Laser flash photolysis and time-resolved CIDNP study of photochemical reactions between aqueous tryptophan and nucleotides

The theory of deuteron spin-lattice relaxation for free D₂ quantum rotors is developed. Relaxation rates are calculated forortho-D₂ andpara-D₂. The spin-rotational interaction as well as quadrupole and dipole-dipole interactions under interference condition are taken into account. Relaxation rates, to be compared with experiment, are derived as weighted sums of contributions from different rotational states according to their Boltzmann populations. The theory is applied to explain relaxation rates measured in a wide temperature range for D₂ molecules in NaY zeolite cages. At high temperatures (above 110 K), a scattering of molecules on the cage walls provides the relaxation mechanism. At low temperatures, molecules stay close to the surface and undergo reorientations in a potential introduced by the adsorption centers.     

Thermal and optical properties of Er-doped oxyfluorotellurite glasses

Er³⁺-doped oxyfluorotellurite glasses with four different concentrations of Er³⁺ ions have been prepared and investigated their thermal, optical absorption, excitation and luminescence properties. From the DSC spectra, glass transition and onset of crystallization temperatures have been found. Judd-Ofelt intensity parameters have been derived from the absorption spectrum and are in turn used to calculate radiative properties for the important luminescent levels of Er³⁺ ions. The calculated radiative properties are comparable to experimental values. The glasses show intense green and weak red emission under normal excitation with 451 nm. The decrease in emission intensities and lifetimes of the ⁴S_3/2 level with concentration of Er³⁺ ions has been explained as due to energy transfer processes between Er³⁺ ions. The stimulated emission cross-sections and quantum efficiencies of the green and infrared emissions have been determined. The results indicate that the glasses may be suitable for use as a laser medium in making solid-state green laser by normal pumping route and as laser medium and optical amplifier in the 1.5 μm region.     

Dosimeter properties of Ce and Eu doped LiCaAlF6

Optical, scintillation properties, optical stimulated luminescence, and thermally stimulated luminescence of Ce 1, 3, and 5% doped and Eu 1, 1.5, and 2% doped LiCaAlF₆ crystals fabricated by Tokuyama Corp. were investigated. In transmittance, absorption was proportional to dopant concentrations and typical optical quantum yield of Ce and Eu-doped LiCaAlF₆ were 40 and 100%, respectively. Scintillation wavelength and decay time profiles were investigated under X-ray irradiation. Ce³⁺ and Eu²⁺ 5d-4f luminescence appeared around 300 nm and 370 nm with typical decay time of 40 ns and 1.5 μs, respectively. Optically stimulated luminescence of Ce-doped ones appeared under 405 nm stimulation with detectable intensity while those of Eu doped ones were quite weak. Thermally stimulated luminescence of Ce- and Eu-doped LiCaAlF₆ were enough strong and they exhibited good response function from 1 to 1000 mGy exposure.     

The photoluminescence excitation spectra of multicomponent media

With no restrictions on the value of optical density, we derive an equation that describes the photoluminescence excitation spectra of separate components with overlapping absorption bands in a multicomponent medium. Based on the equation obtained, we propose methods for measuring the ratios of absorption optical densities of the components and quantum yields of their luminescence. The applicability of the proposed methods is demonstrated by measuring the characteristics of coumarin and porphyrin dissolved in different proportions in ethanol. We have also measured the quantum yield and luminescence decay time of the radiationinduced color centers F ₃ ⁺ in the lithium fluoride crystal and calculated probabilities of radiative and nonradiative transitions from the first excited singlet state of these centers.     

Two state systems in media and “Turing's paradox”

We discuss the coherence properties of two state systems subjected to random influences in a medium. We find an expression for the “damping parameter” characterizing the loss of coherence as a kind of generalization of the optical theorem. We verify previous speculations as to how an asymmetry like optical isomerism ca be stabilized by a neutral environment and suggest an experimental test of the resulting “paradoxical” behaviour where heating will slow down the relaxation rate. This is related to a certain “paradox” of quantum measurement theory and can be verified experimentally by studying the relaxation rate for the optical activity of small molecules at low temperature. As another application of the method, neutrino oscillations in dense media are considered.     

Charge carrier recombination mechanisms in Sb-containing quantum well laser structures

The dynamics of interband luminescence in structures with InGaAsSb-based quantum wells and barriers of different types was studied at different temperatures and excitation levels. The lifetime of optically injected charge carriers in quantum wells at different temperatures and optical excitation levels was determined. An increased recombination rate in structures with deep electron quantum wells was discovered; it is associated with the occurrence of resonance Auger recombination. It was concluded that the application of quinary solid solutions as barriers in laser structures for a 3—4 fum wavelength range is to be preferred.     

