Cr silicate as a prototype for engineering magnetic phases in air-stable two-dimensional transition-metal silicates

Nassar Doudin; Kayahan Saritas; Jin Cheng Zheng; J. Anibal Boscoboinik; Jerzy T. Sadowski; Padraic Shafer; Alpha T. N’Diaye; Min Li; Sohrab Ismail-Beigi; Eric I. Altman

doi:10.1088/2053-1583/acf0d1

Cr silicate as a prototype for engineering magnetic phases in air-stable two-dimensional transition-metal silicates

Nassar Doudin, Kayahan Saritas, Jin Cheng Zheng, J. Anibal Boscoboinik, Jerzy T. Sadowski, Padraic Shafer, Alpha T. N’Diaye, Min Li, Sohrab Ismail-Beigi, Eric I. Altman

Materials Theory

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Abstract

Identifying environmentally inert, ferromagnetic two-dimensional (2D) materials with high Curie temperatures (T _c) down to the single layer limit has been an obstacle to fundamental studies of 2D magnetism and application of 2D heterostructures to spin-polarized devices. To address this challenge, the growth, structure and magnetic properties of a 2D Cr-silicate single layer on Pt(111) was investigated experimentally and theoretically. The layer was grown by sequentially depositing SiO and Cr followed by annealing in O₂. Scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), and low energy electron microscopy all indicated a well-ordered layer that uniformly covered the surface, with STM and LEED indicating that the silicate relaxed to its favored lattice constant. Further experimental characterizations demonstrated that the Cr was nominally 3+ but with a lower electron density than typical trivalent Cr compounds. Comparison with theory identified a Cr₂Si₂O₉ structure that resembles a single layer of a dehydrogenated dioctahedral silicate. Magnetic circular dichroism in x-ray absorption spectroscopy revealed a ferromagnetically ordered state up to at least 80 K. Theoretical analysis revealed that the Cr in a dehydrogenated Cr-silicate/Pt(111) is more oxidized than Cr in freestanding Cr₂Si₂O₉H₄ layers. This greater oxidation was found to enhance ferromagnetic coupling and suggests that the magnetism may be tuned by doping. The 2D Cr-silicate is the first member of a broad series of possible layered first-row transition metal silicates with magnetic order; thus, this paper introduces a new platform for investigating 2D ferromagnetism and the development of magnetoelectronic and spintronic devices by stacking 2D atomic layers.

Original language	English
Article number	045017
Journal	2D Materials
Volume	10
Issue number	4
DOIs	https://doi.org/10.1088/2053-1583/acf0d1
State	Published - Oct 2023

Funding

This Project was supported by the US Army Research Office under Grant Number W911NF-19-1-0371. This research used resources of the Center for Functional Nanomaterials (CFN) and the National Synchrotron Light Source, which are U.S. Department of Energy Office of Science facilities at Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under Contract No. DE-AC02-05CH11231. The authors acknowledge the use of the West Campus Materials Characterization Core Facility within Yale University.

Funders	Funder number
National Synchrotron Light Source	DE-SC0012704
Army Research Office	W911NF-19-1-0371
Office of Science	DE-AC02-05CH11231

Keywords

2D materials
air stable
ferromagnetism
intrinsic magnetic order
spintronic devices
transition metal silicates

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10.1088/2053-1583/acf0d1

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title = "Cr silicate as a prototype for engineering magnetic phases in air-stable two-dimensional transition-metal silicates",

abstract = "Identifying environmentally inert, ferromagnetic two-dimensional (2D) materials with high Curie temperatures (T c) down to the single layer limit has been an obstacle to fundamental studies of 2D magnetism and application of 2D heterostructures to spin-polarized devices. To address this challenge, the growth, structure and magnetic properties of a 2D Cr-silicate single layer on Pt(111) was investigated experimentally and theoretically. The layer was grown by sequentially depositing SiO and Cr followed by annealing in O2. Scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), and low energy electron microscopy all indicated a well-ordered layer that uniformly covered the surface, with STM and LEED indicating that the silicate relaxed to its favored lattice constant. Further experimental characterizations demonstrated that the Cr was nominally 3+ but with a lower electron density than typical trivalent Cr compounds. Comparison with theory identified a Cr2Si2O9 structure that resembles a single layer of a dehydrogenated dioctahedral silicate. Magnetic circular dichroism in x-ray absorption spectroscopy revealed a ferromagnetically ordered state up to at least 80 K. Theoretical analysis revealed that the Cr in a dehydrogenated Cr-silicate/Pt(111) is more oxidized than Cr in freestanding Cr2Si2O9H4 layers. This greater oxidation was found to enhance ferromagnetic coupling and suggests that the magnetism may be tuned by doping. The 2D Cr-silicate is the first member of a broad series of possible layered first-row transition metal silicates with magnetic order; thus, this paper introduces a new platform for investigating 2D ferromagnetism and the development of magnetoelectronic and spintronic devices by stacking 2D atomic layers.",

