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Crystallites and Electric Fields in Solid Ammonia
ChemistryOpen ( IF 2.5 ) Pub Date : 2020-07-16 , DOI: 10.1002/open.202000118
Andrew Cassidy 1 , Rachel L James 2 , Anita Dawes 2 , David Field 1
Affiliation  

Absorption spectra of vacuum‐deposited films of ammonia have been obtained in the range 115 nm to 310 nm for a set of 15 deposition temperatures, Td, between 20 K and 80 K. Results focus upon the region 115 nm to 130 nm in overlapping D, E, F and G←X Rydberg transitions involving Wannier‐Mott excitons. We identify two phases of ammonia, showing the solid to be polymorphic. Peak absorption wavelengths in the region of interest are found to shift to the red by 299 cm−1, for Td between 20 K to 50 K, and 1380 cm−1 for Td between 55 K to 80 K. Shifts provide evidence for the presence of spontaneously generated electric fields in these films, of values in excess of 108 V m−1 for Td of 20 K to 50 K to a few times 107 V m−1 for 55 K to 80 K. Results enable us to place a lower limit of 1.58 nm on the size of crystallites in the low temperature regime. This dimension represents 16 unit cells or 64 species, giving a more quantitative description than the nebulous term amorphous, as applied to solid ammonia. We also determine that crystallites formed in the high temperature regime contain, within ±20 %, 1688, 756 and 236 molecules of ammonia, respectively at Td of 65 K, 60 K and 55 K.

中文翻译:


固体氨中的微晶和电场



在 20 K 至 80 K 之间的一组 15 个沉积温度 T d下,在 115 nm 至 310 nm 范围内获得了氨真空沉积膜的吸收光谱。结果集中在重叠的 115 nm 至 130 nm 区域。 D、E、F 和 G←X 里德伯跃迁涉及万尼尔-莫特激子。我们确定了氨的两相,表明该固体是多晶型的。我们发现,对于 T d在 20 K 至 50 K 之间,感兴趣区域的峰值吸收波长向红色移动 299 cm -1 ,对于 T d在 55 K 至 80 K 之间,峰值吸收波长向红色移动 1380 cm -1 。这些薄膜中存在自发产生的电场,对于 20 K 至 50 K 的 T d ,其值超过 10 8 V m -1 ,对于 55 K 至 80 K,其值超过 10 7 V m -1几倍。我们将低温状态下微晶尺寸的下限设置为 1.58 nm。这个维度代表 16 个晶胞或 64 个物质,比用于固体氨的模糊术语“无定形”给出了更定量的描述。我们还确定,在 T d为 65 K、60 K 和 55 K 时,在高温状态下形成的微晶在 ±20% 范围内分别含有 1688、756 和 236 个氨分子。
更新日期:2020-07-16
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