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Transition metal dichalcogenide (TMD) monolayers (1L) in the 2H-phase are two-dimensional semiconductors with two valleys in their band structure that can be selectively populated using circularly polarized light. The choice of the substrate for monolayer TMDs is an essential factor for the optoelectronic properties and for achieving a high degree of valley polarization at room temperature (RT). In this work, we investigate the RT valley polarization of monolayer WS2 on different substrates. A degree of polarization of photoluminescence (PL) in excess of 27% is found from neutral excitons in 1L-WS2 on graphite at RT, under resonant excitation. Using chemical doping through photochlorination we modulate the polarization of the neutral exciton emission from 27% to 38% for 1L-WS2/graphite. We show that the valley polarization strongly depends on the interplay between doping and the choice of the supporting layer of TMDs. Time-resolved PL measurements, corroborated by a rate equation model accounting for the bright exciton population in the presence of a dark exciton reservoir support our findings. These results suggest a pathway towards engineering valley polarization and exciton lifetimes in TMDs, by controlling the carrier density and/or the dielectric environment at ambient conditions.

Atomically thin two-dimensional (2D) materials can be vertically stacked with van der Waals bonds, which enable interlayer coupling. In the particular case of transition metal dichalcogenide (TMD) bilayers, the relative direction between the two monolayers, coined as twist-angle, modifies the crystal symmetry and creates a superlattice with exciting properties. Here, we demonstrate an all-optical method for pixel-by-pixel mapping of the twist-angle with a resolution of 0.55(°), via polarization-resolved second harmonic generation (P-SHG) microscopy and we compare it with four-dimensional scanning transmission electron microscopy (4D STEM). It is found that the twist-angle imaging of WS2 bilayers, using the P-SHG technique is in excellent agreement with that obtained using electron diffraction. The main advantages of the optical approach are that the characterization is performed on the same substrate that the device is created on and that it is three orders of magnitude faster than the 4D STEM. We envisage that the optical P-SHG imaging could become the gold standard for the quality examination of TMD superlattice-based devices.

We use laser-scanning nonlinear imaging microscopy in atomically thin transition metal dichalcogenides (TMDs) to reveal information on the crystalline orientation distribution, within the 2D lattice. In particular, we perform polarization-resolved second-harmonic generation (PSHG) imaging in a stationary, raster-scanned chemical vapor deposition (CVD)-grown WS2 flake, in order to obtain with high precision a spatially resolved map of the orientation of its main crystallographic axis (armchair orientation). By fitting the experimental PSHG images of sub-micron resolution into a generalized nonlinear model, we are able to determine the armchair orientation for every pixel of the image of the 2D material, with further improved resolution. This pixel-wise mapping of the armchair orientation of 2D WS2 allows us to distinguish between different domains, reveal fine structure, and estimate the crystal orientation variability, which can be used as a unique crystal quality marker over large areas. The necessity and superiority of a polarization-resolved analysis over intensity-only measurements is experimentally demonstrated, while the advantages of PSHG over other techniques are analysed and discussed.

Degenerate minima in momentum space - valleys - provide an additional degree of freedom that can be used for information transport and storage. Notably, such minima naturally exist in the band structure of transition metal dichalcogenides (TMDs). When these atomically thin crystals interact with intense laser light, the second harmonic generated (SHG) field inherits special characteristics that reflect not only the broken inversion symmetry in real space, but also the valley anisotropy in reciprocal space. The latter is present whenever there exists a valley population imbalance (VPI) between the two valleys. In this work, it is shown that the temperature-induced changes of the SHG intensity dependence on the excitation fieldpolarization, is a unique fingerprint of VPI in TMDs. Analysis of such changes, in particular, enables the calculation of the valley-induced to intrinsic second order susceptibilities ratio. Unlike temperature-dependent photoluminescence (PL) measurements of valley polarization and coherence, the proposed polarization resolved SHG (PSHG) methodology is insensitive to the excitation field wavelength, an advantage that renders it ideal for monitoring VPI in large crystalline or stacked areas comprising different TMDs.