Two-photon correlations of luminescence at the Bose-Einstein condensation of dipolar excitons

Correlations of the luminescence intensity (the second-order correlation function g ⁽²⁾(τ)), where τ is the delay time between the photons detected in pairs) under the conditions of the Bose-Einstein condensation (BEC) of dipolar excitons has been studied in a temperature range of 0.45–4.2 K. Photoexcited dipolar excitons have been accumulated in a lateral trap in a GaAs/AlGaAs Schottky diode with a 25-nm wide single quantum well with an electric bias applied across the heterolayers. Two-photon correlations have been measured with the use of a two-beam intensity interferometer with a time resolution of }~0.4 ns according to the well-known classical Hanbury-Brown-Twiss scheme. The photon bunching has been observed at the onset of Bose-Einstein condensation manifested by the appearance of a narrow exciton condensate line in the luminescence spectrum at an increase in the optical pumping (the line width near the threshold is ?200 μeV). At the same time, the two-photon correlation function itself obeys the super-Poisson distribution, g ⁽²⁾(τ) > 1, at time scale τ_c ? 1 ns of the system coherence. The photon bunching is absent at a pumping level substantially below the condensation threshold. The effect of bunching also decreases at pumping significantly above the threshold, when the narrow exciton condensate line starts to dominate in the luminescence spectra, and finally disappears with the further increase in the optical excitation. In this region, the distribution of pair photon correlations is a Poisson distribution manifesting the united quantum coherent state of the exciton condensate. Under the same conditions, the first-order spatial correlation function g ⁽¹⁾(r) determined from the interference pattern of the luminescence signals from the spatially separated parts of the condensate at constant pumping remains noticeable at distances of no less than 4 μm. The discovered effect of photon bunching is very sensitive to temperature and decreases by several times with a temperature increase in the range of 0.45–4.2 K. Assuming that the luminescence of the dipolar excitons directly reflects the coherence properties of the gas of interacting excitons, the discovered photon bunching at the onset of condensation, where the fluctuations of the exciton density and, consequently, of the luminescence intensity are most significant, indicates a phase transition in the interacting Bose gas of excitons, which is an independent way of detecting the Bose-Einstein condensation of excitons.     

The temperature dependence of the photoluminescence from overgrown GaAs/Al0.3Ga0.7As quantum dots and wires

Photoluminescence measurements on GaAs/Al_0.3Ga_0.7As quantum dots and wires fabricated using electron bears lithography and reactive ion etching are reported both before and after regrowth with a layer of Al_0.4Ga_0.6As. Dots exhibit little change in luminescence efficiency from the bulk with a reduction in diameter either before or after regrowth. Surface recombination therefore appears to be suppressed. In wires, however, luminescence intensity is very sensitive to wire width, decreasing rapidly with this parameter, but recovers and becomes independent of size after overgrowth. The temperature dependence of the photoluminescence from the dots and wires showed that dots and wires less than 150nm in width luminesced to higher temperatures than the larger diameter structures and dots liminesced to higher temperatures than wires of comparable width. This suggests that there is a finite coherence area effect which increases the radiative lifetimes of excitons in the quantum structures due to the geometric constraint, in the lateral direction in the wires and in all three directions in the dots. Below 20K bound exciton luminescence dominates in the dots but not in the wires. In wires it is still possible for the excitons to diffuse to nonradiative sites within the exciton lifetime. Regrowth at 750°C causes migration of aluminium into the quantum well and causes the shape of the well to become parabolic resulting shifts in the exciton emission to shorter wavelengths, making it difficult to separate the effect of processing from those due to quantum confinement.     

Spontaneous and stimulated red luminescence of Lu2O3: Eu nanocrystals

The spectra of spontaneous and stimulated luminescence of Lu₂O₃: Eu (7 at %) nanopowders at different optical pumping intensities have been investigated. The obtained results—changes in the shape of the red luminescence spectra and in the lifetime of the ⁵ D ₀ excited state of Eu³⁺ ions—indicate the onset of superluminescence with an increase in the excitation power. It has been found that an increase in the optical pumping intensity leads to a decrease in the luminescence decay time of the Lu₂O₃: Eu (7 at %) phosphor in the stimulated luminescence regime and to an increase in the quantum efficiency of red luminescence with a maximum at 611 nm.     

