Permittivity tensor imaging: modular label-free imaging of 3D dry mass and 3D orientation at high resolution.

The dry mass and the orientation of biomolecules can be imaged without a label by measuring their permittivity tensor (PT), which describes how biomolecules affect the phase and polarization of light. Three-dimensional (3D) imaging of PT has been challenging. We present a label-free computational microscopy technique, PT imaging (PTI), for the 3D measurement of PT. PTI encodes the invisible PT into images using oblique illumination, polarization-sensitive detection and volumetric sampling. PT is decoded from the data with a vectorial imaging model and a multi-channel inverse algorithm, assuming uniaxial symmetry in each voxel. We demonstrate high-resolution imaging of PT of isotropic beads, anisotropic glass targets, mouse brain tissue, infected cells and histology slides. PTI outperforms previous label-free imaging techniques such as vector tomography, ptychography and light-field imaging in resolving the 3D orientation and symmetry of organelles, cells and tissue. We provide open-source software and modular hardware to enable the adoption of the method.

Flexible fluid-based encapsulation platform for water-sensitive materials.

The next-generation semiconductors and devices, such as halide perovskites and flexible electronics, are extremely sensitive to water, thus demanding highly effective protection that not only seals out water in all forms (vapor, droplet, and ice), but simultaneously provides mechanical flexibility, durability, transparency, and self-cleaning. Although various solid-state encapsulation methods have been developed, no strategy is available that can fully meet all the above requirements. Here, we report a bioinspired liquid-based encapsulation strategy that offers protection from water without sacrificing the operational properties of the encapsulated materials. Using halide perovskite as a model system, we show that damage to the perovskite from exposure to water is drastically reduced when it is coated by a polymer matrix with infused hydrophobic oil. With a combination of experimental and simulation studies, we elucidated the fundamental transport mechanisms of ultralow water transmission rate that stem from the ability of the infused liquid to fill-in and reduce defects in the coating layer, thus eliminating the low-energy diffusion pathways, and to cause water molecules to diffuse as clusters, which act together as an excellent water permeation barrier. Importantly, the presence of the liquid, as the central component in this encapsulation method provides a unique possibility of reversing the water transport direction; therefore, the lifetime of enclosed water-sensitive materials could be significantly extended via replenishing the hydrophobic oils regularly. We show that the liquid encapsulation platform presented here has high potential in providing not only water protection of the functional device but also flexibility, optical transparency, and self-healing of the coating layer, which are critical for a variety of applications, such as in perovskite solar cells and bioelectronics.

Three-dimensional laser micromachining system with integrated sub-100†nm resolution in-situ measurement.

In this study, a three-dimensional (3D) laser micromachining system with an integrated sub-100 nm resolution in-situ measurement system was proposed. The system used the same femtosecond laser source for in-situ measurement and machining, avoiding errors between the measurement and the machining positions. It could measure the profile of surfaces with an inclination angle of less than 10°, and the measurement resolution was greater than 100 nm. Consequently, the precise and stable movement of the laser focus could be controlled, enabling highly stable 3D micromachining. The results showed that needed patterns could be machined on continuous surfaces using the proposed system. The proposed machining system is of great significance for broadening the application scenarios of laser machining.

Arbitrary fabrication of complex lithium niobate three-dimensional microstructures for second harmonic generation enhancement.

Lithium niobate (LN) crystal plays important roles in future integrated photonics, but it is still a great challenge to efficiently fabricate three-dimensional micro-/nanostructures on it. Here, a femtosecond laser direct writing-assisted liquid back-etching technology (FsLDW-LBE) is proposed to achieve the three-dimensional (3D) microfabrication of lithium niobate (LN) with high surface quality (Ra = 0.422 nm). Various 3D structures, such as snowflakes, graphic arrays, criss-cross arrays, and helix arrays, have been successfully fabricated on the surface of LN crystals. As an example, a microcone array was fabricated on LN crystals, which showed a strong second harmonic signal enhancement with up to 12 times bigger than the flat lithium niobate. The results indicate that the method provides a new approach for the microfabrication of lithium niobate crystals for nonlinear optics.

