LO phonon effective temperature in highly excited GaAs

We report results for measurements of the ratio of Stokes to anti-Stokes intensities in the LO phonon Raman line of GaAs excited with 1.06 μm radiation that are in conflict with data reported earlier by other workers. It is pointed out that these earlier data are inconsistent both with the model proposed to explain them and with an order-of-magnitude estimate for the density of LO phonons obtainable under the conditions of the experiment. Our data, where no dependence of the ratio of Stokes to anti-Stokes intensities upon peak incident flux is detectable, are consistent with the theory.     

CdSe量子点拉曼谱的共振效应研究

本文介绍了用共振拉曼光谱研究CdSe量子点材料的结果,认为拉曼峰是ZnSe和量子点界面模的叠加。指出当激发光能量逐渐离开ZnSe带隙时,共振减弱,ZnSe峰不再占主导,界面模的拉曼峰出现移动及变宽。     

CdSe/ZnS纳晶中相干电声耦合效应的二维电子光谱研究

Coherent exciton-phonon coupling in CdSe/ZnS nanocrystals have been investigated by temperature-dependent two-dimensional electronic spectroscopy (2DES) measurements. Benefiting from the ability of 2DES to dissect assembles in nanocrystal films, we have clearly identified experimental evidences of coherent coupling between exciton and phonon in CdSe/ZnS nanocrystals. In time domain, 2DES signals of excitonic transitions beat at a frequency resonant to a longitudinal optical phonon mode; in energy domain, phonon side bands are distinct at both Stokes and anti-Stokes sides. When temperature increases, phonon-induced exciton dephasing is observed with dramatic broadening of homogeneous linewidth. The results suggest exciton-phonon coupling is essential in elucidating the quantum dynamics of excitonic transitions in semiconductor nanocrystals.     

CdSe/ZnSe/ZnS多壳层结构量子点的制备与表征

展示了一种简捷的多壳层量子点合成路线。在含有过量Se源的CdSe体系中直接注入Zn源,"一步法"合成了CdSe/ZnSe量子点;进一步以CdSe/ZnSe为"核",表面外延生长ZnS壳层制备了核/壳/壳结构CdSe/ZnSe/ZnS量子点。相对于以往报道的多壳层结构量子点的制备方法,该方法通过减少壳层的生长步骤有效地简化了实验操作,缩短了实验周期,同时减少对原料的损耗。对量子点进行高温退火处理,能够大幅提高CdSe/ZnSe/ZnS量子点的发光量子产率。透射电镜、XRD以及光谱研究表明:所制备的量子点接近球形,核与壳层纳米晶均为闪锌矿结构,最终获得的CdSe/ZnSe/ZnS量子点的光致发光量子产率达到53％。为了实现量子点的表面生物功能化,通过巯基酸进行了表面配体交换修饰,使量子点表面具有水溶性的羧基功能团,并且能够维持较高的光致发光量子产率。     

Acoustic,optical, and interface phonons in BeTe/ZnSe superlattices

Raman scattering in a number of BeTe/ZnSe type-II superlattices which share no common cations or anions in the interfaces was studied. Folded acoustic phonons; LO phonons of the first, second, and third order in the ZnSe layers; and Kliewer-Fuchs-type electrostatic interface phonons were observed when excited in resonance with the direct exciton transition in the ZnSe layers. Nonresonant excitation produced LO phonons in the ZnSe and BeTe layers and a high-frequency mechanical interface mode, assigned tentatively to a local vibration of the interface Be-Se bond.     

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.     

Coherent anti-Stokes Raman scattering and normal anti-Stokes Raman scattering due to LO phonons in GaP using cw diode lasers

Coherent anti-Stokes Raman scattering (CARS) and normal anti-Stokes Raman scattering (NARS) have been measured in (001) GaP at room temperature due to the 403 cm⁻¹ LO phonons using a continuous wave (CW) 785.0 nm fixed-wavelength pump laser and a CW Stokes laser tunable in the 800-830 nm wavelength range. CARS measurements are normally made using pulsed lasers. The use of CW diode lasers allows a more accurate comparison between the measured and calculated values of the CARS signal. The pump and Stokes laser beams were linearly polarized perpendicular to each other, same as the pump and normal Stokes/anti-Stokes scattered light for the GaP sample used in this work. The pump and Stokes laser powers incident upon the GaP sample, located in the focal plane of a 20 mm effective focal length lens, were <20 and 50 mW, respectively. The diameter of the laser beams in the focal plane of the focusing lens was determined to 40±5 μm. The pump and Stokes laser beam intensities incident upon the 0.3 mm thick GaP sample were <2 and 5 kW cm², respectively. The powers of the CARS and NARS signals were measured using a Raman spectrometer. The signal output of the Raman spectrometer was calibrated using the pump laser and several neutral density filters. The Raman linewidth (full-width at half-maximum) of the LO phonons was determined to be 0.95±0.05 cm⁻¹, using the variation of the CARS signal with the wavelength of the Stokes laser. The measured powers of the CARS and NARS signals are about a factor of 5 and 1.5, respectively, smaller than those calculated from the corresponding theoretical expressions.     

