This work describes the use of a broadband spectral source for nonlinear spectroscopy to characterize various materials with potential applications in confocal microscopy, biological sample markers, optical limiting devices and optical switches. The goal is to study the spectrum of nonlinear absorption and the dispersion of nonlinear refraction as well as the dynamics of the nonlinearities by means of femtosecond excite­pro be experiments. The principle is quite simple: if a sample is under the influence of a strong fs excitation pulse and a pro be pulse beam is incident at the same time, or shortly after (within the decay time of the nonlinearity), then the probe pulse will sen_se the nonlinearity induced by the excitation. If the probe pulse is broadband, a femtosecond white-light continuum (WLC) in our case, we can monitor the nonlinearity induced over the entire continuum spectrum in one laser "shot". The use of femtosecond laser pulses to generate WLC will provide femtosecond time resolution for time-resolved spectroscopy. We built the nonlinear spectrometer and allowed for many degrees of flexibility in terms of choice of wavelengths for pump and pr9be beams and a dual detection system to cover both visible and infrared spectral ranges. We have the possibility of performing broad band spectral measurements using a spectrometer or selected narrow bandwidth probes incident on Si or Ge photodiodes for improved SIN ratios. The intrinsic properties of the continuum probe demand a careful characterization of its spatial and temporal profile. Know ledge of the dispersion of the index of refraction in various optical elements, including the sample itself, is also required for a correct analysis of the transient absorption raw data, especially for short time-scale dynamics of nonlinear processes. We tested the system using well-characterized semiconductor samples, and the results came out in excellent agreement with those from previous picosecond Z-scan measurements and theoretical modeling. With confidence, we can now measure various organic dyes with enhanced two-photon and excited-state absorption. Our setup is used to conduct a systematic study on similar compounds with modified molecular structures in order to learn about structure-property relations and draw guidelines for future design work.

Graduation Date





Lee, Chin H.


Master of Science (M.S.)


College of Engineering




138 p.




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Length of Campus-only Access


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Masters Thesis (Open Access)



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