Slides for PowerPoint: Nonlinear and Two-Dimensional Spectroscopy

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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 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

Fourier transform 2D IR spectroscopy

Ultrafast nonlinear spectroscopy mask

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

Peak Shift Measurement ta – tb (fs)

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

2D IR Spectroscopy in pump-probe geometry

Obtaining an Absorptive 2D IR Spectrum

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

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

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

Extra Graphics

2D Lineshapes

Rephasing and Non-rephasing

Rephasing and Non-rephasing

2D IR Spectrum of RDC in Hexane

2D IR Spectrum of RDC in Hexane

Polarization-Selective 2D IR Spectroscopy

Projection Angle from Peak Amplitudes