Abstract Diamond has attracted great interest as an appealing material for various applications ranging from classical to quantum optics. To date, Raman lasers, single photon sources, quantum sensing and quantum communication have been demonstrated with integrated diamond devices. However, studies of the nonlinear optical properties of diamond have been limited, especially at the nanoscale. Here, a metasurface consisting of plasmonic nanogap cavities is used to enhance both χ (2) and χ (3) nonlinear optical processes in a wedge-shaped diamond slab with a thickness down to 12 nm. Multiple nonlinear processes were enhanced simultaneously due to the relaxation of phase-matching conditions in subwavelength plasmonic structures by matching two excitation wavelengths with the fundamental and second-order modes of the nanogap cavities. Specifically, third-harmonic generation (THG) and second-harmonic generation (SHG) are both enhanced 1.6 × 10 7 -fold, while four-wave mixing is enhanced 3.0 × 10 5 -fold compared to diamond without the metasurface. Even though diamond lacks a bulk χ (2) due to centrosymmetry, the observed SHG arises from the surface χ (2) of the diamond slab and is enhanced by the metasurface elements. The efficient, deeply subwavelength diamond frequency converter demonstrated in this work suggests an approach for conversion of color center emission to telecom wavelengths directly in diamond.
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Nonlinear Strong Coupling by Second‐Harmonic Generation Enhancement in Plasmonic Nanopatch Antennas
Enhanced electromagnetic fields within plasmonic nanocavity mode volumes enable multiple significant effects that lead to applications in both the linear and nonlinear optical regimes. In this work, enhanced second‐harmonic generation (SHG) is demonstrated from individual plasmonic nanopatch antennas (NPAs) which are formed by separating silver nanocubes from a smooth gold film using a sub‐10 nm zinc oxide spacer layer. When the NPAs are excited at their fundamental plasmon frequency, a 104‐fold increase in the intensity of the SHG wave is observed. Moreover, by integrating quantum emitters that have an absorption energy at the fundamental frequency, a second‐order nonlinear exciton–polariton strong coupling response is observed with a Rabi splitting energy of 19 meV. The nonlinear frequency conversion using NPAs thus provides an excellent platform for nonlinear control of the light−matter interactions in both weak and strong coupling regimes which will have a great potential for applications in optical engineering and information processing.
more » « less- NSF-PAR ID:
- 10444530
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Optical Materials
- Volume:
- 10
- Issue:
- 16
- ISSN:
- 2195-1071
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract New materials that exhibit strong second-order optical nonlinearities at a desired operational frequency are of paramount importance for nonlinear optics. Giant second-order susceptibility
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Abstract Carbon nanotubes (CNTs) possess extremely anisotropic electronic, thermal, and optical properties owing to their 1D character. While their linear optical properties have been extensively studied, nonlinear optical processes, such as harmonic generation for frequency conversion, remain largely unexplored in CNTs, particularly in macroscopic CNT assemblies. In this work, macroscopic films of aligned and type‐separated (semiconducting and metallic) CNTs are synthesized and polarization‐dependent third‐harmonic generation (THG) from the films with fundamental wavelengths ranging from 1.5 to 2.5 µm is studied. Both films exhibited strongly wavelength‐dependent, intense THG signals, enhanced through exciton resonances, and third‐order nonlinear optical susceptibilities of 2.50 × 10−19 m2 V−2(semiconducting CNTs) and 1.23 × 10−19 m2 V−2(metallic CNTs), respectively are found, for 1.8 µm excitation. Further, through systematic polarization‐dependent THG measurements, the values of all elements of the susceptibility tensor are determined, verifying the macroscopically 1D nature of the films. Finally, polarized THG imaging is performed to demonstrate the nonlinear anisotropy in the large‐size CNT film with good alignment. These findings promise applications of aligned CNT films in mid‐infrared frequency conversion, nonlinear optical switching, polarized pulsed lasers, polarized long‐wave detection, and high‐performance anisotropic nonlinear photonic devices.
