Short-wavelength Sources Research Articles

High-efficiency second-harmonic generation in reverse-polarization dual-layer lithium niobate waveguides.

Second-harmonic (SH) generation is an important way to generate short-wavelength light sources. Thin-film lithium niobate (TFLN) resonators and waveguides featuring tight light confinement are flexible to realize mode- or quasi-phase-matching (MPM or QPM) and thus efficient SH generation. Here, we report an efficient SH with an absolute conversion efficiency of 45% in a reverse-polarized double-layer TFLN waveguide. Such a high conversion efficiency without periodic poling was realized with the pump of 67 mW in the 1550 nm band, benefiting from the employment of the largest nonlinear coefficient d33 and the significant nonlinear interaction of the fundamental transverse electric (TE) mode and the first-order TE mode in the vertical direction. This work paves the way toward on-chip integrated nonlinear optics in terms of harmonic generation and quantum light sources across the telecom and visible bands.

Enhancing the efficiency of high-order harmonics with two-color non-collinear wave mixing in silica

The emission of high-order harmonics from solids under intense laser-pulse irradiation is revolutionizing our understanding of strong-field solid-light interactions, while simultaneously opening avenues towards novel, all-solid, coherent, short-wavelength table-top sources with tailored emission profiles and nanoscale light-field control. To date, broadband spectra in solids have been generated well into the extreme-ultraviolet (XUV), but the comparatively low conversion efficiency in the XUV range achieved under optimal conditions still lags behind gas-based high-harmonic generation (HHG) sources. Here, we demonstrate that two-color high-order harmonic wave mixing in a fused silica solid is more efficient than solid HHG driven by a single color. This finding has significant implications for compact XUV sources where gas-based HHG is not feasible, as solid XUV wave mixing surpasses solid-HHG in performance. Moreover, our results enable utilizing solid high-order harmonic wave mixing as a probe of structure or material dynamics of the generating solid, which will enable reducing measurement times compared to the less efficient regular solid HHG. The emission intensity scaling that follows perturbative optical wave mixing, combined with the angular separation of the emitted frequencies, makes our approach a decisive step for all-solid coherent XUV sources and for studying light-engineered materials.

Analysis of the extreme ultraviolet broadband spectral characteristics and spatiotemporal evolution of laser-produced germanium plasmas

This paper presents comprehensive spectral measurements and a theoretical analysis of laser-produced germanium (Ge) plasma within the 7.5–17 nm wavelength range, with the measurements being performed using spatiotemporally-resolved emission spectroscopy. We obtained and analyzed the extreme ultraviolet (EUV) spectra and their variations meticulously at various positions adjacent to the target surface. The 3p and 3d excitations of Ge ions spanning from Ge4+ to Ge13+ were calculated using the Cowan configuration interaction codes, with particular emphasis being placed on analysis of the spectral line distributions in the 3d-np, 3d-nf, and 3p-3d, 4s, 4d transition arrays. This analysis indicated the contributions made by these transition arrays to the broadband spectral features that were observed experimentally. By using a steady-state collisional radiation model along with a normalized Boltzmann distribution assumption, we clarified the predominant contributions of the 3d-4p and 3p-3d transitions from the Ge7+ to Ge9+ ions in close proximity to the target surface, along with those from the Ge5+ and Ge6+ ions at greater distances. Furthermore, by combining the results above with a plasma dynamics evolution analysis, we gained insights into how the plasma's transient and nonuniform properties influence the analysis of complex EUV band spectral profiles and examine their implications for spectral diagnostics. These results will be useful for plasma spectral diagnosis and for application to development of pulsed short-wavelength light sources.