Tailoring the photoluminescence (PL) properties in two-dimensional (2D) molybdenum disulfide (MoS2) crystals using external factors is critical for its use in valleytronic, nanophotonic and optoelectronic applications. Although significant effort has been devoted towards enhancing or manipulating the excitonic emission in MoS2 monolayers, the excitonic emission in few-layers MoS2 has been largely unexplored. Here, we put forward a novel nano-heterojunction system, prepared with a non-lithographic process, to enhance and control such emission. It is based on the incorporation of few-layers MoS2 into a plasmonic silver metaphosphate glass (AgPO3) matrix. It is shown that, apart from the enhancement of the emission of both A- and B-excitons, the B-excitonic emission dominates the PL intensity. In particular, we observe an almost six-fold enhancement of the B-exciton emission, compared to control MoS2 samples. This enhanced PL at room temperature is attributed to an enhanced exciton–plasmon coupling and it is supported by ultrafast time-resolved spectroscopy that reveals plasmon-enhanced electron transfer that takes place in Ag nanoparticles-MoS2 nanoheterojunctions. Our results provide a great avenue to tailor the emission properties of few-layers MoS2, which could find application in emerging valleytronic devices working with B excitons.

Exploiting the valley degree of freedom to store and manipulate information provides a novel paradigm for future electronics. A monolayer transition-metal dichalcogenide (TMDC) with a broken inversion symmetry possesses two degenerate yet inequivalent valleys, which offers unique opportunities for valley control through the helicity of light. Lifting the valley degeneracy by Zeeman splitting has been demonstrated recently, which may enable valley control by a magnetic field. However, the realized valley splitting is modest (∼0.2 meV T-1). Here we show greatly enhanced valley spitting in monolayer WSe2, utilizing the interfacial magnetic exchange field (MEF) from a ferromagnetic EuS substrate. A valley splitting of 2.5 meV is demonstrated at 1 T by magnetoreflectance measurements and corresponds to an effective exchange field of ∼12 T. Moreover, the splitting follows the magnetization of EuS, a hallmark of the MEF. Utilizing the MEF of a magnetic insulator can induce magnetic order and valley and spin polarization in TMDCs, which may enable valleytronic and quantum-computing applications.

Stacked atomically thin transition metal dichalcogenides (TMDs) exhibit fundamentally new physical properties compared to those of the individual layers. The twist angle between the layers plays a crucial role in tuning these properties. Having a tool that provides high-resolution, large area mapping of the twist angle, would be of great importance in the characterization of such 2D structures. Here we use polarization-resolved second harmonic generation (P-SHG) imaging microscopy to rapidly map the twist angle in large areas of overlapping WS2 stacked layers. The robustness of our methodology lies in the combination of both intensity and polarization measurements of SHG in the overlapping region. This allows the accurate measurement and consequent pixel-by-pixel mapping of the twist angle in this area. For the specific case of 30° twist angle, P-SHG enables imaging of individual layers.

Stacked atomically thin transition metal dichalcogenides (TMDs) exhibit fundamentally new physical properties compared to those of the individual layers. The twist angle between the layers plays a crucial role in tuning these properties. Having a tool that provides highresolution, large area mapping of the twist angle, would be of great importance in the characterization of such 2D structures. Here we use polarization-resolved second harmonic generation (P-SHG) imaging microscopy to rapidly map the twist angle in large areas of overlapping WS2 stacked layers. The robustness of our methodology lies in the combination of both intensity and polarization measurements of SHG in the overlapping region. This allows the accurate measurement and consequent pixel-by-pixel mapping of the twist angle in this area. For the specific case of 30o twist angle, P-SHG enables imaging of individual layers., Comment: 18 pages, 7 Figures

The sufficient control of the carrier density of a single layer WS2 (1L-WS2) has been realized by the pulsed laser irradiation doping technique. Chlorine atoms are incorporated on the surface of the atomically thin lattice in a precursor gas atmosphere. In this work, we demonstrate spin-valley polarization tunability by more than 40% in 1L-WS2 on hBN via photochlorination. Polarization photoluminescence spectroscopy was performed in the temperature range from 4 K to 300 K. The decrease in circular polarization after the photochlorination treatment is attributed to the significant reduction of the active defect sites in 1L-WS2 and, consequently, to the increase in the non-radiative exciton lifetime. Ultrafast time-resolved transient absorption spectroscopy measurements support our findings. The above results indicate a useful approach of controlling the density of the active defect sites and the valley polarized light emission in doped monolayer crystal lattices.

