Room-temperature laser emission of ZnO nanowires explained by many-body theory

Are excitons involved in lasing in ZnO nanowires or not? Our recently developed and experimentally tested quantum many-body theory sheds new light on this question. We measured the laser thresholds and Fabry-Pérot laser modes for three radically different excitation schemes. The thresholds, photon energies, and mode spacings can all be explained by our theory, without invoking enhanced light-matter interaction, as is needed in an earlier excitonic model. Our conclusion is that lasing in ZnO nanowires at room temperature is not of excitonic nature, as is often thought, but instead is electron-hole plasma lasing.     

Condensation effects of excitons

The theory of the electronic excitations in a highly excited semiconductor is presented. The relaxation processes, the formation of excitons and excitonic molecules, the interaction among the various forms of electronic excitations, as well as their optical and thermodynamical properties are analyzed. At low temperatures one expects condensations into the quantum statistically degenerate phases of the excitonic molecules and of the electron-hole plasma. The physical properties of these low temperature phases are investigated. Possibilities and previous attempts to observe the Bose-Einstein condensation in excitonic systems are discussed critically. The experimental observations of the electron-hole liquid phase transition are reviewed.     

Optical properties of highly excited direct gap semiconductors

The electronic excitations in direct gap semiconductors interact strongly with the photon field. We discuss both the experimental and the theoretical aspects of the optical properties of these materials under strong optical excitation. We distinguish between intermediate excitation levels at which the electronic excitations form a dense system of excitons and excitonic molecules and very high excitation levels at which a degenerate electron-hole plasma occurs. The optical spectra of dense excitonic systems, which are mainly observed in copper halides and II–VI compounds, are shown to be determined mainly by the interaction processes between excitonic molecules, polaritons and free carriers. The optical properties of the electron-hole plasma, which has been observed in II–VI and especially in III–V compounds, can be understood only by taking into account many-body effects, such as dynamical screening of the Coulomb interactions, plasmon-assisted transitions and excitonic enhancement.     

From Si nanowires to porous silicon: the role of excitonic effects

We show that the electronic and optical properties of silicon nanowires, with different size and orientation, are dominated by important many-body effects. The electronic and excitonic gaps, calculated within first principles, agree with the available experimental data. Huge excitonic effects, which depend strongly on wire orientation and size, characterize the optical spectra. Modeling porous silicon as a collection of interacting nanowires, we find an absorption spectrum which is in very good agreement with experimental measurements only when the electron-hole interaction is included.     

Excitonic effects in solids described by time-dependent density-functional theory

Starting from the many-body Bethe-Salpeter equation we derive an exchange-correlation kernel f(xc) that reproduces excitonic effects in bulk materials within time-dependent density functional theory. The resulting f(xc) accounts for both self-energy corrections and the electron-hole interaction. It is static, nonlocal, and has a long-range Coulomb tail. Taking the example of bulk silicon, we show that the -alpha/q(2) divergency is crucial and can, in the case of continuum excitons, even be sufficient for reproducing the excitonic effects and yielding excellent agreement between the calculated and the experimental absorption spectrum.     

Nonequilibrium properties of electron-hole plasma in direct-gap semiconductors

The gain spectra of the electron-hole plasma recombination in CdS are investigated as a function of the excitation conditions and of the lattice temperature. From a lineshape analysis which includes such many-body effects as collision broadening, single-particle energy renormalization and excitonic enhancement, average plasma parameters are obtained. In contrast to the predictions of quasi-equilibrium theory, one finds that the electron-hole plasma does not reach a full thermal quasi-equilibrium in direct-gap materials because of the short lifetimes of the carriers. The nonequilibrium effects are shown to lead to the formation of electron-hole plasma density fluctuations. No well-defined coexistence region exists. The experimental results in the phase transition region can consistently be explained by theoretical treatments of this nonequilibrium phase transition.     

Excitons and electron-hole plasma in quasi-two-dimensional systems

A theoretical study of many-body effects in quasi-two-dimensional electron-hole systems is presented. The renormalized single-particle energies and the exciton binding energy are calculated as functions of the carrier density and temperature. A simple model for the nonlinear excitonic absorption and refraction is proposed.     

Terahertz signatures of the exciton formation dynamics in non-resonantly excited semiconductors

A microscopic theory for the induced terahertz (THz) absorption of semiconductors is applied to study the time-dependent system response after non-resonant optical excitation. The formation of excitonic populations from an interacting electron-hole plasma is analyzed and the characteristic THz signatures are computed. Good qualitative agreement with recent experiments is obtained.     

Effect of screening by two-dimensional charge carriers on the binding energy of excitonic states in GaAs/AlGaAs quantum wells

The spectrum of excitonic excited states in GaAs/AlGaAs quantum wells of different width is studied together with its change due to the screening of electron-hole interaction by two-dimensional electrons. The exciton binding energy decreases sharply with an increase in the concentration of two-dimensional electrons. The temperature dependence of screening parameters is studied for the ground and excited excitonic states down to ultralow temperatures T=50 mK.     

