Theory of ferromagnetism in planar heterostructures of (Mn,III)-V semiconductors

A density-functional theory of ferromagnetism in heterostructures of compound semiconductors doped with magnetic impurities is presented. The variable functions in the density-functional theory are the charge and spin densities of the itinerant carriers and the charge and localized spins of the impurities. The theory is applied to study the Curie temperature of planar heterostructures of III-V semiconductors doped with manganese atoms. The mean-field, virtual-crystal and effective-mass approximations are adopted to calculate the electronic structure, including the spin-orbit interaction, and the magnetic susceptibilities, leading to the Curie temperature. By means of these results, we attempt to understand the observed dependence of the Curie temperature of planar δ-doped ferromagnetic structures on variation of their properties. We predict a large increase of the Curie temperature by additional confinement of the holes in a δ-doped layer of Mn by a quantum well.

Single-exciton spectroscopy of semimagnetic quantum dots

A photoexcited II-VI semiconductor quantum dots doped with a few Mn spins is considered. The effects of spin-exciton interactions and the resulting multispin correlations on the photoluminescence are calculated by numerical diagonalization of the Hamiltonian, including exchange interaction between electrons, holes, and Mn spins, as well as spin-orbit interaction. The results provide a unified description of recent experiments on the photoluminesnce of dots with one and many Mn atoms as well as optically induced ferromagnetism in semimagnetic quantum dots.

Single-exciton spectroscopy of single Mn doped InAs quantum dots

The optical spectroscopy of a single InAs quantum dot doped with a single Mn atom is studied using a model Hamiltonian that includes the exchange interactions between the spins of the quantum dot electron-hole pair, the Mn atom, and the acceptor hole. Our model permits linking the photoluminescence spectra to the Mn spin states after photon emission. We focus on the relation between the charge state of the Mn, A0 or A−, and the different spectra which result through either band-to-band or band-to-acceptor transitions. We consider both neutral and negatively charged dots. Our model is able to account for recent experimental results on single Mn doped InAs photoluminescence spectra and can be used to account for future experiments in GaAs quantum dots. Similarities and differences with the case of single Mn doped CdTe quantum dots are discussed.

Mn-doped II-VI quantum dots: artificial molecular magnets

The notion of artificial atom relies on the capability to change the number of carriers one by one in semiconductor quantum dots, and the resulting changes in their electronic structure. Organic molecules with transition metal atoms that have a net magnetic moment and display hysteretic behaviour are known as single molecule magnets (SMM). The fabrication of CdTe quantum dots chemically doped with a controlled number of Mn atoms and with a number of carriers controlled either electrically or optically paves the way towards a new concept in nanomagnetism: the artificial single molecule magnet. Here we study the magnetic properties of a Mn-doped CdTe quantum dot for different charge states and show to what extent they behave like a single molecule magnet.

Transport across two interacting quantum dots: Bulk Kondo, Kondo box, and molecular regimes

We analyze the transport properties of a double quantum dot device with both dots coupled to perfect conducting leads and to a finite chain of N noninteracting sites connecting both of them. The interdot chain strongly influences the transport across the system and the local density of states of the dots. We study the case of a small number of sites, so that Kondo box effects are present, varying the coupling between the dots and the chain. For odd N and small coupling between the interdot chain and the dots, a state with two coexisting Kondo regimes develops: the bulk Kondo due to the quantum dots connected to leads and the one produced by the screening of the quantum dot spins by the spin in the finite chain at the Fermi level. As the coupling to the interdot chain increases, there is a crossover to a molecular Kondo effect, due to the screening of the molecule (formed by the finite chain and the quantum dots) spin by the leads. For even N the two Kondo temperatures regime does not develop and the physics is dominated by the usual competition between Kondo and antiferromagnetism between the quantum dots. We finally study how the transport properties are affected as N is increased. For the study we used exact multiconfigurational Lanczos calculations and finite-U slave-boson mean-field theory at T=0. The results obtained with both methods describe qualitatively and also quantitatively the same physics.

