On the Fresnel factor correction of sum-frequency generation spectra of interfacial water

被引:16
作者
Yu, Xiaoqing [1 ]
Chiang, Kuo-Yang [1 ]
Yu, Chun-Chieh [1 ]
Bonn, Mischa [1 ]
Nagata, Yuki [1 ]
机构
[1] Max Planck Inst Polymer Res, Ackermannweg 10, D-55128 Mainz, Germany
关键词
MOLECULAR-ORIENTATION; AIR/WATER INTERFACE; VAPOR INTERFACE; SURFACE; SPECTROSCOPY; DYNAMICS; TIME; CRYSTALLINE; CHEMISTRY;
D O I
10.1063/5.0133428
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Insights into the microscopic structure of aqueous interfaces are essential for understanding the chemical and physical processes on the water surface, including chemical synthesis, atmospheric chemistry, and events in biomolecular systems. These aqueous interfaces have been probed by heterodyne-detected sum-frequency generation (HD-SFG) spectroscopy. To obtain the molecular response from the measured HD-SFG spectra, one needs to correct the measured ssp spectra for local electromagnetic field effects at the interface due to a spatially varying dielectric function. This so-called Fresnel factor correction can change the inferred response substantially, and different ways of performing this correction lead to different conclusions about the interfacial water response. Here, we compare the simulated and experimental spectra at the air/water interface. We use three previously developed models to compare the experiment with theory: an advanced approach taking into account the detailed inhomogeneous interfacial dielectric profile and the Lorentz and slab models to approximate the interfacial dielectric function. Using the advanced model, we obtain an excellent quantitative agreement between theory and experiment, in both spectral shape and amplitude. Remarkably, we find that for the Fresnel factor correction of the ssp spectra, the Lorentz model for the interfacial dielectric function is equally accurate in the hydrogen (H)-bonded region of the response, while the slab model underestimates this response significantly. The Lorentz model, thus, provides a straightforward method to obtain the molecular response from the measured spectra of aqueous interfaces in the H-bonded region.
引用
收藏
页数:5
相关论文
共 50 条
  • [22] A Theoretical Investigation of Surface-enhanced Sum-frequency Generation
    Yeh, Y. L.
    Lei, J.
    Chen, S. Y.
    Chang, A. H. H.
    Lin, C. K.
    He, R. X.
    Lin, S. H.
    JOURNAL OF THE CHINESE CHEMICAL SOCIETY, 2016, 63 (01) : 136 - 144
  • [23] Revisiting the basic theory of sum-frequency generation
    Shen, Y. R.
    JOURNAL OF CHEMICAL PHYSICS, 2020, 153 (18)
  • [24] Sum-Frequency Generation Spectroscopy of an Adsorbed Monolayer of Mixed Surfactants at an Air-Water Interface
    Saha, Ankur
    Upadhyaya, Hari P.
    Kumar, Awadhesh
    Choudhury, Sipra
    Naik, Prakash D.
    JOURNAL OF PHYSICAL CHEMISTRY C, 2014, 118 (06) : 3145 - 3155
  • [25] Time-dependent vibrational sum-frequency generation spectroscopy of the air-water interface
    Ojha, Deepak
    Kaliannan, Naveen Kumar
    Kuehne, Thomas D.
    COMMUNICATIONS CHEMISTRY, 2019, 2 (1)
  • [26] The mature years of Sum-Frequency Generation are ahead
    Guyot-Sionnest, P
    SURFACE SCIENCE, 2005, 585 (1-2) : 1 - 2
  • [27] Vibrational Sum-Frequency Spectrum of the Water Bend at the Air/Water Interface
    Vinaykin, Mikhail
    Benderskii, Alexander V.
    JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 2012, 3 (22): : 3348 - 3352
  • [28] Communication: Vibrational sum-frequency spectrum of the air-water interface, revisited
    Ni, Yicun
    Skinner, J. L.
    JOURNAL OF CHEMICAL PHYSICS, 2016, 145 (03)
  • [29] Bulklike Vibrational Coupling of Surface Water Revealed by Sum-Frequency Generation Spectroscopy
    Chiang, Kuo-Yang
    Yu, Xiaoqing
    Yu, Chun-Chieh
    Seki, Takakazu
    Sun, Shumei
    Bonn, Mischa
    Nagata, Yuki
    PHYSICAL REVIEW LETTERS, 2023, 131 (25)
  • [30] Structure and sum-frequency generation spectra of water on uncharged Q4 silica surfaces: a molecular dynamics study
    Smirnov, Konstantin S.
    PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2020, 22 (04) : 2033 - 2045