Picosecond studies of highly excited CdS

Results on picosecond luminescence and excite-and-probe transmission as well as transient grating measurements for highly excited CdS measured at a bath temperature of 5 K will be presented. The luminescence and optical gain both due to electron-hole plasma and excitonic molecule recombination are observed. The electron-hole plasma decays very fast by bimolecular recombination of electrons and holes in the plasma and diffusion of the carrier toward the low density regions, and transforms into excitons and excitonic molecules within 100–200 ps. The possibility of electron-hole liquid formation is definitely excluded. The exciton and excitonic molecule decay rather slowly and govern the optical properties for times longer than 200 ps.     

Indirect excitons and double electron-hole layers in a wide single GaAs/AlGaAs quantum well in a strong electric field

The recombination spectra of indirect excitons and double electron-hole layers in a wide single quantum well in an electric field are studied. It is found that electrons and holes in the wide well become spatially separated in a sufficiently strong electric field. This leads to a substantial reorganization of the radiative recombination spectrum and to a significant increase in the carrier lifetime. It is shown that the total charge of the electron-hole system can be changed by varying the photoexcitation frequency and the applied electric field, thus passing from the neutral case of indirect excitons to the case of charged double electron-hole layers. The concentration of excess carriers in the well is measured as a function of the electric field strength. The behavior of the excited states of indirect heavy-hole and light-hole excitions is studied for a neutral excitonic system in a strong electric field. It is shown that the electric-field dependences allow the excited states of indirect excitons with a light hole to be distinguished from the excited states with a heavy hole.     

Excitonic absorption above the Mott transition in Si

We present experimental evidence for the existence of excitonic states above the excitonic Mott transition in both highly doped and highly excited silicon. Previous limitations to resolve the fundamental absorption edge of Si at dense carrier plasmas are overcome employing a novel spatially and time-resolved spectroscopy. We show that the obtained density dependent excess absorption at 75 K represents an excitonic enhancement effect, which is attributed to persisting many-body interactions.     

激发态过程的多体理论方法

描述多电子体系的绝大部分参量可实验测量,如吸收光谱、发光光谱和激子效应等,都涉及电子激发态的正确描述。密度泛函理论(DFT)框架内的局域密度近似(LDA)作为第一性原理基态理论,即基于Kohn-Sham方程的解,是研究多粒子体系基态性质非常有力的工具。然而,体系激发态的第一性原理理论及其计算要比基态的理论计算复杂得多。关键问题在于描写基态和激发态时,粒子间的交换关联相互作用并不相同,而对于非均匀相互作用多粒子体系的交换关联能至今仍不清楚。不过,近年来关于激发态问题的研究,先后发展了许多描述电子激发态的理论,最重要的是基于准粒子概念和Green函数方程的多体微扰理论和含时间密度泛函理论(TDDFT)以及与此相关的描述电子-空穴相互作用的Bethe-Salpeter方程在凝聚态物理问题中的应用。其中最关键的物理量是粒子的自能算符Σ,它描述Hartree近似之外的交换和关联效应。虽然这些理论不可避免地也要引入某些近似,如对于Σ的一个好的近似就是Hedin的GW近似方法。对许多实际凝聚态体系的计算机模拟结果表明,GW近似是描述激发态问题相当成功的理论方法。将Hartree-Fock(HF)理论与LDA相结合,但采用非局域屏蔽交换代替HF方法中的局域非屏蔽交换相互作用,建立广义的KS方程(GKS),得到所谓屏蔽交换局域密度近似(sX-LDA)方法。我们在平面波自洽场方法PWscf程序包的基础上,发展了PW scf-sX-LDA方法,也是处理激发态问题及材料设计的有效方法。将评述激发态过程多体理论各种方法的发展和意义,讨论这些多体理论方法之间的联系和差异,并在此基础上介绍它们在解决半导体带带跃迁(或带隙偏小问题)、半导体及其微结构中的激子效应等重要领域的应用和成果。     

Picosecond luminescence spectroscopy of highly excited GaAs

Time resolved luminescence of highly excited GaAs is studied using a streak camera. We observe the Mott transition from the electron-hole plasma to the excitonic state. This transition is smooth and does not show a phase separation. The plasmon sideband of the electron-hole plasma emission is identified.     

Theory of elementary excitations and the metal-insulator transition of semiconductor surfaces

The microscopic theory of density and spin response of surface systems and its application to elementary excitations is discussed. Particular emphasis is placed on semiconductor surfaces, for which the often-used jellium approximation is not valid. The discussion is based on a solution of Maxwell's equations or, formally, of the Bethe-Salpeter equation for the two-particle Green's function of the surface system. This solution is achieved in a local wave function representation and takes density fluctuations on a microscopic scale (surface profile and local-field effects parallel to the surface) into account. Many-body effects of random-phase (RPA) and electron-hole type are included. The resulting spin and density response functions present a practical scheme for a microscopic calculation of surface elementary excitations in conducting as well as non-conducting solids. As examples, the conditions for the appearance of an electronic (charge- and spin-density) instability at the surface and the coupling of the resulting charge-density wave to the lattice are studied in detail.Results of quantitative calculations of the charge- and spin-density-response function of the Si(111) surface establish the importance of including both excitonic (electron-hole) and (RPA) local-field many-body interactions. In particular, they lead to an instability of the ideal paramagnetic surface with respect to spin-density waves (SDW) with wavelength corresponding to the observed (2 × 1) and (7 × 7) superstructures. Another example deals with an a-priori calculation of the phonons and the electron-phonon interaction of the same surface system. Various results of the theory such as phonon softening due to the coupling of the charge-density fluctuations to the lattice are summarized and general aspects of the importance of many-body effects for the a-priori determination of surface structures via elementary excitations are discussed.     

