钕离子掺杂和钕铝共掺高硅氧玻璃的光谱性质研究

基于多孔玻璃烧结的方法制备了钕离子掺杂和钕铝共掺高硅氧玻璃，测量了掺钕高硅氧玻璃的吸收光谱、荧光光谱和荧光寿命. 利用Judd-Ofelt理论计算得到了钕离子在高硅氧玻璃中的强度参数，计算并对比了掺钕高硅氧玻璃和钕铝共掺高硅氧玻璃的理论荧光寿命、受激发射截面和发光量子效率.讨论了钕铝共掺高硅氧玻璃中铝离子的掺入对玻璃发光性质的影响. 通过与其他掺钕氧化物玻璃和一些商用硅酸盐玻璃的主要光谱性质的比较，掺钕高硅氧玻璃显示了较好的光谱性质，有可能成为一种应用于高能和高频激光领域的新型激光材料. 关键词： 掺钕高硅氧玻璃 钕铝共掺 光谱性质 Judd-Ofelt理论     

基于不同泵浦波形的荧光寿命测量

该文从理论上分析了不同泵浦波形下的荧光衰减规律,提出了一种在不同泵浦波形下测量荧光寿命的新方法——双脉冲探测法,即利用探测泵浦脉冲与荧光衰减脉冲的方法测量荧光寿命。通过对样品钕玻璃及Cr:ZnSe晶体的荧光寿命测量表明:利用该方法在不同泵浦波形下能够实现可见及近红外到中红外激光介质的荧光寿命测量。因此,利用该测量方法能够方便、有效的避免通过解卷积求样品荧光寿命的繁琐过程,对测量激光介质在不同泵浦波形下的荧光寿命具有参考价值。     

A UV–Visible–NIR fluorescence lifetime imaging microscope for laser-based biological sensing with picosecond resolution

This article describes the design and characterization of a wide-field, time-domain fluorescence lifetime imaging microscopy (FLIM) system developed for picosecond time-resolved biological imaging. The system consists of a nitrogen-pumped dye laser for UV–visible–NIR excitation (337.1–960 nm), an epi-illuminated microscope with UV compatible optics, and a time-gated intensified CCD camera with an adjustable gate width (200 ps-10^-3 s) for temporally resolved, single-photon detection of fluorescence decays with 9.6-bit intensity resolution and 1.4-μm spatial resolution. Intensity measurements used for fluorescence decay calculations are reproducible to within 2%, achieved by synchronizing the ICCD gate delay to the excitation laser pulse via a constant fraction optical discriminator and picosecond delay card. A self-consistent FLIM system response model is presented, allowing for fluorescence lifetimes (0.6 ns) significantly smaller than the FLIM system response (1.14 ns) to be determined to 3% of independently determined values. The FLIM system was able to discriminate fluorescence lifetime differences of at least 50 ps. The spectral tunability and large temporal dynamic range of the system are demonstrated by imaging in living human cells: UV-excited endogenous fluorescence from metabolic cofactors (lifetime ∼1.4 ns); and 460-nm excited fluorescence from an exogenous oxygen-quenched ruthenium dye (lifetime ∼400 ns). Received: 23 February 2003 / Published online: 22 May 2003 RID="*" ID="*"Corresponding author. Fax: +1-734/9361-905, E-mail: mycek@umich.edu     

Lifetime measurements with the pinhole method in presence of radiation trapping: II—application to Yb<Superscript>3+</Superscript> doped ceramics and crystals

In this paper, we present an experimental verification of a theoretical model for the evaluation of the results of the so-called pinhole method for the measurement of the upper level lifetime in doped optical materials where the resonant reabsorption of the emitted fluorescence determines significant radiation trapping effects. As an experimental verification of the model, we measured the lifetime of the upper laser level of Yb³⁺ in various crystals and ceramic samples usually employed for the realization of solid state laser sources.     

