bluuebunny/crossref_metadata_2025_split huggingface dataset:
(Invited) Quantitative Photonic Characterization and Modelling of Light Emission, Confinement, and Enhancement in Nanostructured Materials
Authors: Zapien J Antonio , Foo Yishu , Phoo May Thawda , Huqe Md Rashedul , Zhang Yun , Kwong Yee Man 
Published: August 2024

Optical spectroscopy and imaging provide non-destructive, contactless, and fast strategies to study the nature and technological aspects of thin films and nanostructured materials for photonic and optoelectronic applications. Furthermore, the design, engineering, and optimization of such devices requires quantitative information with high-precision standards in measuring and modelling as is the case, for example, in the determination of the optical critical dimension (OCD) in the semiconductor industry. Our application of these strategies to the study of tunable self-assembled nanolasers, hybrid photonic-plasmonic sensors, and photovoltaic devices, among many other materials and devices has led us to the development of i) new modelling strategies based on the Finite-Difference Time-Domain (FDTD) method, and ii) home-made customizable characterization strategies based on spectroscopic ellipsometry (SE). The advantages of the FDTD method include its ability to i) obtain a wide spectral response from one time-domain simulation, ii) model single non-periodic structures, and iii) flexibility and generality to include, for example, non-linear and thermal effects. On its part, SE stands out from other optical techniques because, as a self-referenced and phase sensitive strategy, it can deliver extreme precision and sensitivity and has demonstrated flexibility that has been implemented in multiple spectral ranges and operation conditions. With this in mind, our group has systematically demonstrated the synergic use of FDTD-SE strategy, with complementary strengths and close-matched precision, in a range of materials and devices. We will report the fundamentals, status of our on-going efforts, and a critical review of the perceived limitations and expected outcomes of the FDTD-SE strategy as a quantitative tool for photonic and plasmonic subwavelength structures of interest in optoelectronic, sensing, and energy applications.
We gratefully acknowledge the financial support from the RGC (Projects CityU - 11210218, 11219919, 11215121 and 11310122) and ITC (Project ITS/461/18) of HKSAR, China.
(Invited) Chiral Metamaterials for Polarized Photoluminescence
Authors: Ferry Vivian 
Published: August 2024

Metasurfaces offer compact routes to spatial and polarization control of luminescence from nearby emitters, enabling applications ranging from document security to stereoscopic displays to sensing.
Most of the time, light-emitters are distributed evenly across the surface. This talk will discuss an alternate approach, where we use direct-write electron beam lithography to pattern semiconductor nanocrystals into targeted shapes and locations, creating a highly tailored metasurface. We use a combination of nanoscale fabrication, Fourier-space photoluminescence measurements, and computational methods to study the circularly polarized photoluminescence from these designer structures.
We will discuss the influence of patterning on the resulting optical properties, including the effects of spatial averaging and dipole orientation. We will then show an optimization strategy to produce highly polarized light at chosen angles of outcoupling. The final part of the talk will discuss adding layers of complexity, including the chirality of the underlying pattern, and creating light-emitting solids from intrinsically chiral semiconductor nanocrystals.
Development of High-Performance Cathodes for Inorganic Halide All-Solid-State Li-Ion Batteries
Authors: Deng Sixu 
Published: August 2024

