Tunable UV Research Articles

Preventive conservation of paper-based relics with visible light high-transmittance ultraviolet blocking film based on carbon dots

Paper-based relics is an important carrier for recording and preserving information, however, it faces irreversible UV-induced damage, including photocleavage, oxidation, acidification and discoloration, which seriously affects its value and lifespan. Carbon dots (CDs) possess excellent UV absorption and good chemical stability, making them suitable for UV protection. Herein, we propose a high-security and efficient method utilizing CDs films (CDFs) for preventive protection of paper against UV damage. The CDFs with high tunable UV absorbance and minimal absorbance in the visible light range, effectively shield paper from UV radiation while preserving its visual appeal. Moreover, the UV transmittance of the film can be fine-tuned to the content of CDs and can be easily removed from the paper without residue. Artificial accelerated UV aging experiments demonstrate the deceleration of acidification, oxidation, and photocleavage in the protected bamboo paper and Xuan paper. This research paces a new direction for the protection of paper and paper-based relics and artworks with emerging carbon materials, offering customizable protection effects tailored to specific preservation and exhibition requirements. This research pioneers a novel approach to preventive protection of paper and paper-based relics using emerging carbon dots materials, offering tailored protection for diverse preservation needs.

Electronic Structure, Aromaticity, and Magnetism of Minimum-Sized Regular Dodecahedral Endohedral Metallofullerenes Encapsulating Rare Earth Atoms.

A series of minimally sized regular dodecahedron-embedded metallofullerene REC20 clusters (RE = Sc, Y, La, Ce, Pr, Nd, Pm, Sm, Eu, and Gd) as basic units of nanoassembled materials with tunable magnetism and UV sensitivity have been explored using density functional theory (DFT). The contribution of the 4f orbital of the rare earth atom at the center of the C20 cage to the frontier molecular orbital of REC20 gives the REC20 cluster additional stability. The AdNDP orbitals of the four REC20 superatoms that conform to the spherical jellium model indicate that through natural population analysis and spin density diagrams, we observe a monotonic increase in the magnetic moment from Ce to Gd. This is attributed to the increased number of unpaired electrons in the 4f orbitals of lanthanide rare earth atoms. The UV-visible spectrum of REC20 clusters shows strong absorption in the mid-UV and near-UV bands. REC20 clusters encapsulating lanthanide rare earth atoms stand out for their tunable magnetism, UV sensitivity, and stability, making them potential new self-assembly materials.

Tunable UV ∼ IR frequency comb generation via high-order sideband generation

We propose the generation of a widely tunable UV-to-IR frequency comb by high-order sideband generation (HSB) spectrum emitted from semiconductors. In our theoretical simulations, we demonstrate the high-order sideband signals of two series (2m Ωseed + (2n + 1) ωdriver, and (2m + 1) Ωseed + 2 nωdriver ), where m and n are integers of a seed pulse and a driver laser frequency, respectively. The simulations also reveal the intensity of HSB scale with the driver laser power, both perturbatively and non-perturbatively. We find that the harmonic position and spacing of the high-order sideband emission can be controlled by varying the seed pulse and driver photon energies. In the experiment, we applied a visible ( ℏΩseed = 3.1 eV, ∼400 nm) seed pulse and mid-infrared (MIR, ℏωdriver = 0.4 eV, 3.1 μm) driver pulses to ZnSe target. Our experimental observations confirmed the UV (4.7 eV, 263 nm and 3.9 eV, 317 nm) HSB generation.

Laser spectroscopy of highly charged ions at the storage ring CSRe: Schottky-based spectroscopic investigation and XUV fluorescence detector development

