Rich information on 2D materials revealed by optical second harmonic generation.

The integration of two-dimensional (2D) materials with resonant photonic structures is seen as a promising direction for enhancing its nonlinear optical response. The design of such heterogeneous resonant structures has often relied on multi-parameter sweeps to determine the optimized dimensions of resonant optical structure that results in good resonance characteristics, often in the absence of the 2D material. Such an approach is computationally intensive and may not necessarily result in efficient generation or collection of nonlinear signals from the designed structure. Here, we report hybrid-genetic optimization (HGA) based design and experimental demonstration of second harmonic generation (SHG) enhancement from Fabry-Perot structures of single and double multilayer gallium selenide (GaSe) flakes with bottom silicon dioxide, and index matched polymethyl methacrylate spacer/encapsulation layers. HGA technique utilized here speeds up the multilayer cavity design by 8.8 and 89-times for the single and double GaSe structures when compared to the full parameter-sweep, with measured SHG enhancement of 128- and 400-times, respectively, when compared to a reference sample composed of GaSe layer of optimized thickness on 300nm silicon dioxide layer. SHG conversion efficiencies obtained from the HGA structures are 1-2 orders of magnitude higher than previous reports on 2D material integrated resonant metasurfaces or Bragg cavities.

We theoretically study how the intensity of second harmonic generation (SHG) for a sheet of two-dimensional (2D) material is controlled by an underlying layered structure. By utilizing the transfer matrix method with the inclusion of a nonlinear sheet current to describe the response of the 2D material, an explicit expression for the intensity of upward propagating second harmonic (SH) light is obtained, and the effects of the layered structure can be identified by a structure factor β, defined as the ratio of SH intensity from such a structure to that from a freely suspended 2D material. Our results show that the influence of a layered structure on the SHG intensity arises from interference effects of both the fundamental light and the SH light; the value of the structure factor is 0 ≤ β ≤ 64. Furthermore, when the incident light is pulsed, the interference effects are partially canceled due to the existence of many wave vectors and frequencies, and the cancellation becomes severe for thick films, small beam spots, and short pulses. For a specific structure of 2D material/dielectric film/substrate, the thickness of the dielectric film can effectively tune the value of β in an interval [βmin, βmax], and detailed discussions are performed for the thicknesses when these two extreme values can be obtained. When there is optical loss or the substrate is not perfectly reflective, the extreme value of βmax or βmin cannot reach 64 or 0. A large βmax requires two conditions to be fulfilled: (1) the substrate should be highly reflective, and (2) the refractive indices of the dielectric film at the fundamental and the SH frequencies should differ. Our results indicate how practical substrate structures can be used to achieve high SH signals, and the simple expression we give for the SH enhancement will be useful in characterizing the nonlinear susceptibility of 2D materials.

The layered two-dimensional (2D) materials, e.g., the well-known graphene, transition metal dichalcogenides, and topological insulators, have attracted great interest of researchers from fundamental research as well as industries owing to their intriguing properties in a number of aspects. In practical applications, the efficient modification of the features of 2D materials is compelling and essential to achieve desired functionalities. Ion implantation has been successfully applied to synthesize graphene. The most exotic advantage of ion beam technology is that it offers distinct options of energetic beams, which has recently shown the unique capability to modify and tailor the properties of versatile 2D materials. To name a few, the energetic ion beams could implement the surface morphology or layer-to-layer structural engineering of 2D materials. At the microcosmic level, the introduction of ion beam induced defects and intentional doping of specific ions are the basis of tailoring properties of 2D materials. By manipulating the parameters of ion beams (energies, species, fluences, incident angles, etc.), the modified 2D materials may possess novel properties, which are unprecedented in pristine ones. Promising applications based on these 2D materials with ion beam tailored features have been realized in a broad range of fields. In this work, we systematically review the latest research progress on the deployed techniques and property modifications of graphene and other 2D materials under the treatment of various ion beams. A few selected applications are presented to indicate the practical potentials of ion beam modified 2D materials in distinct areas. Perspectives on future developments are also provided by focusing on several promising topics.

