Microdroplet-tin plasma sources of EUV radiation driven by solid-state-lasers (Topical Review)

Plasma produced from molten-tin microdroplets generates extreme ultraviolet light for state-of-the-art nanolithography. Currently, CO2 lasers are used to drive the plasma. In the future, solid-state mid-infrared lasers may instead be used to efficiently pump the plasma. Such laser systems have promise to be more compact, better scalable, and have higher wall-plug efficiency. In this Topical Review, we present recent findings made at the Advanced Research Center for Nanolithography (ARCNL) on using 1 and 2 μm wavelength solid-state lasers for tin target preparation and for driving hot and dense plasma. The ARCNL research ranges from advanced laser development, studies of fluid dynamic response of droplets to impact, radiation-hydrodynamics calculations of, e.g. ion 'debris', (EUV) spectroscopic studies of tin laser-produced-plasma as well as high-conversion efficiency operation of 2 μm wavelength driven plasma

Characterization of 1- and 2-mu m-wavelength laser-produced microdroplet-tin plasma for generating extreme-ultraviolet light

Experimental spectroscopic studies are presented, in a 5.5-25.5 nm extreme-ultraviolet (EUV) wavelength range, of the light emitted from plasma produced by the irradiation of tin microdroplets by 5-ns-pulsed, 2-mu m-wavelength laser light. Emission spectra are compared to those obtained from plasma driven by 1-mu m-wavelength laser light over a range of laser intensities spanning approximately (0.3-5) x 10(11) W/cm(2), under otherwise identical conditions. Over this range of drive laser intensities, we find that similar spectra and underlying plasma charge state distributions are obtained when keeping the ratio of 1- to 2-mu m laser intensities fixed at a value of 2.1(6), which is in good agreement with RALEF-2D radiation-hydrodynamic simulations. Our experimental findings, supported by the simulations, indicate an approximately inversely proportional scaling similar to lambda(-1) of the relevant plasma electron density, and of the aforementioned required drive laser intensities, with drive laser wavelength lambda. This scaling also extends to the optical depth that is captured in the observed changes in spectra over a range of droplet diameters spanning 16-51 mu m at a constant laser intensity that maximizes the emission in a 2% bandwidth around 13.5 nm relative to the total spectral energy, the bandwidth relevant for EUV lithography. The significant improvement of the spectral performance of the 2-mu m- versus 1-mu m driven plasma provides strong motivation for the development of high-power, high-energy near-infrared lasers to enable the development of more efficient and powerful sources of EUV light

High-energy ions from Nd:YAG laser ablation of tin microdroplets:Comparison between experiment and a single-fluid hydrodynamic model

We present the results of a joint experimental and theoretical study of plasma expansion arising from Nd:YAG laser ablation (laser wavelength λ = 1.064 μm) of tin microdroplets in the context of extreme ultraviolet lithography. Measurements of the ion energy distribution reveal a near-plateau in the distribution for kinetic energies in the range 0.03-1 keV and a peak near 2 keV followed by a sharp fall-off in the distribution for energies above 2 keV. Charge-state resolved measurements attribute this peak to the existence of peaks centered near 2 keV in the Sn3+-Sn8+ ion energy distributions. To better understand the physical processes governing the shape of the ion energy distribution, we have modelled the laser-droplet interaction and subsequent plasma expansion using two-dimensional radiation hydrodynamic simulations. We find excellent agreement between the simulated ion energy distribution and the measurements both in terms of the shape of the distribution and the absolute number of detected ions. We attribute a peak in the distribution near 2 keV to a quasi-spherical expanding shell formed at early times in the expansion

Characterization of angularly resolved EUV emission from 2-μm-wavelength laser-driven Sn plasmas using preformed liquid disk targets

The emission properties of tin plasmas, produced by the irradiation of preformed liquid tin targets by several-ns-long 2 µm-wavelength laser pulses, are studied in the extreme ultraviolet (EUV) regime. In a two-pulse scheme, a pre-pulse laser is first used to deform tin microdroplets into thin, extended disks before the main (2 µm) pulse creates the EUV-emitting plasma. Irradiating 30- to 300 µm-diameter targets with 2 µm laser pulses, we find that the efficiency in creating EUV light around 13.5 nm follows the fraction of laser light that overlaps with the target. Next, the effects of a change in 2 µm drive laser intensity (0.6–1.8 × 1011 W cm−2) and pulse duration (3.7–7.4 ns) are studied. It is found that the angular dependence of the emission of light within a 2% bandwidth around 13.5 nm and within the backward 2π hemisphere around the incoming laser beam is almost independent of intensity and duration of the 2 µm drive laser. With increasing target diameter, the emission in this 2% bandwidth becomes increasingly anisotropic, with a greater fraction of light being emitted into the hemisphere of the incoming laser beam. For direct comparison, a similar set of experiments is performed with a 1 µm-wavelength drive laser. Emission spectra, recorded in a 5.5–25.5 nm wavelength range, show significant self-absorption of light around 13.5 nm in the 1 µm case, while in the 2 µm case only an opacity-related broadening of the spectral feature at 13.5 nm is observed. This work demonstrates the enhanced capabilities and performance of 2 µm-driven plasmas produced from disk targets when compared to 1 µm-driven plasmas, providing strong motivation for the use of 2 µm lasers as drive lasers in future high-power sources of EUV light

