Nonlinear Nano-Imaging of Interlayer Coupling in 2D Graphene-Semiconductor Heterostructures.

The emergent electronic, spin, and other quantum properties of 2D heterostructures of graphene and transition metal dichalcogenides are controlled by the underlying interlayer coupling and associated charge and energy transfer dynamics. However, these processes are sensitive to interlayer distance and crystallographic orientation, which are in turn affected by defects, grain boundaries, or other nanoscale heterogeneities. This obfuscates the distinction between interlayer charge and energy transfer. Here, nanoscale imaging in coherent four-wave mixing (FWM) and incoherent two-photon photoluminescence (2PPL) is combined with a tip distance-dependent coupled rate equation model to resolve the underlying intra- and inter-layer dynamics while avoiding the influence of structural heterogeneities in mono- to multi-layer graphene/WSe2 heterostructures. With selective insertion of hBN spacer layers, it is shown that energy, as opposed to charge transfer, dominates the interlayer-coupled optical response. From the distinct nano-FWM and -2PPL tip-sample distance-dependent modification of interlayer and intralayer relaxation by tip-induced enhancement and quenching, an interlayer energy transfer time of τ ET ≈ ( 0 . 35 - 0.15 + 0.65 ) $\tau _{\rm ET} \approx (0.35^{+0.65}_{-0.15})$  ps consistent with recent reports is derived. As a local probe technique, this approach highlights the ability to determine intrinsic sample properties even in the presence of large sample heterogeneity.

Decoding ultrafast polarization responses in lead halide perovskites by the two-dimensional optical Kerr effect.

The ultrafast polarization response to incident light and ensuing exciton/carrier generation are essential to outstanding optoelectronic properties of lead halide perovskites (LHPs). A large number of mechanistic studies in the LHP field to date have focused on contributions to polarizability from organic cations and the highly polarizable inorganic lattice. For a comprehensive understanding of the ultrafast polarization response, we must additionally account for the nearly instantaneous hyperpolarizability response to the propagating light field itself. While light propagation is pivotal to optoelectronics and photonics, little is known about this in LHPs in the vicinity of the bandgap where stimulated emission, polariton condensation, superfluorescence, and photon recycling may take place. Here we develop two-dimensional optical Kerr effect (2D-OKE) spectroscopy to energetically dissect broadband light propagation and dispersive nonlinear polarization responses in LHPs. In contrast to earlier interpretations, the below-bandgap OKE responses in both hybrid CH3NH3PbBr3 and all-inorganic CsPbBr3 perovskites are found to originate from strong hyperpolarizability and highly anisotropic dispersions. In both materials, the nonlinear mixing of anisotropically propagating light fields results in convoluted oscillatory polarization dynamics. Based on a four-wave mixing model, we quantitatively derive dispersion anisotropies, reproduce 2D-OKE frequency correlations, and establish polarization-dressed light propagation in single-crystal LHPs. Moreover, our findings highlight the importance of distinguishing the often-neglected anisotropic light propagation from underlying coherent quasiparticle responses in various forms of ultrafast spectroscopy.

Extraordinary Five-Wave Mixing in a Zinc Oxide Microwire on a Au Film.

Coherent multiwave mixing is in demand for optical frequency conversion, imaging, quantum information science, etc., but has rarely been demonstrated in solid-state systems. Here, we observed three- and five-wave mixing (5WM) in a c-axis growth zinc oxide microwire on a Au film with picosecond pulses in the near-infrared region. An output 5WM of 4.7 × 10-7 µW, only 2-3 orders smaller than the three-wave mixing, is achieved when the excitation power is as low as 1.5 mW and the peak power density as weak as ∼107 W/cm2. The excitation power dependence of 5WM agrees well with the perturbation limit under the low intensity but exhibits a strong deviation at a high pumping power. This extraordinary behavior is attributed to the cooperative resonant enhancement effect when pumping in the near-infrared range. Our study offers a potential solid-state platform for on-chip multiwave mixing and quantum nonlinear optics, such as generating many-photon entangled states or the construction of photon-photon quantum logic gates.

Integrated Reconfigurable Photon-Pair Source Based on High-Q Nonlinear Chalcogenide Glass Microring Resonators.

