Water Window Region Research Articles

Laser plasma imaging and spectroscopy to enhance radiance for water window source development

Laser produced plasmas (LPPs) offer a compact and affordable route to soft X-ray (SXR) illumination of biological samples for microscopy in the water window (WW), the spectral region between 2.34 and 4.38 nm. The radiance of an LPP source scales with laser repetition rate and individual plasma radiance. The latter is optimised by maximizing conversion efficiency from laser light to SXR radiation while also reducing the emission area of the plasma. This is the first detailed study reporting plasma emission area and its contribution to radiance improvement for a range of solid metal target materials. Based on a 6 ns 1064 nm laser, radiance across the water window region is optimised by illuminating a molybdenum target with 38 mJ to 77 mJ of laser energy, creating a plasma emission area of 65μm2 to 115μm2. An estimate of the absolute radiance is provided for comparison with bending magnets at synchrotrons.

Observation of water-window soft x-ray emission from laser-produced Au plasma under optically thin condition

We present a systematic approach how to characterize the dynamics of a laser-produced Au plasma, generated with a commercial Joule-class laser system. By means of our diagnostic methods, we identify the dominant ionic species within the water-window spectral region, as well as the radiated energy, the x-ray emission duration and the total dimensions of the x-ray source. We present additional analysis through radiation hydrodynamic simulations to provide details about the electron temperature and density profiles and further show that the plasma exhibits nearly 20% self-absorption, while the electron temperature is limited to 400 eV. A comparison with the experimental data further allows us to verify the applied numerical code.

High efficiency ultrafast water-window harmonic generation for single-shot soft X-ray spectroscopy

Fully coherent, soft X-ray attosecond pulses are now available through high-order harmonic generation (HHG); however, the output energy is insufficient for various applications, such as attosecond-scale soft X-ray nonlinear experiments, the seeding of soft X-ray free-electron lasers, attosecond-pump-attosecond-probe spectroscopies, and single-shot imaging. In this paper, we combine a newly developed TW class mid-infrared femtosecond laser and a loose focusing geometry for HHG. A soft X-ray harmonic beam up to the water window region is demonstrated, which is more than 100 times intense compared to previous works. We achieve a high conversion efficiency, low beam divergence and a significantly reduced medium gas pressure. As the first application, we demonstrate near edge X-ray absorption fine structure experiments with clear fine absorption spectra near the K- and L-edges observed. The robust energy scaling method on HHG opens the door for demonstrating single-shot absorption spectrum and live-cell imaging with a femtosecond time resolution.

Metrology of Time-Domain Soft X-Ray Attosecond Pulses and Reevaluation of Pulse Durations of Three Recent Experiments

Attosecond pulses in the soft-X-ray (SXR) to water-window energy region offer the tools for creating and studying target specific localized inner-shell electrons or holes in materials, enable monitoring or controlling charge and energy flows in a dynamic system on attosecond timescales. Recently, a number of laboratories have reported generation of continuum harmonics in the hundred-electron-volt to kilovolt region with few-cycle long-wavelength mid-infrared lasers. These harmonics have the bandwidth to support pulses with duration of few- to few-ten attoseconds. But harmonics generated in a gas medium have attochirps that cannot be fully compensated by materials over a broad spectral range; thus, realistically what are the typical shortest attosecond pulses that one can generate? To answer this question, it is essential that the temporal attosecond pulses be accurately characterized. By re-analyzing the soft X-ray harmonics reported in three recent experiments \cite{chang_natcom2017,Thomas_OE2017,Bieger_2017PRX} using a newly developed broadband phase retrieval algorithm, we show that their generated attosecond pulses are all longer than about 60 as. Since broadband pulses tend to have high-order chirps away from the spectral center of the pulse, the algorithm has to be able to retrieve accurately the phase over the whole bandwidth. Our re-evaluated pulse durations are found to be longer than those previously reported. We also introduce the autocorrelation (AC) of the streaking spectrogram. By comparing the ACs from the experiments and from the retrieved SXR pulses, the accuracy of the retrieved results can be directly visualized to ensure that correct phases have been obtained. Our retrieval method is fast and accurate, and it shall provide a powerful tool for the metrology of few-ten-attosecond pulses in the future.

Effect of fast electrons on emission properties of non-equilibrium nitrogen plasma in soft x-ray spectral range

Soft x-ray emission at 2.3–4.4 nm waveband in nitrogen plasma can be observed mostly from 2p-1s and 3p-1s resonant transitions. Ions of nitrogen in plasma emitting in necessary band have a high energy excited state in comparison with plasma temperature in experiments. Discharge and laser produced plasmas used in radiation sources often have non-equilibrium electron distributions with fast electrons. In this study the radiative properties of non-equilibrium nitrogen plasma with fast electrons are examined and the plasma conditions for optimal soft x-ray emission output in the water-window region are explored. Kinetic parameters for non-equilibrium plasma including major inelastic ion interaction processes, radiation characteristics are obtained in approach based on the Hartree-Fock-Slater quantum-statistical model and the distorted wave approximation. The presence of fast electrons in plasma at relatively small portions may have a significant influence on the ion level populations and the line emission intensities. Emission generation efficiency doubles at a temperature of 60 eV with 1% portion of fast electrons with respect to equilibrium plasma and the corresponding spectral efficiency jumps to 5.5%.

