Effect of electron-hole spatial correlation on spin relaxation dynamics in InAs submonolayer

Using time-resolved photoluminescence and time-resolved Kerr rotation spectroscopy, we explore the unique electron spin behavior in an InAs submonolayer sandwiched in a GaAs matrix, which shows very different spin characteristics under resonant and non-resonant excitations. While a very long spin relaxation lifetime of a few nanoseconds at low temperature is observed under non-resonant excitation, it decreases dramatically under resonant excitation. These interesting results are attributed to the difference in electron-hole interactions caused by non-geminate or geminate capture of photo-generated electron-hole pairs in the two excitation cases, and provide a direct verification of the electron-hole spatial correlation effect on electron spin relaxation.     

Singlet-triplet splitting of geminate electron-hole pairs in conjugated polymers

The singlet-triplet splitting of geminate polaron pairs in a ladder-type conjugated polymer has been studied by the thermally stimulated luminescence technique. The energy gap separating the singlet and triplet states of the geminate pairs is measured to be in the range of 3-6 meV, depending on the polymer morphology. The results of correlated quantum-chemical calculations on a long ladder-type oligomer are fully consistent with the observed values of the geminate polaron pair singlet-triplet gap. Such low splitting values have important implications for the spin-dependent exciton formation in conjugated polymers.     

A geminate recombination model for photoluminescence decay in plasma-deposited amorphous Si:H

We develop a model of geminate electron-hole recombination, including tunnelling and diffusion, to account for photoluminescence decay in amorphous semiconductors. The model correctly predicts the shape of the decay, the luminescence quantum efficiency, and the microscopic electron mobility.     

Luminescence and ESR studies of defects in hydrogenated amorphous silicon

New experimental information on luminescence and light induced ESR (LESR) in hydrogenated amorphous silicon is described. We demonstrate that the two experiments involve identical recombination transitions, and identify two separate processes. One process involves defect states, and from the doping dependence of LESR we deduce that the electronically active defects are dangling bonds with positive electronic correlation energy.     

Non-geminate recombination in amorphous silicon

The excitation power dependence of the light-induced EPR signal in intrinsic a-Si: H is found to be sub-linear over the entire accessible range of excitation power. This result is shown to require a distant-pair model of the recombination of the carriers giving the LESR. If, as is thought, the same carriers give LESR and the 1.4 eV photoluminescence band, we show that the luminescence is also distant-pair.     

Photocurrent generation in polymer-fullerene bulk heterojunctions

The photocurrent in conjugated polymer-fullerene blends is dominated by the dissociation efficiency of bound electron-hole pairs at the donor-acceptor interface. A model based on Onsager's theory of geminate charge recombination explains the observed field and temperature dependence of the photocurrent in PPV:PCBM blends. At room temperature only 60% of the generated bound electron-hole pairs are dissociated and contribute to the short-circuit current, which is a major loss mechanism in photovoltaic devices based on this material system.     

The kinetics of exciton photoluminescence in mercuric iodide

Time-resolved photoluminescence (TRPL) of red mercuric iodide single crystal is measured at low temperatures and its two-photon luminescence is measured at room temperature. Sharp near band-gap luminescence is observed around 530 nm and was ascribed to radiative annihilation of free and bound excitons; the phonon replica of exciton luminescence are found between 533 and 540 nm at low temperatures. TRPL experiment reveals that near band-gap luminescence comprises fast and slow decay components and shows the different relaxation processes between free and bound exciton annihilation. Luminescence of bound excitons steeply lowers with increasing temperature and disappears about 40 K. A luminescence tail band is observed around 540 nm that is ascribed to defects in the anion sublattice. The temporal behavior of the tail band is described by rate equations very well. A broad luminescent band appears at 630 nm. The decay curves suggest that the luminescence is ascribed to the radiative recombination of donor-acceptor pairs and there are two kinds of mechanisms to control the decay. At room temperature, a luminescent band appears at the band-gap region, which shows the band-gap at room temperature is about 2.125 eV.     

Geminate recombination of long-lived electron-hole pairs in doped carbazole-containing amorphous molecular semiconductors

This paper reports an investigation into the features of geminate recombination of long-lived electron-hole pairs in films of poly(N-epoxypropylcarbazole) (PEPC) containing intramolecular charge transfer compounds as centers of photogeneration of charge carriers carried out by measuring the attenuation kinetics of isothermal recombination luminescence over a wide range of temperatures (4.2–300 K) for times t>1 s, along with the kinetics of photoinduced EPR signals. A study is made of how the presence of a potential barrier to the reverse transition of carriers to the recombination center and the initial triplet state of the charged pairs affects the geminate recombination. It is established that the kinetics of isothermal recombintation luminescence attenuation follow the law I(t)∝t ^−m for the times under study, where m takes values from 0.65 to 1.05. The first observations of a nonmonotonic change in m with temperature are reported (m passes through a minimum at a certain temperature), and a mechanism is proposed for recombination of charged pairs in PEPC containing intramolecular charge-transfer compounds as an explanation for this phenomenon. Fiz. Tverd. Tela (St. Petersburg) 39, 1183–1187 (July 1997)     