EUV spectroscopy of Sn5+-Sn(10+)ions in an electron beam ion trap and laser-produced plasmas

Emission spectra from multiply-charged Sn5+ –Sn10+ions are recorded from an electron beam ion trap (EBIT) and from laser-produced plasma (LPP) in the extreme ultraviolet range relevant for nanolithographic applications. Features in the wavelength regime between 12.6 and 20.8 nm are studied. Using the Cowan code, emission line features of the charge-state-resolved Sn ion spectra obtained from the EBIT are identified. Emission features from tin LPP either from a liquid micro-droplet or planar solid target are subsequently identified and assigned to specific charge states using the EBIT data. For the planar solid tin target, the 4d–5p transitions of Sn8+ –Sn10+ions are shown to dominate the long-wavelength part of the measured spectrum and transitions of type 4d–4f + 4p–4d are visible in absorption. For the droplet target case, a clear increase in the charge state distribution with increasing laser intensity is observed. This qualitatively demonstrates the potential of using long-wavelength out-of-band emission features to probe the charge states contributing to the strong unresolved transition array at 13.5 nm relevant for nanolithography

Titanium-45 as a candidate for PET imaging: production, processing & applications

Introduction The 80kD glycoprotein transferrin (TF) and its related receptor (TFR1) play a major role in the recruitment by cancer cells of factors for their multiplication, adhesion, invasion and metastatic potential. Though primarily designed to bind iron and then be internalised into cells with its receptor, TF can also bind most transition metals such as Co, Cr, Mn, Zr, Ni, Cu, V, In & Ga. Under certain conditions TF binds Ti (IV) even more tightly than it does Fe and that this occurs at the N-lobe (as distinct from C) of apoTF. Further, under physiological conditions the species Fe(C)Ti(N)-TF may provide the route for Ti entry into cells via TFR1 (1). Thus, the radiometal PET reporter isotope 45Ti with an ‘intermediate’ (~hrs) half-life suited to tracking cell-focused biological mechanisms is an attractive option for elucidating cellular mechanisms involving TF binding and internalisation, at least in (preclinical) animal models. 45Ti (T½ = 3.08 hr; + branching ratio = 85 %; mean β+ energy = 439keV, no significant dose-conferring non-511keV γ-emissions) was produced using the reaction 45Sc(p,n)45Ti by irradiating (monoisotopic) scandium discs with an energy-degraded proton beam produced by an 18MeV isochronous medical cyclotron. Separation and purification was achieved with an hydroxylamine hydrochloride functionalised resin. Comparative microPET imaging was performed in an immunodeficient mouse model, measuring biodistributions of the radiolabels 45Ti-oxalate and 45Ti-human-TF (45Ti-h-TF), out to 6hr post-injection. Materials and Methods High purity 15mm diameter scandium disc foils (99.5%, Goodfellow, UK) each thickness 0.100 ± 0.005 mm (55 mg) were loaded into an in-house constructed solid-targetry system mounted on a 300mm external beam line utilising helium-gas and chilled water to cool the target body (2). The proton beam was degraded to 11.7 MeV using a graphite disc integrated into the graphite collimator. This energy abolishes the competing ‘contaminant’ reactions 45Sc(p,n+p)44Sc and 45Sc(p,2n)44Ti. Beam current was measured using the well documented 65Cu(p,n)65Zn reaction. Calculations showed that the chosen energy is close to the optimal primary energy (~12 MeV) for maximising the (thin-target) yield from a 0.100 mm thick target. For separation of Ti from the Sc target two methods were examined; (i) ion exchange column separation using 2000 mg AG 50W-X8 resin conditioned with 10mL 9M HCl. Disc is dissolved in 1 mL of 9M HCl, which at completion of reaction is pipetted into column. Successive 1 mL volumes of 9M HCl are added, and subsequent elutions collected. (ii) Following Gagnon et al., (3) a method employing hydroxylamine hydro-chloride functionalised resin (’hydroxamate method’) was applied, similar to its use in our hands for purification and separation of 89Zr (2) following its original description for 89Zr by Holland et al., (4). Disc dissolved in 2mL 6M HCl, then diluted to 2M. Elute through column to waste fraction 1 (w1 – see FIG. 1). Then elute 6 mL of 2M HCl through column to w2, followed by 6 mL of traceSELECT H2O to w3. Finally, elute Ti into successive 1 mL product fractions (p1, 2 etc.) using 5 mL of 1M oxalic acid. This procedure takes approximate 1 hr. 45Ti in elution vials was measured using γ-spectroscopy. Sc in the same vials was determined later using ICP-MS. Results A typical production run using a beam current of 40 μA for 60min on a 0.100mm-thick disc produced an activity of 1.83 GBq. Radionuclidic analysis of an irradiated disc using calibrated cryo-HPGe γ-spectroscopy revealed T½ = 2.97–3.19 hr (95% CI) for 45Ti, and with contaminant 44Sc < 0.19 %, with no other isotopes detected. Despite systematic adjustments to column conditions satisfactory chemical separation was not achieved using the ion exchange column method (i), despite previous reports of its success (5). Typical results of separation using the successful hydroxamate method (ii) are shown on the FIGURE 1. It is seen that significant portion of 45Ti is lost in the initial washing steps leading to waste collection. N = 4 replicate experiments showed a variation (SD) of 10 % of the mean in each elu-tion fraction. Subsequent ICP-MS of the same elutions for (cold) Sc showed approximately 80 % by mass appeared in w1 and 20 % in w2, with negligible total mass (total fraction ~1/6000) of Sc in product (p1–4) vials. However, the FIG. 1 shows that a total of only 30% of the original activity of 45Ti (corrected to EOB) is available in the product vials, with the vial of highest specific activity (p1) containing 14 %. However, using a stack of 2×0.100mm thick Sc discs as a target yields isotope of adequate specific activity with-out need for concentration, for subsequent labelling and small-animal imaging purposes. In a ‘proof-of-principle’ experiment, two groups of healthy Balb/c-nu/nu female adult mice were administered with 45Ti radiotracers. The first group (N = 3) received approximately 20 MBq IP of 45Ti-oxalate buffered to pH = 7.0, and under-went microPET/CT imaging (Super Argus PET, Sedecal, Spain) out to 6hr post-injection, plus biodistribution analysis of radioactivity by dis-section at sacrifice (6hr). The second group (N = 3) received approximately 20 MBq IP of 45Ti-h-TF and were also studied to 6hr post-injection, followed by radioactive analysis after dissection at sacrifice. Organ and tissue biodistributions of the two groups at 6hr were similar but with 45Ti-oxalate showing slightly greater affinity for bone. Biodistribution by dissection results broadly confirmed the findings from PET images. However, TLC results suggested that similarity of radiolabel biodistributions of the two groups may be due to contamination of the TF radiolabel with non-conjugated Ti at time of injection. An alternative explanation is dechelation in vivo of 45Ti from 45Ti-h-TF. Conclusion Despite significant loss of 45Ti to the waste fractions of the separation process (total 53 %, corrected to EOB), 45Ti of acceptable specific activity and high radionuclidic purity has been produced from the reaction 45Sc(p,n)45Ti, with separation and purification of the product by hydroxamate column chemistry, confirming an earlier report. Though microPET in vivo imaging using 45Ti-based radiolabels was shown to be feasible, the similarity in the results for the label 45Ti-h-TF compared with ‘raw’ 45Ti-oxalate suggests further investigations. These may include a direct comparison of in vivo 45Ti-h-TF small-animal imaging plus post-dissection biodistribution with the same procedures using 89Zr labelled h-apotransferrin (6)