In this work, the second harmonic generation (SHG) technique based on embedded piezoelectric (PZT) sensors is developed for the defect assessment of concrete samples. Three different imperfection forms of concrete including internal capillary void during the curing process, cracking damage due to compression, and bending loads are examined and analyzed. Clear second harmonics are observed by Fourier transform of time domain signal, and the square of fundamental signal amplitude shows a linear relation with the second harmonic amplitude as theoretically expected. The nonlinear parameter presents a good distinction for samples in different states of three cases, indicating the well-round feasibility of SHG technique based on embedded sensors. In addition, the nonlinear parameter presents an excellent correlation with the variation of internal capillary void and cracks in concrete. The high sensitivity of the developed SHG technique is further validated through a comparison between the nonlinear parameter and two traditional linear parameters, namely the phase velocity of Rayleigh wave and the resonance frequency of vibrations. Experimental results in this study demonstrate that the embedded sensors are promising for the nonlinear ultrasonic nondestructive evaluation of concrete structures, particularly as a low-cost alternative of commercial ultrasonic transducers.

Recently, the study of ternary organic solar cells (OSCs) has attracted the efforts of the scientific community, leading to significantly higher performance due to the enhanced harvesting of incoming irradiation. Here, for the first time, and in order to promote this OSC architecture, we review the progress implemented by the application of two-dimensional (2D) materials in the field of blend bulk heterojunction ternary OSCs. Power conversion efficiency (PCE) improvements of the order of 40% compared to the reference binary devices, and PCEs in excess of 8% have been reported by incorporating graphene-based or other 2D materials as a third element inside the active layer. These OSCs combine the synergetic advantages of ternary devices and the superb properties of the 2D material family. In conclusion, the incorporation of the unique properties of graphene and other 2D materials inside the active layer opens up a very promising pathway in the design and construction of high-performance, simply fabricated and low- cost photovoltaic devices.

Cost-effective, rapid, and accurate virus detection technologies play key roles in reducing viral transmission. Prompt and accurate virus detection enables timely treatment and effective quarantine of virus carrier, and therefore effectively reduces the possibility of large-scale spread. However, conventional virus detection techniques often suffer from slow response, high cost or sophisticated procedures. Recently, two-dimensional (2D) materials have been used as promising sensing platforms for the high-performance detection of a variety of chemical and biological substances. The unique properties of 2D materials, such as large specific area, active surface interaction with biomolecules and facile surface functionalization, provide advantages in developing novel virus detection technologies with fast response and high sensitivity. Furthermore, 2D materials possess versatile and tunable electronic, electrochemical and optical properties, making them ideal platforms to demonstrate conceptual sensing techniques and explore complex sensing mechanisms in next-generation biosensors. In this review, we first briefly summarize the virus detection techniques with an emphasis on the current efforts in fighting again COVID-19. Then, we introduce the preparation methods and properties of 2D materials utilized in biosensors, including graphene, transition metal dichalcogenides (TMDs) and other 2D materials. Furthermore, we discuss the working principles of various virus detection technologies based on emerging 2D materials, such as field-effect transistor-based virus detection, electrochemical virus detection, optical virus detection and other virus detection techniques. Then, we elaborate on the essential works in 2D material-based high-performance virus detection. Finally, our perspective on the challenges and future research direction in this field is discussed.

While understanding the competitive adsorption behavior of gas sensor is important, it is yet to be unraveled. Especially for the influence of water molecules to the gas adsorbed on 2D materials. This study explores the potential of layered 2D materials as a candidate material for gas sensing, employing non‐destructive measurement, and second harmonic generation (SHG). The investigation focuses on analyzing oxygen, ammonia, and water vapor adsorbed on a WS2 surface by studying the evolutions in electric dipole and electric field. Leveraging the simplified bond hyperpolarizability model (SBHM), a foundation is established for gas sensors utilizing high‐quality 2D materials. This approach facilitates the detection of material modifications in response to environmental influences, including the inevitable water molecules. The obtained hyperpolarizability from SBHM exhibits remarkable consistency with Langmuir's adsorption model, confirming the physical adsorption in the system. In addition, the competitive effects between gases are explored by comparing experimental results with theoretical predictions based on Boltzmann distribution and density functional theory (DFT) calculations. This highlights the effectiveness of SHG and SBHM in studying gas adsorption on layered van der Waals materials.