Fluorescence-lifetime measurements in atmospheric-pressure flames using nanosecond-pulsed lasers

Measurements of fluorescence lifetimes are needed to quantify concentration measurements when using linear laser-induced fluorescence. However, lifetimes are only a few nanoseconds for many important species at atmospheric pressure. When using a typical Q-switched laser with a pulse width of about 10 ns, the fluorescence follows the shape of the laser pulse and the lifetime cannot be easily measured. In this paper, a technique is described for experimentally determining the fluorescence lifetime in atmospheric-pressure flames using a nanosecond-pulsed laser; that is, measurement of a lifetime an order-of-magnitude faster than the laser pulse itself. This technique relies on an observable temporal shift in the fluorescence signal as a function of the lifetime. Simulations show the efficacy of this approach, and data in liquid samples and in an atmospheric-pressure flame show excellent agreement with prior picosecond measurements. This technique is successful because only the temporal shift is examined and details of the fluorescence profile are ignored. Received: 23 August 2001 / Revised version: 19 November 2001 / Published online: 17 January 2002     

An efficient lasing action from pyrromethene 556 dye-doped organically modified silicates

Organically modified solid-state silicates (ORMOSILS) doped with a new laser dye 1,3,5,7,8-pentamethylpyrromethene-2,6-disulfonate-BF₂ complex (pyrromethene 556) have been synthesized by a sol-gel method and the compositional effects on pore characteristics, fluorescence and lasing properties have been investigated. It is found that the use of dimethylsulfoxide and γ-glycidoxypropyltrimethoxysilane could greatly change the structure properties of sol-gel derived ORMOSILS cage, and thus the fluorescence and lasing properties of the materials could improve significantly. A successful laser oscillation from this dye-doped ORMOSILS sample has been achieved upon pumping with a Q-switched frequency-doubled Nd:YAG laser at 532 nm. A slope efficiency of 54% with a useful lifetime greater than 10,000 shots has been demonstrated at a pump repetition rate of 1 Hz and a pump intensity of 1 J/cm² by using the new ORMOSILS cage on our newly designed laser system. Our results have shown that it is possible to obtain a high-efficiency with a long-lifetime for a compact new laser device by low cost dye-doped solid-state ORMOSILS.     

基于激光诱导叶绿素荧光寿命成像技术的植物荧光特性研究

针对植物荧光遥感探测中信号易受干扰的问题, 提出了一种用于评估植物生长状况及环境监测的荧光寿命成像技术. 采用凹透镜对355 nm波长的激光扩束, 再照射植物激发叶绿素荧光, 由增强型电荷耦合器件接收荧光信号. 采用时间分辨测量法, 连续用相同激光脉冲照射植物以激发相同的荧光信号, 同时不断改变激光脉冲触发探测器启动的延时时间, 从而能够得到完整的离散荧光信号分布图像. 对植物特定位置点产生的离散荧光信号进行拟合, 再运用一种改进型的迭代解卷积法可反演高精度的荧光寿命; 进而反演图像各点的荧光寿命以生成植物的荧光寿命分布图. 该方法所绘制的荧光寿命图比荧光强度图能更准确地反映植物内部的叶绿素含量, 并对活体植物叶绿素荧光寿命的物理特性进行了初步研究, 证明叶绿素荧光寿命与植物生理状态存在一定关联; 并且叶绿素荧光寿命与活体植物所处环境存在着复杂的关系. 未来将与生物物理学家们合作, 继续探寻叶绿素荧光寿命与植物生存环境的关系.     

Tunable Two-Frequency Lasers for Lifetime Measurements

We built a compact two-tunable-frequency longitudinally pumped solid-state laser specially designed to measure atomic lifetimes. Weak coupling between the laser eigenstates permits the obtaining of a continuously tunable frequency difference between 0 and 10 GHz. Such a source provides either a linear polarization rotating at such frequencies, or a sinusoidally modulated intensity with a 100% modulation amplitude. As an example, the fluorescence lifetime of the first excited state of Cr⁴⁺ in YAG is measured in the zero-fluence limit using a two-frequency Nd:YAG laser at 1064 nm.     

