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CdSe nanoplatelets show perfectly quantized thicknesses of few monolayers. They present a situation of extreme, yet well defined quantum confinement. Due to large dielectric contrast between the semiconductor and its ligand environment, interaction between carriers and their dielectric images strongly renormalize bare single particle states. We discuss the electronic properties of this original system in an advanced tight-binding model, and show that Coulomb interactions, including self-energy corrections and enhanced electron-hole interaction, lead to exciton binding energies up to several hundred meVs.

We study the dependence of the quantum yield of photoluminescence of a dense, periodic array of semiconductor nanocrystals (NCs) on the level of doping and NC size. Electrons introduced to NCs via doping quench photoluminescence by the Auger process, so that practically only NCs without electrons contribute to the photoluminescence. Computer simulation and analytical theory are used to find a fraction of such empty NCs as a function of the average number of donors per NC and NC size. For an array of small spherical NCs, the quantization gap between 1S and 1P levels leads to transfer of electrons from NCs with large number of donors to those without donors. As a result, empty NCs become extinct, and photoluminescence is quenched abruptly at an average number of donors per NC close to 1.8. The relative intensity of photoluminescence is shown to correlate with the type of hopping conductivity of an array of NCs.

We present a theoretical description of excitons and positively and negatively charged trions in "giant" CdSe/CdS core-shell nanocrystals (NCs). The developed theory provides the parameters describing the fine structure of excitons in CdSe/CdS core/thick shell NCs as a function of the CdSe/CdS conduction band offset and the CdSe core radius. We have also developed a general theory describing the fine structure of positively charged trions created in semiconductor NCs with a degenerate valence band. The calculations take into account the complex structure of the CdSe valence band and inter-particle Coulomb and exchange interaction. Presented in this paper are the CdSe core size and CdSe/CdS conduction band offset dependences (i) of the positively charged trion fine structure, (ii) of the binding energy of the negatively charged trion, and (iii) of the radiative decay time for excitons and trions. The results of theoretical calculations are in qualitative agreement with available experimental data., Comment: Accepted for publication in Phys. Rev. B

We predict a new physical mechanism explaining the electron spin precession frequency focusing effect observed recently in singly charged quantum dots exposed to a periodic train of resonant circularly polarized short optical pulses [A. Greilich et al, Science 317, 1896 (2007), Ref. 1]. We show that electron spin precession in an external magnetic field and a field of nuclei creates a Knight field oscillating at the frequency of nuclear spin resonance. This field drives the projection of the nuclear spin onto magnetic field to the value that makes the electron spin precession frequency a multiple of the train cyclic repetition frequency, which is the condition at which the Knight field vanishes., Comment: 4+ pages, 3 figures

A theory of the electronic structure and excitonic absorption spectra of PbS and PbSe nanowires and nanorods in the framework of a four-band effective mass model is presented. Calculations conducted for PbSe show that dielectric contrast dramatically strengthens the exciton binding in narrow nanowires and nanorods. However, the self-interaction energies of the electron and hole nearly cancel the Coulomb binding, and as a result the optical absorption spectra are practically unaffected by the strong dielectric contrast between PbSe and the surrounding medium. Measurements of the size-dependent absorption spectra of colloidal PbSe nanorods are also presented. Using room-temperature energy-band parameters extracted from the optical spectra of spherical PbSe nanocrystals, the theory provides good quantitative agreement with the measured spectra., Comment: 35 pages, 12 figures

A description of spin Faraday rotation, Kerr rotation and ellipticity signals for single- and multi-layer ensembles of singly charged quantum dots (QDs) is developed. The microscopic theory considers both the single pump-pulse excitation and the effect of a train of such pulses, which in the case of long resident-electron spin coherence time leads to a stationary distribution of the electron spin polarization. The calculations performed for single-color and two-color pump-probe setups show that the three experimental techniques: Faraday rotation, Kerr rotation and ellipticity measurements provide complementary information about an inhomogeneous ensemble of QDs. The microscopic theory developed for a three-dimensional ensemble of QDs is shown to agree with the phenomenological description of these effects. The typical time-dependent traces of pump-probe Faraday rotation, Kerr rotation and ellipticity signals are calculated for various experimental conditions., Comment: 19 pages, 12 figures

