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As described in our original proposal, the goal of this project is to create a new type of engineered nonlinear optical material, orientation-patterned GaAs, and use it to demonstrate improved high-power coherent mid-infrared sources. Considerable effort has been devoted over the past decade to the development of mid-IR coherent sources based on nonlinear optical frequency conversion, e.g., optical parametric oscillator (OPOs), pumped by available high-power near-IR sources such as diode-laser-pumped solid-state lasers or near-IR diode lasers themselves. The rapid development of quasiphasematched materials, especially periodically-poled ferroelectrics, has revolutionized this field for wavelengths in the 2-4 micrometers region. At 4 to 5 micrometers absorption limits the maximum power attainable to the range of several watts, and operation is entirely precluded in the 8 to 12 micrometers band. The orientation-patterned GaAs that we are developing is intended to complement periodically-poled ferroelectrics, providing a lithographically-engineerable low-loss material for high power devices at wavelengths beyond 4 micrometers.
This dissertation deals with the generation of parametric light in the range 1 to 12 μm. Parametric infrared generation turns out to be a challenge at the interface between the fields of nonlinear optics and materials science embodied by the two approaches used to achieve efficient frequency conversion. Birefringent Phase-Matching (BPM) in anisotropic materials has been the traditional solution used in most frequency converter devices. But since the 90's, the quick success of microstructured materials has paved the way for Quasi-Phase-Matching (QPM) even in isotropic materials, leading to a renewed interest in Optical Parametric Oscillators (OPO). The high degree of engineering offered by this technology is now widely recognized as a key competitive advantage. We obtained original results concerning parametric infrared generation using BPM as well as QPM.We have built the first OPO pumped by a 1.064 μm Nd:YAG laser and based on a 5-mm-thick crystal of 5%MgO:PPLN cut as a partial cylinder. This OPO combines a wide and continuous tunability over the range 1.4 μm - 4.4 μm with a good conversion efficiency, up to 30%. Despite the need to resort to pump intensities almost an order of magnitude higher than in a slab OPO, we have shown that the energetical performance of a partial cylinder OPO is now equivalent to that of a slab OPO besides a wider tunability that can be continuously addressed. When the same Nd:YAG laser pumps two such independent OPOs in parallel, we dispose of a highly versatile QPM dual wavelength source with two widely and independently tunable beams. We have built this unique source allowing versatile Difference Frequency Generation (DFG) towards the mid- and far- infrared. We carried out the first BPM DFG experiments with this source in a CdSe slab oriented for angular noncritical phase-matching at two different pump wavelengths, respectively 2.72 μm and 2.79 μm. The second set of DFG experiments were performed in a CdSe crystal cut and polished as a 5-mm-diameter full cylinder. Using a pump wavelength of 2.79 μm, we were able to tune the DFG wavelength from 8.3 μm up to 10.3 μm by rotating the crystal over an angular range of 18°. Contrary to all the BPM DFG experiments reported so far in the single crystal CdSe, tuning was achieved while keeping normal incidence of both the incident and generated beams in the crystal. The implementation of spectral narrowing techniques is already anticipated and will contribute to more accurate measurements of the phase-matching directions of a crystal as well as to a higher DFG conversion efficiency.These experiments with our dual wavelength source are preliminary and encouraging validations of our capability of performing DFG in small crystals and at any pump wavelength between 1.4 μm and 3.5 μm. Even though we investigated the promises held by CdSiP2 when it is only pumped with a Nd:YAG laser at 1.064 μm, there is tremendous prospect in terms of tunable infrared generation between 3.5 μm and 8 μm when this crystal is pumped around 2.4 μm. Such early demonstrations will be highly valuable for future applications requiring compact and tunable sources spanning the infrared spectrum. From a more fundamental point of view, performing DFG experiments at different pump wavelengths in the mid-infrared can lead to a highly accurate determination of the values of the refractive indices of a nonlinear crystal. In this dissertation, we have cast the first stone of a method that leads to the determination of the values of the refractive indices of a nonlinear crystal in the mid- to far- infrared. This new method is based on the unique measurements of the DFG phase-matching angles in spheres or cylinders, and should contribute to further advances in the field of phase-matching metrology.
Coherent optical sources in the mid-infrared region (mid-IR) are important fundamental tools for infrared countermeasures and battlefield remote sensing. Nonlinear optical effects can be applied to convert existing near-IR laser sources to radiate in the mid-IR. This research focused on achieving such a conversion with a quasi-phase matched optical parametric oscillators using orientation-patterned gallium arsenide (OPGaAs), a material that can be quasi- phased matched by periodically reversing the crystal structure during the epitaxial growth process. Although non-linear optical conversion was not ultimately achieved during this research, many valuable lessons were learned from working with this material. This thesis reviews the theory of nonlinear optics and explores the importance of accurate refractive index measurements to proper structure design. The details of four nonlinear optical experiments are presented recommendations are offered for the design of future OPGaAs crystals. Recommendations are also made for improved experimental techniques.
