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裂变碎片撞击CO-NH₃和CO-NH₃-H₂O冰中引起的二次离子发射:CO-NH₃冰结构的改变

Secondary ion emission induced by fission fragment impact in CO-NH(3) and CO-NH(3)-H(2)O ices: modification in the CO-NH(3) ice structure.

作者信息

Martinez R, Farenzena L S, Iza P, Ponciano C R, Homem M G P, de Brito A Naves, Wien K, da Silveira E F

机构信息

Physics Department, Pontifícia Universidade Católica, 22543-900 Rio de Janeiro RJ, Brazil.

出版信息

J Mass Spectrom. 2007 Oct;42(10):1333-41. doi: 10.1002/jms.1241.

Abstract

CO-NH(3) and CO-NH(3)-H(2)O ices at 25-130 K were bombarded by (252)Cf fission fragments ( approximately 65 MeV at the target surface) and the emitted secondary ions were analyzed by time-of-flight mass spectrometry (TOF-SIMS). It is observed that the mass spectra obtained from both ices have similar patterns. The production of hybrid ions (formed from CO and NH(3) molecules) emitted from CO-NH(3) ice has already been reported by R. Martinez et al., Int. J. Mass. Spectrom. 262 (2006) 195; here, the secondary ion emission and the modifications of the CO--NH(3) ice structure during the temperature increase of the ice are addressed. These studies are expected to throw light on the sputtering from planetary and interstellar ices and the possible formation of new organic molecules in CO-NH(3)-H(2)O ice by megaelectronvolt ion bombardment. The presence of water in the CO-NH(3) ice mixture generates molecular ion series such as (NH(3))(p-q)(H(2)O)(q)CO(+) and replaces the cluster series (NH(3))(n)NH(4) (+) emission by the hybrid series (NH(3))(I-i)(H(2)O)(i=1, 2...I)H(+). The distribution of NH(3) and H(2)O molecules within the cluster groups indicates that ammonia and water mix homogeneously in the icy condensate at T = 25 K. The desorption yield distribution of the cluster series (NH(3))(n)NH(4) (+) is described by the sum of two exponential functions: one, slow-decreasing, attributed to the fragmentation of the solid target into clusters; and another, fast-decreasing, due to a local sublimation followed by recombination of ammonia molecules. The analysis of the time-temperature dependence of these two yield components gives information on the formation process of molecular ions, the transient composition of the ice target and structural changes of the ice. Data suggest that the amorphous and porous structure of the NH(3) ice, formed by the condensation of the CO--NH(3) gas at T = 25 K, survives CO sublimation until the occurrence of a phase transition around 80 K, which produces a more fragile ice structure.

摘要

用(252)Cf裂变碎片(在靶表面能量约为65兆电子伏)轰击25 - 130K温度下的CO - NH₃和CO - NH₃ - H₂O冰,并用飞行时间质谱(TOF - SIMS)分析发射出的二次离子。观察到从两种冰获得的质谱图有相似的模式。R. Martinez等人在《国际质谱杂志》262卷(2006年)第195页已经报道了从CO - NH₃冰发射出的混合离子(由CO和NH₃分子形成);在此,研究了冰升温过程中二次离子发射以及CO - NH₃冰结构的变化。这些研究有望阐明行星和星际冰的溅射以及兆电子伏离子轰击CO - NH₃ - H₂O冰中可能形成新有机分子的情况。CO - NH₃冰混合物中存在水会产生诸如(NH₃)(p - q)(H₂O)(q)CO⁺这样的分子离子系列,并将簇系列(NH₃)(n)NH₄⁺发射替换为混合系列(NH₃)(I - i)(H₂O)(i = 1, 2...I)H⁺。簇团组内NH₃和H₂O分子的分布表明,在T = 25K时,氨和水在冰冷凝物中均匀混合。簇系列(NH₃)(n)NH₄⁺的解吸产率分布由两个指数函数之和描述:一个是缓慢下降的,归因于固体靶碎裂成簇;另一个是快速下降的,由于局部升华随后氨分子重新组合。对这两个产率分量的时间 - 温度依赖性分析给出了关于分子离子形成过程、冰靶的瞬态组成以及冰结构变化的信息。数据表明,在T = 25K时由CO - NH₃气体冷凝形成的NH₃冰的无定形和多孔结构在CO升华后仍然存在,直到在80K左右发生相变,相变产生更脆弱的冰结构。

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