Ultrafast photovoltaic responses in ferroelectric thin films

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Abstract/Contents

Abstract
The interaction of ultrashort light pulses with the medium of the ferroelectric is a fundamental question for photonics and photovoltaic applications. I report two advances toward our understanding of this family of materials in the ultrafast regime: (1) Using femtosecond time-resolved x-ray scattering to observe changes in the unit-cell tetragonality of thin films of the prototypical ferroelectric lead titanate, PbTiO3, we show the direction, magnitude and physical mechanisms underlying the photocurrents generated by femtosecond near-bandgap photoexcitation. These findings elucidate the ultrafast photovoltaic response in these ma- terials, illustrate the intrinsic coupling between their electronic and structural degrees of freedom, and show that light can enhance the functional properties of ferroelectrics on nanosecond timescales. In addition, we observe that femtosecond optical pulses can reversibly switch the ferroelectric phase to the non-polar paraelectric phase. (2) In order to further investigate mechanisms for using light to manipulate the ferroelectric polarization, a terahertz (THz) pulse source based on coherent transition radiation has been commissioned, which generates single-cycle pulses lasting roughly 100 fs with peak fields greater than 20 MV/cm and energies in excess of 100 uJ. These pulses contain frequencies resonant with the "soft mode" reaction coordinate of the ferroelectric-paraelectric phase transition, and their high peak fields drive strong nonlinear optical responses in materials. As a first demonstration, I show that this source drives an all-THz response in a silicon photodiode. Recent work shows that such pulses should permit purely optical steering of the ferroelectric polarization.

Description

Type of resource text
Form electronic; electronic resource; remote
Extent 1 online resource.
Publication date 2012
Issuance monographic
Language English

Creators/Contributors

Associated with Daranciang, David Dan Ramelb
Associated with Stanford University, Department of Chemistry
Primary advisor Lindenberg, Aaron Michael
Thesis advisor Lindenberg, Aaron Michael
Thesis advisor Chidsey, Christopher E. D. (Christopher Elisha Dunn)
Thesis advisor Reis, David A, 1970-
Advisor Chidsey, Christopher E. D. (Christopher Elisha Dunn)
Advisor Reis, David A, 1970-

Subjects

Genre Theses

Bibliographic information

Statement of responsibility David Dan Ramelb Daranciang.
Note Submitted to the Department of Chemistry.
Thesis Thesis (Ph.D.)--Stanford University, 2012.
Location electronic resource

Access conditions

Copyright
© 2012 by David Dan Ramelb Daranciang
License
This work is licensed under a Creative Commons Attribution Non Commercial No Derivatives 3.0 Unported license (CC BY-NC-ND).

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