Electric vehicles (EVs), representing the future of transportation, are predicted to be one of the ultimate solutions to eliminate greenhouse gas emissions. Li-ion batteries (LIBs), as the most promising sustainable energy devices, are critical for the development of EVs because of their higher operating voltages compared to other energy storage technologies. However, the development of conventional LIBs touched the ceiling because of three main challenges. (1) The use of flammable and toxic liquid electrolytes brings high safety risks. (2) The limited energy density of LIBs cannot satisfy the requirement for long-range EVs. (3) The increasing market demand for LIBs will cause resource shortage and rise of cost.[1] Accordingly, all-solid-state Li-ion batteries (ASSLIBs) have recently emerged as promising alternative batteries for next-generation EVs because of their ability to overcome the drawbacks of conventional LIBs. Among the developed solid-state electrolytes (SSEs), inorganic SSEs (e.g., sulfide SSEs, halide SSEs) have high Li+ conductivity at 10-3 S cm-1 and improved interfacial stability, demonstrating stable cycling performance in ASSLIBs.[2] However, inorganic ASSLIBs still face some key challenges hindering their application in EVs. For example, the rate capability of inorganic ASSLIBs still falls far below the requirements of fast-charging EVs (full-charged in 15 min). In addition to the effect of Li+ conductivity in SSEs, Li+/e- transfer kinetics at the cathode interface and in cathode materials are also critically important for the high-rate capability of inorganic ASSLIBs. In this talk, I will first review our previous studies on cathode interface in inorganic ASSLIBs.[3-7] After that, I will introduce our most recent research on unveiling the kinetic limitation of cathode interfaces in inorganic ASSLIBs by synchrotron-based spectromicroscopy. Our research suggests that poor Li+/e- transfer kinetics at the cathode/SSE interface and in the cathode bulk structure are the key limitation for the low capacity of inorganic ASSLIBs under high-rate charge-discharge cycles.
References
[1] H. Li, Joule, 3 (2019) 911-914.
[2] S. Randau, D.A. Weber, O. Kötz, R. Koerver, P. Braun, A. Weber, E. Ivers-Tiffée, T. Adermann, J. Kulisch, W.G. Zeier, Nature Energy, 5 (2020) 259-270.
[3] S. Deng, X. Li, Z. Ren, W. Li, J. Luo, J. Liang, J. Liang, M.N. Banis, M. Li, Y. Zhao, Energy Storage Materials, 27 (2020) 117-123.
[4] S. Deng, Y. Sun, X. Li, Z. Ren, J. Liang, K. Doyle-Davis, J. Liang, W. Li, M. Norouzi Banis, Q. Sun, ACS Energy Letters, 5 (2020) 1243-1251.
[5] S. Deng, Q. Sun, M. Li, K. Adair, C. Yu, J. Li, W. Li, J. Fu, X. Li, R. Li, Energy Storage Materials, 35 (2021) 661-668.
[6] S. Deng, M. Jiang, N. Chen, W. Li, M. Zheng, W. Chen, R. Li, H. Huang, J. Wang, C.V. Singh, Advanced Functional Materials, 32 (2022) 2205594.
[7] S. Deng, M. Jiang, A. Rao, X. Lin, K. Doyle‐Davis, J. Liang, C. Yu, R. Li, S. Zhao, L. Zhang, Advanced Functional Materials, 32 (2022) 2200767.
Development of High-Performance LLZO Separators for Solid-State Batteries: Balancing Li Loss, Stability, and Morphology in a Tape Casting Process
Authors: Touidjine Kaouther , Rosen Melanie Finsterbusch , Kiyek Vivien , Ganapathy Swapna , Finsterbusch Martin , Guillon Olivier , Huijben Mark , Kelder Erik , Wagemaker Marnix , Fattakhova-Rohlfing Dina 
Published: August 2024

Ceramic solid-state batteries (SSBs) are considered a viable alternative to lithium-ion batteries with liquid electrolytes, as they offer greater safety at the cell level. The Li7La3Zr2O12 garnet (LLZO) is a promising solid electrolyte for SSBs due to its stability with lithium metal anode and its good ionic conductivity of up to 2 mS cm-1. However, scalable and economically feasible techniques for producing LLZO-based batteries are required to make them competitive in the market.
Tape casting is an industrially scalable process for producing customizable ceramic components. Successful implementation of this method requires a deep understanding of the transformation of the LLZO powder during the whole process chain, especially the effects of Li loss due to air and protic solvents interaction as well as Li evaporation during sintering.
In this talk, a novel approach for fabricating thin LLZO ceramic separators by tape casting will be presented, in which lithium saltis used as a lithium mediator source in different process steps to optimize the separator properties. Using XRD, Raman spectroscopy, NMR spectroscopy, and SEM, we systematically investigate the effects of material composition and process conditions on the compositional and electrochemical performance of tape-cast LLZO separators in symmetric cells. This research provides important insights for optimizing the manufacturing process and enables the development of high-performance LLZO ceramic separators for all-solid-state batteries.
Ab Initio Tomography Analysis of Lithium Incorporation and Diffusion in Multidomain Silicon Suboxide Anode Materials
Authors: Chae Somin , Lim Hyung-Kyu , Lee Sangheon 
Published: August 2024