Chalcogenide glasses (ChGs) have recently emerged as enabling materials for building reconfigurable nanophotonic devices by employing their refractive index changes associated with photosensitive effects. In particular, the availability of low-loss thin-film ChGs and the realization of high-Q microresonators provide exciting opportunities for integrated photonics. So far, the ChG photonic devices are predominately operated in the classical optics regime. In this work, we present the realization on-chip bright photon-pair quantum light sources via spontaneous four-wave mixing in a high-Q microring resonator fabricated on the newly developed ChG Ge25Sb10S65 platform. The emission wavelength of the photon-pair source can be continuously tuned across a double-free spectral range in a reconfigurable manner. Our work serves as a starting point to fully unleash the potential of exploiting ChGs for developing reconfigurable integrated quantum photonic devices.

Long-Lived Exciton Coherence in Mixed-Halide Perovskite Crystals.

Compositional engineering of the optical properties of hybrid organic-inorganic lead halide perovskites is crucial for the realization of efficient solar cells and light-emitting devices. We study the effect of band gap fluctuations on coherent exciton dynamics in a mixed FA0.9Cs0.1PbI2.8Br0.2 perovskite crystal by using photon echo spectroscopy. We reveal a narrow homogeneous exciton line width of 16 µeV at a temperature of 1.5 K. The corresponding exciton coherence time T2 = 83 ps is exceptionally long due to the localization of excitons at the scale of tens to hundreds of nanometers. From spectral and temperature dependences of the two- and three-pulse photon echo decay, we conclude that for low-energy excitons pure decoherence associated with elastic scattering on phonons is comparable with the exciton lifetime, while for excitons with higher energies, inelastic scattering to lower energy states via phonon emission dominates.

Ultrafast Nanoimaging of Electronic Coherence of Monolayer WSe2.

Transition-metal dichalcogenides (TMDs) have demonstrated a wide range of novel photonic, optoelectronic, and correlated electron phenomena for more than a decade. However, the coherent dynamics of their excitons, including possibly long dephasing times and their sensitivity to spatial heterogeneities, are still poorly understood. Here we implement adiabatic plasmonic nanofocused four-wave mixing (FWM) to image the coherent electron dynamics in monolayer WSe2. We observe nanoscale heterogeneities at room temperature with dephasing ranging from T2 ≲ 5 to T2 ≳ 60 fs on length scales of 50-100 nm. We further observe a counterintuitive anticorrelation between FWM intensity and T2, with the weakest FWM emission at locations of longest coherence. We interpret this behavior as a nonlocal nano-optical interplay between spatial coherence of the nonlinear polarization and disorder-induced scattering. The results highlight the challenges associated with heterogeneities in TMDs limiting their photophysical properties, yet also the potential of their novel nonlinear optical phenomena.

Research on Photoacoustic Synthetic Aperture Focusing Technology Imaging Method of Internal Defects in Cylindrical Components.

Cylindrical components are parts with curved surfaces, and their high-precision defect testing is of great significance to industrial production. This paper proposes a noncontact internal defect imaging method for cylindrical components, and an automatic photoacoustic testing platform is built. A synthetic aperture focusing technology in the polar coordinate system based on laser ultrasonic (LU-pSAFT) is established, and the relationship between the imaging quality and position of discrete points is analyzed. In order to verify the validity of this method, small holes of Φ0.5 mm in the aluminum alloy rod are tested. During the imaging process, since a variety of waveforms can be excited by the pulsed laser synchronously, the masked longitudinal waves reflected by small holes need to be filtered and windowed to achieve high-quality imaging. In addition, the influence of ultrasonic beam angle and signal array spacing on imaging quality is analyzed. The results show that the method can accurately present the outline of the small hole, the circumferential resolution of the small hole is less than 1° and the dimensional accuracy and position error are less than 0.1 mm.

Mixing of Non-Collinear Lamb Wave Pulses in Plates with Material Nonlinearity.

