# Microthermoreflectance Characterization of the Band‐Structure Transformations Observed During the Magnetic‐Ordering Transitions of Multilayered 2D Fe3GeTe2 Ferromagnetic Metals

## TL;DR

This paper uses microthermoreflectance to study how the electronic structure of Fe3GeTe2 changes with temperature across different magnetic phases.

## Contribution

The study identifies three distinct optical transitions in Fe3GeTe2 that correlate with specific magnetic phases using μTR spectroscopy.

## Key findings

- Three interband transitions (A1, A2, A3) are identified in Fe3GeTe2 using μTR measurements.
- A1 appears across all temperature ranges, while A2 and A3 are specific to the AI and FM phases.
- DFT calculations show all transitions originate from the spin-down band of Fe 3d electrons.

## Abstract

2D layered ferromagnetic (FM) materials hold significant promise for various applications owing to their hysteretic behavior and the ultrathin magnetic‐ordering control of spin electrons below the Curie temperature (TC). The spin‐polarized order in the FM zone (e.g., T ≤ TC = 225 K for Fe3GeTe2), paramagnetic (PM) zone (e.g., T > TC), and low‐temperature anisotropic (AI) zone (e.g., T < 75 K < TC for Fe3GeTe2) are typically characterized by observing changes in the magnetization and magnetoresistance under the application of an external magnetic (electric) field. However, observing the near‐band‐edge transitions across the FM, PM, and AI regions of a layered magnetic metal is challenging utilizing optical spectroscopy due to its high surface carrier density for shielding incident lights. In this study, three interband transitions, designated as A1, A2, and A3, are measured and identified through temperature‐dependent microthermoreflectance (μTR) measurements of multilayered Fe3GeTe2 metal across a temperature range of 20–300 K, enabling the distinction of the FM, PM, and AI zones using optical methods. The A1 transition (≈1.73 eV) is detected across the entire temperature range of 20–300 K, whereas the A2 transition (≈1.95 eV) appears only in the AI zone below 75 K, and the A3 transition (≈2.23 eV) is observed only in the FM phase below TC (≈225 K). Density functional theory calculations suggest that all transitions (A1–A3) originate from the down‐spin‐polarized band of Fe 3d electrons. Moreover, temperature‐dependent X‐ray diffraction, Raman, magnetization, and magneto‐resistivity measurements are performed to confirm the TC and AI temperatures observed for multilayered FGT by μTR.

Optical band‐edge transitions of metallic hexagonal Fe3GeTe2 multilayers are probed by microthermoreflectance spectroscopy across the temperature ranges associated with the paramagnetic, ferromagnetic (FM), and anisotropic (AI) phases. The A1 transition is detected across all three phases, occurring at the Γ point of the FGT band structure. The A2 feature appears only in the AI phase, and A3 is measured only in the AI and FM phases. All three transitions (A1–A3) originate from the spin‐down band structure of Fe3GeTe2 with Fe d‐d transitions.© 2025 WILEY‐VCH GmbH