Silicon is considered a promising anode material to supplant conventional graphite materials in lithium-ion batteries due to its higher theoretical energy-storage capacity compared to graphite. However, the widespread application of Si anodes has been hindered because the capacity of Si anodes decreases rapidly as the charge/discharge cycle proceeds. The controlled incorporation of oxygen into Si is often considered as a feasible approach for employing Si as an anode material in the form of silicon suboxide. Silicon suboxide exhibits a lower energy capacity compared to pure Si, but offers enhanced stability against volume expansion. Consequently, silicon suboxide materials have been commercialized by blending them with graphite. However, the blending ratio of silicon suboxide with graphite is limited to low levels due to its poor first-cycle efficiency, so-called initial Coulombic efficiency. In-depth understanding of the lithium interaction characteristics within multidomain silicon suboxide is indispensable for optimizing the electrochemical performance of silicon suboxide anode materials for lithium-ion batteries. In this study, we investigate the domain-dependent thermodynamic and kinetic properties of lithium atoms within systematically designed multidomain silicon suboxide models composed of Si, SiO2, and Si/SiO2 interface by performing a series of computational simulations combined with a unique tomography-like sampling scheme. We find that the Si/SiO2 interfacial region exhibits preferential thermodynamics and kinetics for lithiation and can serve as a critical lithium transport channel during charge-discharge cycles, while the SiO2 domain is likely to be excluded from lithiation due to its high resistance to lithium diffusion. Consequently, a significant fraction of lithium is expected to be trapped at the Si/SiO2 interface during the discharge process, which ultimately contributes to a low initial Coulombic efficiency. This theoretical understanding suggests that the formation of continuously connected lithium-transportable Si/SiO2 interfacial channels surrounding the Si domains, along with a well-structured shallow SiO2 framework through the use of appropriate synthesis methods, is essential for maximizing the electrochemical performance of silicon suboxide anode materials. Our theoretical approach offers new insights into the atomistic characteristics of silicon suboxide during lithiation/delithiation processes, ultimately enabling the identification of the origin of low ICE and strategies for addressing it.
References
(1) Chae, S.; Lim, H.-K.; Lee, S. Energy Landscapes for Lithium Incorporation and Diffusion in Multidomain Silicon Suboxide Anode Materials. ACS Applied Materials & Interfaces
2023, 15 (49), 57059-57069. DOI: 10.1021/acsami.3c12846.

Figure 1
Boron-Doped Carbon Scaffold Hosts for Li Metal Batteries
Authors: Freyman Megan C. , Li Sichi , Zhu Cheng , Wang Bo , Xiao Yiran , Wood Marissa 
Published: August 2024

Lithium metal anodes offer the promise of higher energy density batteries. However, the formation of lithium dendrites due to non-uniform plating and stripping of the lithium metal has proven to be a major hurdle for this technology, decreasing the lifetime of the device and causing safety hazards. Utilizing a carbon scaffold host for the lithium metal anode can limit dendrite formation by providing a more uniform electric field and numerous lithium nucleation sites to encourage uniform plating and stripping. In this poster, we present our work developing carbon scaffold hosts for lithium metal anodes. We synthesized scaffolds with various architectures and microstructures using different carbon materials. Our atomistic simulations demonstrated that the addition of boron to the carbon results in stronger binding of lithium to the carbon surface, further improving the lithiophilicity. Therefore, we also prepared boron-doped carbon scaffolds to test this experimentally. Boron was introduced using boric acid and incorporated into the carbon structure during carbonization under nitrogen, and these samples were characterized by XPS, SEM, and BET to try and correlate scaffold properties with performance. In addition, we are investigating other dopants (such as nitrogen), which have also been reported to increase the lithiophilicity of carbon materials. Utilizing these doped carbon scaffolds can help increase the lifetime of lithium metal batteries by improving the cycling uniformity.
This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344
The Voltage-Based Implementation of the Tunneling Mechanism in Aging Models for Lithium-Ion Batteries
Authors: Wang Zhenya , Danilov Dmitri L. , Eichel Rudiger-A , Notten Peter H.L. 
Published: August 2024

