Nonlinear optics, measurement techniques, z scan


This dissertation describes the development of novel techniques for characterization of nonlinear properties of materials. The dissertation is divided into two parts, a background and theory section and a technique development section. In the background and theory section we explain the origins of the nonlinear optical response of materials across many different spatial and temporal scales. The mechanisms that we are most interested in are the electronic nuclear and reorientational responses, which occur on the range of sub-femtosecond to several picoseconds. The electronic mechanism is due to the electrons of a material experiencing a non-parabolic potential well due a strong electric field and occurs on the sub-femtosecond timescale. The nuclear or vibrational effect results from the motion of the nuclei of the atoms and typically occurs on the order of a few hundred femtoseconds. Finally the reorientational nonlinearity is due to the alignment of the molecule to the electric field, which alters the polarizability of the molecule and typically occurs on the scale of a few picoseconds. There are other mechanisms can induce nonlinear optical effects such as thermal effects and electrostriction, but these effects typically occur on much larger timescales than we are interested in, and hence will not be a major focus of this dissertation. In the nonlinear characterization techniques section, we describe previous research into the field of nonlinear optical characterization techniques, describing the techniques used to characterize the nonlinear properties of materials, their applications and limitations. We will trace the development of two recently developed techniques for nonlinear spectroscopy − the Dual Arm iii Z-Scan and the Beam Deflection techniques. The Dual Arm Z-Scan technique is an enhancement of the standard Z-Scan technique that allows for the measurement of small nonlinear signals in the presence of large background signals. This technique allows for the measurement of materials under certain conditions not previously measureable using the standard Z-Scan technique, such materials with low damage thresholds, poor solubility and thin films. In addition to the Dual Arm Z-Scan, we have developed a new method for characterizing nonlinear refraction, the Beam Deflection technique, which is a variation of the photothermal beam deflection technique previously used to measure very weak absorption signals. This technique offers relative ease of use, the ability to measure the absolute magnitude and sign of both the real and imaginary parts of � (3) simultaneously with high sensitivity. We fully develop the theory for materials with instantaneous and non-instantaneous nonlinearities, with nonlinear absorption and group velocity mismatch. We also demonstrate the power of this technique to separate the isotropic and reorientational contributions of liquids by examining the temporal response and polarization dependences. Lastly, we summarize our conclusions and describe two promising future research directions that would benefit from the Dual Arm Z-Scan and Beam Deflection techniques


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Graduation Date





Hagan, David J.


Doctor of Philosophy (Ph.D.)


College of Optics and Photonics


Optics and Photonics

Degree Program

Optics and Photonics








Release Date

May 2014

Length of Campus-only Access


Access Status

Doctoral Dissertation (Open Access)


Dissertations, Academic -- Optics and Photonics, Optics and Photonics -- Dissertations, Academic