Control of the polarization direction of isolated attosecond pulses using inhomogeneous two-color fields

We theoretically demonstrate the control of the polarization direction of isolated attosecond pulses (IAPs) with inhomogeneous two-color fields synthesized by an 800-nm fundamental pulse and a 2000-nm control pulse having crossed linear polarizations. The results show that by using the temporally and spatially shaped field, the high-order harmonic generation (HHG) process can be efficiently controlled. An ultra-broad supercontinuum ranging from 150th to 400th harmonics which covers the water window region is generated. Such a supercontinuum supports the generation of a 64-as linearly polarized IAP, whose polarization direction is at about 45° with respect to the x axis. Moreover, we analyze the influence of the inhomogeneity parameters and the relative angle of the fundamental and control pulses on the IAP generation. It is shown that the polarization direction of the IAP can rotate in a wide range approximately from 8° to 90° relative to the x axis when the inhomogeneity parameters and the relative angle vary.

Electron temperature optimization for efficient water-window soft x-ray emission from discharge-produced highly charged zirconium ions

We determined the optimum electron temperature for water-window soft x-ray emission by observing the spectral behavior in the 2.3–4.4 nm region of highly charged zirconium (Zr) ions in hot hydrogen plasmas produced in a magnetically confined fusion device. In the water-window soft x-ray spectral region, the main emission involved resonant ${3}d - {4}f$3d−4f ($\Delta n = {1}$Δn=1) transitions. According to the collisional-radiative (CR) model verified by the experimental results, the ionic population for the charge states from ${{\rm Zr}^{14 + }}$Zr14+ to ${{\rm Zr}^{20 + }}$Zr20+ required to produce the emission was maximized in the electron temperature range of 80–180 eV. For laboratory-scale water-window soft x-ray source application, it is therefore important to produce an electron temperature significantly lower than 200 eV for the production of the suitable ionic charge states of ${{\rm Zr}^{14 + }} - {{\rm Zr}^{20 + }}$Zr14+−Zr20+.

X-ray imaging of bio/medical samples using laser-plasma-based X-ray sources and LiF detector

This contribution to ECPD2019 is dedicated to the memory of Anatoly Faenov. During a period of approximately thirteen years 1994–2006, Anatoly and his wife Tatiana Pikuz (simply “Tania” for friends), accepting the frequent invitations of the National Institute for Nuclear Physics (INFN) and of the Italian National Agency for New Technologies, Energy and Sustainable Economic Development (ENEA), cooperated with many Italian research laboratories dedicated to EUV and soft X-ray generation, spread in different towns (L'Aquila, Frascati, Milano, Padova, Pisa, Roma, etc.). In spite of the fact that they could stay in Italy only about one or two months per year, their activity was so intense that more than 50 peer- reviewed publications were generated from their experimental and theoretical work (just considering only the results obtained at L'Aquila and Tor Vergata—Rome Universities and at the ENEA Research Center of Frascati), without mentioning the cultural atmosphere that they stimulated in the field of Science and Humanity. The numerous experimental spectra obtained at ENEA by means of their spherically bent mica spectrometers, together with the corresponding theoretical simulations performed in Moscow, allowed to study the changing role of different excitations mechanisms for various plasma conditions, and to characterize at best the ENEA laser-plasma source for different applications: polychromatic and monochromatic micro-radiography of dried biological samples at 1 keV, soft X-ray contact microscopy (SXCM) of living cells in the water-window spectral region, spectroscopy of hollow atoms, etc. In this memorial paper, the main results of biological samples imaging on lithium fluoride (LiF) detectors, obtained with the ENEA and Tor Vergata University laser-plasma sources, are presented. In particular, the improvement of the micro-radiography and of the SXCM techniques obtained after moving from photoresist detectors and photographic films to lithium fluoride (LiF) detectors are discussed, for both dried and wet biological samples.

