Stable aqueous dispersions of optically and electronically active phosphorene.

Understanding and exploiting the remarkable optical and electronic properties of phosphorene require mass production methods that avoid chemical degradation. Although solution-based strategies have been developed for scalable exfoliation of black phosphorus, these techniques have thus far used anhydrous organic solvents in an effort to minimize exposure to known oxidants, but at the cost of limited exfoliation yield and flake size distribution. Here, we present an alternative phosphorene production method based on surfactant-assisted exfoliation and postprocessing of black phosphorus in deoxygenated water. From comprehensive microscopic and spectroscopic analysis, this approach is shown to yield phosphorene dispersions that are stable, highly concentrated, and comparable to micromechanically exfoliated phosphorene in structure and chemistry. Due to the high exfoliation efficiency of this process, the resulting phosphorene flakes are thinner than anhydrous organic solvent dispersions, thus allowing the observation of layer-dependent photoluminescence down to the monolayer limit. Furthermore, to demonstrate preservation of electronic properties following solution processing, the aqueous-exfoliated phosphorene flakes are used in field-effect transistors with high drive currents and current modulation ratios. Overall, this method enables the isolation and mass production of few-layer phosphorene, which will accelerate ongoing efforts to realize a diverse range of phosphorene-based applications.

Silicon-Phosphorene Nanocavity-Enhanced Optical Emission at Telecommunications Wavelengths.

Generating and amplifying light in silicon (Si) continues to attract significant attention due to the possibility of integrating optical and electronic components in a single material platform. Unfortunately, silicon is an indirect band gap material and therefore an inefficient emitter of light. With the rise of integrated photonics, the search for silicon-based light sources has evolved from a scientific quest to a major technological bottleneck for scalable, CMOS-compatible, light sources. Recently, emerging two-dimensional materials have opened the prospect of tailoring material properties based on atomic layers. Few-layer phosphorene, which is isolated through exfoliation from black phosphorus (BP), is a great candidate to partner with silicon due to its layer-tunable direct band gap in the near-infrared where silicon is transparent. Here we demonstrate a hybrid silicon optical emitter composed of few-layer phosphorene nanomaterial flakes coupled to silicon photonic crystal resonators. We show single-mode emission in the telecommunications band of 1.55 µm ( Eg = 0.8 eV) under continuous wave optical excitation at room temperature. The solution-processed few-layer BP flakes enable tunable emission across a broad range of wavelengths and the simultaneous creation of multiple devices. Our work highlights the versatility of the Si-BP material platform for creating optically active devices in integrated silicon chips.

Cross-phase modulation-induced spectral broadening in silicon waveguides.

We analytically and experimentally investigate cross-phase modulation (XPM) in silicon waveguides. In contrast to the well known result in pure Kerr media, the spectral broadening ratio of XPM to self-phase modulation is not two in the presence of either two-photon absorption (TPA) or free carriers. The physical origin of this change is different for each effect. In the case of TPA, this nonlinear absorption attenuates and slightly modifies the pulse shape due to differential absorption in the pulse peak and wings. When free carriers are present two different mechanisms modify the dynamics. First, free-carrier absorption performs a similar role to TPA, but is additionally asymmetric due to the delayed free-carrier response. Second, free-carrier dispersion induces an asymmetric blue phase shift which competes directly with the symmetric Kerr-induced XPM red shift. We confirm this analysis with pump-probe experiments in a silicon photonic crystal waveguide.

Non-degenerate two-photon absorption in silicon waveguides: analytical and experimental study.

We theoretically and experimentally investigate the nonlinear evolution of two optical pulses in a silicon waveguide. We provide an analytic solution for the weak probe wave undergoing non-degenerate two-photon absorption (TPA) from the strong pump. At larger pump intensities, we employ a numerical solution to study the interplay between TPA and photo-generated free carriers. We develop a simple and powerful approach to extract and separate out the distinct loss contributions of TPA and free-carrier absorption from readily available experimental data. Our analysis accounts accurately for experimental results in silicon photonic crystal waveguides.

Phase-sensitive amplification in silicon photonic crystal waveguides.

We experimentally demonstrate phase-sensitive amplification in a silicon photonic crystal waveguide based on pump-degenerate four-wave mixing. An 11 dB phase-extinction ratio is obtained in a record compact 196 µm nanophotonic device due to broadband slow light, in spite of the presence of two-photon absorption and free carriers. Numerical calculations show good agreement with the experimental results.

Heralded single-photon source in a III-V photonic crystal.

In this Letter we demonstrate heralded single-photon generation in a III-V semiconductor photonic crystal platform through spontaneous four-wave mixing. We achieve a high brightness of 3.4×10(7) pairs·s(-1) nm(-1) W(-1) facilitated through dispersion engineering and the suppression of two-photon absorption in the gallium indium phosphide material. Photon pairs are generated with a coincidence-to-accidental ratio over 60 and a low g(2) (0) of 0.06 proving nonclassical operation in the single photon regime.

Energy efficient nonlinear optics in silicon: are slow-light structures more efficient than nanowires?

