bluuebunny/crossref_metadata_2025_split huggingface dataset:
Impact of Data Window on Prediction of Battery Aging and Swelling
Authors: Pannala Sravan , Siegel Jason , Stefanopoulou Anna 
Published: November 2022

Lithium-ion batteries degrade over time, based on their usage and these changes can be observed in the terminal voltage and cell expansion curves with respect to SOC. Physics-based battery models augmented with degradation modes can describe the changes in battery electrical and mechanical response as the battery ages and can be tuned to predict the observed rate of change. Tuning these models is computationally intensive, because it requires multiple simulations of the battery aging process over the entire lifetime. Accelerated simulations that use an adaptive inter-cycle extrapolation algorithm [1] can reduce simulation time and thus enable use of optimization algorithms to automatically tune degradation models [2].
In this work, we investigate how the amount of aging data used to train the model impacts the prediction of future battery aging assuming the battery continues to operate under the same conditions. The electrode-specific state of health (eSOH) parameters are computed from the reference performance testing performed at periodic intervals throughout the battery's lifetime. These four parameters include the capacities of positive and negative electrodes Cp and Cn, and the corresponding electrode stoichiometric windows y0 and x100. These 4 parameters extracted from a cell aged at C/5 constant current charging rate were used for training the model.
The aging model includes SEI growth in the negative electrodes which causes a loss of cyclable lithium/loss of lithium inventory (LLI) and loss of electrode active material (LAM) due to particle cracking at both the negative and positive electrodes. Simulation results show us that a shorter training window of three eSOH reference points (every 25 cycles) over (Cycles 41 to 98) over-predicts battery degradation because the rate of degradation during these initial cycles is larger than the degradation which happens later in the battery's life. The battery degradation parameters that are predicted (and shown in the figure) include battery capacity, maximum reversible swelling in the battery, loss of active material in the negative electrode and loss of lithium inventory. If we increase the model training window to five eSOH data points (Cycles 41 to 175), the prediction of battery degradation is much better because the model now accounts for both the initial higher rate of degradation and subsequent lower rate of degradation.

References:

V Sulzer et al. Accelerated Battery Lifetime Simulations Using Adaptive Inter-Cycle Extrapolation Algorithm, Journal of Electrochemical Society (2021)

S. Pannala et al. Methodology for Accelerated Inter-Cycle Simulations of Li-ion Battery Degradation with Intra-Cycle Resolved Degradation Mechanisms, American Controls Conference (2022)

Figure 1
A Battery Aging Mode Identification Framework: Encompassing Multiple Cell Chemistries, Electrode Designs, and Use Conditions
Authors: Chen Bor-Rong , Walker Cody M. , Kunz M. Ross , Tanim Tanvir R. , Dufek Eric J. 
Published: November 2022

A key challenge for Lithium-ion batteries (LiB) is the capability to manage battery performance and predict the battery’s lifetime, which are crucial information for optimum operation of electric-vehicles (EVs). In that regard, early detection of battery-aging phenomena and their implications on performance is necessary for maintaining warranty and avoiding safety-related liabilities. However, rapid diagnosis of the root causes of battery degradation has not yet been well-developed nor studied upon a broad mixture of cell designs and use cases.
Here, a machine-learning (ML)- based framework is presented that aims at identifying aging modes or mechanisms during battery cycling. Cycle-by-cycle electrochemical signatures (e.g., end-of-rest voltages, columbic efficiency, and capacity fade) were analyzed then correlated with aging modes, such as loss of active materials in the cathode (LAMPE) or loss of Li inventory (LLI). Multiple battery designs and use conditions were analyzed to develop this ML framework, including 44 single layer pouch cells representing two cathode chemistries (NMC532 and NMC811), two electrode loadings (low and moderate), and five charging rates (1, 4, 4.5, 6, and 9C CC-CV profiles). Predominant aging behaviors depend on both the cell design and use. Aging behaviors can be classified into a combination of LAMPE and LLI. A classification accuracy of 90% was achieved using only the first 200aging cycles, and the percentage of LAMPE was predicted with 4.3% of error after 600 cycles. As seen here, the overall aging behavior of the battery was found to be dependent on cathode chemistry, electrode build, and usage conditions.
This ML framework is promising for battery developers to save the time and effort that is typically associated with prolonged testing. The ML framework will also advise on innovative design strategies to counter specific degradation modes, thus significantly accelerating the development cycle for building longer lasting batteries. From the end user’s perspective, this aging-mode diagnosis framework enables the ability to fine-tune battery service scenarios to minimize degradations thereby improving both lifetime and safety in EVs or stationary storage systems.