We show that the spins of all electrons, each confined in a quantum dot of an (In,Ga)As/GaAs dot ensemble, can be driven into a single mode of precession about a magnetic field. This regime is achieved by allowing only a single mode within the electron spin precession spectrum of the ensemble to be synchronized with a train of periodic optical excitation pulses. Under this condition a nuclei induced frequency focusing leads to a shift of all spin precession frequencies into the synchronized mode. The macroscopic magnetic moment of the electron spins that is created in this regime precesses without dephasing., Comment: 5 pages, 4 figures

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., Comment: 15 pages, 3 figures; submitted

In a recent Letter [PRL 96, 226802 (2006)], Dalpian and Chelikowsky claimed that formation energies of Mn impurities in CdSe nanocrystals increase as the size of the nanocrystal decreases, and argued that this size dependence leads to "self-purification" of small nanocrystals. They presented density-functional-theory (DFT) calculations showing a strong size dependence for Mn impurity formation energies, and proposed a general explanation. In this Comment we show that several different DFT codes, pseudopotentials, and exchange-correlation functionals give a markedly different result: We find no such size dependence. More generally, we argue that formation energies are not relevant to substitutional doping in most colloidally grown nanocrystals., Comment: 1 page, 1 figure

Using the recently reported mode locking effect we demonstrate a highly robust control of electron spin coherence in an ensemble of (In,Ga)As quantum dots during the single spin coherence time. The spin precession in a transverse magnetic field can be fully controlled up to 25 K by the parameters of the exciting pulsed laser protocol such as the pulse train sequence, leading to adjustable quantum beat bursts in Faraday rotation. Flipping of the electron spin precession phase was demonstrated by inverting the polarization within a pulse doublet sequence., Comment: 5 Pages, 3 figures

Electron spin coherence has been generated optically in n-type modulation doped (In,Ga)As/GaAs quantum dots (QDs) which contain on average a single electron per dot. The coherence arises from resonant excitation of the QDs by circularly-polarized laser pulses, creating a coherent superposition of an electron and a trion state. Time dependent Faraday rotation is used to probe the spin precession of the optically oriented electrons about a transverse magnetic field. Spin coherence generation can be controlled by pulse intensity, being most efficient for (2n+1)pi-pulses., Comment: 5 pages, 4 figures

A theory of Electric Dipole Spin Resonance (EDSR), that is caused by various mechanisms of spin-orbit coupling, is developed as applied to free electrons in a parabolic quantum well. Choosing a parabolic shape of the well has allowed us to find explicit expressions for the EDSR intensity and its dependence on the magnetic field direction in terms of the basic parameters of the Hamiltonian. By using these expressions, we have investigated and compared the effect of specific mechanisms of spin orbit (SO) coupling and different polarizations of ac electric field on the intensity of EDSR. Angular dependences of the EDSR intensity are indicative of the relative contributions of the competing mechanisms of SO coupling. Our results show that electrical manipulating electron spins in quantum wells is generally highly efficient, especially by an in-plane ac electric field., Comment: 45 pages 6 figure

We present a comprehensive examination of optical pumping of spins in individual GaAs quantum dots as we change the charge from positive to neutral to negative using a Schottky diode. We observe that photoluminescence polarization memory has the same sign as the net charge of the dot. Optical pumping of ground state electron spins enhances this effect, as demonstrated through the first measurements of the Hanle effect on an individual quantum dot. With the Overhauser effect in a high longitudinal magnetic field, we demonstrate efficient optical pumping of the quantum dot's nuclear spins for all three charge states.

We have theoretically shown that optical properties of semiconductor nanorods are controlled by 1D excitons. The theory, which takes into account anisotropy of spacial and dielectric confinement, describes size dependence of interband optical transitions, exciton binding energies. We have demonstrated that the fine structure of the ground exciton state explains the linear polarization of photoluminescence. Our results are in good agreement with the measurements in CdSe nanorods.

Electron spins in a semiconductor quantum well couple to an electric field {\it via} spin-orbit interaction. We show that the standard spin-orbit coupling mechanisms can provide extraordinary efficient electron spin manipulation by an in-plane ac electric field.

