Kinetics of the Decay of Prolonged Luminescence of Disordered Chrysene under the Conditions of Nonequilibrium Transfer of Energy

We present the results obtained in investigation of the decay of the prolonged luminescence of disordered chrysene in a microsecond range. At the temperature of liquid nitrogen, a highly nonexponential decay of both phosphorescence and annihilation of delayed fluorescence is observed. The observed character of decay is due to relaxation of the energy of electronic excitation in a system of energydisordered centers, when the value of kT is much smaller than the width of the excitedstate energy distribution. At the same time, in the system investigated there is a classical relationship between phosphorescence and delayed fluorescence, i.e., the rate coefficient for the reaction of triplettriplet annihilation is a constant.     

Annihilation kinetics for triplet excitations in organic glasses

The results of investigations of delayed luminescence decay are presented for disordered phenanthrene in the microsecond, millisecond, and second time ranges. At liquid nitrogen temperature, the highly non-exponential decay of both the phosphorescence and the annihilation delayed fluorescence is observed. This character of decay is caused by the relaxation of the electron-excitation energy in the system of energy-disordered centers when a quantity kT is much less than the width of the distribution for the excited-state energy. At the same time, the analysis of the time dependence for the triplet-triplet-annihilation rate exhibits two time intervals in which different kinetics is observed for the triplet excitations annihilation. In the microsecond range, the classical relationship between the phosphorescence and the delayed fluorescence takes place for the system under investigation; i.e., the triplet-triplet-annihilation rate is constant. At large times, the reaction-rate time dependence is described by the power law characteristic of inhomogeneous and low-dimensional systems. When the temperature increases, a transition to the classical behavior is observed throughout the entire time interval.     

A role of solvent in vibrational energy relaxation of metalloporphyrins

The formation of a vibrationally excited photoproduct of metalloporphyrins upon (π, π*) excitation and its subsequent vibrational energy relaxation were monitored by picosecond time-resolved resonance Raman spectroscopy. Stokes Raman bands due to a photoproduct of nickel octaethylporphyrin (NiOEP) instantaneously appeared upon the photoexcitation. Their intensities decayed with a time constant of 300 ps, which indicates electronic relaxation from the (d, d) excited state (B_1g) to the ground state (A_1g), being consistent with the results of transient absorption measurements by Holten and coworkers. Anti-Stokes ν₄ and ν₇ bands for vibrationally excited (d, d) state of NiOEP decayed with time constants of 10 and 300 ps. The former is ascribed to vibrational relaxation, while the latter corresponds to the electronic relaxation from the (d, d) excited state to the electronic ground state. While the rise of anti-Stokes ν₄ intensity was instrument-limited, the rise of anti-Stokes ν₇ intensity was delayed by 2.6±0.5 ps, which indicates that intramolecular vibrational energy redistribution has not been completed in subpicosecond time regime. To study a mechanism of intermolecular energy transfer, solvent dependence of the time constants of anti-Stokes kinetics was investigated using various solvents. No significant solvent dependence of the rise and decay constants was observed for NiOEP. For an iron porphyrin, we observed two phases in intermolecular energy transfer. The fast phase was insensitive to solvent and the slow phase depended on solvents. A model of classical thermal diffusion qualitatively reproduced this behavior. For solute-solvent energy transfer process, low-frequency modes of proteins seem to be less important.     

Effect of Temperature on the Rate of Triplet–Triplet Annihilation of 1,2-Benzanthracene in a Polymer Matrix

The process of triplet–triplet annihilation (TTA) of 1,2-benzanthracene (1,2-BA) incorporated into polymer films of polyvinyl butyral has been investigated in the temperature interval 80–360 K. An analysis of the kinetics of the decay of delayed annihilation fluorescence (DAF) of 1,2-BA has shown that the process of the triplet excitation energy transfer in a disperse medium of the polymer at distant times of the DAF decay can be described using the approximation of random walks of the triplet energy in the inhomogeneous medium of the polymer. At low temperatures, at the initial times of DAF decay the TTA process is described with the aid of a model of static annihilation.     

