High-harmonic Generation in Metallic Titanium Nitride

Improved performance of Free Electron Laser (FEL) light sources in terms of timing stability, pulse shape and spectral properties of the amplified FEL pulses is of interest in many fields of science. A promising scheme is direct seeding with High-Harmonic Generation (HHG) in a noble gas target. A Free-Electron-Laser seeded by an external XUV-source is planned for FLASH II at DESY in Hamburg. The requirements for the XUV/soft X-ray source can be summarized as follows: A repetition rate of at least 100 kHz in a 10 Hz burst is needed at variable wavelengths from 10 to 40 nm and pulse energies of several nJ within single harmonics. This application requires a laser amplifier system with exceptional parameters, mJ-level pulse energy, sub-10 fs pulse duration at 100 kHz (1 MHz) burst repetition rate. A new OPCPA system is under development in order to meet these requirements, and very promising results has been achieved. In parallel to this development, a new High- Harmonic Generation concept is necessary to sustain the high average power of the driving laser system and for the need of high conversion efficiencies. Highest conversion efficiency in High Harmonic Generation has been shown using gas-filled capillary targets, up to now. For our application, only a free-jet target is applicable for high harmonic generation at high repetition rate, to overcome damage threshold limitations of HHG target optics. A new multi-jet target is under development and first tests show a good performance of this nozzle configuration.

Separating the infrared driving laser from the extreme ultraviolet (XUV) pulses after high-order harmonic generation has been a long-standing difficulty. In this Letter, we propose and demonstrate that the driving laser can be blocked by simply installing a microchannel plate (MCP) into the beam line. In addition to its high damage threshold, the MCP filter also transmits photons over the entire XUV region. This paves the way for attosecond pulse generation with unprecedented bandwidth.

Coherent extreme ultraviolet (XUV) radiation produced by table-top high-harmonic generation (HHG) sources provides a wealth of possibilities in research areas ranging from attosecond physics to high resolution coherent imaging. However, it remains challenging to fully exploit the coherence of such sources for interferometry and Fourier transform spectroscopy (FTS). This is due to the need for a measurement system that is stable at the level of a wavelength fraction, yet allowing a controlled scanning of time delays. Here we demonstrate XUV interferometry and FTS in the 17-55 nm wavelength range using an ultrastable common-path interferometer suitable for high-intensity laser pulses that drive the HHG process. This approach enables the generation of fully coherent XUV pulse pairs with sub-attosecond timing variation, tunable time delay and a clean Gaussian spatial mode profile. We demonstrate the capabilities of our XUV interferometer by performing spatially resolved FTS on a thin film composed of titanium and silicon nitride.

Processing of AC-coupled n-in-p pixel detectors on MCz silicon using atomic layer deposited aluminium oxide

Nonlinear optical (NLO) crystal is one of the important opt-electrical functional materials that can convert laser frequency and obtain wide band tunable coherent sources, thus it possesses crucial strategic and application value in military and civil fields. On the basis of more than 30 years' efforts, the NLO crystals in visible and near infrared region, including -BaB2O4 LiB3O5 and KTiOPO4, have been basically mature. However, there are still many shortcomings for those NLO crystals used in deep ultraviolet (DUV) and mid/far-infrared (IR) regions, thus putting forward more requirements for high performance crystals. For DUV KBe2BO3F2 (KBBF) crystals, the main shortcomings are the use of toxic BeO raw materials and strong layer growth tendency. Wide transparent region and high second harmonic generation (SHG) effect are also expected in new developed DUV NLO crystals. More importantly, a large enough birefringence is highlighted to satisfy the phase-matchable condition and DUV harmonic generation capacity below 200 nm. On the other hand, the main requirement for mid/far-infrared NLO crystals is to maintain the balance between high laser damage threshold and strong SHG response. Indeed, it is a very difficult task to search for good NLO crystals through the traditional trial and error experimental methods. Theoretical studies, especially first principles calculations, can provide an efficient way to investigate and design new NLO materials with superior properties. In this paper, the recent progress of deep-UV and mid-IR NLO crystals is summarized. In addition, the crucial role of first principles calculations in new material exploration and design is highlighted by introducing several typical new NLO crystals, including defect diamond-like compound AgZnPS4, trigonal alkaline metal fluorooxoborate KB4O6F and alkaline earth fluorooxoborate SrB5O7F3. Moreover, some advanced analysis tools are introduced, such as real space atomic cutting method, SHG-weighted mapping, flexible dipole moment model, and non-bonding atomic orbitals analysis, and used to investigate the structure-property relationship in langasite La3SnGa5O14, metal cyanurate Ca3(C3N3O3)2, vanadium-carbonate K3[V(O2)2O]CO3, etc. Further, the flow chart of high-throughput first principles calculations of NLO crystal is proposed. According to the known or predicted crystal structure, we can obtain the chemical stability, band gap, NLO coefficient, birefringence and phase-matchable capacity quickly, thus easily judging the research potential of a new NLO material. On the basis of these ideas, a great blueprint for NLO crystal material genome engineering is highly put forward. Finally, the difficulties in research and challenges in NLO material investigations are discussed, and the direction of future research priorities based on first principles calculations are pointed out.

