Broadband nonlinear conversion and random quasi-phase-matching in transparent glass composite.

With the development of laser technology, nonlinear optics plays a crucial role in frequency conversion. However, the generation of second harmonics in nonlinear optical crystals is generally subject to rigorous phase-matching conditions that hinder the performance of broadband tunability. It is believed that introducing disorders in nonlinear optical materials is helpful to overcome this obstacle. In this work, we have prepared a nonlinear microcrystal-doped glass (NMG) composite material, allowing for tunable and polarization-independent nonlinear conversion from visible to near-infrared. The linear dependence of SHG intensity versus sample thickness indicated the facilitation of random quasi-phase matching by using the NMG. Our results provide a more stable and promising platform for disordered nonlinear photonic materials and suggest the possibility of more efficient nonlinear conversions using the NMG composite glass fibers in future.

Boosted Second Harmonic Generation and Cascaded Sum Frequency Generation from a Surface Crystallized Glass Ceramic Microcavity.

The development of novel materials and structures for efficient second-order nonlinear micro/nano devices remains a significant challenge. In this study, the remarkable enhancement of second-harmonic generation (SHG) and cascaded sum frequency generation in whispering gallery mode microspheres made of surface-crystallized glass with a 6-µm Ba2TiSi2O8 crystal layer are demonstrated. Attributed to the core-shell design, the Ba2TiSi2O8 located on the surface can be efficiently coupled with whispering gallery modes, resulting in a highly efficient micron-scale cavity-enhanced second-order optical nonlinearity. Greatly enhanced SHG of the microcavity is observed, which is up to 80 times stronger than that of a non-resonant sample. Furthermore, owing to the wavelength non-selectivity of random quasi-phase matching, ultra-wideband SHG with a strong response ranging from 860 to 1600 nm and high-contrast polarization characteristics is demonstrated. The glass-ceramic-based microsphere cavity also boosts the cascading optical nonlinearity, manifested by a two-magnitude enhancement of cascaded sum frequency generation. This work delineates an efficient strategy for boosting nonlinear optical response in glass ceramics, which will open up new opportunities for applications in photonics and optical communications.

Efficient Mode Conversion from a Standard Single-Mode Fiber to a Subwavelength-Diameter Microfiber.

Efficient mode conversion is crucial for hybrid photonic systems. We present efficient light transition from a standard single-mode fiber (SMF) to a subwavelength-diameter microfiber via a relatively short tapered fiber. Numerical simulations were performed to design the tapered morphology with high transmittance (approximately 86%) for the fundamental modes. The designed tapered fiber was successfully fabricated on the top of a cleaved SMF tip by the direct laser writing (DLW) method. For the 1550 nm wavelength, the transmittance from the standard SMF to the subwavelength-diameter microfiber was determined to be 77%, accompanied by a change in the effective mode area from 38 µm2 to 0.47 µm2 within a very short length of 150 µm. Our result demonstrated the versatility of the DLW technique for boosting the mode conversion efficiency of fiber-to-chip devices, enabling various applications in the future.

589†nm yellow laser pumped Kerr-lens mode-locked Alexandrite laser producing sub-50†fs pulses.

We report a femtosecond Kerr-lens mode-locked (KLM) Alexandrite laser resonantly pumped by a 589 nm yellow laser. The 4 nJ pulses as short as 42 fs were obtained corresponding to a peak power of 100 kW. With the repetition rate of 104 MHz, the average power of 420 mW was attained. The time-bandwidth product of generated laser pulse was measured to be 0.324 with a beam quality factor of M2 ≤ 1.13. The exceptional performance of visible femtosecond laser may find potential applications in various fields.

450†W pulsed laser system with M2 < 1.2 based on a 969-nm laser diode end-pumped Yb:YAG rod amplifier.