Excitation of self-trapped-exciton luminescence in the recombination of frenkel defects in BeO

Polarized luminescence and transient optical absorption (TOA) induced by pulsed electron irradiation in beryllium oxide crystals were studied. Exponential stages with decay times τ = 6.5 ms were observed to exist in luminescence bands at 4.0, 5.0, and 6.7 eV, which coincide in spectral composition and polarization characteristics with the luminescence of self-trapped excitons (STEs) of two types. The formation efficiency of centers with a 6.5-ms decay time is comparable to that of triplet STEs. The general characteristics of the kinetics and the decay times of the TOA of these centers do not depend on electron fluence and are governed by the monomolecular recombination process. The spectra of TOA centers with a decay time of 6.5 ms were found to be similar to those of V-type hole centers and STE hole components. The mechanism by which recombination of closely spaced, spatially correlated Frenkel pairs, Be⁺ and V^? centers, brings about an exponential component with a 6.5-ms decay time in the luminescence of STEs of two types in BeO is discussed.     

Exciplex parameters: key factors in the dielectric behaviour of magnetodynamics

Photoinduced electron transfer reactions in solution produce two primary geminate radical ion pairs: contact ion pair or exciplex and solvent-separated ion pair. The magnetodynamics of radical ion pairs involves suppression of the spin-evolution between singlet and triplet states of a fraction of solvent-separated ion pairs, the partners of which undergo prior diffusion to attain the distance where exchange interaction is negligible, in the presence of an external low magnetic field of the order of the hyperfine interactions present in the system. This results in an increase in geminate recombination of the singlet solvent-separated ion pairs and enhancement in exciplex luminescence since the precursor radical ion pair is singlet. Although seemingly magnetodynamics is a diffusion-controlled phenomenon that should depend mainly on the dielectric constant of the medium (keeping viscosity almost constant), it is not true for all the exciplex systems since the nature of the magnetic field effect versus medium dielectric curves differ from each other in peak positions, peak heights and onset points. To investigate this differential nature, magnetic field effects among exciplex systems consisting of different derivatives of carbazole as electron donors are compared with a universal acceptor, 1,4-dicyano-benzene, with the pyrene—N,N-dimethylaniline exciplex system as reference. It was found that, apart from the solvent dielectric, the exciplex energy and the bulk effect of the steric constraints present on either donor or acceptor site, regulating the optimum inter-radical distance in the initially formed radical ion pair, are the key factors in controlling the magnetodynamic behaviour.     

Luminescence of different modifications of crystalline silicon dioxide: Stishovite and coesite

Luminescence of very small samples of single crystals of coesite and stishovite has been studied. The spectra were detected under ionizing radiation (X-ray and electron beam) and the decay kinetics of cathodoluminescence in the range of time from 10 ns to 3 ms was measured. The coesite luminescence possesses a broad band at 3 eV with exponential decay about 680 μs at 80 K. The nature of this luminescence was explained as a self-trapped exciton creation in tetrahedron framework. The stishovite luminescence possesses two bands—blue (2.8 eV) and UV (4.7 eV). The UV band intensity grows more than 20 times with irradiation dose from initial level. This shows that the corresponding luminescence centers could be induced by the radiation. The decay of the UV band possesses a fast and a slow component. The determination of the fast decay parameters is beyond the capabilities of our apparatus (less than 10 ns), whereas the slow decay of the UV is non-exponential and takes place in the range of hundreds of microsecond. The blue band decay kinetics can be well approximated by power law ∼t⁻², which may correspond to recombination of defects created by radiation. The stishovite single crystal luminescence is very similar to that of germanium dioxide single crystal of rutile structure. The nature of the stishovite luminescence is explained as recombination of defects created by irradiation in octahedron-structured lattice.     

Phosphorescence of pi-conjugated oligomers and polymers

We observed phosphorescence from a ladder-type poly-(para-phenylene) and an analogous oligomer containing five phenylene rings. The spectra are similar to the intrinsic fluorescence spectra and bear out a singlet-triplet splitting of 5000 cm(-1) (polymer) and 6800 cm(-1) (oligomer). Phosphorescence decay of the polymer occurs on a 10-100-micros scale obeying a power law and suggestive of nonradiative quenching, while that of the oligomer is asymptotically exponential with an intrinsic decay time of approximately 250 ms. The polymer also exhibits delayed fluorescence. It originates from delayed recombination of geminate electron-hole pairs rather than from triplet-triplet annihilation.     

Cooperative luminescence and absorption in ytterbium doped aluminosilicate glass optical fibres and preforms

The cooperative luminescence and absorption properties of Yb³⁺ doped aluminosilicate glass optical fibres and preforms are investigated in detail. In accordance with previous investigations, both the visible cooperative luminescence and the infrared luminescence decay measurements have been resolved into a single exponential decay component. We show that for a glass with similar Yb³⁺ dopant concentration but more Al³⁺, the glass emits less visible luminescence. Absorption loss measurements completed on fibre samples revealed a broad absorption in the 350-500 nm range, which we propose is due to a combination of Yb²⁺ absorption and cooperative absorption from Yb³⁺ ion pairs.     

