Spectroscopy of Plasmon-Excitons in Semiconductor-Metal Nanostructures

The results of the theory considering mixed plasmon-excitonic modes and their spectroscopy are presented. The plasmon-excitons are formed owing to strong Coulomb coupling between quasi-two-dimensional excitons of a quantum well and dipole plasmons of nanoparticles. The effective polarizability associated with a nanoparticle is calculated in a self-consistent approximation taking into account the local field determined by in-layer dipole plasmons and their image charges due to the excitonic polarization of a near quantum well. The spectra of elastic scattering and specular reflection of light are investigated in cases of a single silver nanoparticle and a monolayer of such particles situated in close proximity to a quantum well GaAs/AlGaAs. The optical spectra show a two-peak structure with a deep and narrow dip in the resonant range of plasmon-excitons. Propagation of plasmon-excitonic polaritons is discussed for periodic superlattices whose unit cell consists of a quantum well and a layer of metal nanoparticles. The superradiance regime originating in the Bragg diffraction of plasmon-excitonic polaritons by the superlattice is investigated. It is shown that the broad spectrum of plasmonic reflection depending on the number of unit cells in a superlattice also has a narrow dip at the exciton frequency.

     

PLE spectra analysis of the sub-structure in the absorption spectra of CdSeS quantum dots

The semiconductor CdSeS quantum dots (QDs) embedded in glass are analysed by means of absorption spectra, photoluminescence (PL) spectra and photoluminescence excitation (PLE) spectra. The peaks of absorption spectra shift to lower energies with the size of QD increasing, which obviously shows a quantum-size effect. Using the PLE spectra, the physical origin of the lowest absorption peak is analysed. In PLE spectra, the lowest absorption peak can be deconvoluted into two peaks that stem from the transitions of 1S_3/2--1S_e and 2S_3/2--1S_e respectively. The measured energy difference between the two peaks is found to decrease with the size of QD increasing, which agrees well with the theoretical calculation for the two transitions. The luminescence peak of defect states is also analysed by PLE spectra. Two transitions are present in the PLE, which indicates that the transitions of 1S_3/2--1S_e and 2S_3/2--1S_e are responsible for the defect states luminescence.     

Resonant Raman scattering of optical phonons in self-assembled quantum dots

We have investigated the carrier relaxation mechanism in InGaAs/GaAs quantum dots by photoluminescence excitation (PLE) spectroscopy. Near-field scanning optical microscope successfully shows that a PLE resonance at a relaxation energy of 36 meV can be seen in all single-dot luminescence spectra, and thus can be attributed to resonant Raman scattering by a GaAs LO phonon to the excitonic ground state. In addition, a number of sharp resonances observed in single-dot PLE spectra can be identified as resonant Raman features due to localized phonons, which are observed in the conventional Raman spectrum. The results reveal the mechanism for the efficient relaxation of carriers observed in self-assembled quantum dots: the carriers can relax within the continuum states, and make transitions to the excitonic ground state by phonon emission.     

Excitonic surface polaritons in ZnTe

Excitonic surface polaritons are excited resonantly in ZnTe utilizing attenuated total reflection (ATR). Lineshape analyses of ATR and normal-incidence-reflection spectra yield the eigenenergies of excitonic surface and bulk polaritons. Comparison of ATR and reflection spectra with luminescence spectra invalidates a recently published attribution of luminescence maxima to excitonic surface polaritons.     

Optical properties of 1.3 μm room temperature emitting InAs quantum dots covered by In0.4Ga0.6As/GaAs hetero-capping layer

Room temperature 1.3 μm emitting InAs quantum dots (QDs) covered by an In_0.4Ga_0.6As/GaAs strain reducing layer (SRL) have been fabricated by solid source molecular beam epitaxy (SSMBE) using the Stranski–Krastanov growth mode. The sample used has been investigated by temperature and excitation power dependent photoluminescence (PL), photoluminescence excitation (PLE), and time resolved photoluminescence (TRPL) experiments. Three emission peaks are apparent in the low temperature PL spectrum. We have found, through PLE measurement, a single quantum dot ground state and the corresponding first excited state with relatively large energy spacing. This attribute has been confirmed by TRPL measurements which allow comparison of the dynamics of the ground state with that of the excited states. Optical transitions related to the InGaAs quantum well have been also identified. Over the whole temperature range, the PL intensity is found to exhibit an anomalous increase with increasing temperatures up to 100 K and then followed by a drop by three orders of magnitude. Carrier’s activation energy out of the quantum dots is found to be close to the energy difference between each two subsequent transition energies. PACS 68.65.Ac; 68.65.Hb; 78.67.Hc     

Picosecond spectroscopy of polaritons in anthracene crystals II. Luminescence

The low-temperature luminescence spectrum of anthracene crystals is investigated by applying simultaneous time and frequency resolution. The complicated kinetics of the emission in the polariton bottleneck region reflects directly the evolution and relaxation of the polariton distribution in the crystal. Three distinct relaxation stages are distinguished: (1) the ultrafast decay of initial vibronic excitations, mediated by optical phonons and resulting in a broad distribution of polaritons near the band bottom; (2) the formation of a narrow distribution of polaritons with a characteristic time of 30 ps, which is caused by scattering on acoustic phonons; (3) relaxation through the bottleneck region on a subnanosecond time scale. It is suggested that the polaritons immediately below the resonance frequency are responsible for the observed excitonic energy transfer in anthracene crystals.     