Replacing the two sublattices of carbon atoms in graphene with transition metal atoms and chalcogenide dimers results in single layers of transition metal dichalcogenides (TMDCs). TMDCs are promising new materials for light and energy harvesting, transistors, sensors and quantum information processing. One way to access the distinctive functionality of these materials is via their optical selection rules. In particular, light with positive or negative helicity is absorbed differently, therefore, understanding the interaction of circularly polarized light with various TMDCs should enable future applications. Using the examples of MoS2 and WS2 we summarize some recent results that illustrate the potential of these materials. First, when optically excited with circularly polarized light, single layers of MoS2 can emit light with an appreciable polarization.Depolarization mechanisms can be subsequently explored by monitoring the polarization of emitted photoluminescence as a function of the excess energy supplied to the system. As the energy of the pumping light increases further from the emission channel, the emission quickly becomes depolarized. The dominant relaxation mechanism is identified as phonon-assisted intervalley scattering. In single layers of WS2 containing electron gas, the main emission channel is from negatively charged excitons, or trions. In the presence of a two-dimensional electron gas this trion emission is circularly polarized at zero magnetic field, even when excited with linearly polarized light. This spontaneous circular polarization of the trion has a linear dependence on magnetic field and can be attributed to the existence of a valley polarized state of the two-dimensional electron gas. (© 2015 WILEY-VCH Verlag GmbH &Co. KGaA, Weinheim)

© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Solution-processed organic–inorganic lead halide perovskite solar cells (PSCs) are considered as one of the most promising photovoltaic technologies thanks to both high performance and low manufacturing cost. However, a key challenge of this technology is the lack of ambient stability over prolonged solar irradiation under continuous operating conditions. In fact, only a few studies (carried out in inert atmosphere) already approach the industrial standards. Here, it is shown how the introduction of MoS2 flakes as a hole transport interlayer in inverted planar PSCs results in a power conversion efficiency (PCE) of ≈17%, overcoming the one of the standard reference devices. Furthermore, this approach allows the realization of ultrastable PSCs, stressed in ambient conditions and working at continuous maximum power point. In particular, the photovoltaic performances of the proposed PSCs represent the current state-of-the-art in terms of lifetime, retaining 80% of their initial performance after 568 h of continuous stress test, thus approaching the industrial stability standards. Moreover, it is further demonstrated the feasibility of this approach by fabricating large-area PSCs (0.5 cm2 active area) with MoS2 as the interlayer. These large-area PSCs show improved performance (i.e., PCE = 13.17%) when compared with the standard devices (PCE = 10.64%).

Bismuth ferrite (BiFeO3) is an important multiferroic oxide material because of its unique magnetic and ferroelectric properties. Here, we synthesize for the first time a highly ordered mesoporous BiFeO3 semiconductor using tartaric acid-assisted growth of the BiFeO3 compound inside the pores of a carbon template. Powder X-ray diffraction (XRD), transmission electron microscopy (TEM) and N2 physisorption measurements reveal that the template-free material possesses a three-dimensional hexagonal mesostructure with a large internal BET surface area (141 m2 g−1) and narrow sized pores (ca. 4 nm). Also, the pore walls comprise single-phase BiFeO3 nanocrystals according to the high-resolution TEM, electron diffraction and magnetic experiments. The mesoporous BiFeO3 shows high activity for the photocatalytic oxygen evolution reaction (OER) under UV-visible light (λ > 380 nm), affording an average oxygen evolution rate of 66 μmol h−1 g−1. We also show that the propensity of photogenerated holes for the OER can be significantly enhanced when 1 wt% Au nanoparticles are deposited on the BiFeO3 surface. The Au/BiFeO3 heterostructure exerts excellent OER activity (586 μmol h−1 g−1) and long-term cycling stability, raising the possibility for the design of effective and robust OER photocatalysts.

Monolayers of transition metal dichalcogenides (TMDs) are promising new materials for future 2D nanoelectronic systems.1 With their tunable direct gap in the visible range of the optical spectrum and high surface-to-volume ratio, these 2D semiconducting systems are ideal for field-effect transistors, photovoltaics, light-emitting diodes (LEDs), single-atom storage, molecule sensing, quantum-state metamaterials and electrocatalytic water splitting applications.2 Furthermore, the outstanding stretchability of 2D crystals is promising for strain engineering and related applications.

