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

Cavity quantum electrodynamics (QED) studies the interaction between a quantum emitter and a single radiation-field mode. When an atom is strongly coupled to a cavity mode, it is possible to realize important quantum information processing tasks, such as controlled coherent coupling and entanglement of distinguishable quantum systems. Realizing these tasks in the solid state is clearly desirable, and coupling semiconductor self-assembled quantum dots to monolithic optical cavities is a promising route to this end. However, validating the efficacy of quantum dots in quantum information applications requires confirmation of the quantum nature of the quantum-dot-cavity system in the strong-coupling regime. Here we find such confirmation by observing quantum correlations in photoluminescence from a photonic crystal nanocavity interacting with one, and only one, quantum dot located precisely at the cavity electric field maximum. When off-resonance, photon emission from the cavity mode and quantum-dot excitons is anticorrelated at the level of single quanta, proving that the mode is driven solely by the quantum dot despite an energy mismatch between cavity and excitons. When tuned to resonance, the exciton and cavity enter the strong-coupling regime of cavity QED and the quantum-dot exciton lifetime reduces by a factor of 145. The generated photon stream becomes antibunched, proving that the strongly coupled exciton/photon system is in the quantum regime. Our observations unequivocally show that quantum information tasks are achievable in solid-state cavity QED.

Quantum nature of a strongly coupled single quantum dot–cavity system

It is shown that the ordinary semiclassical theory of the absorption of light by exciton states is not completely satisfactory (in contrast to the case of absorption due to interband transitions). A more complete theory is developed. It is shown that excitons are approximate bosons, and, in interaction with the electromagnetic field, the exciton field plays the role of the classical polarization field. The eigenstates of the system of crystal and radiation field are mixtures of photons and excitons. The ordinary one-quantum optical lifetime of an excitation is infinite. Absorption occurs only when "three-body" processes are introduced. The theory includes "local field" effects, leading to the Lorentz local field correction when it is applicable. A Smakula equation for the oscillator strength in terms of the integrated absorption constant is derived.

a Quantum-Mechanical Theory of the Contribution of Excitons to the Complex Dielectric Constant of Crystals.

In the past decade, a two-dimensional matter-light system called the microcavity exciton-polariton has emerged as a new promising candidate of Bose-Einstein condensation BEC in solids. Many pieces of important evidence of polariton BEC have been established recently in GaAs and CdTe microcavities at the liquid helium temperature, opening a door to rich many-body physics inaccessible in experiments before. Technological progress also made polariton BEC at room temperatures promising. In parallel with experimental progresses, theoretical frameworks and numerical simulations are developed, and our understanding of the system has greatly advanced. In this article, recent experiments and corresponding theoretical pictures based on the Gross-Pitaevskii equations and the Boltzmann kinetic simulations for a finite-size BEC of polaritons are reviewed.

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Exciton-polariton Bose-Einstein condensation

The recent development of techniques to produce optical semiconductor cavities of very high quality has prepared the stage for observing cavity quantum-electrodynamic effects in solid-state materials. Among the most promising systems for these studies are semiconductor quantum dots inside photonic crystal, micropillar or microdisk resonators. We review the progress so far in obtaining true quantum-optical strong-coupling effects in semiconductors. We discuss the recent results on vacuum Rabi splitting with a single quantum dot, emphasizing the differences from quantum-well systems. Finally, we propose nonlinear tests for the true quantum limit and speculate about applications in quantum information devices.

Vacuum Rabi splitting in semiconductors

Comparisons are made of a classical and a quantum mechanical model of polariton energy splitting inside a microcavity in the linear excitation regime. Analytical expressions are obtained for the splitting energy as a function of temperature, detuning, and exciton-photon coupling constants. Experimental results are compared with theory, and agreements are found only if the effect of inhomogeneity is taken into account.

Microcavity exciton-polariton splitting in the linear regime.

Department of Physics and Astronomy, Northwestern University, Evanston, Illinois 60208-3112~Received 27 August 2001; revised manuscript received 2 November 2001; published 2 January 2002!We experimentally investigate the dynamic response of random lasers using picosecond optical pumping. Itis found that the turn-on time of a random laser is less than 100 ps. Above the lasing threshold, the emissionpulse is shortened dramatically. The dynamics of each individual lasing mode is different. Lasing starts andgets to a maximum value at different times. In addition, lasing in different modes lasts for different periods oftime, and the frequency of some lasing modes also shifts with time. Relaxation oscillations of lasing modes areobserved for a random laser. The theoretical simulations based on the semiclassical laser theory and ﬁnitedifferent time domain reproduce most of the experimental observations and provide an understanding of thedynamic response of a random laser.DOI: 10.1103/PhysRevB.65.041103 PACS number~s!: 42.25.Bs, 71.55.Jv, 42.55.2f

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Dynamic response and relaxation oscillations in random lasers

The optical modes in finite partially ordered arrays of dielectric particles are studied within the coupled dipole approach. It is shown that high-quality modes can be attained under conditions of small enough interparticle distance when the light-cone constraint is satisfied. We performed analytical and numerical investigations of these modes to determine their dependence on system size, dimensionality, and extent of disordering. The opportunity to use these modes to make high-performance random lasers is discussed.

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High-quality optical modes in low-dimensional arrays of nanoparticles: application to random lasers

We present experimental evidence of spontaneous buildup of coherent exciton polariton population in a microcavity, i.e., an exciton polariton laser. The laser phase transition was confirmed by the increased differential quantum efficiency and decreased linewidth of the lasing polariton mode due to onset of final-state stimulations and the decreased differential quantum efficiency of a nonlasing polariton due to onset of gain clamping at threshold. The exciton polariton laser is distinctly different from an optical laser because of its density-dependent scattering mechanism. The rate equations, taking into account phonon-assisted polariton emission and the polariton-reservoir exciton scattering rate, explain the measurement results well.

Observation of a laserlike transition in a microcavity exciton polariton system.

We have utilized hybrid zinc oxide∕silica microdisk lasers to sense volatile organic compounds, such as toluene and nitrobenzene. Nonspecific adsorption of these organic molecules onto the microdisk surface causes an increase in the disk refractive index, ultimately resulting in a redshift of the observed lasing wavelengths. The monitoring of these shifts provides the sensing modality. Microdisk lasers were found to respond rapidly and reversibly to the investigated chemicals demonstrating, in principal, the chemical and biological sensing capabilities of such devices.

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H. Cao

Papers

Microcavity exciton-polariton splitting in the linear regime.

Dynamic response and relaxation oscillations in random lasers

High-quality optical modes in low-dimensional arrays of nanoparticles: application to random lasers

Observation of a laserlike transition in a microcavity exciton polariton system.

Detection of chemical species using ultraviolet microdisk lasers