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The need for precise manipulation of nanoparticles in gaseous or near-vacuum environments is encountered in many studies that include aerosol morphology, nanodroplet physics, nanoscale optomechanics, and biomolecular physics. Photophoretic forces, whereby momentum exchange between a particle and surrounding gas is induced with optical light, were recently shown to be a robust means of trapping and manipulating nanoparticles in air. We previously proposed a photophoretic "optical funnel" concept for the delivery of bioparticles to the focus of an x-ray free-electron laser (XFEL) beam for femtosecond x-ray diffractive imaging. Here, we describe the formation of a high-aspect-ratio optical funnel and provide a first experimental demonstration of this concept by transversely compressing and concentrating a high-speed beam of aerosolized viruses by a factor of three in a low-pressure environment. These results pave the way toward improved sample delivery efficiency for XFEL imaging experiments as well as other forms of imaging and spectroscopy.

We put forward a co-axial pump(optical)-probe(X-rays) experimental concept and show performance of the optical component. A Bessel beam generator with a central 100 micrometers-diameter hole (on the optical axis) was fabricated using femtosecond (fs) laser structuring inside a silica plate. This flat-axicon optical element produces a needle-like axial intensity distribution which can be used for the optical pump pulse. The fs-X-ray free electron laser (X-FEL) beam of sub-1 micrometer diameter can be introduced through the central hole along the optical axis onto a target as a probe. Different realisations of optical pump are discussed. Such optical elements facilitate alignment of ultra-short fs-pulses in space and time and can be used in light-matter interaction experiments at extreme energy densities on the surface and in the volume of targets. Full advantage of ultra-short 10 fs X-FEL probe pulses with fs-pump(optical) opens an unexplored temporal dimension of phase transitions and the fastest laser-induced rates of material heating and quenching. A wider field of applications of fs-laser-enabled structuring of materials and design of specific optical elements for astrophotonics is presented.

Confined microexplosions induced in silicon by powerful ultrashort laser pulses can lead to new Si phases. Some of these have not previously been observed via near-equilibrium compression of silicon. In this study, confocal Raman micro-spectroscopy and Raman imaging of arrays of microexplosions have been conducted to search for Raman signatures of these novel allotropes of silicon. A microexplosion is generated at the interface between a thick silicon dioxide confinement layer and underlying silicon. It is characterised by a void at the interface above a region of compressed silicon. Raman data show a rich assembly of silicon phases within the modified silicon. Residual stresses up to 4.5 GPa in the modifications have been determined from the shift in the main diamond-cubic Si Raman peak. The computed Raman spectra for a number of Si allotropes show reasonable agreement with the experimental spectra. Two structurally similar tetragonal phases of silicon (the rhombohedral r8 and the body-centred bc8) phases as well as recently identified bt8-Si are all highly likely to be contained in Raman spectra from many laser-modified sites. Although the st12-Si phase, previously observed in our electron diffraction studies of the highly compressively stressed laser-modified regions, was not reliably identified from Raman data, we suggest this could be due to the possible difference in residual stress level in the sites analysed by the electron diffraction and Raman spectra. Several other unidentified Raman peaks were observed, suggesting the presence of other unknown silicon phases. All of these silicon phases are expected to have attractive semiconducting properties including narrow band gap that open up novel applications., Comment: 18 pages, 6 figures

The emergence of high repetition-rate X-ray free-electron lasers (XFELs) powered by superconducting accelerator technology enables the measurement of significantly more experimental data per day than was previously possible. The European XFEL will soon provide 27,000 pulses per second, more than two orders of magnitude more than any other XFEL. The increased pulse rate is a key enabling factor for single-particle X-ray diffractive imaging, which relies on averaging the weak diffraction signal from single biological particles. Taking full advantage of this new capability requires that all experimental steps, from sample preparation and delivery to the acquisition of diffraction patterns, are compatible with the increased pulse repetition rate. Here, we show that single-particle imaging can be performed using X-ray pulses at megahertz repetition rates. The obtained results pave the way towards exploiting high repetition-rate X-ray free-electron lasers for single-particle imaging at their full repetition rate.