Coherent optical sources in the mid-infrared region (mid-IR) are important fundamental tools for infrared countermeasures and battlefield remote sensing. Nonlinear optical effects can be applied to convert existing near-IR laser sources to radiate in the mid-IR. This research focused on achieving such a conversion with a quasi-phase matched optical parametric oscillators using orientation-patterned gallium arsenide (OPGaAs), a material that can be quasi-phased matched by periodically reversing the crystal structure during the epitaxial growth process. Although non-linear optical conversion was not ultimately achieved during this research, many valuable lessons were learned from working with this material. This thesis reviews the theory of nonlinear optics and explores the importance of accurate refractive index measurements to proper structure design. The details of four nonlinear optical experiments are presented recommendations are offered for the design of future OPGaAs crystals. Recommendations are also made for improved experimental techniques.
The ability to manipulate frequency of light, through parametric frequency conversion sources based on X(2) nonlinear materials, offers an effective route to spectral regions unapproachable by conventional lasers. Most importantly, three-wave mixing processes provide tunable coherent radiation over a broad spectral range. Among the most important tunable devices, narrow linewidth continuous-wave (cw) infrared (IR) optical parametric oscillators (OPOs) are indispensable excitation sources for many applications in molecular spectroscopy and precision metrology. In order to exploit such applications, the development of cw OPOs deploying different wavelength tuning schemes and novel nonlinear materials is highly dezirable, as presented in this thesis. We demonstrated a rapidly tunable cw OPO based on fan-out grating design periodically-poled KTiOPO4 (PPKTP) crystal at room temperature. This approach allows continuous wavelength tuning by avoiding increased thermal fluctuations at higher operating crystal temperatures. The 532 nm-pumped, output-coupled singly-resonant oscillator (OC-SRO) provides widely tunable near-IR radiation across 741-922 nm and 1258-1884 nm, with total output power of 1.65 W. The use of output coupling for the resonating wave reduces thermal loading and enables 30% enhancement in the OPO extraction efficiency over the pure SRO configuration. Towards the goal of developing a next-generation cw source >4 μm using a new found quasi-phase-matched semiconductor material, orientation-patterned gallium phosphide (OP-GaP), we demonstrated the first realization of a tunable cw mid-IR source based on OP-GaP by exploiting single-pass difference-frequency-generation (DFG) between a Tm-fiber laser at 2010 nm and a home-built OPO based on MgO-doped periodically-poled LiNbO3 (MgO:PPLN) crystal. The DFG source generates up to 43 mW of output power, with >30 mW across 96% of the tuning range 4608-4694 nm, in high beam quality. As the tunable mid-IR sources are making great strides, the availabilityof fast and sensitive mid-IR detectors become equally important. However, the conventional mid-IR detectors demand cryogenic systems for low-noise operation which sets a major drawback as these devices are often bulky and expensive. In this context, the nonlinear frequency upconversion technique has emerged as a promising alternative to the direct detection of mid-IR radiation at room temperature. An upconversion detector (UCD) can be further optimized by identifying and suppressing its noise sources. In order to do so, we experimentally and theoretically investigated noise properties of 1064 nm-pumped single-pass UCD designed for signal detection in telecom and mid-IR range using MgO:PPLN crystals. We studied the dependence of newly discovered SHG (532 nm)-induced spontaneous parametric downconversion (SHG-SPDC) noise intensity on the pump power and crystal temperature, and compared it with the well-known UCD noise source upconverted spontaneous parametric downconversion (USPDC). The measurements deduce that SHG-SPDC must be given a careful consideration since it can act as a dominant noise source under certain operating conditions. However, SHG-SPDC can be avoided by choosing a proper combination of MgO:PPLN grating period,operating temperature, and bandpass filter.
The book describes the most advanced techniques for generating coherent light in the mid-infrared region of the spectrum. These techniques represent diverse areas of photonics and include heterojunction semiconductor lasers, quantum cascade lasers, tunable crystalline lasers, fiber lasers, Raman lasers, and optical parametric laser sources. Offering authoritative reviews by internationally recognized experts, the book provides a wealth of information on the essential principles and methods of the generation of coherent mid-infrared light and on some of its applications. The instructive nature of the book makes it an excellent text for physicists and practicing engineers who want to use mid-infrared laser sources in spectroscopy, medicine, remote sensing and other fields, and for researchers in various disciplines requiring a broad introduction to the subject.