Evidence for the novel type of orbital Fulde-Ferrell-Larkin-Ovchinnikov state in the bulk limit of 2H-NbSe2

The Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state, an unusual superconducting state, defies high magnetic fields beyond the Pauli paramagnetic limit. It exhibits a spatial modulation of the superconducting order parameter in real space and is exceptionally rare. Recently, an even more exotic variant - the orbital FFLO state - was predicted and identified in the transition metal dichalcogenide superconductor 2H-NbSe2. This state emerges in thin samples with thicknesses below ~40 nm, at the boundary between two and three dimensions. The complex interplay between Ising spin orbit coupling and the Pauli paramagnetic effect can lead to a stabilization of the FFLO state in a relatively large range of the magnetic phase diagram, even well below the Pauli limit. In this study, we present experimental evidence of the formation of this orbital FFLO state in bulk 2H-NbSe2 samples. This evidence was obtained using high-resolution DC magnetization and magnetic torque experiments in magnetic fields applied strictly parallel to the NbSe2 basal plane. Both quantities display a crossover to a discontinuous first-order superconducting transition at the normal state boundary in magnetic fields of 4 T and above. This is usually seen as a sign that Pauli paramagnetic pair breaking effects affect the superconducting state. The magnetic torque reveals a small step-like reversible anomaly, indicating a magnetic field-induced thermodynamic phase transition within the superconducting state. This anomaly bears many similarities to the FFLO transitions in other FFLO superconductors, suggesting the potential existence of an orbital FFLO state in bulk 2H-NbSe2 samples. Additionally, we observe a pronounced in-plane 6-fold symmetry of the upper critical field in the field range above this phase transition, which has previously been interpreted as a hallmark of the orbital FFLO state in thin 2H-NbSe2.