Resonant Raman scattering by strained and relaxed germanium quantum dots

This paper reports on the results of resonant Raman scattering investigations of the fundamental vibrations in Ge/Si structures with strained and relaxed germanium quantum dots. Self-assembled strained Ge/Si quantum dots are grown by molecular-beam epitaxy on Si(001) substrates. An ultrathin SiO₂ layer is grown prior to the deposition of a germanium layer with the aim of forming relaxed germanium quantum dots. The use of resonant Raman scattering (selective with respect to quantum dot size) made it possible to assign unambiguously the line observed in the vicinity of 300 cm^?1 to optical phonons confined in relaxed germanium quantum dots. The influence of confinement effects and mechanical stresses on the vibrational spectra of the structures with germanium quantum dots is analyzed.     

Relaxation of mechanical stresses in an array of Ge quantum dots obtained in Si

Raman scattering on optical phonons in Si/Ge/Si structures with Ge quantum dots grown by molecular beam epitaxy at low temperatures 200–300°C has been investigated. A pseudomorphic state of an array of Ge quantum dots to a Si matrix with an ideally sharp interface has been obtained. Features associated with the inelastic relaxation of mechanical stresses have been revealed in the Raman spectrum. Two mechanisms of stress relaxation are separated. It has been shown that the spectrum of the electronic states of the array differs significantly from the set of the discrete levels of a single quantum dot, because the relaxation is inhomogeneous.     

Raman scattering of Ge dot superlattices

Self-organised Ge dot superlattices grown by molecular beam epitaxy of Ge and Si layers utilizing Stranski-Krastanov growth mode were investigated by Raman spectroscopy. An average size of Ge quantum dots was obtained from transmission electron microscopy measurements. The strain and interdiffusion of Ge and Si atoms in Ge quantum dots were estimated from the analysis of frequency positions of optical phonons observed in the Raman spectra. Raman scattering by folded longitudinal acoustic phonons in the Ge dot superlattices was observed and explained using of elastic continuum theory. Received 25 January 2000     

Phonons in Ge/Si superlattices with Ge quantum dots

Ge/Si superlattices containing Ge quantum dots were prepared by molecular beam epitaxy and studied by resonant Raman scattering. It is shown that these structures possess vibrational properties of both two-and zero-dimensional objects. The folded acoustic phonons observed in the low-frequency region of the spectrum (up to 15th order) are typical for planar superlattices. The acoustic phonon lines overlap with a broad emission continuum that is due to the violation of the wave-vector conservation law by the quantum dots. An analysis of the Ge and Ge-Si optical phonons indicates that the Ge quantum dots are pseudoamorphous and that mixing of the Ge and Si atoms is insignificant. The longitudinal optical phonons undergo a low-frequency shift upon increasing laser excitation energy (2.54–2.71 eV) because of the confinement effect in small-sized quantum dots, which dominate resonant Raman scattering.     

Raman E 1, E 1+Δ1 resonance in unstrained germanium quantum dots

Raman scattering by optical phonons in unstrained Ge quantum dots obtained in GaAs/ZnSe/Ge/ZnSe structures was studied using molecular beam epitaxy. A shift in the E ₁, E ₁+Δ1 resonance energy due to the quantization of the spectrum of electron and hole states in quantum dots was observed. The properties observed were explained with the use of a simplest model of localization with allowance for the spectrum of Ge electron states.     

Optical phonons in Ge quantum dots obtained on Si(111)

The Raman light scattering from optical phonons of Ge quantum dots grown by molecular beam epitaxy on a Si(111) surface is studied. A series of Raman lines related to the quantization of phonon spectrum is observed. It is shown that phonon frequencies are adequately described in terms of the elastic properties and the dispersion of the optical phonons of bulk Ge. The strain experienced by the Ge quantum dots is estimated.     

