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DOE OSTI2025

Molecular Layer Deposited Aluminum‐Based Hybrid Resist for High‐Resolution Nanolithography and Direct Ultra‐High Aspect Ratio Pattern Transfer

Inorganic-containing hybrid photoresists are critical for next-generation extreme ultraviolet (EUV) lithography and angstrom-era semiconductor miniaturization. However, associated conventional solution processing struggles to achieve ultrathin, uniform films with high conformality and compositional control, limiting overall patterning performance. Here, this study reports the systematic lithographic patterning characterization of an Al-based hybrid resist synthesized via vapor-phase molecular layer deposition (MLD), using the trimethylaluminum (TMA) metal precursor and the hydroquinone (HQ) aromatic organic linker. The resist supports both sub-20 nm high-resolution nanolithography and virtually infinite silicon plasma etch selectivity. Lithographic performance studied using electron beam lithography (EBL) as a proxy for EUV shows that, under an optimized process adopting post-exposure bake, the resist achieves the best resolution of 15.4 nm linewidth under stringent 1:1 line-space high-density patterning—limited only by the minimum beam size of the EBL system. The resist also shows wide dose latitude and balanced performance in resolution, roughness, and sensitivity. The infinite silicon etch selectivity, stemming from spontaneous aluminum oxyfluoride passivation layer formation, enables fabrication of micrometer-tall, 40 nm-wide silicon nanofin structures using only a ≈30 nm-thick resist layer, without no hard mask. These results highlight the potential of MLD-based hybrid resists for developing next-generation resist materials for micro/nanoelectronics manufacturing.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Tin removal by an annular surface wave plasma antenna in an extreme ultraviolet lithography source

Tin contamination of the collector mirror surface remains one of the crucial issues of EUV (Extreme Ultraviolet) sources, directly impacting the availability of the tool. Hydrogen plasma-based tin removal processes employ hydrogen radicals and ions to interact with tin deposits to form gaseous tin hydride (SnH 4 ), which can be removed through pumping. An annular surface wave plasma (SWP) source developed at the University of Illinois—Urbana Champaign is integrated into the cone and perimeter of the collection mirror for in situ tin removal. The SWP is characterized by high ion and radical densities, low electron temperature, and local generation where etching is needed. This method has the potential to significantly reduce downtime and increase mirror lifetime. Radical probe measurements show hydrogen radical densities in the order of 10 19 m -3 , while Langmuir probe measurements show electron temperatures of up to 6 eV and plasma densities on the order of 10 17–18 m -3 . The generated ions are essential to the tin cleaning and have sufficiently low energy to cause no damage to the collector capping layer. Tin etch rates of up to 270 nm/min were observed in a variety of experimental conditions, including various powers, pressures, flowrates, and temperatures. In conclusion, the high etch rates demonstrated in this study exceed the expected contamination rate of the EUV source.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Optical design and efficiency measurement of an extreme ultraviolet high-resolution spectrometer for unresolved transition array research

Understanding the structures of the unresolved transition array (UTA) observed in extreme ultraviolet (EUV) spectra from many-electron atoms is crucial for various applications, including fusion science and nanolithography. Here, to measure the fine structure of the UTA from tungsten and tin at around 5 and 13.5 nm at the Tokyo electron beam ion trap, we developed a high-resolution EUV spectrometer. The designed spectrometer achieves a resolving power of λ/dλ > 5000 at 5 and 13.5 nm. The fabricated large-area grating was experimentally examined at beamline BL5B of the UVSOR synchrotron facility to evaluate the diffraction efficiencies and their variation across the ruled area. The measured diffraction efficiencies are 0.65% ± 0.07% at 5 nm (second order) and 7.9% ± 0.2% at 13.5 nm (first order). The variation in the diffraction efficiency across the ruled area is 2.2%, 13.6%, and 10.0% in zeroth, first, and second order diffractions, respectively. The discrepancies in diffraction efficiencies between the experiments and the calculations were 5.2%, 29%, and 35% for the zeroth, first, and second diffraction orders, respectively.