Lithium-ion batteries (LIBs) have become one of the most crucial power sources for electronics and electric vehicles due to high energy density, long cycle life, environmental friendliness, etc. Precise explanation and prediction of the aging behavior of LIBs is quickly becoming a hotspot. A solid electrolyte interface (SEI) growth is regarded as the dominant factor of capacity losses in LIBs. However, the previous SEI growth and aging models were based on energy levels. That means the energy barrier related to the Fermi level of SEI and electrode was used as the input parameter. It is not straightforward to implement, especially for industrial applications. Furthermore, the state-of-charge (SoC) and the energy barrier were usually assumed to be constant during (dis)charging, contradicting common sense and affecting the calculations' accuracy.
The present work proposes and experimentally validates an advanced voltage-based aging model. The voltage of the anode electrode is adopted as an input parameter in this model. It is easier to introduce dependence of aging on the voltage/SoC of the electrode with this model. It is found that deep delithiation of the anodes and lower SoC of LIBs will mitigate electron tunneling, lower SEI growth, and reduce calendar aging. Commonly used anode materials, such as graphite, Li4Ti5O12, and blended Si/C, are presented as interesting cases to investigate the effects of different electrode materials on the tunneling current profiles during (dis)charging for the first time. The model is instructive and can predict aging in LIBs with various electrode materials. This model and related analyses are beneficial for further optimizing LIB's electronic and electrode properties and as interesting limiting cases for testing battery modeling software.
(Keynote) Monodisperse Nanoparticles of Ternary Spinels for Electrochemical Energy Conversion and Storage
Authors: Robinson Richard D. , Rowell Jonathan L. , Meyer Talisi E. 
Published: August 2024

Ternary spinel nanoparticles are an exciting materials system that have been increasingly pursued for a variety of energy applications such as supercapacitors and as electrocatalysts for the oxygen reduction reaction. For example, Cobalt-manganese spinel oxides, in particular, have demonstrated outstanding performance as supercapacitors and electrocatalysts.
Despite their exemplary performance in multiple electrochemical applications, there are few reports in the literature with high-quality ternary spinel nanoparticles, such as Co-Mn-O. Most reports show aggregated and polydisperse products that typically contain impurity phases like rock salt.
In this work, we demonstrate the synthesis of monodisperse nanoparticles of ternary spinels using colloidal chemistry. To overcome challenges for ternary spinel oxides we use oxidized amines as a route to form the high-oxidation state complexes needed for stable spinel oxides, and modify the ligand binding to obtain colloidally stable nanoparticles. For the sulfide spinel system, we show the use of amino acids as a low-cost sulfur source. Finally, we extend this work to access high entropy nanoparticles for electrochemical applications.
(Invited) Parameter Prediction in Colloidal Quantum Dot Solar Cells Using Residual Neural Networks Trained on Experimental Data
Authors: Lee Hoon Jeong , Chiu Arlene , Lin Yida , Chintapalli Sreyas , Kamal Serene , Thon Susanna Mitrani 
Published: August 2024

