Coherent x-ray diffraction imaging with nanofocused illumination

Coherent x-ray diffraction imaging is an x-ray microscopy technique with the potential of reaching spatial resolutions well beyond the diffraction limits of x-ray microscopes based on optics. However, the available coherent dose at modern x-ray sources is limited, setting practical bounds on the spatial resolution of the technique. By focusing the available coherent flux onto the sample, the spatial resolution can be improved for radiation-hard specimens. A small gold particle (size <100 nm) was illuminated with a hard x-ray nanobeam (E=15.25 keV, beam dimensions approximately 100 x 100 nm2) and is reconstructed from its coherent diffraction pattern. A resolution of about 5 nm is achieved in 600 s exposure time.     

Three-dimensional GaN-Ga2O3 core shell structure revealed by x-ray diffraction microscopy

In combination of direct phase retrieval of coherent x-ray diffraction patterns with a novel tomographic reconstruction algorithm, we, for the first time, carried out quantitative 3D imaging of a heat-treated GaN particle with each voxel corresponding to 17 x 17 x 17 nm3. We observed the platelet structure of GaN and the formation of small islands on the surface of the platelets, and successfully captured the internal GaN-Ga2O3 core shell structure in three dimensions. This work opens the door for nondestructive and quantitative imaging of 3D morphology and 3D internal structure of a wide range of materials at the nanometer scale resolution that are amorphous or possess only short-range atomic organization.     

Single-pulse coherent diffraction imaging using soft x-ray laser

We report a coherent diffraction imaging (CDI) using a single 8 ps soft x-ray laser pulse at a wavelength of 13.9 nm. The soft x-ray pulse was generated by a laboratory-scale intense pumping laser providing coherent x-ray pulses up to the level of 10(11) photons/pulse. A spatial resolution below 194 nm was achieved with a single pulse, and it was shown that a resolution below 55 nm is feasible with improved detector capability. The single-pulse CDI might provide a way to investigate dynamics of nanoscale molecules or particles.     

Nanoscale imaging of buried structures with elemental specificity using resonant x-ray diffraction microscopy

We report the first demonstration of resonant x-ray diffraction microscopy for element specific imaging of buried structures with a pixel resolution of approximately 15 nm by exploiting the abrupt change in the scattering cross section near electronic resonances. We performed nondestructive and quantitative imaging of buried Bi structures inside a Si crystal by directly phasing coherent x-ray diffraction patterns acquired below and above the Bi M5 edge. We anticipate that resonant x-ray diffraction microscopy will be applied to element and chemical state specific imaging of a broad range of systems including magnetic materials, semiconductors, organic materials, biominerals, and biological specimens.     

Hard X ray holographic diffraction imaging

We determine the absolute electron density of a lithographically grown nanostructure with 25 nm resolution by combining hard x-ray Fourier transform holography with iterative phase retrieval methods. While holography immediately reveals an unambiguous image of the object, we deploy in addition iterative phase retrieval algorithms for pushing the resolution close to the diffraction limit. The use of hard (8 keV) x rays eliminates practically all constraints on sample environment and enables a destruction-free investigation of relatively thick or buried samples, making holographic diffraction imaging a very attractive tool for materials science. We note that the technique is ideally suited for subpicosecond imaging that will become possible with the emerging hard x-ray free-electron lasers.     

One-dimensional Wolter optics with a sub-50 nm spatial resolution

We studied an imaging system consisting of an elliptical mirror and a hyperbolic mirror [i.e., one-dimensional (1D) Wolter optics] to realize an achromatic full-field hard x-ray microscopy with a resolution better than 50 nm. We report the performance of this 1D Wolter optical system when the mirrors were ultraprecisely figured by elastic emission machining. Experiments to form a demagnified image (demagnification factor of 385) of a 10 μm slit were conducted at an x-ray energy of 11.5 keV at BL29XUL of SPring-8. The system could form a demagnified image with a resolution better than 50 nm over a 12.1 μm field.     

