Margaret Dobrowolska

Giant Zeeman splitting in nucleation-controlled doped CdSe:Mn2+ quantum nanoribbons

Doping of semiconductor nanocrystals by transition-metal ions has attracted tremendous attention owing to their nanoscale spintronic applications. Such doping is, however, difficult to achieve in low-dimensional strongly quantum confined nanostructures by conventional growth procedures. Here we demonstrate that the incorporation of manganese ions up to 10% into CdSe quantum nanoribbons can be readily achieved by a nucleation-controlled doping process. The cation-exchange reaction of (CdSe)(13) clusters with Mn(2+) ions governs the Mn(2+) incorporation during the nucleation stage. This highly efficient Mn(2+) doping of the CdSe quantum nanoribbons results in giant exciton Zeeman splitting with an effective g-factor of approximately 600, the largest value seen so far in diluted magnetic semiconductor nanocrystals. Furthermore, the sign of the s-d exchange is inverted to negative owing to the exceptionally strong quantum confinement in our nanoribbons. The nucleation-controlled doping strategy demonstrated here thus opens the possibility of doping various strongly quantum confined nanocrystals for diverse applications.

Spin-polarizable excitonic luminescence in colloidal Mn2+-doped CdSe quantum dots.

The photoluminescence of colloidal Mn2+-doped CdSe nanocrystals has been studied as a function of nanocrystal diameter. These nanocrystals are shown to be unique among colloidal doped semiconductor nanocrystals reported to date in that quantum confinement allows tuning of the CdSe bandgap energy across the Mn2+ excited-state energies. At small diameters, the nanocrystal photoluminescence is dominated by Mn 2+ emission. At large diameters, CdSe excitonic photoluminescence dominates. The latter scenario has allowed spin-polarized excitonic photoluminescence to be observed in colloidal doped semiconductor nanocrystals for the first time.

Controlling the Curie temperature in (Ga,Mn)As through location of the Fermi level within the impurity band

The ferromagnetic semiconductor (Ga,Mn)As has emerged as the most studied material for prototype applications in semiconductor spintronics. Because ferromagnetism in (Ga,Mn)As is hole-mediated, the nature of the hole states has direct and crucial bearing on its Curie temperature T(C). It is vigorously debated, however, whether holes in (Ga,Mn)As reside in the valence band or in an impurity band. Here we combine results of channelling experiments, which measure the concentrations both of Mn ions and of holes relevant to the ferromagnetic order, with magnetization, transport, and magneto-optical data to address this issue. Taken together, these measurements provide strong evidence that it is the location of the Fermi level within the impurity band that determines T(C) through determining the degree of hole localization. This finding differs drastically from the often accepted view that T(C) is controlled by valence band holes, thus opening new avenues for achieving higher values of T(C).

Four-Wave Mixing in Perovskite Photovoltaic Materials Reveals Long Dephasing Times and Weaker Many-Body Interactions than GaAs

Perovksite semiconductors have shown promise for low-cost solar cells, lasers and photodetectors, yet their fundamental photophysical properties are not well understood. Recent observations of a low exciton binding energy and evidence of hot phonon effects in the room temperature phase suggest that perovskites are much closer to inorganic semiconductors than the absorber layers in traditional organic photovoltaics, signaling the need for experiments that shed light on the placement of perovskite materials within the spectrum of semiconductors used in optoelectronics and photovoltaics. Here we use four-wave mixing (FWM) to contrast the coherent optical response of CH3NH3PbI3 thin films and crystalline GaAs. At carrier densities relevant for solar cell operation, our results show that carriers interact surprisingly weakly via the Coulomb interaction in perovskite, much weaker than in inorganic semiconductors. These weak many-body effects lead to a dephasing time in CH3NH3PbI3 ∼ 3× longer than in GaAs. Our r...

Room temperature weak ferromagnetism in Sn1−xMnxSe2 2D films grown by molecular beam epitaxy

We discuss growth and magnetic properties of high-quality two dimensional (2D) Sn1−xMnxSe2 films. Thin films of this 2D ternary alloy with a wide range of Mn concentrations were successfully grown by molecular beam epitaxy. Mn concentrations up to x ≈ 0.60 were achieved without destroying the crystal structure of the parent SnSe2 2D system. Most important, the specimens show clear weak ferromagnetic behavior above room temperature, which should be of interest for 2D spintronic applications.

Measurement of coherence decay in GaMnAs using femtosecond four-wave mixing.

