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DOE OSTI2023

A 32-channels readout ASIC for X-ray spectrometry and tracking in the GAPS experiment

Here this work describes the architecture and the experimental results from the characterization of a 32-channels mixed-signal Application-Specific Integrated Circuit (ASIC) developed for the readout of the lithium-drifted silicon, Si(Li), detectors of the General AntiParticle Spectrometer (GAPS) experiment dedicated to searching for dark matter. The instrument is designed for the identification of antiprotons, antideuterons and antihelium nuclei from cosmic rays during an Antarctic balloon mission scheduled for late 2024. A full custom integrated circuit, named SLIDER32 (32-channels Si-LI DEtector Readout) ASIC, has been produced in a commercial 180 nm CMOS technology. The ASIC is comprised of 32 low-noise analog readout channels featuring dynamic signal compression to comply with the wide input range, an 11-bit SAR ADC and a digital back-end section which is responsible for channel setting and for sending digital information to the data acquisition system (DAQ). The circuit design criteria and the experimental results are discussed in the paper.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Experimental results from the characterization of a 32-channels mixed-signal processor for the GAPS experiment

This work describes the experimental results obtained from the characterization of a 32-channels readout ASIC that is the core of a module composed by 4 Lithium-drifted Silicon, Si(Li), detectors. The module is the building block of a tracker in an upcoming balloon experiment. The activity is carried out within the General AntiParticle Spectrometer (GAPS) international collaboration, whose objective is the indirect detection of dark matter through the detection of antiparticles present in cosmic rays at low energies. The balloon flight is foreseen in 2024 from the McMurdo station in Antarctica. The ASIC is designed in a 180 nm CMOS technology and has 32 low-noise analog readout channels featuring a dynamic compression of the signal, an 11-bit SAR ADC, and a digital back-end section responsible for channel setting and for sending digital information to the data acquisition system of the tracker. This work has a twofold goal: it intends on the one hand to verify the performance of the circuit, on the other to select at least 300 good samples to be used for the assembly of the GAPS Si(Li) tracker.

Riceputi, Elisa↗
DOE OSTI2026

Long cycle and calendar life of Si-based Li-ion batteries enabled by localized high-concentration electrolytes and their surprising water tolerance

Silicon-based anodes promise an increase in energy density for Li-ion batteries, yet they suffer from a poor calendar life. Researchers have posited that fluorinated lithium salt forms reactive side products that destroy the solid electrolyte interphase (SEI), even without cycling. HF is one such reactive side product formed from trace water contamination in the electrolyte. Some electrolytes, such as localized high concentration electrolytes (LHCEs) may improve cell stability in highly reactive systems, such as Li metal and Si. In the present study, LHCEs containing 200-300 ppm of water retained up to 8% greater capacity (1200-1300 mAh/g Si) in calendar life tests over 200 days compared to dried electrolytes (< 20 ppm water). Calendar aging took place at 100% state of charge. Cells with 200-300 ppm water performed comparably to cells with 20 ppm water in cycle life tests (900-1000 mAh/g Si) . Even adding 1000 ppm water did not lead to rapid capacity fade in cells undergoing cycle life tests. Nano-FTIR spectroscopy revealed chemical and structural differences in the SEI for cells with 1000 ppm water compared to 200-300 ppm water. The SEI differences, including increased Li2O concentration, may have contributed to improved calendar life. This research reveals the capabilities of LHCEs to improve the calendar and cycle life of Si-based Li-ion batteries, despite the presence of a highly reactive contaminant.

25 ENERGY STORAGE↗
DOE OSTI2023

Electrochemical Formation of Li-M-(M')-Si Phases Using Multivalent Electrolyte Salt Additives

Lithium-rich silicides (Li 15 Si 4 ), formed during the electrochemical lithiation of silicon, show high reactivity with electrolyte components that contribute to capacity decay, formal lithium loss, and low coulombic efficiency. Recently, the reactivity of lithium silicides was found to be suppressed by substituting a multivalent cation (i.e. Mg, Ca) for lithium that results in the room temperature formation of a ternary Li-M-Si phase. In this study, we explored a range of multivalent electrolyte salt additives (M = Ni, Cu, La, Ce, Sr, Ba, and Ca-Mg mixed salt) in a lithium-ion cell configuration and identified a room temperature electrochemical route to the formation of new ternary and quaternary lithium silicides. Using this method, both nickel and copper salts were found to plate onto the silicon electrode surface upon lithiation. Further, based on refined synchrotron XRD data, multivalent cations with an ionic radius similar to Na (~1.03 Å) or smaller can be inserted electrochemically into a formally cation-deficient Li 15 Si 4 host lattice to form new ternary (or quartenary) phases. The electrochemical synthesis of a new quaternary Li-M-M’-Si phase represents a facile route to preparing and scaling materials isostructural to the Heusler phase and electron-precise Li 14 MgSi 4 phase that results in enhanced cycling and calendar life performance.