We compare the energy performance of four-wave mixing in nanowires and slow-light photonic crystals and outline the regimes where each platform exhibits salient advantages and limitations, including analysis of the impact of future fabrication improvement. These results suggest a route towards energy efficient silicon integrated photonics.

Effect of multiphoton absorption and free carriers in slow-light photonic crystal waveguides.

We examine the effects of multiphoton absorption, free carriers, and disorder-induced linear scattering in slow-light photonic crystal waveguides. We derive an analytic formulation for self-phase modulation including the group velocity scaling of the nonlinear phase shift in materials limited by three-photon absorption as a representative nonlinear process. We investigate the role of free carriers and derive an approximate critical intensity at which these effects begin to strongly modify the optical field. This critical intensity is employed to determine an optimal group index for the self-phase modulation in the slow-light devices. These observations are confirmed with numerical modeling.

Non-trivial scaling of self-phase modulation and three-photon absorption in III-V photonic crystal waveguides.

We investigate the nonlinear response of photonic crystal waveguides with suppressed two-photon absorption. A moderate decrease of the group velocity (approximately c/6 to c/15, a factor of 2.5) results in a dramatic (x 30) enhancement of three-photon absorption well beyond the expected scaling, proportional, variant 1/v3g. This non-trivial scaling of the effective nonlinear coefficients results from pulse compression, which further enhances the optical field beyond that of purely slow-group velocity interactions. These observations are enabled in mm-long slow-light photonic crystal waveguides owing to the strong anomalous group-velocity dispersion and positive chirp. Our numerical physical model matches measurements remarkably.

Physical origin of higher-order soliton fission in nanophotonic semiconductor waveguides.

Supercontinuum generation in Kerr media has become a staple of nonlinear optics. It has been celebrated for advancing the understanding of soliton propagation as well as its many applications in a broad range of fields. Coherent spectral broadening of laser light is now commonly performed in laboratories and used in commercial "white light" sources. The prospect of miniaturizing the technology is currently driving experiments in different integrated platforms such as semiconductor on insulator waveguides. Central to the spectral broadening is the concept of higher-order soliton fission. While widely accepted in silica fibers, the dynamics of soliton decay in semiconductor waveguides is yet poorly understood. In particular, the role of nonlinear loss and free carriers, absent in silica, remains an open question. Here, through experiments and simulations, we show that nonlinear loss is the dominant perturbation in wire waveguides, while free-carrier dispersion is dominant in photonic crystal waveguides.

Free-carrier-induced soliton fission unveiled by in situ measurements in nanophotonic waveguides.

Solitons are localized waves formed by a balance of focusing and defocusing effects. These nonlinear waves exist in diverse forms of matter yet exhibit similar properties including stability, periodic recurrence and particle-like trajectories. One important property is soliton fission, a process by which an energetic higher-order soliton breaks apart due to dispersive or nonlinear perturbations. Here we demonstrate through both experiment and theory that nonlinear photocarrier generation can induce soliton fission. Using near-field measurements, we directly observe the nonlinear spatial and temporal evolution of optical pulses in situ in a nanophotonic semiconductor waveguide. We develop an analytic formalism describing the free-carrier dispersion (FCD) perturbation and show the experiment exceeds the minimum threshold by an order of magnitude. We confirm these observations with a numerical nonlinear Schrödinger equation model. These results provide a fundamental explanation and physical scaling of optical pulse evolution in free-carrier media and could enable improved supercontinuum sources in gas based and integrated semiconductor waveguides.

Pure-quartic solitons.

Temporal optical solitons have been the subject of intense research due to their intriguing physics and applications in ultrafast optics and supercontinuum generation. Conventional bright optical solitons result from the interaction of anomalous group-velocity dispersion and self-phase modulation. Here we experimentally demonstrate a class of bright soliton arising purely from the interaction of negative fourth-order dispersion and self-phase modulation, which can occur even for normal group-velocity dispersion. We provide experimental and numerical evidence of shape-preserving propagation and flat temporal phase for the fundamental pure-quartic soliton and periodically modulated propagation for the higher-order pure-quartic solitons. We derive the approximate shape of the fundamental pure-quartic soliton and discover that is surprisingly Gaussian, exhibiting excellent agreement with our experimental observations. Our discovery, enabled by precise dispersion engineering, could find applications in communications, frequency combs and ultrafast lasers.

Multi-photon absorption limits to heralded single photon sources.

Single photons are of paramount importance to future quantum technologies, including quantum communication and computation. Nonlinear photonic devices using parametric processes offer a straightforward route to generating photons, however additional nonlinear processes may come into play and interfere with these sources. Here we analyse spontaneous four-wave mixing (SFWM) sources in the presence of multi-photon processes. We conduct experiments in silicon and gallium indium phosphide photonic crystal waveguides which display inherently different nonlinear absorption processes, namely two-photon (TPA) and three-photon absorption (ThPA), respectively. We develop a novel model capturing these diverse effects which is in excellent quantitative agreement with measurements of brightness, coincidence-to-accidental ratio (CAR) and second-order correlation function g((2))(0), showing that TPA imposes an intrinsic limit on heralded single photon sources. We build on these observations to devise a new metric, the quantum utility (QMU), enabling further optimisation of single photon sources.