Raman光激射器

本文从哈密顿量出发,导出描写受激Raman过程的方程式:Laser光、一级Stokes与反Stokes光及相干的声子场的耦合方程,并唯象地引入弛豫耗散。在分子属于远共振情形及比介电常数近似更高一级的近似下,分析了方程的性质。由平衡点稳定性的讨论给出了Raman光激射器的阈值,发现反Stokes激射光的产生并不要求附加的阈条件,即在受激Raman效应中,反Stokes光总是必然出现的。对于Raman光激射器诸工作点的性质及工作过程也作了进一步的讨论,发现在一定条件下,在强激射光源辐照下,存在着Stokes与反Stokes成分几乎各占一半的唯一的稳定平衡点(Raman光激射器的工作点)。文中也顺便讨论了声子弛豫所起的作用及有长寿命的声子时Raman光激射器的行为。     

Multiplasmon replicas of the emission lines of bound excitons in ZnSe crystals

This paper reports on the results of investigations into the cathodoluminescence spectra of ZnSe crystals grown from a vapor phase and annealed in a bismuth melt [ZnSe(Bi) crystals], as well as in a bismuth melt containing aluminum [ZnSe(Bi,Al) crystals], at a temperature of 1200 K for 120 h. The longitudinal optical (LO) phonon replicas of the emission lines of free excitons are dominant in the cathodoluminescence spectra of the samples subjected to annealing in the bismuth melt with subsequent quenching. The emission spectra of all the samples studied, including the initial crystals, contain series of I ₁ ^s,d -nLO lines of bound excitons. It is revealed that plasmon replicas are characteristic not only of the I ₁ ^s -nLO lines. A weak exciton-plasmon interaction manifests itself in the form of single-plasmon Stokes satellites of the I ₁ ^d -nLO spectral lines. A theory describing the multiphoton optical transitions of bound excitons with the participation of mixed plasmonphonon vibrational modes is proposed. This theory makes it possible to calculate the shape function of an emission spectrum without recourse to model concepts. The results of the theoretical calculations are in agreement with the experimental data.     

Double resonance Raman scattering of second-order Raman modes from an individual graphite whisker

Resonant Raman scattering of second-order Raman modes from an individual graphite whisker synthesized by a high-temperature heat-treatment method at a special pressure was discussed here. The dependence of phonon frequencies on the incoming laser light and the frequency difference between Stokes and anti-Stokes scattering show their origin from double resonance Raman scattering. Our results show that all the experimental results of second-order Raman modes in graphite whiskers, such as the excitation-energy dependence on the mode frequency, the frequency shift between a second-order Raman mode and its fundamentals, and the frequency discrepancy between Stokes and anti-Stokes components of a second-order Raman mode can be well understood by double resonance Raman scattering.     

New method to induce 2D–3D transition of strained CdSe/ZnSe layers

We present new growth conditions for growing high-quality CdSe/ZnSe quantum dots with photoluminescence emission measurable up to room temperature. The surface morphology is characterized in situ by Reflective High Energy Electron Diffraction (RHEED). The key point is the introduction of a new step in the growth process using amorphous selenium to induce a 2D–3D transition of a CdSe strained layer on ZnSe to form the dots. Optical characterizations by photoluminescence of CdSe/ZnSe quantum dots obtained that way, as well as X-ray diffraction results are also discussed here.     

Evidence for exciton binding at Ni impurity sites in ZnSe

A broad charge transfer band is observed in the photoluminescence excitation (PLE) spectrum of the 2.5 μ Ni²⁺ luminescence in ZnSe : Ni. This band lies above the highest energy d-d excitation bands and exhibits a ZPL at 1.8163 eV and LO(#38;0lambda;) phonon replicas at higher energy. In contrast, PLE spectra of Co²⁺ luminescence in ZnSe:Co contain only d-d excitation bands. The charge transfer band in ZnSe:Ni is interpreted as evidence for bound exciton formation at the Ni site. The recombination energy of this exciton is transferred efficiently to the excited d-band states of the Ni ion, leading to characteristic Ni²⁺d-d luminescence.     

Low-Temperature Anti-Stokes Luminescence in Zn1-xMgxSe Mixed Crystals

Investigations of photoluminescence and Raman scattering in the ternary Zn_1-xMg_xSe compounds at 4.2 K were performed both in the Stokes and anti-Stokes regions using cw laser excitation with various wavelengths within the transparency band of the crystals. The anti-Stokes luminescence was observed for the first time in the ternary Zn_1-xMg_xSe compounds. We have found variations in the shape and position of the Stokes and anti-Stokes luminescence bands with an increase in the band gap energy, which depends on magnesium content. We assume that the anti-Stokes emission is generated by two-step excitation via deep-level centers. It is shown that the low-temperature anti-Stokes photoluminescence can probe the spatial distribution profiles of impurities in the bulk of crystals.     