25 ENERGY STORAGE↗
DOE OSTI2020

Materials Data on Li21Si5 by Materials Project

Li21Si5 crystallizes in the cubic F-43m space group. The structure is three-dimensional. there are twelve inequivalent Li sites. In the first Li site, Li is bonded in a 3-coordinate geometry to two equivalent Li and three Si atoms. Both Li–Li bond lengths are 2.65 Å. There are a spread of Li–Si bond distances ranging from 2.62–2.85 Å. In the second Li site, Li is bonded in a distorted trigonal planar geometry to six Li and three equivalent Si atoms. There are three shorter (2.70 Å) and three longer (2.87 Å) Li–Li bond lengths. All Li–Si bond lengths are 2.72 Å. In the third Li site, Li is bonded in a 10-coordinate geometry to six Li and four Si atoms. All Li–Li bond lengths are 2.44 Å. There are one shorter (2.72 Å) and three longer (2.80 Å) Li–Si bond lengths. In the fourth Li site, Li is bonded in a 11-coordinate geometry to seven Li and four Si atoms. There are two shorter (2.65 Å) and one longer (2.67 Å) Li–Li bond lengths. There are a spread of Li–Si bond distances ranging from 2.83–2.99 Å. In the fifth Li site, Li is bonded in a distorted trigonal non-coplanar geometry to three equivalent Si atoms. All Li–Si bond lengths are 2.72 Å. In the sixth Li site, Li is bonded in a 1-coordinate geometry to three Li and three Si atoms. The Li–Li bond length is 2.69 Å. There are one shorter (2.66 Å) and two longer (2.92 Å) Li–Si bond lengths. In the seventh Li site, Li is bonded in a 3-coordinate geometry to two equivalent Li and three Si atoms. Both Li–Li bond lengths are 2.66 Å. There are one shorter (2.68 Å) and two longer (2.84 Å) Li–Si bond lengths. In the eighth Li site, Li is bonded in a 3-coordinate geometry to two equivalent Li and three Si atoms. All Li–Si bond lengths are 2.76 Å. In the ninth Li site, Li is bonded in a 3-coordinate geometry to nine Li and three equivalent Si atoms. There are three shorter (2.77 Å) and three longer (2.88 Å) Li–Li bond lengths. All Li–Si bond lengths are 2.82 Å. In the tenth Li site, Li is bonded in a 12-coordinate geometry to nine Li and three equivalent Si atoms. There are three shorter (2.65 Å) and three longer (2.90 Å) Li–Li bond lengths. All Li–Si bond lengths are 2.79 Å. In the eleventh Li site, Li is bonded in a distorted bent 150 degrees geometry to two Li and two Si atoms. There are one shorter (2.62 Å) and one longer (2.63 Å) Li–Si bond lengths. In the twelfth Li site, Li is bonded in a distorted trigonal planar geometry to three equivalent Li and three equivalent Si atoms. All Li–Si bond lengths are 2.70 Å. There are four inequivalent Si sites. In the first Si site, Si is bonded to twelve Li atoms to form distorted face-sharing SiLi12 cuboctahedra. In the second Si site, Si is bonded in a 9-coordinate geometry to thirteen Li atoms. In the third Si site, Si is bonded in a 9-coordinate geometry to thirteen Li atoms. In the fourth Si site, Si is bonded in a 10-coordinate geometry to thirteen Li atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on K7LiSi8 by Materials Project

KK6LiSi8 crystallizes in the cubic Pa-3 space group. The structure is three-dimensional and consists of four potassium molecules and one K6LiSi8 framework. In the K6LiSi8 framework, K1+ is bonded in a 6-coordinate geometry to six Si1- atoms. There are a spread of K–Si bond distances ranging from 3.41–3.52 Å. Li1+ is bonded in a distorted hexagonal planar geometry to six equivalent Si1- atoms. All Li–Si bond lengths are 2.71 Å. There are two inequivalent Si1- sites. In the first Si1- site, Si1- is bonded in a 1-coordinate geometry to four equivalent K1+, one Li1+, and three Si1- atoms. There are one shorter (2.41 Å) and two longer (2.46 Å) Si–Si bond lengths. In the second Si1- site, Si1- is bonded in a 9-coordinate geometry to six equivalent K1+ and three equivalent Si1- atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on Li13Si4 by Materials Project