Laser spectroscopy stands out as a powerful tool to investigate atomic and nuclear properties and also test fundamental theories by precisely measuring the energy levels in highly charged ions. In this work, the fine-structure splitting 1s22s2S1/2−1s22p2P1/2 transition in lithium-like 16O5+ has been investigated in a laser spectroscopy experiment at the heavy-ion storage ring CSRe. The excitation resonance of the tunable narrowband UV laser and the ions was observed using a Schottky resonator with very high sensitivity. The experimental uncertainties including the ion beam velocity determination, the space charge effects, laser wavelength calibration, and angular misalignment between the laser and ion beam were analyzed, and the 2S1/2−2P1/2 transition wavelength was determined to be λ0= 103.45(38) nm. The primary source of experimental uncertainty arises from the inaccurate measurement of the high voltage applied on the electron cooler and therewith the ion beam velocity at the CSRe. In order to solve this problem, a high-precision divider to precisely measure the high-voltage of the electron cooler is under construction, which is expected to improve the present experimental accuracy by three orders of magnitude. In addition, an XUV optical detector equipped with an off-axis parabolic mirror has been developed and installed at the CSRe for the investigation of slow dipole-forbidden transitions in highly charged ions, such as hyperfine splitting and M1 transitions. The experimental studies presented here pave the way for future laser spectroscopy experiments at the CSRe as well as at the future larger-scale scientific facility HIAF in China.

High-efficiency narrow-bandwidth KTP optical parametric oscillator for kHz-MHz planar laser-induced fluorescence.

The electronic excitation of key combustion species or flow tagging of chemical species requires a narrowband tunable UV source. In this work, a potassium titanyl phosphate (KTP) burst-mode optical parametric oscillator (OPO) pumped by a 532 nm laser is developed to generate a spectrally narrow signal and an idler output with 1.48 ± 0.19 cm-1 bandwidth without the need for injection seeding. The idler (1410-1550 nm range) is further mixed with 355 or 266 nm to generate 284 or 226 nm for OH or NO planar laser-induced fluorescence (PLIF), respectively, with up to 1.9% conversion efficiency from 1064 nm to the UV. MHz-rate burst profiles are reported, and OH and NO PLIF are demonstrated in a rotating detonation combustor at rates up to 200 kHz.

Physical Trace Gas Identification with the Photo Electron Ionization Spectrometer (PEIS).

Chemosensor technology for trace gases in the air always aims to identify these compounds and then measure their concentrations. For identification, traceable methods are sparse and relate to large appliances such as mass spectrometers. We present a new method that uses the alternative traceable measurement of the ionization energies of trace gases in a way that can be miniaturized and energetically tuned. We investigate the achievable performance. Since tunable UV sources are not available for photoionization, we take a detour via impact ionization with electrons, which we generate using the photoelectric effect and bring to sharp, defined energies on a nanoscale in the air. Electron impact ionization is thus possible at air pressures of up to 900 hPa. The sensitivity of the process reaches 1 ppm and is equivalent to that of classic PID. With sharpened energy settings, substance identification is currently possible with an accuracy of 30 meV. We can largely explain the experimental observations with the known quantum mechanical models.

UV Laser-Induced Photodecomposition of Matrix-Isolated Salicylhydroxamic Acid: Identification of New Isocyanate Complexes.

Photochemical reactions of salicylhydroxamic acid were induced using tunable UV laser radiation followed by FTIR spectroscopy. Four pairs of co-products were experimentally found to appear in the photolysis: C6H4(OH)NCO⋯H2O (1), C6H4(OH)C(O)N⋯H2O (2), C6H4(OH)2⋯HNCO (3), and C6H4(OH)NHOH⋯CO (4). The comparison of the theoretical spectra with the experimental ones allowed us to determine the structures of the complexes formed in the matrices. The mechanisms of the reaction channels leading to the formation of the photoproducts were proposed. It was concluded that the first step in the formation of the complexes (1), (2), and (3) was the scission of the N-O bond, whereas the creation of complex (4) was due to cleavage of the C-N bond.

Tunable UV Laser for External Seeding of the High Repetition Rate Soft X-ray Free Electron Laser FLASH

We are currently developing a tunable high-repetition rate femtosecond UV laser system for external seeding superconducting soft X-ray Free Electron Laser FLASH. Initial results show excellent power and wavelength stability of the Optical Parametric Chirped Pulse Amplification system.

Nonlinear post-compression of a hybrid vortex mode in a gas-filled capillary.

We demonstrate nonlinear temporal compression of a vortex beam by propagation in a gas-filled capillary. Starting from an ytterbium-based laser delivering 700 μJ 640 fs pulses at a 100 kHz repetition rate, the vortex beam is generated using a spiral phase plate and coupled to a capillary where it excites a set of four modes that have an overlap integral of 97% with a Laguerre-Gauss LG10 mode. Nonlinear propagation of this hybrid, orbital angular momentum (OAM)-carrying mode results in temporal compression down to 74 fs at the output. Beam and pulse characterizations are carried out to determine the spatial profile and temporal duration of compressed pulses. This result in multimode nonlinear optics paves the way towards the generation of OAM-carrying few-cycle pulses, isolated attosecond XUV pulses, and tunable UV pulses through resonant dispersive wave emission.