We demonstrated a compact and power-efficient multi-stage pulsed end-pumped amplifier with stabilized output power of 450 W and near-diffraction-limited beam quality (M2 < 1.2) at a repetition rate of 1 MHz. The pulsed amplifier produced an exceptional average power and optimal beam quality achieved in laser diode (LD) end-pumped Yb:YAG thin rod configuration at room temperature. A preliminary pulse compression with a chirped volume Bragg grating (CVBG) was performed reducing pulse duration to ∼730 fs at a compression efficiency of 90%. With the combined features, including compactness, reliability, and efficiency, of the end-pumped scheme, the demonstrated laser system would be of great value in both industry and scientific research.

Watt-level tunable Ti:Sapphire laser directly pumped with green laser diodes.

We demonstrate a Ti:Sapphire laser generating in excess of 1.2 W in continuous-wave operation when pumped directly with four green laser diodes eliminating the need for a complex pump laser. As a result, improvement of laser efficiency is achieved without sacrificing beam quality. Tunability within the range of 740-840 nm is attained validating the concept of a direct laser-diode pumped Ti:Sapphire laser.

Functionalization of Pentacene: A Facile and Versatile Approach to Contorted Polycyclic Aromatic Hydrocarbons.

In this work, a facile and versatile strategy for the synthesis of contorted polycyclic aromatic hydrocarbons (PAHs) starting from the functionalized pentacene was established. A series of novel PAHs 1-4 and their derivatives were synthesized through a simple two-step synthesis procedure involving an intramolecular reductive Friedel-Crafts cyclization of four newly synthesized pentacene aldehydes 5-8 as a key step. All the molecules were confirmed by single-crystal X-ray diffraction and their photophysical and electrochemical properties were studied in detail. Interestingly, the most striking feature of 1-4 is their highly contorted carbon structures and the accompanying helical chirality. In particular, the optical resolution of 2 was successfully achieved by chiral-phase HPLC, and the enantiomers were characterized by circular dichroism and circularly polarized luminescence spectroscopy. Despite the highly nonplanar conformations, these contorted PAHs exhibited emissive properties with moderate-to-good fluorescence quantum yields, implying the potential utility of this series PAHs as high-quality organic laser dyes. By using a self-assembly method with the help of epoxy resin, a bottle microlaser based on 3 a was successfully illustrated with a lasing wavelength of 567.8 nm at a threshold of 0.3 mJ/cm2 . We believe that this work will shed light on the chemical versatility of pentacene and its derivatives in the construction of novel functionalized PAHs.

Intense and Superflat White Laser with 700-nm 3-dB Bandwidth and 1-mJ Pulse Energy Enabling Single-Shot Subpicosecond Pulse Laser Spectroscopy.

An optical spectrometer is a basic spectral instrument that probes microscopic physical and chemical properties of macroscopic objects but generally suffers from difficulty in broadband time-resolved measurement. In this work, we report the creation of ultrabroadband white-light laser with a 3-dB bandwidth covering 385 to 1,080 nm, pulse energy of 1.07 mJ, and pulse duration of several hundred femtoseconds by passing 3-mJ pulse energy, 50-fs pulse duration Ti:Sapphire pulse laser through a cascaded fused silica plate and chirped periodically poled lithium niobate crystal. We utilize this unprecedented superflat, ultrabroadband, and intense femtosecond laser light source to build a single-shot (i.e., single-pulse) subpicosecond pulse laser ultraviolet-visible-near-infrared spectrometer and successfully measure various atomic and molecular absorption spectra. The single-shot ultrafast spectrometer may open up a frontier to monitor simultaneously the ultrafast dynamics of multiple physical and chemical processes in various microscopic systems.

Magnetically Tunable One-Dimensional Plasmonic Photonic Crystals.

