In the past ten years we have witnessed a revival of, and subsequent rapid expansion in, the research on zinc oxide (ZnO) as a semiconductor. Being initially considered as a substrate for GaN and related alloys, the availability of high-quality large bulk single crystals, the strong luminescence demonstrated in optically pumped lasers and the prospects of gaining control over its electrical conductivity have led a large number of groups to turn their research for electronic and photonic devices to ZnO in its own right. The high electron mobility, high thermal conductivity, wide and direct band gap and large exciton binding energy make ZnO suitable for a wide range of devices, including transparent thin-film transistors, photodetectors, light-emitting diodes and laser diodes that operate in the blue and ultraviolet region of the spectrum. In spite of the recent rapid developments, controlling the electrical conductivity of ZnO has remained a major challenge. While a number of research groups have reported achieving p-type ZnO, there are still problems concerning the reproducibility of the results and the stability of the p-type conductivity. Even the cause of the commonly observed unintentional n-type conductivity in as-grown ZnO is still under debate. One approach to address these issues consists of growing high-quality single crystalline bulk and thin films in which the concentrations of impurities and intrinsic defects are controlled. In this review we discuss the status of ZnO as a semiconductor. We first discuss the growth of bulk and epitaxial films, growth conditions and their influence on the incorporation of native defects and impurities. We then present the theory of doping and native defects in ZnO based on density-functional calculations, discussing the stability and electronic structure of native point defects and impurities and their influence on the electrical conductivity and optical properties of ZnO. We pay special attention to the possible causes of the unintentional n-type conductivity, emphasize the role of impurities, critically review the current status of p-type doping and address possible routes to controlling the electrical conductivity in ZnO. Finally, we discuss band-gap engineering using MgZnO and CdZnO alloys.

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Fundamentals of zinc oxide as a semiconductor

The detection and measurement of gas concentrations using the characteristic optical absorption of the gas species is important for both understanding and monitoring a variety of phenomena from industrial processes to environmental change. This study reviews the field, covering several individual gas detection techniques including non-dispersive infrared, spectrophotometry, tunable diode laser spectroscopy and photoacoustic spectroscopy. We present the basis for each technique, recent developments in methods and performance limitations. The technology available to support this field, in terms of key components such as light sources and gas cells, has advanced rapidly in recent years and we discuss these new developments. Finally, we present a performance comparison of different techniques, taking data reported over the preceding decade, and draw conclusions from this benchmarking.

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Optical gas sensing: a review

Two complementary effects modify the GHz magnetization dynamics of nanoscale heterostructures of ferromagnetic and normal materials relative to those of the isolated magnetic constituents. On the one hand, a time-dependent ferromagnetic magnetization pumps a spin angular-momentum flow into adjacent materials and, on the other hand, spin angular momentum is transferred between ferromagnets by an applied bias, causing mutual torques on the magnetizations. These phenomena are manifestly nonlocal: they are governed by the entire spin-coherent region that is limited in size by spin-flip relaxation processes. This review presents recent progress in understanding the magnetization dynamics in ferromagnetic heterostructures from first principles, focusing on the role of spin pumping in layered structures. The main body of the theory is semiclassical and based on a mean-field Stoner or spin-density-functional picture, but quantum-size effects and the role of electron-electron correlations are also discussed. A growing number of experiments support the theoretical predictions. The formalism should be useful for understanding the physics and for engineering the characteristics of small devices such as magnetic random-access memory elements.

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Nonlocal magnetization dynamics in ferromagnetic heterostructures

The body of research on (III,Mn)V diluted magnetic semiconductors initiated during the 1990's has concentrated on three major fronts: i) the microscopic origins and fundamental physics of the ferromagnetism that occurs in these systems, ii) the materials science of growth and defects and iii) the development of spintronic devices with new functionalities. This article reviews the current status of the field, concentrating on the first two, more mature research directions. From the fundamental point of view, (Ga,Mn)As and several other (III,Mn)V DMSs are now regarded as textbook examples of a rare class of robust ferromagnets with dilute magnetic moments coupled by delocalized charge carriers. Both local moments and itinerant holes are provided by Mn, which makes the systems particularly favorable for realizing this unusual ordered state. Advances in growth and post-growth treatment techniques have played a central role in the field, often pushing the limits of dilute Mn moment densities and the uniformity and purity of materials far beyond those allowed by equilibrium thermodynamics. In (III,Mn)V compounds, material quality and magnetic properties are intimately connected. In the review we focus on the theoretical understanding of the origins of ferromagnetism and basic structural, magnetic, magneto-transport, and magneto-optical characteristics of simple (III,Mn)V epilayers, with the main emphasis on (Ga,Mn)As. The conclusions we arrive at are based on an extensive literature covering results of complementary ab initio and effective Hamiltonian computational techniques, and on comparisons between theory and experiment.

