Radiative and non-radiative transitions in ErP5O14 single crystals

The radiative and non-radiative transitions from excited states of ErP₅O₁₄ were studied on the basis of the Judd-Ofelt theory and experimental data. It was shown that the non-radiative relaxations, predominantly multiphonon emission, are very effective in the depopulation of excited states of erbium in erbium pentaphosphate crystals. The concentration quenching of erbium fluorescence is found to be small.     

Absorption cross-sections and lifetimes as a function of size in Si nanocrystals embedded in SiO2

The photoluminescence (PL) emission yield of Si nanocrystals embedded in SiO₂ depends on their size and on Si–SiO₂ interface passivation. In this work we aim at clarifying the relative importance of both contributions by studying lifetimes and absorption cross-sections as a function of size, for samples with and without passivation in forming gas. We find that while the PL lifetime increases steadily (quasi-linear dependence), the radiative lifetime increases exponentially with the nanocrystal size. Thus, as expected, radiative oscillator strengths are much smaller for large nanocrystals, but this reduction is partially compensated by a less effective quenching at interfacial non-radiative states. The absorption cross-section per nanocrystal rises as the nanocrystal size decreases, for all excitation wavelengths, implying that the variation of oscillator strength dominates over the reduction of the density of states. Passivation processes do not affect the emission mechanism and increase the emission yield while reducing the density of non-radiative recombination centers at the Si–SiO₂ interface (P_b centers).     

晶格弛豫和多声子跃迁理论

近年的发展日益证明,固体中的局域电子态所导致的晶格弛豫(晶格原子位置移动)是局域电子态的一项基本特征,能够引起许多重要的效应。在局域态的吸收和发射光谱中,由于晶格弛豫而引起斯托克斯位移和光谱的多声子结构(多声子的光跃迁)。晶格弛豫又可以在不同电子态之间引起无辐射跃迁,其中的能量变化完全由多声子的发射或吸收来补偿(多声子无辐射跃迁)。本文以线性的电子—声子作用和简谐近似的晶格模型为基础,系统地总结阐明多声子的光跃迁理论和多声子的无辐射跃迁理论。关于光跃迁的部份既介绍了直接计算跃迁几率的方法,也介绍了采用傅里叶变换的理论,并分析了连续谱和多声子结构相互叠加的一个光谱实例。关于无辐射跃迁的部份着重分析和澄清了多年来环绕所谓“康登近似”出现的矛盾,从而把近年来不同的理论发展置于统一的基础之上。介绍了估算跃迁几率的最陡下降法。最后讨论了强耦合和弱耦合的情形。     

Luminescence related processes in semiconductor nanocrystals —The strong confinement regime

This paper summarizes systematic studies on the luminescence from CdSe nanocrystals in the situation of strong zero-dimensional confinement. We discuss the role of surface and defect states, the origin of the photo-darkening and demonstrate by calorimetric adsorption measurements that the internal quantum efficiency is in the range of some 10%. The lifetimes of the intrinsic excitations are strongly size-dependent. While the radiative recombination (≈ 1 ns) is dominant for larger nanocrystals, we observe a dramatic increase of the non-radiative rate below 4 nm as a result of the reduced volume to surface ratio. The combination of ultra-fast and size-selective excitation allows us to observe a progression of sharp LO-phonon lines signifying the zero-dimensional character of the nanocrystals and providing information on the strength of the phonon coupling and the homogeneous width of the quantum-confined ground state.     

Recombination processes in structures with GaN/ALN quantum dots

Mechanisms of the generation and the radiative and nonradiative recombination of carriers in structures with GaN quantum dots in the AlN matrix are studied experimentally and theoretically. Absorption, stationary and nonstationary photoluminescence of quantum dots at different temperatures are investigated. It is found that the photoluminescence intensity considerably decreases with the temperature while the photoluminescence kinetics weakly depends on the temperature. The photoluminescence kinetics is shown to be determined by radiative recombination inside quantum dots. A mechanism of nonradiative recombination is proposed, according to which the main reason for the thermal quenching of photoluminescence is nonradiative recombination of charge carriers, generated by optical transitions between quantum dots and wetting layer states.     