Single femtosecond pulse writing of a bifocal lens.

In this Letter, a method for the fabrication of bifocal lenses is presented by combining surface ablation and bulk modification in a single laser exposure followed by the wet etching processing step. The intensity of a single femtosecond laser pulse was modulated axially into two foci with a designed computer-generated hologram (CGH). Such pulse simultaneously induced an ablation region on the surface and a modified volume inside the fused silica. After etching in hydrofluoric acid (HF), the two exposed regions evolved into a bifocal lens. The area ratio (diameter) of the two lenses can be flexibly adjusted via control of the pulse energy distribution through the CGH. Besides, bifocal lenses with a center offset as well as convex lenses were obtained by a replication technique. This method simplifies the fabrication of micro-optical elements and opens a highly efficient and simple pathway for complex optical surfaces and integrated imaging systems.

Genome-wide identification and comparative analysis of DNA methyltransferase and demethylase gene families in two ploidy Cyclocarya paliurus and their potential function in heterodichogamy.

BACKGROUND: DNA methylation is one of the most abundant epigenetic modifications, which plays important roles in flower development, sex differentiation, and regulation of flowering time. Its pattern is affected by cytosine-5 DNA methyltransferase (C5-MTase) and DNA demethylase (dMTase). At present, there are no reports on C5-MTase and dMTase genes in heterodichogamous Cyclocarya paliurus. RESULTS: In this study, 6 CpC5-MTase and 3 CpdMTase genes were identified in diploid (2n = 2 × = 32) C. paliurus, while 20 CpC5-MTase and 13 CpdMTase genes were identified in autotetraploid (2n = 4 × = 64). 80% of identified genes maintained relatively fixed positions on chromosomes during polyploidization. In addition, we found that some DRM subfamily members didn't contain the UBA domain. The transcript abundance of CpC5-MTase and CpdMTase in male and female flowers of two morphs (protandry and protogyny) from diploidy was analyzed. Results showed that all genes were significantly up-regulated at the stage of floral bud break (S2), but significantly down-regulated at the stage of flower maturation (S4). At S2, some CpC5-MTase genes showed higher expression levels in PG-M than in PG-F, whereas some CpdMTase genes showed higher expression levels in PA-M than in PA-F. In addition, these genes were significantly associated with gibberellin synthesis-related genes (e.g. DELLA and GID1), suggesting that DNA methylation may play a role in the asynchronous floral development process through gibberellin signal. CONCLUSIONS: These results broaden our understanding of the CpC5-MTase and CpdMTase genes in diploid and autotetraploid C. paliurus, and provide a novel insight into regulatory mechanisms of DNA methylation in heterodichogamy.

Ultralow birefringent glass waveguide fabricated by femtosecond laser direct writing.

Optical waveguides prepared by femtosecond laser direct writing have birefringent properties, which can affect polarization encoding and entanglement on chips. Here, we first propose a shape-stress dual compensation fabrication scheme to decrease birefringence. Ultralow birefringent waveguides (1 × 10-9) were obtained by controlling the cross sectional shape of the main waveguide and adjusting the position of the auxiliary lines. In addition, we prepared polarization-independent directional coupler and demonstrated the evolution of polarization-independent waveguide array with different polarized light. In the future, ultralow birefringent waveguides will be widely applied in polarization encoding and entangled quantum photonic integrated circuits.

Machine vision-based high-precision and robust focus detection for femtosecond laser machining.

We propose a machine vision-based focus detection method (MVFD) for femtosecond laser machining. By analyzing the laser focus pattern, the defocus direction and distance are obtained simultaneously. The proposed technique presents high precision with an average error of 0.047 µm and a root mean square error (RMSE) of 0.055 µm. Moreover, the method is robust and is less affected by the tilted sample. For the curved surface sample, the average error and RMSE are 0.093 and 0.145 µm, respectively. Thus, the proposed focus detection method can be easily combined with laser processing equipment, which is widely used in large-range and high-precision femtosecond laser processing.