Metal nitrides have been proposed to replace noble metals in plasmonics for some specific applications. In particular, while titanium nitride (TiN) and zirconium nitride (ZrN) possess localized plasmon resonances very similar to gold in magnitude and wavelength, they benefit from a much higher sustainability to temperature. For this reason, they are foreseen as ideal candidates for applications in nanoplasmonics that require high material temperature under operation, such as heat assisted magnetic recording (HAMR) or thermophotovoltaics. This article presents a detailed investigation of the plasmonic properties of TiN and ZrN nanoparticles in comparison with gold nanoparticles, as a function of the nanoparticle morphology. As a main result, metal nitrides are shown to be poor near-field enhancers compared to gold, no matter the nanoparticle morphology and wavelength. The best efficiencies of metal nitrides as compared to gold in term of near-field enhancement are obtained for small and spherical nanoparticles, and they do not exceed 60%. Nanoparticle enlargements or asymmetries are detrimental. These results mitigate the utility of metal nitrides for high-temperature applications such as HAMR, despite their high temperature sustainability. Nevertheless, at resonance, metal nitrides behave as efficient nanosources of heat and could be relevant for applications in thermoplasmonics, where heat generation is not detrimental but desired.

This study reports a pulsed laser deposition-assisted synthesis of highly metallic titanium nitride (TiN) and a series of semiconducting titanium oxynitride (TiNxOy) compounds in thin film form with tunable plasmonic properties by carefully altering the nitrogen (N)-oxygen (O) ratio. The N/O ratio was controlled from 0.3 (highest oxygen doping of TiN) to ~ 1.0 (no oxygen doping of TiN) by growing the TiN films under nitrogen pressures of 50, 35, and 10 mTorr and high vacuum conditions of 2 × 10−6 Torr with no external gas introduced. The presence of nitrogen in the deposition chamber during the film growth affects the gas phase oxidation of TiN to TiNxOy by increasing the mean free path-dependent N and O inter-collisions per second by two to three orders of magnitudes. The evidence of increased oxidation of TiN to TiNxOy with an increase in nitrogen deposition pressure was obtained using X-ray photoelectron spectroscopy analysis. While the TiN samples deposited in high vacuum conditions had the highest reflectance, TiNxOy thin films were also found to possess high reflectance at low frequency with a well-defined edge around 20,000 cm−1. Furthermore, the vacuum-deposited TiN samples showed a large negative dielectric constant of -330 and the largest frequency of zero-crossing at 25,000 cm−1; the TiNxOy samples deposited in the presence of nitrogen ambient also showed promising plasmonic applications at the near-mid infrared range. A comparison of the dielectric constant and loss function data of this research with the literature values for noble metals seems to indicate that TiN and TiNxOy have the potential to replace gold and silver in the visible and near-infrared spectral regions.