Modelling the thermal quenching mechanism in quartz based on time-resolved optically stimulated luminescence

This paper presents a new numerical model for thermal quenching in quartz, based on the previously suggested Mott-Seitz mechanism. In the model electrons from a dosimetric trap are raised by optical or thermal stimulation into the conduction band, followed by an electronic transition from the conduction band into an excited state of the recombination center. Subsequently electrons in this excited state undergo either a direct radiative transition into a recombination center, or a competing thermally assisted non-radiative process into the ground state of the recombination center. As the temperature of the sample is increased, more electrons are removed from the excited state via the non-radiative pathway. This reduction in the number of available electrons leads to both a decrease of the intensity of the luminescence signal and to a simultaneous decrease of the luminescence lifetime. Several simulations are carried out of time-resolved optically stimulated luminescence (TR-OSL) experiments, in which the temperature dependence of luminescence lifetimes in quartz is studied as a function of the stimulation temperature. Good quantitative agreement is found between the simulation results and new experimental data obtained using a single-aliquot procedure on a sedimentary quartz sample.     

Induced radiative transitions of intermediate molecules in heavy ion collisions

Three types of transitions exists in intermediate molecules occuring in heavy ion scattering: spontaneous radiative, induced non-radiative, and induced radiative decay. The latter ones yield an asymmetric angular distribution for molecular X-rays with respect to the ion-beam axis. The experimental verification of this effect would furnish an experimentum crucis for both, the existence of molecular X-rays and the induced radiative transitions.     

Fluorescence Dynamics of Three UV-B Sunscreens

Polarity of the surrounding medium affects the excited states of UV-B sunscreens. Therefore understanding excited state processes in a mixed polarity model system similar to skin is essential. We report the excited state lifetimes, quantum yields, radiative and non-radiative rates of three sunscreens. Among the three UV-B sunscreens studied, octyl salicylate emits from a single excited state, while padimate O and octyl methoxy cinnamate show multiple states. The radiative rates of salicylate and cinnamate are approximately constant, while that of padimate O depends strongly on solvent. The non-radiative rates of all sunscreens vary with solvent polarity. Compared to salicylate and cinnamate, padimate O is complex to analyze because of its two emission peaks and one peak’s strong dependence on the dielectric constant. High absorbance, broad absorption peak with small fluorescence quantum yield, and low radiative rate make octyl methoxy cinnamate a superior UV-B sunscreen ingredient. The complexity in excited-state analysis shows that the lifetimes of the sunscreens are critical parameters, in addition to absorbance and quantum yield. Fluorescence lifetime substantiates the use of polystyrene nanospheres as a model host to study the photo-physical properties of sunscreen in a heterogeneous environment.     

Ionization equilibrium and radiative energy loss rates for C,N, and O ions in low-density plasmas

The results of calculations of the ionization equilibrium and radiative energy loss rates for C, N and O ions in low-density plasmas are presented for electron temperatures in the range 10⁴–10⁷ °K (～1–10³ eV). The ionization structure is determined using the steady-state corona model, in which electron impact ionization from the ground states is balanced by direct radiative and dielectronic recombination. Using an improved theory, detailed calculations are carried out for the dielectronic recombination rates in which account is taken of all radiative and autoionization processes involving a single-electron electricdipole transition of the recombining ion. The radiative energy loss processes considered are electron-impact excitation of resonance line emission, direct radiative recombination, dielectronic recombination, and electron-ion bremsstrahlung. For all three elements, resonance line emission resulting from 2s?2p transitions produces a broad maximum in the energy loss rate near 10⁵°K(～ 10 eV).     

