Self-probed ptychography from semiconductor high-harmonic generation.

We demonstrate a method to image an object using a self-probing approach based on semiconductor high-harmonic generation. On the one hand, ptychography enables high-resolution imaging from the coherent light diffracted by an object. On the other hand, high-harmonic generation from crystals is emerging as a new source of extreme-ultraviolet ultrafast coherent light. We combine these two techniques by performing ptychography measurements with nanopatterned crystals serving as the object as well as the generation medium of the harmonics. We demonstrate that this strong field in situ approach can provide structural information about an object. With the future developments of crystal high harmonics as a compact short-wavelength light source, our demonstration can be an innovative approach for nanoscale imaging of photonic and electronic devices in research and industry.

Polarization spectroscopy of high-order harmonic generation in gallium arsenide.

An interesting property of high harmonic generation in solids is its laser polarization dependent nature which in turn provides information about the crystal and band structure of the generation medium. Here we report on the linear polarization dependence of high-order harmonic generation from a gallium arsenide crystal. Interestingly, we observe a significant evolution of the anisotropic response of above bandgap harmonics as a function of the laser intensity. We attribute this change to fundamental microscopic effects of the emission process comprising a competition between intraband and interband dynamics. This intensity dependence of the anisotropic nature of the generation process offers the possibility to drive and control the electron current along preferred directions of the crystal, and could serve as a switching technique in an integrated all-solid-state petahertz optoelectronic device.

Single-shot spatial coherence characterization of x-ray ultrafast sources.

Spatial coherence is an impactful source parameter in many applications ranging from atomic and molecular physics to metrology or imaging. In lensless imaging, for example, it can strongly affect the image formation, especially when the source exhibits shot-to-shot variations. Single-shot characterization of the spatial coherence length of a source is thus crucial. However, current techniques require either parallel intensity measurements or the use of several masks. Based on the method proposed by González et al. [J. Opt. Soc. Am. A28, 1107 (2011)JOAOD60740-323210.1364/JOSAA.28.001107], we designed a specific arrangement of a two-dimensional non-redundant array of apertures, which allows, through its far field interference pattern, for a single-shot measurement of the spatial coherence, while being robust against beam-pointing instabilities. The strategic configuration of the pinholes allows us to disentangle the degree of spatial coherence from the intensity distribution, thus removing the need for parallel measurement of the beam intensity. An experimental validation is performed using a high-harmonic source. A statistical study in different regimes shows the robustness of the method.

Lensless microscopy platform for single cell and tissue visualization.

Today, 3D imaging techniques are emerging, not only as a new tool in early drug discovery but also for the development of potential therapeutics to treat disease. Particular efforts are directed towards in vivo physiology to avoid perturbing the system under study. Here, we assess non-invasive 3D lensless imaging and its impact on cell behavior and analysis. We test our concept on various bio-applications and present here the first results. The microscopy platform based on in-holography provides large fields of view images (several mm2 compared to several hundred µm2) with sub-micrometer spatial resolution. 3D image reconstructions are achieved using back propagation functions post-processing.

Author Correction: All semiconductor enhanced high-harmonic generation from a single nanostructured cone.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Generating Ultrabroadband Deep-UV Radiation and Sub-10 nm Gap by Hybrid-Morphology Gold Antennas.

We experimentally investigate the interaction between hybrid-morphology gold optical antennas and a few-cycle Ti:sapphire laser up to ablative intensities, demonstrating rich nonlinear plasmonic effects and promising applications in coherent frequency upconversion and nanofabrication technology. The two-dimensional array of hybrid antennas consists of elliptical apertures combined with bowties in its minor axis. The plasmonic resonance frequency of the bowties is red-shifted with respect to the laser central frequency and thus mainly enhances the third harmonic spectrum at long wavelengths. The gold film between two neighboring elliptical apertures forms an hourglass-shaped structure, which acts as a "plasmonic lens" and thus strongly reinforces surface currents into a small area. This enhanced surface current produces a rotating magnetic field that deeply penetrates into the substrate. At resonant frequency, the magnetic field is further intensified by the bowties. The resonant frequency of the hourglass is blueshifted with respect to the laser central frequency. Consequently, it spectacularly extends the third harmonic spectrum toward short wavelengths. The resultant third harmonic signal ranges from 230 to 300 nm, much broader than the emission from a sapphire crystal. In addition, the concentration of surface current within the neck of the hourglass antenna results in a structural modification through laser ablation, producing sub-10 nm sharp metallic gaps. Moreover, after laser illumination the optical field hotspots are imprinted around the antennas, allowing us to confirm the subwavelength enhancement of the electric near-field intensity.

All semiconductor enhanced high-harmonic generation from a single nanostructured cone.

