find no evidence for carrier-mediated itinerant ferromagnetism. Phase-pure, crystallographically excellent ZnO:Co is uniformly paramagnetic. Superparamagnetism arises when phase separation or defect formation occurs, due to nanometer-sized metallic precipitates. Other compounds like ZnO:(Li,Ni) and ZnO:Cu do not exhibit indication of ferromagnetism. Second, its small spin-orbit coupling and correspondingly large spin coherence length makes ZnO suitable for transporting or manipulating spins in spintronic devices. From optical pump/optical probe experiments, we find a spin dephasing time of the order of 15 ns at low temperatures which we attribute to electrons bound to Al donors. In all-electrical magnetotransport measurements, we successfully create and detect a spin-polarized ensemble of electrons and transport this spin information across several nanometers. We derive a spin lifetime of 2.6 ns for these itinerant spins at low temperatures, corresponding well to results from an electrical pump/optical probe experiment.
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