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Slides for PowerPoint: Nonlinear and Two-Dimensional Spectroscopy

Slides for PowerPoint: Nonlinear and Two-Dimensional Spectroscopy. Andrei Tokmakoff MIT Department of Chemistry. Complete Slides. Why 2D IR Spectroscopy?. IR spectroscopy IR probes vibrations intrinsic to all molecules Each vibration gives different information Structure and dynamics

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Slides for PowerPoint: Nonlinear and Two-Dimensional Spectroscopy

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  1. Slides for PowerPoint: Nonlinear and Two-Dimensional Spectroscopy Andrei Tokmakoff MIT Department of Chemistry

  2. Complete Slides

  3. Why 2D IR Spectroscopy? • IR spectroscopy • IR probes vibrations intrinsic to all molecules • Each vibration gives different information • Structure and dynamics • Intrinsic time-scale of ~1 ps • 2D IR spectroscopy: A more sensitive probe • Characterize vibrational correlations • Couplings, orientation, exchange • Resolves congested spectra & suppresses inhomogeneous broadening • Quantitative structure-based modeling

  4. Fourier transform 2D IR spectroscopy

  5. Ultrafast nonlinear spectroscopy mask

  6. Polarization-selective pump-probe experiment Magic Angle: Vibrational Lifetime Anisotropy: Reorientation

  7. ta – tb (fs) Peak Shift Measurement

  8. 2D IR Interferometer time/frequency detection time/time detection

  9. 2D IR Spectroscopy in pump-probe geometry

  10. Obtaining an Absorptive 2D IR Spectrum

  11. 2D IR spectroscopy • Related to the joint probability t2 = 0 t2 > tc Frequency Fluctuations Vibrational Couplings Chemical Exchange

  12. Chemical exchange and spectral diffusion • Excite: Initial frequency w1 • Wait for period t2 • Detect: Final frequency w3 t2 →  t2 = 0

  13. Absorptive a b 2D lineshapes: Loss of frequency correlation Phase Ellipticity Phase slope

  14. Extra Graphics

  15. 2D Lineshapes

  16. Rephasing and Non-rephasing

  17. Rephasing and Non-rephasing

  18. 2D IR Spectrum of RDC in Hexane

  19. 2D IR Spectrum of RDC in Hexane

  20. Polarization-Selective 2D IR Spectroscopy

  21. Projection Angle from Peak Amplitudes

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