The role of interdiffusion and spatial confinement in the formation of resonant raman spectra of Ge/Si(100) heterostructures with quantum-dot arrays

The phonon modes of self-assembled Ge/Si quantum dots grown by molecular-beam epitaxy in an apparatus integrated with a chamber of the scanning tunneling microscope into a single high-vacuum system are investigated using Raman spectroscopy. It is revealed that the Ge-Ge and Si-Ge vibrational modes are considerably enhanced upon excitation of excitons between the valence band Λ₃ and the conduction band Λ₁ (the E ₁ and E ₁ + Δ₁ transitions). This makes it possible to observe the Raman spectrum of very small amounts of germanium, such as one layer of quantum dots with a germanium layer thickness of ≈10 Å. The enhancement of these modes suggests a strong electron-phonon interaction of the vibrational modes with the E ₁ and E ₁ + Δ₁ excitons in the quantum dot. It is demonstrated that the frequency of the Ge-Ge mode decreases by 10 cm^?1 with a decrease in the thickness of the Ge layer from 10 to 6 Å due to the spatial-confinement effect. The optimum thickness of the Ge layer for which the size dispersion of quantum dots is minimum is determined.     

Resonant Raman scattering in nanostructures with InGaAs/AlAs quantum dots

Raman scattering by optical phonons in In_xGa_{1 ? x} As/AlAs nanostructures with quantum dots has been studied experimentally for compositions corresponding to x = 0.3?1 under out-resonance conditions. Features due to scattering by GaAs-and InAs-like optical phonons in quantum dots have been detected, and the phonon frequencies have been determined as a function of the dot composition. With increasing excitation energy, a red shift is observed in the frequency of the GaAs-like phonon in quantum dots, which testifies to Raman scattering selective by the size of quantum dots. Under resonant conditions, multiphonon light scattering by optical and interface phonons is observed up to the third order, including overtones of the first-order phonons of InGaAs and AlAs materials and their combinations.     

Ge dots on Si (1 1 1) and (1 0 0) surfaces with SiO2 coverage: Raman study

Germanium quantum dots formed on Si (1 1 1) and (1 0 0)-oriented surfaces coated with ultra-thin oxide layers are studied using Raman spectroscopy technique. Some structural properties (height, stoichiometry and mechanical stresses) of the dots were estimated from Raman data. For analysis of the experimental data, the Raman spectra of Ge nanoclusters containing some hundreds of Ge atoms were calculated numerically. The effects of the resonance enhancement of the intensity of Raman scattering in the Ge-nanoclusters–SiO₂–Si system were discussed. The influence of the lateral sizes of Ge nano-clusters on the frequencies of phonons localized in them was studied using numerical simulation. The influence of multi-layer growth on the structure of the Ge quantum dots was investigated.     

Raman E 1 and E 1 + Δ1 resonances in a system of unstrained germanium quantum dots

The positions and shapes of the Raman E ₁ and E ₁ + Δ₁ resonances of optical phonons are studied as functions of the size of unstrained germanium quantum dots. The quantum dots are grown by molecular-beam epitaxy in GaAs/ZnSe/Ge/ZnSe structures on GaAs(111) wafers. The positions of the E ₁ and E ₁ + Δ₁ resonances are found to shift by at most 0.3 eV. This shift is shown to be well described in terms of a cylindrical model using the quantization of the spectrum of bulk electron-hole states in germanium that form an exciton in a two-dimensional critical point. The fact that the peaks of the E ₁ and E ₁ + Δ₁ resonances appear separately has been detected for the first time, and it is related to the transformation of the interband density of states into a delta function because of spectrum quantization. An increase in the resonance amplitudes in quantum dots as compared to the bulk case is related to the degeneracy multiplicity of the exciton state in the (111) direction.     

