Evolution of Highly Anisotropic Magnetism in the Titanium-Based Kagome Metals LnTi3Bi4 (Ln: La···Gd3+, Eu2+, Yb2+)

Brenden R. Ortiz; Hu Miao; David S. Parker; Fazhi Yang; German D. Samolyuk; Eleanor M. Clements; Anil Rajapitamahuni; Turgut Yilmaz; Elio Vescovo; Jiaqiang Yan; Andrew F. May; Michael A. McGuire

doi:10.1021/acs.chemmater.3c02289

Evolution of Highly Anisotropic Magnetism in the Titanium-Based Kagome Metals LnTi₃Bi₄ (Ln: La···Gd³⁺, Eu²⁺, Yb²⁺)

Brenden R. Ortiz, Hu Miao, David S. Parker, Fazhi Yang, German D. Samolyuk, Eleanor M. Clements, Anil Rajapitamahuni, Turgut Yilmaz, Elio Vescovo, Jiaqiang Yan, Andrew F. May, Michael A. McGuire

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Abstract

Here, we present a family of titanium-based kagome metals of the form LnTi₃Bi₄ (Ln: La···Gd³⁺, Eu²⁺, Yb²⁺). Four previously unreported compounds are presented: YbTi₃Bi₄, GdTi₃Bi₄, NdTi₃Bi₄, and PrTi₃Bi₄. Single-crystal growth methods are provided alongside detailed magnetic and thermodynamic measurements across the entire series. The LnTi₃Bi₄ family of compounds are orthorhombic (Fmmm), layered compounds that exhibit slightly distorted titanium-based kagome nets interwoven with zigzag lanthanide-based (Ln) chains. Crystals are easily exfoliated parallel to the kagome sheets, and angular resolved photoemission (ARPES) measurements highlight the intricacy of the electronic structure in these compounds. Density functional theory (DFT) and ARPES studies find Dirac points near the Fermi level, consistent with the kagome-derived band structure. The magnetic properties and the associated anisotropy emerge from the quasi-1D zigzag chains of Ln and impart a wide array of magnetic ground states ranging from anisotropic ferromagnetism to complex antiferromagnetism with a cascade of metamagnetic transitions. The combination of the kagome-based electronic structure and highly anisotropic Ln-based magnetism on an exfoliatable platform cements the LnTi₃Bi₄ family as an interesting addition to the ever-expanding suite of kagome metals.

Original language	English
Pages (from-to)	9756-9773
Number of pages	18
Journal	Chemistry of Materials
Volume	35
Issue number	22
DOIs	https://doi.org/10.1021/acs.chemmater.3c02289
State	Published - Nov 28 2023

Funding

The work of H.M., F.Y., E.M.C., D.S.P., J.Y., A.F.M., and M.A.M. was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division. Research directed by B.R.O. and G.D.S. is sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the US Department of Energy. The authors thank the X-ray laboratory of the Oak Ridge National Laboratory Spallation Neutron Source for use of their MWL120 Real-Time Back-Reflection Laue Camera System used to orient single crystals. This research utilized beamline 21-ID-1 of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. The authors thank Pyeongjae Park, Andrew D. Christianson, Denver Strong, Ganesh Pokharel, and David Rujivachirapong for their support, editing, and proofreading. Research directed by B.R.O. and G.D.S. is sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the US Department of Energy. The work of H.M., F.Y., E.M.C., D.S.P., J.Y., A.F.M., and M.A.M. was supported by the U.S. Department of Energy (DOE), Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division. The authors thank the X-ray laboratory of the Oak Ridge National Laboratory Spallation Neutron Source for use of their MWL120 Real-Time Back-Reflection Laue Camera System used to orient single crystals. This research utilized beamline 21-ID-1 of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. The authors thank Pyeongjae Park, Andrew D. Christianson, Denver Strong, Ganesh Pokharel, and David Rujivachirapong for their support, editing, and proofreading.

Funders	Funder number
Andrew D. Christianson, Denver Strong
Ganesh Pokharel
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Brookhaven National Laboratory	DE-SC0012704
Division of Materials Sciences and Engineering

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Ortiz, B. R., Miao, H., Parker, D. S., Yang, F., Samolyuk, G. D., Clements, E. M., Rajapitamahuni, A., Yilmaz, T., Vescovo, E., Yan, J., May, A. F., & McGuire, M. A. (2023). Evolution of Highly Anisotropic Magnetism in the Titanium-Based Kagome Metals LnTi₃Bi₄ (Ln: La···Gd³⁺, Eu²⁺, Yb²⁺). Chemistry of Materials, 35(22), 9756-9773. https://doi.org/10.1021/acs.chemmater.3c02289