Analysis of extreme ultraviolet radiation and hydrodynamics simulation at the core of laser-produced nickel plasmas

The non-uniformity and transient nature of laser-produced plasma are critical factors that affect the analysis of the extreme ultraviolet spectra of highly charged ions and the diagnosis of plasma states. This paper systematically investigates the characteristics of extreme ultraviolet radiation and the hydrodynamic evolution of laser-produced nickel plasmas from two perspectives: high-spatio-temporal-resolution extreme-ultraviolet spectroscopic measurement and radiation hydrodynamics simulation. The consistency between the four-band experimental spectra and their theoretically simulated spectra confirms the accuracy of the atomic structure parameters and plasma state parameters. We also analyze the significant contribution of the 3d-4f double-excited state radiation to the spectral profile and discuss the influence of the self-absorption caused by plasma opacity on the characteristics of extreme ultraviolet radiation. The findings are crucial for accurately understanding the characteristics of extreme ultraviolet radiation, the hydrodynamic evolution, and the application of medium- and high-Z laser-produced plasma as a pulsed short-wavelength light source.

Azimuthally extreme-ultraviolet focal splitter by modified spiral photon sieves

Extreme Ultraviolet (EUV) radiation is a short-wavelength light source that has important applications in many fields, such as optical communication, particle manipulation, and ultrahigh resolution imaging. However, the highly absorptive nature of EUV light makes it challenging to design suitable focusing optics, such as focal splitters, to properly manipulate the energetic light. Here, we propose modified spiral photon sieves to transform EUV laser light into azimuthally splitting focusing. A genetic algorithm was used to design and optimize the azimuthally focal splitters. A capillary discharge EUV laser at 46.9 nm was used to verify the effectiveness of our proposed method, and PMMA targets were used to record the focused laser spot. The profile of the recorded patterns measured by atomic force microscopy shows that the focal spots in the experiment are diffraction-limited and agreed with the theoretical analysis. The proposed technique provides a new way for manipulating EUV light and further extends the applications ranging from EUV to soft x rays.

High-resolution imaging enabled by 100-kW-peak-power parametric source at 5.7 THz

Similar to x-ray imaging, THz imaging will require high power and high resolution to advance relevant applications. Previously demonstrated THz imaging usually experiences one or several difficulties in insufficient source power, poor spectral tunability, or limited resolution from a low-wavelength source. A short-wavelength radiation source in the 5–10 THz is relatively scarce. Although a shorter wavelength improves imaging resolution, widely used imaging sensors, such as microbolometers, Schottky diodes, and photoconductive antennas, are usually not sensitive to detect radiation with frequencies above 5 THz. The radiation power of a high-frequency source becomes a key factor to realize low-noise and high-resolution imaging by using an ordinary pyroelectric detector. Here, we report a successful development of a fully coherent, tunable, > 100-kW-peak-power parametric source at 5.7 THz. It is then used together with a low-cost pyroelectric detector for demonstrating high-resolution 5.7-THz imaging in comparison with 2-THz imaging. To take advantage of the wavelength tunability of the source, we also report spectrally resolved imaging between 5.55 and 5.87 THz to reveal the spectroscopic characteristics and spatial distribution of a test drug, Aprovel.

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.

Phase-matched high-order harmonic generation in pre-ionized noble gases

One of the main difficulties of efficiently generating high-order harmonics in long neutral-gas targets is to reach the phase-matching conditions. The issue is that the medium cannot be sufficiently ionized by the driving laser due to plasma defocusing. We propose a method to improve the phase-matching by pre-ionizing the gas using a weak capillary discharge. We have demonstrated this mechanism, for the first time, in absorption-limited XUV generation by an 800 nm femtosecond laser in argon and krypton. The ability to control phase-mismatch is confirmed by an analytical model and numerical simulations of the entire generation process. Our method allows to increase the efficiency of the harmonic generation significantly, paving the way towards photon-hungry applications of these compact short-wavelength sources.