Measurement of the electronic dephasing time via the weak localization effect in a narrow channel

We have utilized the the weak localization effect in a narrow channel to measure the phase coherence time (τφ) at temperatures between 0.42 K and 4.25 K for electrons in a two-dimensional electron gas formed in a GaAs/Al_xGa_1-xAs heterostructure. The measured values agree well with electron-electron scattering theory in a one-dimensional channel including both single particle and collective contributions.     

Sensitivity to anharmonicity of vibrational energy in a diatomic gasdynamic laser

A parameter for evaluating the sensitivity of quantum vibrational energy to anharmonicity in a diatomic gasdynamic laser is defined and calculated by considering the corresponding diatomic molecules as quantum anharmonic oscillators under an interatomic Morse potential. The variation of the above parameter in terms of the vibrational states and in terms of an involved anharmonic coefficient is discussed. In particular, the parameter in question at the classical limit is examined. Both weak and strong anharmonicities are discussed.     

Kerr相互作用下量子相干性分布和量子信息流动

本文针对Kerr相互作用下系统中量子相干性的动力学分布进行了研究.所讨论系统包含两个没有相互作用的原子,每个原子都被囚禁在各自的光腔中,同时光腔被充满了非线性Kerr介质.研究发现非线性Kerr相互作用能够增加两原子间的量子相干性,而且增大的幅度会随着Kerr相互作用强度的增加而得以提高.其次,借助迹距离的方法,还探讨了非线性Kerr相互作用对于原子与光腔之间的量子信息流动的影响,发现Kerr相互作用可以加快量子信息回流到原子子系统中,抑制原子子系统与其余子系统间的量子信息交换,阻碍量子信息在系统中不同子系统间的流动,从而保护原子子系统中拥有的量子信息.     

双原子分子振动能级半量子化及量子理论的数值计算

利用半经典量子化理论和量子理论，分别采用Ｌｅｎｎａｒｄ－Ｊｏｎｅｓ势和Ｍｏｒｓｅ势，对双原子分子的振动能级给予了较为详细的数值计算。并将所得结果与部分实验数据进行比较，峄双原子分子的振动能级作了较为详细的 讨论。     

Influences of control coherence and decay coherence on optical bistability in a semiconductor quantum well

We discuss the influences of two different types of mechanisms of quantum coherence on optical bistability in a semiconductor quantum well structure.In the first mechanism,only quantum coherence induced by the resonant coupling of a strong control laser is considered.In the second mechanism,the decay coherence is taken into account under the condition where the control field is weak.In two different cases,optical bistability can be obtained through choosing appropriate physical parameters.Our studies show quantum coherence makes the optical nonlinear effect of the system become stronger,which takes an important role in the process of generating optical bistability.A semiconductor quantum well with flexibility and easy integration in design could potentially be exploited in real solid-state devices.     

Long lived coherence in self-assembled quantum dots

We report measurements of ultralong coherence in self-assembled quantum dots. Transient four-wave mixing experiments at 5 K show an average dephasing time of 372 ps, corresponding to a homogeneous linewidth of 3.5 microeV, which is significantly smaller than the linewidth observed in single-dot luminescence. Time-resolved luminescence measurements show a lifetime of the dot ground state of 800 ps, demonstrating the presence of pure dephasing at finite temperature. The homogeneous width is lifetime limited only at temperatures approaching 0 K.     

弱抽运下光学参量过程中压缩真空场的光子统计性质

在理论和实验上研究了光学参量振荡中产生的弱压缩真空场的光子统计行为. 弱压缩真空具有强烈的光子聚束效应,这种比热光场更强的聚束效应在量子光学和量子测量中具有重要的应用. 利用远离阈值的光学参量振荡(optical parametric oscillator, OPO )过程,在实验上产生了该弱压缩真空输出,运转波长在铯原子线附近. 通过Hanbury-Brown-Twiss(HBT)测量了OPO输出光场的二阶关联函数,实验结果与理论分析基本一致. 关键词： 压缩真空态 二阶相干度 光学参量振荡     

Cu(100)表面上H2/D2散射的六维态-态量子动力学研究：位点平均模型的有效性

基于由optPBE-vdW密度泛函计算的数千个数据点拟合得到的精确的神经网络势能面,本文采用含时波包方法对H₂/D₂在刚性Cu(100)表面上的态-态散射进行了六维量子动力学计算. 与以往的理论和实验比较了H₂和D₂在Cu(100)中的振转(非)弹性散射的结果. 特别是通过将六维的(非)弹性散射几率与从十五个位点加权平均四维几率的结果比较,测试了在该体系中位点平均近似模型的有效性. 具体来说,位点平均模型很好地重现了振动弹性散射几率,尽管对于高能下的振动非弹性散射结果没那么好. 结果说明在未来研究重双原子或多原子分子从金属表面的态-态散射动力学时,可以使用位点平均模型来降低全维计算过高的成本.     