Ab initio calculation of optical spectra of liquids: many-body effects in the electronic excitations of water

We present ab initio calculations of the excited state properties of liquid water in the framework of many-body Green's function formalism. Snapshots taken from molecular dynamics simulations are used as input geometries to calculate electronic and optical spectra, and the results are averaged over the different configurations. The optical absorption spectra with the inclusion of excitonic effects are calculated by solving the Bethe-Salpeter equation. The insensitivity of screening effects to a particular configuration make these calculations feasible. The resulting spectra, which are strongly modified by many-body effects, are in good agreement with experiments.     

Fast initial decay of molecular excitations at insulator surfaces

We investigate the initial decay of electron-hole excitations in a molecular layer after adsorption on an insulator substrate surface. This is done within ab initio many-body perturbation theory by calculating the time propagation of excited two-particle states. For a CO monolayer adsorbed on the MgO(001) surface we find very fast decay processes with lifetimes that are about 5 times shorter than the transfer of single charge carriers. This is due to a strong coupling of the molecular excitations to charge-transfer-exciton states between the adlayer and the substrate.     

Frequency and density dependent radiative recombination processes in III–V semiconductor quantum wells and superlattices

In this paper we review the radiative recombination processes occurring in semiconductor quantum wells and superlattices under different excitation conditions. We consider processes whose radiative efficiency depends on the photogenerated density of elementary excitations and on the frequency of the exciting field, including luminescence induced by multiphoton absorption, exciton and biexciton radiative decay, luminescence arising from inelastic excitonic scattering, and electron-hole plasma recombination.

Semiconductor quantum wells are ideal systems for the investigation of radiative recombination processes at different carrier densities owing to the peculiar wavefunction confinement which enhances the optical non-linearities and the bistable behaviour of the crystal. Radiative recombination processes induced by multi-photon absorption processes can be studied by exciting the crystal in the transparency region under an intense photon flux. The application of this non-linear spectroscopy gives direct access to the excited excitonic states in the quantum wells owing to the symmetry properties and the selection rules for artificially layered semiconductor heterostructures.

Different radiative recombination processes can be selectively tuned at exciting photon energies resonant with real states or in the continuum of the conduction band depending on the actual density of photogenerated carriers. We define three density regimes in which different quasi-particles are responsible for the dominant radiative recombination mechanisms of the crystal: (i) The dilute boson gas regime, in which exciton density is lower than 10¹⁰ cm^-2. Under this condition the decay of free and bound excitons is the main radiative recombination channel in the crystal. (ii) The intermediate density range (n < 10¹¹ cm^-2) at which excitonic molecules (biexcitons) and inelastic excitonic scattering processes contribute with additional decay mechanisms to the characteristic luminescence spectra. (iii) The high density range (n ?10¹² cm^-2) where screening of the Coulomb interaction leads to exciton ionization. The optical transitions hence originate from the radiative decay of free-carriers in a dense electron-hole plasma.

The fundamental theoretical and experimental aspects of the radiative recombination processes are discussed with special attention to the GaAs/Al _x Ga_1-x As and Ga _x In_1-x As/Al _y In_1-y As materials systems. The experimental investigations of these effects are performed in the limit of intense exciting fields by tuning the density of photogenerated quasi-particles and the frequency of the exciting photons. Under these conditions the optical response of the quantum well strongly deviates from the well-known linear excitonic behaviour. The optical properties of the crystal are then no longer controlled by the transverse dielectric constant or by the first-order dielectric susceptibility. They are strongly affected by many-body interactions between the different species of photogenerated quasi-particles, resulting in dramatic changes of the emission properties of the semiconductor.

The systematic investigation of these radiative recombination processes allows us to selectively monitor the many-body induced changes in the linear and non-linear optical transitions involving quantized states of the quantum wells. The importance of these effects, belonging to the physics of highly excited semiconductors, lies in the possibility of achieving population inversion of states associated with different radiative recombination channels and strong optical non-linearities causing laser action and bistable behaviour of two-dimensional heterostructures, respectively.     

Absence of current-density-wave excitonic states

It is shown that certain conditions on the anomalous quasiaverages of electron-hole pairing are satisfied by all eigenstates of the hamiltonian. These conditions are imposed on approximate states with electron-hole pairing such as those in the Hartree-Fock theory of Halperin and Rice. In Hartree-Fock theory at least, no current-density-wave excitonic states exist.