Laser-stimulated formation and stabilization of antihydrogen atoms

Laser-stimulated radiative transitions from states close to the ionization threshold to low-lying atomic levels are considered for protons (antiprotons) in a cold electron (positron) plasma and estimates for the resulting formation rate of hydrogen (antihydrogen) atoms in the ground state are given. The estimates apply to both laser-stimulated recombination and induced radiative stabilization of high Rydberg levels. First experiments concerning laser-stimulated recombination in merged beams of electrons and protons are discussed, which have confirmed the rate predictions for this process. In view of antihydrogen formation in a cold trapped positron plasma, the use of two successive stimulated transitions is considered for obtaining a high formation rate of ground-state atoms at relatively low radiation intensity.     

Radiative and non-radiative decays from the excited state of Ti3+ ions in oxide crystals

The fluorescence spectra of Ti³⁺ in Y₃Al₅O₁₂ (YAG), Al₂O₃ (sapphire), YAlO₃ (YAP) observed at 10 K are composed of zero-phonon lines accompanied by the broad vibronic sidebands. The temperature dependence of the fluorescence lifetime and of the total intensity of the broadband measured in YAG and Al₂O₃ indicate that the radiative decay times from the excited states are nearly constant in the range 10–300 K. This demonstrates that the broadband radiative emissions in Ti³⁺:YAG and Ti³⁺:Al₂O₃ are due to magnetic dipole transitions or to electric dipole transitions induced by static odd-parity distortion, respectively. The decrease of the fluorescence lifetime with increasing temperature in Ti³⁺:YAG and Ti³⁺:Al₂O₃ is due to non-radiative decay from the excited state which occurs through phonon-assisted tunnelling between the excited and ground states. The radiative decay of Ti³⁺:YAP is enhanced with increasing temperature, indicating that radiative decay rate contains a term associated with odd-parity phonons. Nevertheless, a non-radiative decay rate of 3.6 × 10⁴ s^–1 observed in the temperature range 10–300 K is due to excited state absorption, which depopulates the excited state and quenches the fluorescence at the laser wavelength.     

Influence of the charge transfer state on the luminescence characteristics of Er3+ in alkaline-earth thiogallates MGa2S4

The luminescence properties of Er³⁺ in thiogallates have been analyzed in terms of a single-configurational-coordinate diagram. The minimum of the charge transfer state parabola decreases with increasing size of the substituted alkaline-earth cation, leading to a decrease in the quenching temperature of the emission from the higher levels. Calculations of the transition rates show that non-radiative transitions from the charge transfer states essentially populate the 4f levels emitting in the visible.     

On the role of the dangling bond as a radiative centre in a-Si:H

A comparison of recent ODMR results a-Si : H with previously reported ESR and LESR measurements suggests that a principal radiative electron centre has g=2.0055 and may therefore be identified as the dangling board. Our results suggest that the dangling bond (DB) can participate in two distinct PL transitions, centred near 1.25 eV and 0.9 eV, which are present to a measurable extent in all samples examined, in the medium-to-high quantum efficiency range (η_PL ～ 0.1?1.0). This conclusion is in contrast with the generally accepted role of the dangling bond in a-Si : H as primarily a non-radiative recombination centre, but is consistent with a variety of data from other experimental techniques.     

Radiative and non-radiative relaxation of excitons in strain-compensated quantum dots

We have investigated the population dynamics of excitons in strain-compensated InAs quantum dots (QDs) using a pump–probe technique under resonant excitation. Precise control of polarization directions of incident pulses enabled us to selectively estimate population lifetimes for two orthogonally polarized exciton ground states according to polarization selection rules. Measured decay times of the probe transmissions were highly dependent on the polarization directions of the exciton states. We found that the ratio of the decay times for the orthogonally polarized states is in quantitative agreement with the ratio of square of the transition dipole moments. This indicates that radiative recombination processes have a dominant effect on the population dynamics and that non-radiative and spin relaxations are negligible in our QDs. As a result, we can estimate the radiative lifetimes to be 1.0±0.1 and 1.7±0.2 ns for orthogonally polarized exciton ground states.     

