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.

Coherent transport in graphene nanoconstrictions

We study the effect of a structural nanoconstriction on the coherent transport properties of otherwise ideal zigzag-edged infinitely long graphene ribbons. The electronic structure is calculated with the standard one-orbital tight-binding model and the linear conductance is obtained using the Landauer formula. We find that, since the zero-bias current is carried in the bulk of the ribbon, this is very robust with respect to a variety of constriction geometries and edge defects. In contrast, the curve of zero-bias conductance versus gate voltage departs from the (2n+1)e2∕h staircase of the ideal case as soon as a single atom is removed from the sample. We also find that wedge-shaped constrictions can present nonconducting states fully localized in the constriction close to the Fermi energy. The interest of these localized states in regards to the formation of quantum dots in graphene is discussed.

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.

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 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.

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.

Single-electron transport in electrically tunable nanomagnets

We study a single-electron transistor (SET) based upon a II–VI semiconductor quantum dot doped with a single-Mn ion. We present evidence that this system behaves like a quantum nanomagnet whose total spin and magnetic anisotropy depend dramatically both on the number of carriers and their orbital nature. Thereby, the magnetic properties of the nanomagnet can be controlled electrically. Conversely, the electrical properties of this SET depend on the quantum state of the Mn spin, giving rise to spin-dependent charging energies and hysteresis in the Coulomb blockade oscillations of the linear conductance.