DOI: 10.1002/smll.201704514. Impact of Stoichiometry on the Structure of van der Waals Layered GeTe/Sb<sub>2</sub>Te<sub>3</sub> Superlattices Used in Interfacial Phase‐Change Memory (iPCM) Devices

Impact of Stoichiometry on the Structure of van der Waals Layered GeTe/Sb2Te3 Superlattices Used in Interfacial Phase‐Change Memory (iPCM) Devices

10.1002/smll.201704514

Crossref journal-article

Wiley

Small (311)

Abstract

AbstractVan der Waals layered GeTe/Sb2Te3 superlattices (SLs) have demonstrated outstanding performances for use in resistive memories in so‐called interfacial phase‐change memory (iPCM) devices. GeTe/Sb2Te3 SLs are made by periodically stacking ultrathin GeTe and Sb2Te3 crystalline layers. The mechanism of the resistance change in iPCM devices is still highly debated. Recent experimental studies on SLs grown by molecular beam epitaxy or pulsed laser deposition indicate that the local structure does not correspond to any of the previously proposed structural models. Here, a new insight is given into the complex structure of prototypical GeTe/Sb2Te3 SLs deposited by magnetron sputtering, which is the used industrial technique for SL growth in iPCM devices. X‐ray diffraction analysis shows that the structural quality of the SL depends critically on its stoichiometry. Moreover, high‐angle annular dark‐field‐scanning transmission electron microscopy analysis of the local atomic order in a perfectly stoichiometric SL reveals the absence of GeTe layers, and that Ge atoms intermix with Sb atoms in, for instance, Ge2Sb2Te5 blocks. This result shows that an alternative structural model is required to explain the origin of the electrical contrast and the nature of the resistive switching mechanism observed in iPCM devices.

Bibliography

Kowalczyk, P., Hippert, F., Bernier, N., Mocuta, C., Sabbione, C., BatistaâPessoa, W., & NoÃ©, P. (2018). Impact of Stoichiometry on the Structure of van der Waals Layered GeTe/Sb2Te3 Superlattices Used in Interfacial PhaseâChange Memory (iPCM) Devices. Small, 14(24). Portico.

Authors 7

Philippe Kowalczyk (first)
Françoise Hippert (additional)
Nicolas Bernier (additional)
Cristian Mocuta (additional)
Chiara Sabbione (additional)
Walter Batista‐Pessoa (additional)
Pierre Noé (additional)

References 44 Referenced 51

10.1038/nmat2009
10.1016/j.sse.2016.07.006
10.1109/IMW.2013.6582084
10.1088/1361-6641/aa7c25
10.1038/nnano.2011.96
10.7567/JJAP.53.04ED02
{'key': 'e_1_2_7_7_1', 'first-page': 'T130', 'author': 'Takaura N.', 'year': '2013', 'journal-title': '2013 Symposium on VLSI Technology'} / 2013 Symposium on VLSI Technology by Takaura N. (2013)
10.1088/1468-6996/16/1/014402
10.1002/adfm.201702243
10.1063/1.4958708
10.1021/acsami.6b11418
{'volume-title': '2014 Symp. VLSI Technol.', 'year': '2014', 'author': 'Tai M.', 'key': 'e_1_2_7_12_1'} / 2014 Symp. VLSI Technol. by Tai M. (2014)
10.1109/IRPS.2013.6532096
10.1002/adma.201505865
10.1039/C5NR04530D
10.1016/j.jallcom.2016.03.159
10.1107/S0567740874004729
10.1002/pssb.201552335
10.1063/1.4974464
10.1088/0022-3719/20/10/012
10.1002/admi.201300027
10.1063/1.4886119
10.1038/srep12612
10.1038/ncomms11983
10.1088/2399-1984/aa8434
10.1021/acs.cgd.5b01714
10.1007/s12274-017-1785-y
10.1038/srep05727
10.1557/jmr.2016.334
10.1107/S0108768104022906
10.1038/srep23843
10.1038/s41598-017-02710-3
10.1016/S0925-8388(97)00625-7
10.1063/1.4948536
10.1111/j.1365-2818.2006.01551.x
10.1039/c3ce26956f
10.1016/j.matdes.2016.11.003
10.1063/1.5000338
10.1039/C7NR01684K
10.1038/nmat3456
10.1038/s41598-016-0001-8
{'key': 'e_1_2_7_42_1', 'first-page': '33', 'volume': '6', 'author': 'Kataoka Y.', 'year': '1989', 'journal-title': 'Rigaku J.'} / Rigaku J. by Kataoka Y. (1989)
10.1016/j.jsb.2016.12.006
{'volume-title': 'Sample Preparation Handbook for Transmission Electron Microscopy: Methodology', 'year': '2010', 'author': 'Ayache J.', 'key': 'e_1_2_7_44_1'} / Sample Preparation Handbook for Transmission Electron Microscopy: Methodology by Ayache J. (2010)

