Hot carrier relaxation in InP and GaAs on a subpicosecond time scale

Hot carrier relaxation in InP and GaAs is investigated in a comparative study using three different time resolved optical techniques. At carrier densities between 10¹⁷ to 10¹⁸ cm⁻³ in both materials the relaxation is strongly influenced by carrier-carrier-scattering. Internal thermalization of electrons and holes occurs on a femtosecond time scale comparable to the duration of the excitation. The temperatures of electrons and holes, however, remain different on a time scale of picoseconds.     

ZnSe纳米晶材料的超快吸收谱

通过改进的溶剂热方法,以KBH4作为还原剂,在三乙胺溶液介质中制备了ZnSe纳米晶材料.与ZnSe体材料相比,其纳米材料的稳态吸收边发生了蓝移,而且纳米颗粒的尺寸越小,蓝移量越大,这是由于随着尺度减少而引起的量子限制效应增强造成的.对在溶液中的ZnSe纳米颗粒的超快吸收谱的研究表明,当纳米颗粒的平均尺寸为75nm时,电子-声子散射时间为8.74ps;当平均尺寸为45nm时,散射时间为2.77ps.随着纳米颗粒尺寸的减小,载流子与颗粒表面的非弹性碰撞几率增加,从而使载流子-声子耦合的强度增强,导致载流子-声子散射时间缩短.     

RBa_2Cu_3O_（7－δ）（R＝Y，Pr）薄膜中非平衡载流子的超快弛豫动力学

通过拟合ＹＢａ２Ｃｕ３Ｏ（７－δ）（δ＝０．１，０．４，０．８）和ＰｒＢａ２Ｃｕ３Ｏ７外延膜的室温飞秒瞬态反射谱，研究了其非平衡载流子的超快弛豫动力学，计算了电声耦合常数λ．发现随着氧含量的降低及用Ｐｒ替代Ｙ，Ｃｕ－Ｏ面上载流子浓度降低，非平衡载流子的弛豫时间增加而电声耦合常数明显减小．这表明电声耦合与载流子浓度的依赖关系，电声相互作用可能是一种实空间局域相互作用．     

Secondary phase formation in Zn‐rich Cu2ZnSnSe4‐based solar cells annealed in low pressure and temperature conditions

Zn‐rich Cu₂ZnSnSe₄ (CZTSe) films were prepared by a two‐step process consisting in the DC‐magnetron sputtering deposition of a metallic stack precursor followed by a reactive anneal under a Se + Sn containing atmosphere. Precursor composition and annealing temperature were varied in order to analyze their effects on the morphological, structural, and optoelectronic properties of the films and solar cell devices. Raman scattering measurements show the presence of ZnSe as the main secondary phase in the films, as well as the presence of SnSe at the back absorber region of the films processed with lower Zn‐excess values and annealing temperatures. The ZnSe phase is found to accumulate more towards the surface of the absorber in samples with lower Zn‐excess and lower temperature annealing, while increasing Zn‐excess and annealing temperature promote its aggregation towards the back absorber region of the devices. These measurements indicate a strong dependence of these process variables in secondary phase formation and accumulation. In a preliminary optimization of both the composition and reactive annealing process, a solar cell with 4.8% efficiency has been fabricated, and potential mechanisms limiting device efficiency in these devices are discussed. Copyright © 2014 John Wiley & Sons, Ltd.     

ZnSe／ZnS多量子阱光开关的优化设计

提出了ZnSe/ZnS多量子阱光开关的综合优化设计方案。根据Kronig-Penney模型对多量子阱结构进行优化,根据实验结果对多量子阱构成的非线性F-P进行了优化设计。     

飞秒时间分辨质谱技术在超快动力学中的应用进展

飞秒时间分辨质谱技术是飞秒抽运-探测技术与飞行时间质谱技术的结合。可以测得在不同抽运-探测时间延迟下,分子电子激发态电离或解离而来的离子质谱; 不同抽运-探测时间延迟下,质谱信号强弱的变化反映了激发态布居数的时态信息; 给出了分子激发态和里德堡态中准确的寿命信息、分子激发态势能面非绝热耦合信息以及分子过渡态信息。介绍了飞秒时间分辨质谱技术在分子激发态研究中的最新应用进展,以及在里德堡态解离、异构化、内转换、系间交叉等超快动力学过程研究中的最新进展。指出飞秒时间分辨质谱技术将在一些新现象的研究中发挥重要的作用。     

Energy exchange via electron-electron scattering in many-valley semiconductors

The theoretical treatment of electron-electron (e-e) scattering in semiconductor transport has always posed formidable problems, due to the long range and to the non-linearity of the interaction. Here we present a Monte Carlo study of the e-e interaction based on a molecular-dynamics approach. The full long range of the Coulomb interaction is accounted for, and no assumptions are needed on the screening process. This is particularly important when different valleys are involved, and a multi-component plasma has to be simulated. The Monte Carlo algorithm is applied to the study of the relaxation of photo-excited electrons in GaAs looking in particular at the energy exchange between electrons in different valleys. Such type of interaction has never been considered up to now in Monte Carlo simulations. The dependence of the e-e interaction on the electron density is discussed in detail. A comparison with a different approach, that treats the e-e scattering in k-space using a screened potential formulation, is also presented.     