X-ray Lasers in Cluster Flows and in Nanostructured Targets

The paper presents a brief review of recent works concerning the modeling of X-ray lasers in cluster flows and in nanostructured targets. Calculations of the atomic characteristics are based on relativistic perturbation theory with a model potential of zero approximation. Two new results are discussed: (1) it is shown that a subpicosecond X-ray laser with λ = 41.8 nm formed in a xenon cluster flow can serve as an alternative to a free-electron laser and (2) in heavy Ni-like ions (Z ≥ 60), the ionization of ions and recombination of electrons are balanced at electronic temperatures ≥1500 eV; thus, the state of a Ni-like ion is quasi-steady-state. The inversions of many transition levels of an X-ray laser are also quasi-steady-state. The possibility of experimental observation of X-ray lasers based on 3p54d104p [J = 0] – 3p63d94p [J = 1] intrashell transitions in Gd36+ with wavelengths in the water window region is discussed.

Generation of water window single attosecond pulse from multi-cycle mid-infrared laser field with chirp gating modulation

A potential scheme to produce the water window single attosecond pulses (SAPs) from the multi-cycle mid-infrared (MIR) laser field has been investigated with the help of the chirp gating modulation. It is found that with the introduction of the laser chirp (i.e. up-chirp or down-chirp modulation), the extension of the harmonic cutoff can be achieved and the single harmonic radiation peak (HRP) can be selected during the harmonic emission process. Moreover, the chirp gating modulation on the high-order harmonic generation (HHG) is sensitive to the few-cycle pulse duration, but it is not very sensitive to the multi-cycle pulse duration. Moreover, a larger extension of the harmonic cutoff covering the whole water window region can be found with the help of the multi-cycle down-chirp modulation. Further, by properly choosing the coherent superposition of the ground state and the high Rydberg state as the initial state, the efficiency of HHG can be enhanced by 5 orders of magnitude. Finally, a series of high-intensity sub-40as pulses covering the water window region can be obtained.

Improvement of High-Order Harmonic Generation Via Controlling Multiple Acceleration–Recombination Process

Abstract The multiple acceleration–recombination process in high-order harmonic generation (HHG) has been investigated and discussed. Generally, the HHG can be explained through the ionization–acceleration–recombination process in each half-cycle waveform of the laser field. In this article, through the waveform control via the two-colour frequency-chirping laser field, the multiple acceleration–recombination process of the free electron in a specific “W” waveform structure can be found, which will lead to the larger emitted photon energies. Moreover, with the optimization of this “W” waveform by changing the frequency chirps, the carrier envelope phases, and the delay time, not only the efficiency of HHG can be enhanced compared with that from the original chirp-free pulse, but also the larger harmonic cutoff can be obtained. Further, with the assistance of the unipolar pulses, the cutoff and the efficiency of HHG can be further improved, showing a water window spectral continuum with the intensity enhancement of 66 times. As a result, by properly superposing some selected harmonics on the spectral continuum, three intense 38-as pulses in the water window region can be obtained.

Рентгеновские лазеры в потоках кластеров и в наноструктурированных мишенях

AbstractThe paper presents a brief review of recent works concerning the modeling of X-ray lasers in cluster flows and in nanostructured targets. Calculations of the atomic characteristics are based on relativistic perturbation theory with a model potential of zero approximation. Two new results are discussed: (1) it is shown that a subpicosecond X-ray laser with λ = 41.8 nm formed in a xenon cluster flow can serve as an alternative to a free-electron laser and (2) in heavy Ni-like ions ( Z ≥ 60), the ionization of ions and recombination of electrons are balanced at electronic temperatures ≥1500 eV; thus, the state of a Ni-like ion is quasi-steady-state. The inversions of many transition levels of an X-ray laser are also quasi-steady-state. The possibility of experimental observation of X-ray lasers based on 3 p ^54 d ^104 p [ J = 0] – 3 p ^63 d ^94 p [ J = 1] intrashell transitions in Gd^36+ with wavelengths in the water window region is discussed.

Attosecond chirp compensation in water window by plasma dispersion.

Compensating attosecond chirp (atto-chirp) of broadband high-order harmonic pulses in the water window region (282 to 533 eV) is a major challenge, due to the lack of natural materials that exhibit negative group velocity dispersion and low loss. Analysis shows that the amount of dispersion of fully ionized hydrogen plasma with suitable density-length product is sufficient to compensate the chirp of attosecond pulses with center photon energy above 300 eV. This is confirmed by numerical simulations based on the Strong Field Approximation.

Towards GW-Scale Isolated Attosecond Pulse Far beyond Carbon K-Edge Driven by Mid-Infrared Waveform Synthesizer

We discuss the efficient generation of intense “water window” (0.28–0.54 keV) isolated attosecond pulses (IAPs) using a mid-infrared (MIR) waveform synthesizer. Our numerical simulations clearly indicate that not only a longer-wavelength driving laser but also a weak control pulse in the waveform synthesizer helps extend the continuum cutoff region and reduce the temporal chirp of IAPs in high-order harmonic generation (HHG). This insight indicates that a single-cycle laser field is not an optimum waveform for generating the shortest IAP from the veiwpoints of reducing the attochirp and increasing the efficiency of HHG. By combining a waveform synthesizer technology and a 100 mJ MIR femtosecond pulse based on a dual-chirped optical parametric amplification (DC-OPA) method, a gigawatt-scale IAP (55 as with 10 nJ order) in the water window region can be generated even without attochirp compensation. The MIR waveform synthesizer is highly beneficial for generating a shorter IAP duration in the soft X-ray region because there are no suitable transparent dispersive materials that can be used for compressing the attochirp.