47 OTHER INSTRUMENTATION↗

DOE OSTI2021

Multiply-excited states and their contribution to opacity in CO 2 laser-driven tin-plasma conditions

A recent study (2020 Nat. Commun. 11 2334) has found that transitions between multiply-excited configurations in open 4d-subshell tin ions are the dominant contributors to intense EUV emission from dense, Nd:YAG-driven (laser wavelength λ = 1.064 μm) tin plasmas. In the present study, we employ the Los Alamos Atomic code to investigate the spectral contribution from these transitions under industrially-relevant, CO 2 laser-driven (λ = 10.6 μm) tin plasma conditions. First, we employ Busquet's ionisation temperature method to match the average charge state < Z > of a non-local-thermodynamic equilibrium (non-LTE) plasma with an LTE one. This is done by varying the temperature of the LTE calculations until a so-called ionisation temperature T Z is established. Importantly, this approach generates LTE-computed configuration populations in excellent agreement with the non-LTE populations. A corollary of this observation is that the non-LTE populations are well-described by Boltzmann-type exponential distributions having effective temperatures T eff ≈ T Z . In the second part of this work, we perform extensive level-resolved LTE opacity calculations at T Z . It is found that 66% of the opacity in the industrially-relevant 2% bandwidth centred at 13.5 nm arises from transitions between multiply-excited states. These results reinforce the need for the consideration of complex, multiply-excited states in modelling the radiative properties of laser-driven plasma sources of EUV light.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2021

Experimental inference of neutral and impurity transport in Alcator C-Mod using high-resolution x-ray and ultra-violet spectra

We present experimental inferences of cross-field impurity transport coefficients for AlcatorC-Mod plasmas without edge-localized modes, leveraging a novel forward model for the entire Ca Kα spectrum, including satellite lines within the spectral range, to compare to high-resolution x-ray imaging crystal spectroscopy (XICS). These measurements are complemented by extreme ultra-violet (EUV) spectroscopy that constrains transport closer to the edge. Using new atomic data sets for both XICS and EUV analysis has enabled consideration of line ratios across both spectral ranges and has increased the accuracy of inferred transport coefficients. Inclusion of charge exchange between edge thermal neutrals and impurities is shown to be extremely important in C-Mod pedestals. Atomic D neutral densities from experimental D Lyα measurements at the midplane are compared to SOLPS-ITER simulations, finding good agreement. Bayesian inferences of impurity transport coefficients are presented for L-, EDA H-, and I-mode discharges, making use of the Aurora package for forward modeling and combining our spectroscopic constraints. Experimentally inferred diffusion profiles are found to match turbulent transport models at midradius within uncertainties, using both quasilinear gyro-fluid TGLF SAT-1 and nonlinear ion-scale gyrokinetic CGYRO simulations. Furthermore, significant discrepancies in convection are observed in some cases, suggesting difficulties in predictions of flat or hollow impurity profiles.

neutrals↗

DOE OSTI2022

Study of the electrothermal and MHD instabilities in exploding cylindrical foil liner

Abstract An experimental and numerical study of the plasma instabilities in an electrical exploding cylindrical Al liner is reported. The Al liner 3 mm in diameter and 10 μ m in thickness is exploded at the Qin-1 facility (450 ns, 400 kA). Various diagnostics, such as multi-frame laser shadowgraphy, an x-ray framing camera, and an x-ray backlighting system are developed. The different imaging systems are sensitive to plasma of different areal densities based on the comparison between the experiments and simulation, which reveal the dynamics of the exploding liner in more detail. The laser shadow images show the low-density plasma (∼1–2 × 10 −4 g cm −2 ) at the edge of the liner, and both the amplitude and wavelength of the plasma instabilities increase over time, which are considered to be magnetohydrodynamic (MHD) instabilities rather than electrothermal instabilities. During the ablation of the liner, quasi-periodic azimuthally correlated striations are directly observed in extreme ultraviolet (EUV) self-emission images. Meanwhile, the vertical filaments, which are electrothermal instabilities for plasma under the condition of ∂ η /∂ T < 0, are also observed in EUV self-emission images. The x-ray backlighting images of the exploding liner are obtained by placing an X -pinch load on the current-return path to serve as an x-ray point source (∼1 ns, ∼10 μ m). The x-ray backlighting results show the behavior of the high-density plasma (∼1.89 × 10 −3 g cm −2 ), which includes the transition from electrothermal to MHD instabilities. Finally, we realized a 2D MHD simulation of the exploding liner under experimental conditions, which shows good agreement with the results of the experimental perturbation.