It was demonstrated during the past decade that ultrashort intense laser pulse tightly focused deep inside a transparent dielectric generates the energy density in excess of several MJ/cm3. Such energy concentration with extremely high heating and quenching rates leads to unusual solid-plasma-solid transformation paths overcoming kinetic barriers to formation of previously unknown high-pressure material phases, which are preserved in the surrounding pristine crystal. These results were obtained with the pulse of Gaussian shape in space and in time. Recently it was shown that the Bessel-shaped pulse could transform much larger amount of a material and allegedly create even higher energy density than that was achieved with the Gaussian (GB) pulses. Here we present a succinct review of previous results and discuss the possible routes for achieving higher energy density employing the Bessel beams (BB) and take advantage of its unique properties., Comment: 6 pages

It has been proven that the intense tightly focused Gauss beam (GB) generates pressures in excess of a few TPa creating the novel super-dense phases of Aluminium and silicon [1-5]. Recently it was demonstrated that the Bessel beam (BB) focused inside sapphire produced the cylindrical void being two orders of magnitude larger than that generated by the GB [6-8]. Analysis of the experimental data presented below allows making the remarkable conclusions based solely on the void size measurements without any ad hoc assumptions about the interaction process. First, the void size is direct evidence of strong (>40%) absorption of the pulse energy. Second, it is a direct experimental evidence of the high-energy concentration in the central spike of the focus. The unique features of the intense Bessel beam interaction then allow understanding the experimental observation. This interaction generates early in the pulse time the spatial distribution of excited permittivity changing from positive to negative values. Then the light interacts with zero-real-permittivity surface, separating plasma and dielectric areas, which leads to high energy concentration near the axis of cylindrical focus up to several MJ/cm3 (pressure range of 4-8 TPa). The effect depends on the angle between the permittivity gradient and the field polarisation. High pressure generates intense cylindrical shock/ rarefaction waves, which led to formation of void and compressed shell. We demonstrate that the Bessel beam proves to be an effective tool for producing extreme pressure/temperature conditions on the laboratory tabletop. It appears that adjusting polarisation and permittivity gradient might be a novel way for increasing the maximum pressure. This tool allows for search of novel high-pressure material phases, for the 3D laser machining and for creating Warm Dense Matter as those in star cores., Comment: Draft-01, 18 pages, 4 figures, presented at International Conference on Laser Ablation COLA-2017 in Marseille, 4-8 September 2017. The latest version has updated text and figures

The swift excitation of the transparent dielectrics by intense short laser pulse produces ultra-fast re-structuring of the electronic landscape generating a wealth of material states continuously changing in space and in time in accord with the variations of the intensity. These unconventional transient material states combine simultaneously dielectric and metal properties (Die-Met). The laser excitation transforms a transparent dielectric into electrically inhomogeneous state early in the pulse time [1]. The permittivity of excited material varies in time and in space changing from positive to negative values that strongly affects the interaction process. The interplay between the transient permittivity gradient and polarisation of the incident laser becomes the major process of the new interaction mode. In a particular relation between the polarization and the permittivity gradient the incident field amplitude grows up while the wave is approaching to the surface where the real part of permittivity turns to zero. That results in the local increase in the absorbed energy density. The complex 3D structure of the permittivity makes a transparent part of excited dielectric (at ${\epsilon}0 > {\epsilon}re > 0$) optically active. The electro-magnetic wave passing through such a medium gets a twisted trajectory and accrues the geometric phase [2]. The plane of polarisation rotation and phase depends on the 3D permittivity structure [3]. Measuring the polarisation and phase of the probe beam allows quantitatively identify this new transient state. We discuss the revelations of this effect in different experimental situations and possible applications., Comment: Draft-02; 11 pages, 6 figures; to be presented at International Conference on Laser Ablation, Marseille, 4-8 September 2017

We demonstrate near-atomic-resolution Bragg diffraction from aerosolized single granulovirus crystals using an x-ray free-electron laser. The form of the aerosol injector is nearly identical to conventional liquid-microjet nozzles, but the x-ray-scattering background is reduced by several orders of magnitude by the use of helium carrier gas rather than liquid. This approach provides a route to study the weak diffuse or lattice-transform signal arising from small crystals. The high speed of the particles is particularly well suited to upcoming MHz-repetition-rate x-ray free-electron lasers.