Single layers of WS2 are direct gap semiconductors with high photoluminescence (PL) yield holding great promise for emerging applications in optoelectronics. The spatial confinement in a 2D monolayer together with the weak dielectric screening lead to huge binding energies for the neutral excitons as well as other excitonic complexes, such as trions and biexcitons whose binding energies scale accordingly. Here, we report on the existence of biexcitons in mechanically exfoliated WS2 flakes from 78 K up to room temperature. Performing temperature and power dependent PL measurements, we identify the biexciton emission channel through the superlinear behavior of the integrated PL intensity as a function of the excitation power density. On the contrary, neutral and charged excitons show a linear to sublinear dependence in the whole temperature range. From the energy difference between the emission channels of the biexciton and neutral exciton, a biexciton binding energy of 65-70 meV is determined., 21 pages, 7 figures

We present theoretical calculations based on Density Functional Theory for MoS 2 nanoribbons. By studying nanoribbons with various widths, the energy for the (10) edge in single-layer MoS 2 is obtained. We calculate their electronic structure and use linear-response theory to obtain the dielectric function and other optoelectronic properties such as static relative permittivity, refractive index and reflectivity. We compare the dielectric properties of bulk (3D), single-layer (2D) and ribbons (quasi-1D) of MoS 2 to find, among other trends, that the dielectric constant is almost halved when the dimensionality is reduced by one. The static relative permittivity drops from 7.1 in 3D to 3.7 in 2D, which is consistent with experimental data, and down to 2.4 in the quasi-1D case. We discuss the edge conducting states in ribbon MoS 2 , an otherwise semiconducting material, as well as its dielectric properties as a function of the ribbon width.

Monolayer transition metal dichalcogenides, MX2 (M = Mo, W and X = S, Se), are direct-gap semiconductors with many interesting properties capable of producing an all-surface material applicable to sensing, single-atom storage and other quantum-based technologies. Here we report on the optical control of single layers of MX2 such that the photoluminescence (PL) is solely from the trion state. After trion isolation, changes in the Raman spectra were observed: there is a decrease in the intensity of the out of plane mode and an enhancement of the 2LA mode. The effect is reversible, and our results suggest that the changes of the strength of a particular excitonic state are due to surface interactions with ambient environment. In addition, spatial non-uniformity is probed by studying variations of strain and the PL emission as a function of position on our sample. The boundaries of mechanically exfoliated MX2 as well as boundaries intentionally created via fs laser ablation were investigated. The edges exhibit significant Raman shifts as well as remarkably enhanced PL emission compared to their respective central area. Finally, we probe the degree of circular polarization of the emitted PL as a function of the photo-excitation energy and temperature to elucidate spin-dependent inter- and intra-valley relaxation mechanisms. This work was supported by the FP7-REGPOT-2012-2013-1, under grant agreement 316165.

Exploiting the valley degree of freedom to store and manipulate information provides a novel paradigm for future electronics. A monolayer transition-metal dichalcogenide (TMDC) with a broken inversion symmetry possesses two degenerate yet inequivalent valleys, which offers unique opportunities for valley control through the helicity of light. Lifting the valley degeneracy by Zeeman splitting has been demonstrated recently, which may enable valley control by a magnetic field. However, the realized valley splitting is modest (∼0.2 meV T

Monolayers of Transition Metal Dichalcogenides (TMDs) are atomically thin two-dimensional crystals with attractive optoelectronic properties, which are promising for emerging applications in nanophotonics. Here, we report on the extraordinary spatial non-uniformity of the photoluminescence (PL) and strain properties of WS2 monolayers exfoliated from the natural crystal. Specifically, it is shown that the edges of such monolayers exhibit remarkably enhanced PL intensity compared to their respective central area. A comprehensive analysis of the recombination channels involved in the PL process demonstrates a spatial non-uniformity across the monolayer's surface and reflects on the non-uniformity of the intrinsic electron density across the monolayer. Auger electron imaging and spectroscopy studies complemented with PL measurements in different environments indicate that oxygen chemisorption and physisorption are the two fundamental mechanisms responsible for the observed non-uniformity. At the same time Raman spectroscopy analysis shows remarkable strain variations among the different locations of an individual monolayer, however such variations cannot be strictly correlated with the non-uniform PL emission. Our results shed light on the role of the chemical bonding on the competition between exciton complexes in monolayer WS2, providing a way of engineering new nanophotonic functions using WS2 monolayers. It is therefore envisaged that our findings could find diverse applications towards the development of TMDs-based optoelectronic devices., 23 pages, 12 figures

In this paper the authors review their work on spin-LEDs they have carried out. The general operating principles as well as the measuring techniques of spin-LEDs are discussed. Then particular examples of work on spin-LEDs are given using paramagnetic ZnMnSe and ferromagnetic Fe contacts are presented. Finally injection of spin polarized electrons into Si LEDs is described.

