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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Luminescence of Atomic Barium in Rare Gas Matrices: A Two-Dimensional Excitation/Emission Spectroscopy Study
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Luminescence of Atomic Barium in Rare Gas Matrices: A Two-Dimensional Excitation/Emission Spectroscopy Study

机译：稀有气体矩阵中原子钡的发光：二维激发/发射光谱研究

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A detailed characterization is made of the distinct sites occupied by atomic barium isolated in the three rare gas hosts Ar, Kr, and Xe in excitation scans extracted from the recorded total 6s6p P-1(1) - (6s)(2) S-1(0) fluorescence. Extensive use has been made of two-dimensional excitation/emission (2D-EE) spectroscopy to achieve a comprehensive characterization for the wide variety of sites present in the Ba/RG matrix systems. The 2D-EE technique has proved to be a very powerful method to probe the effects of strong intersite reabsorption when extensive spectral overlap occurs between emission and resonance 6s6p P-1( )- (6s)(2) S-1(0) absorption of barium atoms occupying multiple sites. Two-dimensional excitation/emission scans have also been used in this study to monitor the effects of sample annealing and thereby identify the thermally stable sites of isolation. Sites of the same type occupied by atomic barium in the three host solids are identified in resolved excitation spectra and are associated on the basis of the observed matrix shift versus host polarizability. Following site associations, the photophysical properties of each matrix site were characterized revealing that the Stokes shift was greatest in the blue site, smallest for the violet site, and intermediate for the green site. The emission temperature dependences and excited state lifetimes were recorded, indicating that measured radiative lifetimes of 4-5 ns were in good agreement with the gas phase value of 8.4 ns when corrected for the effective field of the solids. The only exception to this was the blue site in Ba/Xe, where a nonradiative quenching channel exists even at 9.8 K that competes effectively with the nanosecond fluorescence. An unusual, asymmetric 2 + 1 excitation band has been recorded for atomic barium in the three rare gas hosts in addition to the threefold split, Jahn-Teller bands typically observed for P - S absorptions of matrix-isolated metal atoms. Possible assignm
机译：详细表征由三种稀有气体宿主Ar，Kr和Xe中分离的原子钡占据的不同位点，从记录的总6S6P P-1（1） - ＆GT中提取的激发扫描中。 （6S）（2）S-1（0）荧光。已经由二维激发/发射（2D-EE）光谱进行了广泛的用途，以实现BA / RG矩阵系统中存在的各种网站的综合表征。已经证明，当在发射和共振6S6P P-1（）＆（6S）（2）S-1（0）之间发生广泛的光谱重叠时，2D-EE技术是探测强的谱重叠时强的频谱重叠当发生广泛的光谱重叠时的效果。（6S）（2）S-1（0 ）吸收钡原子占用多个位点。本研究也使用二维激发/发射扫描来监测样品退火的影响，从而识别隔离的热稳定位点。在分辨的激发光谱中鉴定出三个宿主固体中的原子钡占据的相同类型的位点，并且基于观察到的矩阵偏移与主体极化性相关联。在现场关联之后，每个基质部位的光物理性质的表征揭示了斯托克斯班次在蓝地中最大，对于紫罗兰地点而言，以及绿色部位的中间体。记录发射温度依赖性和激发的状态寿命，表明当校正固体有效场时，4-5 ns的测量辐射寿命与8.4ns的气体相值很好。唯一的例外是Ba / XE中的蓝色部位，即使在9.8k中，甚至存在与纳秒荧光有效竞争的9.8k。除了三重分裂之外，还记录了三个稀有气体宿主中的原子钡的异常，不对称的2 + 1激发带，其通常观察到的基质隔离金属原子的P＆LT。可能的分配

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