High-performance frequency stabilization of ultraviolet diode lasers by using dichroic atomic vapor spectroscopy and transfer cavity

We develop a high-performance ultraviolet(UV)frequency stabilization technique implemented directly on UV diode lasers by combining the dichroic atomic vapor laser lock and the resonant transfer cavity lock.As an example,we demonstrate a stable locking with measured frequency standard deviations of approximately 200 kHz and 300 kHz for 399 nm and 370 nm diode lasers in 20 min.We achieve a long-term frequency drift of no more than 1 MHz for the target 370 nm laser within an hour,which is further verified with fluorescence count rates of a single trapped ^171Yb+ion.We also find strong linear correlations between lock points and environmental factors such as temperature and atmospheric pressure.Our approach provides a simple and stable solution at a relatively low cost,and features flexible control,high feedback bandwidth and minimal power consumption of the target UV laser.

Diode-pumped high-power continuous-wave intracavity frequency-doubled Pr^(3+):YLF ultraviolet lasers around 349 nm

High-power continuous-wave ultraviolet lasers are useful for many applications.As ultraviolet laser sources,the wavelength switching capability and compact structure are very important to extend the applicability and improve the flexibility in practical applications.In this work,we present two simple and relatively compact schemes by laser diode pumping to obtain a watt-level single-wavelength 348.7-nm laser and discrete wavelength tunable ultraviolet lasers around 349 nm(from 334.7 to 364.5 nm)by intracavity frequency doubling based on Pr^(3+):YLF andβ-BBO crystals.The maximum output power of the single-wavelength 348.7-nm laser is 1.033 W.The output powers of the discrete wavelength tunable lasers are at the level of tens of milliwatts,except for two peaks at 348.7 and 360.3 nm with output powers of approximately 500 mW.In addition,simulations are carried out to explain the experimental results and clarify the tuning mechanisms.

High-power ultraviolet 278-nm laser from fourth-harmonic generation of an Nd：YAG amplifier in CsB3O5 crystal

We report on the experimental investigation and theoretical analysis of a nanosecond pulse high power ultraviolet（UV） 278 nm laser by fourth-harmonic generation（FHG） of a 1112-nm Nd：YAG amplifier in LiB3O5（LBO） and CsB3O5（CBO） crystals. The UV laser delivers a maximum average power of 10.3 W at 278 nm with peak power of 36.8 k W under input pump power of 41 W at 556 nm. This is, to the best of our knowledge, the highest output power at the specific UV wavelength of 278 nm. We also performed the theoretical investigation on the FHG with a model in the Gaussian approximation of both spatial and temporal profiles, especially accounting for the two-photon absorption effect in CBO crystal for the first time. The average output power, pulse width, and beam spatial distribution of the UV laser were simulated. The theoretical calculations are in close agreement with the experimental results.

Vacuum Ultraviolet Free-Electron Laser Photoionization Mass Spectrometry of Alpha-pinene Ozonolysis

α-pinene is the most abundant monoterpene that represents an important family of volatile organic compounds.Molecular identification of key transient compounds during theα-pinene ozonolysis has been proven to be a challenging experimental target because of a large number of intermediates and products involved.Here we exploit the recently developed hybrid instruments that integrate aerosol mass spectrometry with a vacuum ultraviolet free-electron laser to study theα-pinene ozonolysis.The experiments ofα-pinene ozonolysis are performed in an indoor smog chamber,with reactor having a volume of 2 m^(3) which is made of fluorinated ethylene propylene film.Distinct mass spectral peaks provide direct experimental signatures of previously unseen compounds produced from the reaction ofα-pinene with O_(3).With the aid of quantum chemical calculations,plausible mechanisms for the formation of these new compounds are proposed.These findings provide crucial information on fundamental understanding of the initial steps ofα-pinene oxidation and the subsequent processes of new particle formation.

Infrared Spectroscopy of Neutral Clusters Based on a Vacuum Ultraviolet Free Electron Laseri

Spectroscopic characterization of clusters is crucial to understanding the structures and reaction mechanisms at the microscopic level,but it has been proven to be a grand challenge for neutral clusters because the absence of a charge makes it di伍cult for the size selection and detection.Infrared(IR)spectroscopy based on threshold photoionization using a tunable vacuum ultraviolet free electron laser(VUV-FEL)has recently been developed in the lab.The IR-VUV depletion and IR+VUV enhancement spectroscopic techniques open new avenues for size-selected IR spectroscopies of a large variety of neutral clusters without confinement(i.e.,an ultraviolet chromophore,a messenger tag,or a host matrix).The spectroscopic principles have been demonstrated by investigations of some neutral water clusters and some metal carbonyls.Here,the spectroscopic principles and their applications for neutral clusters are reviewed.