Hot exciton effects and relaxation in coupled quantum wells

By studying photoluminescence and photoluminescence excitation in coupled quantum wells, we have studied the influence of the tunneling time on the relaxation of the photoexcited carriers. The ability to vary the coupling strength by the barrier thickness, allowed us to evidence hot exciton relaxation effects as well as resonant Raman scattering.     

Characteristics of deep levels in Al-doped ZnSe grown by molecular beam epitaxy

We investigated the characteristics of deep levels in heavily Al-doped ZnSe layers grown by molecular beam epitaxy, whose electron concentration is saturated. Low-temperature photoluminescence showed deep level emission around 2.25 eV, and its intensity increases with Al concentration. This deep-level is located at 0.55 eV above valence band maximum, implying a point defect such as a self-activated center, Al_ZnV_Zn. Deep-level transient spectroscopy was used to investigate non-radiative trap centers in Al-doped ZnSe layers, and showed the presence of two electron trap centers at depths of 0.16 and 0.80 eV below conduction band minimum, with the electron capture cross-sections of 810⁻¹² and 1×10⁻⁷ cm², respectively. It is suggested the carrier compensation in heavily Al-doped ZnSe layers be ascribed to the deep levels.     

ZnSe/ZnS quantum dots as emitting material in blue QD-LEDs with narrow emission peak and wavelength tunability

Quantum dots are a highly attractive class of materials for the use in light-emitting devices, since they allow high color purity, facile tunability and solution-processing methods. Here, zinc selenide QDs are investigated for their suitability as emissive material in cadmium-free blue QD-LEDs. By adjusting the stoichiometry in the synthesis the emission wavelength can be tuned in the range of 390–435 nm. For the assembly of the QD-LED, the device setup was adjusted to the low-lying ZnSe valence band energy by choosing a suitable hole-transport material. A first promising QD-LED result is achieved showing the characteristic narrow QD emission peak with a luminance of 25 cd/m².     

半导体纳米颗粒载流子的超快弛豫过程

分析了纳米颗粒的能级结构,建立了载流子弛豫的简化模型,运用数值模拟方法讨论了激发密度、表面态密度及俘获态电子的弛豫率对弛豫过程的影响。讨论结果表明,激发密度的增大及表面态的减少都会导致表面态上电子的饱和,使导带上出现电子的积累,导带电子寿命增大;深俘获态电子的弛豫是影响材料响应速度的主要因素。最后应用此模型对近红外泵浦探测实验的结果进行分析,表明模型可望在实验结果分析上得到应用。     

Hot electron energy relaxation via acoustic phonon emission in GaAs/Al0.24Ga0.76As single and multiple quantum wells

The energy relaxation associated with acoustic phonons has been investigated in a series of modulation doped GaAs/AlGaAs single and multiple quantum wells grown by molecular beam epitaxy, using the hot electron Shubnikov — de Haas effect. The power loss is shown to be proportional to (T_e² − T_L²) for electron temperatures 2.2K < T_e < 8K and proportional to (T_e³ − T_L³) for 8K < T_e < 20K. The energy loss rates due to acoustic phonon scattering via both deformation potential coupling and piezoelectric coupling have been calculated. The total energy loss rate as a function of electron temperature is compared with the experimental results. Good agreement is obtained for 2.2K < T_e < 8K. Above 8K the energy loss rate is seen to rise above the predicted values, indicating the onset of an extra energy relaxation mechanism. The application of a high electric field (E = 3kV/cm) at low lattice temperatures is shown to induce persistent parallel conduction and a subsequent reduction of the low field well mobility.     