Guided waves have been extensively studied in the past few years, and more recently nonlinear guided waves have attracted significant research interest for their potential for early damage detection and material state characterization. Combined harmonic generation due to wave mixing can offer some advantages over second harmonic generation. However, studies focused on Lamb wave mixing are still very limited, and have mainly focused on collinear wave mixing and used plane wave assumption. In this paper, numerical simulations and experiments are conducted to understand the interaction of mixing non-collinear Lamb wave pulses with non-planar wavefronts. The results demonstrate that the generated secondary wave is cumulative under internal resonance conditions and the sum-frequency component of the combined harmonics is useful for characterizing material nonlinearities.

Sum-Frequency Generation in High-Q GaP Metasurfaces Driven by Leaky-Wave Guided Modes.

Resonant metasurfaces provide a unique platform for enhancing multiwave nonlinear interactions. However, the difficulties over mode matching and material transparency place significant challenges in the enhancement of these multiwave processes. Here we demonstrate efficient nonlinear sum-frequency generation (SFG) in multiresonant GaP metasurfaces based on guided-wave bound-state in the continuum resonances. The excitation of the metasurface by two near-infrared input beams generates strong SFG in the visible spectrum with a conversion efficiency of 2.5 × 10-4 W-1, 2 orders of magnitude higher than the one reported in Mie-type resonant metasurfaces. In addition, we demonstrate the nontrivial polarization dependence on the SFG process. In contrast to harmonic generation, the SFG process is enhanced when using nonparallel polarized input-beams. Importantly, by varying the input pump beam polarization it is possible to direct the SFG emission to different diffraction orders, thereby opening up new opportunities for nonlinear light sources and infrared to visible light conversion.

Bright and Dark Exciton Coherent Coupling and Hybridization Enabled by External Magnetic Fields.

Magnetic field- and polarization-dependent measurements on bright and dark excitons in monolayer WSe2 combined with time-dependent density functional theory calculations reveal intriguing phenomena. Magnetic fields up to 25 T parallel to the WSe2 plane lead to a partial brightening of the energetically lower lying exciton, leading to an increase of the dephasing time. Using a broadband femtosecond pulse excitation, the bright and partially allowed excitonic state can be excited simultaneously, resulting in coherent quantum beating between these states. The magnetic fields perpendicular to the WSe2 plane energetically shift the bright and dark excitons relative to each other, resulting in the hybridization of the states at the K and K' valleys. Our experimental results are well captured by time-dependent density functional theory calculations. These observations show that magnetic fields can be used to control the coherent dephasing and coupling of the optical excitations in atomically thin semiconductors.

Broadband Plasmon-Enhanced Four-Wave Mixing in Monolayer MoS2.

Two-dimensional transition-metal dichalcogenide monolayers have remarkably large optical nonlinearity. However, the nonlinear optical conversion efficiency in monolayer transition-metal dichalcogenides is typically low due to small light-matter interaction length at the atomic thickness, which significantly obstructs their applications. Here, for the first time, we report broadband (up to ∼150 nm) enhancement of optical nonlinearity in monolayer MoS2 with plasmonic structures. Substantial enhancement of four-wave mixing is demonstrated with the enhancement factor up to three orders of magnitude for broadband frequency conversion, covering the major visible spectral region. The equivalent third-order nonlinearity of the hybrid MoS2-plasmonic structure is in the order of 10-17 m2/V2, far superior (∼10-100-times larger) to the widely used conventional bulk materials (e.g., LiNbO3, BBO) and nanomaterials (e.g., gold nanofilms). Such a considerable and broadband enhancement arises from the strongly confined electric field in the plasmonic structure, promising for numerous nonlinear photonic applications of two-dimensional materials.

Multimode Nonlinear Coupling Induced by Internal Resonance in a Microcantilever Resonator.

Coupled resonators represent a generic model for many physical systems. In this context, a microcantilever is a multimode resonator clamped at one end, and it finds extensive application in high-precision metrology and is expected to be of great potential use in emerging quantum technologies. Here, we explore the microcantilever as a flexible platform for realizing multimode nonlinear interactions. Multimode nonlinear coupling is achieved by (1:2) internal resonance (IR) and parametric excitation with efficient coherent energy transfer. Specifically, we demonstrate abundant tunable parametric behaviors via frequency and voltage sweeps; these behaviors include mode veering, degenerate four-wave mixing (D4WM) with satellite resonances, partial amplitude suppression, acoustic frequency comb (AFC) generation, mechanically induced transparency (MIT), and normal-mode splitting. The experiments depict a new scheme for manipulating multimode microresonators with IR and parametric excitation.