Ionization and Dissociation of Benzene and Aniline under Deep Ultraviolet Laser Irradiation

We report a study on photo-ionization of benzene and aniline with incidental subsequent dissociation by the customized reflection time-of-flight mass spectrometer utilizing a deep ultraviolet 177.3 nm laser.Highly efficient ionization of benzene is observed with a weak C4H3+fragment formed by undergoing disproportional C-C bond dissociation.In comparison,a major C5H6+·fragment and a minor C6H6+·radical are produced in the ionization of aniline pertaining to the removal of CNH·and NH·radicals,respectively.First-principles calculation is employed to reveal the photo-dissociation pathways of these two molecules having a structural difference of just an amino group.It is demonstrated that hydrogen atom transfer plays an important role in the cleavage of C-C or C-N bonds in benzene and aniline ions.This study is helpful to understand the underlying mechanisms of chemical bond fracture of benzene ring and related aromatic molecules.

Ultraviolet laser ionization studies of 1-fluoronaphthalene clusters and density functional theory calculations

This paper studies supersonic jet-cooled 1-fluoronaphthalene （1FN） clusters by ultraviolet （UV） laser ionization at 281 nm in a time-of-flight mass spectrometer. The （1FN）＋ （n=1-3） series cluster ions are observed where the signal intensity decreases with increasing cluster size. The effects of sample inlet pressures and ionization laser fluxes to mass spectral distribution are measured. Using density functional theory calculations, it obtains a planar geometric structure of 1FN dimer which is combined through two hydrogen bonds. The mass spectra indicate that the intensity of 1FN trimer is much weaker than that of 1FN dimer and this feature is attributed to the fact that the dimer may form the first ＂shell＂ in geometric structure while the larger clusters are generated based on this fundamental unit.

Photoreflectance system based on vacuum ultraviolet laser at 177.3 nm

Photoreflectance(PR)spectroscopy is a powerful and non-destructive experimental technique to explore interband transitions of semiconductors.In most PR systems,the photon energy of the pumping beam is usually chosen to be higher than the bandgap energy of the sample.To the best of our knowledge,the highest energy of pumping laser in reported PR systems is 5.08 eV(244 nm),not yet in the vacuum ultraviolet(VUV)region.In this work,we report the design and construction of a PR system pumped by VUV laser of 7.0 eV(177.3 nm).At the same time,dual-modulated technique is applied and a dual channel lock-in-amplifier is integrated into the system for efficient PR measurement.The system’s performance is verified by the PR spectroscopy measurement of well-studied semiconductors,which testifies its ability to probe critical-point energies of the electronic band in semiconductors from ultraviolet to near-infrared spectral region.

Increase in functional groups for POSS by introducing branched phenylglycidylether

In the selected experimental conditions, firstly, the branched products with functional groups, N-（2-hydroxylpropylphenylether） （3-aminopropyl） triethoxysilane （APES-PGE, containing one hydroxyl group） and N-[di（2-hydroxylpropylphenylether）]（3-aminopropyl） triethoxysilane （APES-PGE2, containing two hydroxyl groups）, were synthesized by reacting 1 mole of （3-aminopropyl）triethoxysilane （APES） with 2 mole of phenylglycidylether （PGE）. Then the hydrolytic condensation of APES-PGE and APES-PGE2 was performed by dissolving 1 g of the corresponding silane in 1.5 ml tetrahydrofuran （THF）, adding water and eventually a catalyst （molar ratios: [H2O]/Si=3, [NaOH]/Si=0.05）, and heating at 50 ℃ for 24 h, allowing continuous evaporation of volatiles. The final products with branches containing hydroxyl groups were polyhedral oligomeric silsesquioxanes （POSS）. The products from two reactions were characterized by standard spectroscopic techniques, gel partition chromatography （GPC）, Fourier-transformed infrared spectroscopy （FTIR） and matrix-assisted ultraviolet laser desorption/ionization time-of-flight mass spectrometry （UV-MALDI-TOF MS）. Additionally, a narrow mass distribution of multifunctionalized POSS was shown by UV-MALDI-TOF MS and assignments of the MS peaks.