Figure 1
Isoxazole-Based Electrolytes for Lithium Metal Protection and Lithium-Sulfurized Polyacrylonitrile (SPAN) Battery Operating at Low Temperature
Authors: Tan Sha , Liu Haodong , Wu Zhaohui , Ronne Arthur , Shadike Zulipiya , Liu Ping , Hu Enyuan , Yang Xiao-Qing 
Published: November 2022

A new electrolyte system using isoxazole as the salt dissolving solvent has been developed and studied for lithium metal batteries. By using fluoroethylene carbonate (FEC) as an additive and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropyl ether (TTE) as a diluent for localized high concentration electrolyte (LHCE), isoxazole-based electrolytes were successfully implemented in lithium metal batteries, demonstrating excellent lithium metal protection capability. Utilizing several advanced characterization techniques (including synchrotron-based X-ray absorption spectroscopy and photoelectron spectroscopy), the solid electrolyte interphase (SEI) formed on the Li-metal anode in cells using these electrolytes was thoroughly investigated. The high ionic conductivity of isoxazole at low temperature and the low impedance of SEI formed in LHCE significantly improved the low-temperature performance of Li-sulfurized polyacrylonitrile (SPAN) batteries, delivering 273.8 mAh g-1 capacity at -30°C with 99.85% capacity retention after 50 cycles.
Acknowledgment: The work done at Brookhaven National Laboratory was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the US Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) Program, including Battery500 Consortium under contract number DE-SC0012704. This research used beamline 8-BM (TES) and 7-ID-2 (SST-2) of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities, operated for the DOE Office of Science by Brookhaven National Laboratory under contract number DE-SC0012704. SEM measurements for this manuscript were performed at Center for Functional Nanomaterials, a U.S. DOE office of Science User Facility, at Brookhaven National Laboratory under the contract number DE-SC0012704.
Simulations and Analyses of Li4 and Li6 Boracites and Thioboraocites As Promising Li Ion Conducting Electrolytes
Authors: Lynch David , Li Yan , Holzwarth Natalie 
Published: November 2022

The naturally occurring magnesium borate mineral, Mg3B7O13Cl, is characterized by a rigid
framework of B-O bonds together with a regular void structure, ideally forming crystals in the
face-centered cubic structure and characterized by the space group F-43c (#219). Recently,
several structurally related Li ion conducting boracites and thioboracites have been synthesized
and computationally investigated, including Li4B7O12Cl [1], Li4Al3B4O12Cl [2], and Li6B7S13I [3].
The high ionic conductivity of all of these materials is related to the occurrence of natural
interstitial Li sites due to the high symmetry of the crystalline structures. In this presentation, we
report the results of computational analysis and simulations of the large family of Li4 and Li6

ion-conducting boracites and thioboracites, including the experimentally identified materials and
several computationally predicted materials. The simulation results provide guidance on the
detailed mechanisms of Li ion mobility, the stability of materials with respect to decomposition,
and the structural stability of the materials with respect to rhombohedral and other distortions.
-----------------------------------------------------------------------------------------------------------
[1] Y. Li and N. A. W. Holzwarth, Phys. Rev. Materials 6, 025401 (2022)
https://doi.org/10.1103/PhysRevMaterials.6.025401.
[2] K. Kajihara, N. Tezuka, M. Shoji, J. Wakasugi, H. Munakata, and K. Kanamura, Bulletin of
the Chemical Society of Japan 90, 1279 (2017) https://doi.org/10.1246/bcsj.20170242.
[3] K. Kaup, K. Bishop, A. Assoud, J. Liu, and L. F. Nazar, J. Am. Chem. Soc. 143, 6952 (2021)
https://doi.org/10.1021/jacs.1c00941.
------------------------------------------------------------------------------------------------------------
The work was supported by NSF Grant No. DMR-1940324. Computations were performed on the Wake Forest University DEAC cluster, a centrally managed resource with support provided in part by the university.
Interfacial Chemistry and Electrolyte Approaches for Enabling Metal Anode Batteries
Authors: Popovic-Neuber Jelena 
Published: November 2022