High-energy acousto-optic Q-switched alexandrite laser with wavelength tunable fundamental and UV second harmonic generation

We investigate high-energy mJ-class diode-pumped acousto-optic (AO) Q-switched alexandrite lasers with broad tunability at both the fundamental near-IR wavelength range and second harmonic generation (SHG) in the UV wavelength range. An AO Q-switched alexandrite laser with continuous-wave diode-pumping has been operated at up to 10 kHz and producing pulse energy of 700 µJ at repetition rate of 1 kHz. With pulsed double-pass diode-pumping, we demonstrate higher pulse energy of 2.6 mJ. With wavelength tuning, this laser system demonstrated broad fundamental tuning range from 719 to 787 nm with diffraction-limited beam quality (M2 = 1.05). By external cavity second harmonic generation in a Type-I LBO crystal, pulse energy of 0.66 mJ is generated at 375 nm and with UV tuning range from 361 to 391 nm. To our knowledge, this is the first demonstration of AO Q-switched alexandrite laser with broad wavelength tuning in the near-IR and UV wavelength ranges and shows its excellent potential as a pulsed source for future applications.

XUV Fluorescence Detection of Laser-Cooled Stored Relativistic Ions

An improved moveable in vacuo XUV fluorescence detection system was employed for the laser cooling of bunched relativistic (β = 0.47) carbon ions at the Experimental Storage Ring (ESR) of GSI Helmholtzzentrum Darmstadt, Germany. Strongly Doppler boosted XUV fluorescence (∼90 nm) was emitted from the ions in a forward light cone after laser excitation of the 2s–2p transition (∼155 nm) by a new tunable pulsed UV laser system (257 nm). It was shown that the detected fluorescence strongly depends on the position of the detector around the bunched ion beam and on the delay (∼ns) between the ion bunches and the laser pulses. In addition, the fluorescence information could be directly combined with the revolution frequencies of the ions (and their longitudinal momentum spread), which were recorded using the Schottky resonator at the ESR. These fluorescence detection features are required for future laser cooling experiments at highly relativistic energies (up to γ∼ 13) and high intensities (up to 1011 particles) of ion beams in the new heavy ion synchrotron SIS100 at FAIR.

Pulsed-ramped-field-ionisation zero-kinetic-energy photoelectron spectroscopy of the metastable rare-gas atoms Ar, Kr and Xe.

The photoionisation of the metastable rare-gas atoms Rg = Ar, Kr and Xe is investigated at the Rg+ […](ns)2(np)5 2P3/2 ← Rg[…](ns)2(np)5((n + 1)s) 13P2 photoionisation threshold (n = 3, 4 and 5 for Ar, Kr and Xe) using the technique of pulsed-ramped-field-ionisation zero-kinetic-energy (PRFI-ZEKE) photoelectron spectroscopy. This technique, which monitors the field ionisation of high Rydberg states induced by a slowly growing electric-field ramp after a prepulse of opposite polarity, was recently introduced to record photoelectron spectra with high resolution and high sensitivity [Harper, Chen, Boyé-Péronne and Gans, Phys. Chem. Chem. Phys., 2022, 117, 9353]. A tunable UV laser system with a bandwidth of 30 MHz is used here to establish the factors determining the resolution and overall accuracy of this new method. In particular, the effects of stray electric fields, and of the magnitude of the prepulse and the field ramp on PRFI-ZEKE photoelectron spectra are studied by combining experiments with numerical simulations of the field-ionisation of high Rydberg states and of the electron flight times from the ionisation spot to the detector. A spectral resolution of 0.05 cm-1 is demonstrated in the photoelectron spectrum of metastable Ar.