Cascaded third-harmonic-generation converter based on a single ADP crystal

Based on a specially designed optical structure, an efficient cascaded third-harmonic-generation（THG） output of a 1064-nm, pico-seconds pulse laser is successively realized by using an NH_4H_2PO_4（ADP） crystal that acts as the secondharmonic-generation component and sum-frequency-generation component. The maximum THG output is 1.61 mJ, and the highest conversion efficiency from 1064 nm to 355 nm reaches 35%, which are obviously superior to the results obtained using a KDP crystal under the same circumstance. The further phase-matching analysis indicates that this THG configuration of ADP crystal can be applied to various fundamental wavelengths in a range of 1 μm–1.1 μm. Compared with the previously reported KDP THG converter, which is based on a similar principle, the present ADP THG converter is favorable for large-energy, high-efficiency operation because of the larger effective nonlinear optical coefficient deffand higher laser damage threshold.

Electron localization of H_2^+ in a dc electric field

A dc electric field is utilized to steer the electron motion after the molecular ion H2-＋ is excited by an ultrashort ultraviolet laser pulse. The numerical simulation shows that the electron localization distribution and the dissociation control ratio are dependent on the polarization direction and amplitude of the dc electric field. Most electrons of the dissociation state move opposite to the dc electric field and stabilize at the dressed-up potential well, for the dressed-down well is occupied by the electrons of the 1 sσg state.

Electron localization of linear symmetric molecular ion H3-(2＋)

Electron localization in the dissociation of the symmetric linear molecular ion H3-（2＋） is investigated. The numerical simulation shows that the electron localization distribution is dependent on the central frequency and peak electric field amplitude of the external ultrashort ultraviolet laser pulse. When the electrons of the ground state are excited onto the 2pσ-2Σu-＋ by a one-photon process, most electrons of the dissociation states are localized at the protons on both sides symmetrically. Almost no electron is stabilized at the middle proton due to the odd symmetry of the wave function. With the increase of the frequency of the external ultraviolet laser pulse, the electron localization ratio of the middle proton increases, for more electrons of the ground state are excited onto the higher 3pσ-2Σu-＋ ustate. 50.9% electrons of all the dissociation events can be captured by the middle Coulomb potential well through optimizing the central frequency and peak electric field amplitude of the ultraviolet laser pulse. Besides, a direct current（DC） electric field can be utilized to control the electron motions of the dissociation states after the excitation of an ultraviolet laser pulse, and 68.8% electrons of the dissociation states can be controlled into the middle proton.

Studies of Laser-induced-MOCVDZinc Oxide Films

hin films of ZnO were prepared using the double photobeams ultraviolet laserinduced-metallorganic chemical vapour deposition (MOCVD)technique. The struc-ture and transparent photoconductive properties of these films were investigated us-ing X-ray diffraction (XRD) , reflecting electron diffraction (RED) .scanning elec-tron microscopy (SEM) and ultraviolet visible absorption spectrometry (UV) .Theexperiments showed that the technique produced superior quality films of polycrys-tal ZnO_(1-x) (the O-vacancies in the ZnO lattice) , and possessed higher depositionrate, lower growth temperature conipared with CVD or MOCVD technique and thethin films had far better transparent photoconductive properties than tliose grownby the conventional CVD or MOCVD technique.

Fabrication of room temperature continuous-wave operation GaN-based ultraviolet laser diodes

Two kinds of continuous-wave GaN-based ultraviolet laser diodes（LDs） operated at room temperature and with different emission wavelengths are demonstrated.The LDs epitaxial layers are grown on GaN substrate by metalorganic chemical vapor deposition,with a 10 × 600 μm^2 ridge waveguide structure.The electrical and optical characteristics of the ultraviolet LDs are investigated under direct-current injection at room temperature.The stimulated emission peak wavelength of first LD is 392.9 nm,the threshold current density and voltage is 1.5kA/cm^2 and 5.0 V,respectively.The output light power is 80 mW under the 4.0 kA/cm^2 injection current density.The stimulated emission peak wavelength of second LD is 381.9 nm,the threshold current density the voltage is2.8 kA/cm^2 and 5.5 V,respectively.The output light power is 14 mW under a 4.0 kA/cm^2 injection current density.

Ultraviolet laser photolysis of hydrocarbons for nondiamond carbon suppression in chemical vapor deposition of diamond films

In this work,we demonstrate that ultraviolet(UV)laser photolysis of hydrocarbon species alters the flame chemistry such that it promotes the diamond growth rate and film quality.Optical emission spectroscopy and laser-induced fluorescence demonstrate that direct UV laser irradiation of a diamond-forming combustion flame produces a large amount of reactive species that play critical roles in diamond growth,thereby leading to enhanced diamond growth.The diamond growth rate is more than doubled,and diamond quality is improved by 4.2%.Investigation of the diamond nucleation process suggests that the diamond nucleation time is significantly shortened and nondiamond carbon accumulation is greatly suppressed with UV laser irradiation of the combustion flame in a laser-parallel-to-substrate geometry.A narrow amorphous carbon transition zone,averaging 4 nm in thickness,is identified at the film–substrate interface area using transmission electron microscopy,confirming the suppression effect of UV laser irradiation on nondiamond carbon formation.The discovery of the advantages of UV photochemistry in diamond growth is of great significance for vastly improving the synthesis of a broad range of technically important materials.