Optical initialization, readout, and dynamics of a Mn spin in a quantum dot

We have investigated the spin preparation efficiency by optical pumping of individual Mn atoms embedded in CdTe/ZnTe quantum dots. Monitoring the time dependence of the intensity of the fluorescence during the resonant optical pumping process in individual quantum dots allows to directly probe the dynamics of the initialization of the Mn spin. This technique presents the convenience of including preparation and readout of the Mn spin in the same step. Our measurements demonstrate that Mn spin initialization, at zero magnetic field, can reach an efficiency of 75% and occurs in the tens of nanoseconds range when a laser resonantly drives at saturation one of the quantum-dot transition. We observe that the efficiency of optical pumping changes from dot-to-dot and is affected by a magnetic field of a few tens of millitesla applied in Voigt or Faraday configuration. This is attributed to the local strain distribution at the Mn location which predominantly determines the dynamics of the Mn spin under weak magnetic field. The spectral distribution of the spin-flip-scattered photons from quantum dots presenting a weak optical pumping efficiency reveals a significant spin relaxation for the exciton split in the exchange field of the Mn spin.

Impurity states in the quantum spin Hall phase in graphene

Two-dimensional insulators with time-reversal symmetry can have two topologically different phases, the quantum spin Hall and the normal phase. The former is revealed by the existence of conducting edge states that are topologically protected. Here we show that the reaction to impurity, in bulk, is radically different in the two phases and can be used as a marker for the topological phase. Within the context of the Kane-Mele model for graphene, we find that strictly normalizable in-gap impurity states only occur in the quantum spin Hall phase and carry a dissipationless current whose chirality is determined by the spin and pseudospin of the residing electron.

Optical control of the spin state of two Mn atoms in a quantum dot

We report on the optical spectroscopy of the spin of two magnetic atoms (Mn) embedded in an individual quantum dot interacting with a single electron, a single exciton, or a single trion. As a result of their interaction to a common entity, the Mn spins become correlated. The dynamics of this process is probed by time-resolved spectroscopy, which permits us to determine an optical orientation time in the range of a few tens of nanoseconds. In addition, we show that the energy of the collective spin states of the two Mn atoms can be tuned through the optical Stark effect induced by a resonant laser field.

Ferromagnetism mediated by few electrons in a semimagnetic quantum dot

A (II,Mn)VI diluted magnetic semiconductor quantum dot with an integer number of electrons controlled with a gate voltage is considered. We show that a single electron is able to induce a collective spontaneous magnetization of the Mn spins, overcoming the short range antiferromagnetic interactions, at a temperature order of 1 K, 2 orders of magnitude above the ordering temperature in bulk. The magnetic behavior of the dot depends dramatically on the parity of the number of electrons in the dot.

Electrical control of a single Mn atom in a quantum dot

We report on the reversible electrical control of the magnetic properties of a single Mn atom in an individual quantum dot. Our device permits us to prepare the dot in states with three different electric charges, 0, +1e, and -1e which result in dramatically different spin properties, as revealed by photoluminescence. Whereas in the neutral configuration the quantum dot is paramagnetic, the electron-doped dot spin states are spin rotationally invariant and the hole-doped dot spins states are quantized along the growth direction.

Quantum Hall effect in gapped graphene heterojunctions

We model the quantum Hall effect in heterostructures made of two gapped graphene stripes with different gaps, Δ1 and Δ2. We consider two main situations, Δ1=0,Δ2≠0, and Δ1=−Δ2. They are different in a fundamental aspect: only the latter features kink states that, when intervalley coupling is absent, are protected against backscattering. We compute the two-terminal conductance of heterostructures with channel length up to 430 nm, in two transport configurations, parallel and perpendicular to the interface. By studying the effect of disorder on the transport along the boundary, we quantify the robustness of kink states with respect to backscattering. Transport perpendicular to the boundary shows how interface states open a backscattering channel for the conducting edge states, spoiling the perfect conductance quantization featured by the homogeneously gapped graphene Hall bars. Our results can be relevant for the study of graphene deposited on hexagonal boron-nitride, as well as to model graphene with an interaction-driven gapped phase with two equivalent phases separated by a domain wall.