The fascinating two-dimensional (2D) materials are being unconsciously applied in various fields from science to engineering, which is benefited from the glamorous physical and chemical properties of mechanics, optics, electronics, and magnetism. The representative 2D thermoelectric/piezoelectric materials can directly convert thermal/mechanical energy into electrical energy, which can resolve the energy issues and avoid further environmental deterioration. The thermoelectric or piezoelectric properties of various 2D materials, such as graphene, hexagonal boron nitride, black phosphorus, transition metal dichalcogenides (TMDs), arsenene, metal carbides and nitrides (MXenes), and so on, have been investigated in detail. Although tremendous progress has been achieved in the past few years, these properties still need to be improved for their practical application by designing new 2D materials, strain engineering, chemical functionalization, etc. In addition to this, in 2D materials, there are many other novel physical properties, such as magnetism, topology, valley, and so on. The combination of thermoelectricity/piezoelectricity with other unique properties may lead to novel device applications or scientific breakthroughs in new physics. Overall, the emergence of 2D thermoelectric and piezoelectric materials has expanded energy conversion research dramatically. By combing this new device concept with the novel 2D materials, original devices should have potential applications in energy harvesting.

This chapter describes the prospects of integration of Two-dimensional (2D) materials with photonic nanostructures to enable future active nanophotonic devices. It focuses on development of controlling light emission from transition metal dichalcogenides (TMD) by nanophotonic integration. The monolayer form demonstrates a range of novel optical effects, including strong excitonic effects, photo-luminescence , valley polarisation, single-photon emission and second-harmonic generation, which show great potential for fabricating novel “flat” active nanophotonic devices in the future. Integration with photonic nanostructures is a solution to such challenges, since photonic nanostructures such as plasmonic nanoparticles show great capability to manipulate light–matter interaction at the nanoscale. A greater understanding of the coupling between photonic nanostructures and 2D materials is required, thus potentially better controlling the properties of these materials. For example, non-linear coupling between 2D materials, especially second-order non-linearity, has attracted intense interest. Dielectric nanostructures, such as photonic crystal cavities, have also been proposed for enhancing the emission from TMD monolayers.

Wide bandgap semiconductors such as gallium nitride (GaN) are essential constituents of future optical circuits, as their optical response can accommodate a broad wavelength range while suppressing two-photon absorption and free-carrier absorption effects that are encountered with silicon (Si) structures. Their direct wide bandgap is also favourable for the incorporation of active elements. Furthermore, nonlinear optical processes can be harnessed by exploiting the higher-order susceptibility tensors of the crystal structure to achieve advanced light control modalities, enabling all-optical processing and the generation of entangled photon states. We will report on nonlinear frequency conversion from the telecom range via second harmonic generation (SHG) and third harmonic generation (THG) in suspended gallium nitride slab photonic crystal (PhC) cavities on silicon, under continuous-wave resonant excitation. Genetic optimization is applied to sweep parameter space for the highest cavity quality factors, and simultaneously accounting for power in-coupling. While there is a clear trade-off theoretically between coupling efficiency and Q-factor for a given cavity design, the upper limit on the Q-factor that is imposed by loss channels, given the disorder figure of current fabrication technology, makes room for introducing improved far-field coupling to enhance nonlinear processes without sacrificing the experimentally achievable light confinement. Far-field coupling is addressed through various PhC cavity designs, which enable the excitation of the fundamental mode with a Gaussian beam. Optimized two-dimensional PhC cavities with increased far-field coupling have been characterized with quality factors as high as 44′000, approaching the computed theoretical values. The strong enhancement in light confinement has enabled second harmonic generation (SHG) under continuous-wave excitation, with up-conversion from both 1300 nm and 1550 nm wavelength bands, confirmed by spectral and power dependence measurements. At 1550 nm, normalized SHG conversion efficiency as large as 2.4×10−3 W−1 are measured as well as simultaneous THG. SHG emission power of up to 0.74 nW has been detected without saturation