A localized view on molecular dissociation via electron-ion partial covariance

Inner-shell photoelectron spectroscopy provides an element-specific probe of molecular structure, as core-electron binding energies are sensitive to the chemical environment. Short-wavelength femtosecond light sources, such as Free-Electron Lasers (FELs), even enable time-resolved site-specific investigations of molecular photochemistry. Here, we study the ultraviolet photodissociation of the prototypical chiral molecule 1-iodo-2-methylbutane, probed by extreme-ultraviolet (XUV) pulses from the Free-electron LASer in Hamburg (FLASH) through the ultrafast evolution of the iodine 4d binding energy. Methodologically, we employ electron-ion partial covariance imaging as a technique to isolate otherwise elusive features in a two-dimensional photoelectron spectrum arising from different photofragmentation pathways. The experimental and theoretical results for the time-resolved electron spectra of the 4d3/2 and 4d5/2 atomic and molecular levels that are disentangled by this method provide a key step towards studying structural and chemical changes from a specific spectator site.

Optical design of a laser wavefront sensor applicable under strong diffraction effects by irreproducible microscale high-density plasma

Accurate measurements of electron density in irreproducible microscale high-density plasmas are indispensable for improving laser processing and plasma processing technology because the dynamics of these plasmas are strongly influenced by their electron density. Because single-path laser wavefront sensors are capable of acquiring the two-dimensional electron density distribution with a single shot, the electron density of irreproducible millimeter-scale low-density plasmas has been measured by using such sensors. However, the strong diffraction effects caused by the irreproducible microscale high-density plasmas pose challenges for the measurement. In this study, we numerically and experimentally demonstrate a suitable optical configuration of single-path laser wavefront sensors for accurate measurements of irreproducible microscale high-density plasmas with minimal measurement errors. Our Fresnel diffraction-based numerical simulation indicates that the serious measurement errors caused by the strong diffraction effects can be significantly reduced through the use of relay lenses with high magnification and a short-wavelength laser source. In addition, we propose an alignment procedure for the optical setup to minimize the measurement errors and experimentally validated the procedure by measuring a laser wavefront shaped by a spatial light modulator. Finally, we applied the verified laser wavefront sensor to the measurement of a laser-induced plasma with a two-dimensional line-integrated electron density higher than 1 × 1021 m−2 in an approximately 40 × 50 μm region. This study provides a new strategy to rigorously analyze the dynamics of irreproducible microscale high-density plasmas using a laser wavefront sensor.

Klystron-like Cyclotron Amplification of a Transversely Propagating Wave by a Spatially Developed Electron Beam

A klystron-like gyro-amplifier based on the excitation of a wave propagating across a spatially developed (in the transverse direction) electron beam is described within the simplest 2-D model. Such a configuration is attractive as a way of implementation of a short-wavelength source with a relatively high level of output power and with the possibility of quasicontinuous frequency tuning. We study the peculiarities of the 2-D process (developing in both the axial and transverse directions) of electron bunching and “free” wave emission from the electron beam in the open drift space, as well as the excitation of the output cavity used to provide formation of a compact and powerful output wave signal. The main problem of this 2-D process is that different fractions of the electron beam (located at different points of its cross-section) move in different wave fields. In addition, excitation of the parasitic wave propagating in the opposite direction relative to the operating wave is possible. However, we show that it is possible to organize effective electron–wave energy exchange for almost all fractions of the electron beam.

Dips in high-order harmonics spectra from a subcycle-driven two-level system reflected in the negativity structure of the time-frequency Wigner function

We investigate high-order harmonics spectra radiated from a two-level model system driven by strong, ultrabroadband, half- and single-cycle pulses, which are shorter than the inverse of the transition frequency. In this driving regime, the plateau in frequency spectra typical for radiation from strongly driven systems, has noticeable modulation in amplitude due to interference between waves of same frequency and emitted at different time instants. Specifically, there are characteristic ‘dip’ structures at a set of frequencies in the radiation spectra, where the corresponding amplitudes are suppressed by several orders of magnitude. Understanding these structures is required for applications such as the generation of attosecond pulse, where the number of composing modes and their relative phases are important. Therefore, we demonstrate a systematic way to find frequencies at which the dips are formed. To further illustrate the interference mechanism, we extract the phase information with the help of time-frequency distribution functions, namely the Husimi and Wigner functions. In particular, we found that the negativity structure of the Wigner function corresponds to each dip frequency and that the information regarding the type of interference is encoded in the pattern of the negative region of the Wigner function. Since such time-frequency Wigner function can actually be measured, we envisage utilizing its negativity structure to extract the phase information between radiation components emitted at time points within a subcycle timescale. This should provide an efficient tool for understanding and designing photonic applications, including short-wavelength coherent light sources.