The application of femtosecond four-wave mixing to the study of fundamental properties of diluted magnetic semiconductors ((s,p)-d hybridization, spin-flip scattering) is described, using experiments on GaMnAs as a prototype III-Mn-V system. Spectrally-resolved and time-resolved experimental configurations are described, including the use of zero-background autocorrelation techniques for pulse optimization. The etching process used to prepare GaMnAs samples for four-wave mixing experiments is also highlighted. The high temporal resolution of this technique, afforded by the use of short (20 fsec) optical pulses, permits the rapid spin-flip scattering process in this system to be studied directly in the time domain, providing new insight into the strong exchange coupling responsible for carrier-mediated ferromagnetism. We also show that spectral resolution of the four-wave mixing signal allows one to extract clear signatures of (s,p)-d hybridization in this system, unlike linear spectroscopy techniques. This increased sensitivity is due to the nonlinearity of the technique, which suppresses defect-related contributions to the optical response. This method may be used to measure the time scale for coherence decay (tied to the fastest scattering processes) in a wide variety of semiconductor systems of interest for next generation electronics and optoelectronics.

MBE growth of few-layer 2H-MoTe 2 on 3D substrates

Abstract MoTe2 is the least explored material in the Molybdenum-chalcogen family. Molecular beam epitaxy (MBE) provides a unique opportunity to tackle the small electronegativity difference between Mo and Te while growing layer by layer away from thermodynamic equilibrium. We find that for a few-layer MoTe2 grown at a moderate rate of ∼6 min per monolayer, a narrow window in temperature (above Te cell temperature) and Te:Mo ratio exists, where we can obtain pure phase 2H-MoTe2. This is confirmed using reflection high-energy electron diffraction (RHEED), Raman spectroscopy and X-ray photoemission spectroscopy (XPS). For growth on CaF2, Grazing incidence X-ray diffraction (GI-XRD) reveals a grain size of ∼90 A and presence of twinned grains. In this work, we hypothesis the presence of excess Te incorporation in MBE grown few layer 2H-MoTe2. For film on CaF2, it is based on >2 Te:Mo stoichiometry using XPS as well as ‘a’ and ‘c’ lattice spacing greater than bulk 2H-MoTe2. On GaAs, its based on observations of Te crystallite formation on film surface, 2 × 2 superstructure observed in RHEED and low energy electron diffraction, larger than bulk c-lattice spacing as well as the lack of electrical conductivity modulation by field effect. Finally, thermal stability and air sensitivity of MBE 2H-MoTe2 is investigated by temperature dependent XRD and XPS, respectively.

Structural evolution of dilute magnetic (Sn,Mn)Se films grown by molecular beam epitaxy

We describe the structural evolution of dilute magnetic (Sn,Mn)Se films grown by molecular beam epitaxy on GaAs (111) substrates, as revealed by transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. When the Mn concentration is increased, the lattice of the ternary (Sn,Mn)Se films evolves quasi-coherently from a SnSe2 two-dimensional (2D) crystal structure into a more complex quasi-2D lattice rearrangement, ultimately transforming into the magnetically concentrated antiferromagnetic MnSe 3D rock-salt structure as Mn approaches 50 at. % of this material. These structural transformations are expected to underlie the evolution of magnetic properties of this ternary system reported earlier in the literature.

Anisotropic AC Magnetic Susceptibility in (Ga,Mn)As Films

We report a systematic investigation of ac magnetic susceptibility in (Ga,Mn)As films as a function of temperature and magnetic field, carried out in parallel with dc magnetization measurements. The temperature dependence of ac susceptibility χac shows anisotropic behavior: 1) a single peak in χac is observed close to T for the [11̅0] orientation of the driving ac field; 2) a single peak is also seen close to 22 K for the field along [110]; and 3) peaks at both these temperatures are observed for the field applied along [100]. A detailed analysis of the ac and dc data unambiguously indicates that the peak near T is related to the paramagnetic-to-ferromagnetic phase transition, with the ferromagnetic domains nucleating with their easy axes aligned with the [11̅0] direction, providing a clear picture of uniaxial domain behavior near T . The peak near 22 K, on the other hand, is related to the onset of biaxial domain structure in (Ga,Mn)As induced by the competition between uniaxial and cubic anisotropy. More specifically, the ac susceptibility peak near TC involves 180° magnetization flips along the [11̅0] easy axis of the domains, while the peak near 22 K originates from magnetization wobbling between two biaxial easy axes separated by a small angle.

Field-free manipulation of magnetization alignments in a Fe/GaAs/GaMnAs multilayer by spin-orbit-induced magnetic fields

We investigate the process of selectively manipulating the magnetization alignment in magnetic layers in the Fe/GaAs/GaMnAs structure by current-induced spin-orbit (SO) magnetic field. The presence of such fields manifests itself through the hysteretic behavior of planar Hall resistance observed for two opposite currents as the magnetization in the structure switches directions. In the case of the Fe/GaAs/GaMnAs multilayer, hystereses are clearly observed when the magnetization switches direction in the GaMnAs layer, but are negligible when magnetization transitions occur in Fe. This difference in the effect of the SO-field in the two magnetic layers provides an opportunity to control the magnetization in one layer (in the presence case in GaMnAs) by a current, while the magnetization in the other layer (i.e., Fe) remains fixed. Owing to our ability to selectively control the magnetization in the GaMnAs layer, we are able to manipulate the relative spin configurations in our structure between collinear and non-collinear alignments simply by switching the current direction even in the absence of an external magnetic field.