Two-dimensional (2D) materials, such as graphene and transition-metal dichalcogenide monolayers, have unique properties that are distinctly different from those of their bulk counterparts, and hopefully possess a wide range of applications in 2D semiconductor device. Structural defects are known to have profound influences on the properties of crystalline materials; thus, correlating the defect structure with local properties in 2D material is of fundamental importance. However, electron microscopy studies of 2D materials on an atomic scale have become a challenge as most of these materials are susceptible to electron beam irradiation damage under high voltage and high dose experimental conditions. The development of low voltage aberration-corrected scanning transmission electron microscopy (STEM) has made it possible to study 2D materials at a single atom level without damaging their intrinsic structures. In addition, controllable structural modification by using electron beam becomes feasible by controlling the electron beam-sample interaction. New nanostructures can be created and novel 2D materials can be fabricated in-situ by using this approach. In this article, we review some of our recent studies of graphene and transition-metal dichalcogenides to showcase the applications of low voltage aberration corrected STEM in 2D material research.

In this contribution we report on the results of an experimental comparative study of high order harmonic generation (HHG) from strong mid-IR femtosecond laser pulses in two-dimensional (2D) materials consisting of a single layer. Beside their promising application in electronics and photonics, these materials allow to study microscopic light-condensed-matter interaction on the atomic scale. HHG in 2D materials, in comparison to a bulk, have several distinct qualitative features: single atom layer essentially excludes propagation effects and minimizes absorption, whereas weak charge screening results in significantly higher exciton binding energy. Here we report on comparative study of intensity and polarization dependence of HHG in polycrystalline single layers of MoS 2 and WS 2 .

Two-dimensional (2D) materials have attracted increasing interest in the last few years due to their unique morphology and properties and their use in a variety of applications, ranging from electronics to energy storage or catalysis, to name a few. Apart from various well-established 2D materials, such as graphene, h-BN, or MoS2, black phosphorus (BP) has received considerable attention over the last two years because its direct bandgap and his appealing properties for electronic and ultrafast optoelectronic applications. However, its lack of environmental stability severely limits its synthesis and processing. We have recently demonstrated that high-quality, few-layer BP nanosheets, with controllable size and observable photoluminescence, can be produced in large quantities by liquid phase exfoliation under ambient conditions.1 Beyond this success, a more sophisticated chemical modification is highly desirable, like the molecular doping, that is an effective and flexible method towards modulating the electronic properties of 2D materials. Herein, we have developed a chemical route for the non-covalent functionalization of BP with different moieties, including electron-withdrawing organic molecules or tailor-made surfactants.2 Moreover we have extended these concepts towards a new 2D material: antimonene, creating stable suspensions in water and developing its non-covalent functionalization.3 1) D. Hanlon, C. Backes, E. Doherty, C. S. Cucinotta, N. C. Berner, C. Boland, K. Lee, A. Harvey, P. Lynch, Z. Gholamvand, S. F. Zhang, K. P. Wang, G. Moynihan, A. Pokle, Q. M. Ramasse, N. McEvoy, W. J. Blau, J. Wang, G. Abellan, F. Hauke, A. Hirsch, S. Sanvito, D. D. O’Regan, G. S. Duesberg, V. Nicolosi, J. N. Coleman, Nat. Commun. 2015, 6, 8563. 2) G. Abellán, V. Lloret, U. Mundloch, M. Marcia, C. Neiss, A. Görling, M. Varela, F. Hauke, A. Hirsch, Angew. Chem. In. Ed., 2016, 55 (47), 14557. 3) C. Gibaja, D. Rodriguez-San-Miguel, P. Ares, J. Gómez-Herrero, M. Varela, R. Gillen, J. Maultzsch, F. Hauke, A. Hirsch, G. Abellán, F. Zamora, Angew. Chem. In. Ed., 2016, 55 (46), 14345.

Second-Harmonic Generation in Two-Dimensional Materials

Two-dimensional (2D) materials with dangling-bond-free surfaces have attracted considerable attention in next-generation electronic applications due to their distinctive properties, such as high carrier mobility, short-channel immunity, and strong light-matter interactions. Recently, various methods have been developed for the preparation of 2D materials, including mechanical exfoliation, chemical vapor deposition, and chemical solution-based processes. Among these, solution processing provides a cost-effective and low-temperature approach for large-scale production. This review highlights recent advancements in solution-processed 2D materials, focusing on preparation methods and their applications in electronic and optoelectronic devices. Additionally, future perspectives are proposed to advance the breakthrough and commercialization of solution technologies for value-added chemical production.