The enhancement and control of non-linear phenomena at a nanometer scale has a wide range of applications in science and in industry. Among these phenomena, high-harmonic generation in solids is a recent focus of research to realize next generation petahertz optoelectronic devices or compact all solid state EUV sources. Here, we report on the realization of the first nanoscale high harmonic source. The strong field regime is reached by confining the electric field from a few nanojoules femtosecond laser in a single 3D semiconductor waveguide. We reveal a strong competition between enhancement of coherent harmonics and incoherent fluorescence favored by excitonic processes. However, far from the band edge, clear enhancement of the harmonic emission is reported with a robust sustainability offering a compact nanosource for applications. We illustrate the potential of our harmonic nano-device by performing a coherent diffractive imaging experiment. Ultra-compact UV/X-ray nanoprobes are foreseen to have other applications such as petahertz electronics, nano-tomography or nano-medicine.

Orbital angular momentum from semiconductor high-order harmonics.

Light beams carrying orbital angular momentum (OAM) have led to stunning applications in various fields from quantum information to microscopy. We examine OAM from the recently observed high-harmonic generation (HHG) in semiconductor crystals. HHG from solids could be a valuable approach for integrated high-flux short-wavelength coherent light sources. First, we verify the transfer and conservation of the OAM in the strong-field regime of interaction from the generation laser to the harmonics. Secondly, we create OAM beams by etching a spiral zone structure directly at the surface of a zinc oxide crystal. Such diffractive optics act on the generated harmonics and produces focused optical vortices with sub-micrometric size.

Nano-plasmonic near field phase matching of attosecond pulses.

Nano-structures excited by light can enhance locally the electric field when tuned to plasmonic resonances. This phenomenon can be used to boost non-linear processes such as harmonic generation in crystals or in gases, Raman excitation, and four wave mixing. Here we present a theoretical investigation of the near-field phase matching of attosecond pulses emitted by high-order harmonic generation (HHG) of an atom immersed in a multi-cycle femtosecond infrared laser field and a spatially inhomogeneous plasmonic field. We demonstrate that the spatial inhomogeneity factor of the plasmonic field strongly affects the electron trajectory and recombination time which can be used to control the attosecond emission. For further insight into the plasmonic field effect, we monitor the phase of each quantum path as a function of the inhomogeneity strength. Moreover, we investigate the attosecond emission as a function of near-field phase matching effects. This is achieved by calculating the coherent field superposition of attosecond pulses emitted from various intensities or field inhomogeneities. Finally, far-field and near-field phase matching effects are combined to modulate the harmonic spectral phase towards the emission of a single attosecond pulse.

Spectral-phase interferometry for direct electric-field reconstruction applied to seeded extreme-ultraviolet free-electron lasers.

We present a setup for complete characterization of femtosecond pulses generated by seeded free-electron lasers (FELs) in the extreme-ultraviolet spectral region. Two delayed and spectrally shifted replicas are produced and used for spectral phase interferometry for direct electric field reconstruction (SPIDER). We show that it can be achieved by a simple arrangement of the seed laser. Temporal shape and phase obtained in FEL simulations are well retrieved by SPIDER reconstructions, allowing to foresee the implementation of this diagnostics tool on existing and future sources. This will be a significant step towards an experimental investigation and control of FEL spectral phase.

Laser-induced ultrafast demagnetization in the presence of a nanoscale magnetic domain network.

Femtosecond magnetization phenomena have been challenging our understanding for over a decade. Most experiments have relied on infrared femtosecond lasers, limiting the spatial resolution to a few micrometres. With the advent of femtosecond X-ray sources, nanometric resolution can now be reached, which matches key length scales in femtomagnetism such as the travelling length of excited 'hot' electrons on a femtosecond timescale. Here we study laser-induced ultrafast demagnetization in [Co/Pd](30) multilayer films, which, for the first time, achieves a spatial resolution better than 100 nm by using femtosecond soft X-ray pulses. This allows us to follow the femtosecond demagnetization process in a magnetic system consisting of alternating nanometric domains of opposite magnetization. No modification of the magnetic structure is observed, but, in comparison with uniformly magnetized systems of similar composition, we find a significantly faster demagnetization time. We argue that this may be caused by direct transfer of spin angular momentum between neighbouring domains.

Isolated attosecond pulses using a detuned second-harmonic field.

Calculations are presented for the generation of an isolated attosecond pulse in a multicycle two-color strong-field regime. We show that the recollision of the electron wave packet can be confined to half an optical cycle using pulses of up to 40 fs in duration. The scheme is proven to be efficient using two intense beams, one producing a strong field at omega and the other a strong field detuned from 2omega. The slight detuning deltaomega of the second harmonic is used to break the symmetry of the electric field over many optical cycles and provides a coherent control for the formation of an isolated attosecond pulse.

Submicrometer digital in-line holographic microscopy at 32 nm with high-order harmonics.

Soft-x-ray digital in-line microscopic holography is achieved using a fully coherent high-order harmonic source emitting at 32 nm. Combination of commercial-grade soft-x-ray optics and a back-illuminated CCD detector allows a compact and versatile holographic setup. Different experimental geometries have been tested by imaging calibrated 50 nm tips and 1 microm wires. Spatial resolution of 800 nm is measured with magnifications ranging from 30 to 110 and a numerical aperture around 0.01. Finally, the potentiality of three-dimensional numerical reconstruction from a single hologram acquisition is shown experimentally.