Physics↗

DOE OSTI2024

Towards Full Field-of-View Fourier Ptychography for Extreme Ultraviolet Microscope

We evaluate various Fourier ptychographic microscopy (FPM) reconstruction algorithms using both simulated and experimental data acquired from an Extreme Ultraviolet (EUV, 13.5 nm wavelength) microscope. We specifically focus on the algorithms' ability to robustly address field-dependent aberrations, which enables increased spatial resolution and quantitative phase imaging across an expanded field of view. We systematically compare the algorithms' performance under aberrations for a single zoneplate imaging system, utilizing Fourier Ring Correlation (FRC) as a systematic metric for assessing reconstruction quality. Furthermore, we explore the impact of systematic errors on the reconstruction of experimental data, aiming to increase the effective field of view by 25-fold, from the nominal 5x5 um2 diffraction-limited area. Additionally, our evaluation incorporates innovative FPM-adjacent methodologies, including the Angular Ptychographic Imaging with Closed-form method (APIC), for reconstructing EUV images.

Gu, Chaoying↗

DOE OSTI2020

Study of a linear surface wave plasma source for tin removal in an extreme ultraviolet source

Tin deposition mitigation employs hydrogen radicals and ions, formed in a hydrogen plasma, to interact with tin to form tin hydride (SnH 4 ) in the gaseous state, which is then pumped away. Surface wave plasma (SWP) technology developed at Illinois generates hydrogen radicals and ions, resulting in tin etch rates that are high enough to keep extreme ultraviolet (EUV) lithographic tools clean. An advantage of an SWP antenna is the ability to generate a high density of hydrogen radicals and hydrogen ions directly at the desired etching location. In situ etching of tin enables high availability EUV tools by maintaining high reflectivity of the multilayer mirror of the collector. Additionally, the SWP is characterized with low ion energies and low electron temperature, such that the multilayer mirror does not suffer any damage from sputtering or implantation of hydrogen ions during operation. Here, experiments elucidating the fundamental processes of tin removal are conducted by varying pressure, power, surface temperature, and gas flow rate in order to observe the etch rate behavior. Our results have shown that the presence of hydrogen ions increases etch rates because ion bombardment weakens Sn–Sn bonds, which, in turn, allows for a higher rate of chemical etching by the radicals. The ion bombardment reduces the number of radicals needed to etch a single tin atom to the range of 10 2 –10 3 . The linear SWP antenna yields plasma densities on the order of 10 17 to 10 18 m -3 and radical densities on the order of 10 18 to 10 19 m -3 , allowing for greater utilization of ion etch enhancement. Etch rates of up to 200 nm/min have been achieved. The surface temperature of the samples is an important factor in the etching process such that the decrease in the surface temperature increases the etch rates and decreases the hydrogen desorption rates. In addition, a kinetic etch model is developed to explain the behavior of etch rates as a function of surface temperature. Furthermore, results from experiments performed in an Illinois NXE:3100 chamber will be discussed.

42 ENGINEERING↗

DOE OSTI2024

Realizing Steady-State Microbunching with Optical Stochastic Crystallization

Optical Stochastic Cooling (OSC) is a state-of-the-art beam cooling technology first demonstrated in 2021 at the IOTA storage ring at Fermilab's FAST facility. A second phase of the research program is planned to run in early 2025 and will incorporate an optical amplifier to enable significantly increased cooling rates and greater operational flexibility. In addition to beam cooling, an OSC system can be configured to enable advanced control over the phase space of the beam. An example operational mode could enable crystallization, where the particles in a bunch are locked into a self-reinforcing, regular microstructure at the OSC fundamental wavelength; we refer to this as Optical Stochastic Crystallization (OSX). OSX represents a new path toward Steady-State Microbunching (SSMB), which may enable light sources combining the high brightness of a free-electron laser with the high repetition rate of a storage ring. Such a source has applications from the terahertz to the extreme ultraviolet (EUV), including high-power EUV generation for semiconductor lithography. This contribution will discuss the status of the OSC experimental program and its potential to achieve the first demonstration of SSMB during the upcoming experimental run.

Wallbank, M.↗

DOE OSTI2024

Unlocking the Sun's Secrets: Laboratory Insights into the Sun's Outer Atmosphere

The Sun’s corona, its outermost and hottest atmospheric layer, emits brightly in the extreme ultraviolet (EUV) and X-rays. This emission comes from atoms that have been highly ionized by the high temperature, forming a plasma of atomic ions and free electrons. By studying this light, scientists learn about the complex and dynamic drivers of solar activity. Many past, current, and future solar observatories focus on measuring EUV spectra from the Fe IX ion, as this ion provides powerful diagnostics for solar physics. Using Fe IX spectra, solar physicists can measure the plasma temperature, density, elemental abundances, and flow velocities in the corona. However, atomic data uncertainties concerning spectral line identification and plasma density diagnostics are a major problem for the accurate interpretation of these spectra.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2025

