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Quantitative Anisotropic Analysis of Molecular Orientation in Amorphous N2O at 6 K by Infrared Multiple-Angle Incidence Resolution Spectrometry

Cite this: J. Phys. Chem. Lett. 2020, 11, 18, 7857–7866
Publication Date (Web):September 8, 2020
https://doi.org/10.1021/acs.jpclett.0c01585
Copyright © 2020 American Chemical Society

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    Abstract

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    The existence of molecular orientational order in nanometer-thick films of molecules has long been implied by surface potential measurements. However, direct quantitative determination of the molecular orientation is challenging, especially for metastable amorphous thin films at low temperatures. This study quantifies molecular orientation in amorphous N2O at 6 K using infrared multiple-angle incidence resolution spectrometry (IR-MAIRS). The intensity ratio of the weak antisymmetric stretching vibration band of the 14N15NO isotopomer between the in-plane and out-of-plane IR-MAIRS spectra provides an average molecular orientation angle of 65° from the surface normal. No discernible change is observed in the orientation angle when a different substrate material is used (Si and Ar) at 6 K or the Si substrate temperature is changed in the range of 6–14 K. This suggests that the transient mobility of N2O during physisorption is key in governing the molecular orientation in amorphous N2O.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.0c01585.

    • Typical single-beam spectra measured at an angle of incidence of 45° at various polarization angles from 0° (s-polarization) to 90° (p-polarization) in 15° steps before the MAIRS analysis (Figures S1 and S2); IP and OP spectra of the ν3 band of amorphous CH4 at 6 K calculated assuming n = 1.33 (Figure S3); photograph of Si substrate connected with copper sample holder with indium solder by ultrasonic soldering (Figure S4); summary of AIP, n4HAOP, 2AIPn4HAOP, and orientation angle α for the ν3 band of amorphous CH4 on a Si substrate at 6 K (Table S1); summary of the dependence of the n (n4H) value on AIP, n4HAOP, 2AIPn4HAOP, and orientation angle α for the ν3 band of amorphous CH4 on a Si substrate at 6 K (Table S2); summary of AIP, n4HAOP, 2AIPn4HAOP, and orientation angle α for the 14N14NO ν3 band of amorphous N2O on a Si substrate at 6 K (Table S3) (PDF)

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    Cited By

    This article is cited by 5 publications.

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    2. Andrew Cassidy, Martin R. S. McCoustra, David Field. A Spontaneously Electrical State of Matter. Accounts of Chemical Research 2023, 56 (14) , 1909-1919. https://doi.org/10.1021/acs.accounts.3c00094
    3. Wei-Chih Wang, Kyohei Nakano, Daisuke Hashizume, Chain-Shu Hsu, Keisuke Tajima. Tuning Molecular Conformations to Enhance Spontaneous Orientation Polarization in Organic Thin Films. ACS Applied Materials & Interfaces 2022, 14 (16) , 18773-18781. https://doi.org/10.1021/acsami.2c03496
    4. Takumi Nagasawa, Naoki Numadate, Tetsuya Hama. Infrared multiple‐angle incidence resolution spectrometry for vapor‐deposited amorphous water. Journal of Raman Spectroscopy 2022, 53 (10) , 1748-1772. https://doi.org/10.1002/jrs.6377
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