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Register a new userAnomalous Suppression of Valley Splittings in Lead Salt Nanocrystals without Inversion Center
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Added by
Alexander N. Poddubny
Publication date
2011
fields
Physics
and research's language is
English
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Atomistic sp3d5s* tight-binding theory of PbSe and PbS nanocrystals is developed. It is demonstrated, that the valley splittings of confined electrons and holes strongly and peculiarly depend on the geometry of a nanocrystal. When the nanocrystal lacks a microscopic center of inversion and has T_d symmetry, the splitting is strongly suppressed as compared to the more symmetric nanocrystals with O_h symmetry, having an inversion center.
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Auger recombination (AR) of the ground biexciton state in quantum-confined lead salt nanowires (NWs) with a strong coupling between the conduction and the valence bands is shown to be strongly suppressed, and only excited biexciton states contribute to Auger decay. The AR rate is predicted to be greatly reduced when temperature or the NW radius are decreased, and the effect is explained by decrease in both the population of excited biexciton states and overlap of phonon-broadened single- and biexciton states. Suppression of AR of multiexciton states exhibiting strong radiative decay makes obviously lead salt NWs a subject of special interest for numerous lasing applications.
We use an empirical tight-binding approach to calculate electron and hole states in [111]-grown PbSe nanowires. We show that the valley-orbit and spin-orbit splittings are very sensitive to the atomic arrangement within the nanowire elementary cell and differ for [111]-nanowires with microscopic $D_{3d}$, $C_{2h}$ and $D_{3}$ symmetries. For the nanowire diameter below 4 nm the valley-orbit splittings become comparable with the confinement energies and the $boldsymbol{k}cdotboldsymbol{p}$ method is inapplicable. Nanowires with the $D_{3}$ point symmetry having no inversion center exhibit giant spin splitting $E = alpha k_z$, linear in one-dimensional wave vector $k_z$, with the constant $alpha$ up to 1 eV$cdot$AA.
An important challenge in silicon quantum electronics in the few electron regime is the potentially small energy gap between the ground and excited orbital states in 3D quantum confined nanostructures due to the multiple valley degeneracies of the conduction band present in silicon. Understanding the valley-orbit (VO) gap is essential for silicon qubits, as a large VO gap prevents leakage of the qubit states into a higher dimensional Hilbert space. The VO gap varies considerably depending on quantum confinement, and can be engineered by external electric fields. In this work we investigate VO splitting experimentally and theoretically in a range of confinement regimes. We report measurements of the VO splitting in silicon quantum dot and donor devices through excited state transport spectroscopy. These results are underpinned by large-scale atomistic tight-binding calculations involving over 1 million atoms to compute VO splittings as functions of electric fields, donor depths, and surface disorder. The results provide a comprehensive picture of the range of VO splittings that can be achieved through quantum engineering.
Inversion symmetry breaking allows contrasted circular dichroism in different k-space regions, which takes the extreme form of optical selection rules for interband transitions at high symmetry points. In materials where band-edges occur at noncentral valleys, this enables valley dependent interplay of electrons with light of different circular polarizations, in analogy to spin dependent optical activities in semiconductors. This discovery is in perfect harmony with the previous finding of valley contrasted Bloch band features of orbital magnetic moment and Berry curvatures from inversion symmetry breaking [Phys. Rev. Lett. 99, 236809 (2007)]. A universal connection is revealed between the k-resolved optical oscillator strength of interband transitions, the orbital magnetic moment and the Berry curvatures, which also provides a principle for optical measurement of orbital magnetization and intrinsic anomalous Hall conductivity in ferromagnetic systems. The general physics is demonstrated in graphene where inversion symmetry breaking leads to valley contrasted optical selection rule for interband transitions. We discuss graphene based valley optoelectronics applications where light polarization information can be interconverted with electronic information.
We study the low-temperature magneto-photoluminescence (PL) from individual CdSe nanocrystals. Nanocrystals having a small bright exciton fine structure splitting ($<$0.5 meV) exhibit a conventional left- and right-circularly polarized Zeeman PL doublet in applied magnetic fields. In contrast, nanocrystals with large fine structure splitting ($>$1 meV) show an anomalous magneto-PL polarization, wherein the lower-energy peak becomes circularly polarized with increasing field, while the higher-energy peak remains linearly polarized. This unusual behavior arises from strong mixing between the absorbing and emitting bright exciton levels due to strong anisotropic exchange interactions.
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