Infrared spectroscopy of intraband transitions in Ge/Si quantum dot superlattices

We report the study of infrared spectroscopy of intraband transitions in Ge/Si quantum dot superlattices. The superlattices, which were grown on (001) oriented Si substrates by a solid source molecular beam epitaxy system, are composed mainly of 20 or 30 periods of Ge dot layers and Si spacer films. The structural properties of them and of the uncapped Ge dots grown on the surfaces of some of them were tested by cross-sectional transmission electron and atomic force microscopes, respectively. It is found that the Ge quantum dots have flat lens-like shapes. Infrared absorption signals peaking in the mid-infrared range were observed using Fourier transform infrared and Raman scattering spectroscopy techniques. Experimental and theoretical analysis suggests that the mid-infrared response be attributed to intraband transitions within the valence band of the Ge quantum dots in the superlattices. The fact that the intraband absorption is strongly polarized along the growth axis of the superlattices signifies that the Ge quantum dots with flat lens-like shapes perform as Ge/Si-based quantum wells. This study demonstrates the application potential of these kinds of Ge/Si quantum dot superlattices for developing mid-infrared photodetectors.     

Folded acoustic phonons in Si/Ge superlattices with Ge quantum dots

The spectra of Raman scattering by folded acoustic phonons in Si/Ge superlattices with pseudomorphic layers of Ge quantum dots (QDs) grown by low-temperature (T = 250°C) molecular beam epitaxy are studied. New features of the folded phonon lines related to the resonant enhancement and unusual intensity ratio of the doublet lines that cannot be explained by the existing theory have been observed. The observed modes are shown to be related to the vibrations localized to the QDs and induced by the folded phonons of the Si spacer layers. The calculations performed in the model of a one-dimensional chain of atoms have allowed the nature of the localization of acoustic phonons attributable to a modification of the phonon spectrum of a thin QD layer to be explained. The observed intensity ratio of the folded phonon doublet lines is caused by asymmetry of the relief of the QD layers.     

Optical phonon spectrum of germanium quantum dots

We have observed additional lines, shifted in both directions relative to the frequency of the bulk phonon of Ge, in the Raman scattering spectra from optical phonons in germanium quantum dots. The observed phonon modes are shown to be due to the straining of the quantum dots as a result of the lattice mismatch of the Ge and Si matrices. The observed frequency shifts, with allowance for optical-phonon localization effects, make it possible to determine the sizes of the regions with different strain states in the quantum dots. Pis’ma Zh. éksp. Teor. Fiz. 70, No. 4, 279–283 (25 August 1999)     

Intersubband cyclotron resonance of holes in strained Ge/GeSi(111) heterostructures with germanium wide quantum wells and cyclotron resonance of 1<Emphasis Type="Italic">L</Emphasis> electrons in GeSi layers

The submillimeter (?ω=0.5–5 meV) magnetoabsorption spectra of strained Ge/Ge_1?xSi_x(111) multilayer heterostructures with thick Ge layers (d_Ge=300–850 Å, d_GeSi≈200 Å, x≈0.1) are investigated at T=4.2 K upon band-gap optical excitation. It is revealed that the absorption spectra contain cyclotron resonance lines of 1L electrons localized in GeSi solid solution layers (unlike the previously studied structures with thin Ge layers as quantum wells for 3L electrons). The absorption spectra of the samples with thick Ge layers (d_Ge=800–850 Å) exhibit cyclotron resonance lines of holes due to transitions from the lower Landau levels in the first quantum-well subband to the Landau levels belonging to the third and fifth higher subbands.     

Raman scattering of light by optical phonons in Si-Ge-Si structures with quantum dots

Raman scattering of light by optical phonons in Si-Ge-Si structures with pseudomorphic germanium quantum dots has been investigated. Resonance amplification of the scattering intensity on E ₀ (Γ₇−Γ₈) transitions has been observed. It is shown that as a result of the formation of the layer of germanium quantum dots, the resonance energy is ∼0.3 eV higher than in the two-dimensional case. Pis’ma Zh. éksp. Teor. Fiz. 64, No. 3, 203–207 (10 August 1996)     

Self-assembling of Ge quantum dots in the CaF<Subscript>2</Subscript>/Ge/CaF<Subscript>2</Subscript>/Si heteroepitaxial system and the development of tunnel-resonance diode on its basis

A CaF₂/Ge/CaF₂/Si(111) heteroepitaxial structure with Ge quantum dots was grown by molecular-beam epitaxy. A negative differential conductivity and conductivity oscillations caused by resonant hole tunneling were observed at room temperature. The energy spacing between the levels in quantum dots, as determined from the oscillation period, is 40–50 meV depending on the Ge dot size.     