We used nonlinear laser scanning optical microscopy to study atomically thin transition metal dichalcogenides (TMDs) and revealed, with unprecedented resolution, the orientational distribution of armchair directions and their degree of organization in the two-dimensional (2D) crystal lattice. In particular, we carried out polarization-resolved second-harmonic generation (PSHG) imaging for monolayer WS2 and obtained, with high-precision, the orientation of the main crystallographic axis (armchair orientation) for each individual 120 × 120 nm2 pixel of the 2D crystal area. Such nanoscale resolution was realized by fitting the experimental PSHG images, obtained with sub-micron precision, to a new generalized theoretical model that accounts for the nonlinear optical properties of TMDs. This enabled us to distinguish between different crystallographic domains, locate boundaries and reveal fine structure. As a consequence, we can calculate the mean orientational average of armchair angle distributions in specific regions of interest and define the corresponding standard deviation as a figure-of-merit for the 2D crystal quality.

Microstructure and interfacial phase formation of CdCr2Se4 thin films deposited by molecular beam epitaxy on GaAs, Al0.1Ga0.9As and ZnSe/Al0.1Ga0.9As have been investigated with high-resolution transmission electron microscopy, fine-probe energy-dispersive spectroscopy and Z-contrast imaging. For CdCr2Se4 grown epitaxially on GaAs and/or Al0.1Ga0.9As, Cr tends to segregate to the interface forming either a layer enriched with Cr or trapezoidal-shaped Cr-rich precipitates. On ZnSe, CdCr2Se4 grows epitaxially at temperatures >300 °C, but when grown at 350 °C, the interface is quite rough or wavy. When the CdCr2Se4 is grown at 300 °C, the CdCr2Se4/ZnSe interface is more planar, but the CdCr2Se4 film is only epitaxial up to a thickness of about 5 nm, and then becomes polycrystalline as the thickness of the film increases. An interfacial phase, CdxZn1−xSe, forms at the CdCr2Se4/ZnSe interface, the thickness of which is determined by specific growth conditions.

The electron’s spin angular momentum is one of several alternative state variables under consideration on the International Technology Roadmap for Semiconductors (ITRS) for processing information in the fundamentally new ways that will be required beyond the ultimate scaling limits of silicon-based complementary metal–oxide–semiconductor technology1. Electrical injection/transport of spin-polarized carriers is prerequisite for developing such an approach2,3. Although significant progress has been realized in GaAs (ref. 4), little progress has been made in Si, despite its overwhelming dominance of the semiconductor industry. Here, we report successful injection of spin-polarized electrons from an iron film through an Al2O3 tunnel barrier into Si(001). The circular polarization of the electroluminescence resulting from radiative recombination in Si and in GaAs (in Si/AlGaAs/GaAs structures) tracks the Fe magnetization, confirming that these spin-polarized electrons originate from the Fe contact. The polarization reflects Fe majority spin. We determine a lower bound for the Si electron spin polarization of 10%, and obtain an estimate of ∼30% at 5 K, with significant polarization extending to at least 125 K. We further demonstrate spin transport across the Si/AlGaAs interface.

Monolayer transition metal dichalcogenides, MX2 (M = Mo, W and X = S, Se), are direct-gap semiconductors with some interesting properties. First, the low-dimensional hexagonal structure leads to two inequivalent K-points, K and K’, in the brillioun zone. Second, this valley index and spin are intrinsically coupled, and spin-dependent selection rules enable one to independently populate and interrogate a unique K valley with circularly polarized light. Here we probe the degree of circular polarization of the emitted photoluminescence as function of the photo-excitation energy and temperature to elucidate spin-dependent inter- and intra-valley relaxation mechanisms. Monolayer flakes of MoS2 and MoSe2 show a strong depolarization as the excitation energy is increased. However, WS2 maintains significant polarization for high excitation energies, even at room temperature when properly prepared. We discuss the behavior of the polarization in terms of various phonon assisted intervalley scattering processes. This work was supported by NRL and the NRL Nanoscience Institute

The effect of femtosecond laser irradiation on bulk and single-layer MoS2 on silicon oxide is studied. Optical, Field Emission Scanning Electron Microscopy (FESEM) and Raman microscopies were used to quantify the damage. The intensity of A1g and E2g1 vibrational modes was recorded as a function of the number of irradiation pulses. The observed behavior was attributed to laser-induced bond breaking and subsequent atoms removal due to electronic excitations. The single-pulse optical damage threshold was determined for the monolayer and bulk under 800nm and 1030nm pulsed laser irradiation and the role of two-photon versus one photon absorption effects is discussed., 14 pages, 4 figures, 24 references, PDF