In-situ generation and global property profiling of metal nanoclusters by ultraviolet laser dissociation-mass spectrometry

Metal nanoclusters are promising nanomaterials with unique properties, but only a few ones with specific numbers of metal atoms can be obtained and studied up to now. In this study, we establish a new paradigm of in-situ generation and global study of metal nanoclusters with different sizes, constitutions, and charge states, including both accurate constitution characterization and global activity profiling. The complex mixtures of metal nanoclusters are produced by employing single-pulsed 193-nm laser dissociation of monolayer-protected cluster(MPC) precursors within a high-resolution mass spectrometry(HRMS). More than400 types of bare gold nanoclusters including novel multiply charged(2+ and 3+), S-/P-doped, and silver alloy ones can be efficiently generated and accurately characterized. A distinct size(1 to 142 atoms)-and charge(1+ to 3+)-hierarchy reactivity is clearly observed for the first time. This global cluster study might greatly promote the developments and applications of novel metal nanoclusters.

Advances in deep ultraviolet laser based high-resolution photoemission spectroscopy

We briefly review recent results on photoemission spectroscopy based on the deep and vacuum ultraviolet diode pumped solid-state lasers which we have developed.Cascaded second harmonic generation with the nonlinear crystal KBe2BO3F2(KBBF)is used to generate deep ultraviolet and vacuum ultraviolet laser radiation,which complements traditional incoherent light sources such as gas discharge lamps and synchrotron radiation,and has greatly improved resolution with respect to energy,momentum,and spin of photoemission spectroscopy.Many new functions have been developed with the advantages of high photon energy,narrow linewidth,high photon flux density,and so on.These have led to the observation of various new phenomena and the amassment of new data in the fields of high temperature superconductivity,topological electronics,Fermi semi-metals,and so forth.These laser systems have revived the field of photoemission spectroscopy and provided a new platform in this frontier research field.

Micropatterning of Superhydrophobic Silicone Nanofilaments by a Near-Ultraviolet Nd:YAG Laser

We demonstrate that a recently developed coating composed of superhydrophobic silicone nanofilaments can be selectively functionalized to yield well defined micron-scale patterns of contrasting wettabilities(superhydrophobic/hydrophilic and amphiphobic/amphiphilic).Nanofilament ablation was performed using a near-ultraviolet(UV)laser with a wavelength of 355 nm and a repetition rate of 10 kHz.This is a highly promising approach for open channel microfluidics and microarray analysis due to its simplicity,the chemical and environmental stability of the coating,and the low cost.

High-energy,high-repetition-rate ultraviolet pulses from an efficiency-enhanced,frequency-tripled laser

In this study,a high-energy,temporally shaped picosecond ultraviolet(UV)laser running at 100 Hz is demonstrated,with its pulses boosted to 120 mJ by cascaded regenerative and double-pass amplifiers,resulting in a gain of more than 10^(8).With precise manipulation and optimization,the amplified laser pulses were flat-top in the temporal and spatial domains to maintain high filling factors,which significantly improved the conversion efficiency of the subsequent third harmonic generation(THG).Finally,91 mJ,470 ps pulses were obtained at 355 nm,corresponding to a conversion efficiency as high as 76%,which,as far as we are aware of,is the highest THG efficiency for a high-repetition-rate picosecond laser.In addition,the energy stability of the UV laser is better than 1.07%(root mean square),which makes this laser an attractive source for a variety of fields including laser conditioning and micro-fabrication.

Frequency stabilization of a 214.5-nm ultraviolet laser

An improved method for stabilizing a frequency-quadrupled 214.5-nm tunable diode laser system is re- ported. Improvements to the method include a homemade logic circuit and the use of a Fabry-Perot optical spectrum analyzer as a transfer cavity. Lasers locked with this method exhibit megahertz-level frequency stability measured with an optical frequency comb referenced to a cesium atomic standard. The laser can be locked for hours to days, depending on experiment requirements. Being relatively inexpensive, stable, and robust, the control method can be applied to stabilizing essentially all lasers of deep ultraviolet wavelengths.