用时间分辨光谱研究红细胞悬液的荧光发射

实验获得了激光照射红细胞悬液的荧光光谱,并分别监测不同荧光峰值波长处强度随时间的衰变过程,测试了其相应的荧光寿命。结果表明,在波长为407nm的激光照射下,红细胞悬液向外发射中心波长分别位于596,628,692nm的荧光光谱,各荧光峰对应衰变过程的平均荧光寿命分别为1.97,13.31,14.58ns。利用荧光强度和吸收率的加和性表示了混合物的总吸收率和总荧光发射强度,通过理论计算获得了红细胞悬液中锌卟啉、原卟啉和其他游离物参与荧光发射的相对含量和相对强度在不同荧光峰位的变化关系,进一步解释了不同峰位处荧光发射强度和平均荧光寿命的变化原因。     

Radiation-power broadening of the Na-D lines in a vapour cell

We have measured the time-resolved fluorescence spectrum of both Na-D lines in a vapour cell. The atoms were excited with a spectrally broadband pulsed dye laser, tuned to resonance. The width of the Na-D lines turned out to be a linear function of the laser intensity, as is predicted by a simple theory based on lifetime considerations. The experimental results are in quantitative agreement with this theory.     

Fluorescence saturation measurements of 3-pentanone

The saturation characteristics of 3-pentanone fluorescence were investigated in an ambient temperature and pressure cell by imaging the fluorescence produced by a focused quadrupled Nd:YAG laser beam. The onset of fluorescence saturation was observed at laser fluences around 0.06 J/cm², which is only about 1.3% of estimates that assume a two-level model and use measured values of the fluorescence lifetime and absorption cross-section. A spatially resolved model indicated that the saturation fluence changed only 10% when a Gaussian profile was used instead of a top-hat profile. Laser sources with significantly different temporal profiles will have different threshold fluence levels, but the present results suggest that saturation effects should be monitored in planar laser-induced fluorescence imaging experiments using 3-pentanone.     

A study of the fluorescence lifetime of Pr3+ in SBN40

The fluorescence lifetime τ₁ of Pr³⁺ doped in the ferroelectric solid solution SNB40 (Ba_0.4Sr_0.6Nb₂O₆) was measured ar various temperatures. The fluorescence lifetime decreases gradually with increasing temperature. Furthermore, an anomalous increase of τ₁ was observed at a specific temperature. The fluorescence linewidth and the peak wavelength of fluorescence also showed an anomalous change at this temperature. It is likely that this phenomenon is due to the phase transition of the host crystal SBN40.     

激光诱导叶绿素荧光寿命的测量及其特性分析

提出了一种用于评估植物生长状况及环境监测的激光诱导叶绿素荧光寿命测量方法. 采用波长355 nm的激光作为光源激发叶绿素荧光, 由光电倍增管接收其荧光信号, 由于被测叶绿素荧光衰减函数与激光脉冲、仪器响应函数卷积在一起, 根据它们的特性, 运用时间分辨测量法分别测得叶绿素荧光及其背景信号, 并结合一种新型解卷积算法可分离出真实的叶绿素荧光衰减函数, 从而获取叶绿素的荧光寿命. 测试结果表明: 该方法能够实现叶绿素荧光寿命的高精度实时监测, 对不同叶绿素含量的溶液荧光寿命进行了测试, 证明叶绿素含量与其荧光寿命具有相关性, 并且拟合了叶绿素含量与荧光寿命的标定曲线. 关键词： 荧光寿命 激光诱导荧光 时间分辨测量法 叶绿素含量     

Mid-infrared photo-luminescence and energy transfer around 2.8 μm from Dy3+/Tm3+ co-doped tellurite glass

Tellurite glasses co-doped with Dy³⁺ and Dy³⁺/Tm³⁺ have been synthesized. Emission around 2.8 μm is successfully obtained in present glass upon excitation of a conventional 808 nm laser diode. Judd-Ofelt intensity parameters and radiative properties of Dy³⁺ ions are calculated using the Judd-Ofelt theory. The luminescence characteristics and energy transfer mechanism are investigated and discussed. According to the absorption, fluorescence spectra and lifetime measurements, Tm³⁺ ions can effectively absorb excitation and transfer their energy to Dy³⁺ ions with high efficiency (up to 86.80%). Hence, the results demonstrate that Dy³⁺/Tm³⁺ co-doped tellurite glasses possessing excellent spectroscopic properties is a potential medium for mid-infrared laser.     