Ultrafast laser-inscribed nanogratings in sapphire for geometric phase elements.

We systematically studied femtosecond laser-inscribed self-organized nanogratings and geometric phase elements such as a polarization diffraction focusing lens and Q-plate in sapphire crystal. Besides the void structures observed in the focus, nanogratings with periods of 150~300 nm were observed, depending on a nanoslit that took the role of a seeding effect by localized light field enhancement. The non-polarized refractive index change and birefringence were measured with values around 1∼2×10-3 and 6×10-4, respectively. Based on the laser-inscribed form birefringence, a geometric phase lens and Q-plate were successfully demonstrated in sapphire with high imaging and a focusing effect. We expect that our findings may promote the understanding of laser-induced nanogratings in bulk and potential applications in geometric phase elements.

Metastable Intermediates in Amorphous Titanium Oxide: A Hidden Role Leading to Ultra-Stable Photoanode Protection.

Metastable intermediates represent a non-equilibrium state of matter that may impose profound impacts to materials properties beyond our understandings of monolithic and equilibrium systems. Here, we report a discovery of hidden metastable intermediates in amorphous TiO2 thin films and their critical role in electrochemical damage. These intermediates have a non-bulk crystal-like structure and exhibit significantly higher electrical conductivity than both the amorphous and the crystalline phases. When these TiO2 films are applied to protect Si photoelectrochemical (PEC) photoanodes, the intermediates can induce localized high electrical currents that largely accelerate the etching of the TiO2 film and the Si electrode underneath. The intermediates can be effectively suppressed by raising their nucleation barrier via reducing the film thickness from 24 to 2.5 nm. The homogeneous amorphous TiO2-film-coated Si photoanodes achieved more than 500 h of PEC water oxidation at a steady photocurrent density of over 30 mA·cm-2.

Mirror-rotation-symmetrical single-focus spiral zone plates.

In this Letter, we report mirror-rotation-symmetrical single-focus spiral zone plates (MS-SZPs) fabricated by femtosecond laser direct writing. The novel optical element can generate a single-focus vortex beam, owing to the element's complicated continuous surface. The MS-SZP surface possesses reverse mirror-rotation symmetry, which ensures that the transfer element has the same surface morphology as the original element. Both the transfer element and original element have good optical properties. The single-focus behavior was investigated by a microscopic imaging system and found to be in good agreement with theoretical simulation results. The innovative optical component is expected to be widely used in optical communication, quantum computation, optical manipulation, and other fields.

Air-Stable Porous Fe2N Encapsulated in Carbon Microboxes with High Volumetric Lithium Storage Capacity and a Long Cycle Life.

The development of inexpensive electrode materials with a high volumetric capacity and long cycle-life is a central issue for large-scale lithium-ion batteries. Here, we report a nanostructured porous Fe2N anode fully encapsulated in carbon microboxes (Fe2N@C) prepared through a facile confined anion conversion from polymer coated Fe2O3 microcubes. The resulting carbon microboxes could not only protect the air-sensitive Fe2N from oxidation but also retain thin and stable SEI layer. The appropriate internal voids in the Fe2N cubes help to release the volume expansion during lithiation/delithiation processes, and Fe2N is kept inside the carbon microboxes without breaking the shell, resulting in a very low electrode volume expansion (the electrode thickness variation upon lithiation is ∼9%). Therefore, the Fe2N@C electrodes maintain high volumetric capacity (1030 mA h cm-3 based on the lithiation-state electrode volume) comparable to silicon anodes, stable cycling performance (a capacity retention of over 91% for 2500 cycles), and excellent rate performance. Kinetic analysis reveals that the Fe2N@C shows an enhanced contribution of capacitive charge mechanism and displays typical pseudocapacitive behavior. This work provides a new direction on designing and constructing nanostructured electrodes and protective layer for air unstable conversion materials for potential applications as a lithium-ion battery/capacitor electrode.

Single-mode unidirectional microcavity laser.

