Vacuum Ultraviolet Spectral Range Research Articles

High Harmonic Generation near the Low-Frequency Edge of a Plateau under Nonlinear Propagation of 1.24-μm Near-Infrared Femtosecond Laser Radiation in a Dense Argon Jet

High (15–25) harmonic generation in the vacuum ultraviolet spectral range (83–50 nm) has been realized by focused (NA = 0.033) near-infrared femtosecond laser radiation (wavelength λ = 1.24 μm) with a vacuum intensity of ~7.5 × 1014 W/cm2 irradiating a dense gas jet. It has been shown experimentally that the use of such a high-numerical aperture focusing requires high (up to 10 bar) gas jet pressures to optimize phase matching. The use of the dense gas jet results in a noticeable manifestation of nonlinear propagation effects for generating radiation, which affect the generation process through the change in the phase matching conditions. Furthermore, it has been shown that the prechirping of the generating pulse makes it possible to compensate a chirp appearing due to self-phase modulation and to increase the harmonic generation efficiency because of the nonlinear compression of the generating pulse. This approach has allowed 17th (73 nm) harmonic generation with an energy of 2 pJ in a pulse and a generation efficiency of 5.4 × 10–9. The estimates obtained have shown that this radiation can be used for single-pulse maskless photolithography in the extreme ultraviolet range.

Below-threshold harmonic generation in gas-jets for Th-229 nuclear spectroscopy.

The generation of below-threshold harmonics in gas-jets constitutes a promising path towards optical frequency combs in the vacuum ultra-violet (VUV) spectral range. Of particular interest is the 150 nm range, which can be exploited to probe the nuclear isomeric transition of the Thorium-229 isotope. Using widely available high-power, high-repetition-rate Ytterbium-based laser sources, VUV frequency combs can be generated through the process of below-threshold harmonic generation, in particular 7th harmonic generation of 1030 nm. Knowledge about the achievable efficiencies of the harmonic generation process is crucial for the development of suitable VUV sources. In this work, we measure the total output pulse energies and conversion efficiencies of below-threshold harmonics in gas-jets in a phase-mismatched generation scheme using Argon and Krypton as nonlinear media. Using a 220 fs, 1030 nm source, we reach a maximum conversion efficiency of 1.1 × 10-5 for the 7th harmonic (147 nm) and 0.78 × 10-4 for the 5th harmonic (206 nm). In addition, we characterize the 3rd harmonic of a 178 fs, 515 nm source with a maximum efficiency of 0.3%.

A Model Surface for Calculating the Reflectance of Smooth and Rough Aluminum Layers in the Vacuum Ultraviolet Spectral Range

We present a systematic approach to calculating the reflectance of aluminum thin films. In our approach, the rough aluminum surface is modelled as a square array of submicrometer-sized oblate cylinders. The focus of the study is on the vacuum ultraviolet (VUV) spectral range, with wavelengths ranging from 120 nm to 200 nm. The VUV reflectance of aluminum films is calculated by using the rigorous coupled wave approach in order to take the surface roughness of aluminum into account. The modelled reflectance spectra are compared to experimental data from unprotected and protected aluminum films.

The new PTB beamline for vacuum-ultraviolet radiometry

At the Metrology Light Source, a 630 MeV electron storage ring for the use of synchrotron radiation for metrology applications, a new beamline is dedicated to radiometry in the vacuum-ultraviolet spectral range. The emphasis lies on the traceability of measurements and profound uncertainty analysis. To replace the previously existing normal incidence monochromator beamline which serviced for more than 20 years now at different facilities, a newly designed 2 m off-plane Eagle monochromator beamline concept was developed. Different reflective coatings for mirrors and gratings in combination with order-sorting filters ensure highest spectral purity of the monochromatized radiation in combination with optimized photon flux characteristics. The beamline is planned to go into full operation in late 2022.

Chiroptical activity of gas-phase propylene oxide predicting the handedness of interstellar circular polarization in the presolar nebula.

Propylene oxide, the first chiral molecule recently detected in the interstellar medium, has once again raised the question whether biomolecular chirality might have cosmic origins. However, accurate chiroptical properties of propylene oxide in the ultraviolet spectral range necessary to suggest possible asymmetric synthetic routes in the gas phase are scarce. Here, we report on the first experimental measurements of the anisotropy spectra of gas-phase propylene oxide in the vacuum ultraviolet spectral range. Our experimental results provide novel insights into the handedness of interstellar circular polarization at the dawn of molecular evolution of our star- and planet-forming region. Besides the fundamental importance of this new investigation for understanding the origin and evolution of homochirality on Earth, our high-resolution experimental electronic circular dichroism data will inspire new efforts in quantum computational spectroscopy.