Indium-incorporation-induced transformation of optical, photoluminescence and lasing properties of InGaN epilayers

A comparative combined study of photoluminescence (PL), PL kinetics, stimulated emission (SE) and photoreflectance (PR) properties in In_xGa_1−xN epilayers is carried out in the composition range 0≤x≤0.19. In-incorporation up to 4% leads to the sufficient longer radiative recombination decay time due to the decrease in non-radiative recombination channels, which are peculiar to GaN, and band-to-band optical transitions predominate the spontaneous PL spectrum. Further In-incorporation (x>4%) leads to the localization of carriers and/or excitons at band-tails in the In-rich areas. Correlation between the position of dominant low-energy PR oscillation due to the main band gap and SE peak position shows that band-to-band transitions are responsible for lasing and dominate the PL spectrum in all highly pumped In_xGa_1−xN samples.     

Theory of radiative and nonradiative transitions for semiconductor nanocrystals

Existing calculations on the radiative and nonradiative transitions in semiconductor crystallites are reviewed with particular emphasis on indirect band-gap materials like silicon for which the quantum confinement effects are more spectacular. It is shown that the crystallite gaps and radiative recombination rates can be predicted with fair accuracy. Effects related to atomic relaxation in the excited state (Stokes shift) are calculated and it is shown that small enough crystallites lead to self-trapped excitons which provide another source of luminescence, much less dependent on size effects. Nonradiative processes are then examined: intrinsic, due to Auger recombination, and extrinsic, due to dangling bond surface states. Both are found to play an essential role in the interpretation of experimental data. Finally, dielectric screening is studied, justifying the use of a reduced internal dielectric constant and providing an estimate of the Coulomb shift due to charging effects.     

键合氢对GDa—Si:H薄膜光致发光性质的影响

测量了在不同衬底温度下制备的GDa-Si:H膜的光致发光谱和光吸收谱。实验发现键合氢含量的增加导致光致发光峰强度、发光峰能量、发光带半宽度、Stokes位移和热淬灭的增大。由此导出:(1)键合氢不仅能消除无辐射复合中心,而且能产生辐射复合中心;(2)随着键合氢含量的增加电子-声子相互作用增强,带尾宽度缓慢变窄。 关键词：     

钕玻璃的光谱性质

本文分析了Nd³⁺在玻璃中的stark分裂情况,描写了确定荧光能级的实验方法,并给出了钕在四种硅酸盐玻璃中亚稳态和基态能级Stark分裂的实验结果。同时,对十三种不同成份的玻璃,通过光谱实验确定了Nd^{3+ 4}F_3/2态的辐射和无辐射跃迁速率,受激发射截面σ,辐射量子效率η,荧光分支比β和亚稳态寿命τ等激光常用参数。并对实验结果进行了讨论。 关键词：     

Spin Physics of Excitons in Colloidal Nanocrystals

We present a review of spin-dependent properties of excitons in semiconductor colloidal nanocrystals. The photoluminescences (PL) properties of neutral and charged excitons (trions) are compared. The mechanisms and the polarization of radiative recombination of a “dark” (spin-forbidden) exciton that determines the low-temperature PL of colloidal nanocrystals are discussed in detail. The radiative recombination of a dark exciton becomes possible as a result of simultaneous flips of the surface spin and electron spin in a dark exciton that leads to admixture of bright exciton states. This recombination mechanism is effective in the case of a disordered state of the spin system and is suppressed if the polaron ferromagnetic state forms. The conditions and various mechanisms of formation of the spin polaron state and possibilities of its experimental detection are discussed. The experimental and theoretical studies of magnetic field-induced circular polarization of PL in ensembles of colloidal nanocrystals are reviewed.