Parametric Nonlinear Optics with Layered Materials and Related Heterostructures

Nonlinear optics is of crucial importance in several fields of science and technology with applications in frequency conversion, entangled-photon generation, self-referencing of frequency combs, crystal characterization, sensing, and ultra-short light pulse generation and characterization. In recent years, layered materials and related heterostructures have attracted huge attention in this field, due to their huge nonlinear optical susceptibilities, their ease of integration on photonic platforms, and their 2D nature which relaxes the phase-matching constraints and thus offers a practically unlimited bandwidth for parametric nonlinear processes. In this review the most recent advances in this field, highlighting their importance and impact both for fundamental and technological aspects, are reported and explained, and an outlook on future research directions for nonlinear optics with atomically thin materials is provided

Ultrafast Spectroscopy of Graphene-Protected Thin Copper Films

© 2016 American Chemical Society. We studied by broad-band pump-probe spectroscopy the ultrafast optical response of thin copper films covered by a monolayer of graphene. It is demonstrated that graphene protection does not alter the thermo-modulational nonlinearity of copper in the whole visible range. Also, we provide a quantitative validation of a theoretical model for this optical nonlinearity, derived from a semiclassical description of electron thermalization dynamics and subsequent modulation of copper dielectric function from 450 to 700 nm wavelength. Our results extend to the nonlinear domain the capability of graphene-protected copper nanolayers to serve as a low cost optical grade material, with major potential impact on nonlinear plasmonics and metamaterials

Electrostatic Tuning of the Ligand Binding Mechanism by Glu27 in Nitrophorin 7.

Nitrophorins (NP) 1-7 are NO-carrying heme proteins found in the saliva of the blood-sucking insect Rhodnius prolixus. The isoform NP7 displays peculiar properties, such as an abnormally high isoelectric point, the ability to bind negatively charged membranes, and a strong pH sensitivity of NO affinity. A unique trait of NP7 is the presence of Glu in position 27, which is occupied by Val in other NPs. Glu27 appears to be important for tuning the heme properties, but its influence on the pH-dependent NO release mechanism, which is assisted by a conformational change in the AB loop, remains unexplored. Here, in order to gain insight into the functional role of Glu27, we examine the effect of Glu27 → Val and Glu27 → Gln mutations on the ligand binding kinetics using CO as a model. The results reveal that annihilation of the negative charge of Glu27 upon mutation reduces the pH sensitivity of the ligand binding rate, a process that in turn depends on the ionization of Asp32. We propose that Glu27 exerts a through-space electrostatic action on Asp32, which shifts the pKa of the latter amino acid towards more acidic values thus reducing the pH sensitivity of the transition between open and closed states

Exciton-exciton annihilation and biexciton stimulated emission in graphene nanoribbons

Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron-hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton-exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of \ue2 \u2030250 meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. These observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics

Optoelectronic mixing with high-frequency graphene transistors

Graphene is ideally suited for optoelectronics. It offers absorption at telecom wavelengths, high-frequency operation and CMOS-compatibility. We show how high speed optoelectronic mixing can be achieved with high frequency (~20 GHz bandwidth) graphene field effect transistors (GFETs). These devices mix an electrical signal injected into the GFET gate and a modulated optical signal onto a single layer graphene(SLG) channel. The photodetection mechanism and the resulting photocurrent sign depend on theSLG Fermi level (EF). At low EF (<130 meV), a positive photocurrent is generated, while at large EF (>130 meV), a negative photobolometric current appears. This allows our devices to operate up to at least 67 GHz. Our results pave the way for GFETs optoelectronic mixers for mm-wave applications, such as telecommunications andradio/light detection and ranging(RADAR/LIDARs.)

Author Correction: Optoelectronic mixing with high-frequency graphene transistors.

Graphene is ideally suited for optoelectronics. It offers absorption at telecom wavelengths, high-frequency operation and CMOS-compatibility. We show how high speed optoelectronic mixing can be achieved with high frequency (~20 GHz bandwidth) graphene field effect transistors (GFETs)