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Main Authors: Philip, Reshna Elsa, Vyas, Pooja, Joy, Nikhil Joseph, Kuila, Sandip Kumar, Beniwal, Sonia, Magar, Akshata, Shukla, Dinesh Kumar, Jana, Partha Pratim, Kumar, Amit, Alam, Aftab, Balakrishnan, Jayakumar, Manni, Soham
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2512.10885
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author Philip, Reshna Elsa
Vyas, Pooja
Joy, Nikhil Joseph
Kuila, Sandip Kumar
Beniwal, Sonia
Magar, Akshata
Shukla, Dinesh Kumar
Jana, Partha Pratim
Kumar, Amit
Alam, Aftab
Balakrishnan, Jayakumar
Manni, Soham
author_facet Philip, Reshna Elsa
Vyas, Pooja
Joy, Nikhil Joseph
Kuila, Sandip Kumar
Beniwal, Sonia
Magar, Akshata
Shukla, Dinesh Kumar
Jana, Partha Pratim
Kumar, Amit
Alam, Aftab
Balakrishnan, Jayakumar
Manni, Soham
contents Spin-gapless semiconductors (SGSs) that simultaneously host fully compensated ferrimagnetism are highly sought for energy-efficient and stray-field-free spintronic technologies, yet their realization in chemically disordered systems has remained elusive. Here, we demonstrate that the binary Heusler alloy Cr3Al despite adopting a fully A2-disordered structure exhibits a rare coexistence of SGS transport and a fully compensated ferrimagnetic (FCF) ground state. Single-crystalline and polycrystalline Cr3Al samples were synthesized, and comprehensive structural analyses using single crystal XRD, synchrotron powder XRD, and neutron powder diffraction reveal complete Cr/Al site mixing. Remarkably, this chemical disorder does not disrupt magnetic order; instead, magnetization, X-ray magnetic circular dichroism (XMCD), and temperature-dependent neutron diffraction establish a robust compensated ferrimagnetic state with a vanishingly small ordered moment of 0.1(1) muB/f.u and a high Curie temperature of 773(2) K. Electrical and thermal transport measurements uncover clear SGS characteristics, including weak temperature-dependent conductivity, very low Seebeck coefficients, and electron-hole compensated transport. Hall measurements show unusual temperature-dependent carrier concentrations consistent with disorder-modified electronic states. First-principles calculations on an A2-disordered SQS structure reproduce the experimentally observed negligibly small magnetization (0.0072 muB/f.u) and reveal a vanishing spin-up band gap unambiguously supporting SGS behavior driven by chemical disorder. Our results identify Cr3Al as the first experimentally verified A2-disordered Heusler alloy exhibiting both fully compensated ferrimagnetism and spin-gapless semiconducting transport, positioning it as a robust and disorder-tolerant platform for next-generation, high-temperature spintronic devices.
format Preprint
id arxiv_https___arxiv_org_abs_2512_10885
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Disorder mediated fully compensated ferrimagnetic spin-gapless semiconducting behaviour in Cr3Al Heusler alloy
Philip, Reshna Elsa
Vyas, Pooja
Joy, Nikhil Joseph
Kuila, Sandip Kumar
Beniwal, Sonia
Magar, Akshata
Shukla, Dinesh Kumar
Jana, Partha Pratim
Kumar, Amit
Alam, Aftab
Balakrishnan, Jayakumar
Manni, Soham
Materials Science
Strongly Correlated Electrons
Spin-gapless semiconductors (SGSs) that simultaneously host fully compensated ferrimagnetism are highly sought for energy-efficient and stray-field-free spintronic technologies, yet their realization in chemically disordered systems has remained elusive. Here, we demonstrate that the binary Heusler alloy Cr3Al despite adopting a fully A2-disordered structure exhibits a rare coexistence of SGS transport and a fully compensated ferrimagnetic (FCF) ground state. Single-crystalline and polycrystalline Cr3Al samples were synthesized, and comprehensive structural analyses using single crystal XRD, synchrotron powder XRD, and neutron powder diffraction reveal complete Cr/Al site mixing. Remarkably, this chemical disorder does not disrupt magnetic order; instead, magnetization, X-ray magnetic circular dichroism (XMCD), and temperature-dependent neutron diffraction establish a robust compensated ferrimagnetic state with a vanishingly small ordered moment of 0.1(1) muB/f.u and a high Curie temperature of 773(2) K. Electrical and thermal transport measurements uncover clear SGS characteristics, including weak temperature-dependent conductivity, very low Seebeck coefficients, and electron-hole compensated transport. Hall measurements show unusual temperature-dependent carrier concentrations consistent with disorder-modified electronic states. First-principles calculations on an A2-disordered SQS structure reproduce the experimentally observed negligibly small magnetization (0.0072 muB/f.u) and reveal a vanishing spin-up band gap unambiguously supporting SGS behavior driven by chemical disorder. Our results identify Cr3Al as the first experimentally verified A2-disordered Heusler alloy exhibiting both fully compensated ferrimagnetism and spin-gapless semiconducting transport, positioning it as a robust and disorder-tolerant platform for next-generation, high-temperature spintronic devices.
title Disorder mediated fully compensated ferrimagnetic spin-gapless semiconducting behaviour in Cr3Al Heusler alloy
topic Materials Science
Strongly Correlated Electrons
url https://arxiv.org/abs/2512.10885