Experimental and Numerical Investigation of the Micro-Crack Damage in Elastic Solids by Two-Way Collinear Mixing Method.

This study experimentally and numerically investigated the nonlinear behavior of the resonant bulk waves generated by the two-way collinear mixing method in 5052 aluminum alloy with micro-crack damage. When the primary longitudinal and transverse waves mixed in the micro-crack damage region, numerical and experimental results both verified the generation of resonant waves if the resonant condition ωL/ωT=2κ/(κ-1) was satisfied. Meanwhile, we found that the acoustic nonlinearity parameter (ANP) increases monotonously with increases in micro-crack density, the size of the micro-crack region, the frequency of resonant waves and friction coefficient of micro-crack surfaces. Furthermore, the micro-crack damage in a specimen generated by low-temperature fatigue experiment was employed. It was found that the micro-crack damage region can be located by scanning the specimen based on the two-way collinear mixing method.

Theoretical and Experimental Investigation of the Effect of Pump Laser Frequency Fluctuations on Signal-to-Noise Ratio of Brillouin Dynamic Grating Measurement with Coherent FMCW Reflectometry.

Signal-dependent speckle-like noise has constituted a serious factor in Brillouin-grating based frequency-modulated continuous-wave (FMCW) reflectometry and it has been indispensable for improving the signal-to-noise ratio (S/N) of the Brillouin dynamic grating measurement to clarify the noise generation mechanism. In this paper we show theoretically and experimentally that the noise is generated by the frequency fluctuations of the pump light from a laser diode (LD). We could increase the S/N from 36 to 190 merely by driving the LD using a current source with reduced technical noise. On the basis of our experimental result, we derived the theoretical formula for S/N as a function of distance, which contained the second and fourth-order moments of the frequency fluctuations, by assuming that the pump light frequency was modulated by the technical noise. We calculated S/N along the 1.35 m long optical fiber numerically using the measured power spectral density of the frequency fluctuations, and the resulting distributions agreed with the measured values in the 10 to 190 range. Since higher performance levels are required if the pump light source is to maintain the S/N as the fiber length increases, we can use the formula to calculate the light source specifications including the spectral width and rms value of the frequency fluctuations to achieve a high S/N while testing a fiber of a given length.

Nonlinear Guided-Wave Mixing for Condition Monitoring of Bolted Joints.

Bolted joints are fundamental to numerous structural components in engineering practice. Nevertheless, their failure or even their loosening can lead to insufficient performance and reduced structural safety. This study presents a theoretical development and experimental investigation into nonlinear guided-wave mixing for integrity monitoring of bolted joints in plates. Combinational harmonics generated due to nonlinear Lamb wave mixing and contact acoustic nonlinearity at the bolted joints were used to evaluate the applied torque level in the joint. The area of the power spectral density in the region of the sum combinational harmonic bandwidth is found to be highly correlated to the applied torque level at the joint. Moreover, the effect of the number of cycles and thus the time duration of the excitation is investigated. The results show that the combinational harmonics remain robust for different numbers of cycles in detecting bolt loosening. The findings presented in this study also provide physical insight into the phenomena of nonlinear Lamb wave mixing for evaluating applied torque in bolted joints, and the results help further advance the use of nonlinear guided waves for damage detection.

Wavelength-Tunable L-Band High Repetition Rate Erbium-Doped Fiber Laser Based on Dissipative Four-Wave Mixing.

A wavelength-tunable high repetition rate (HRR) erbium-doped fiber laser in L-band based on dissipative four-wave mixing (DFWM) mechanism is demonstrated. The cavity can generate a single-soliton train and bound-soliton train with a fixed repetition rate of ~126 GHz, which is determined by the free spectral range of the intra-cavity Lyot filter. A wide wavelength-tuning operation can also be obtained by rotating the polarization controllers. The wavelength-tuning ranges of the HRR single-soliton state and HRR bound-soliton state are ~38.3 nm and ~22.6 nm, respectively. This laser provides useful references for the area of a wavelength-tunable fiber laser with high repetition rate. The laser may also find useful applications in high-speed communication, sensing, etc.