Dates

Type	When
Created	7 years, 3 months ago (May 15, 2018, 2:36 a.m.)
Deposited	1 year, 11 months ago (Sept. 16, 2023, 6:39 p.m.)
Indexed	1 month ago (Aug. 2, 2025, 1:02 a.m.)
Issued	7 years, 3 months ago (May 14, 2018)
Published	7 years, 3 months ago (May 14, 2018)
Published Online	7 years, 3 months ago (May 14, 2018)
Published Print	7 years, 3 months ago (June 1, 2018)

Funders 1

Agence Nationale de la Recherche 10.13039/501100001665
Region: Europe
gov (National government)
Labels3
1. French National Research Agency
2. French National Agency for Research
3. ANR
Awards1
1. 10‐LABX‐55‐01

BibTeX

@article{Kowalczyk_2018, title={Impact of Stoichiometry on the Structure of van der Waals Layered GeTe/Sb2Te3 Superlattices Used in Interfacial Phase‐Change Memory (iPCM) Devices}, volume={14}, ISSN={1613-6829}, url={http://dx.doi.org/10.1002/smll.201704514}, DOI={10.1002/smll.201704514}, number={24}, journal={Small}, publisher={Wiley}, author={Kowalczyk, Philippe and Hippert, Françoise and Bernier, Nicolas and Mocuta, Cristian and Sabbione, Chiara and Batista‐Pessoa, Walter and Noé, Pierre}, year={2018}, month=may }