Delivering sub-micrometer particles to an intense x-ray focus is a crucial aspect of single-particle diffractive-imaging experiments at x-ray free-electron lasers. Enabling direct visualization of sub-micrometer aerosol particle streams without interfering with the operation of the particle injector can greatly improve the overall efficiency of single-particle imaging experiments by reducing the amount of time and sample consumed during measurements. We have developed in-situ non-destructive imaging diagnostics to aid real-time particle injector optimization and x-ray/particle-beam alignment, based on laser illumination schemes and fast imaging detectors. Our diagnostics are constructed to provide a non-invasive rapid feedback on injector performance during measurements, and have been demonstrated during diffraction measurements at the FLASH free-electron laser., Comment: 15 pages

Photoluminescence (PL) from femtosecond laser modified regions inside cubic-boron nitride (c-BN) was measured under UV and visible light excitation. Bright PL at the red spectral range was observed, with a typical excited state lifetime of $\sim 4$~ns. Sharp emission lines are consistent with PL of intrinsic vibronic defects linked to the nitrogen vacancy formation (via Frenkel pair) observed earlier in high energy electron irradiated and ion-implanted c-BN. These, formerly known as the radiation centers, RC1, RC2, and RC3 have been identified at the locus of the voids formed by single fs-laser pulse. The method is promising to engineer color centers in c-BN for photonic applications., Comment: 4 figures

This letter is the first demonstration of material modification using tightly focused femtosecond laser vortex beams. Double-charge femtosecond vortices were synthesized with the polarization-singularity beam converter described in Ref [1] and then focused using moderate and high numerical aperture optics (viz., NA = 0.45 and 0.9) to ablate fused silica and soda-lime glasses. By controlling the pulse energy we consistently machine high-quality micron-size ring-shaped structures with less than 100 nm uniform groove thickness., Comment: 8 pages, 3 figures, 10 references; submitted to Appl. Phys. Lett. on May 31, 2010

This letter is the first demonstration of material modification using tightly focused femtosecond laser vortex beams. Double-charge femtosecond vortices were synthesized with the polarization-singularity beam converter described in Ref [1] and then focused using moderate and high numerical aperture optics (viz., NA = 0.45 and 0.9) to ablate fused silica and soda-lime glasses. By controlling the pulse energy we consistently machine high-quality micron-size ring-shaped structures with less than 100 nm uniform groove thickness., Comment: 8 pages, 3 figures, 10 references; submitted to Apl. Phys. Lett. 31 May 2010

We describe an optical beam converter for an efficient transformation of Gaussian femtosecond laser beams to single- or double-charge vortex beams showing no spatial or topological charge dispersion. The device achieves a conversion efficiency of 75% for single- and 50% for double-charge vortex beams and can operate with high energy broad bandwidth pulses. We also show that the topological charge of a femtosecond vortex beam can be determined by analyzing its intensity distribution in the focal area of a cylindrical lens., Comment: 9 pages, 4 figures, submitted to Optics Letters 10 March 2010

Transient state of femtosecond laser excited bismuth has been studied by various groups with time-resolved optical, x-ray, and electron probes at the deposited energy density from below through up to several times the equilibrium enthalpy of melting. However, the interpretations of the experimental results are controversial: the optical probes reveal the absence of transition to the melting phase while the authors of x-ray and electron diffraction experiments claim the observation of ultrafast non-thermal melting. The presented analysis, based on temperature dependence of bismuth optical properties, unequivocally shows a purely thermal nature of all the observed fs-laser induced transformations in bismuth., Comment: 20 pages, 6 figures, to be presented at the Conference on Laser Ablation COLA'2009, Singapore, 21-26 November 2009

We introduce a novel approach for all-optical trapping and manipulation of absorbing aerosol particles based on a photophoretic force. We demonstrate experimentally, in open air, the robust three-dimensional guiding of agglomerates of carbon nanoparticles with the size spanned for two orders of magnitude, from 100 nanometers to 10 microns, over the distances of a few millimeters, as well as their acceleration up to velocities of 1 cm/s and simultaneous trapping of a large number of particles., Comment: 12 pages including 8 figures. First presented at SPIE Conference 7038 on Optical Trapping and Optical Micromanipulation V, San Diego, USA, 13 August 2008, paper 7038-69