X-ray diffraction microscopy of magnetic structures

We report the first proof-of-principle experiment of iterative phase retrieval from magnetic x-ray diffraction. By using the resonant x-ray excitation process and coherent x-ray scattering, we show that linearly polarized soft x rays can be used to image both the amplitude and the phase of magnetic domain structures. We recovered the magnetic structure of an amorphous terbium-cobalt thin film with a spatial resolution of about 75 nm at the Co L3 edge at 778 eV. In comparison with soft x-ray microscopy images recorded with Fresnel zone plate optics at better than 25 nm spatial resolution, we find qualitative agreement in the observed magnetic structure.     

Lensless diffractive imaging using tabletop coherent high-harmonic soft-X-ray beams

We present the first experimental demonstration of lensless diffractive imaging using coherent soft x rays generated by a tabletop soft-x-ray source. A 29 nm high harmonic beam illuminates an object, and the subsequent diffraction is collected on an x-ray CCD camera. High dynamic range diffraction patterns are obtained by taking multiple exposures while blocking small-angle diffraction using beam blocks of varying size. These patterns reconstruct to images with 214 nm resolution. This work demonstrates a practical tabletop lensless microscope that promises to find applications in materials science, nanoscience, and biology.     

Three‐dimensional coherent diffractive imaging on non‐periodic specimens at the ESRF beamline ID10

The progress of tomographic coherent diffractive imaging with hard X‐rays at the ID10 beamline of the European Synchrotron Radiation Facility is presented. The performance of the instrument is demonstrated by imaging a cluster of Fe₂P magnetic nanorods at 59 nm 3D resolution by phasing a diffraction volume measured at 8 keV photon energy. The result obtained shows progress in three‐dimensional imaging of non‐crystalline samples in air with hard X‐rays.     

Nanoscale imaging of mineral crystals inside biological composite materials using X-ray diffraction microscopy

We for the first time applied x-ray diffraction microscopy to the imaging of mineral crystals inside biological composite materials--intramuscular fish bone--at the nanometer scale resolution. We identified mineral crystals in collagen fibrils at different stages of mineralization. Based on the experimental results and biomineralization analyses, we suggested a dynamic model to account for the nucleation and growth of mineral crystals in the collagen matrix. The results obtained from this study not only further our understanding of the complex structure of bone, but also demonstrate that x-ray diffraction microscopy will become an important tool to study biological materials.     

Breaking the diffraction barrier in fluorescence microscopy by optical shelving

We report the breaking of the diffraction resolution barrier in far-field fluorescence microscopy by transiently shelving the fluorophore in a metastable dark state. Using a relatively modest light intensity of several kW/cm(2) in a focal distribution featuring a local zero, we confine the fluorescence emission to a spot whose diameter is a fraction of the wavelength of light. Nanoscale far-field optical resolution down to 50 nm is demonstrated by imaging microtubules in a mammalian cell and proteins on the plasma membrane of a neuron. The presence of dark states in virtually any fluorescent molecule opens up a new venue for far-field microscopy with resolution that is no longer limited by diffraction.     

Nanoscale imaging with resonant coherent X rays: extension of multiple-wavelength anomalous diffraction to nonperiodic structures

The methodology of multiple-wavelength anomalous diffraction, widely used for macromolecular structure determination, is extended to the imaging of nonperiodic nanostructures. We demonstrate the solution of the phase problem by a combination of two resonantly recorded coherent scattering patterns at the carbon K edge (285 eV). Our approach merges iterative phase retrieval and x-ray holography approaches, yielding unique and rapid reconstructions. The element, chemical, and magnetic state specificity of our method further renders it widely applicable to a broad range of nanostructures, providing a spatial resolution that is limited, in principle, by wavelength only.     

Atomic resolution three-dimensional electron diffraction microscopy

We report the development of a novel form of diffraction-based 3D microscopy to overcome resolution barriers inherent in high-resolution electron microscopy and tomography. By combining coherent electron diffraction with the oversampling phasing method, we show that the 3D structure of a nanocrystal can be determined ab initio at a resolution of 1 A from 29 simulated noisy diffraction patterns. This new form of microscopy can be used to image the 3D structures of nanocrystals and noncrystalline samples, with resolution limited only by the quality of sample diffraction.     

Fresnel coherent diffractive imaging

We present an x-ray coherent diffractive imaging experiment utilizing a nonplanar incident wave and demonstrate success by reconstructing a nonperiodic gold sample at 24 nm resolution. Favorable effects of the curved beam illumination are identified.     