Monolayer transition-metal dichalcogenides are direct gap semiconductors with great promise for optoelectronic devices. Although spatial correlation of electrons and holes plays a key role, there is little experimental information on such fundamental properties as exciton binding energies and band gaps. We report here an experimental determination of exciton excited states and binding energies for monolayer WS2 and WSe2. We observe peaks in the optical reflectivity/absorption spectra corresponding to the ground- and excited-state excitons (1s and 2s states). From these features, we determine lower bounds free of any model assumptions for the exciton binding energies as E2sA - E1sA of 0.83 eV and 0.79 eV for WS2 and WSe2, respectively, and for the corresponding band gaps Eg >= E2sA of 2.90 and 2.53 eV at 4K. Because the binding energies are large, the true band gap is substantially higher than the dominant spectral feature commonly observed with photoluminescence. This information is critical for emerging applications, and provides new insight into these novel monolayer semiconductors., 15 page manuscript, 5 figures, 10 page supplemental information

X-ray reflectivity and angular dependence of x-ray fluorescence (ADXRF) techniques have been employed for a quantitative study of the Te depth profile and structural changes in a series of CdS/CdTe heterojuctions annealed at various temperatures. The temperature dependence of surface roughening and Te migration is observed in both reflectivity and fluorescence experiments. Changes in the interface morphology and Te distribution are quantified by detailed analysis of the ADXRF data with the aid of reflectivity measurements. The results show that a large amount of Te up to 50% could migrate into the CdS layer and suggest that an extra layer of compounds can be formed near the CdS top surface. We have thus demonstrated that the x-ray reflectivity and ADXRF methods can be used as effective tools for nondestructive characterization of the concentration depth profile and interface morphology in layered structures on a nanometer scale.

Microstructural evolution has been investigated as a function of substrate temperature in Ge–4 at.%Cr films grown by molecular beam epitaxy (MBE), by employing transmission electron microscopy (TEM); the TEM results have been correlated to the magnetic properties. Magnetometry measurements show that samples grown at substrate temperatures of 200 °C and above are paramagnetic. Significantly different microstructures have been shown to evolve, depending on the substrate temperature ( T s ) during MBE growth. For T s =200 °C, the film consists of elongated rods, or “noodles” of the equilibrium Cr 11 Ge 19 phase. For T s =400 °C, a nanodispersion of metastable Cr 11 Ge 8 equiaxed precipitates form within the Ge-matrix. It is thus proposed that for T s =400 °C a supersaturated Ge–Cr solid-solution is initially formed from the vapor phase, followed by solid-state precipitation. At T s =200 °C, precipitation analogous to a cellular/discontinuous transformation results in the formation of cooperatively grown rod-like or noodle shaped microstructures.

Materials often exhibit fundamentally new phenomena in reduced dimensions that potentially lead to novel applications. This is true for single-layer, two-dimensional semiconductor crystals of transition-metal dichalcogenides, MX2 (M = Mo, W and X = S, Se). They exhibit direct bandgaps with energies in the visible region at the two non-equivalent valleys in the Brillouin zone. This makes them suitable for optoelectronic applications that range from light-emitting diodes to light harvesting and light sensors, and to valleytronics. Here, we report the results of a magnetoluminescence study of WS2 single-layer crystals in which the strong spin–orbit interaction additionally locks the valley and spin degrees of freedom. The recombination of the negatively charged exciton in the presence of a two-dimensional electron gas (2DEG) is found to be circularly polarized at zero magnetic field despite being excited with unpolarized light, which indicates that the existence of a valley polarized 2DEG is caused by valley and spin locking and strong electron–electron interactions.

We report efficient electrical injection of spin-polarized carriers from a non-lattice-matched magnetic contact into a semiconductor heterostructure. The semimagnetic semiconductor ${\mathrm{Zn}}_{1\ensuremath{-}x}{\mathrm{Mn}}_{x}\mathrm{Se}$ is used as a spin-injecting contact on a GaAs-based light-emitting diode. Spin-polarized electrons are electrically injected across the II-VI/III-V interface, where they radiatively recombine in a GaAs quantum well and emit circularly polarized light. An analysis of the optical polarization which includes quantum confinement effects yields a lower bound of 50% for the spin injection efficiency.