Quantum Dot-Sensitized Solar Cells Based on Directly Adsorbed Zinc Copper Indium Sulfide Colloids

Heavy metal-based quantum dots (QDs) have demonstrated to behave as efficient sensitizers in QD-sensitized solar cells (QDSSCs), as attested by the countless works and encouraging efficiencies reported so far. However, their intrinsic toxicity has arisen as a major issue for the prospects of commercialization. Here, we examine the potential of environmentally friendly zinc copper indium sulfide (ZCIS) QDs for the fabrication of liquid-junction QDSSCs by means of photoelectrochemical measurements. A straightforward approach to directly adsorb ZCIS QDs on TiO2 from a colloidal dispersion is presented. Incident photon-to-current efficiency (IPCE) spectra of sensitized photoanodes show a marked dependence on the adsorption time, with longer times leading to poorer performances. Cyclic voltammograms point to a blockage of the channels of the mesoporous TiO2 film by the agglomeration of QDs as the main reason for the decrease in efficiency. Photoanodes were also submitted to the ZnS treatment. Its effects on electron recombination with the electrolyte are analyzed through electrochemical impedance spectroscopy and photopotential measurements. The corresponding results bring out the role of the ZnS coating as a barrier layer preventing electron leakage toward the electrolyte, as argued in other QD-sensitized systems. The beneficial effect of the ZnS coating is ultimately reflected on the power conversion efficiency of complete devices, reaching values of 2 %. In a more general vein, through these findings, we aim to call the attention to the potentiality of this quaternary alloy, virtually unexplored as a light harvester for sensitized devices.

Consequences of Kondo exchange on quantum spins

When individual quantum spins are placed in close proximity to conducting substrates, the localized spin is coupled to the nearby itinerant conduction electrons via Kondo exchange. In the strong coupling limit this can result in the Kondo effect — the formation of a correlated, many body singlet state — and a resulting renormalization of the density of states near the Fermi energy. However, even when Kondo screening does not occur, Kondo exchange can give rise to a wide variety of other phenomena. In addition to the well known renormalization of the g factor and the finite spin decoherence and relaxation times, Kondo exchange has recently been found to give rise to a newly discovered effect: the renormalization of the single ion magnetic anisotropy. Here we put these apparently different phenomena on equal footing by treating the effect of Kondo exchange perturbatively. In this formalism, the central quantity is ρJ, the product of the density of states at the Fermi energy ρ and the Kondo exchange constant J. We show that perturbation theory correctly describes the experimentally observed exchange induced shifts of the single spin excitation energies, demonstrating that Kondo exchange can be used to tune the effective magnetic anisotropy of a single spin.

Interplay Between Structure, Stoichiometry, and Electron Transfer Dynamics in SILAR-based Quantum Dot-Sensitized Oxides

We quantify the rate and efficiency of picosecond electron transfer (ET) from PbS nanocrystals, grown by successive ionic layer adsorption and reaction (SILAR), into a mesoporous SnO2 support. Successive SILAR deposition steps allow for stoichiometry- and size-variation of the QDs, characterized using transmission electron microscopy. Whereas for sulfur-rich (p-type) QD surfaces substantial electron trapping at the QD surface occurs, for lead-rich (n-type) QD surfaces, the QD trapping channel is suppressed and the ET efficiency is boosted. The ET efficiency increase achieved by lead-rich QD surfaces is found to be QD-size dependent, increasing linearly with QD surface area. On the other hand, ET rates are found to be independent of both QD size and surface stoichiometry, suggesting that the donor–acceptor energetics (constituting the driving force for ET) are fixed due to Fermi level pinning at the QD/oxide interface. Implications of our results for QD-sensitized solar cell design are discussed.

Quantum spin Hall phase in multilayer graphene

The so-called quantum spin Hall phase is a topologically nontrivial insulating phase that is predicted to appear in graphene and graphenelike systems. In this paper we address the question of whether this topological property persists in multilayered systems. We consider two situations: purely multilayer graphene and heterostructures where graphene is encapsulated by trivial insulators with a strong spin-orbit coupling. We use a four-orbital tight-binding model that includes full atomic spin-orbit coupling and we calculate the Z2 topological invariant of the bulk states as well as the edge states of semi-infinite crystals with armchair termination. For homogeneous multilayers we find that even when the spin-orbit interaction opens a gap for all possible stackings, only those with an odd number of layers host gapless edge states while those with an even number of layers are trivial insulators. For heterostructures where graphene is encapsulated by trivial insulators, it turns out that interlayer coupling is able to induce a topological gap whose size is controlled by the spin-orbit coupling of the encapsulating materials, indicating that the quantum spin Hall phase can be induced by proximity to trivial insulators.