Metasurfaces, introduced as a compact 2D alternative of metamaterials, have developed into a vast field in recent times for light manipulation at an ultra-compact scale. Metasurface applications have found a place in the literature for compact alternatives to lens, holograms, polarizers, color filters. Plasmonic metasurfaces consisting of noble metals such as gold and silver provide light confinement on an unprecedented scale. Gold and silver grown conventionally on transparent substrates are polycrystalline, and exhibit losses and limit performance of the device. Moreover, these materials have a lower damage threshold and melting point. To circumvent the lower melting point and damage thresholds, new materials, and material growing techniques need to be researched. <br>In the first part of this work, a metasurface for color holography with an epitaxially grown silver thin film on a transparent substrate is shown. The demonstrated metasurface has been the first ever epitaxial silver metasurface that operated in the transmission mode. This plasmonic hologram has also been the thinnest metasurface hologram operating in transmission mode at the time of its reporting. The holographic image of all three basic color components of red, green, and blue has been demonstrated in the transmission mode. The control of color has been achieved by resonant sub-wavelength slits and the phase can be manipulated through altering slit orientation. This amplitude and phase control pave the way to applications of ultra-compact polychromatic plasmonic metasurfaces for advanced light manipulation. In the second part, we explore temperature rise due to the optical absorption in plasmonic structures. Titanium Nitride based metasurfaces structures are fabricated, that work in harsh environmental conditions and high temperature. A time domain thermo reflectance technique for rapid measurement of temperature is explored. Finally, a practical design prototype for thermo-photovoltaic (TPV) emitters using plasmonic metasurfaces is fabricated and characterized.<br><br>

Titanium nitride (TiN) has been identified as a promising refractory material for high temperature plasmonic applications such as surface plasmon polaritons (SPPs) waveguides, lasers and light sources, and near field optics. Such SPPs are sensitive not only to the highly metallic nature of the TiN, but also to its low loss. We have formed highly metallic, low-loss TiN thin films on MgO substrates to create SPPs with resonances between 775-825 nm. Scanning near-field optical microscopy (SNOM) allowed imaging of the SPP fringes, the accurate determination of the effective wavelength of the SPP modes, and propagation lengths greater than 10 microns. Further, we show the engineering of the band structure of the plasmonic modes in TiN in the mid-IR regime and experimentally demonstrate, for the first time, the ability of TiN to support Spoof Surface Plasmon Polaritons in the mid-IR (6 microns wavelength).

Advances in alternative plasmonic materials, specifically CMOS-­-compatible materials including refractory transition metal nitrides and transparent conducting oxides (TCOs), have propelled a new generation of nanophotonic devices for applications in on-­-chip optics, data storage, and energy conversion. As a plasmonic component, gold (Au) or silver (Ag) have some of drawbacks such as difficulty in fabricating ultrathin films, incompatibility with well-­-established processes for silicon-­-based products and lack of tunability, preventing them to be realized as practical devices in the telecommunication range. One potential transition metal nitride is titanium nitride (TiN), with a permittivity cross-­-over near 500 nm. TiN can attain ultra-­-thin, ultra-­-smooth epitaxial films on substrates such as c-­-sapphire, MgO, and silicon. Partnering TiN with CMOS-­-compatible silicon nitride enables a fully solid-­-state waveguide which is able to achieve a propagation length greater than 1 cm for a ~8 μm mode size at 1.55 μm. In fact, designs using TiN have outperformed similarly structured gold waveguides due in large part to the reduced scattering loss of epitaxial quality films.

Complex examinations were performed of the structure of films of metallic titanium, titanium nitride and titanium oxide deposited by means of PLD with a Nd:YAG laser. The influence of the deposition parameters on the film morphology was examined. The films revealed a nano-structure of good quality. A new tetragonal Ti(N) phase was revealed in the deposition of metallic titanium in a reactive chamber with an argon atmosphere. The TiN phase was formed during deposition of titanium nitride, independently of the nitrogen flow in the chamber. The transition of oxides from Ti2O via TiO to TiO2 was observed with an increasing flow of oxygen in the chamber for deposition of titanium oxide. TEM examinations of the microstructure in cross-sections of the film revealed a micro- columnar structure. All the examined films were characterised by a strong axial crystallographic preferred orientation on the basis of the measured pole figures. The axial texture was identified within the deposited metallic titanium for the Ti(N) tetragonal phase as well as for the TiO oxide, while the texture was observed in the case of TiN nitride. Measurements of the residual stresses of the first order in the TiN phase, by using the X-ray sin2ψ method, showed stress levels of -5000 to -7000 MPa. The residual stresses measured in the substrate of ferritic steel were about -150 MPa.

