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Register a new userPositron studies of surfaces, structure and electronic properties of nanocrystals
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A brief review is given of recent positron studies of metal and semiconductor nanocrystals. The prospects offered by positron annihilation as a sensitive method to access nanocrystal (NC) properties are described and compared with other experimental methods. The tunability of the electronic structure of nanocrystals underlies their great potential for application in many areas. Owing to their large surface-to-volume ratio, the surfaces and interfaces of NCs play a crucial role in determining their properties. Here we focus on positron 2D angular correlation of annihilation radiation (2D-ACAR) and (two-detector) Doppler studies for investigating surfaces and electronic properties of CdSe NCs.
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The electronic structure of Si(110)16 x 2 double-domain, single-domain and 1 x 1 surfaces have been investigated using spin- and angle-resolved photoemission at sample temperatures of 77 K and 300 K. Angle-resolved photoemission was conducted using horizontally- and vertically-polarised 60 eV and 80 eV photons. Band-dispersion maps revealed four surface states ($S_1$ to $S_4$) which were assigned to silicon dangling bonds on the basis of measured binding energies and photoemission intensity changes between horizontal and vertical light polarisations. Three surface states ($S_1$, $S_2$ and $S_4$), observed in the Si(110)16 x 2 reconstruction, were assigned to Si adatoms and Si atoms present at the edges of the corrugated terrace structure. Only one of the four surface states, $S_3$, was observed in both the Si(110)16 x 2 and 1 x 1 band maps and consequently attributed to the pervasive Si zigzag chains that are components of both the Si(110)16 x 2 and 1 x 1 surfaces. A state in the bulk-band region was attributed to an in-plane bond. All data were consistent with the adatom-buckling model of the Si(110)16 x 2 surface. Whilst room temperature measurements of $P_y$ and $P_z$ were statistically compatible with zero, $P_x$ measurements of the enantiomorphic A-type and B-type Si(110)16 x 2 surfaces gave small average polarisations of around 1.5% that were opposite in sign. Further measurements at 77 K on A-type Si(110)16 x 2 surface gave a smaller value of +0.3%. An upper limit of $sim1%$ may thus be taken for the longitudinal polarisation.
The atomic structure, energy of formation, and electronic states of vacancies in H-passivated Ge nanocrystals are studied by density functional theory (DFT) methods. The competition between quantum self-purification and the free surface relaxations is investigated. The free surfaces of crystals smaller than 2 nm distort the Jahn-Teller relaxation and enhance the reconstruction bonds. This increases the energy splitting of the quantum states and reduces the energy of formation to as low as 1 eV per defect in the smallest nanocrystals. In crystals larger than 2 nm the observed symmetry of the Jahn-Teller distortion matches the symmetry expected for bulk Ge crystals. Near the nanocrystals surface the vacancy is found to have an energy of formation no larger than 0.5 to 1.4 eV per defect, but a vacancy more than 0.7 nm inside the surface has an energy of formation that is the same as in bulk Ge. No evidence of the self-purification effect is observed; the dominant effect is the free surface relaxations, which allow for the enhanced reconstruction. From the evidence in this paper, it is predicted that for moderate sized Ge nanocrystals a vacancy inside the crystal will behave bulk-like and not interact strongly with the surface, except when it is within 0.7 nm of the surface.
The effect of temperature controlled annealing on the confined valence electron states in CdSe nanocrystal arrays, deposited as thin films, was studied using two-dimensional angular correlation of annihilation radiation (2D-ACAR). A reduction in the intensity by ~35% was observed in a feature of the positron annihilation spectrum upon removal of the pyridine capping molecules above 200 degrees Celsius in a vacuum. This reduction is explained by an increased electronic interaction of the valence orbitals of neighboring nanocrystals, induced by the formation of inorganic interfaces. Partial evaporation of the nanoporous CdSe layer and additional sintering into a polycrystalline thin film was observed at a relatively low temperature of ~486 degrees Celsius.
In this paper we show that spinel ferrite nanocrystals (NiFe2O4, and CoFe2O4) can be texturally embedded inside a ZnO matrix by ion implantation and post-annealing. The two kinds of ferrites show different magnetic properties, e.g. coercivity and magnetization. Anomalous Hall effect and positive magnetoresistance have been observed. Our study suggests a ferrimagnet/semiconductor hybrid system for potential applications in magneto-electronics. This hybrid system can be tuned by selecting different transition metal ions (from Mn to Zn) to obtain various magnetic and electronic properties.
Most recent observation of topological Fermi arcs on the surface of manyfold degenerate B20 systems, CoSi and RhSi, have attracted enormous research interests. Although an another isostructural system, FeSi, has been predicted to show bulk chiral fermions, it is yet to be clear theoretically and as well experimentally that whether FeSi possesses the topological surface Fermi arcs associated with the exotic chiral fermions in vicinity of the Fermi level. In this contribution, using angle-resolved photoemission spectroscopy (ARPES) and density functional theory (DFT), we present the low-energy electronic structure of FeSi. We further report the surface state calculations to provide insights into the surface band structure of FeSi near the Fermi level. Unlike in CoSi or RhSi, FeSi has no topological Fermi arcs near the Fermi level as confirmed both from ARPES and surface state calculations. Further, the ARPES data show spin-orbit coupling (SOC) band splitting of 40 meV, which is in good agreement with bulk band structure calculations. We noticed an anomalous temperature dependent resistivity in FeSi which can be understood through the electron-phonon interactions as we find a Debye energy of 80 meV from the ARPES data.
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