Observation of long-lived excitons in InAs quantum dots under thermal redistribution temperature

We study the temperature-dependent time-resolved photoluminescence (TRPL) of self-assembled InAs quantum dots (QDs). Under low excitation power, a surprisingly long PL decay time is observed at about 60 K, under the thermal redistribution temperature. The long decay time decreases with increasing excitation power but is nearly independent of the detection energy of TRPL measurements. A model considering the spin relaxation through the excited excitonic state is proposed to quantitatively explain the unusual phenomena. The rate equation analysis indicates that the observation of long-lived excitons is caused by the shortened spin-flip time.     

Elementary relaxation processes investigated by femtosecond photoelectron spectroscopy of two‐dimensional materials

Elementary scattering processes in solid matter occur on ultrafast timescales and photoelectron spectroscopy in the time domain represents an excellent tool for their analysis. Conventional photoemission accesses binding energies of electronic states and their momentum dispersion. The use of femtosecond laser pulses in pump‐probe experiments allows obtaining direct insights to the energy and momentum dependence of ultrafast dynamics. This article introduces the elementary interaction processes and emphasizes recent work performed in this rapidly developing field. Decay processes in the low excitation limit are addressed, where electrons decay according to their interaction with carriers in equilibrium. Here, hot electron relaxation in epitaxial metallic film is reviewed. In the limit of an intense optical excitation, scattering of the excited electrons among each other establishes a non‐equilibrium state. Results on charge‐density wave materials and the effect of coherent nuclear motion on the electronic structure, which can break low symmetry ground states, are discussed. Figure reprinted with permission from [71].     

飞秒激光在可饱和吸收体中的动力学特性

从激光动力学的自洽理论出发，推导出适用于含有可饱和吸收体的激光系统动力学方程组，研究了激光振荡的稳定性与系统参数的依赖关系，包括激励强度参数、饱和系数和能级寿命，并讨论了满足激光振荡稳定性的条件下B类激光的弛豫振荡特性。结果表明，增大激励强度与饱和系数有利于系统形成稳定的振荡输出，而且当激励强度超过一定阈值时，B类激光会产生弛豫振荡行为。     

Kinetics of long-lived luminescence of eosin in Langmuir-Blodgett films

The spectral and kinetic properties of photoluminescence of mixed Langmuir-Blodgett (LB) films of eosin decyl ether and palmitic acid on a solid substrate are studied. The electronic absorption and fluorescence spectra of the films are identical to the spectra of the dye in ethanol. An increase in the dye concentration in a monolayer results in the appearance of a dimer absorption band, quenching of fluorescence of monomers, and the red shift of the spectral bands. At 90 K, the distinct phosphorescence and delayed fluorescence bands of LB films were observed. The decay kinetics of phosphorescence and delayed fluorescence is nonexponential. It is shown that the decay curve of delayed fluorescence is determined by triplet-triplet annihilation (TTA) and T ₁→S₁ triplet-singlet intersystem crossing (IS). The initial nonexponential phosphorescence decay is caused the dominant contribution of TTA to the decay of triplet molecules. The experimental data are interpreted based on the mechanisms of exchange-resonance and inductive-resonance annihilation.     

Measurement of the nuclear spin diffusion coefficient in organic glasses doped with paramagnetic centers: Orthoterphenyl and polymeric glasses

We have recently developed a method of studying spin diffusion coefficients by doping the materials with paramagnetic centers and measuring the nuclear relaxation in a tilted rotating frame. Using this method, we measure here the spin diffusion coefficient of orthoterphenyl, a molecular organic glass, and of three polymer glasses: poly(4-vinylpyridine), poly(vinylacetate) and poly(methyl methacrylate). We explore a possible dependence of the measured orthoterphenyl spin diffusion coefficient on the electronic relaxation time and concentration of the paramagnetic centers. We conclude that the experiments can be performed at higher concentrations than previously thought. We also show that our method applies to polymers in the glassy state if one works at sufficiently small tilt angle, in spite of a short value ofT _1ρ. We had anticipated that the distribution of proton pairs in these materials precludes the standard dependence of the spin diffusion coefficient on the proton density and free induction decay characteristic decay time. Our results fully confirm such expectation.     