JSON

{
  "indexed": {
    "date-parts": [
      [
        2025,
        8,
        2
      ]
    ],
    "date-time": "2025-08-02T05:02:37Z",
    "timestamp": 1754110957998,
    "version": "3.41.2"
  },
  "reference-count": 44,
  "publisher": "Wiley",
  "issue": "24",
  "license": [
    {
      "start": {
        "date-parts": [
          [
            2018,
            5,
            14
          ]
        ],
        "date-time": "2018-05-14T00:00:00Z",
        "timestamp": 1526256000000
      },
      "content-version": "vor",
      "delay-in-days": 0,
      "URL": "http://onlinelibrary.wiley.com/termsAndConditions#vor"
    }
  ],
  "funder": [
    {
      "DOI": "10.13039/501100001665",
      "name": "Agence Nationale de la Recherche",
      "doi-asserted-by": "publisher",
      "award": [
        "10\u2010LABX\u201055\u201001"
      ],
      "id": [
        {
          "id": "10.13039/501100001665",
          "id-type": "DOI",
          "asserted-by": "publisher"
        }
      ]
    }
  ],
  "content-domain": {
    "domain": [
      "onlinelibrary.wiley.com"
    ],
    "crossmark-restriction": true
  },
  "published-print": {
    "date-parts": [
      [
        2018,
        6
      ]
    ]
  },
  "abstract": "<jats:title>Abstract</jats:title><jats:p>Van der Waals layered GeTe/Sb<jats:sub>2</jats:sub>Te<jats:sub>3</jats:sub> superlattices (SLs) have demonstrated outstanding performances for use in resistive memories in so\u2010called interfacial phase\u2010change memory (iPCM) devices. GeTe/Sb<jats:sub>2</jats:sub>Te<jats:sub>3</jats:sub> SLs are made by periodically stacking ultrathin GeTe and Sb<jats:sub>2</jats:sub>Te<jats:sub>3</jats:sub> crystalline layers. The mechanism of the resistance change in iPCM devices is still highly debated. Recent experimental studies on SLs grown by molecular beam epitaxy or pulsed laser deposition indicate that the local structure does not correspond to any of the previously proposed structural models. Here, a new insight is given into the complex structure of prototypical GeTe/Sb<jats:sub>2</jats:sub>Te<jats:sub>3</jats:sub> SLs deposited by magnetron sputtering, which is the used industrial technique for SL growth in iPCM devices. X\u2010ray diffraction analysis shows that the structural quality of the SL depends critically on its stoichiometry. Moreover, high\u2010angle annular dark\u2010field\u2010scanning transmission electron microscopy analysis of the local atomic order in a perfectly stoichiometric SL reveals the absence of GeTe layers, and that Ge atoms intermix with Sb atoms in, for instance, Ge<jats:sub>2</jats:sub>Sb<jats:sub>2</jats:sub>Te<jats:sub>5</jats:sub> blocks. This result shows that an alternative structural model is required to explain the origin of the electrical contrast and the nature of the resistive switching mechanism observed in iPCM devices.</jats:p>",
  "DOI": "10.1002/smll.201704514",
  "type": "journal-article",
  "created": {
    "date-parts": [
      [
        2018,
        5,
        15
      ]
    ],
    "date-time": "2018-05-15T06:36:19Z",
    "timestamp": 1526366179000
  },
  "update-policy": "https://doi.org/10.1002/crossmark_policy",
  "source": "Crossref",
  "is-referenced-by-count": 51,
  "title": "Impact of Stoichiometry on the Structure of van der Waals Layered GeTe/Sb<sub>2</sub>Te<sub>3</sub> Superlattices Used in Interfacial Phase\u2010Change Memory (iPCM) Devices",
  "prefix": "10.1002",
  "volume": "14",
  "author": [
    {
      "given": "Philippe",
      "family": "Kowalczyk",
      "sequence": "first",
      "affiliation": [
        {
          "name": "Universit\u00e9 Grenoble Alpes CEA LETI  17, rue des Martyrs F 38054 Grenoble Cedex 9 France"
        },
        {
          "name": "Universit\u00e9 Grenoble Alpes CNRS LTM  17, rue des Martyrs F 38054 Grenoble Cedex 9 France"
        }
      ]
    },
    {
      "given": "Fran\u00e7oise",
      "family": "Hippert",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "LNCMI\u2010EMFL\u2010CNRS Universit\u00e9 Grenoble Alpes INSA UPS  25, rue des Martyrs F 38042 Grenoble Cedex 9 France"
        }
      ]
    },
    {
      "given": "Nicolas",
      "family": "Bernier",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "Universit\u00e9 Grenoble Alpes CEA LETI  17, rue des Martyrs F 38054 Grenoble Cedex 9 France"
        }
      ]
    },
    {
      "given": "Cristian",
      "family": "Mocuta",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "Synchrotron SOLEIL l'Orme des Merisiers  Saint\u2010Aubin \u2013 BP 48 F\u201091192 Gif\u2010sur\u2010Yvette Cedex France"
        }
      ]
    },
    {
      "given": "Chiara",
      "family": "Sabbione",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "Universit\u00e9 Grenoble Alpes CEA LETI  17, rue des Martyrs F 38054 Grenoble Cedex 9 France"
        }
      ]
    },
    {
      "given": "Walter",
      "family": "Batista\u2010Pessoa",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "Universit\u00e9 Grenoble Alpes CEA LETI  17, rue des Martyrs F 38054 Grenoble Cedex 9 France"
        }
      ]
    },
    {
      "ORCID": "https://orcid.org/0000-0003-4397-959X",
      "authenticated-orcid": false,
      "given": "Pierre",
      "family": "No\u00e9",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "Universit\u00e9 Grenoble Alpes CEA LETI  17, rue des Martyrs F 38054 Grenoble Cedex 9 France"
        }
      ]
    }
  ],
  "member": "311",
  "published-online": {
    "date-parts": [
      [
        2018,
        5,
        14
      ]
    ]
  },
  "reference": [
    {
      "key": "e_1_2_7_1_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1038/nmat2009"
    },
    {
      "key": "e_1_2_7_2_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1016/j.sse.2016.07.006"
    },
    {
      "key": "e_1_2_7_3_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1109/IMW.2013.6582084"
    },
    {
      "key": "e_1_2_7_4_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1088/1361-6641/aa7c25"
    },
    {
      "key": "e_1_2_7_5_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1038/nnano.2011.96"
    },
    {
      "key": "e_1_2_7_6_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.7567/JJAP.53.04ED02"
    },
    {
      "key": "e_1_2_7_7_1",
      "first-page": "T130",
      "author": "Takaura N.",
      "year": "2013",