Continuous solid electrolyte interphase (SEI) and dendrite growth, as well as formation of ion blocking interfaces are some of the crucial issues preventing the commercialization of batteries depending on the implementation of Li/Na/K/Mg/Ca metal anodes.[1,2] In the first part of my talk, I will focus on the chemistry of formed interfaces, including growth and ion transport control. Second part of my talk deals with bulk liquid, polymer and hybrid electrolyte molecular structure approaches for circumventing dendrite formation.
Understanding of the SEI growth on alkali and alkaline earth metals in contact with liquid electrolytes under open circuit potential conditions important for shelf aging is still in its infancy. I will show that the SEI formed on Li in contact with glyme-based electrolyte grows via reaction-controlled mechanism that is rapidly substituted by the diffusion-controlled one.[3] The ionic transport and stability of the complex composite SEI material under current is highly dependent on the salt chemistry, with detrimental effects of LixSy and positive effects of the Li3N constituents. Most recent ion transport and morphological studies show that the initial SEI formed in contact with liquid electrolytes on Li, Na and Mg is nanoporous.[4,5] Based on the electrochemical impedance spectroscopy measurements in symmetric cells and related equivalent circuit models, I will discuss potential growth mechanism via SEI densification. Finally, I will present a possibility of using gas/solid synthesis for preparation of sulfide-based artificial SEIs for both liquid-based and solid-state batteries.[6]
Dendrite formation on alkali and alkaline earth metal anodes is closely related to the ion concentration gradients formed near the electrodes in contact with the electrolytes. I will discuss the method to circumvent this problem by using electrolytes with high cationic transference number. In soft matter electrolytes this is possible when (i) interfacial effect enables preferential anionic adsorption in liquid/solid electrolytes,[7] (ii) the size and steric effects control the association and mobility of the anion in the liquid electrolytes,[8] (iii) ion transport proceeds through percolating amorphous clusters in polymer-in-salt electrolytes. [9]
References:
[1] J. Popovic, Nat. Comm., 12, 6240 (2021) [2] J. Popovic, J. Electrochem. Soc., 3, 169 030510 (2022) [3] M. Nojabaee, K. Küster, U. Starke, J. Popovic, J. Maier, Small, 16, 23, 2000756 (2020) [4] K. Lim, B. Fenk, J. Popovic, J. Maier, ACS App. Mat. Int., 13 (43), 51767 (2021) [5] J. Popovic, Energy Technol., 9, 4, 2001056 (2021) [6] K. Lim, B. Fenk, K. Küster, T. Acartürk, J. Weis, U. Starke, J. Popovic, J. Maier, ACS App. Mat. Int., 10.1021/acsami.1c23923 (2022) [7] J. Popovic, G. Hasegawa, I. Moudrakovski, J. Maier, J. Mat. Chem. A, 1, 40, 7135 (2016) [8] J. Popovic, D. Höfler, J. Melchior, A. Münchinger, B. List, J. Maier, J. Phys. Chem. Lett., 9, 17, 5116 (2018) [9] J. Popovic, Macromol. Chem. Phys, 10.1002/macp.202100344 (2021)
Gesn Alloys: From Optical to Electrical Pumped Lasers
Authors: Buca Dan , El-kurdi Moustafa , Witzens Jeremy , Oehme Michael , Capellini Giovanni , Gruetzmacher Detlev 
Published: November 2022

