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Includes bibliographical references (pages 180-188).
This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections.
This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections.
This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections.
Coherent two-dimensional infrared (2D IR) spectroscopy is used as a tool for investigating the molecular structure and dynamics of coupled vibrations in solution on a picosecond timescale. The strongly coupled asymmetric and symmetric carbonyl stretches of Rh(CO)₂C₅H₇0₂ (RDC) dissolved in hexane serve as a convenient model system. Fourier transform 2D IR spectra are obtained from heterodyne-detected third-order nonlinear signals using a sequence of broad bandwidth femtosecond IR pulses. A 2D IR correlation spectrum with absorptive lineshapes results from the addition of 2D rephasing and non-rephasing spectra, which sample conjugate frequencies in the evolution time period. The 2D IR correlation spectrum contains peaks with different positions, signs, amplitudes and lineshapes. The positions of the peaks map the transition frequencies b...
This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections.
Includes bibliographical references (leaves 82-85).