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Register a new userPotential of attosecond coherent diffractive imaging
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Attosecond science has been transforming our understanding of electron dynamics in atoms, molecules and solids. However, to date almost all of the attoscience experiments have been based on spectroscopic measurements because attosecond pulses have intrinsically very broad spectra due to the uncertainty principle and are incompatible with conventional imaging systems. Here we report an important advance towards achieving attosecond coherent diffractive imaging. Using simulated attosecond pulses, we simultaneously reconstruct the spectrum, 17 probes and 17 spectral images of extended objects from a set of ptychographic diffraction patterns. We further confirm the principle and feasibility of this method by successfully performing a ptychographic coherent diffractive imaging experiment using a light-emitting diode with a broad spectrum. We believe this work clear the way to an unexplored domain of attosecond imaging science, which could have a far-reaching impact across different disciplines.
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Attosecond science promises to reveal the most fundamental electronic dynamics occurring in matter and it can develop further by meeting two linked technological goals related to high-order harmonic sources: higher photon flux (permitting to measure low cross-section processes) and improved spectral tunability (allowing selectivity in addressing specific electronic transitions). New developments come through parametric waveform synthesis, which provides control over the shape of high-energy electric field transients, enabling the creation of highly-tunable isolated attosecond pulses via high-harmonic generation. Here we show that central energy, spectral bandwidth/shape and temporal duration of the attosecond pulses can be controlled by shaping the laser pulse waveform via two key parameters: the relative-phase between two halves of the multi-octave spanning optical spectrum, and the overall carrier-envelope phase. These results not only promise to expand the experimental possibilities in attosecond science, but also demonstrate coherent strong-field control of free-electron trajectories using tailored optical waveforms.
The inversion of a diffraction pattern offers aberration-free diffraction-limited 3D images without the resolution and depth-of-field limitations of lens-based tomographic systems, the only limitation being radiation damage. We review our experimental results, discuss the fundamental limits of this technique and future plans.
We present the experimental reconstruction of sub-wavelength features from the far-field intensity of sparse optical objects: sparsity-based sub-wavelength imaging combined with phase-retrieval. As examples, we demonstrate the recovery of random and ordered arrangements of 100 nm features with the resolution of 30 nm, with an illuminating wavelength of 532 nm. Our algorithmic technique relies on minimizing the number of degrees of freedom; it works in real-time, requires no scanning, and can be implemented in all existing microscopes - optical and non-optical.
Coherent diffractive imaging (CDI) has been widely applied in the physical and biological sciences using synchrotron radiation, XFELs, high harmonic generation, electrons and optical lasers. One of CDIs important applications is to probe dynamic phenomena with high spatio-temporal resolution. Here, we report the development of a general in situ CDI method for real-time imaging of dynamic processes in solution. By introducing a time-invariant overlapping region as a real-space constraint, we show that in situ CDI can simultaneously reconstruct a time series of the complex exit wave of dynamic processes with robust and fast convergence. We validate this method using numerical simulations with coherent X-rays and performing experiments on a materials science and a biological specimen in solution with an optical laser. Our numerical simulations further indicate that in situ CDI can potentially reduce the radiation dose by more than an order of magnitude relative to conventional CDI. As coherent X-rays are under rapid development worldwide, we expect in situ CDI could be applied to probe dynamic phenomena ranging from electrochemistry, structural phase transitions, charge transfer, transport, crystal nucleation, melting and fluid dynamics to biological imaging.
Characterizing buried layers and interfaces is critical for a host of applications in nanoscience and nano-manufacturing. Here we demonstrate non-invasive, non-destructive imaging of buried interfaces using a tabletop, extreme ultraviolet (EUV), coherent diffractive imaging (CDI) nanoscope. Copper nanostructures inlaid in SiO2 are coated with 100 nm of aluminum, which is opaque to visible light and thick enough that neither optical microscopy nor atomic force microscopy can image the buried interfaces. Short wavelength (29 nm) high harmonic light can penetrate the aluminum layer, yielding high-contrast images of the buried structures. Moreover, differences in the absolute reflectivity of the interfaces before and after coating reveal the formation of interstitial diffusion and oxidation layers at the Al-Cu and Al-SiO2 boundaries. Finally, we show that EUV CDI provides a unique capability for quantitative, chemically-specific imaging of buried structures, and the material evolution that occurs at these buried interfaces, compared with all other approaches.
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