Realizing Steady-State Microbunching with Optical Stochastic Crystallization

Optical Stochastic Cooling (OSC) is a state-of-the-art beam cooling technology first demonstrated in 2021 at the IOTA storage ring at Fermilab's FAST facility. A second phase of the research program is planned to run in 2026 and will incorporate an optical amplifier to enable significantly increased cooling rates and greater operational flexibility. In addition to beam cooling, an OSC system can be configured to enable advanced control over the phase space of the beam. An example operational mode could enable crystallization, where the particles in a bunch are locked into a self-reinforcing, regular microstructure at the OSC fundamental wavelength; we refer to this as Optical Stochastic Crystallization (OSX). OSX represents a new path toward Steady-State Microbunching (SSMB), which may enable light sources combining the high brightness of a free-electron laser with the high repetition rate of a storage ring. Such a source has applications from the terahertz to the extreme ultraviolet (EUV), including high-power EUV generation for semiconductor lithography. This contribution will discuss the integration of OSX development as part of the OSC program at IOTA. The design of an accelerator lattice to enable the mechanism and associated high fidelity simulations will be shown, and a path to realizing an experimental demonstration will be discussed.

Wallbank, Michael James [Fermilab]↗

DOE OSTI2025

Steady-State Microbunching using Optical Stochastic Cooling

Optical Stochastic Cooling (OSC) is a state-of-the-art beam cooling technology first demonstrated in 2021 at the IOTA storage ring at Fermilab's FAST facility. A second phase of the research program is planned to run in 2026 and will incorporate an optical amplifier to enable significantly increased cooling rates and greater operational flexibility. In addition to beam cooling, an OSC system can be configured to enable advanced control over the phase space of the beam. An example operational mode could enable crystallization, where the particles in a bunch are locked into a self-reinforcing, regular microstructure at the OSC fundamental wavelength; we refer to this as Optical Stochastic Crystallization (OSX). OSX represents a new path toward Steady-State Microbunching (SSMB), which may enable light sources combining the high brightness of a free-electron laser with the high repetition rate of a storage ring. Such a source has applications from the terahertz to the extreme ultraviolet (EUV), including high-power EUV generation for semiconductor lithography. This contribution will discuss the integration of OSX development as part of the OSC program at IOTA. The design of an accelerator lattice to enable the mechanism and associated high fidelity simulations demonstrating the beam dynamics will be shown, and a path to realizing an experimental demonstration will be discussed.

Wallbank, Michael James [Fermilab]↗

DOE OSTI2022

The Energetics of the Central Engine in the Powerful Quasar 3C 298

The compact steep-spectrum radio source 3C 298 (redshift of 1.44) has the largest 178 MHz luminosity in the Third Cambridge Revised Catalogue (3CR); its radio lobes are among the most luminous in the universe. The plasma state of the radio lobes is modeled with the aid of interferometric radio observations (in particular, the new Low Frequency Array observation and archival MERLIN data) and archival single-station data. It is estimated that the long-term time-averaged jet power required to fill these lobes with leptonic plasma is $\overline{Q}\,\approx 1.28\pm 0.51\times {10}^{47}\,\mathrm{erg}\,{{\rm{s}}}^{-1}$, rivaling the largest time-averaged jet powers from any quasar. Supporting this notion of extraordinary jet power is a 0.5–10 keV luminosity of ≈ 5.2 × 10 46 erg s –1 , comparable to luminous blazars, yet there is no other indication of strong relativistic beaming. We combine two new high signal-to-noise ratio optical spectroscopic observations from the Hobby-Eberly Telescope with archival Hubble Space Telescope, Two Micron All Sky Survey, and Galaxy Evolutionary Explorer data to compute a bolometric luminosity from the accretion flow of L bol ≈ 1.55 ± 0.15 × 10 47 erg s –1 . The ratio, $\overline{Q}/{L}_{\mathrm{bol}}\approx 1$, is the approximate upper limit for quasars. Characteristic of a large $\overline{Q}/{L}_{\mathrm{bol}}$, we find an extreme-ultraviolet (EUV) spectrum that is very steep (the "EUV deficit" of powerful radio quasars relative to radio-quiet quasars), and this weak ionizing continuum is likely a contributing factor to the relatively small equivalent widths of the broad emission lines in this quasar.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2026

Energy Evolution from the Chromosphere to the Heliosphere in the 2021 October 28 Solar Eruption