Luminescence and Vacuum Ultraviolet Excitation Spectroscopy of Nanophosphors under Synchrotron Irradiation

Vacuum ultraviolet (VUV) excitation spectroscopy under synchrotron irradiation is a powerful tool for the investigation of luminescence properties of wide bandgap nanocrystalline phosphor materials. The advantages of selective excitation in a wide spectral range present the possibility to explore the different aspects of luminescence processes in nanophosphors separately. It is shown that direct excitations of emission centers in wide bandgap materials need excitations in VUV spectral range and such excitations provide valuable information about f–f, f–d transitions, defects, and excitonic transitions in wide bandgap nanophosphors. It is also demonstrated that size‐dependent luminescence properties of nanophosphors are significant if the electron thermalization length becomes larger than the size of the nanoparticles. In this case, multiplication of electronic excitations processes well‐known in bulk materials are suppressed strongly in nanophosphors.

Identification of free and bound exciton emission of MgO single crystal in vacuum ultraviolet spectral range

Temperature dependencies of optical reflectance and cathodoluminescence (CL) spectra were measured for the MgO single crystal using a custom-built vacuum ultraviolet (VUV) spectroscopic system. Simultaneous observation enabled us to identify free exciton (FE) and bound exciton (BE) emissions by comparing the CL emission with the exciton resonance structures. The results indicated that the BE emission dominates the near-band edge emission, and the FE emission was observed as a shoulder at 300 K. The results ensure strong excitonic nature and potential of a rock salt-structured MgO-based material system for an active element in the VUV light emitter.

Image converter tubes with diamond photocathodes and electron flow multipliers

The results of investigations of solar-blind image converter tubes (ICTs), sensitive in the vacuum-ultraviolet (VUV) spectral range are presented. Sensitive-conversion layers of photocathodes based on boron-doped polycrystalline diamond films were grown up on sapphire substrates for the first time. Electron flow multipliers (EFMs) were fabricated in the form of diamond grid. Solar-blind VUV ICTs without the EFM are characterized by spectral sensitivity range of 180…250 nm, estimate of the threshold sensitivity value ~10-9 W/Hz0.5 and current sensitivity ~12 - 15 mA/W. Solar-blind VUV ICTs comprising the electron flow multipliers are characterized by extended spectral sensitivity range of 180…270 nm, improved estimate of the threshold sensitivity value 10-11… 5 × 10-12 W/Hz 0.5 and current sensitivity 50 mA/W.

Vacuum ultraviolet coherent undulator radiation from attosecond electron bunches

Attosecond duration relativistic electron bunches travelling through an undulator can generate brilliant coherent radiation in the visible to vacuum ultraviolet spectral range. We present comprehensive numerical simulations to study the properties of coherent emission for a wide range of electron energies and bunch durations, including space-charge effects. These demonstrate that electron bunches with r.m.s. duration of 50 as, nominal charge of 0.1 pC and energy range of 100–250 MeV produce 10^9 coherent photons per pulse in the 100–600 nm wavelength range. We show that this can be enhanced substantially by self-compressing negatively chirped 100 pC bunches in the undulator to produce 10^{14} coherent photons with pulse duration of 0.5–3 fs.

Catalog and Statistical Examinations of Lyα Solar Flares from GOES/EUVS-E Measurements

Abstract The Lyman-alpha (Lyα) line of neutral hydrogen at 121.6 nm is by far the brightest emission line in the vacuum ultraviolet spectral range of the Sun. The emission at this line could be a major energy input to the upper layers of the Earth’s atmosphere, strongly impacting the geospace environment. The Geostationary Operational Environmental Satellite (GOES) series, starting with GOES-13, began to carry a multichannel Extreme UltraViolet Sensor (EUVS) with one channel (E-channel) targeting the Lyα line. In the present work, we produce a Lyα flare catalog from the GOES-15/EUVS-E data between 2010 April 8 and 2016 June 6 with an automatic flare detection algorithm. This algorithm is designed to search events at various scales and find their real start and end times. Based on the obtained flare list, statistics on the temporal behavior such as the duration, rise, and decay times, and the event asymmetries of Lyα flares is presented. On average (defined by the median of the distributions), the duration, rise and decay times of the flares were estimated to be 20.8 minutes, 5.6 minutes, and 14.2 minutes, respectively. We also discuss the frequency distributions of the peak flux and the fluence of Lyα flares, both of which reveal power-law behaviors with power-law indices of 2.71 ± 0.06 and 2.42 ± 0.06, respectively, implying that more flares are accumulated at small scales and these small-scale events play an important role in explaining the violent solar energy release.