Colloidal quantum dots (CQDs) are an attractive third-generation material for photovoltaics, especially as infrared materials for multi-junction solar cells. Characterization and materials parameter prediction both play a critical role in the rising efficiencies in this field. However, there are numerous materials properties that need to be measured in order to fully characterize a device, leading to high research costs and slow development times. Here, we leverage recent advancements in machine learning (ML), along with a recently-demonstrated multimodal spectral characterization method [1], to predict complex materials parameters in CQD solar cells from simple current density-voltage (JV) curves, using an algorithm trained on experimental data.[2]
Past work ML prediction of materials properties has focused on using simulated data due to the difficulty in collecting enough experimental data to fully train an algorithm. While it is not feasible to fabricate thousands of devices in a typical research lab, it is possible to measure several thousand points on a single device. We used a micrometer-resolution 2D characterization method with millimeter-scale field of view to acquire enough training data using only a handful of devices, while learning the spatial relationships between materials parameters. Photoluminescence, trap state density, transient photovoltage, transient photocurrent, and carrier mobility were predicted (Figure 1) by five different residual neural networks, each using a ResNet block and containing over 300k learnable parameters. The design of the networks were based on the ResNet50 architecture [3]. We also implemented a novel neighborhood approach to reduce errors and account for spatial correlations in device behavior, leading to insights into transport mechanisms and correlation lengths in CQD thin films. This method could be used to study a wide range of material systems and devices, ultimately leading to a universal prediction model that greatly simplifies the characterization process for optoelectronic devices and accelerates development times.

References

[1] Y. Lin, T. Gao, X. Pan, M. Kamenetska & S. M. Thon, Local Defects in Colloidal Quantum Dot Thin Films Measured via Spatially-Resolved Multi-Modal Optoelectronic Spectroscopy. Advanced Materials 32, 1906602 (2020).
[2] H. J. Lee, A. Hofelmann, Y. Lin, & S. M. Thon, Predicting Materials Parameters in Colloidal Quantum Dot Photovoltaic Devices Using Machine Learning Models Trained On Experimental Data. 2022 IEEE 49th Photovoltaic Specialists Conference, 0862-0866 (2022).
[3] O. Elharrouss, N. Almaadeed, S. Al-Maadeed, & Y. Akbari, Image inpainting: A review. Neural Processing Letters 51, 2007–2028 (2020).

Figure 1
(Invited) Extended Hubbard Functionals for Accurate Modeling of Li-Ion Battery Cathode Materials
Authors: Timrov Iurii 
Published: August 2024

Designing novel cathode materials for Li-ion batteries necessitates accurate first-principles predictions of their properties. Density-functional theory (DFT) employing standard (semi-)local functionals encounters challenges due to pronounced self-interaction errors within the partially filled d shells of transition-metal (TM) elements. Here, we demonstrate the efficacy of DFT with extended Hubbard functionals in accurately predicting the "digital" change in oxidation states of TM ions for mixed-valence phases at intermediate Li concentrations in phospho-olivine and spinel cathode materials. The resulting voltages exhibit remarkable agreement with experimental data [1,2].
Our approach involves the use of onsite U and intersite V Hubbard parameters computed from density-functional perturbation theory with Lowdin-orthogonalized atomic orbitals, thus circumventing empirical factors [3,4]. Notably, the incorporation of intersite Hubbard V interactions proves indispensable for the precise prediction of thermodynamic quantities, particularly when electronic localization occurs amid inter-atomic orbital hybridization.
Extending our investigation to vibrational spectroscopy, we calculate Raman spectra for these materials and find very good agreement with available experimental data [5]. Leveraging the robust and accurate computational framework based on extended Hubbard functionals, we embark on a high-throughput screening of Li-containing compounds, aiming to unveil novel and promising candidates for cathodes [6]. Our findings underscore the pivotal role of advanced DFT methodologies in advancing the discovery and design of high-performance battery materials.
[1] I. Timrov, F. Aquilante, M. Cococcioni, N. Marzari, PRX Energy 1, 033003 (2022).
[2] I. Timrov, M. Kotiuga, N. Marzari, Phys. Chem. Chem. Phys. 25, 9061 (2023).
[3] I. Timrov, N. Marzari, M. Cococcioni, Phys. Rev. B 98, 045141 (2021).
[4] I. Timrov, N. Marzari, M. Cococcioni, Phys. Rev. B 103, 085127 (2018).
[5] L. Bastonero, N. Marzari, I. Timrov, in preparation.
[6] C. Malica, L. Bastonero, M. Bercx, N. Marzari, I. Timrov, in preparation.