We perform a detailed study of the energetics for a well-observed solar eruption and flare that occurred on 2021 October 28. This event included a GOES class X1.0 flare, a global extreme-UV (EUV) wave, and a coronal mass ejection (CME) that reached speeds of >2000 km s −1 . The event was observed from a variety of spacecraft in NASA’s Heliophysics System Observatory, including multiple missions near Earth, STEREO-A off the Sun-Earth line, and Solar Orbiter, near the Sun-Earth line at about 0.8 au. Using remote sensing, in situ observations, and in some cases scaling laws based on previous observations, we characterize the following quantities: free magnetic energy, energy in nonthermal electrons, energy in nonthermal ions, bolometric energy, energy deposited in the chromosphere, thermal energy radiated in the flare loops, energy dissipated by the EUV wave, CME kinetic and gravitational potential energy, CME energy flux in the heliosphere, and the energy partition in the CME shock. We find that the total energy released during the event is consistent with estimates of the pre-event stored magnetic energy, and the CME kinetic + potential energy dominates the energy partition.

solar coronal mass ejection shocks↗

DOE OSTI2024

Realizing Steady-State Microbunching with Optical Stochastic Crystallization

43 PARTICLE ACCELERATORS↗

DOE OSTI2025

Initial Stage of Nanoscale Imaging in Positive Tone Extreme UV Photoresists: The Influence of the Polymer Sequence

Photolithographic patterning using extreme ultraviolet (EUV, 92.5 eV) light is a radiolytic process that initially forms electrons, radical cations, anions, and neutral radicals in the polymeric photoresist matrix. These species may participate in the chemical reactions that define the ultimate resolution of the printed image, and their concentrations and nanometer-scale stochastic variations in their formation influence printed image quality. Proposals have been made that polymer chain uniformity may be advantageous in reducing stochastics due to spatial inhomogeneities, and this aspect of radiolysis is examined in this work. We have simulated the initial subpicosecond stages of the imaging process for a series of photoresist films that are identical in composition but vary in their polymer chain structures. We use detailed, physically accurate stochastic reaction-diffusion calculations to evaluate the influence of defined sequence and random copolymer structures on radiolytic spur formation, i.e., a cluster of species formed by electron-polymer interactions that defines the initial spatial characteristic of the imaging process. Predictions of electron thermalization in the present work are shown to be consistent with the literature, indicating that our overall computational approach for ultrafast nanoscale processes is sound. The computational results show that the polymer sequence has no significant effect on the spur composition. This suggests that any potential imaging improvements to be gained by sequence control must originate from postimaging lithographic process steps.

Absorption↗

DOE OSTI2020

Infiltration synthesis of hybrid nanocomposite resists for advanced nanolithography

In this work, we demonstrate a simple ex-situ inorganic infiltration route for transforming standard organic resists into highperformance positive tone hybrid resist platform. A model thin film PMMA-AlOx hybrid resist system has been synthesized by hybridization of PMMA with AlOx and investigated for electron beam lithography. The approach possesses full controllability of the resist performance in terms of critical does, patterning contrast reaching up to 30 and etch resistance for plasma-based pattern transfer processes. The high selectivity Si etching capability demonstrated using a lowtemperature cryo-Si etch process, based on the controlled infiltration outperforms commercial resists and typical hard mask material thermal SiO 2 , with estimated achievable selectivity in excess of ~300. Si nanostructures down to ~30 nm with aspect ratio up to ~17 are also transferred into the Si substrate. Easy implementation and adaptability for different inorganic infiltrations, this platform is well capable of potentially delivering the resist performance and throughput necessary for EUV lithography.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2022

Atomic structure considerations for the low-temperature opacity of Xenon

Here, we have begun a preliminary investigation into the opacity of Xe at low temperatures (<50 eV). The emissivity and opacity of Xe is a crucial factor in determining the utility of Xe in EUV lithography, with numerous industrial applications. To this end, we have been exploring the accuracy of some approximations used in opacity models for the relevant ion stages of Xe (6 times ionized through 20 times ionized). Due to the complexity of Xe atomic structure, one needs to use full configuration-interaction to properly describe the strong mixing in the various n=4 sub-shells that give rise to the Δn=0 and Δn=1 transitions that dominate the opacity spectrum at low temperatures. Since calculations that include full configuration-interaction for large numbers of configurations quickly become computationally prohibitive, we have explored hybrid calculations, in which full configuration-interaction is retained for the most important transitions, while intermediate coupling is employed for all other transitions. After verifying atomic structure properties, local-thermodynamic-equilibrium (LTE) opacities are generated using the ATOMIC code at selected temperatures and densities and compared to various experimental results.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