In this Letter, we report a suspended whispering gallery mode microdisk with a hole pierced through its surface. The novel disk is made up of Rhodamine B-doped resin, which is fabricated by femtosecond laser direct writing technology. The pierced microcavity achieves highly directional emission of single-mode lasing with a far field divergence angle of about 10 deg, and its high Q factor exceeds 2.6×103. The excellent properties are confirmed by numerical simulation based on the finite-difference time-domain method. The effect of the pierced hole on the microcavity performance is discussed in detail. The method is easy to implement and has a guiding significance for improving the characteristics of an existing microcavity by simple modification.

Multilevel phase-type diffractive lens embedded in sapphire.

Herein, we report a kinoform phase-type lens (KPL), which is fabricated by femtosecond (fs)-laser-induced refractive index change inside sapphire crystal. By fabricating volume phase gratings in sapphire and measuring the energy ratio of the grating's first and second diffraction orders, the refractive index change in sapphire induced by fs-laser modification was obtained. Then a four-level KPL was designed and fabricated inside sapphire following the experimentally established scaling of the refractive index change and fs-laser power. Importantly, the KPL has unique UV focusing and imaging capability as well as a stable optical performance in different refractive index environments. The KPL embedded in sapphire has the same optical performance after a high-temperature (1050°C) annealing for 30 min. The KPLs in sapphire have great potential to increase light extraction efficiency in GaN blue-UV light-emitting diodes and can be used in micro-optical sensor applications in chemically harsh and high-temperature environments.

Fabrication of an anti-reflective microstructure on sapphire by femtosecond laser direct writing.

Herein, we report a facile approach for the maskless production of subwavelength-structured antireflective surfaces on sapphire with high and broadband transmittance in the mid-IR: femtosecond laser direct writing assist with wet etching. With this method, inverted pyramid and cone arrays with a pitch of about 2 µm and a total height of near 900 nm on the sapphire were produced. The resulting subwavelength structures greatly suppress specular reflection at normal incidence. The transmission measurements between 3 and 5 µm are in agreement with the simulations performed using VirtualLab, and the transmittance reached a maximum value of 92.5% at 4 µm. The sapphire with subwavelength structures also exhibits angle-independent transmittance characteristics up to a high θ=60°. Therefore, these subwavelength structures on sapphire are of great technological importance in mid-IR optics, especially for the harsh-condition-applicable windows of military mid-IR devices.

Mesoporous Piezoelectric Polymer Composite Films with Tunable Mechanical Modulus for Harvesting Energy from Liquid Pressure Fluctuation.

Harvesting mechanical energy from biological systems possesses great potential for in vivo powering implantable electronic devices. In this paper, a development of flexible piezoelectric nanogenerator (NG) is reported based on mesoporous poly(vinylidene fluoride) (PVDF) films. Monolithic mesoporous PVDF is fabricated by a template-free sol-gel-based approach at room temperature. By filling the pores of PVDF network with poly(dimethylsiloxane) (PDMS) elastomer, the composite's modulus is effectively tuned over a wide range down to the same level of biological systems. A close match of the modulus between NG and the surrounding biological component is critical to achieve practical integration. Upon deformation, the composite NG exhibits appreciable piezoelectric output that is comparable to or higher than other PVDF-based NGs. An artificial artery system is fabricated using PDMS with the composite NG integrated inside. Effective energy harvesting from liquid pressure fluctuation (simulating blood pressure fluctuation) is successfully demonstrated. The simple and effective approach for fabricating mesoporous PVDF with tunable mechanical properties provides a promising route toward the development of self-powered implantable devices.

Ferroelectric Polarization-Enhanced Photoelectrochemical Water Splitting in TiO2-BaTiO3 Core-Shell Nanowire Photoanodes.