We report a reflectance-based optically detected resonance (ODR) study of neutral and negatively charged donors in ${\mathrm{G}\mathrm{a}\mathrm{A}\mathrm{s}/\mathrm{A}\mathrm{l}}_{x}{\mathrm{Ga}}_{1\ensuremath{-}x}\mathrm{As}$ quantum-well structures. The intensity of the ${e}_{1}{h}_{1}(1s)$ excitonic reflectance feature was modulated by resonant absorption of a monochromatic far-infrared (FIR) laser beam. An externally applied magnetic field was used to bring the internal transitions among various impurity states in resonance with the FIR photon energy. Predicted, but not previously reported, internal transitions of negatively charged donors were observed and were found to be in good agreement with theoretical calculations. This study establishes that the reflectance-based ODR technique is a sensitive tool for the investigation of donor states (both neutral and negatively charged) in semiconductor quantum wells.

Internal spin-singlet and spin-triplet transitions of charged excitons X- in magnetic fields in quantum wells have been studied experimentally and theoretically. The allowed X- transitions are photoionizing and exhibit a characteristic double-peak structure, which reflects the rich structure of the magnetoexciton continua in higher Landau levels (LL's). We discuss a novel exact selection rule, a hidden manifestation of translational invariance, that governs transitions of charged mobile complexes in a magnetic field., 4 pages, 2 figures, submitted to Physica E

We report on a magnetophotoluminescence study of an n-type modulation doped ${\mathrm{Al}}_{0.3}{\mathrm{Ga}}_{0.7}{\mathrm{As}\mathrm{ }(\mathrm{Si})/\mathrm{A}\mathrm{l}\mathrm{A}\mathrm{s}/\mathrm{G}\mathrm{a}\mathrm{A}\mathrm{s}/\mathrm{A}\mathrm{l}\mathrm{A}\mathrm{s}/\mathrm{A}\mathrm{l}}_{0.3}{\mathrm{Ga}}_{0.7}\mathrm{As}\mathrm{ }(\mathrm{Si})$ quantum-well structure in which a dense electron gas populates the AlAs X valleys. The interband transitions in this system are type II and exhibit GaAs and AlAs LO-phonon replicas. In the presence of a magnetic field applied perpendicular to the structure's layers luminescence features associated with the l=0 and l=1 Landau levels of the AlAs ${X}_{z}$ valleys were resolved. The slope $dE/dB$ of these transitions yield an in-plane effective mass ${m}^{*}$ of 0.44.

We have studied the band-edge photoluminescence from two n-type modulation-doped ZnSe/${\mathrm{Zn}}_{\mathrm{x}}$${\mathrm{Cd}}_{1\mathrm{\ensuremath{-}}\mathrm{x}}$Se single quantum-well structures with electron areal densities of 1.1\ifmmode\times\else\texttimes\fi{}${10}^{12}$ and 1.9\ifmmode\times\else\texttimes\fi{}${10}^{12}$${\mathrm{fcm}}^{\mathrm{\ensuremath{-}}2}$ in magnetic fields up to 30 T. The sharp excitonic transitions observed in undoped samples are replaced by a broad luminescence band. In a magnetic field, the luminescence spectra consist of distinct features associated with interband transitions between electrons occupying the conduction-band Landau levels and photoexcited holes. The energies of these transitions exhibit anomalies for even filling factors due to many-body effects.

We report electrical spin injection from an Fe contact into a (110)-oriented light-emitting diode (LED) structure, and compare results with data obtained from (001)-oriented structures to address the dependence of spin injection on interface and orientation. Fe∕AlGaAs∕GaAs LEDs were grown by molecular-beam epitaxy, and processed to form surface emitting structures. Electroluminescence results obtained using a reverse-biased Fe Schottky tunnel barrier injector show that a 13% electron spin polarization is achieved in the GaAs(110) quantum well due to injection across the Fe∕AlGaAs(110) interface. Analysis of the transport data indicates that tunneling is a significant transport mechanism at low temperatures. The temperature dependence of the spin polarization is similar to that of (001)-oriented spin LEDs, and is dominated by the GaAs electron spin lifetime.

We compare electrical spin injection from Fe films into identical GaAs-based light-emitting diodes (LEDs) using different tunnel barriers—a reverse-biased Fe/AlGaAs Schottky contact and an Fe/Al2O3 barrier. Both types of structures are formed in situ using a multichamber molecular-beam epitaxy system. A detailed analysis of the transport data confirms that tunneling occurs in each case. We find that the spin polarization achieved in the GaAs using the Al2O3 barrier is 40% (best case; 30% typical), but the electrical efficiency is significantly lower than that of the Fe Schottky contact.