Integrating plasmonic resonance into photonic bandgap nanostructures promises additional control over their optical properties. Here, one-dimensional (1D) plasmonic photonic crystals with angular-dependent structural colors are fabricated by assembling magnetoplasmonic colloidal nanoparticles under an external magnetic field. Unlike conventional 1D photonic crystals, the assembled 1D periodic structures show angular-dependent colors based on the selective activation of optical diffraction and plasmonic scattering. They can be further fixed in an elastic polymer matrix to produce a photonic film with angular-dependent and mechanically tunable optical properties. The magnetic assembly enables precise control over the orientation of the 1D assemblies within the polymer matrix, producing photonic films with designed patterns displaying versatile colors from the dominant backward optical diffraction and forward plasmonic scattering. The combination of optical diffraction and plasmonic properties within a single system holds the potential for developing programmable optical functionalities for applications in various optical devices, color displays, and information encryption systems.

Ionic-Wind-Enhanced Raman Spectroscopy without Enhancement Substrates.

Raman spectra are often masked by strong fluorescence, which severely hinders the applications of Raman spectroscopy. Herein, for the first time, we report ionic-wind-enhanced Raman spectroscopy (IWERS) incorporated with photobleaching (PB) as a noninvasive approach to detect fluorescent and vulnerable samples without a substrate. In this study, ionic wind (IW) generated by needle-net electrodes transfers charges to the sample surface in air on the scale of millimeters rather than nanometers in surface-enhanced Raman spectroscopy. Density functional theory calculations reveal that the ionic particles in IW increase the susceptibility of the sample molecules, thus enhancing the Raman signals. Meanwhile, the incorporation of IW with PB yields a synergistic effect to quench fluorescence. Therefore, this approach can improve the signal-to-noise ratio of Raman peaks up to three times higher than that with only PB. At the same time, IWERS can avoid sample pollution and destruction without substrates as well as high laser power. For archeological samples and a red rock as an analogue to Mars geological samples, IWERS successfully identified weak but key Raman peaks, which were masked by strong florescence. It suggests that IWERS is a promising tool for characterizations in the fields of archeology, planetary science, biomedicine, and soft matter.

3,6-Carbazoylene Octaphyrin (1.0.0.0.1.0.0.0) and Its Bis-BF2 Complex.

3,6-Carbazole precursors were used to prepare an octaphyrin. The conformation and electronic structure of the system could be modulated through trifluoroacetate (TFA) protonation and BF2 complexation. The resulting nonaromatic macrocyclic complexes, 2-2TFA and 2-2BF2, displayed noteworthy photophysical properties. For instance, the diprotonated species 2-2TFA showed a strong panchromic absorption up to 800 nm, while the bis-BF2-chelated dipyrromethene (BODIPY)-like complex 2-2BF2 exhibited an intense visible absorption feature (ε535nm = 2.1 × 105 M-1 cm-1), as well as a relatively red-shifted emission at 640 nm characterized by a large Stokes shift. It was found that 2-2BF2 could be used to construct a high-quality organic microlaser that functions under optical pumping. The present study highlights the potential utility of expanded porphyrins as possible laser dyes.

Manipulating Nonlinear Optical Response via Domain Control in Nanocrystal-in-Glass Composites.

Nanocrystal-in-glass (NIG) is an exciting class of composites, because it can not only combine the advantages of crystal and glass materials but also potentially generate new physical phenomenon in a cooperative manner. Herein, the nonlinear light-matter interaction processes in a broad range of NIG composites homogeneously embedded with LiNbO3 are investigated. It is shown that, by rational control of the organization manner of crystal and glass phases, second-harmonic generation (SHG) can be precisely tuned. Importantly, an unusual SHG phenomenon, transverse SHG (TSHG), can be realized in the special region of the microstructure map combined with the features of high loading, nanoscale size, and homogenous distribution of nanocrystals. Furthermore, NIG composites exhibit broadband optical response, allowing TSHG in a wide waveband region to be achieved. Based on the above effects, the applications of the constructed NIG composite for precise measurement of the group velocity and duration of ultrashort optical pulses with femtosecond time scales are demonstrated. Indeed, the findings outline a fundamental principle to design NIG configurations for creating new properties, providing new directions for expanding the scope of NIG functional materials.

Plasmon-driven nanowire actuators for on-chip manipulation.

