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Asian Journal of Physics Vol 32, Nos 1 & 2 (2023) 11-20

Systematic study of the effect of small-molecules on the low-frequency Raman spectrum of water

Julian Hniopeka,b, Julian Plitzkoa,b, James Carrierec, Peter Vogtd, Michael Schmitta and Jürgen Poppa,b
aInstitute for Physical Chemistry and Abbe Center of Photonics,
Friedrich Schiller University Jena, Helmholtzweg 4, 07743, Jena, Germany.
bLeibniz Institute of Photonic Technology (IPHT), Member of Leibniz Research Alliance – Leibniz Health Technologies and of the Leibniz Centre for Photonics in Infection Research (LPI), Albert-Einstein-Str. 9, 07745, Jena, Germany.
cCoherent, Inc.- Ondax, 850 E. Duarte Rd., Monrovia, CA 91016, United States of America.
d Coherent Shared Services B.V., Dieselstrasse 5b, 64807 Dieburg, Germany.

Low-frequency Raman, which is Raman spectroscopy focused onto the wavenumber region below 100 cm–1, has gained considerable interest over the last decades due to better availability of instrumentation. However, so far it has mostly been restricted to the investigation of solid structures, where clear features are present. For dissolved, especially aqueous, samples, the use of low-frequency Raman is hindered by a lack of sharp features and strong background signal of water. Nevertheless, by influencing hydrogen bonding, dissolved species affect the low-frequency spectrum of water. To use these changes analytically, a systematic knowledge of the effects is necessary. Therefore, we present a systematic study of the effect of small molecules ranging from apolar to salts on the low-frequency spectrum of water. Changes to the hydrogen-bonding associated vibrations could be detected for all molecules that correlate well with their physicochemical properties. Furthermore, by employing two-dimensional correlation spectroscopy, it could be revealed that the changes to the hydrogen bonding environment often follow more complicated complex mechanisms, which helps to understand the mechanism behind hydrogen bonding in heterogenous systems. The present study is a first step to understand the low-frequency spectra of aqueous solutions. © Anita Publications. All rights reserved.
Keywords: Low-frequency Raman, THz-spectroscopy, 2D correlation spectroscopy, hydrogen-bonding.

