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Nonlinear Optical Effects in the Picosecond Regime for Chemical Sensing and Polycrystalline Semiconductor Frequency Conversion
Abstract
In this work, we employ nonlinear optical spectroscopic techniques using picosecond visible, near-IR, and mid-IR laser pulses to resolve knowledge gaps in light-matter interactions of organic molecules and semiconductors. Nonlinear optics provides an array of different and unique capabilities compared to linear optics including dual-detection of IR-active vibrational modes and Raman-active modes of biomolecules and the generation of broadband IR continuum using high harmonic generation in polycrystalline semiconductors like zinc selenide.
Sections 2-4 utilize hyper-Raman scattering to study biomolecules in solution. In Section 2, we outline the design of a hyper-Raman microscope and present early work on dual detection of Raman and hyper-Raman scattered light from biomolecules. In Section 3, the hyper-Raman microscope system was used to explore the hyper-Raman allowed transitions of organic molecules in solution, and polarization resolved spectra of biomolecules was reported. In Section 4, we utilize the sensitivity of hyper-Raman to water librations to study water solvation chemistry in a mixed solution of water with dimethyl sulfoxide.
Sections 5-6 study high harmonic generation (HHG) in poly-crystalline Zinc Selenide (poly-ZnSe). Sections 5 and 6 contrast each other by performing the same experiment in different laser excitation regimes. In Section 5/6, the experiment is performed using high power (TW/cm2)/lower power (GW/cm2), broadband/narrowband, femtosecond (100 fs)/picosecond (30 ps), mid-IR laser pulses. In Section 5, we observe efficient frequency conversion via HHG resulting in a broad supercontinuum spanning the near-IR and visible region, a result that has been replicated by other research groups. However, understanding this efficient conversion is complicated by numerous nonlinear effects simultaneously occurring in the material. In Section 6, we approach frequency conversion in poly-ZnSe at lower power at the threshold of HHG generation to study the different nonlinear effects that contribute to broadband continuum generation. We find that random quasi-phase matching is an essential ingredient to the efficient frequency conversion in disordered, polycrystalline semiconductors like poly-ZnSe.
Subject
OpticsOptical spectroscopy
Nonlinear spectroscopy
Chemical sensing
Hyper-Raman spectroscopy
Hyper-Raman scattering
Raman spectroscopy
Raman scattering
Visible Laser
Picosecond laser
Ultraviolet
Organic molecules
Biomolecules
Hyper-Raman signal of biomolecules
Water
Dimethyl sulfoxide
Methanol
Ethanol
D-glucose
L-alanine
L-arabinose
L-tartaric acid
Hydrogen bonding
Semiconductors
Optical properties of semiconductors
Polycrystalline semiconductor materials
Zinc selenide
Random quasi-phase matching
Harmonic generation
High harmonic generation
Self-focusing
Self-phase modulation
Supercontinuum generation
Filamentation
Femtosecond laser
Ultrafast laser
Mid-infrared laser
Near-infrared
Laser-eye safety standards
ANSI Z136.1
Citation
Marble, Christopher Brian (2023). Nonlinear Optical Effects in the Picosecond Regime for Chemical Sensing and Polycrystalline Semiconductor Frequency Conversion. Doctoral dissertation, Texas A&M University. Available electronically from https : / /hdl .handle .net /1969 .1 /200022.
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