Chemically synthesized metal nanowires are promising building blocks for next-generation photonic integrated circuits, but technological implementation in monolithic integration will be severely hampered by the lack of controllable and precise manipulation approaches, due to the strong adhesion of nanowires to substrates in non-liquid environments. Here, we demonstrate this obstacle can be removed by our proposed earthworm-like peristaltic crawling motion mechanism, based on the synergistic expansion, friction, and contraction in plasmon-driven metal nanowires in non-liquid environments. The evanescently excited surface plasmon greatly enhances the heating effect in metal nanowires, thereby generating surface acoustic waves to drive the nanowires crawling along silica microfibres. Advantages include sub-nanometer positioning accuracy, low actuation power, and self-parallel parking. We further demonstrate on-chip manipulations including transporting, positioning, orientation, and sorting, with on-situ operation, high selectivity, and great versatility. Our work paves the way to realize full co-integration of various functionalized photonic components on single chips.

Efficient Organic Light-Emitting Transistors Based on High-Quality Ambipolar Single Crystals.

A cyano-substituted styrene derivative is synthesized and successfully prepared to lamellate single crystals through precisely controlling the crystal growth conditions. The lamellate single crystals with regular edge and smooth surface display intrinsically ordered stacking and high quality, all of which are of importance for high optoelectronic performance. The single-component light-emitting transistors based on the lamellate crystals offer striking device performance in terms of record external quantum efficiency of 2.02%, exceeding the benchmark value in this field. Such organic light-emitting single crystals provide a versatile platform for designing and engineering their structures and optoelectronic properties toward light-emitting devices.

Microlasers from AIE-Active BODIPY Derivative.

Organic microlasers have attracted much attention due to their unique features such as high mechanical flexibility, facile doping of gain materials, high optical quality, simplicity and low-cost fabrication. However, organic gain materials usually suffer from aggregation-caused quenching (ACQ), preventing further advances of organic microlasers. Here, a new type of microlaser from aggregation-induced emission (AIE) material is successfully demonstrated. By introducing a typical noncrystalline AIE material, a high quality microlaser is obtained via a surface tension-induced self-assembly approach. Distinct from conventional organic microlasers, the organic luminescent material used here is initially nonluminescent but can shine after aggregation under optical pumping. Further investigations demonstrate that AIE-based microlasers exhibit advantages to enable much higher doping concentrations, which provides an alternative way to improved lasing performance including dramatically reduced threshold and favorable lasing stability. It is believed that these results could provide a promising way to extend the content of microlasers and open a new avenue to enable applications ranging from chemical sensing to biology.

A highly emissive AIE-active luminophore exhibiting deep-red to near-infrared piezochromism and high-quality lasing.

Further development of high-efficiency and low-cost organic fluorescent materials is intrinsically hampered by the energy gap law and spin statistics, especially in the near-infrared (NIR) region. Here we design a novel building block with aggregation-induced emission (AIE) activity for realizing highly efficient luminophores covering the deep-red and NIR region, which originates from an increase in the orbital overlap and electron-withdrawing ability. An organic donor-acceptor molecule (BPMT) with the building block is prepared and can readily form J-type molecular columns with multiple C-H⋯N/O interactions. Notably, such synthesized materials can emit fluorescence centered at 701 nm with extremely high photoluminescence quantum yields (PLQYs) of 48.7%. Experimental and theoretical investigations reveal that the formation of the hybridized local and charge-transfer (HLCT) state and substantial C-H⋯N/O interactions contribute to a fast radiative decay rate and a slow nonradiative decay rate, respectively, resulting in high PLQYs in the solid state covering the NIR range. Remarkably, such BPMT crystals, as a first example, reveal strong-penetrability piezochromism along with a distinct PL change from the deep-red (λ max = 704 nm) to NIR (λ max = 821 nm) region. Moreover, such typical AIE-active luminophores are demonstrated to be a good candidate as a lasing medium. Together with epoxy resin by a self-assembly method, a microlaser is successfully illustrated with a lasing wavelength of 735.2 nm at a threshold of 22.3 kW cm-2. These results provide a promising approach to extend the contents of deep-red/NIR luminophores and open a new avenue to enable applications ranging from chemical sensing to lasing.