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References

  1. Yarwood J, Spectroscopic studies of intermolecular forces in dense phases, Annual Reports Section C (Physical Chemistry), 76(1979)99–130.
  2. Nielsen O F, Low-frequency spetroscopic studies of interactions in liquids, Annual Reports Section C (Physical Chemistry), 90(1993)3–44.
  3. Bērziņš K, S. J. Fraser-Miller S J, Recent advances in low-frequency Raman spectroscopy for pharmaceutical applications, Gordon K C, Int J Pharm, 592(2021)120034; doi.org/10.1016/j.ijpharm.2020.120034.
  4. Ueno Y, Ajito K, Analytical terahertz spectroscopy, Anal Sci, 24(2008)185–192.
  5. Shuang B, Wang C X, Xia L, Xu B, Zhang S L, Stray light in low wavenumber Raman spectra and secondary maxima of grating diffraction, J Raman Spectrosc, 42(2011)2149–2153.
  6. Ivanda M, Babocsi K, Dem C, Schmitt M, Montagna M, Kiefer W, Low-wave-number Raman scattering from CdSxSe1–x quantum dots embedded in a glass matrix, Phys Rev B, 67(2003)235329; doi.org/10.1103/PhysRevB.67.235329.
  7. Carriere J T A, Havermeyer F, Ultra-low frequency Stokes and anti-Stokes Raman spectroscopy at 785 nm with volume holographic grating filters, Proc SPIE 8219, Biomedical Vibrational Spectroscopy V: Advances in Research and Industry, 821905, 2012.
  8. Heyler R A, Carriere J T A, Havermeyer F, THz-Raman: accessing molecular structure with Raman spectroscopy for enhanced chemical identification, analysis, and monitoring, Proc SPIE 8726, Next-Generation Spectroscopic Technologies VI, 87260J, 2013.
  9. Mariotto G, Montagna M, Viliani G, Campostrini R, Carturan G, Low-frequency Raman scattering in thermally treated silica gels: observation of phonon-fracton crossover, J Phys C: Solid State Physics, 21(1988)L797; doi.10.1088/0022-3719/21/22/005.
  10. Kostić R, Aškrabić S, Dohčević-Mitrović Z, Popović Z V, Scattering from CeO2 nanoparticles, Appl Phys A, 90(2008)679–683.
  11. Holomb R, Mitsa V, Johansson P, Veres M, Boson peak in low-frequency Raman spectra of AsxS100–x glasses: nanocluster contribution, Phys Status Solidi C, 7(2010)885–888.
  12. Noda I, Roy A, Carriere J, Sobieski B J, Chase D B, Rabolt J F, Two-dimensional Raman correlation spectroscopy study of poly [(R)-3-hydroxybutyrate-co-(R)-3-hydroxyhexanoate] copolymers, Appl Spectrosc, 71(2017)1427–1431.
  13. Larkin P J, Dabros M, Sarsfield B, Chan E, Carriere J T, Smith B C, Polymorph Characterization of Active Pharmaceutical Ingredients (APIs) Using Low-Frequency Raman Spectroscopy, Appl Spectrosc, 68(2014)758–776.
  14. Damle V H, Aviv H, Tischler Y R, Identification of Enantiomers Using Low-Frequency Raman Spectroscopy, Anal Chem, 94(2022)3188–3193.
  15. Suresh S J, Satish A V, Choudhary A, Influence of electric field on the hydrogen bond network of water, J Chem Phys, 124(2006)074506; doi.org/10.1063/1.2162888.
  16. Hniopek J, Schmitt M, Popp J, Bocklitz T, PC 2D-COS: A Principal Component Base Approach to Two-Dimensional Correlation Spectroscopy, Appl Spectrosc, 74(2020)460–472.
  17. Padró J A, Martı J, An interpretation of the low-frequency spectrum of liquid wateŕ, J Chem Phys, 118(2003)452; doi.org/10.1063/1.1524619.
  18. Mizoguchi K, Hori Y, Tominaga Y, Study on dynamical structure in water and heavy water by low-frequency Raman spectroscopy, J Chem Phys, 97(1992)1961; doi.org/10.1063/1.463133.
  19. Kusalik P G, Svishchev I M, The spatial structure in liquid water, Science, 265(1994)1219–1221.
  20. Corsaro R D, Atkinson G, Ultrasonic Investigation of Acetic Acid Hydrogen Bond Formation. II Acetic Acid–Water Solutions, J Chem Phys, 55(1971)1971; doi.org/10.1063/1.1676336.
  21. Noda I, Generalized two-dimensional correlation method applicable to infrared, Raman, and other types of spectroscopy, Appl Spectrosc, 47(1993)1329–1336.
  22. Noda I, Dowrey A E, Marcott C, Story G M, Ozaki Y, Generalized two-dimensional correlation spectroscopy, Appl Spectrosc, 54(2000)236A–248A.
  23. Noda I, Close-up view on the inner workings of two-dimensional correlation spectroscopy, Vib Spectrosc, 60(2012)146–153.
  24. Te J A, Tan M.-L, Ichiye T, Solvation of glucose, trehalose, and sucrose by the soft-sticky dipole–quadrupole–octupole water model, Chem Phys Lett, 491(2010)218–223.
  25. Liu J, Yan Y, Yan Y, Zhang J, Tetrahydrofuran (THF)-Mediated Structure of THF·(H2O)n=1–10: A Computational Study on the Formation of the THF Hydrate, Crystals, 9(2019)73; doi.org/10.3390/cryst9020073.
  26. Czarnecki M A, Interpretation of two-dimensional correlation spectra: science or art?, Appl Spectrosc, 52(1998)1583–1590.
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