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Theory of ferromagnetic (III, Mn) V semiconductors

This review compiles results of experimental and theoretical studies on thin films and quantum structures of semiconductors with randomly distributed Mn ions, which exhibit spintronic functionalities associated with collective ferromagnetic spin ordering. Properties of p-type Mn-containing III-V as well as II-VI, IV-VI, V-2 -VI3, I-II-V, and elemental group IV semiconductors are described, paying particular attention to the most thoroughly investigated system (Ga, Mn)As that supports the hole-mediated ferromagnetic order up to 190 K for the net concentration of Mn spins below 10%. Multilayer structures showing efficient spin injection and spin-related magnetotransport properties as well as enabling magnetization manipulation by strain, light, electric fields, and spin currents are presented together with their impact on metal spintronics. The challenging interplay between magnetic and electronic properties in topologically trivial and nontrivial systems is described, emphasizing the entangled roles of disorder and correlation at the carrier localization boundary. Finally, the case of dilute magnetic insulators is considered, such as (Ga, Mn)N, where low-temperature spin ordering is driven by short-ranged superexchange that is ferromagnetic for certain charge states of magnetic impurities.

Dilute ferromagnetic semiconductors: Physics and spintronic structures

Wurtzite Zn1−xMgxO thin films with Mg contents between x=0 and x=0.37 were grown on c-plane sapphire substrates by plasma assisted molecular beam epitaxy using a MgO/ZnMgO buffer layer. The a-lattice parameter is independent from the Mg concentration, whereas the c-lattice parameter decreases from 5.20 A for x=0 to 5.17 A for x=0.37, indicating pseudomorphic growth. The near band edge photoluminescence shows a blueshift with increasing Mg concentration to an emission energy of 4.11 eV for x=0.37. Simultaneously, the energetic position of the deep defect luminescence shows a linear shift from 2.2 to 2.8 eV. Low temperature transmission measurements reveal strong excitonic features for the investigated composition range and alloy broadening effects for higher Mg contents. The Stokes shift as well as the Urbach energy is increased to values of up to 125 and 54 meV for x=0.37, respectively, indicating exciton localization due to alloy fluctuations.

Optical properties and structural characteristics of ZnMgO grown by plasma assisted molecular beam epitaxy

We report ferromagnetic resonance experiments on Ga1−xMnxAs thin films. For the dc magnetic field perpendicular to the sample plane, we observe up to eight distinct resonances, which we attribute to spin wave modes. To account for the spacing of the resonances, we infer a linear gradient in the magnetic properties, which is ascribed to a linear variation of the uniaxial magnetic anisotropy with film thickness. Values of D=(1±0.4)×10−9 Oe cm2 for the spin stiffness and JMnMn≈1 meV for the exchange integral between Mn spins are obtained.

Spin wave resonance in Ga1−xMnxAs

We show that upon exposure to a remote dc hydrogen plasma, the magnetic and electronic properties of the dilute magnetic semiconductor ${\mathrm{Ga}}_{1\ensuremath{-}x}{\mathrm{Mn}}_{x}\mathrm{As}$ change qualitatively. While the as-grown ${\mathrm{Ga}}_{1\ensuremath{-}x}{\mathrm{Mn}}_{x}\mathrm{As}$ thin films are ferromagnetic at temperatures $T\ensuremath{\lesssim}70\text{ }\mathrm{K}$, the samples are found to be paramagnetic after the hydrogenation, with a Brillouin-type magnetization curve even at $T=2\text{ }\mathrm{K}$. Comparing magnetization and electronic transport measurements, we conclude that the density of free holes $p$ is significantly reduced by the plasma process, while the density of Mn magnetic moments does not change.

Hydrogen Control of Ferromagnetism in a Dilute Magnetic Semiconductor

The characteristics of the excitonic absorption and emission around the fundamental bandgap of wurtzite MgxZn1−xO grown on c-plane sapphire substrates by plasma assisted molecular beam epitaxy with Mg contents between x = 0 and x = 0.23 are studied using spectroscopic ellipsometry and photoluminescence (PL) measurements. The ellipsometric data were analyzed using a multilayer model yielding the dielectric function (DF). The imaginary part of the DF for the alloys exhibits a pronounced feature which is attributed to exciton-phonon coupling (EPC) similar to the previously reported results for ZnO. Thus, in order to determine reliable transition energies, the spectral dependence is analyzed by a model which includes free excitonic lines, the exciton continuum, and the enhanced absorption due to EPC. A line shape analysis of the temperature-dependent PL spectra yielded in particular the emission-related free excitonic transition energies, which are compared to the results from the DF line-shape analysis. The ...

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Optical properties of MgZnO alloys: Excitons and exciton-phonon complexes

MEMS micro heater devices capable of long-term operation at temperatures up to 1000 °C are presented. The enhanced long-term stability has been achieved by employing antimony-doped tin oxide (SnO2:Sb) as a substitute for the conventionally used noble metal heater resistors. A detailed investigation of its high-temperature stability reveals that degradation is caused by out-diffusion of Sb impurities from the SnO2 film.

Thomas Wassner

Papers

Optical properties and structural characteristics of ZnMgO grown by plasma assisted molecular beam epitaxy

Spin wave resonance in Ga1−xMnxAs

Hydrogen Control of Ferromagnetism in a Dilute Magnetic Semiconductor

Optical properties of MgZnO alloys: Excitons and exciton-phonon complexes

SnO2:Sb – A new material for high-temperature MEMS heater applications: Performance and limitations