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Light modulation is an essential operation in photonics and optoelectronics. With existing and emerging technologies increasingly demanding compact, efficient, fast and broadband optical modulators, high-performance light modulation solutions are becoming indispensable. The recent realization that two-dimensional layered materials could modulate light with superior performance has prompted intense research and significant advances, paving the way for realistic applications. In this review, we cover the state-of-the-art of optical modulators based on two-dimensional layered materials including graphene, transition metal dichalcogenides and black phosphorus. We discuss recent advances employing hybrid structures, such as two-dimensional heterostructures, plasmonic structures, and silicon/fibre integrated structures. We also take a look at future perspectives and discuss the potential of yet relatively unexplored mechanisms such as magneto-optic and acousto-optic modulation.
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Silica-based optical fibers are a workhorse of nonlinear optics. They have been used to demonstrate nonlinear phenomena such as solitons and self-phase modulation. Since the introduction of the photonic crystal fiber, they have found many exciting applications, such as supercontinuum white light sources and third-harmonic generation, among others. They stand out by their low loss, large interaction length, and the ability to engineer its dispersive properties, which compensate for the small chi(3) nonlinear coefficient. However, they have one fundamental limitation: due to the amorphous nature of silica, they do not exhibit second-order nonlinearity, except for minor contributions from surfaces. Here, we demonstrate significant second-harmonic generation in functionalized optical fibers with a monolayer of highly nonlinear MoS2 deposited on the fiber guiding core. The demonstration is carried out in a 3.5 mm short piece of exposed core fiber, which was functionalized in a scalable process CVD-based process, without a manual transfer step. This approach is scalable and can be generalized to other transition metal dichalcogenides and other waveguide systems. We achieve an enhancement of more than 1000x over a reference sample of equal length. Our simple proof-of-principle demonstration does not rely on either phase matching to fundamental modes, or ordered growth of monolayer crystals, suggesting that pathways for further improvement are within reach. Our results do not just demonstrate a new path towards efficient in-fiber SHG-sources, instead, they establish a platform with a new route to chi(2)-based nonlinear fiber optics, optoelectronics, and photonics platforms, integrated optical architectures, and active fiber networks.
We propose an optical method of shining circularly polarized and spatially periodic laser fields to imprint superlattice structures in two-dimensional electronic systems. By changing the configuration of the optical field, we synthesize various lattice structures with different spatial symmetry, periodicity, and strength. We find that the wide optical tunability allows one to tune different properties of the effective band structure, including Chern number, energy bandwidths, and band gaps. The in situ tunability of the superlattice gives rise to unique physics ranging from the topological transitions to the creation of the flat bands through the kagome superlattice, which can allow a realization of strongly correlated phenomena in Floquet systems. We consider the high-frequency regime where the electronic system can remain in the quasiequilibrium phase for an extended amount of time. The spatiotemporal reconfigurability of the present scheme opens up possibilities to control light-matter interaction to generate novel electronic states and optoelectronic devices.
Nonlinear optical (NLO) phenomena such as harmonic generation, Kerr, and Pockels effects are of great technological importance for lasers, frequency converters, modulators, switches, etc. Recently, two-dimensional (2D) materials have drawn significant attention due to their strong and unique NLO properties. Here, we describe an efficient first-principles workflow for calculating the quadratic optical response and apply it to 375 non-centrosymmetric semiconductor monolayers from the Computational 2D Materials Database (C2DB). Sorting the non-resonant nonlinearities with respect to bandgap $E_g$ reveals an upper limit proportional to $E_g^{-4}$, which is neatly explained by two distinct generic models. We identify multiple promising candidates with giant nonlinearities and bandgaps ranging from 0.4 to 5 eV, some of which approach the theoretical upper limit and greatly outperform known materials. Our comprehensive library of ab initio NLO spectra for all 375 monolayers is freely available via the C2DB website. We expect this work to pave the way for highly efficient and compact opto-electronic devices based on 2D materials.
Layered materials have uncommonly anisotropic thermal properties due to their strong in-plane covalent bonds and weak out-of-plane van der Waals interactions. Here we examine heat flow in graphene (graphite), h-BN, MoS2, and WS2 monolayers and bulk films, from diffusive to ballistic limits. We determine the ballistic thermal conductance limit (Gball) both in-plane and out-of-plane, based on full phonon dispersions from first-principles calculations. An overall phonon mean free path ({lambda}) is expressed in terms of Gball and the diffusive thermal conductivity, consistent with kinetic theory if proper averaging of phonon group velocity is used. We obtain a size-dependent thermal conductivity k(L) in agreement with available experiments, and find that k(L) only converges to >90% of the diffusive thermal conductivity for sample sizes L > 16{lambda}, which ranges from ~140 nm for MoS2 cross-plane to ~10 um for suspended graphene in-plane. These results provide a deeper understanding of microscopic thermal transport, revealing that device scales below which thermal size effects should be taken into account are generally larger than previously thought.
Unprecedented material compatibility and ease of integration, in addition to the unique and diverse optoelectronic properties of layered materials have generated significant interest in their utilization in nanophotonic devices. While initial nanophotonic experiments primarily focused on light-sources, modulators, and detectors, recently researchers have demonstrated nonlinear optical devices using layered materials. In this paper, we review the current state of cavity-enhanced nonlinear optics with layered materials. Along with conventional nonlinear optics related to harmonic generation, we report on emerging directions of nonlinear optics, where the layered materials can potentially play a significant role.
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