      "journal-title": "2013 Symposium on VLSI Technology"
    },
    {
      "key": "e_1_2_7_8_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1088/1468-6996/16/1/014402"
    },
    {
      "key": "e_1_2_7_9_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1002/adfm.201702243"
    },
    {
      "key": "e_1_2_7_10_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1063/1.4958708"
    },
    {
      "key": "e_1_2_7_11_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1021/acsami.6b11418"
    },
    {
      "volume-title": "2014 Symp. VLSI Technol.",
      "year": "2014",
      "author": "Tai M.",
      "key": "e_1_2_7_12_1"
    },
    {
      "key": "e_1_2_7_13_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1109/IRPS.2013.6532096"
    },
    {
      "key": "e_1_2_7_14_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1002/adma.201505865"
    },
    {
      "key": "e_1_2_7_15_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1039/C5NR04530D"
    },
    {
      "key": "e_1_2_7_16_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1016/j.jallcom.2016.03.159"
    },
    {
      "key": "e_1_2_7_17_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1107/S0567740874004729"
    },
    {
      "key": "e_1_2_7_18_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1002/pssb.201552335"
    },
    {
      "key": "e_1_2_7_19_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1063/1.4974464"
    },
    {
      "key": "e_1_2_7_20_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1088/0022-3719/20/10/012"
    },
    {
      "key": "e_1_2_7_21_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1002/admi.201300027"
    },
    {
      "key": "e_1_2_7_22_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1063/1.4886119"
    },
    {
      "key": "e_1_2_7_23_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1038/srep12612"
    },
    {
      "key": "e_1_2_7_24_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1038/ncomms11983"
    },
    {
      "key": "e_1_2_7_25_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1088/2399-1984/aa8434"
    },
    {
      "key": "e_1_2_7_26_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1021/acs.cgd.5b01714"
    },
    {
      "key": "e_1_2_7_27_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1007/s12274-017-1785-y"
    },
    {
      "key": "e_1_2_7_28_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1038/srep05727"
    },
    {
      "key": "e_1_2_7_29_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1557/jmr.2016.334"
    },
    {
      "key": "e_1_2_7_30_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1107/S0108768104022906"
    },
    {
      "key": "e_1_2_7_31_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1038/srep23843"
    },
    {
      "key": "e_1_2_7_32_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1038/s41598-017-02710-3"
    },
    {
      "key": "e_1_2_7_33_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1016/S0925-8388(97)00625-7"
    },
    {
      "key": "e_1_2_7_34_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1063/1.4948536"
    },
    {
      "key": "e_1_2_7_35_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1111/j.1365-2818.2006.01551.x"
    },
    {
      "key": "e_1_2_7_36_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1039/c3ce26956f"
    },
    {
      "key": "e_1_2_7_37_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1016/j.matdes.2016.11.003"
    },
    {
      "key": "e_1_2_7_38_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1063/1.5000338"
    },
    {
      "key": "e_1_2_7_39_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1039/C7NR01684K"
    },
    {
      "key": "e_1_2_7_40_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1038/nmat3456"
    },
    {
      "key": "e_1_2_7_41_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1038/s41598-016-0001-8"
    },
    {
      "key": "e_1_2_7_42_1",
      "first-page": "33",
      "volume": "6",
      "author": "Kataoka Y.",
      "year": "1989",
      "journal-title": "Rigaku J."
    },
    {
      "key": "e_1_2_7_43_1",
      "doi-asserted-by": "publisher",
      "DOI": "10.1016/j.jsb.2016.12.006"
    },
    {
      "volume-title": "Sample Preparation Handbook for Transmission Electron Microscopy: Methodology",
      "year": "2010",
      "author": "Ayache J.",
      "key": "e_1_2_7_44_1"
    }
  ],
  "container-title": "Small",
  "original-title": [],
  "language": "en",
  "link": [
    {
      "URL": "https://api.wiley.com/onlinelibrary/tdm/v1/articles/10.1002%2Fsmll.201704514",
      "content-type": "application/pdf",
      "content-version": "vor",
      "intended-application": "text-mining"
    },
    {
      "URL": "https://onlinelibrary.wiley.com/doi/pdf/10.1002/smll.201704514",
      "content-type": "unspecified",
      "content-version": "vor",
      "intended-application": "similarity-checking"
    }
  ],
  "deposited": {
    "date-parts": [
      [
        2023,
        9,
        16
      ]
    ],
    "date-time": "2023-09-16T22:39:33Z",
    "timestamp": 1694903973000
  },
  "score": 1,
  "resource": {
    "primary": {
      "URL": "https://onlinelibrary.wiley.com/doi/10.1002/smll.201704514"
    }
  },
  "subtitle": [],
  "short-title": [],
  "issued": {
    "date-parts": [
      [
        2018,
        5,
        14
      ]
    ]
  },
  "references-count": 44,
  "journal-issue": {
    "issue": "24",
    "published-print": {
      "date-parts": [
        [
          2018,
          6
        ]
      ]
    }
  },
  "alternative-id": [
    "10.1002/smll.201704514"
  ],
  "URL": "http://dx.doi.org/10.1002/smll.201704514",
  "relation": {},
  "ISSN": [
    "1613-6810",
    "1613-6829"
  ],
  "subject": [],
  "container-title-short": "Small",
  "published": {
    "date-parts": [
      [
        2018,
        5,
        14
      ]
    ]
  },
  "assertion": [
    {
      "value": "2017-12-26",
      "order": 0,
      "name": "received",
      "label": "Received",
      "group": {
        "name": "publication_history",
        "label": "Publication History"
      }
    },
    {
      "value": "2018-05-14",
      "order": 2,
      "name": "published",
      "label": "Published",
      "group": {
        "name": "publication_history",
        "label": "Publication History"
      }
    }
  ],
  "article-number": "1704514"
}