Li13Si4 crystallizes in the orthorhombic Pbam space group. The structure is three-dimensional. there are seven inequivalent Li sites. In the first Li site, Li is bonded in a 3-coordinate geometry to one Li and four Si atoms. The Li–Li bond length is 2.78 Å. There are a spread of Li–Si bond distances ranging from 2.80–3.03 Å. In the second Li site, Li is bonded in a 2-coordinate geometry to six Li and five Si atoms. There are a spread of Li–Li bond distances ranging from 2.55–2.77 Å. There are a spread of Li–Si bond distances ranging from 2.71–2.93 Å. In the third Li site, Li is bonded in a 3-coordinate geometry to two equivalent Li and four Si atoms. There are a spread of Li–Si bond distances ranging from 2.66–2.89 Å. In the fourth Li site, Li is bonded in a 2-coordinate geometry to one Li and two equivalent Si atoms. There are one shorter (2.60 Å) and one longer (2.61 Å) Li–Si bond lengths. In the fifth Li site, Li is bonded in a distorted trigonal planar geometry to three Si atoms. There are two shorter (2.64 Å) and one longer (2.65 Å) Li–Si bond lengths. In the sixth Li site, Li is bonded in a 3-coordinate geometry to three Si atoms. There are one shorter (2.69 Å) and two longer (2.75 Å) Li–Si bond lengths. In the seventh Li site, Li is bonded in a linear geometry to two equivalent Li and two equivalent Si atoms. Both Li–Si bond lengths are 2.50 Å. There are two inequivalent Si sites. In the first Si site, Si is bonded in a 11-coordinate geometry to ten Li and one Si atom. The Si–Si bond length is 2.38 Å. In the second Si site, Si is bonded in a 12-coordinate geometry to twelve Li atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on SrLi2Si by Materials Project

SrLi2Si is Cyanogen Chloride-like structured and crystallizes in the orthorhombic Immm space group. The structure is zero-dimensional and consists of two strontium molecules and two Li2Si clusters. In each Li2Si cluster, Li1+ is bonded in a single-bond geometry to one Si4- atom. The Li–Si bond length is 2.45 Å. Si4- is bonded in a linear geometry to two equivalent Li1+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on BaLi2Si by Materials Project

BaLi2Si crystallizes in the orthorhombic Pmmn space group. The structure is three-dimensional. Li1+ is bonded in a trigonal planar geometry to three equivalent Si4- atoms. There are one shorter (2.69 Å) and two longer (2.78 Å) Li–Si bond lengths. Ba2+ is bonded to four equivalent Si4- atoms to form a mixture of distorted edge and corner-sharing BaSi4 tetrahedra. There are two shorter (3.46 Å) and two longer (3.61 Å) Ba–Si bond lengths. Si4- is bonded in a 10-coordinate geometry to six equivalent Li1+ and four equivalent Ba2+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on LiSiB by Materials Project

LiBSi is half-Heusler structured and crystallizes in the cubic F-43m space group. The structure is three-dimensional. Li1+ is bonded in a 6-coordinate geometry to six equivalent Si4- atoms. All Li–Si bond lengths are 2.50 Å. B3+ is bonded to four equivalent Si4- atoms to form distorted corner-sharing BSi4 tetrahedra. All B–Si bond lengths are 2.17 Å. Si4- is bonded in a distorted q6 geometry to six equivalent Li1+ and four equivalent B3+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on LiCo2Si by Materials Project

LiCo2Si is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Li1+ is bonded in a 8-coordinate geometry to eight equivalent Co+1.50+ and six equivalent Si4- atoms. All Li–Co bond lengths are 2.37 Å. All Li–Si bond lengths are 2.74 Å. Co+1.50+ is bonded in a distorted body-centered cubic geometry to four equivalent Li1+ and four equivalent Si4- atoms. All Co–Si bond lengths are 2.37 Å. Si4- is bonded in a 8-coordinate geometry to six equivalent Li1+ and eight equivalent Co+1.50+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on LiGaSi by Materials Project