Ultrafast dynamics of intersubband relaxation in GaAs quantum wells: hot carrier and phonon populations effects

The dynamics of intersubband relaxation in GaAs quantum wells and the role of hot carriers and the phonon distributions have been investigated using two different optical techniques with femtosecond resolution: 1) time-resolved photoluminescence and 2) pump and probe experiments. The (2→1) intersubband relaxation times have been measured as functions of well widths (100Å < L_well < 220Å), under different experimental conditions (15K < T_lattice < 300K, and 1×10¹⁰ cm^-2 < excitation densities < 1×10¹² cm^-2). The electron intersubband relaxation time is deduced from the decay time of the n=2 well luminescence (or differential transmission) intensity. For thin wells (<150Å), a fast intersubband (2→1) relaxation time ≤ 3 ps has been measured. For thicker wells, the measured decay times are found to be critically dependent on the excitation conditions (vary from 5 ps to 40 ps). The well width dependence of the intersubband relaxation time does not show the strong dependence (2 orders of magnitude) predicted theoretically for electron-LO phonon scattering. Our results show that the hot phonon populations and the slow carrier cooling rate limit the observation of subpicosecond relaxation time. For thick well widths, our results also suggest that hot carriers effects play an important role in the intersubband relaxation mechanisms.     

Rapid decrease of fragment emission time in the range of 3–5 MeV/u excitation energy

Multifragment emission processes from highly excited nuclei produced in ⁴⁰Ar + ¹⁹⁷Au reactions at incident energies of 30 and 60 MeV/u are compared. At the lowest bombarding energy and 3.3 MeV/u excitation energy, the composite system decay process supports the hypothesis of long-lived equilibrated nucleu decaying by successive binary splittings. For excited nuclei around 5 MeV/u, the depletion observed at small relative angles in the correlation functions is interpreted as the result of a strong reduction in the fragment emission time scale.     

InGaAs/GaAs量子链的光学特性研究

研究了InGaAs/GaAs量子链的稳态和瞬态光谱特性,特别是载流子的动力学过程.实验发现荧光寿命有很强的探测能量依赖关系,荧光寿命随发光能量的增加而减小;实验还发现,当激发功率较小时,荧光寿命随激发功率增大而增大,当激发功率足够大时,荧光寿命趋于饱和.这些结果清楚地表明,在量子链结构中,参与发光的载流子之间存在明显的耦合和输运现象,进一步分析表明,这种输运主要是由于载流子沿量子链方向的耦合造成的.发光的偏振特性研究进一步证实了载流子沿量子链方向输运过程. 关键词： InGaAs/GaAs 量子点 量子链     

稀土粉末Eu:Y2O3的自由感应衰减量子拍

稀土固体是重要的激光和光电子材料。目前,由于以宽带信号和太赫兹比特数据传输率为特征的信息技术的发展,稀土固体材料的相干瞬态动力学过程成为宽带与高速信息光子学的基本物理问题之一。研究了室温下稀土粉末样品Eu³⁺:Y₂O₃自由感应衰减的相干瞬态光谱,这有助于理解有效的光吸收动力学、激发态弛豫、相干能量传递和超短光脉冲在稀土固体中的传播。用一对紫外飞秒相干光脉冲作用于稀土粉末样品Eu³⁺:Y₂O₃,然后监测物质激发态的布居数随两个激发脉冲之间的延时的变化,测量到其自由感应衰减量子拍(FID),从拍频周期分析确定了其能级精细结构,能级的退相时间长达皮秒量级。理论分析和实验结果符合得很好。对稀土离子的量子干涉的研究,表明其在受激受控光放大方面具有潜在的应用前景。     