Highly efficient and tunable broadband UV excitable Ba9Lu2Si6O24:Eu2+, Mn2+ single-phase white-light-emitting phosphors

Based on crystal site engineering, a series of inorganic Ba9Lu2Si6O24: Eu2+ (BLSO: Eu2+) and Ba9Lu2Si6O24:Eu2+, Mn2+ phosphors were synthesized. These phosphors exhibit broad emission throughout the whole visible spectrum range. More specifically, a systematic cation substitution favored efficient energy transfer. Hence, the produced Ba9Lu2−zSczSi6O24: 0.2Eu2+, 0.4Mn2+ (BLSSO: 0.2Eu2+, 0.4Mn4+) were effective single-phase white-light-emitting phosphors. Particularly, Ba9Lu2Si6O24: Eu2+ phosphors emit a broadband blue emission peaking at 462 nm with a long tail. The results of the emission spectrum's Gaussian fitting (and deconvolution), low-temperature photoluminescence, and decay time observations point to the existence of many luminescence centers in the host lattice of BLSO. Partial cation substitution favors the occupation of Eu2+ ions in other available crystallographic sites, i.e., Ba(2) and Ba(3), resulting in the emission spectrum broadening in the green spectral region. The energy transfer from the doped Eu2+ to the co-doped Mn2+ ions broadens the emission in the red spectral region (618 nm). Accordingly, the broadband emission covers the entire visible spectral region. Furthermore, the make-up of these phosphors provides a powerful method for obtaining continuous tuning throughout the whole visible spectrum. The above features, in conjunction with the color coordinates and the remarkable thermal stability, qualify the optimized Ba9Lu2−zSczSi6O24: 0.2Eu2+, 0.4Mn2+ phosphor for potential use in single-phase white-light-emitting phosphors.

2D material inorganic liquid crystals for tunable deep UV light modulation.

2D material inorganic liquid crystals for tunable deep UV light modulation.

Single frequency tunable UV laser at 308 nm based on all-fiberized master oscillator power amplifiers.

A tunable narrow linewidth UV laser near 308 nm is necessary for highly sensitive hydroxyl (OH) radical measurement. We demonstrated a high-power fiber-based single frequency tunable pulsed UV laser at 308 nm. The UV output is generated from the sum frequency of a 515 nm fiber laser and a 768 nm fiber laser, which are harmonic generations from our proprietary high-peak-power silicate glass Yb- and Er-doped fiber amplifiers. A 3.50 W single frequency UV laser with 100.8 kHz pulse repetition rate, 3.6 ns pulse width, 34.7 µJ pulse energy, and 9.6 kW peak power has been achieved, which represents the first demonstration, to the best of our knowledge, of a high-power fiber-based 308 nm UV laser. With temperature control of the single frequency distributed feedback seed laser, the UV output is tunable for up to 792 GHz at 308 nm.

(Invited) Imaging and Measuring Electronic Materials

Photoemission (PES) has been an essential metrology in the field of materials physics for over 30 years. The electronic band structure of a solid is a fundamental property which defines how a material will be used and integrated into device form. Topographic features and defects can impact electronic structure, therefore influence extrinsic properties when integrated in device form. Developing metrology that is sensitive to electronic properties at these length scales is desired. Here, we apply lab-based photoemission electron microscopy (PEEM) to gain insight in key structure – function relationships.Controlling doping during growth of semiconductors is critical as it has impact on device engineering – whether to form components in logical circuits or regions for Ohmic contact formation. For some semiconductor nanowires (NW), the doping density is varied along the long axis of the NW and knowing where the transition and its strength between doping regimes is important for device engineers. Here, we have imaged GaN NW grown with n-doped and n++-doped regions of approximately 6 μm in length and 200 nm in diameter that have been dispersed on a silicon substrate. Using a deep ultraviolet photon source, we observe an inflected change in the contrast along the long axis of the NWs (about 2 μm from one end) which we attribute to the n-n++ interface. This inflection is about 100 nm wide, and provides insight into the space-charge region formed at this electronic interface.We will also present on expanding our lab-based PEEM capability with integration to a tunable laser-based deep UV system (80 MHz, 140 fs). This added capability will provide additional imaging sensitivity to polar semiconductors such as III-nitrides. We will present some initial results with this system currently being commissioned on device-grade GaN and β-Ga2O3.