We prepare single-layer WS2 films such that the photoluminescence is from either the neutral exciton or the negatively charged trion. While the neutral exciton emission has zero polarization at room temperature, we observe a room temperature optical polarization in excess of 40% for the trion. Using an applied gate voltage, we can modulate the electron density, and subsequently the polarization of the trion emission continuously from 20-40%. Both the polarization and the emission energy monotonically track the gate voltage with the emission energy increasing by 45 meV. We discuss the role electron capture by the exciton has on suppressing the intervalley scattering process.

The local environment surrounding magnetic impurity atoms and the host crystal structure of codoped TiO2 (TiO2:Co) nanocrystal ferromagnetic semiconductors have been investigated using the x-ray absorption fine structure and powder diffraction techniques. It has been found that the magnetic Co impurity atoms substitute for the Ti sites in an anataselike local environment through a structural phase transition when the material changes from an amorphous phase to a mixture of anatase and rutile crystal structures and then to a rutile structure as a result of increasing the anneal temperature. This result reveals an interesting feature that the local structure around magnetic impurity atoms can remain practically unchanged while the material undergoes drastic structural variations and a loss of room-temperature ferromagnetism.

ZnSe nanoparticles were synthesized by reacting vapors of (CH3)2Zn:N(C2H5)3 and H2Se, diluted in H2, in an opposed flow reactor operating at room temperature and 120 Torr. The particles were collected as random aggregates on silicon substrates and transmission electron microscopy (TEM) grids placed downstream of the reaction zone. Particle characterization using TEM and electron diffraction revealed the presence of polycrystalline nanoparticles with diameter of about 40 nm that were apparently formed from coagulation of smaller nanocrystals with characteristic size of about 4 nm. Raman spectra of the nanoparticles revealed an asymmetrically broadened feature associated with the LO phonon of ZnSe, indicating the presence of smaller single-crystalline grains.

Local structure and effective chemical valency of Mn atoms in Mn/GaAs digital alloys have been investigated using the x-ray absorption fine structure techniques. The samples were prepared by molecular-beam epitaxy with different thickness of GaAs layers separating the nominal Mn monolayers. Lattice constants of the digital alloys are found by x-ray diffraction to increase linearly in a very narrow range (about 0.3%) with the Mn/GaAs ratio in the samples. Our data show that Mn atoms in the nominal Mn monolayers actually combine with GaAs to form (Ga, Mn)As alloys with Mn atoms substituting for the Ga sites in GaAs. This result clearly rules out the possibility of dominant MnAs formation.

Grazing incidence x-ray scattering (GIXS) and x-ray diffraction (XRD) techniques have been employed to study the microscopic structure of magnetic digital layers of Mn/GaAs and MnGa/GaAs. Samples with various GaAs layer thickness (8 to 16 monolayers) and a half monolayer of either Mn or MnGa were prepared by low-temperature molecular-beam epitaxy. All digital alloys consist of 50 periods of magnetic layers separated by GaAs. High crystalline quality was verified and the periodicity and layer thickness were determined from the GIXS and XRD data. In order to investigate the magnetic properties, we performed magnetization measurements on all samples using superconducting quantum interference device magnetometry (SQUID).

An efficient electron spin-relaxation mechanism has been observed in InAs quantum dots (QDs) that manifests itself as a sharp drop in the circular polarization of the light emitted by Fe spin-light emitting diodes, which incorporate a single layer of InGaAs QDs, for a narrow range of magnetic fields around 5 T. The underlying mechanism occurs when the QDs are occupied by three-electron-hole pairs forming a tri-exciton (3X) and is a two-step process. The first step involves the spin flip of one of the three electrons mediated by the spin-orbit interaction; in the second step the 3X relaxes to its ground state via phonon emission. © 2011 American Physical Society.

Local structure around Ge in Si/Ge superlattices containing the “inverted hut” nanocrystals has been investigated by using the extended x-ray absorption fine structure (EXAFS) technique. In contrast to the usual nanometer-sized Ge “hut clusters” commonly grown on top of Si layers using the conventional Stranski–Krastanow self-organized growth mode, SiGe-alloy nanocrystals can be formed beneath the Ge wetting layer and grown into the Si layer in Si/Ge superlattices prepared in a low-temperature molecular beam epitaxy growth mode, and exhibit inverted hut nanocrystal structures regularly spaced along the Si/Ge interface. The EXAFS results obtained with varying Ge wetting layer thickness provide a direct evidence that intermixing of Ge and Si atoms takes place in a zone of about 1–3 monolayers on each side of the Si/Ge interface. The intermixing of constituent atoms allows a mechanism other than the usual formation of misfit dislocations to release the strain energy resulted from lattice mismatch between Si ...