Electrically Tunable Four-Wave-Mixing in Graphene Heterogeneous Fiber for Individual Gas Molecule Detection.

Detection of individual molecules is the ultimate goal of any chemical sensor. In the case of gas detection, such resolution has been achieved in advanced nanoscale electronic solid-state sensors, but it has not been possible so far in integrated photonic devices, where the weak light-molecule interaction is typically hidden by noise. Here, we demonstrate a scheme to generate ultrasensitive down-conversion four-wave-mixing (FWM) in a graphene bipolar-junction-transistor heterogeneous D-shaped fiber. In the communication band, the FWM conversion efficiency can change steeply when the graphene Fermi level approaches 0.4 eV. In this condition, we exploit our unique two-step optoelectronic heterodyne detection scheme, and we achieve real-time individual gas molecule detection in vacuum. Such combination of graphene strong nonlinearities, electrical tunability, and all-fiber integration paves the way toward the design of versatile high-performance graphene photonic devices.

Simplified Near-Degenerate Four-Wave-Mixing Microscopy.

Four-wave-mixing microscopy is widely researched in both biology and medicine. In this paper, we present a simplified near-degenerate four-wave-mixing microscopy (SNDFWM). An ultra-steep long-pass filter is utilized to produce an ultra-steep edge on the spectrum of a femtosecond pulse, and a super-sensitive four-wave-mixing (FWM) signal can be generated via an ultra-steep short-pass filter. Compared with the current state-of-the-art FWM microscopy, this SNDFWM microscopy has the advantages of simpler experimental apparatus, lower cost, and easier operation. We demonstrate that this SNDFWM microscopy has high sensitivity and high spatial resolution in both nanowires and biological tissues. We also show that the SNDFWM microscopy can achieve an ultra-sensitive detection based on the electron-resonance effect. This method might find an important application in tracking of nano drugs in vivo.

2D Layered Graphene Oxide Films Integrated with Micro-Ring Resonators for Enhanced Nonlinear Optics.

Layered 2D graphene oxide (GO) films are integrated with micro-ring resonators (MRRs) to experimentally demonstrate enhanced nonlinear optics. Both uniformly coated (1-5 layers) and patterned (10-50 layers) GO films are integrated on complementary-metal-oxide-semiconductor (CMOS)-compatible doped silica MRRs using a large-area, transfer-free, layer-by-layer GO coating method with precise control of the film thickness. The patterned devices further employ photolithography and lift-off processes to enable precise control of the film placement and coating length. Four-wave-mixing (FWM) measurements for different pump powers and resonant wavelengths show a significant improvement in efficiency of ≈7.6 dB for a uniformly coated device with 1 GO layer and ≈10.3 dB for a patterned device with 50 GO layers. The measurements agree well with theory, with the enhancement in FWM efficiency resulting from the high Kerr nonlinearity and low loss of the GO films combined with the strong light-matter interaction within the MRRs. The dependence of GO's third-order nonlinearity on layer number and pump power is also extracted from the FWM measurements, revealing interesting physical insights about the evolution of the GO films from 2D monolayers to quasi bulk-like behavior. These results confirm the high nonlinear optical performance of integrated photonic resonators incorporated with 2D layered GO films.

Theoretical Investigation of an Alcohol-Filled Tellurite Photonic Crystal Fiber Temperature Sensor Based on Four-Wave Mixing.

For this study, a temperature sensor utilizing a novel tellurite photonic crystal fiber (PCF) is designed. In order to improve the sensor sensitivity, alcohol is filled in the air holes of the tellurite PCF. Based on the degenerate four-wave mixing theory, temperature sensing in the mid-infrared region (MIR) can be achieved by detecting the wavelength shift of signal waves and idler waves during variations in temperature. Simulation results show that at a pump wavelength of 3550 nm, the temperature sensitivity of this proposed sensor can be as high as 0.70 nm/°C. To the best of our knowledge, this is the first study to propose temperature sensing in the MIR by drawing on four-wave mixing (FWM) in a non-silica PCF.