Vacuum ultraviolet photoabsorption spectroscopy of space-related ices: formation and destruction of solid carbonic acid upon 1 keV electron irradiation

Context. Carbonic acid (H2CO3) is a weak acid relevant to astrobiology which, to date, remains undetected in space. Experimental work has shown that the β-polymorph of H2CO3 forms under space relevant conditions through energetic (UV photon, electron, and cosmic ray) processing of CO2- and H2O-rich ices. Although its α-polymorph ice has been recently reassigned to the monomethyl ester of carbonic acid, a different form of H2CO3 ice may exist and is synthesized without irradiation through surface reactions involving CO molecules and OH radicals, that is to say γ-H2CO3. Aims. We aim to provide a systematic set of vacuum ultraviolet (VUV) photoabsorption spectroscopic data of pure carbonic acid that formed and was destroyed under conditions relevant to space in support of its future identification on the surface of icy objects in the Solar System by the upcoming Jupiter ICy moons Explorer mission and on interstellar dust by the James Webb Space Telescope spacecraft. Methods. We present VUV photoabsorption spectra of pure and mixed CO2 and H2O ices exposed to 1 keV electrons at 20 and 80 K to simulate different interstellar and Solar System environments. Ices were then annealed to obtain a layer of pure H2CO3 which was further exposed to 1 keV electrons at 20 and 80 K to monitor its destruction pathway. Fourier-transform infrared (FT-IR) spectroscopy was used as a secondary probe providing complementary information on the physicochemical changes within an ice. Results. Our laboratory work shows that the formation of solid H2CO3, CO, and O3 upon the energetic processing of CO2:H2O ice mixtures is temperature-dependent in the range between 20 and 80 K. The amorphous to crystalline phase transition of H2CO3 ice is investigated for the first time in the VUV spectral range by annealing the ice at 200 and 225 K. We have detected two photoabsorption bands at 139 and 200 nm, and we assigned them to β-H2CO3 and γ-H2CO3, respectively. We present VUV spectra of the electron irradiation of annealed H2CO3 ice at different temperatures leading to its decomposition into CO2, H2O, and CO ice. Laboratory results are compared to Cassini UltraViolet Imaging Spectrograph observations of the 70−90 K ice surface of Saturn’s satellites Enceladus, Dione, and Rhea.

Low-temperature luminescence of catangasite single crystals under excitation by vacuum ultraviolet synchrotron radiation

The luminescent properties of Ca3TaGa3Si2O14 (CTGS, catangasite) single crystals have been studied by means of the vacuum ultraviolet excitation spectroscopy utilizing synchrotron radiation from 1.5 GeV storage ring of MAX IV synchrotron facility. Two emission bands at 320 nm (3.87 eV) and 445 nm (2.78 eV) have been detected. Examining excitation spectra in vacuum ultraviolet spectral range, the 320 nm emission band was explained as the emission band of self-trapped exciton in CTGS single crystal. Its atomic structure is discussed. It is also proposed that the 445 nm (2.78 eV) emission in the CTGS is due to the F centers, which have shown a well-resolved excitation (absorption) band at 5.1 eV (243 nm).

Low-temperature luminescence of ScF3 single crystals under excitation by VUV synchrotron radiation

Photoluminescence and excitation spectra of ScF3 single crystals have been measured under vacuum ultraviolet excitations utilizing undulator synchrotron radiation from 1.5 GeV storage ring of MAX IV synchrotron. The emission peak at 280 nm is explained as emission band of self-trapped excitons in ScF3. This emission is quenched at 50 K and activation energy of thermal quenching was obtained. The excitation spectrum in vacuum ultraviolet spectral range exhibits that the luminescence of self-trapped excitons effectively occurs under direct excitation in the excitonic absorption band, whereas under higher energies this excitation is strongly suppressed, however, multiplication of electronic excitation processes have been successfully identified.