Noise correlations in a doubly-resonant atomic optical parametric oscillator

The simultaneous generations of bright Stokes and anti-Stokes fields are realized by using only one pump field in a Doppler-broadened atomic medium confined in an optical ring cavity. A vacuum-induced absorption phenomenon is also observed in such a system. By utilizing an external Fabry-Perot cavity to separate the Stokes and anti-Stokes fields, we investigate the noise correlation and anticorrelation properties between the Stokes, anti-Stokes, and the pump fields.     

CdSe/ZnSe核-壳结构纳米粒子合成新方法

报道用“一步”合成新方法制备了CdSe/ZnSe核-壳结构的发光纳米粒子.该方法是将锌的前驱体注入表面Se富集的CdSe发光纳米粒子溶液中,通过Zn²⁺与Se共价键结合,从而在CdSe发光纳米粒子的表面形成ZnSe壳.分别通过X射线粉末衍射、光电子能谱、透射电镜、紫外-可见吸收光谱和光致发光光谱,对核-壳结构的发光纳米粒子的结构及光学性质进行了表征.结果表明,以较宽带隙的ZnSe在较窄带隙的CdSe纳米粒子表面形成的壳层有效地钝化了CdSe纳米粒子的表面缺陷,明显地提高了室温下CdSe纳米粒子的光致发光效率.X射线粉末衍射表明随着Zn²⁺的不断注入,CdSe/ZnSe的衍射峰逐渐移向ZnSe衍射峰.光电子能谱数据显示,Zn2p的双峰分别位于1020,1040eV附近,通过与体材料ZnO相比,确定为Zn²⁺的光电子发射,说明Zn是以共价键形式存在于CdSe纳米粒子的表面.透射电镜照片显示纳米粒子具有良好的单分散性,核-壳结构的发光纳米粒子直径较CdSe核的直径明显增加.     

不同厚度CdSe阱层的表面上自组织CdSe量子点的发光性质

利用变温和变激发功率分别研究了不同厚度CdSe阱层的自组织CdSe量子点的发光。稳态变温光谱表明:低温下CdSe量子阱有很强的发光,高温猝灭,而其表面上的量子点发光可持续到室温,原因归结于量子点的三维量子尺寸限制效应;变激发功率光谱表明:量子点激子发光是典型的自由激子发光,且在功率增加时。宽阱层表面上的CdSe量子点有明显的带填充效应。通过比较不同CdSe阱层厚度的样品的发光,发现其表面上量子点的发光差异较大,这可以归结为阱层厚度不同导致应变弛豫的程度不同,直接决定了所形成量子点的大小与空间分布^[1]。     

Transition behavior from uncoupled to coupled multiple stacked CdSe/ZnSe self-assembled quantum-dot arrays

Transition behavior from uncoupled to coupled multiple stacked CdSe/ZnSe quantum-dot (QD) arrays grown by molecular beam epitaxy were investigated. Transmission electron microscopy showed that vertically stacked self-assembled CdSe QD arrays were embedded in the ZnSe barriers. The results for the photoluminescence (PL) data at 18 K demonstrated clearly that the transition behavior from uncoupled to coupled peaks depended on the ZnSe barrier thickness. The temperature-dependent PL measurements showed that the activation energy of the electrons confined in the CdSe QDs increased dramatically with decreasing ZnSe spacer layer thickness due to the strong coupling between CdSe/ZnSe QD arrays. The present observations can help improve understanding of the dependence of the coupling behavior and activation energy in CdSe/ZnSe QDs on the spacer layer thickness.     

ZnSe/ZnCdSe超晶格的共振拉曼散射特性

ＺｎＳｅ／ＺｎＣｄＳｅ超晶格的共振拉曼散射特性李文深池元斌＊李岩梅＊范希武申德振杨宝均王敬伯（中国科学院长春物理研究所，激发态物理开放实验室长春１３００２１）＊（吉林大学超硬材料国家重点实验室，长春１３００２３）ＲｅｓｏｎａｎｔＲａｍａｎＳｐｅｃｔｒ...     

Observation of stokes and anti-stokes vibrational sidebands in the optical emission spectrum of Eu atoms isolated in an argon matrix

The 4f⁶5d6s² → 4f⁷ 6s² emission spectrum of Eu atoms isolated in an argon matrix shows (a) zero-phonon lines and (b) Stokes vibrational sidebands due to resonance modes in the $\text{Ar}$: Eu phonon spectrum. In addition, unexpected anti-Stokes vibrational side bands are observed, which might be due to “hot luminescence”.     

Wavelength and time evolution of multiple stimulated Raman spectra in CCl4 excited by an intense picosecond laser pulse

By focussing a Nd³⁺ YAG laser beam or its second harmonic into liquid CCl₄, many rather narrow bands are generated, both on the Stokes and the anti-Stokes sides of the pump. The spectral interval between consecutive bands (or pump) ranges from 460 to 400 cm^-1. The time evolution of the bands shows that their life-times decrease steadily as their spectral distance to the pump increases.