Bulletin of the Korean Chemical Society

Korean Chemical Society (대한화학회)
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Extracting Frequency-Frequency Correlation Function from Two-Dimensional Infrared Spectroscopy: Peak Shift Measurement

  • Received : 2012.07.13
  • Accepted : 2012.07.20
  • Published : 2012.10.20
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Abstract

Two-dimensional infrared (2D-IR) spectroscopy can probe the fast structural evolution of molecules under thermal equilibrium. Vibrational frequency fluctuation caused by structural evolution produced the time-dependent line shape change in 2D-IR spectrum. A variety of methods has been used to connect the evolution of 2D-IR spectrum with Frequency-Frequency Correlation Function (FFCF), which connects the experimental observables to a molecular level description. Here, a new method to extract FFCF from 2D-IR spectra is described. The experimental observable is the time-dependent frequency shift of maximum peak position in the slice spectrum of 2D-IR, which is taken along the excitation frequency axis. The direct relation between the 2D-IR peak shift and FFCF is proved analytically. Observing the 2D-IR peak shift does not need the full 2D-IR spectrum which covers 0-1 and 1-2 bands. Thus data collection time to determine FFCF can be reduced significantly, which helps the detection of transient species.

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References

  1. Cho, M. Bull. Korean Chem. Soc. 2006, 27, 1940. https://doi.org/10.5012/bkcs.2006.27.12.1940
  2. Zheng, J. R.; Kwak, K.; Asbury, J.; Chen, X.; Piletic, I. R.; Fayer, M. D. Science 2005, 309, 1338. https://doi.org/10.1126/science.1116213
  3. Zheng, J. R.; Kwak, K. W.; Xie, J.; Fayer, M. D. Science 2006, 313, 1951. https://doi.org/10.1126/science.1132178
  4. Kwak, K. W.; Park, S.; Fayer, M. D. Proc. Natl. Acad. Sci. U. S. A. 2007, 104, 14221. https://doi.org/10.1073/pnas.0701710104
  5. Kim, Y. S.; Hochstrasser, R. M. J. Phys. Chem. B 2009, 113, 8231. https://doi.org/10.1021/jp8113978
  6. Fayer, M. D. Accounts Chem. Res. 2012, 45, 3. https://doi.org/10.1021/ar2000088
  7. Hamm, P.; Zanni, M. Concepts and Methods of 2D Infrared Spectroscopy; Cambridge University Press: UK, 2011.
  8. Cho, M. Two-Dimensional Optical Spectroscopy; CRC Press: 2009.
  9. Mukamel, S. Annu. Rev. Phys. Chem. 2000, 51, 691. https://doi.org/10.1146/annurev.physchem.51.1.691
  10. Roberts, S. T.; Loparo, J. J.; Tokmakoff, A. J. Chem. Phys. 2006, 125.
  11. Asbury, J. B.; Steinel, T.; Kwak, K.; Corcelli, S. A.; Lawrence, C. P.; Skinner, J. L.; Fayer, M. D. J. Chem. Phys. 2004, 121, 12431. https://doi.org/10.1063/1.1818107
  12. Kwak, K.; Park, S.; Finkelstein, I. J.; Fayer, M. D. J. Chem. Phys. 2007, 127.
  13. Kwak, K.; Rosenfeld, D. E.; Fayer, M. D. J. Chem. Phys. 2008, 128.
  14. Kim, Y. S.; Liu, L.; Axelsen, P. H.; Hochstrasser, R. M. Proc. Natl. Acad. Sci. U. S. A. 2009, 106, 17751. https://doi.org/10.1073/pnas.0909888106
  15. Finkelstein, I. J.; Ishikawa, H.; Kim, S.; Massari, A. M.; Fayer, M. D. Proc. Natl. Acad. Sci. U. S. A. 2007, 104, 2637. https://doi.org/10.1073/pnas.0610027104
  16. Shim, S. H.; Zanni, M. T. Phys. Chem. Chem. Phys. 2009, 11, 748. https://doi.org/10.1039/b813817f
  17. Chung, J. K.; Thielges, M. C.; Fayer, M. D. Proc. Natl. Acad. Sci. U. S. A. 2011, 108, 3578. https://doi.org/10.1073/pnas.1100587108

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