Nonresonant Multiphoton Ionization of Stark Decelerated Molecules by Femtosecond Laser Pulses

Nonresonant multiphoton ionization by femtosecond laser pulses can be applied to any molecule virtually, thereby greatly enhancing the scope of Stark decelerated molecules. For comparison, we detect decelerated and trapped ammonia molecules using two different schemes: (i) nonresonant multiphoton ionization using intense femtosecond (fs) pulses in the near infrared, and (ii) resonance-enhanced multiphoton ionization using nanosecond (ns) pulses from a tunable UV laser. The observed number of ions per shot for both schemes is similar. The fs laser detection scheme suffers from an increased background, which can be effectively eliminated by subsequent mass and velocity selection. To determine the detection volume of the ns laser detection scheme, we present measurements in which the decelerated ammonia molecules are bunched to a packet with a longitudinal spread well below ∼100 μm. It is concluded that the detection volume for the ns laser detection scheme is 1.5–2 times larger than that of the fs laser detection scheme.

β-Ga2O3 Nanostructures: Chemical Vapor Deposition Growth Using Thermally Dewetted Au Nanoparticles as Catalyst and Characterization.

β-Ga2O3 nanostructures, including nanowires (NWs), nanosheets (NSHs), and nanorods (NRs), were synthesized using thermally dewetted Au nanoparticles as catalyst in a chemical vapor deposition process. The morphology of the as-grown β-Ga2O3 nanostructures depends strongly on the growth temperature and time. Successful growth of β-Ga2O3 NWs with lengths of 7–25 μm, NSHs, and NRs was achieved. It has been demonstrated that the vapor–liquid–solid mechanism governs the NW growth, and the vapor–solid mechanism occurs in the growth of NSHs and NRs. The X-ray diffraction analysis showed that the as-grown nanostructures were highly pure single-phase β-Ga2O3. The bandgap of the β-Ga2O3 nanostructures was determined to lie in the range of 4.68–4.74 eV. Characteristic Raman peaks were observed with a small blue and red shift, both of 1–3 cm−1, as compared with those from the bulk, indicating the presence of internal strain and defects in the as-grown β-Ga2O3 nanostructures. Strong photoluminescence emission in the UV-blue spectral region was obtained in the β-Ga2O3 nanostructures, regardless of their morphology. The UV (374–377 nm) emission is due to the intrinsic radiative recombination of self-trapped excitons present at the band edge. The strong blue (404–490 nm) emissions, consisting of five bands, are attributed to the presence of the complex defect states in the donor (VO) and acceptor (VGa or VGa–O). These β-Ga2O3 nanostructures are expected to have potential applications in optoelectronic devices such as tunable UV–Vis photodetectors.

Photoionization, Structures, and Energetics of Na-Doped Formic Acid-Water Clusters.

The influence of formic acid on water cluster aggregation has been investigated experimentally by mass spectrometry and tunable UV laser ionization applied to Na‐doped clusters formed in the supersonic expansion of water vapors seeded with formic acid (FA) as well as theoretically using high level quantum chemistry methods. The mass spectra of Na−FA(H2O)n clusters show an enlarging of mass distribution toward heavier clusters with respect to the Na−(H2O)n clusters, suggesting similar mass distribution in neutral clusters and an influence of formic acid in water aggregation. Density functional theory and coupled‐cluster type (DLPNO‐CCSD(T)) calculations have been used to calculate structures and energetics of neutral and ionized Na−FA(H2O)n as well as neutral FA(H2O)n. Na‐doped clusters are characterized by very stable geometries. The theoretical adiabatic ionization potential values match pretty well the measured appearance energies and the calculated first six electronic excited states show Rydberg‐type characters, indicating possible autoionization contributions in the mass spectra. Finally, theoretical calculations on neutral FA(H2O)n clusters show the possibility of similarly stable structures in small clusters containing up to n=4–5 water molecules, where FA interacts significantly with waters. This suggests that FA can compete with water molecules in the starting stage of the aggregation process, by forming stable nucleation seed.

Photooxidation of tetrahydrobiopterin as the basis of vitiligo phototherapy

The kinetics of photooxidation of tetrahydrobiopterin was investigated, the quantum yields of the formation of dihydropterin dimers were calculated when using a xenon lamp, a tunable UV laser and a UV LED as UV radiation sources. A comparative analysis of the effectiveness of these sources for the photooxidation process of tetrahydrobiopterin allowed us to conclude that the most effective for the purposes of vitiligo phototherapy are, apparently, UV LED sources with emission maxima in the region of 325 nm. Keywords: vitiligo, tetrahydrobiopterin, melanin, oxidative stress, H2O2, UVB vitiligo phototherapy.