Unraveling the Nanoscale Heterogeneity of Solid Electrolyte Interphase Using Tip-Enhanced Raman Spectroscopy

Nanda, Jagjit; Yang, Guang; Hou, Thomas Y.; Voylov, Dmitry; Li, Xin; Ruther, Rose E.; Naguib, Michael; Persson, Kristin A.; Veith, Gabriel M.; Sokolov, Alexei P.

doi:10.1016/j.joule.2019.05.026

Cited by 118 publications

(156 citation statements)

References 60 publications

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“…This is due to that the surface plasma resonance (SPR) on a noble metal (such as Ag) coated tip apex upon laser illumination leads to a greatly enhanced EM-eld or a hot spot in the gap between the tip and sample surface (< 5 nm in depth) ( Figure S1(b)). 18 The Raman scattering cross-section from the analyte in the hot spot is boosted, contributing to the far eld enhanced Raman scattering (i.e. TERS spectrum).…”

Section: Resultsmentioning

confidence: 99%

“…The area of a typical hot spot on the tip apex is on the scale of 10 nm, thereby breaking the light diffraction limit of the standard confocal micro-Raman spectroscopy. 18,22 However, the routine TERS mapping composes of innumerable spectra, precluding an easy insight of the underlying structure. This is particularly true for amorphous materials.…”

Section: Resultsmentioning

confidence: 99%

“…intensity of a single TERS band) insu cient to lead to a comprehensive understanding of the surface structure of the a-Si. 18 Analysis based on an individual TERS band by its nature fails to capture the overall spectral pattern of TERS mapping. To retain the global features embedded in the full set of TERS spectra, we then performed manifold learning and clustering of TERS spectral dataset (see details in method section).…”

Section: Resultsmentioning

confidence: 99%

“…it becomes di cult to extract physical information from unmixed components). 18 This explains why the nanoscale structural heterogeneity of a-Si or other amorphous materials has been much underexplored by TERS so far.…”

Section: Introductionmentioning

confidence: 99%

“…17 Tip-enhanced Raman spectroscopy (TERS) provides an apertureless means of mapping Raman scattering at nanometer scale (~ 10 nm) in-sample plane. 18,19 This is based on that the surface plasmon (i.e. enhanced electromagnetic eld or EM-eld) resides at the metallized tip apex of a scanning probe microscope (SPM), providing a localized "hot-spot" underneath the SPM tip.…”

Section: Introductionmentioning

confidence: 99%

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Distilling Nanoscale Heterogeneity of Amorphous Silicon using Tip-enhanced Raman Spectroscopy (TERS) via Multiresolution Manifold Learning

Yang

Cheng

et al. 2020

Preprint

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Accurately identifying the local structural heterogeneity of complex, disordered amorphous materials such as amorphous silicon (a-Si) is crucial for accelerating technology development. However, short-range atomic ordering quantification and nanoscale spatial resolution over a large area on a-Si have remained major challenges and practically unexplored. We resolve phonon vibrational modes of a-Si at a lateral resolution of 20 nm by tip-enhanced Raman spectroscopy (TERS). To project the high dimensional TERS imaging to a low dimensional (i.e. 2D) manifold space and categorize a-Si structure, we developed a multiresolution manifold learning (MML) algorithm. It allows for quantifying average Si-Si distortion angle and the strain free energy at nanoscale without a human-specified threshold. The MML multiresolution feature allows for distilling local defects of ultra-low abundance (< 0.3%), presenting a new Raman mode at finer resolution grids. This work promises a general paradigm of resolving nanoscale structural heterogeneity and updating domain knowledge for highly disordered materials.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Distilling Nanoscale Heterogeneity of Amorphous Silicon using Tip-enhanced Raman Spectroscopy (TERS) via Multiresolution Manifold Learning

Yang

Cheng

et al. 2020

Preprint

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Synchrotron X ‐ray Spectroscopy and Imaging for Metal Oxide Intercalation Cathode Chemistry

Tian¹,

Lin²

2022

Transition Metal Oxides for Electrochemical Energy Storage

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Toward Critical Electrode/Electrolyte Interfaces in Rechargeable Batteries

Yan

Xiao

et al. 2020

Adv Funct Materials

323

234

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The electrode/electrolyte interface plays a critical role in stabilizing the cycling performance and prolonging the service life of rechargeable batteries to meet the sustainable energy requirements of the mobile society. The understanding of interfaces is still at the preliminary stage due to the limited research techniques and variable properties with time and potential. Herein, the latest developments focused on the interfaces in rechargeable systems including the cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) are reviewed. The possible formation mechanisms of the electrode/electrolyte interface are discussed, followed by the introduction of two key influencing factors, specific adsorption and solvated coordinate structure, which will dominate the formation of the interface. Finally, the structure and chemical composition of the interface as well as the possible transport mechanism of lithium ions in the interface and the strategies to regulate the pathway through the interface are presented in detail. This work sheds light on the fundamental understanding of the interface and provides rational scientific principles in designing the electrode/electrolyte interface and inspires the rational design of long‐term cycling rechargeable batteries.

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Unraveling the Nanoscale Heterogeneity of Solid Electrolyte Interphase Using Tip-Enhanced Raman Spectroscopy

Cited by 118 publications

References 60 publications

Distilling Nanoscale Heterogeneity of Amorphous Silicon using Tip-enhanced Raman Spectroscopy (TERS) via Multiresolution Manifold Learning

Distilling Nanoscale Heterogeneity of Amorphous Silicon using Tip-enhanced Raman Spectroscopy (TERS) via Multiresolution Manifold Learning

Synchrotron X ‐ray Spectroscopy and Imaging for Metal Oxide Intercalation Cathode Chemistry

Toward Critical Electrode/Electrolyte Interfaces in Rechargeable Batteries

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