An electrically tunable nonlinear optical device working at near‐infrared wavelength is theoretically and experimentally demonstrated. Ultrahigh optical second‐order nonlinearity from titanium‐nitride‐based coupled metallic quantum wells can be electrically tuned by external electric field. Tunability of second‐order susceptibility
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
- Award ID(s):
- 1807891
- NSF-PAR ID:
- 10153477
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- Light: Science & Applications
- Volume:
- 8
- Issue:
- 1
- ISSN:
- 2047-7538
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
more » « less
Abstract χ (2)reaches a 63% modulation depth with an average tunability of 10.5% per volt. In addition, electro‐optic modulation of second‐harmonic signal is presented by continuous tuning ofχ (2)over a long period of time with high stability. These results provide a new material platform with actively controllable strong nonlinearity for future nonlinear photonic systems, such as ultra‐compact opto‐electronic modulation devices and reconfigurable nonlinear metamaterials and metasurfaces. -
BACKGROUND Electromagnetic (EM) waves underpin modern society in profound ways. They are used to carry information, enabling broadcast radio and television, mobile telecommunications, and ubiquitous access to data networks through Wi-Fi and form the backbone of our modern broadband internet through optical fibers. In fundamental physics, EM waves serve as an invaluable tool to probe objects from cosmic to atomic scales. For example, the Laser Interferometer Gravitational-Wave Observatory and atomic clocks, which are some of the most precise human-made instruments in the world, rely on EM waves to reach unprecedented accuracies. This has motivated decades of research to develop coherent EM sources over broad spectral ranges with impressive results: Frequencies in the range of tens of gigahertz (radio and microwave regimes) can readily be generated by electronic oscillators. Resonant tunneling diodes enable the generation of millimeter (mm) and terahertz (THz) waves, which span from tens of gigahertz to a few terahertz. At even higher frequencies, up to the petahertz level, which are usually defined as optical frequencies, coherent waves can be generated by solid-state and gas lasers. However, these approaches often suffer from narrow spectral bandwidths, because they usually rely on well-defined energy states of specific materials, which results in a rather limited spectral coverage. To overcome this limitation, nonlinear frequency-mixing strategies have been developed. These approaches shift the complexity from the EM source to nonresonant-based material effects. Particularly in the optical regime, a wealth of materials exist that support effects that are suitable for frequency mixing. Over the past two decades, the idea of manipulating these materials to form guiding structures (waveguides) has provided improvements in efficiency, miniaturization, and production scale and cost and has been widely implemented for diverse applications. ADVANCES Lithium niobate, a crystal that was first grown in 1949, is a particularly attractive photonic material for frequency mixing because of its favorable material properties. Bulk lithium niobate crystals and weakly confining waveguides have been used for decades for accessing different parts of the EM spectrum, from gigahertz to petahertz frequencies. Now, this material is experiencing renewed interest owing to the commercial availability of thin-film lithium niobate (TFLN). This integrated photonic material platform enables tight mode confinement, which results in frequency-mixing efficiency improvements by orders of magnitude while at the same time offering additional degrees of freedom for engineering the optical properties by using approaches such as dispersion engineering. Importantly, the large refractive index contrast of TFLN enables, for the first time, the realization of lithium niobate–based photonic integrated circuits on a wafer scale. OUTLOOK The broad spectral coverage, ultralow power requirements, and flexibilities of lithium niobate photonics in EM wave generation provides a large toolset to explore new device functionalities. Furthermore, the adoption of lithium niobate–integrated photonics in foundries is a promising approach to miniaturize essential bench-top optical systems using wafer scale production. Heterogeneous integration of active materials with lithium niobate has the potential to create integrated photonic circuits with rich functionalities. Applications such as high-speed communications, scalable quantum computing, artificial intelligence and neuromorphic computing, and compact optical clocks for satellites and precision sensing are expected to particularly benefit from these advances and provide a wealth of opportunities for commercial exploration. Also, bulk crystals and weakly confining waveguides in