The performances of heterojunction-based electronic devices are extremely sensitive to the interfacial electronic band structure. Here we report a largely enhanced performance of photoelectrochemical (PEC) photoanodes by ferroelectric polarization-endowed band engineering on the basis of TiO2/BaTiO3 core/shell nanowires (NWs). Through a one-step hydrothermal process, a uniform, epitaxial, and spontaneously poled barium titanate (BTO) layer was created on single crystalline TiO2 NWs. Compared to pristine TiO2 NWs, the 5 nm BTO-coated TiO2 NWs achieved 67% photocurrent density enhancement. By numerically calculating the potential distribution across the TiO2/BTO/electrolyte heterojunction and systematically investigating the light absorption, charge injection and separation properties of TiO2 and TiO2/BTO NWs, the PEC performance gain was proved to be a result of the increased charge separation efficiency induced by the ferroelectric polarization of the BTO shell. The ferroelectric polarization could be switched by external electric field poling and yielded PEC performance gain or loss based on the direction of the polarization. This study evidence that the piezotronic effect (ferroelectric or piezoelectric potential-induced band structure engineering) holds great promises in improving the performance of PEC photoelectrodes in addition to chemistry and structure optimization.

Focal varying microlens array.

We report a novel microlens array with different curvature unit lenses (MLADC) fabricated with femtosecond laser direct writing technology. The MLADC consisted of hexagonal hyperboloid unit microlenses, which have different heights and curvatures from others. The unique optical performance of imaging and focusing capability were demonstrated. An object was imaged at different positions from the MLADC by unit lenses, as the ability of adjusting the curvature of the image plane for overall MLADC. In addition, the experiment had a good agreement with simulation results, which was based on the analysis of the finite element method. The novel MLADC will have important applications in improving the performance of optical systems, especially in field curvature correction and real-time three-dimensional imaging.

Evolution of hollow TiO2 nanostructures via the Kirkendall effect driven by cation exchange with enhanced photoelectrochemical performance.

Hollow nanostructures are promising building blocks for electrode scaffolds and catalyst carriers in energy-related systems. In this paper, we report a discovery of hollow TiO2 nanostructure evolution in a vapor-solid deposition system. By introducing TiCl4 vapor pulses to ZnO nanowire templates, we obtained TiO2 tubular nanostructures with well-preserved dimensions and morphology. This process involved the cation exchange reaction between TiCl4 vapor and ZnO solid and the diffusion of reactants and products in their vapor or solid phases, which was likely a manifestation of the Kirkendall effect. The characteristic morphologies and the evolution phenomena of the hollow nanostructures from this vapor-solid system were in a good agreement with the Kirkendall effect discovered in solution systems. Complex hollow TiO2 nanostructures were successfully acquired by replicating various ZnO nanomorphologies, suggesting that this unique cation exchange process could also be a versatile tool for nanostructure replication in vapor-solid growth systems. The evolution of TiO2 nanotubes from ZnO NW scaffolds was seamlessly integrated with TiO2 NR branch growth and thus realized a pure TiO2-phased 3D NW architecture. Because of the significantly enlarged surface area and the trace amount of Zn left in the TiO2 crystals, such 3D TiO2 nanoforests demonstrated enhanced photoelectrochemical performance particularly under AM (air mass) 1.5G illumination, offering a new route for hierarchical functional nanomaterial assembly and application.

Stretchable Electrodes with Interfacial Percolation Network.

Stretchable electrodes are an essential component that determines the functionality and reliability of stretchable electronics, but face the challenge of balancing conductivity and stretchability. This work proposes a new conducting concept called the interfacial percolation network (PN) that results in stretchable electrodes with high conductivity, large stretchability, and high stability. The interfacial PN is composed of a 2D silver nanowires (AgNWs) PN and a protruding 3D AgNWs PN embedded on the surface and in the near-surface region of an elastic polymer matrix, respectively. The protruded PN is obtained by changing the arrangements of AgNWs from horizontal to quasi-vertical through introducing foreign polymer domains in the near-surface region of the polymer matrix. The resulting electrode achieves a conductivity of 13 500 S cm-1 and a stretchability of 660%. Its resistance changes under stretched conditions are orders of magnitude lower than those of conventional 2D PN and 2D + 3D PN. An interfacial PN electrode made from liquid metal remained its conductivity at 46 750 S cm-1 after the electrode underwent multiple stretch-release cycles with a deformation of >600%. The concept of interfacial PN provides fruitful implications for the design of stretchable electronics.