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title = "Evolution of Highly Anisotropic Magnetism in the Titanium-Based Kagome Metals LnTi3Bi4 (Ln: La···Gd3+, Eu2+, Yb2+)",

abstract = "Here, we present a family of titanium-based kagome metals of the form LnTi3Bi4 (Ln: La···Gd3+, Eu2+, Yb2+). Four previously unreported compounds are presented: YbTi3Bi4, GdTi3Bi4, NdTi3Bi4, and PrTi3Bi4. Single-crystal growth methods are provided alongside detailed magnetic and thermodynamic measurements across the entire series. The LnTi3Bi4 family of compounds are orthorhombic (Fmmm), layered compounds that exhibit slightly distorted titanium-based kagome nets interwoven with zigzag lanthanide-based (Ln) chains. Crystals are easily exfoliated parallel to the kagome sheets, and angular resolved photoemission (ARPES) measurements highlight the intricacy of the electronic structure in these compounds. Density functional theory (DFT) and ARPES studies find Dirac points near the Fermi level, consistent with the kagome-derived band structure. The magnetic properties and the associated anisotropy emerge from the quasi-1D zigzag chains of Ln and impart a wide array of magnetic ground states ranging from anisotropic ferromagnetism to complex antiferromagnetism with a cascade of metamagnetic transitions. The combination of the kagome-based electronic structure and highly anisotropic Ln-based magnetism on an exfoliatable platform cements the LnTi3Bi4 family as an interesting addition to the ever-expanding suite of kagome metals.",

author = "Ortiz, {Brenden R.} and Hu Miao and Parker, {David S.} and Fazhi Yang and Samolyuk, {German D.} and Clements, {Eleanor M.} and Anil Rajapitamahuni and Turgut Yilmaz and Elio Vescovo and Jiaqiang Yan and May, {Andrew F.} and McGuire, {Michael A.}",

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T1 - Evolution of Highly Anisotropic Magnetism in the Titanium-Based Kagome Metals LnTi3Bi4 (Ln: La···Gd3+, Eu2+, Yb2+)

AU - Ortiz, Brenden R.

AU - Miao, Hu

AU - Parker, David S.

AU - Yang, Fazhi

AU - Samolyuk, German D.

AU - Clements, Eleanor M.

AU - Rajapitamahuni, Anil

AU - Yilmaz, Turgut

AU - Vescovo, Elio

AU - Yan, Jiaqiang

AU - May, Andrew F.

AU - McGuire, Michael A.

PY - 2023/11/28

Y1 - 2023/11/28

N2 - Here, we present a family of titanium-based kagome metals of the form LnTi3Bi4 (Ln: La···Gd3+, Eu2+, Yb2+). Four previously unreported compounds are presented: YbTi3Bi4, GdTi3Bi4, NdTi3Bi4, and PrTi3Bi4. Single-crystal growth methods are provided alongside detailed magnetic and thermodynamic measurements across the entire series. The LnTi3Bi4 family of compounds are orthorhombic (Fmmm), layered compounds that exhibit slightly distorted titanium-based kagome nets interwoven with zigzag lanthanide-based (Ln) chains. Crystals are easily exfoliated parallel to the kagome sheets, and angular resolved photoemission (ARPES) measurements highlight the intricacy of the electronic structure in these compounds. Density functional theory (DFT) and ARPES studies find Dirac points near the Fermi level, consistent with the kagome-derived band structure. The magnetic properties and the associated anisotropy emerge from the quasi-1D zigzag chains of Ln and impart a wide array of magnetic ground states ranging from anisotropic ferromagnetism to complex antiferromagnetism with a cascade of metamagnetic transitions. The combination of the kagome-based electronic structure and highly anisotropic Ln-based magnetism on an exfoliatable platform cements the LnTi3Bi4 family as an interesting addition to the ever-expanding suite of kagome metals.

AB - Here, we present a family of titanium-based kagome metals of the form LnTi3Bi4 (Ln: La···Gd3+, Eu2+, Yb2+). Four previously unreported compounds are presented: YbTi3Bi4, GdTi3Bi4, NdTi3Bi4, and PrTi3Bi4. Single-crystal growth methods are provided alongside detailed magnetic and thermodynamic measurements across the entire series. The LnTi3Bi4 family of compounds are orthorhombic (Fmmm), layered compounds that exhibit slightly distorted titanium-based kagome nets interwoven with zigzag lanthanide-based (Ln) chains. Crystals are easily exfoliated parallel to the kagome sheets, and angular resolved photoemission (ARPES) measurements highlight the intricacy of the electronic structure in these compounds. Density functional theory (DFT) and ARPES studies find Dirac points near the Fermi level, consistent with the kagome-derived band structure. The magnetic properties and the associated anisotropy emerge from the quasi-1D zigzag chains of Ln and impart a wide array of magnetic ground states ranging from anisotropic ferromagnetism to complex antiferromagnetism with a cascade of metamagnetic transitions. The combination of the kagome-based electronic structure and highly anisotropic Ln-based magnetism on an exfoliatable platform cements the LnTi3Bi4 family as an interesting addition to the ever-expanding suite of kagome metals.

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SN - 0897-4756

VL - 35

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EP - 9773

JO - Chemistry of Materials

JF - Chemistry of Materials

IS - 22

ER -

Evolution of Highly Anisotropic Magnetism in the Titanium-Based Kagome Metals LnTi₃Bi₄ (Ln: La···Gd³⁺, Eu²⁺, Yb²⁺)

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