Enhancement of attosecond pulse in water window region by using pump-probe approach

An effective scheme to enhance the harmonic yield and the attosecond (as) pulse signal from H[Formula: see text] has been proposed by using the pump-probe laser field. It is found that with the help of the multi-cycle pump pulse, H[Formula: see text] can be steered into the resonance ionization regions, where the ionization probability can be remarkably enhanced. Thus, the harmonic yield can be remarkably enhanced when a sequential mid-infrared probe pulse is added. Further, by modulating the phase of the probe pulse and by adding a controlling pulse, the harmonic cutoff can be extended up to the water window region. Finally, by the Fourier transformation of the selected harmonics on the harmonic supercontinuum, the water window attosecond pulses as short as 25 as can be obtained.

Intense water-window soft x-ray emission by spectral control using dual laser pulses.

We demonstrate intense emission in the water-window soft x-ray spectral region by controlling the spectral behavior through changing the balance between emissivity and self-absorption in an expanding plasma. The number of photons obtained from a dual laser irradiated target with a 150-ps pre-pulse was maximized at 3.8 × 1014 photons/sr in λ = 2.34 - 4.38 nm at a pulse separation time of 7 - 10 ns. Enhancement of the number of photons is attributed to efficient coupling with the main laser pulse while maintaining a tiny source size.

Extension of water-window harmonic cutoff by laser defocusing-assisted phase matching.

We extend a recently demonstrated scheme [Optica4, 976 (2017)OPTIC82334-253610.1364/OPTICA.4.000976] to overcome the limit of conventional harmonic cutoff for different pulse durations, laser wavelengths, and gas targets. By tuning the truncation of long wavelength lasers, we show that the defocusing-assisted phase matching (DAPM) can be achieved in a tightly focused beam and highly ionized short gas cell, and can be used to effectively extend the harmonic cutoff energy and optimize its yield. An analysis of phase matching reveals that at longer wavelengths, greater cutoff extension to the water window region is achieved because of the larger harmonic intrinsic phase (proportional to the cube of laser wavelength), and because DAPM works at relatively higher laser intensities using a Ne target. This scheme provides a promising method for efficiently generating intense attosecond light sources in the extreme ultraviolet to x-rays.

Selection and Enhancement of the Single Harmonic Emission Event in the Water Window Region

Abstract The control of the high-order harmonic generation in the half-cycle region has been investigated by using the improved polarization gating (PG) technology. It is found that by properly controlling the delay time of the PG pulse, the contribution of the harmonic plateau is nearly coming from the single harmonic emission event, which is much better for producing the single attosecond pulses (SAPs). Further, by properly adding an ultraviolet pulse and a half-cycle pulse in the driven laser polarization direction, the harmonic yield can be enhanced and the harmonic cutoff can be extended, showing a high-intensity harmonic plateau covering the whole water window region. Finally, through the Fourier transformation of some selected harmonics, a 35 as SAP in the water window region can be obtained.

Spectral dynamics of soft X-ray emission in dual-laser-produced medium-Z plasma

Laser-produced medium element plasma sources are being considered as strong candidates for in vivo photographic imaging of biological samples in laboratory-scale water-window soft X-ray microscopes. We explored spectral changes in the emission from dual-laser-produced zirconium (Zr) plasmas in the water-window soft X-ray spectral region. The emission was enhanced at a delay time of 5 ns between the pre- and main-laser pulses and found to possess a source size of $$38\,\upmu \hbox {m }\times 68\,\upmu \hbox {m}$$ very similar to that obtained without any pre-pulse. We also investigated the decrease in emission observed at longer delay times, in the context of the collisional-radiative (CR) model-calculated absorption coefficient.

Selection of target elements for laser-produced plasma soft x-ray sources.

We demonstrated the upper limitation to the number of shots, i.e., target lifetime, together with the number of photons emitted in the water-window soft x-ray spectral region from a number of targets used as sources in this spectral region, for multi-shot irradiation at the same position on the target surface. The spectra involved result from unresolved transition arrays originating from n=3-n=4 transitions in medium-Z element plasmas and from n=4-n=4 transitions originating in high-Z plasmas. The output flux was maintained for the highest number of shots in the case of the high melting point element molybdenum, and the total output in the water window was 7.7×1013 photons/sr at a laser power density of 1.2×1014 W/cm2.