光合作用PSII Chl分子传能超快光谱学

利用ICCD皮秒、飞秒扫描成像和飞秒时间分辨光谱装置实验研究了高等植物捕光天线LHCⅡ三聚体和PSⅡ颗粒复合物及PSⅡ核心复合物的超快光谱动力学,经过吸收光谱和发射光谱分析,确定在LHCⅡ三聚体中至少存在7种Chl分子光谱特性,它们是:Chlb653/656658.7、Chla662。0665。2、Chla/b670/671671.6、Chla675.0677.1、Chla680/681682.9、Chla685689.1和Chla695.0695.6。采用光强103光子/cm2/脉冲激励浓度为30μg/ml的捕光天线LHCⅡ三聚体,在650nm到705nm谱段逐点探测分析处理,产生了两组短寿命组分210fs、520fs和5.2ps、36.7ps及两个长寿命组分1.8ns、2ns。最快的三个寿命210fs、520fs和5.2ps反映了三聚体Chlb分子向Chla分子的激发能传递过程;寿命36.7ps反映了Chla分子向相邻单体Chla分子的激发能传递过程;最长的两个寿命1.8ns和2ns是在三聚体中Chla分子通过中间体Chla分子辐射荧光,分别跃迁回基态的过程。获得的六个寿命组分有把激发能传递时间与Chla/b分子发射光谱相结合的特点。经拟合处理解析PSⅡ颗粒复合物光谱,得到三个组分谱,其峰值分别为686.8nm、692.2nm和694.9nm,与LHCⅡ比较分析,说明天然构型的PSⅡ有很强的吸收光能和有效传递光能的本领、PSⅡ核心复合物的核心天线CP43和CP47,各自含有三种不同状态     

光合作用PSⅡ Chl分子传能超快光谱学

利用ICCD皮秒，飞秒扫描成像和飞秒时间分辨光谱装置实验研究了高等植物捕光天线LHCⅡ三聚体和PSⅡ聚粒复合物及PSⅡ核心复合物的超快光谱动力学。经过吸收光谱和发射光谱分析。确定在LHCⅡ三聚体中至少存在7种Chl分子光谱特性，它们是：Chlb653/656^658.7，Chla662.0^665.2,Chla/b670/671^671.6,Chla675.0^677.1,Chla680/681^682.9,Chla685^689.1和Chla695.0^695.6。采用光强10^13光子/cm^2/脉冲激励浓度为30μg/ml的捕光天线LHCⅡ三聚体，在650nm到705nm谱段逐点探测分析处理，产生了两组短寿命组分210fs,520fs和5.2ps,36.7ps及两个长寿命组分1.8ns,2ns。最快的三个寿命210fs,520fs和5.2ps反映了三聚体Chlb分子向Chla分子的激发能传递过程；寿命36.7ps反映了Chla分子向相邻单体Chla分子的激发能传递过程；最长的两个寿命1.8ns和2ns是在三聚体中Chla分子通过中间体Chla分子辐射荧光，分别跃迁回基态的过程，获得的六个寿命组分有把激发能传递时间与Chla/b分子发射光谱相结合的特点，经拟合处理解析PSⅡ颗粒复合物光谱，得到三个组分谱，其峰值分别为686.8nm,692.2nm和694.9nm，与LHCⅡ比较分析，说明天然构型的PSⅡ有很强的吸收光能和有效传递光能的本领，PSⅡ核心复合物的核心天线CP43和CP47，各自含有三种不同状态的Chla分子，CP43有Chla660^661,Chla669^670,Chla682^686,CP47有Chla660^661,Chla669^670,Chla680^681。     

Direct and Indirect Exciton Dynamics in Few‐Layered ReS2 Revealed by Photoluminescence and Pump‐Probe Spectroscopy

Atomically thin‐layered ReS₂ with a distorted 1T structure has attracted attention because of its intriguing optical and electronic properties. Here, the direct and indirect exciton dynamics of a three‐layered ReS₂ is investigated by polarization‐resolved transient photoluminescence (PL) and ultrafast pump‐probe spectroscopy. The various time scales of the decay signals of the time‐resolved PL (<10 ps), with monitoring of the populations of electron–hole pairs (exciton), and the transient differential reflectance (≈1 and 100 ps), with monitoring of the populations of electrons and/or holes in the excited states, are observed. These results reveal the characteristic exciton dynamics: rapid relaxation of direct excitons (electron–hole pairs) and slow relaxation of the momentum‐mismatched indirect excitons accompanied by a one‐phonon emission process. These findings provide important information regarding the indirect bandgap nature of few‐layered ReS₂ and its characteristic exciton dynamics, boosting the understanding of the novel electronic and optical properties of atomically thin‐layered ReS₂.     