LiGaSi is half-Heusler structured and crystallizes in the cubic F-43m space group. The structure is three-dimensional. Li1+ is bonded to six equivalent Si4- atoms to form distorted LiSi6 octahedra that share corners with six equivalent LiSi6 octahedra, corners with twelve equivalent GaSi4 tetrahedra, edges with twelve equivalent LiSi6 octahedra, and faces with four equivalent GaSi4 tetrahedra. The corner-sharing octahedral tilt angles are 0°. All Li–Si bond lengths are 2.94 Å. Ga3+ is bonded to four equivalent Si4- atoms to form distorted GaSi4 tetrahedra that share corners with twelve equivalent LiSi6 octahedra, corners with twelve equivalent GaSi4 tetrahedra, and faces with four equivalent LiSi6 octahedra. The corner-sharing octahedral tilt angles are 55°. All Ga–Si bond lengths are 2.55 Å. Si4- is bonded in a distorted q6 geometry to six equivalent Li1+ and four equivalent Ga3+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on LiAlSi by Materials Project

LiAlSi is half-Heusler structured and crystallizes in the cubic F-43m space group. The structure is three-dimensional. Li1+ is bonded to four equivalent Si4- atoms to form LiSi4 tetrahedra that share corners with four equivalent AlSi4 tetrahedra, corners with twelve equivalent LiSi4 tetrahedra, and edges with six equivalent AlSi4 tetrahedra. All Li–Si bond lengths are 2.57 Å. Al3+ is bonded to four equivalent Si4- atoms to form AlSi4 tetrahedra that share corners with four equivalent LiSi4 tetrahedra, corners with twelve equivalent AlSi4 tetrahedra, and edges with six equivalent LiSi4 tetrahedra. All Al–Si bond lengths are 2.57 Å. Si4- is bonded in a body-centered cubic geometry to four equivalent Li1+ and four equivalent Al3+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on LiCu2Si by Materials Project

LiCu2Si is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Li1+ is bonded in a 8-coordinate geometry to eight equivalent Cu+1.50+ and six equivalent Si4- atoms. All Li–Cu bond lengths are 2.48 Å. All Li–Si bond lengths are 2.86 Å. Cu+1.50+ is bonded in a distorted body-centered cubic geometry to four equivalent Li1+ and four equivalent Si4- atoms. All Cu–Si bond lengths are 2.48 Å. Si4- is bonded in a 8-coordinate geometry to six equivalent Li1+ and eight equivalent Cu+1.50+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on Li2CaSi by Materials Project

Li2CaSi is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Li1+ is bonded to four equivalent Ca2+ and four equivalent Si4- atoms to form a mixture of corner, edge, and face-sharing LiCa4Si4 tetrahedra. All Li–Ca bond lengths are 2.84 Å. All Li–Si bond lengths are 2.84 Å. Ca2+ is bonded in a 6-coordinate geometry to eight equivalent Li1+ and six equivalent Si4- atoms. All Ca–Si bond lengths are 3.28 Å. Si4- is bonded in a distorted body-centered cubic geometry to eight equivalent Li1+ and six equivalent Ca2+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on Li2YbSi by Materials Project

Li2YbSi is Heusler structured and crystallizes in the cubic Fm-3m space group. The structure is three-dimensional. Li1+ is bonded to four equivalent Yb2+ and four equivalent Si4- atoms to form a mixture of face, edge, and corner-sharing LiYb4Si4 tetrahedra. All Li–Yb bond lengths are 2.83 Å. All Li–Si bond lengths are 2.83 Å. Yb2+ is bonded in a 6-coordinate geometry to eight equivalent Li1+ and six equivalent Si4- atoms. All Yb–Si bond lengths are 3.26 Å. Si4- is bonded in a distorted body-centered cubic geometry to eight equivalent Li1+ and six equivalent Yb2+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on Li2InSi by Materials Project

LiLiInSi is alpha bismuth trifluoride-derived structured and crystallizes in the cubic F-43m space group. The structure is three-dimensional and consists of four lithium molecules and one LiInSi framework. In the LiInSi framework, Li1+ is bonded to four equivalent Si4- atoms to form LiSi4 tetrahedra that share corners with four equivalent InSi4 tetrahedra, corners with twelve equivalent LiSi4 tetrahedra, and edges with six equivalent InSi4 tetrahedra. All Li–Si bond lengths are 2.88 Å. In2+ is bonded to four equivalent Si4- atoms to form InSi4 tetrahedra that share corners with four equivalent LiSi4 tetrahedra, corners with twelve equivalent InSi4 tetrahedra, and edges with six equivalent LiSi4 tetrahedra. All In–Si bond lengths are 2.88 Å. Si4- is bonded in a body-centered cubic geometry to four equivalent Li1+ and four equivalent In2+ atoms.

36 MATERIALS SCIENCE↗