1. Direct measurements of multi-photon induced nonlinear lattice dynamics in semiconductors via time-resolved x-ray scattering
- Author
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Wonhuyk Jo, Sooheyong Lee, G. Jackson Williams, Michael Watson, Eric C. Landahl, Dong Ryeol Lee, and Donald A. Walko
- Subjects
Diffraction ,Materials science ,Photon ,Physics::Optics ,02 engineering and technology ,01 natural sciences ,Molecular physics ,Article ,law.invention ,Gallium arsenide ,Crystal ,Condensed Matter::Materials Science ,chemistry.chemical_compound ,law ,0103 physical sciences ,010306 general physics ,Multidisciplinary ,business.industry ,Scattering ,021001 nanoscience & nanotechnology ,Laser ,Semiconductor ,chemistry ,0210 nano-technology ,business ,Excitation - Abstract
Nonlinear optical phenomena in semiconductors present several fundamental problems in modern optics that are of great importance for the development of optoelectronic devices. In particular, the details of photo-induced lattice dynamics at early time-scales prior to carrier recombination remain poorly understood. We demonstrate the first integrated measurements of both optical and structural, material-dependent quantities while also inferring the bulk impulsive strain profile by using high spatial-resolution time-resolved x-ray scattering (TRXS) on bulk crystalline gallium arsenide. Our findings reveal distinctive laser-fluence dependent crystal lattice responses, which are not described by previous TRXS experiments or models. The initial linear expansion of the crystal upon laser excitation stagnates at a laser fluence corresponding to the saturation of the free carrier density before resuming expansion in a third regime at higher fluences where two-photon absorption becomes dominant. Our interpretations of the lattice dynamics as nonlinear optical effects are confirmed by numerical simulations and by additional measurements in an n-type semiconductor that allows higher-order nonlinear optical processes to be directly observed as modulations of x-ray diffraction lineshapes.
- Published
- 2016
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