Rapid Suppression of Quantum Many-Body Magnetic Exciton in Doped van der Waals Antiferromagnet (Ni,Cd)PS<sub>3</sub>

Kim, Junghyun; Na, Woongki; Kim, Jonghyeon; Park, Pyeongjae; Zhang, Kaixuan; Hwang, Inho; Son, Young-Woo; Kim, Jae Hoon; Cheong, Hyeonsik; Park, Je-Geun

doi:10.1021/acs.nanolett.3c02677

Nano Lett.

2023

DOI: 10.1021/acs.nanolett.3c02677

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Rapid Suppression of Quantum Many-Body Magnetic Exciton in Doped van der Waals Antiferromagnet (Ni,Cd)PS₃

Junghyun Kim,

Woongki Na,

Jonghyeon Kim

et al.

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2024

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Cited by 4 publications

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Optical Probe of Magnetic Ordering Structure and Spin‐Entangled Excitons in Mn‐Substituted NiPS₃

Lee,

Choi

et al. 2024

Adv Funct Materials

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In van der Waals magnets, the interplay between magneto‐excitonic coupling and optical phenomena opens avenues for directly probing magnetic ordering structures, manipulating excitonic properties through magnetic fields, and exploring quantum entanglement between electronic and magnetic states. Notably, NiPS3 stands out for its capacity to host spin‐entangled excitons, where the excitonic states are intricately tied with the material's spin configuration. Herein, it is experimentally showcased that the spin‐entangled excitons can be utilized for detecting the magnetic easy axis in Ni1‐xMnxPS3 (x = 0–0.1). The end members of this series exhibit distinct magnetic ordering patterns and easy axes: zigzag ordering with magnetic moments aligned along the a‐axis for NiPS3 versus Néel ordering with the out‐of‐plane easy axis for MnPS3. By combining angle‐resolved exciton photoluminescence with magnetic susceptibility measurements, it is observed that the magnetic easy axis rotates away from the local spin chain direction with increasing Mn content. Moreover, through a comprehensive thermal and substitution study, it is demonstrated that the energy and lifetime of spin‐entangled excitons are governed by two spin‐flip processes and are drastically influenced by disparate electronic states. These findings not only provide optical means to map out magnetic ordering structures but also offer insights into decoherence processes in spin‐exciton entangled states.

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Optical Probe of Magnetic Ordering Structure and Spin‐Entangled Excitons in Mn‐Substituted NiPS₃

Lee,

Choi

et al. 2024

Adv Funct Materials

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Optical Detection of Weak Magnetic Transitions via Photoluminescence in Cr‐Doped Van Der Waals Antiferromagnets

Xing,

Chen,

Zhang

et al. 2024

Advanced Optical Materials

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Abstract2D van der Waals antiferromagnets, MPX3 (M = Fe, Cr, and Mn; X = S and Se), are promising candidates for spintronic devices owing to their advantageous structural and magnetic properties. However, their insulating properties and high‐field requirements make magnetic characterization in 2D MPX3 challenging. Fortunately, the correlation between magnetic and optical properties in MPX3 crystals provides an optical approach to investigate their magnetic properties. Herein, Cr atoms are used to modulate the magnetic properties of MnPS3, with photoluminescence (PL) techniques used to investigate the effect of doping. Results show a new PL peak in Cr‐doped MnPS3 crystals, with distinct temperature‐dependent PL behaviors compared to the undoped host. The influence of doping concentration, temperature, and thickness on PL is investigated. Surprisingly, even when long‐range magnetic ordering is completely disrupted, the temperature‐dependent PL properties of Cr‐doped MnPS3 (CrxMn1 − xPS3) still follow the Néel transition behavior of MnPS3, showing the presence of local antiferromagnetism in CrxMn1 − xPS3. This study further substantiates the correlation between magnetic ordering and PL in MnPS3 and demonstrates that PL is a powerful tool for detecting weak local magnetism in 2D MPX3 crystals.

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Charge-driven first-order magnetic transition in NiPS₃

Hwang,

Park,

Hyun Kim

et al. 2024

J. Phys.: Condens. Matter

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Cross-coupling among the fundamental degrees of freedom in solids has been a long-standing problem in condensed matter physics. Despite its progress using predominantly three-dimensional materials, how the same physics plays out for two-dimensional materials is unknown. Here, we show that using 31P nuclear magnetic resonance (NMR), the van der Waals antiferromagnet NiPS3 undergoes a first-order magnetic phase transition due to the strong charge-spin coupling in a honeycomb lattice. Our 31P NMR spectrum near the N´eel ordering temperature TN = 155 K exhibits the coexistence of paramagnetic and antiferromagnetic phases within a finite temperature range. Furthermore, we observed a discontinuity in the order parameter at TN and the complete absence of critical behavior of spin fluctuations above TN , decisively establishing the first-order nature of the magnetic transition. We propose that a charge stripe instability arising from a Zhang-Rice triplet ground state triggers the first-order magnetic transition.

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Rapid Suppression of Quantum Many-Body Magnetic Exciton in Doped van der Waals Antiferromagnet (Ni,Cd)PS₃

Cited by 4 publications

References 16 publications

Optical Probe of Magnetic Ordering Structure and Spin‐Entangled Excitons in Mn‐Substituted NiPS₃

Optical Probe of Magnetic Ordering Structure and Spin‐Entangled Excitons in Mn‐Substituted NiPS₃

Optical Detection of Weak Magnetic Transitions via Photoluminescence in Cr‐Doped Van Der Waals Antiferromagnets

Charge-driven first-order magnetic transition in NiPS₃

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Rapid Suppression of Quantum Many-Body Magnetic Exciton in Doped van der Waals Antiferromagnet (Ni,Cd)PS3

Cited by 4 publications

References 16 publications

Optical Probe of Magnetic Ordering Structure and Spin‐Entangled Excitons in Mn‐Substituted NiPS3

Optical Probe of Magnetic Ordering Structure and Spin‐Entangled Excitons in Mn‐Substituted NiPS3

Optical Detection of Weak Magnetic Transitions via Photoluminescence in Cr‐Doped Van Der Waals Antiferromagnets

Charge-driven first-order magnetic transition in NiPS3

Contact Info

Product

Resources

About

Rapid Suppression of Quantum Many-Body Magnetic Exciton in Doped van der Waals Antiferromagnet (Ni,Cd)PS₃

Optical Probe of Magnetic Ordering Structure and Spin‐Entangled Excitons in Mn‐Substituted NiPS₃

Optical Probe of Magnetic Ordering Structure and Spin‐Entangled Excitons in Mn‐Substituted NiPS₃

Charge-driven first-order magnetic transition in NiPS₃