Band‐Edge Exciton Fine Structure and Exciton Recombination Dynamics in Single Crystals of Layered Hybrid Perovskites

2D perovskite materials have recently reattracted intense research interest for applications in photovoltaics and optoelectronics. As a consequence of the dielectric and quantum confinement effect, they show strongly bound and stable excitons at room temperature. Here, the band‐edge exciton fine structure and in particular its exciton and biexciton dynamics in high quality crystals of (PEA)₂PbI₄ are investigated. A comparison of bulk and surface exciton lifetimes yields a room temperature surface recombination velocity of 2 × 10³ cm s^?1 and an intrinsic lifetime of 185 ns. Biexciton emission is evidenced at room temperature, with a binding energy of ≈45 meV and a lifetime of 80 ps. At low temperature, exciton state splitting is observed, which is caused by the electron–hole exchange interaction. Transient photoluminescence resolves the low‐lying dark exciton state, with a bright/dark splitting energy estimated to be 10 meV. This work contributes to the understanding of the complex scenario of the elementary photoexcitations in 2D perovskites.     

Investigation of carrier relaxation dynamics in single CdSe/ZnSe self-organized quantum dot by time-resolved micro-photoluminescence

We have investigated carrier relaxation dynamics in single CdSe/ZnSe quantum dot (QD) by time-resolved micro-photoluminescence (PL). The discrete sharp lines, originated from individual QD states, exhibit various rise and decay time constants. The decay times of the sharp lines from ground states and excited states are estimated to be 700≈800 psec and 400≈500 psec, respectively, and the rise times of the ground states become longer compared with those of the excited states. There results are in contrast to successive change of the rise and decay times observed in time-resolved macro-PL with varying the detection wave-length. The quasi-continuum higher states with much shorter decay times are clearly observed over the discrete states of the QDs.     

Evaluation of Zn{N[Si(CH3)3]2}2 as ap-type dopant in OMVPE growth of ZnSe

We have grown nominally undoped ZnSe on GaAs from the precursors H₂Se and Et₂Zn. Replacement of Et₂Zn by Zn[N(TMS)₂]₂ produced crystalline ZnSe of a lesser quality. Data indicate incorporation of nitrogen into the films when Et₂Zn is utilized as the main zinc source with Zn[N(TMS)₂]₂ being introduced at dopant levels. Characterization techniques employed include NMR, XRD, SIMS, SEM, PL, RGA, GC/MS, and Raman spectroscopy.     

Conformational Freedom-Enhanced Optomechanical Energy Conversion Efficiency in Bulk Azo-Polyimides

Azobenzene-doped glassy polyimides (azo-polyimides) offer some of the most efficient optomechanical power densities to date rivaling electrostrictive polymers. Despite such potential attributes, the optomechanical efficiency remains low in comparison to other smart materials. Using high-fidelity coarse-grained molecular dynamics simulations, the authors reconcile both experimental and theoretical challenges to understand the limiting factors for the optomechanical conversion in photostrictive polymers. Interestingly, the ideal optomechanical efficiency of 10–24% for a single-chain azo-imide monomer predicted here is equal to or a little higher than experimental reports, suggesting experimental design space. The time-dependent optomechanical efficiency of bulk azo-polyimide is quantified, for the first time, to be strongly correlated with the initial free volumes, a measure of polymer conformational freedom. This trend is elaborated by conformational order parameters and viscoelastic relaxation moduli. Resembling the role of porosity in azobenzene-contained metal/covalent organic frameworks to enhance the photo-switching efficiency, a larger conformational freedom enables >10 times increase in optomechanical efficiency comparing to existing experiments. This is primarily due to facilitated viscoelastic relaxation after photo-switching which alleviates residual stresses quickly and reduces heat dissipation. These findings suggest opportunities to improve the optomechanical performance through targeted strategies, such as porosity control and thermal annealing.     

Ultrafast Plasmon Thermalization in Epitaxial Graphene Probed by Time-Resolved THz Spectroscopy

The control of carrier transport by electrical, chemical, or optical Fermi level tuning is central to graphene electronics. Here, an optical pump—terahertz (THz) probe spectroscopy—is applied to investigate ultrafast sheet conductivity dynamics in various epitaxially grown graphene layers representing a large variety of carbon allotropes, including H₂ intercalated films. The graphene layers display a prominent plasmonic response connected with induced THz transparency spectra on ultrashort timescale. It is generally believed that the plasmonic excitations appear due to wrinkles, and substrate terraces that bring about natural confinement potentials. It is shown that these potentials act within micrometer-sized domains with essentially isotropic character. The measured ultrafast dynamics are entirely controlled by the quasi-Fermi level of laser-excited carriers through their temperature. The photocarriers undergo a disorder-enabled super-collision cooling process with an initial picosecond transfer of the optically deposited heat to the lattice followed by a sub-nanosecond relaxation governed by the lattice cooling. The transient spectra is described by a two-temperature Drude-Lorentz model revealing the ultrafast evolution of the carrier temperature and chemical potential and providing crucial material parameters such as Fermi energy, carrier mobility, carrier confinement length, and disorder mean free path.