Spin state selective coherence transfer: a method for discrimination and complete analyses of the overlapped and unresolved 1H NMR spectra of enantiomers

In general, the proton NMR spectra of chiral molecules aligned in the chiral liquid crystalline media are broad and featureless. The analyses of such intricate NMR spectra and their routine use for spectral discrimination of R and S optical enantiomers are hindered. A method is developed in the present study which involves spin state selective two dimensional correlation of higher quantum coherence to its single quantum coherence of a chemically isolated group of coupled protons. This enables the spin state selective detection of proton single quantum transitions based on the spin states of the passive nuclei. The technique provides the relative signs and magnitudes of the couplings by overcoming the problems of enantiomer discrimination, spectral complexity and poor resolution, permitting the complete analyses of the otherwise broad and featureless spectra. A non-selective 180 degrees pulse in the middle of MQ dimension retains all the remote passive couplings. This accompanied by spin selective MQ-SQ conversion leads to spin state selective coherence transfer. The removal of field inhomogeneity contributes to dramatically enhanced resolution. The difference in the cumulative additive values of chemical shift anisotropies and the passive couplings, between the enantiomers, achieved by detecting Nth quantum coherence of N magnetically equivalent spins provides enhanced separation of enantiomer peaks. The developed methodology has been demonstrated on four different chiral molecules with varied number of interacting spins, each having a chiral centre.     

Blue luminescence from the InGaN multiple quantum wells

We have fabricated very high-quality In_0.13Ga_0.87N/GaN multiple quantum wells with thickness as small as on (0 0 0 1) sapphire substrate using metal organic chemical vapour deposition (MOCVD). We have investigated these ultra-thin multiple quantum wells by continuous wave (cw) and time resolved spectroscopy in the picosecond time scales in a wide range of temperatures from 10 K to 290 K. In the luminescence spectrum at 10 K we observed a broad peak at 3.134 eV which was attributed to the quantum wells emission of InGaN. The full-width at half-maximum of this peak was 129 meV at 10 K and the broadening at low temperatures which was mostly inhomogeneous was thought to be due to compositional fluctuations and interfacial disorder in the alloy. The ultra narrow width of the quantum well was found to have a very profound effect in increasing the emission linewidth. We also observed an intense and narrow peak at 3.471 eV due to the GaN barrier. The temperature dependence of the luminescence was studied. The peak positions and intensities of the different peaks were obtained after a careful Lorentzian analysis. The activation energy of the InGaN quantum well emission peak was estimated as 69 meV. The lifetime of the quantum well emission was found to be 720 ps at 10 K. The results were explained by considering the localization of the excitons due to potential fluctuations. At higher temperatures the non-radiative recombination was found to be very dominant.     

中性原子量子计算研究进展

相互作用可控、相干时间较长的中性单原子体系具备在1 mm2的面积上提供成千上万个量子比特的规模化集成的优势,是进行量子模拟、实现量子计算的有力候选者.近几年中性单原子体系在实验上取得了快速的发展,完成了包括50个单原子的确定性装载、二维和三维阵列中单个原子的寻址和操控、量子比特相干时间的延长、基于里德伯态的两比特量子门的实现和原子态的高效读出等,这些工作极大地推动了该体系在量子模拟和量子计算方面的应用.本文综述了该体系在量子计算方面的研究进展,并介绍了我们在其中所做的两个贡献:一是实现了"魔幻强度光阱",克服了光阱中原子退相干的首要因素,将原子相干时间提高了百倍,使得相干时间与比特操作时间的比值高达105;二是利用异核原子共振频率的差异建立了低串扰的异核单原子体系,并利用里德伯阻塞效应首次实现了异核两原子的量子受控非门和量子纠缠,将量子计算的实验研究拓展至异核领域.最后,分析了中性单原子体系在量子模拟和量子计算方面进一步发展面临的挑战与瓶颈.