Dependence of the activation energies on the well width in CdTe/ZnTe strained single quantum wells

Photoluminescence (PL) measurements on the CdTe/ZnTe strained single quantum wells grown by using the molecular beam epitaxy technique showed that the sharp excitonic peaks corresponding to the transition from the first electronic subband to the first heavy-hole (E₁–HH₁) were shifted to lower energy with increasing well width. The (E₁–HH₁) interband transitions were calculated by using an envelope function approximation taking into account the strain effects, and the values were in reasonable agreement with those obtained from the (E₁–HH₁) excitonic transitions of the PL spectra. The activation energies of the confined electrons in the CdTe quantum well were obtained from the temperature-dependent PL spectra, and their values increased with increasing CdTe well width due to the quantum confinement effect. The present results can help to improve the understanding of the activation energies dependent on the CdTe well width in CdTe/ZnTe single quantum wells.     

Magneto-absorption in cylindrical quantum dots

The absorption of light in an ensemble of non-interacting cylindrical quantum dots in the presence of a magnetic field is discussed using a model consisting of dots with rectangular infinitely-high potential barriers. The ensemble’s absorption coefficient is calculated — as well as the threshold frequency of absorption — as a function of the applied magnetic field and the quantum dot size. Theoretical results are compared with experimental data on magneto-luminescence in an In_0.53Ga_0.47As/InP cylindrical quantum dot system. In addition, using a perturbation theory framework, the influence of excitonic effects on the behaviour of the electron-hole energetic spectrum of said system is discussed.     

磷化铟纳米晶的制备及光学性质研究

阐述了目前国内外的磷化铟纳米晶研究状况。用有机溶剂回流退火法制备出了磷化铟纳米晶，并通过XRD谱计算出平均粒径为55nm。喇曼光谱表明：由于纳米颗粒的量子尺寸效应, 2个散射峰都向低能量方向发生了较大的移动。UV VIS表明样品的吸收边相对于体块InP（970nm）发生了显著的蓝移，说明带隙变宽，表现出明显的量子尺寸效应。PLE谱在380nm时，PL谱峰在573nm时,相对于体块InP的红外区的荧光光谱发光峰发生了显著的蓝移，说明磷化铟纳米晶在光电子器件领域和非线性光学领域有非常好的应用前景。     

Experimental determination of additional boundary conditions for excitonic polaritons in CdS

By analyzing simultaneously measured transmission and reflection spectra of thin CdS crystals in the spectral region of excitonic polaritons, we succeded in determining the energy dependence of γ to be proportional to the group velocity dω/dk of the polaritons. Such a dependence can be explained by polariton scattering at charged impurities. With the help of this known energy dependence of the abc's it could be unambiguously shown that Pekar's assumption is the only one to explain all the experimental results.     

Resonance Raman scattering by excitonic polaritons in CuGaS2

Resonance Raman scattering by exciton polaritons in crystals of CuGaS₂ under excitation with the 4880 and 4765 Å lines of an Ar⁺ laser at 9 K is studied. Lines of one-and two-phonon scattering of excitonic polaritons are found and studied. It is shown that the 1LO and 2LO phonons are arranged in accordance with their energies as the Stokes shifts move farther away from the excitation energy.     

用巯基乙酸作稳定剂制备CdSe纳米晶的光学性质

以巯基乙酸为稳定剂制备了CdSe纳米晶，通过尺寸选择沉淀得到2nm到3nm之间不同尺寸的纳米晶，利用室温光吸收，光致发光（PL）和光致发光激发（PLE）谱来研究了CdSe纳米团簇的光学性质。紫外－可见吸收谱给了具有清晰激光特征的尖锐吸收边，这表明样品的尺寸分布很窄。光致发光研究表明，样品有两个发射带，一个具有较高能量位于吸收边，来自电子－空穴对从最低激发态能级弛豫后的辐射复合，另一个低能发射带归属于基质与纳米晶界面存在的俘获中心。PLE谱中有2个吸收带，分别是S－S和P－P跃迁。最后还给出了不同激发能量下的发光特性。     

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.     

Exciton polariton in an organic–inorganic multiple-quantum-well crystal (C4H9NH3)2PbBr4

Exciton polariton in an organic–inorganic multiple-quantum-well (MQW) single crystal (C₄H₉NH₃)₂PbBr₄ at low temperature has been investigated by photoluminescence excitation (PLE), reflection, and time-resolved photoluminescence measurements. Since (C₄H₉NH₃)₂PbBr₄ has ideal two-dimensional excitons with an extremely large oscillator strength and forms self-organized MQW with a very short well-period (d～10 Å), polaritonic coupling among excitons is strong and extends over a large number of wells. Therefore, observed MQW polariton features were the same as those of bulk polaritons. We have also investigated relaxation dynamics of the MQW polariton in the same framework as discussions on bulk polaritons.     