Photoconductivity of Si/Ge/SiO<Subscript>x</Subscript> and Si/Ge/Si structures with germanium quantum dots

A nonmonotonic dependence of the lateral photoconductivity (PC) on the interband light intensity is observed in Si/Ge/Si and Si/Ge/SiO_x structures with self-organized germanium quantum dots (QDs): in addition to a stepped increase in PC, a stepped decrease in PC is also observed. The effect of temperature and drive field on these features of the PC for both types of structures with a maximum nominal thickness of the Ge layer (N_Ge) is studied. The results obtained are discussed in the context of percolation theory for nonequilibrium carriers localized in different regions of the structure: electrons in the silicon matrix and holes in QDs.     

Hole states in artificial molecules formed by vertically coupled Ge/Si quantum dots

In the tight binding approximation, the spatial configuration of the ground state and the binding energy of a hole in a “diatomic” artificial molecule formed by vertically coupled Ge/Si(001) quantum dots are studied. The inhomogeneous spatial distribution of elastic strain arising in the medium due to the lattice mismatch between Ge and Si is taken into account. The strain is calculated using the valence-force-field model with a Keating interatomic potential. The formation of the hole states is shown to be determined by the competition of two processes: the appearance of a common hole due to the overlapping of “atomic” wavefunctions and the appearance of asymmetry in the potential energy of a hole in the two quantum dots because of the superposition of the elastic strain fields from the vertically aligned Ge nanoclusters. When the thickness of the Si layer separating the Ge dots (t _Si) is greater than 2.3 nm, the binding energy of a hole in the ground state of the two-dot system proves to be lower than the ionization energy of a single quantum dot because of the partial elastic stress relaxation due to the coupling of the quantum dots and due to the decrease in the depth of the potential well for holes. For the values of the parameter t _Si, an intermediate region is revealed, where the covalent molecular bond fails and the hole is localized in one of the two quantum dots, namely, in the dot characterized by the highest strain values.     

Resonant Raman scattering of discrete hole states in self-assembled Si/Ge quantum dots

We report the first resonant electronic Raman spectroscopy study of discrete electronic transitions within small p-doped self-assembled Si/Ge quantum dots (QDs). A heavy hole (hh) to light hole (lh) Raman transition with a dispersionless energy of 105 meV and a resonance energy of the hh states to virtually localised electrons at the direct band gap of 2.5 eV are observed. The hh–lh transition energy shifts to lower values with increasing annealing temperature due to significant intermixing of Si and Ge in the QDs. Structural parameters of the small Si/Ge dots have been determined and introduced into 6-band k·p valence band structure calculations. Both the value of the electronic Raman transition of localised holes as well as the resonance energy at the E₀ gap are in excellent agreement with the calculations.     

Resonant Raman scattering spectra in a ZnCdSe/ZnSe structure with a quantum well and open nanowires

Resonance Raman scattering (RS) spectra of a ZnCdSe/ZnSe sample containing a single quantum well and quantum well-based open nanowires were studied at T=300 K. The longitudinal optical (LO) phonons involved in the formation of the observed spectra of the quantum-well and nanowire regions differ noticeably in energy. The LO phonon energies in the structures under study were calculated taking into account the compositional effect (doping of Cd into ZnSe) and biaxial strain. When excited in the exciton resonance region, RS is shown to occur via free (extended) excitonic states with the involvement of LO phonons of the ZnCdSe strained layer with final wave vectors near the Brillouin zone center. When excited below the excitonic resonance in the ZnCdSe layer, resonance scattering via localized exciton states provides a noticeable contribution to the observed RS lines. Because of the finite size of a localized state, phonons with large wave vectors are involved in these scattering processes. The RS lines produced under excitation in the excitonic region of the thick barrier layers are due to scattering from the ZnSe barrier phonons.