Scale matters: simulation of nanoscopic dendrite initiation in the lithium solid electrolyte interphase using a machine learning potential Article Swipe

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Sherif Abdulkader Tawfik , Linh La , Tri Minh Nguyen , Truyen Tran , Sunil Gupta , Svetha Venkatesh ·

YOU? · · 2025 · Open Access · · DOI: https://doi.org/10.26434/chemrxiv-2024-86s6m-v2

Although lithium solid state electrolytes promise to mitigate the chemical instabilities of liquid electrolytes in today's mainstream rechargeable batteries, solid state electrolytes still suffer from dendrite formation which leads to battery degradation and short circuiting. Dendrite initiation and propagation in specific solid state electrolyte materials has been explained, at a microscopic scale, as emerging from the lithium-filling of pores within the solid state electrolytes via microcracks. At the atomistic scale, the thermodynamic instability of many solid state electrolyte materials can explain their susceptibility to crystal decomposition upon contact with the lithium anode. However, for a more complete picture of the dendrite formation mechanisms, an understanding of the dendrite initiation mechanism at the intermediate nanoscopic scale is required. This work applies a machine learning potential (DIEP) for simulating six different solid state electrolyte-lithium interfaces at 300 K and 1000 K, with model sizes ranging from 24k to 36k atoms, for durations exceeding 20 ps. Our simulations show that the lithium dendrite initiation process can have an underpinning nanoscopic mechanism, in which the crystal decomposition by direct lithium interaction leads to the clustering of lithium. The simulations also suggest a possible mechanism for the creation of voids within the solid-electrolyte interphase, which have been observed in the Li$|$Li$_6$PS$_5$Cl$|$Li interface.

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Interphase Nanoscopic scale Dendrite (mathematics) Lithium (medication) Electrolyte Scale (ratio) Materials science Nanotechnology Computer science Artificial intelligence Chemistry Psychology Physics Biology Mathematics Electrode Physical chemistry Geometry Cell biology Psychiatry Quantum mechanics

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Type: preprint
Language: en
Landing Page: https://doi.org/10.26434/chemrxiv-2024-86s6m-v2
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DOI: https://doi.org/10.26434/chemrxiv-2024-86s6m-v2

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Title: Scale matters: simulation of nanoscopic dendrite initiation in the lithium solid electrolyte interphase using a machine learning potential

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Type: preprint

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Language: en

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Publication year: 2025

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Publication date: 2025-01-10

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Authors: Sherif Abdulkader Tawfik, Linh La, Tri Minh Nguyen, Truyen Tran, Sunil Gupta, Svetha Venkatesh

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Landing page: https://doi.org/10.26434/chemrxiv-2024-86s6m-v2

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Concepts: Interphase, Nanoscopic scale, Dendrite (mathematics), Lithium (medication), Electrolyte, Scale (ratio), Materials science, Nanotechnology, Computer science, Artificial intelligence, Chemistry, Psychology, Physics, Biology, Mathematics, Electrode, Physical chemistry, Geometry, Cell biology, Psychiatry, Quantum mechanics

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abstract_inverted_index.liquid	12
abstract_inverted_index.scale,	51, 69
abstract_inverted_index.suffer	23
abstract_inverted_index.within	59, 195
abstract_inverted_index.applies	119
abstract_inverted_index.battery	30
abstract_inverted_index.contact	87
abstract_inverted_index.crystal	84, 171
abstract_inverted_index.explain	80
abstract_inverted_index.lithium	1, 90, 158, 175
abstract_inverted_index.machine	121
abstract_inverted_index.picture	97
abstract_inverted_index.process	161
abstract_inverted_index.promise	5
abstract_inverted_index.ranging	142
abstract_inverted_index.suggest	186
abstract_inverted_index.today's	15
abstract_inverted_index.Although	0
abstract_inverted_index.Dendrite	35
abstract_inverted_index.However,	92
abstract_inverted_index.chemical	9
abstract_inverted_index.complete	96
abstract_inverted_index.creation	192
abstract_inverted_index.dendrite	25, 100, 107, 159
abstract_inverted_index.emerging	53
abstract_inverted_index.learning	122
abstract_inverted_index.lithium.	182
abstract_inverted_index.mitigate	7
abstract_inverted_index.observed	202
abstract_inverted_index.possible	188
abstract_inverted_index.specific	40
abstract_inverted_index.atomistic	68
abstract_inverted_index.different	128
abstract_inverted_index.durations	149
abstract_inverted_index.exceeding	150
abstract_inverted_index.formation	26, 101
abstract_inverted_index.materials	44, 78
abstract_inverted_index.mechanism	109, 189
abstract_inverted_index.potential	123
abstract_inverted_index.required.	116
abstract_inverted_index.batteries,	18
abstract_inverted_index.clustering	180
abstract_inverted_index.explained,	47
abstract_inverted_index.initiation	36, 108, 160
abstract_inverted_index.interface.	206
abstract_inverted_index.interfaces	132
abstract_inverted_index.mainstream	16
abstract_inverted_index.mechanism,	167
abstract_inverted_index.nanoscopic	113, 166
abstract_inverted_index.simulating	126
abstract_inverted_index.circuiting.	34
abstract_inverted_index.degradation	31
abstract_inverted_index.electrolyte	43, 77
abstract_inverted_index.instability	72
abstract_inverted_index.interaction	176
abstract_inverted_index.interphase,	198
abstract_inverted_index.mechanisms,	102
abstract_inverted_index.microscopic	50
abstract_inverted_index.propagation	38
abstract_inverted_index.simulations	154, 184
abstract_inverted_index.electrolytes	4, 13, 21, 63
abstract_inverted_index.intermediate	112
abstract_inverted_index.microcracks.	65
abstract_inverted_index.rechargeable	17
abstract_inverted_index.underpinning	165
abstract_inverted_index.decomposition	85, 172
abstract_inverted_index.instabilities	10
abstract_inverted_index.thermodynamic	71
abstract_inverted_index.understanding	104
abstract_inverted_index.susceptibility	82
abstract_inverted_index.lithium-filling	56
abstract_inverted_index.solid-electrolyte	197
abstract_inverted_index.electrolyte-lithium	131
abstract_inverted_index.Li$\|$Li$_6$PS$_5$Cl$\|$Li	205
cited_by_percentile_year
countries_distinct_count	1
institutions_distinct_count	6
citation_normalized_percentile.value	0.00918454
citation_normalized_percentile.is_in_top_1_percent	False
citation_normalized_percentile.is_in_top_10_percent	False