TIME-RESOLVED PHOTOLUMINESCENCE OF SINTERED ZnO CERAMICS

The time-resolved photoluminescence (TRPL) of sintered ZnO ceramics was measured at low temperatures. A broad luminescence band was observed in the visible region. The TRPL experiment shows that photoluminescence decay behaviour can be depicted as t^-n(r). The decay rate n(r) and lifetime are wavelength dependent, and the former varies exponentially with wavelength. The power-lowering behaviour of the luminescence intensity indicates that the luminescence band originates from the recombination of donor-acceptor pairs.     

The TL and room temperature OSL properties of the glow peak at 110 °C in natural milky quartz: A case study

The LM–OSL signal of quartz, while measured at room temperature, is dominated by an intermediate, broad and intense OSL component, so that its contribution and general characteristics are derived very accurately. Through a series of dose–response, bleaching and thermal decay at room temperature experiments, in conjunction with curve fitting studies, a component resolved analysis is carried out studying the correlation between this specific component, termed as LM–OSL component C₂ and the 110 °C TL glow peak in quartz. The dose–response of these two luminescence components behaves exactly similar being linear at low doses and saturating at almost 100 Gy. Both signals decay exponentially under illumination, providing identical optical detrapping cross-section values. Residual of both luminescence signals after thermal decay at room temperature follows an exponential law, yielding similar mean half-lives. All previous luminescence features provide strong evidence for the electron trap being the same for both the 110 °C TL trap and the LM–OSL component C₂. The results of the present work are very promising and clearly support the possibility of extrapolating the TL pre-dose methodology to the OSL pre-dose effect using only the LM–OSL component C₂.     

Exciton-induced defect formation in KJ-T1 crystal and the defect participation in thallium luminescence

Abstract

The interaction of excitons with lattice defects - Tl ions in the activated KJ crystal is studied at low temperatures. Luminescence of Tl under the excitation in the 1s exciton absorption band (5.85 eV) is examined. The participation of the localized excitons created and trapped near Tl ions during that process is shown. Those localized excitons decay into lattice defect pairs which take part directly in the excitation and luminescence of Tl and cause a broadening of Tl luminescence bands.     

The luminescence of ZnO ceramics

The luminescence properties of ZnO ceramics with grains 100–5000 nm sintered by different techniques from nanopowders were studied. The luminescence decay times were compared with that obtained for ZnO single crystal. The temperature dependence of non-exponential decay of defect luminescence (2.0–2.6 eV) was measured in wide time, intensity and temperature range. The luminescence decay kinetic at T ≤ 20 K shows the decay close to I(t) ～ t^?1 dependence. At temperature region 50–250 K the decay kinetics is more complicate since the TSL was observed in this temperature region. It is shown that the luminescence properties of NP and ceramics strongly depend on defect distribution on grains surface and the volume/surface ratio determine the luminescence decay in ZnO nanostructures and ceramics.     

带-NH2的嘧啶环对钌配合物与DNA相互作用的瞬态发光特性的影响

采用时间分辨的发光光谱技术,分别测量了两种新合成的钌配合物[Ru(bpy)2 (dpbpd(NH2)2)]2 和[Ru(phen)2(dpbpd(NH2)2)]2 与小牛胸腺脱氧核糖核酸(ctDNA)相互作用时的瞬态发光动力学过程,并与以往对[Ru(phen)2dppz]2 等的研究结果进行对比,从而研究带-NH2的嘧啶环对配合物与DNA作用动力学过程的影响.结果表明:这两种含有带-NH2的嘧啶环的钌配合物与DNA相互作用时的发光按双指数规律衰减,发光寿命为几十纳秒,比dppz类钌配合物与DNA作用时的发光衰变寿命(几百纳秒)小一个数量级.归因于嘧啶环上的N和-NH2可能与水分子、DNA的碱基对或磷酸骨架形成氢键,从而加快激发态的无辐射弛豫,削弱发射光强,缩短发光寿命.该结论为进一步研究配合物分子与DNA的相互作用的机理提供了一定的依据.     

Luminescence decay in spray-pyrolyzed Cds

We report the room temperature luminescence decay of spray pyrolyzed CdS, which is extremely similar to the luminescence decay of amorphous silicon hydrogen alloys at liquid helium temperatures. We suggest that the luminescence decay in both of these materials is due to localized electrons and holes recombining by radiative tunnelling.     

能量传递过程的计算机模拟

通过对供体(D)—受体(A)间传递速率静态分布的模拟,得到了静态能量传递情况下D的发光衰减曲线,与Inokuti-Hirayama模型结果一致.模拟并讨论了D—D传递与D—A传递相关和非相关情况下D—D传递对D发光衰减的影响. 关键词：