Convergence of bark investment according to fire and climate structures ecosystem vulnerability to future change

Fire regimes in savannas and forests are changing over much of the world. Anticipating the impact of these changes requires understanding how plants are adapted to fire. Here we test whether fire imposes a broad selective force on a key fire-tolerance trait, bark thickness, across 572 tree species distributed worldwide. We show that investment in thick bark is a pervasive adaptation in frequently burned areas across savannas and forests in both temperate and tropical regions where surface fires occur. Geographic variability in bark thickness is largely explained by annual burned area and precipitation seasonality. Combining environmental and species distribution data allowed us to assess the vulnerability to future climate and fire conditions: tropical rainforests are especially vulnerable, whereas seasonal forests and savannas are more robust. The strong link between fire and bark thickness provides an avenue for assessing the vulnerability of tree communities to fire and demands inclusion in global models

Radiation transport and scaling of optical depth in Nd:YAG laser-produced microdroplet-tin plasma

Experimental scaling relations of the optical depth are presented for the emission spectra of a tin-droplet-based, 1-μm-laser-produced plasma source of extreme-ultraviolet (EUV) light. The observed changes in the complex spectral emission of the plasma over a wide range of droplet diameters (16-65 μm) and laser pulse durations (5-25 ns) are accurately captured in a scaling relation featuring the optical depth of the plasma as a single, pertinent parameter. The scans were performed at a constant laser intensity of 1.4 × 1011 W/cm2, which maximizes the emission in a 2% bandwidth around 13.5 nm relative to the total spectral energy, the bandwidth relevant for industrial EUV lithography. Using a one-dimensional radiation transport model, the relative optical depth of the plasma is found to linearly increase with the droplet size with a slope that increases with the laser pulse duration. For small droplets and short laser pulses, the fraction of light emitted in the 2% bandwidth around 13.5 nm relative to the total spectral energy is shown to reach high values of more than 14%, which may enable conversion efficiencies of Nd:YAG laser light into - industrially - useful EUV radiation rivaling those of current state-of-the-art CO2-laser-driven sources