Polarization-Dependent Lateral Optical Force of Subwavelength-Diameter Optical Fibers.

It is highly desirable to design optical devices with diverse optomechanical functions. Here, we investigate lateral optical force exerted on subwavelength-diameter (SD) optical fibers harnessed by input light modes with different polarizations. It is interesting to find that input light modes of circular or elliptical polarizations would bring about lateral optical force in new directions, which has not been observed in previous studies. By means of finite-difference time-domain (FDTD) simulations, detailed spatial distributions of the asymmetric transverse force density are revealed, meanwhile dependence of optical force on input light polarizations, fiber diameters, and inclination angles of fiber endfaces are all carefully discussed. It is believed that polarization-sensitive reflection, refraction, and diffraction of optical fields occur at the interface, i.e., fiber oblique endfaces, resulting in asymmetrically distributed optical fields and thereafter non-zero transverse optical force. We believe our new findings could be helpful for constructing future steerable optomechanical devices with more flexibility.

Transverse optical forces and sideways deflections in subwavelength-diameter optical fibers.

We investigate transverse optical forces exerted on the endface of subwavelength-diameter (SD) optical fiber by using a finite-difference time-domain (FDTD) method. Detailed spatial distributions of transverse optical force along the fiber axis can now be accessible, based on which the dependence of transverse optical force on transverse cross sections, oblique-cut endfaces and high-order mode are carefully studied. Our numerical results demonstrate that either asymmetric cross section or oblique-cut endface would dominantly contribute to the transverse optical force and the corresponding sideways deflection of SD fiber, which is in good agreement with previous experimental observations. The novel behavior of transverse optical force by the high-order mode would give rise to new guidelines for constructing high-performance optomechanical devices.

Anisotropically Shaped Magnetic/Plasmonic Nanocomposites for Information Encryption and Magnetic-Field-Direction Sensing.

Instantaneous control over the orientation of anisotropically shaped plasmonic nanostructures allows for selective excitation of plasmon modes and enables dynamic tuning of the plasmonic properties. Herein we report the synthesis of rod-shaped magnetic/plasmonic core-shell nanocomposite particles and demonstrate the active tuning of their optical property by manipulating their orientation using an external magnetic field. We further design and construct an IR-photoelectric coupling system, which generates an output voltage depending on the extinction property of the measured nanocomposite sample. We employ the device to demonstrate that the nanocomposite particles can serve as units for information encryption when immobilized in a polymer film and additionally when dispersed in solution can be employed as a new type of magnetic-field-direction sensor.

High-Efficiency Light-Emitting Diodes of Organometal Halide Perovskite Amorphous Nanoparticles.

Organometal halide perovskite has recently emerged as a very promising family of materials with augmented performance in electronic and optoelectronic applications including photovoltaic devices, photodetectors, and light-emitting diodes. Herein, we propose and demonstrate facile solution synthesis of a series of colloidal organometal halide perovskite CH3NH3PbX3 (X = halides) nanoparticles with amorphous structure, which exhibit high quantum yield and tunable emission from ultraviolet to near-infrared. The growth mechanism and photoluminescence properties of the perovskite amorphous nanoparticles were studied in detail. A high-efficiency green-light-emitting diode based on amorphous CH3NH3PbBr3 nanoparticles was demonstrated. The perovskite amorphous nanoparticle-based light-emitting diode shows a maximum luminous efficiency of 11.49 cd/A, a power efficiency of 7.84 lm/W, and an external quantum efficiency of 3.8%, which is 3.5 times higher than that of the best colloidal perovskite quantum-dot-based light-emitting diodes previously reported. Our findings indicate the great potential of colloidal perovskite amorphous nanoparticles in light-emitting devices.