lithium niobate are expected to keep playing a crucial role in the near future because of their advantages in high-power and loss-sensitive quantum optics applications. As such, lithium niobate photonics holds great promise for unlocking the EM spectrum and reshaping information technologies for our society in the future. Lithium niobate spectral coverage. The EM spectral range and processes for generating EM frequencies when using lithium niobate (LN) for frequency mixing. AO, acousto-optic; AOM, acousto-optic modulation; χ (2) , second-order nonlinearity; χ (3) , third-order nonlinearity; EO, electro-optic; EOM, electro-optic modulation; HHG, high-harmonic generation; IR, infrared; OFC, optical frequency comb; OPO, optical paramedic oscillator; OR, optical rectification; SCG, supercontinuum generation; SHG, second-harmonic generation; UV, ultraviolet.more » « less
-
more » « less
Abstract Reconfiguration of chiral ceramic nanostructures after ion intercalation should favor specific nanoscale twists leading to strong chiroptical effects. In this work, V2O3nanoparticles are shown to have “built‐in” chiral distortions caused by binding of tartaric acid enantiomers to the nanoparticle surface. As evidenced by spectroscopy/microscopy techniques and calculations of nanoscale chirality measures, the intercalation of Zn2+ions into the V2O3lattice results in particle expansion, untwist deformations, and chirality reduction. Coherent deformations in the particle ensemble manifest as changes in sign and positions of circular polarization bands at ultraviolet, visible, mid‐infrared (IR), near‐IR (NIR), and IR wavelengths. The
g‐ factors observed for IR and NIR spectral diapasons are ≈100–400 times higher than those for previously reported dielectric, semiconductor, and plasmonic nanoparticles. Nanocomposite films layer‐by‐layer assembled (LBL) from V2O3nanoparticles reveal cyclic‐voltage‐driven modulation of optical activity. Device prototypes for IR and NIR range problematic for liquid crystals and other organic materials are demonstrated. High optical activity, synthetic simplicity, sustainable processability, and environmental robustness of the chiral LBL nanocomposites provide a versatile platform for photonic devices. Similar reconfigurations of particle shapes are expected for multiple chiral ceramic nanostructures, leading to unique optical, electrical, and magnetic properties. -
more » « less
Silicon is a common material for photonics due to its favorable optical properties in the telecom and mid-wave IR bands, as well as compatibility with a wide range of complementary metal–oxide semiconductor (CMOS) foundry processes. Crystalline inversion symmetry precludes silicon from natively exhibiting second-order nonlinear optical processes. In this work, we build on recent works in silicon photonics that break this material symmetry using large bias fields, thereby enabling
χ (2)interactions. Using this approach, we demonstrate both second-harmonic generation (with a normalized efficiency of 0.20%W−1cm−2) and, to our knowledge, the first degenerateχ (2)optical parametric amplifier (with an estimated normalized gain of 0.6dBW−1/2cm−1) using silicon-on-insulator waveguides fabricated in a CMOS-compatible commercial foundry. We expect this technology to enable the integration of novel nonlinear optical devices such as optical parametric amplifiers, oscillators, and frequency converters into large-scale, hybrid photonic–electronic systems by leveraging the extensive ecosystem of CMOS fabrication. -
more » « less
Abstract Atomically thin transition metal dichalcogenides (TMDs) in their excited states can serve as exceptionally small building blocks for active optical platforms. In this scheme, optical excitation provides a practical approach to control light‐TMD interactions via the photocarrier generation, in an ultrafast manner. Here, it is demonstrated that via a controlled generation of photocarriers the second‐harmonic generation (SHG) from a monolayer MoS2crystal can be substantially modulated up to ≈55% within a timeframe of ≈250 fs, a set of performance characteristics that showcases the promise of low‐dimensional materials for all‐optical nonlinear data processing. The combined experimental and theoretical study suggests that the large SHG modulation stems from the correlation between the second‐order dielectric susceptibility χ(2)and the density of photoexcited carriers in MoS2. Indeed, the depopulation of the conduction band electrons, at the vicinity of the high‐symmetry
K/K′ points of MoS2, suppresses the contribution of interband electronic transitions in the effective χ(2)of the monolayer crystal, enabling the all‐optical modulation of the SHG signal. The strong dependence of the second‐order optical response on the density of photocarriers reveals the promise of time‐resolved nonlinear characterization as an alternative route to monitoring carrier dynamics in excited states of TMDs.