Internet of Things applications, including medical diagnostics, imaging and industrial process controls, pollution monitoring or real-time motion control, push the extension of the Si photonics towards mid-infrared range.
In recent years, group IV SiGeSn-based optoelectronic devices including light emitting, detectors, modulators, and CMOS devices have been developed. The main advantage of SiGeSn is the bandgap tunability in the range between 1.5 to 5 µm via Si and Sn compositions. Remarkably, the GeSn binary alloy becomes a direct bandgap semiconductor at a relative low Sn content of about 7-8 at.% opening the quest for the realization of monolithically integrated laser sources on Si. In this direction, from the first laser emission proof in 2015 remarkable progress has been done. Supported by epitaxial growth success, processing technology, and cavity design, the laser emission of optically pumped was continuously increased from 80K to 270K. The main role here was played by increasing the Sn content up a concentration of 17 at.%.
The next major improvement came from layer transfer technology allowing defect engineering and heat management. Their combination made possible room temperature lasing. However, the real life application requires low laser threshold. Here the use of multiple quantum wells based on SiGeSn/GeSn heterostructures and strain engineering allow a remarkable threshold reduction to values of about 1 kA/cm2. Interestingly, modeling shows that the very epitaxial challenging of having high Sn contents can be reduced by band structure engineering via introducing tensile strain and, in addition, larger gains are possible compared with high-Sn strain free layers. The optical laser spectrum at 0 °C for a GeSn layer under 1 % biaxial tensile strain is shown in Fig 1a.
The next step is the realization of an electrical pumped GeSn laser. The first data indicate that both waveguide and microdisk cavities can be electrically pumped leading to low temperature laser emission. The effect of the geometry and strain relaxation of under-etched cavities on the laser emission is under study. Figure 1b shows an exemplary spectrum and current-in light-out (LI) curve for a device with a SiGeSn/GeSn heterostructure taken at 50 K.

Figure 1
A Near-Infrared pin Photodetector of Strain-Enhanced Ge Layer Epitaxially Grown on a Bonded Si-on-Quartz Wafer
Authors: Kuzutani Mikiya , Furuya Satoki , Piedra Lorenzana Jose Alberto , Hizawa Takeshi , Ishikawa Yasuhiko 
Published: November 2022

In Si photonics, photodetectors (PDs) of a Ge epitaxial layer on Si have been widely used, which show a high photodetection efficiency, or a high responsivity in the O (1.260–1.360 µm) and C (1.530–1.565 µm) bands. However, an issue lies in a low responsivity in the longer wavelength range of L band (1.565–1.625 µm). In this regard, we have proposed a method using a Ge layer epitaxially grown on a Si-on-quartz (SOQ) wafer [1]. The tensile in-plane lattice strain, derived from the thermal expansion mismatch between the Ge layer and base substrate, is enhanced more than 0.3% in Ge on SOQ, despite ~0.2% on Si (or Si-on-insulator). The enhanced strain in Ge on SOQ extends the fundamental optical absorption edge to about 1.65 µm, leading to a potential increase in the L-band responsivity. In this study, a vertical pin PD is fabricated using a Ge layer on SOQ, showing an increased responsivity in the L band.
A bonded SQQ wafer was used as the starting substrate, fabricated by Shin-Etsu Chemical Co. Ltd. The top Si (001) layer was 200 nm in thickness, and was heavily doped p-type by B implantation. An undoped Ge epitaxial layer (500 nm) was grown by chemical vapor deposition using GeH4 as the source gas, followed by a growth of Si cap layer (50 nm) using Si2H6. In the top region of Ge layer as well as in the Si cap layer, a heavily n-type doping was carried out by P implantation, forming a vertical pin junction. Finally, a Ti/TiN electrode was formed. Responsivity spectra were measured in the wavelength range of 1.46–1.64 µm at a normal incidence. A reference pin PD was also fabricated using a Ge layer on a standard bulk Si wafer. According to x-ray diffraction measurements, the Ge layer on SOQ showed a tensile strain of 0.33%, despite 0.14% for the reference Ge on Si.
Figure 1(a) shows typical current–voltage curves for a pin diode of Ge on SOQ measured under dark and under an illumination of 1.55-µm light (1.1 mW). The diode showed a good rectifying property under dark, while under the illumination, the current in the reverse bias significantly increased, showing a reasonable PD operation. Figure 1(b) shows typical responsivity spectra at a reverse bias of 1 V for PDs of Ge on SOQ and reference Ge on Si. Circles and lines correspond to experimental data points and theoretical curves, respectively. The responsivity for Ge on SOQ was larger in the measured wavelength range of 1.46–1.64 µm, including the L band. The increased responsivity is ascribed to the enhanced tensile strain. However, the increase in the L band was found to be suppressed by a high reflectance because of the multiple reflections at the interfaces. An optimized Si cap thickness as well as an anti-reflection coating with SiO2 can increase the normal-incidence responsivity as high as 0.3 (0.1) A/W up to 1.60 (1.64) µm without an increase in the Ge thickness.
[1] Noguchi et al., J. Appl. Phys. 128, 133107 (2020).