We describe theoretically the resonant optical excitation of a trion with circularly polarized light and discuss how this trion permits the read-out of a single electron spin through a recycling transition. Optical pumping through combination of circularly polarized optical $\pi$--pulses with permanent or $\pi$-- pulsed transverse magnetic fields suggests feasible protocols for spin initialization.

A theory of spin manipulation of quasi-two-dimensional (2D) electrons by a time-dependent gate voltage applied to a quantum well is developed. The Dresselhaus and Rashba spin-orbit coupling mechanisms are shown to be rather efficient for this purpose. The spin response to a perpendicular-to-plane electric field is due to a deviation from the strict 2D limit and is controlled by the ratios of the spin, cyclotron and confinement frequencies. The dependence of this response on the magnetic field direction is indicative of the strenghts of the competing spin-orbit coupling mechanisms.

The structure of the electron quantum size levels in spherical nanocrystals is studied in the framework of an eight--band effective mass model at zero and weak magnetic fields. The effect of the nanocrystal surface is modeled through the boundary condition imposed on the envelope wave function at the surface. We show that the spin--orbit splitting of the valence band leads to the surface--induced spin--orbit splitting of the excited conduction band states and to the additional surface--induced magnetic moment for electrons in bare nanocrystals. This additional magnetic moment manifests itself in a nonzero surface contribution to the linear Zeeman splitting of all quantum size energy levels including the ground 1S electron state. The fitting of the size dependence of the ground state electron g factor in CdSe nanocrystals has allowed us to determine the appropriate surface parameter of the boundary conditions. The structure of the excited electron states is considered in the limits of weak and strong magnetic fields., Comment: 11 pages, 4 figures, submitted to Phys. Rev. B

We report on the optical manipulation of the electron spin relaxation time in a GaAs based heterostructure. Experimental and theoretical study shows that the average electron spin relaxes through hyperfine interaction with the lattice nuclei, and that the rate can be controlled by the electron-electron interactions. This time has been changed from 300 ns down to 5 ns by variation of the laser frequency. This modification originates in the optically induced depletion of n-GaAs layer.

Time-resolved Faraday rotation is used to study both transverse and longitudinal spin relaxation in chemically-synthesized CdSe nanocrystals (NCs) 22-80 Angstroms in diameter. The precession of optically-injected spins in a transverse magnetic field occurs at distinct frequencies whose assignment to electron and exciton spins is developed through systematic studies of the size-dependence and theoretical calculations. It is shown that the transverse spin lifetime is limited by inhomogeneous dephasing to a degree that cannot be accounted for by the NC size distribution alone. Longitudinal spin relaxation in these NCs occurs on several distinct timescales ranging from 100 ps-10 microseconds and exhibits markedly different dependencies on temperature and field in comparison to transverse spin relaxation., Comment: 25 pages, 11 figures, table

We have studied theoretically the electron spin relaxation in semiconductor quantum dots via interaction with nuclear spins. The relaxation is shown to be determined by three processes: (i) -- the precession of the electron spin in the hyperfine field of the frozen fluctuation of the nuclear spins; (ii) -- the precession of the nuclear spins in the hyperfine field of the electron; and (iii) -- the precession of the nuclear spin in the dipole field of its nuclear neighbors. In external magnetic fields the relaxation of electron spins directed along the magnetic field is suppressed. Electron spins directed transverse to the magnetic field relax completely in a time on the order of the precession period of its spin in the field of the frozen fluctuation of the nuclear spins. Comparison with experiment shows that the hyperfine interaction with nuclei may be the dominant mechanism of electron spin relaxation in quantum dots.

We have derived general boundary conditions (BC) for the multiband envelope functions (which do not contain spurious solutions) in semiconductor heterostructures with abrupt heterointerfaces. These BC require the conservation of the probability flux density normal to the interface and guarantee that the multiband Hamiltonian be self--adjoint. The BC are energy independent and are characteristic properties of the interface. Calculations have been performed of the effect of the general BC on the electron energy levels in a potential well with infinite potential barriers using a coupled two band model. The connection with other approaches to determining BC for the envelope function and to the spurious solution problem in the multiband k.p model are discussed., Comment: 15 pages, 2 figures; to be published in Phys. Rev. B 65, March 15 issue 2002