Transition metal nitride materials exhibit unique optical characteristics and have attracted much interest for various applications, including waveguiding, photovoltaics, and nonlinear optical devices. Herein, titanium nitride (TiN), as a typical representative of biocompatible transition metal nitrides, is prepared and modified with gold nanoclusters (Au NCs) for promoting the carrier mobility, and the corresponding physical characteristics are systematically characterized. The TiN‐based saturable absorber (SA) on microfiber is fabricated and its nonlinear optical absorption property is also studied experimentally. Furthermore, the TiN‐decorated SA is applied in an ultrafast fiber laser at the communication bands. The fiber laser can generate the stable ultrashort pulses with a pulse width of 1.66 ps, a fundamental repetition rate of 7.49 MHz, and a spectral bandwidth of 2.61 nm. More importantly, the chaotic multiple pulses can be obtained, which is reported for the first time in the fiber laser based on the TiN SA on microfiber as far as it is known. The chaotic multiple pulses show many interesting characteristics, including high average pulse energy, varying pulse separations, and pulse intensities. These results have proved that the TiN shows great potential in many fields, such as advanced optical‐intensity modulator, ultrafast pulse dynamics, and optical fiber communications.

It is well known that metal oxide films are useful as hard mask material in semiconductor industry for their excellent etch resistance against plasma etches. In the advanced lithography processes, in addition to good etch resistance, they also need to possess good wet removability, fill capability, in high aspect ratio contacts or trenches. Conventional metal containing materials can be applied by chemical vapor deposition (CVD) or atomic layer deposition (ALD). Films derived from these techniques have difficulty in controlling wet etch, have low throughput and need special equipment. This leads to high costs. Therefore it is desirable to develop simple spin-on coating materials to generate metal oxide hard masks that have good trench or via filling performances using spin track friendly processing conditions. In this report, novel spin-on type inorganic formulations providing Ti, W, Hf and Zr oxide hard masks will be described. The new materials have demonstrated high etch selectivity, good filling performances, wet removal capability, low trace metals and good shelf-life stability. These novel AZ® Spin-on metal hard mask formulations can be used in several new applications and can potentially replace any metal, metal oxide, metal nitride or silicon-containing hard mask films currently deposited using CVD process in the semiconductor manufacturing process.

This study investigates recent advances in photoelectron emission generated by irradiating ultrashort lasers on metallic nanostructures and low-dimensional carbon materials. Recently, primary focus has been on improving the efficiency of emitters, i.e. increasing the number of field-emitted electrons and their respective kinetic energies. An example of this is the modification of the conventional metal nanotip through adiabatic nanofocusing and various plasmonic metal structures, such as nanorods and bowtie antenna. The coherent emission control with two color irradiation enabled modulation in the emission yield. In addition, THz waves near the metallic nanostructure induced a highly accelerated, monochromatic energy. Alternative to metallic nanotips, carbon nanotubes are emerging as efficient photoelectron emitters, due to the large enhancement factor associated with their high aspect ratio and damage threshold. They particularly allowed the use of femtosecond light sources with a relatively short wavelength, resulting in the generation of photoelectrons with a narrow bandwidth. Additionally, electronic control over the single-walled nanotubes band structure added a degree of freedom for controlling the electron emission yield. Finally, we review the strong-field tunneling emission in graphene edge, with the emission yield showing an anomalous increase of nonlinear order, corresponding to the deep strong tunneling regime.

We report on reflection gratings produced entirely of dielectric materials. This gives the opportunity to enhance the laser damage threshold over that occurring in conventional metal gratings used for chirped-pulse-amplification, high-power lasers. The design of the system combines a dielectric mirror and a well-defined corrugated top layer to obtain optimum results. The rules that have to be considered for the design optimization are described. We optimized the parameters of a dielectric grating with a binary structure and theoretically obtained 100% reflectivity for the -1 order in the Littrow mounting for a 45 degrees angle of incidence. Subsequently we fabricated gratings by structuring a low-refractive-index top layer of a multilayer stack with electron-beam lithography. The multilayer system was fabricated by conventional sputtering techniques onto a flat fused-silica substrate. The parameters of the device were measured and controlled by light scatterometer equipment. We measured 97% diffraction efficiency in the -1 order and damage thresholds of 4.4 and 0.18 J/cm(2) with 5-ns and 1-ps laser pulses, respectively, at a wavelength of 532 nm in working conditions.