Figure 1
(Digital Presentation) Nanowire Transistors with Bound‐Charge Engineering
Authors: Guo Hong , Prentki Raphaël 
Published: November 2022

Low-dimensional electronic systems such as silicon nanowires exhibit weak screening which is detrimental to the performance and scalability of nanodevices, e.g., tunnel field-effect transistors. By atomistic quantum transport simulations, we show how bound charges can be engineered at interfaces of Si and low-κ oxides to strengthen screening. To avoid compromising gate control, low-κ and high-κ oxides are
used in conjunction. In Si nanowire tunnel field-effect transistors, we demonstrate that bound charge engineering increases the on-state current by orders of magnitude, and the combination of oxides yields minimal subthreshold swing. Finally, an analytical model is developed for Si nanowire FET assisted by bound charge engineering. We conclude that the proposed bound-charge engineering paves a way toward improved low-power transistors.
Growth and Properties of Graphene and Graphene Nanoribbons on Ge
Authors: Arnold Michael S. 
Published: November 2022

The synthesis of graphene directly on Ge and on Ge deposited on Si provides a scalable route toward integrating graphene onto conventional semiconductors. This presentation will first survey the growth modes of graphene on Ge(001), Ge(011), Ge(111), Ge(112), Ge(001)-6°, and Ge(001)-9° via chemical vapor deposition (CVD), reporting on the effect of Ge surface orientation on graphene island formation and shape, strain in large-area graphene films, and the nanofaceting of the Ge below graphene.[1] We will then focus on the anisotropic growth of semiconducting graphene nanoribbons on Ge(001) and Ge(001)-9° and of nominally single crystal graphene on Ge(110).
On Ge(001), we have discovered how to drive graphene crystal growth with a large shape anisotropy through control of kinetics.[2-6] This discovery enables the direct synthesis of narrow, armchair, semiconducting nanoribbons. The ribbons are self-orienting, self-defining, and have smooth edges. The ribbons exhibit excellent transport properties (e.g., high on-state conductance and on/off ratio at room temperature) and provide a promising pathway towards the direct integration of high-performance nanocarbon electronics onto conventional semiconductor wafer platforms.
On Ge(001), nominally single crystal graphene has been reported in limited cases; however, conflicting studies have evidenced polycrystallinity. Here, the factors affecting the mosaicity of graphene on Ge(110) will be elucidated using low energy electron diffraction and microscopy data.[7]
[1] R. M. Jacobberger, D. E. Savage, X. Zheng, P. Sookchoo, R. R. Delgado, M. G. Lagally, M. S. Arnold, SUBMITTED (2022).
[2] R. M. Jacobberger, M. S. Arnold, et al., Direct Oriented Growth of Armchair Graphene Nanoribbons on Germanium, NATURE COMMUNICATIONS, 6, 8006 (2015).
[3] B. Kiraly, M. S. Arnold, M. C. Hersam, N. P. Guisinger et al., Sub-5 nm, Globally Aligned Graphene Nanoribbons on Ge (001), APPLIED PHYSICS LETTERS, 108, 213101 (2016).
[4] A. J. Way, R. M. Jacobberger, M. S. Arnold, Seed-Initiated Anisotropic Growth of Unidirectional Armchair Graphene Nanoribbon Arrays on Germanium, NANO LETTERS, 18, 898 (2018).
[5] V. Saraswat, Y. Yamamoto, H.J. Kim, R.M. Jacobberger, K.R. Jinkins, A.J. Way, N.P. Guisinger, M.S. Arnold Synthesis of armchair graphene nanoribbons on germanium-on-silicon, THE JOURNAL OF PHYSICAL CHEMISTRY C 123 (30), 18445-18454 (2019).
[6] A. J. Way, R. M. Jacobberger, N. P. Guisinger, V. Saraswat, X. Zheng, A. Suresh, J. H. Dwyer, P. Gopalan, Michael S. Arnold, SUBMITTED (2022).
[7] R. M. Jacobberger, Z. Miao, T. Yu, V. Saraswat, M. G. Lagally, M. S. Altman, M. S. Arnold, SUBMITTED (2022).