Neighboring Atom Collisions in Solid-State High Harmonic Generation

High harmonic generation (HHG) from solids shows great application prospects in compact short-wavelength light sources and as a tool for imaging the dynamics in crystals with subnanometer spatial and attosecond temporal resolution. However, the underlying collision dynamics behind solid HHG is still intensively debated and no direct mapping relationship between the collision dynamics with band structure has been built. Here, we show that the electron and its associated hole can be elastically scattered by neighboring atoms when their wavelength approaches the atomic size. We reveal that the elastic scattering of electron/hole from neighboring atoms can dramatically influence the electron recombination with its left-behind hole, which turns out to be the fundamental reason for the anisotropic interband HHG observed recently in bulk crystals. Our findings link the electron/hole backward scattering with Van Hove singularities and forward scattering with critical lines in the band structure and thus build a clear mapping between the band structure and the harmonic spectrum. Our work provides a unifying picture for several seemingly unrelated experimental observations and theoretical predictions, including the anisotropic harmonic emission in MgO, the atomic-like recollision mechanism of solid HHG, and the delocalization of HHG in ZnO. This strongly improved understanding will pave the way for controlling the solid-state HHG and visualizing the structure-dependent electron dynamics in solids.

An open-source, end-to-end workflow for multidimensional photoemission spectroscopy

Characterization of the electronic band structure of solid state materials is routinely performed using photoemission spectroscopy. Recent advancements in short-wavelength light sources and electron detectors give rise to multidimensional photoemission spectroscopy, allowing parallel measurements of the electron spectral function simultaneously in energy, two momentum components and additional physical parameters with single-event detection capability. Efficient processing of the photoelectron event streams at a rate of up to tens of megabytes per second will enable rapid band mapping for materials characterization. We describe an open-source workflow that allows user interaction with billion-count single-electron events in photoemission band mapping experiments, compatible with beamlines at 3rd and 4rd generation light sources and table-top laser-based setups. The workflow offers an end-to-end recipe from distributed operations on single-event data to structured formats for downstream scientific tasks and storage to materials science database integration. Both the workflow and processed data can be archived for reuse, providing the infrastructure for documenting the provenance and lineage of photoemission data for future high-throughput experiments.

Beating absorption in solid-state high harmonics

Since the new millennium coherent extreme ultra-violet and soft x-ray radiation has revolutionized the understanding of dynamical physical, chemical and biological systems at the electron’s natural timescale. Unfortunately, coherent laser-based upconversion of infrared photons to vacuum-ultraviolet and soft x-ray high-order harmonics in gaseous, liquid and solid targets is notoriously inefficient. In dense nonlinear media, the limiting factor is strong re-absorption of the generated high-energy photons. Here we overcome this limitation by generating high-order harmonics from a periodic array of thin one-dimensional crystalline silicon ridge waveguides. Adding vacuum gaps between the ridges avoids the high absorption loss of the bulk and results in a ~ 100-fold increase of the extraction depth. As the grating period is varied, each high harmonic shows a different and marked modulation, indicating their waveguiding in the vacuum slots with reduced absorption. Looking ahead, our results enable bright on-chip coherent short-wavelength sources and may extend the usable spectral range of traditional nonlinear crystals to their absorption windows. Potential applications include on-chip chemically-sensitive spectro-nanoscopy.