keywords = "2D materials, air stable, ferromagnetism, intrinsic magnetic order, spintronic devices, transition metal silicates",

author = "Nassar Doudin and Kayahan Saritas and Zheng, {Jin Cheng} and Boscoboinik, {J. Anibal} and Sadowski, {Jerzy T.} and Padraic Shafer and N{\textquoteright}Diaye, {Alpha T.} and Min Li and Sohrab Ismail-Beigi and Altman, {Eric I.}",

note = "Publisher Copyright: {\textcopyright} 2023 The Author(s). Published by IOP Publishing Ltd",

year = "2023",

month = oct,

doi = "10.1088/2053-1583/acf0d1",

language = "English",

volume = "10",

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T1 - Cr silicate as a prototype for engineering magnetic phases in air-stable two-dimensional transition-metal silicates

AU - Doudin, Nassar

AU - Saritas, Kayahan

AU - Zheng, Jin Cheng

AU - Boscoboinik, J. Anibal

AU - Sadowski, Jerzy T.

AU - Shafer, Padraic

AU - N’Diaye, Alpha T.

AU - Li, Min

AU - Ismail-Beigi, Sohrab

AU - Altman, Eric I.

PY - 2023/10

Y1 - 2023/10

N2 - Identifying environmentally inert, ferromagnetic two-dimensional (2D) materials with high Curie temperatures (T c) down to the single layer limit has been an obstacle to fundamental studies of 2D magnetism and application of 2D heterostructures to spin-polarized devices. To address this challenge, the growth, structure and magnetic properties of a 2D Cr-silicate single layer on Pt(111) was investigated experimentally and theoretically. The layer was grown by sequentially depositing SiO and Cr followed by annealing in O2. Scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), and low energy electron microscopy all indicated a well-ordered layer that uniformly covered the surface, with STM and LEED indicating that the silicate relaxed to its favored lattice constant. Further experimental characterizations demonstrated that the Cr was nominally 3+ but with a lower electron density than typical trivalent Cr compounds. Comparison with theory identified a Cr2Si2O9 structure that resembles a single layer of a dehydrogenated dioctahedral silicate. Magnetic circular dichroism in x-ray absorption spectroscopy revealed a ferromagnetically ordered state up to at least 80 K. Theoretical analysis revealed that the Cr in a dehydrogenated Cr-silicate/Pt(111) is more oxidized than Cr in freestanding Cr2Si2O9H4 layers. This greater oxidation was found to enhance ferromagnetic coupling and suggests that the magnetism may be tuned by doping. The 2D Cr-silicate is the first member of a broad series of possible layered first-row transition metal silicates with magnetic order; thus, this paper introduces a new platform for investigating 2D ferromagnetism and the development of magnetoelectronic and spintronic devices by stacking 2D atomic layers.

AB - Identifying environmentally inert, ferromagnetic two-dimensional (2D) materials with high Curie temperatures (T c) down to the single layer limit has been an obstacle to fundamental studies of 2D magnetism and application of 2D heterostructures to spin-polarized devices. To address this challenge, the growth, structure and magnetic properties of a 2D Cr-silicate single layer on Pt(111) was investigated experimentally and theoretically. The layer was grown by sequentially depositing SiO and Cr followed by annealing in O2. Scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), and low energy electron microscopy all indicated a well-ordered layer that uniformly covered the surface, with STM and LEED indicating that the silicate relaxed to its favored lattice constant. Further experimental characterizations demonstrated that the Cr was nominally 3+ but with a lower electron density than typical trivalent Cr compounds. Comparison with theory identified a Cr2Si2O9 structure that resembles a single layer of a dehydrogenated dioctahedral silicate. Magnetic circular dichroism in x-ray absorption spectroscopy revealed a ferromagnetically ordered state up to at least 80 K. Theoretical analysis revealed that the Cr in a dehydrogenated Cr-silicate/Pt(111) is more oxidized than Cr in freestanding Cr2Si2O9H4 layers. This greater oxidation was found to enhance ferromagnetic coupling and suggests that the magnetism may be tuned by doping. The 2D Cr-silicate is the first member of a broad series of possible layered first-row transition metal silicates with magnetic order; thus, this paper introduces a new platform for investigating 2D ferromagnetism and the development of magnetoelectronic and spintronic devices by stacking 2D atomic layers.

KW - 2D materials

KW - air stable

KW - ferromagnetism

KW - intrinsic magnetic order

KW - spintronic devices

KW - transition metal silicates

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U2 - 10.1088/2053-1583/acf0d1

DO - 10.1088/2053-1583/acf0d1

M3 - Article

AN - SCOPUS:85169897287

SN - 2053-1583

VL - 10

JO - 2D Materials

JF - 2D Materials

IS - 4

M1 - 045017

ER -

Cr silicate as a prototype for engineering magnetic phases in air-stable two-dimensional transition-metal silicates

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