Tunable room-temperature cw laser action in Cr3+: GdScGa-Garnet

We report for the first time on tunable room temperature cw laser action of a transition metal laser material. In Cr³⁺:GdScGa-garnet crystals almost the total fluorescence is channelled into the broad band⁴ T ₂→⁴ A ₂ transition. The fluorescence lifetime is τ=120 μs. Laser pumping in the blue-green and yellow-red spectral range yields pump thresholds around 250 mW and slope efficiencies up to 11%. The wavelength of the free running Cr³⁺ laser is centered at 777 nm.     

Laser linewidth effects in intensity correlations in resonance fluorescence

The influence of partially coherent light on photon correlations in resonance fluorescence is discussed. We show that the laser bandwidth changes the intensity correlations in a very different way depending on whether the Rabi oscillation is greater or smaller than the natural lifetime of the excited state. For low intensity excitation we predict a generalization of the Heitler-Weisskopf effect extended to intensity correlations. A comparison with an inhomogenous theory of laser band-width is also presented.     

Determination of the effective upper laser level lifetime from an end-pumped Tm,Ho:YLF laser

We report the measurement of the effective upper laser level lifetime from an end-pumped Q-switched Tm,Ho:YLF laser. When the pump power is 1.58 W, the effective upper laser level lifetime is only 2.5 ms, which is less than the fluorescence lifetime (∼16 ms) of the upper laser level. The dependences of the effective upper laser level lifetime on the pump power and the temperature of laser crystal are firstly obtained experimentally. The experimental results show that the effective upper laser level lifetime decreases with increasing the pump power and the temperature of laser crystal, respectively. Furthermore, the experimental results are compared with the theoretical results.     

凝聚相有机分子的激发能传递研究(Ⅱ)——激光染料二甲基-POPOP和DCM分子间的激发能传递

利用荧光发射及其衰变动力学测量,研究了激光染料分子二甲基-POPOP和DCM在溶液中的分子间能量传递。所得结果证实:激发态二甲基-POPOP分子荧光被猝灭的程度,随所加入DCM浓度的增大而增大。尽管DCM的荧光寿命随二甲基-POPOP的猝灭而增加。然而,DCM的加入并不改变二甲基-POPOP的荧光寿命。在固定DCM浓度,而增加二甲基-POPOP浓度时,相似的结果同样被观测到。这些结果表明:激发态二甲基-POPOP分子通过辐射传能机理向基态DCM传递激发能,其结果将入射光的波长从紫外直接转换到波长大于600nm的光谱区。在本文中也简要讨论了进一步改善这一传能过程效率的措施。     

Characterization of Standard Reference Material 2941, uranyl-ion-doped glass, spectral correction standard for fluorescence

Standard Reference Material^® (SRM^®) 2941 is a cuvette-shaped, uranyl-ion-doped glass, recommended for use for relative spectral correction of emission and day-to-day performance validation of fluorescence spectrometers. Properties of this standard that influence its effective use or contribute to the uncertainty in its certified emission spectrum have been explored here. These properties include its photostability, absorbance, dissolution rate in water, anisotropy, temperature coefficient of fluorescence intensity, and fluorescence lifetimes. The expanded uncertainties in the certified spectrum are about 4% around the peak maximum at 526 nm, using an excitation wavelength of 427 nm. The SRM also exhibits a strong resistance to photodegradation, with no measurable decrease in fluorescence intensity even after 8 h of laser irradiation.     

Radiative lifetimes of excited W II levels

Radiative lifetimes of 19 selected W II levels with energies between 36 000 cm^-1 and 55 000 cm^-1 have been measured with the time-resolved laser-induced fluorescence technique. The ions are generated in a hollow cathode discharge and stored in a linear Paul trap. Selected states are populated with tunable dye laser pulses and the subsequent fluorescence is measured by means of a 5 Gigasample transient digitizer and a fast photodetector with a risetime of 700 ps. By taking into account both the temporal profile of the laser pulses and the separately measured response function of the system, the lifetime can be determined from the full decay curve. A refined evaluation procedure, taking into account saturation effects in the signals, reduces the uncertainty in our data to around 1%. Received: 30 July 1998 / Revised: 18 August 1998