PbWO<Subscript>4</Subscript> crystal for laser energy accumulation and transformation

The picosecond interband two-photon laser excitation of PbWO₄ crystals at a temperature of 10 K leads to electronic excitation energy accumulation, which results in almost 100% induced absorption in the 450–750 nm spectral range. The relaxation time of this induced absorption exceeds 100 min. The electronic excitation energy accumulated in the PbWO₄ crystal at T = 10 K excites the intrinsic luminescence with a decay time longer than 45 min. The decay kinetics and the spectra of the intrinsic luminescence of the PbWO₄ crystal at a temperature of 10 K were measured under two-photon and single-photon excitation. The luminescence under two-photon and single-photon excitation revealed a difference in the structure of the spectra.     

Dephasing of a superconducting flux qubit

In order to gain a better understanding of the origin of decoherence in superconducting flux qubits, we have measured the magnetic field dependence of the characteristic energy relaxation time (T(1)) and echo phase relaxation time (T(2)(echo)) near the optimal operating point of a flux qubit. We have measured T(2)(echo) by means of the phase cycling method. At the optimal point, we found the relation T(2)(echo) approximately 2T(1). This means that the echo decay time is limited by the energy relaxation (T(1) process). Moving away from the optimal point, we observe a linear increase of the phase relaxation rate (1/T(2)(echo)) with the applied external magnetic flux. This behavior can be well explained by the influence of magnetic flux noise with a 1/f spectrum on the qubit.     

Size effects in triplet-triplet annihilation: II. Monte carlo simulations

The dynamics of triplet-triplet annihilation (TTA) is theoretically studied in linear chains and nanoparticles, modeled as 1D, 2D, and 3D regular lattices, as a function of size M, of the rate of excitation migration W, and of the rate of excitation annihilation V in the diffusion-influenced limit (V ≫ W). It is shown that a sum of two exponentials is usually sufficient for fitting experimental phosphorescence and triplet-triplet absorption decays. The first term describes the decay of domains containing initially one triplet, while the second one reflects the disappearance of domains containing initially two triplets. Monte Carlo calculations were carried out to compute the survival probability of an annihilating pair of triplets, yielding expressions for the dependence of the rate constant of TTA on the parameters M, W, and V in one, two, and three dimensions. The text was submitted by the authors in English.     

Time-resolved spectrum for resonant light scattering in an exciton-phonon system

A formula is given for the time-resolved spectrum of the resonantly- scattered radiation from an exciton-phonon system, and it is applied to the calculation of two-LO-phonon assisted spectrum. Both the Raman component associated with virtual intermediate states and the luminescence with real intermediate states are obtained. A Raman-like component with an oscillatory behavior can be seen, when the exciton relaxation time is shorter than the excitation pulse duration. It is proposed that the energy dependence of exciton relaxation rate can be directly measured from the time decay of a hot luminescence spectrum.     

Energy relaxation mechanism in Landau level system of quantum wells

Kinetics of intrasubband energy relaxation of electrons in the system of Landau levels lying below the optical phonon energy is studied. Extraordinary behavior of the relaxation of electronic subsystem excitation energy is detected. Despite the fact that its main channel is optical phonon emission, the total relaxation time exceeds the characteristic times of scattering on optical phonons by several orders of magnitude.     

Luminescence of a ZnO:Ga crystal upon excitation in vacuum UV region

The spectral-kinetic characteristics of a ZnO:Ga single crystal upon excitation in the vacuum UV region have been studied. At a temperature of 8 K, the exciton luminescence line peaking at 3.356 eV has an extremely small half-width (7.2 meV) and a short decay time (360 ps). In the visible range, a wide luminescence band peaking at ～2.1 eV with a long luminescence time at 8 K and a decay time in the nanosecond range at 300 K is observed. The luminescence excitation spectra of ZnO:Ga have been measured in the range of 4–12.5 eV.