远场超分辨随机光重建显微镜(STORM)研究进展

了解细胞内分子尺度的动态和结构的特征是生命科学迫切需要解决的问题,要求远场光学成像要求纳米或亚纳米量级的空间分辨率.介绍了一种实现打破衍射极限的远场荧光显微成像技术--随机光重建显微术(STORM),其分辨率可以达到横向分辨率20 nm,轴向分辨率50 nm,理论上这种方法的空间分辨率可以达到单分子定位的精度.具体介绍...     

相干X射线衍射成像三维重建的数字模拟研究

利用相干X射线衍射成像“过采样”采集样品的远场相干衍射图样, 结合相位重建迭代算法重建物空间样品信息. 三维重建过程中, 边界约束条件是相位重建算法中最为关键的部分. 本文采用数字模拟的方法, 利用灰度值图像作为物空间的样品, 研究并实现了边界条件的自动寻找, 重建结果显示比以往采用较“松”的边界约束更为精确. 利用噪声模拟方法, 研究了衍射图样中不同噪声类型的滤除对重建结果的影响. 研究发现传统的去噪方法在高噪声情况下不能直接应用于相干X射线衍射成像, 并找到了适用于相干X射线衍射成像噪声滤除的有效方法. 研究表明, 此方法能非常有效地降低噪声对重建结果的影响. 利用模拟三维纳米金颗粒作为样品, 完成了对纳米金颗粒中电子密度分布的三维重建, 在有随机噪声的影响下, 也得到了很好的重建结果, 并找到了成功实现三维重建的噪声限为信噪比不低于27. 关键词： X射线相干衍射成像 过采样 三维相位重建 显微成像     

On influence of collimating slit imperfections on the quality of experimental data in high-resolution x-ray diffraction

High-resolution x-ray diffraction and imaging techniques commonly assume a well-defined plane wave incident on the sample. Experimentally, the wave-front is limited by a collimating slit. Slit imperfections, such as surface roughness on the edges, may significantly contribute to the formation of the diffraction pattern from a specimen placed behind the slit. These effects become more profound when imaging at the nano-scale. This Letter presents experimental and simulated x-ray diffraction data quantitatively demonstrating the influence of slit edge imperfections on the formation of the diffraction pattern in the far-field regime.     

Sodium D2 resonance radiation in single-pass sum-frequency generation with actively mode-locked Nd:YAG lasers

We report on a sodium D(2) resonance coherent light source achieved in single-pass sum-frequency generation in periodically poled MgO-doped stoichiometric lithium tantalate with actively mode-locked Nd:YAG lasers. Mode-locked pulses at 1064 and 1319 nm are synchronized with a time resolution of 37 ps with the phase adjustment of the radio frequencies fed to acousto-optic mode lockers. An output power of 4.6 W at 589.1586 nm is obtained, and beam quality near the diffraction limit is also achieved in a simple design.     

Far-field optical microscopy with a nanometer-scale resolution based on the in-plane image magnification by surface plasmon polaritons

A new far-field optical microscopy capable of reaching nanometer-scale resolution is developed using the in-plane image magnification by surface plasmon polaritons. This approach is based on the optical properties of a metal-dielectric interface that may provide extremely large values of the effective refractive index neff up to 10(3) as seen by surface polaritons, and thus the diffraction limited resolution can reach nanometer-scale values of lambda/2neff. The experimental realization of the microscope has demonstrated the optical resolution better than 60 nm at 515 nm illumination wavelength.     

Superresolution vibrational imaging by simultaneous detection of Raman and hyper-Raman scattering

We have developed a superresolution vibrational imaging method by simultaneous detection of Raman and hyper-Raman scattering. Raman and hyper-Raman images obtained with the same laser spot carry independent information on the sample spatial distribution, owing to different signal dependence (linear in Raman and quadratic in hyper-Raman) on the incident light intensity. This information can be quantitatively analyzed to recover the incident light intensity distribution at the focal plane. A superresolution vibrational image is then derived by the constrained deconvolution of the images by the obtained incident light intensity distribution. This method has been applied to a TiO? nanostructure and the obtained superresolution image was compared with a scanning electron microscopy image. The spatial resolution achieved by the present method is evaluated to be 160 nm, which is more than twice better than the diffraction limited resolution.