Linear Magnetoelectric Phase in Ultrathin <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:msub><mml:mrow><mml:mi>MnPS</mml:mi></mml:mrow><mml:mn>3</mml:mn></mml:msub></mml:math> Probed by Optical Second Harmonic Generation
Hao Chu, Chang Jae Roh, Joshua O. Island, Chen Li, Sungmin Lee, Jingjing Chen, Je‐Geun Park, Andrea F. Young, Jong Seok Lee, David Hsieh
Abstract
The transition metal thiophosphates MPS_{3} (M=Mn, Fe, Ni) are a class of van der Waals stacked insulating antiferromagnets that can be exfoliated down to the ultrathin limit. MnPS_{3} is particularly interesting because its Néel ordered state breaks both spatial-inversion and time-reversal symmetries, allowing for a linear magnetoelectric phase that is rare among van der Waals materials. However, it is unknown whether this unique magnetic structure of bulk MnPS_{3} remains stable in the ultrathin limit. Using optical second harmonic generation rotational anisotropy, we show that long-range linear magnetoelectric type Néel order in MnPS_{3} persists down to at least 5.3 nm thickness. However an unusual mirror symmetry breaking develops in ultrathin samples on SiO_{2} substrates that is absent in bulk materials, which is likely related to substrate induced strain.