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Register a new userStrong nonlinear optical response of graphene flakes measured by four-wave mixing
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We present the first experimental investigation of nonlinear optical properties of graphene flakes. We find that at near infrared frequencies a graphene monolayer exhibits a remarkably high third-order optical nonlinearity which is practically independent of the wavelengths of incident light. The nonlinear optical response can be utilized for imaging purposes, with image contrasts of graphene which are orders of magnitude higher than those obtained using linear microscopy.
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The ability to tune the optical response of a material via electrostatic gating is crucial for optoelectronic applications, such as electro-optic modulators, saturable absorbers, optical limiters, photodetectors and transparent electrodes. The band structure of single layer graphene (SLG), with zero-gap, linearly dispersive conduction and valence bands, enables an easy control of the Fermi energy E$_F$ and of the threshold for interband optical absorption. Here, we report the tunability of the SLG non-equilibrium optical response in the near-infrared (1000-1700nm/0.729-1.240eV), exploring a range of E$_F$ from -650 to 250 meV by ionic liquid gating. As E$_F$ increases from the Dirac point to the threshold for Pauli blocking of interband absorption, we observe a slow-down of the photobleaching relaxation dynamics, which we attribute to the quenching of optical phonon emission from photoexcited charge carriers. For E$_F$ exceeding the Pauli blocking threshold, photobleaching eventually turns into photoinduced absorption, due to hot electrons excitation increasing SLG absorption. The ability to control both recovery time and sign of nonequilibrium optical response by electrostatic gating makes SLG ideal for tunable saturable absorbers with controlled dynamics.
We investigate quantum transport properties of triangular graphene flakes with zigzag edges by using first principles calculations. Triangular graphene flakes have large magnetic moments which vary with the number of hydrogen atoms terminating its edge atoms and scale with its size. Electronic transmission and current-voltage characteristics of these flakes, when contacted with metallic electrodes, reveal spin valve and remarkable rectification features. The transition from ferromagnetic to antiferromagnetic state under bias voltage can, however, terminate the spin polarizing effects for specific flakes. Geometry and size dependent transport properties of graphene flakes may be crucial for spintronic nanodevice applications.
The unique linear and massless band structure of graphene, in a purely two-dimensional Dirac fermionic structure, have led to intense research spanning from condensed matter physics to nanoscale device applications covering the electrical, thermal, mechanical and optical domains. Here we report three consecutive first-observations in graphene-silicon hybrid optoelectronic devices: (1) ultralow power resonant optical bistability; (2) self-induced regenerative oscillations; and (3) coherent four-wave mixing, all at a few femtojoule cavity recirculating energies. These observations, in comparison with control measurements with solely monolithic silicon cavities, are enabled only by the dramatically-large and chi(3) nonlinearities in graphene and the large Q/V ratios in wavelength-localized photonic crystal cavities. These results demonstrate the feasibility and versatility of hybrid two-dimensional graphene-silicon nanophotonic devices for next-generation chip-scale ultrafast optical communications, radio-frequency optoelectronics, and all-optical signal processing.
Focusing on the twist angle for the minimal commensurate structure, we perform nonperturbative calculations of electron dynamics in the twisted bilayer graphene (TBG) under intense laser fields. We show that the TBG exhibits enriched high-harmonic generation that cannot occur in monolayer or conventional bilayers. We elucidate the mechanism of these nonlinear responses by analyzing dynamical symmetries, momentum-resolved dynamics, and roles of interlayer coupling. Our results imply nonlinear optotwistronics, or controlling optical properties of layered materials by artificial twists.
We report the application of femtosecond four-wave mixing (FWM) to the study of carrier transport in solution-processed CH3NH3PbI3. The diffusion coefficient was extracted through direct detection of the lateral diffusion of carriers utilizing the transient grating technique, coupled with simultaneous measurement of decay kinetics exploiting the versatility of the boxcar excitation beam geometry. The observation of exponential decay of the transient grating versus interpulse delay indicates diffusive transport with negligible trapping within the first nanosecond following excitation. The in-plane transport geometry in our experiments enabled the diffusion length to be compared directly with the grain size, indicating that carriers move across multiple grain boundaries prior to recombination. Our experiments illustrate the broad utility of FWM spectroscopy for rapid characterization of macroscopic film transport properties.
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