Time-resolved luminescence and excitation spectroscopy of co-doped Gd3Ga3Al2O12 scintillating crystals

Cerium doped Gd3Ga3Al2O12 (GGAG) single crystals as well as GGAG:Ce single crystals co-doped by divalent (Mg2+, Ca2+) and tetravalent (Zr4+, Ti4+) ions have been studied by means of time-resolved luminescence as well as the excitation luminescence spectroscopy in vacuum ultraviolet (VUV) and soft X-ray (XUV) spectral range. Tunable laser excitation was applied for time-resolved experiments in order to obtain luminescence decay curves under excitations in Ce3+, Gd3+ and excitonic absorption bands. The influence of the co-dopant ions on the Ce3+ luminescence decay kinetics is elucidated. The fastest luminescence decay was observed for the Mg2+ co-doped crystals under any excitation below bandgap energy indicating the perturbation of the 5d states of Ce3+ by Mg2+ ions. Synchrotron radiation was utilized for the luminescence excitation in the energy range from 4.5 to 800 eV. Special attention was paid to the analysis of Ce3+ excitation spectra in VUV and XUV spectral range where multiplication of electronic excitation (MEE) processes occur. Our results demonstrated that GGAG:Ce single crystals co-doped by Mg2+ ions as well as the GGAG:Ce crystal annealed in vacuum reveal the most efficient excitation of Ce3+ emission in VUV-XUV excitation range. The role of intrinsic defects in MEE processes in the co-doped as well as in the annealed GGAG:Ce single crystals is discussed.

Optics of epitaxial strained strontium titanate films

Diverse effects of lattice strain on the optical properties in the near-infrared to vacuum ultraviolet spectral range are experimentally revealed in cube-on-cube-type epitaxial perovskite SrTiO3 films grown on compressive substrate. Compared to the reference crystal, the tetragonal antiferrodistortive film exhibits spectral blueshifts, which are consistent with the theoretically predicted bandgap widening. In addition to this strain-induced interband effect, the peculiar near-edge absorption and smearing of interband transitions are found. It is shown that Fröhlich-type electron–phonon coupling can be enhanced by strain and lead to this behavior. It is suggested that electron–phonon interactions can play an important role in optical properties of ferroelectric films and deserve further studies.

Research on the irradiance calibration of a VUV dual-grating spectrometer based on synchrotron radiation

A high accuracy instrument calibration is the guarantee of obtaining high precision atmospheric inversion data from a wavelength-dispersive space remote sensing instrument in the orbit. To improve the relative calibration uncertainty of a dual-grating spectrometer in the vacuum-ultraviolet (VUV) band, conventional secondary standard light sources, such as deuterium lamps, used in laboratory calibrating stations are not suited to meet high precision. In this paper we present the calibration of the space instrument based on the Metrology Light Source (MLS) of the Physikalisch-Technische Bundesanstalt (PTB) operated as a primary synchrotron radiation (SR) source with calculable spectral radiant intensity to overcome the limit imposed by secondary transfer standards. For taking into account the difference between the highly linearly polarized SR source and the un-polarized solar radiation, which will be observed by the dual-grating spectrometer in orbit, the calibration was performed at two orientations of the instrument, which are perpendicular to each other with respect to the incident SR. The factors contributing to the uncertainty budget were analyzed. It could be shown that a total relative uncertainty of 2.52% can be achieved, which has greatly improved the calibrating accuracy compared with that obtainable with the conventional standard light source calibrating stations in the VUV spectral range.

Multiple optical impacts of anion doping in epitaxial barium titanate films

Multiple strong impacts of anion doping Λ (Λ = oxygen vacancy, nitrogen, or hydrogen) on the optical properties in the near-infrared to vacuum ultraviolet spectral range are experimentally revealed in cube-on-cube-type epitaxial perovskite BaTiO3−δΛδ films (δ ≤ 0.01) grown on (001)SrTiO3 substrates. Compared to the reference undoped films and bulk crystal, the anion-doped films exhibit massive changes of the index of refraction in the transparency range Δn of ∼0.1 to 0.2, a profound bandgap widening ΔEg of ∼0.3 eV to 0.4 eV, a dopant-specific near-edge absorption, and doping-induced interband transitions. Both the conduction-band uplift and the changes in the index of refraction are ascribed to the internal stress and electric field, which result from epitaxially controlled dopant locations in the [Ba–O](001) planes. The dopant-induced in-gap states are responsible for the near-edge absorption, whereas the dopant-induced conduction-band states are suggested to modify the interband transitions and the intrinsic elasto- and electro-optic coefficients.