Excitonic polarons in quasi-two-dimensional structures

A theory of excitonic polarons in semiconductor quantum wells is presented. Using a unitary transformation, we have diagonalized the exciton-phonon interaction operator in a quasi-two-dimensional system partially and then calculated the ground-state energy of an excitonic polaron. We have numerically evaluated the energy gap shift and effective mass of an excitonic polaron. We have numerically evaluated the energy gap shift and effective mass of an excitonic polaron in GaAs-Al _x Ga_1–x As systems. The results obtained here indicate that the polaronic effect is significant in the case of the light hole excitons in quantum wells of small well widths.     

Combined effects of hydrostatic pressure and temperature on nonlinear properties of an exciton in a spherical quantum dot under the applied electric field

Within the framework of the effective-mass approximation, we have calculated the combined effects of hydrostatic pressure, temperature and applied electric field on an exciton confined in a typical GaAs/Ga_0.7Al_0.3As quantum dot. Several inputs of the confinement potential, hydrostatic pressure, temperature, and applied electric field have been considered. Our findings suggest that (1) the effect of the confinement strength is dominant over the electric field effect, (2) the oscillator strength is an increasing function of the hydrostatic pressure, (3) the absorption coefficients and energy difference depend strongly on the hydrostatic pressure but weakly on the temperature, (4) the absorption coefficients with considering excitonic effects are stronger than those without considering excitonic effects and the absorption peak will move to the right side induced by the electron-hole interaction, (5) the applied electric field may effect either the size or the position of absorption peaks of excitons.     

Two-photon echo method to determine the transverse relaxation time of excitonic molecules

A nonlinear optical method to determine the transverse relaxation time of excitonic molecules by means of two-photon echo is proposed. In the case of two-photon transition such as excitonic molecule one needs three pulses to obtain an echo signal. When the wave-vector and frequency of the three successive pulses are denoted by k₁,ω₁, k₂,ω₂ and k₃,ω₃, the two-photon echo can be observed in the direction of 4k₂-2k₁-k₃ with frequency 4ω₂-2ω₁-ω₃. Tuning both ω₁ and ω₂ to be two-photon resonant with excitonic molecule, we can satisfy the phase-matching condition rather easily for appropriate values of ω₃ due to the large dispersion of excitonic polaritons. From the correlation trace of the two-photon echo we can determine directly the transverse relaxation time of excitonic molecules.     

Optical absorptions of an exciton in a disc-like quantum dot under an electric field

An exciton in a disc-like quantum dot (QD) with the parabolic confinement, under applied electric field, is studied within the framework of the effective-mass approximation. Both the electric field and the confinement effects on the transition energy and the oscillator strength were investigated. Based on the computed energies and wave functions, the linear, the third-order nonlinear and the total optical absorption coefficients were also calculated. We found that the optical absorption coefficients with considering excitonic effects are stronger than those without considering excitonic effects and the absorption peak will move to the right side induced by the electron-hole interaction, which shows an excitonic effect blue-shift of the resonance in QDs. The applied electric field may affect either the size or the position of absorption peaks of excitons. However, the applied electric field may only affect the size of absorption peaks of an electron-hole pair without considering excitonic effects. It is very important to take excitonic effects into account when we study the optical absorption for disc-like QDs. We may observe the excitonic effect induced by the external electric field.     

A phenomenological model for optical properties of dielectric surfaces

A phenomenological model is proposed for the surfaces of dielectric or excitonic media. The reflection of the eleme$\text{n}$tary excitations is described in terms of a parameter of the form p = p₀exp(iφ). This describes a change of phase upon reflection and, with 0 ? P₀ ? 1, allows for surface roughness, which entails amplitude damping of the reflected excitation. The model is developed consistently with energy conservation, which plays a central role in this analysis. Combined with the idea of a dead layer this model reproduces the essential observed features of the normal incidence excitonic reflectance spectra without need to assume too large changes in the dead layer thickness.     

Time-resolved spectroscopy of excitonic transitions in ZnO/(Zn, Mg)O quantum wells

We report on the optical spectroscopy of a series of ZnO/(Zn, Mg)O quantum wells of different widths, using time-resolved photoluminescence. The samples were grown by molecular beam epitaxy on ZnO templates, themselves deposited on sapphire substrates. The barriers consist of Zn_0.78Mg_0.22O layers. The presence of large internal electric fields in these quantum wells results in a competition between quantum confinement and the quantum confined Stark effect as the quantum well width is varied. A transition energy lying 0.5 eV below the ZnO excitonic gap was observed for the widest of our wells. The PL spectra of the wide quantum wells were obtained using time-integrated photoluminescence, taking a great care with screening effects induced by their very slow dynamics. The effect of the built-in electric field on the excitonic properties was investigated. The excitonic fine structure is shown to depend strongly on the enhancement or suppression of the exchange interaction as a function of the quantum well width.