Pulsed laser-plasma soft X-ray source as a compact tool for X-ray absorption spectroscopy of metal oxides

Laser-plasma short-wavelength source based on double-stream gas-puff target and emitting soft X-rays (SXR) is demonstrated as a compact tool suitable for X-ray absorption spectroscopy (XAS) of metal oxides. The source, optimized for emission in the spectral range between 1.5 and 5 nm from a krypton/helium target appears to be useful for the near edge X-ray absorption spectroscopy (NEXAFS) close to the Ti L-edge and Mo M-edge, as well as the K-edge of oxygen. High photon flux from the source enabled the simultaneous acquisition of the reference and transmission spectra using a flat-field grating spectrometer. The measurements conducted in the transmission mode revealed the spectral features near the absorption edges (Ti-L2,3 and Mo-M5) in metal oxides.

Near-field sub-diffraction photolithography with an elastomeric photomask

Photolithography is the prevalent microfabrication technology. It needs to meet resolution and yield demands at a cost that makes it economically viable. However, conventional far-field photolithography has reached the diffraction limit, which imposes complex optics and short-wavelength beam source to achieve high resolution at the expense of cost efficiency. Here, we present a cost-effective near-field optical printing approach that uses metal patterns embedded in a flexible elastomer photomask with mechanical robustness. This technique generates sub-diffraction patterns that are smaller than 1/10th of the wavelength of the incoming light. It can be integrated into existing hardware and standard mercury lamp, and used for a variety of surfaces, such as curved, rough and defect surfaces. This method offers a higher resolution than common light-based printing systems, while enabling parallel-writing. We anticipate that it will be widely used in academic and industrial productions.

Five-photon absorption upconversion lasing from on-chip whispering gallery mode.

In the progress of ultrafast optics, nonlinear interactions between light and matter are very important in scientific and technical fields. In particular, the high-order nonlinear effect induced by multi-photon absorption (MPA) upconversion lasing has injected new impetus into the research on short-wavelength laser sources. Here, we report the realization of amplified spontaneous emission (ASE) by MPA simultaneously in an epitaxy thin film. In addition, by virtue of the excellent optical confinement of cylindrical microcavities with high Q (∼4 × 103) on-chip, we demonstrated, for the first time, low-threshold upconversion lasing of five-photon absorption enhanced by a microcavity at room temperature. The resonant whispering-gallery mode (WGM) distribution in cylindrical microcavities was simulated comprehensively by the finite difference time domain (FDTD) method. We found that the high-order nonlinear optical process could be significantly enhanced in the microcavity with an increase in the lifetime of radiation photons.

Application of Quasi-Phase Matching Concept for Enhancement of High-Order Harmonics of Ultrashort Laser Pulses in Plasmas

Novel methods of coherent short-wavelength sources generation require thorough analysis for their further amendments and practical implementations. In this work, we report on the quasi-phase matching (QPM) of high-order harmonics generation during the propagation of single- and two-color femtosecond pulses through multi-jet plasmas, which allows the enhancement of groups of harmonics in different ranges of extreme ultraviolet. The role of the number of coherent zones; sizes of plasma jets and the distance between them; plasma formation conditions, and the characteristics of the fundamental radiation on the harmonic efficiency at quasi-phase matching (QPM) conditions are analyzed. We demonstrate the ~40× enhancement factor of the maximally-enhanced harmonic with respect to the one generated at ordinary conditions in the imperforated plasma.

Resonant Excitation of Volume and Surface Fields on Complex Electrodynamic Surfaces

Analytical, numerical, and experimental studies of volume and surface-field coupling in planar metal periodic surface lattice (PSL) structures superimposed on dielectric substrates with a metallic backing (PSLDM) are presented. We show the formation of frequency-locked PSLDM-coupled eigenmodes and unlocked surface-field resonances (PSL without substrate). These experimental observations are in excellent agreement with theoretical and numerical predictions. For the first time, the derivation of a field coupling coefficient α is demonstrated. By comparing theoretical and numerical dispersions, we obtain α . Detailed analysis of possible scattering mechanisms and dispersive behavior in subwavelength “effective metadielectric” PSLs is shown. The theory and measurements presented in this paper are applicable over a broad frequency range from optical frequencies to THz and are fundamental to the innovation of high-power short-wavelength sources, solar cells, and alternative subwavelength absorbers.