Ramsey-comb precision spectroscopy in xenon at vacuum ultraviolet wavelengths produced with high-order harmonic generation

The remarkable progress in the field of laser spectroscopy induced by the invention of the frequency-comb laser has enabled many new high-precision tests of fundamental theory and searches for new physics. Extending frequency-comb based spectroscopy techniques to the vacuum (VUV) and extreme ultraviolet (XUV) spectral range would enable measurements in e.g. heavier hydrogen-like systems and open up new possibilities for tests of quantum electrodynamics and measurements of fundamental constants. The main approaches rely on high-harmonic generation (HHG), which is known to induce spurious phase shifts from plasma formation. After our initial report (Physical Review Letters 123, 143001 (2019)), we give a detailed account of how the Ramsey-comb technique is used to probe the plasma dynamics with high precision, and enables accurate spectroscopy in the VUV. A series of Ramsey fringes is recorded to track the phase evolution of a superposition state in xenon atoms, excited by two up-converted frequency-comb pulses. Phase shifts of up to 1 rad induced by HHG were observed at ns timescales and with mrad-level accuracy at $110$ nm. Such phase shifts could be reduced to a negligible level, enabling us to measure the $5p^6 \rightarrow 5p^5 8s~^2[3/2]_1$ transition frequency in $^{132}Xe$ at 110 nm (seventh harmonic) with sub-MHz accuracy. The obtained value is $10^4$ times more precise than the previous determination and the fractional accuracy of $2.3 \times 10^{-10}$ is $3.6$ times better than the previous best spectroscopic measurement using HHG. The isotope shifts between $^{132}Xe$ and two other isotopes were determined with an accuracy of $420$ kHz. The method can be readily extended to achieve kHz-level accuracy, e.g. to measure the $1S-2S$ transition in $He^+$. Therefore, the Ramsey-comb method shows great promise for high-precision spectroscopy of targets requiring VUV and XUV wavelengths.

Luminescence and vacuum ultraviolet excitation spectroscopy of cerium doped Gd3Ga3Al2O12 single crystalline scintillators under synchrotron radiation excitations

Cerium doped Gd3Ga3Al2O12 (GGAG) single crystals as well as GGAG:Ce single crystals co-doped by divalent (Mg2+, Ca2+), trivalent (Sc3+) or tetravalent (Zr4+, Ti4+) ions have been studied by means of the excitation luminescence spectroscopy in vacuum ultraviolet spectral range. Synchrotron radiation from the undulator beam was utilized for the luminescence excitation in the energy range from 4.5 to 800 eV. The influence of the co-dopant ions on the excitonic transitions as well as on the intrinsic defects in GGAG was revealed examining the luminescence emission and excitation spectra of both Gd3+ and Ce3+ ions in all single crystals studied. Special attention was paid to the analysis of Ce3+ excitation spectra in VUV spectral range (4.5–45 eV) where multiplication of electronic excitation (MEE) processes occur. It was obtained that GGAG:Ce single crystals having different co-dopant ions reveal distinguished efficiency of MEE. The role of intrinsic defects in MEE processes in the co-doped GGAG:Ce single crystals was elucidated.

Effects of deposition temperature on optical properties of MgF2 over-coated Al mirrors in the VUV**Project supported by the West Light Foundation of the Chinese Academy of Sciences and the National Natural Science Foundation of China (Grant No. 61805247).

Both long-term environmental durability and high reflectance of protected-Al mirrors are of great importance for developing the optical instruments in the vacuum ultraviolet (VUV) applications. In this paper, the dependence of spectral property and environmental durability of MgF2 over-coated Al mirrors using a 3-step method on deposition temperature of the outermost MgF2 layer are investigated in detail. Optics (reflectance), structure (surface morphology and crystalline), and environmental durability (humidity test) are characterized and discussed. The results show that both optical and moisture-resistant properties of MgF2 over-coated Al mirrors are dependent on MgF2 deposition temperature, and the optimal deposition temperature for the outermost MgF2 layer should be between 250 °C and 300 °C for MgF2 over-coated Al mirrors to have both reasonably high reflectance in the VUV spectral range and high moisture resistance for long lifetime applications.