As a result of their ability to amplify input light, ultra-high quality factor (Q) whispering gallery mode optical resonators fabricated from silica have demonstrated extremely low threshold Raman lasing behavior. However, the efficiency of the lasing has been poor due to the intrinsic low Raman gain of silica (~5%). By grafting oriented monolayers of highly nonlinear organic small molecules to the surface of conventional silica whispering gallery mode optical resonators, we demonstrate a new strategy for fabricating Raman lasers. The laser efficiency is improved from 4% to over 40%. Density functional theory is performed to understand the mechanism giving rise to the improvement. This chemistry-based approach could be applied to nearly any whispering gallery mode cavity geometry to improve performance, providing a universal strategy for device performance improvement.
Whispering gallery mode optical resonators integrated on silicon have demonstrated low threshold Raman lasers. One of the primary reasons for their success is their ultra-high quality factors (Q) which result in an amplification of the circulating optical field. Therefore, to date, the key research focus has been on maintaining high Q factors, as that determines the lasing threshold and linewidth. However, equally important criteria are lasing efficiency and wavelength. These parameters are governed by the material, not the cavity Q. Therefore, to fully address this challenge, it is necessary to develop new materials. We have synthesized a suite of metal-doped silica and small molecules to enable the development of higher performance Raman lasers. The efficiencies and thresholds of many of these devices surpass the previous work. Specifically, the silica sol-gel lasers are doped with metal nanoparticles (eg Ti, Zr) and are fabricated using conventional micro/nanofabrication methods. The intercalation of the metal in the silica matrix increases the silica Raman gain coefficient by changing the polarizability of the material. We have also made a new suite of small molecules that intrinsically have increased Raman gain values. By grafting the materials to the device surface, the overall Raman gain of the device is increased. These approaches enable two different strategies of improving the Raman efficiency and threshold of microcavity-based lasers.
As a result of their ability to amplify input light, ultra-high quality factor (Q) whispering gallery mode optical resonators have found numerous applications spanning from basic science through applied technology. Because the Q is critical to the device’s utility, an ever-present challenge revolves around maintaining the Q factor over long timescales in ambient environments. The counter-approach is to increase the nonlinear coefficient of relevance to compensate for Q degradation. In the present work, we strive to accomplish both, in parallel. For example, one of the primary routes for Q degradation in silica cavities is the formation of water monolayers. By changing the surface functional groups, we can inhibit this process, thus stabilizing the Q above 100 million in ambient environments. In parallel, using a machine learning strategy, we have intelligently designed, synthesized, and verified the next generation of small molecules to enable ultra-low threshold and high efficiency Raman lasing. The molecules are verified using the silica microcavity as a testbed cavity. However, the fundamental design strategy is translatable to other whispering gallery mode cavities.
High quality whispering gallery mode resonators can greatly enhance the optical field by trapping the light through total internal reflection, which makes these resonators a promising platform for many areas of research, including optical sensing, frequency combs, Raman lasing and cavity QED. Among these resonators, silica microtoroidal resonators are widely used because of their ability to be integrated and to achieve ultrahigh quality factors (above 100 million). However, quality factors of traditional silica toroids gradually decrease over time because there is an intrinsic layer of hydroxyl groups on the silica surface. This layer of hydroxyl groups attracts water molecules in the atmosphere and results in high optical losses. This property of silica degrades the behavior and limits the applications of the integrated silica toroids. In this work, we address this limitation by fabricating integrated microtoroids from silicon oxynitride. The surface of silicon oxynitride has a mixture of hydroxyl groups and fluorine groups. This mixture prevents the formation of a layer of water molecules that causes the optical losses. Our experiments demonstrate that the quality factors of the silicon oxynitride toroids exceed 100 million, and these values are maintained for over two weeks without controlling the storage conditions. As a comparison, quality factors of traditional silica toroids fabricated and stored under same conditions decayed by approximately an order of magnitude over the same duration.
Optical cavities are able to confine and store specific wavelengths of light, acting as optical amplifiers at those wavelengths. Because the amount of amplification is directly related to the cavity quality factor (Q) (or the cavity finesse), frequency comb research has focused on high-Q and ultra-high Q microcavities fabricated from a range of materials using a variety of methods. In all cases, the comb generation relies on a nonlinear process known as parametric frequency conversion which is based on a third order nonlinear interaction and which results in four wave mixing (FWM). Clearly, this approach requires significant optical power, which was the original motivation for using ultra-high-Q cavities. In fact, the majority of research to date has focused on pursuing increasingly high Q factors. However, another strategy is to improve the nonlinearity of the resonator through intelligently designing materials for this application. In the present work, a suite of nanomaterials (organic and inorganic) have been intelligently designed with the explicit purpose to enhance the nonlinearity of the resonator and reducing the threshold for frequency comb generation in the near-IR. The nanomaterials do not change the structure of the comb and only act to reduce the comb threshold. The silica microcavity is used as a testbed for initial demonstration and verification purposes. However, the fundamental strategy is translatable to other whispering gallery mode cavities.
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