Lee, Mi Jung Kim, Sung-Hoon Lee, Sangik Yoon, Chansoo Min, Kyung-Ah Choi, Hyunsoo Hong, Suklyun Lee, Sungmin Park, Je-Geun Ahn, Jae-Pyoung Park, Bae Ho 2024-01-19T16:01:26Z 2024-01-19T16:01:26Z 2022-01-25 2020-12 1884-4049 https://pubs.kist.re.kr/handle/201004/117709 Memristive electrochemical metallization (ECM) devices based on cation migration and electrochemical metallization in solid electrolytes are considered promising for neuromorphic computing systems. Two-dimensional (2D) layered materials are emerging as potential candidates for electrolytes in reliable ECM devices due to their two-dimensionally confined material properties. However, electrochemical metallization within a single-crystalline 2D layered material has not yet been verified. Here, we use transmission electron microscopy and energy-dispersive X-ray spectroscopy to investigate the resistive switching mechanism of an ECM device containing a single-crystalline 2D layered CrPS4 electrolyte. We observe the various conductive filament (CF) configurations induced by an applied voltage in an Ag/ CrPS4/Au device in the initial/low-resistance/high-resistance/breakdown states. These observations provide concrete experimental evidence that CFs consisting of Ag metal can be formed inside single-crystalline 2D layered CrPS4 and that their configuration can be changed by an applied voltage. Density functional theory calculations confirm that the sulfur vacancies in single-crystalline CrPS4 can facilitate Ag ion migration from the active electrode layer. The electrically induced changes in Ag CFs inside single-crystalline 2D layered CrPS4 raise the possibility of a reliable ECM device that exploits the properties of two-dimensionally confined materials. English NATURE RESEARCH Understanding filamentary growth and rupture by Ag ion migration through single-crystalline 2D layered CrPS4 Article 10.1038/s41427-020-00272-x 1 NPG ASIA MATERIALS, v.12, no.1 NPG ASIA MATERIALS 12 1 N scie scopus 000600111500001 2-s2.0-85097750353 Materials Science, Multidisciplinary Materials Science Article TOTAL-ENERGY CALCULATIONS SWITCHES DEVICES