Pressure-correlation phase diagram unraveling quantum phase transitions in altermagnetic $ε$-FeOOH and realization of piezo-anomalous Hall effect

Abstract

We establish a pressure-correlation phase diagram that yields multiple pressure-tunable quantum phase transitions in iron oxyhydroxide ($ε$-FeOOH) across three critical pressures, $P_{c1}>P_{c2}>P_{c3}$. The transitions arise from the competition among electron-correlation, crystal-field, and Hund's coupling. First-principles calculations reveal that the earlier reported high-spin (HS) to low-spin (LS) crossover at correlation-sensitive $P_{c1}$ is accompanied by a transition from charge-transfer to Mott insulating (CTI-MI) phase, and a change in the spin-quantization axis (SQA) from $\hat{y}$ to $\hat{x}$. The HS-LS crossover and CTI-MI transition is driven by the simultaneous increase in crystal-field splitting and decrease in Hund's coupling. The critical pressure $P_{c2}$ governing the structural transition from centrosymmetric $Pnnm$ phase to noncentrosymmetric $P2_1nm$ phase is found to be independent of electron-correlation. When correlation is strong, a third critical pressure ($P_{c3}$) emerges in the lower-pressure regime of the phase diagram. Validating the recent experimental observation, $P_{c3}$ is responsible for changing the SQA from $\hat{z}$ to $\hat{y}$. By exhibiting altermagnetism in both $P2_1nm$ and $Pnnm$ phases and possessing finite anomalous Hall conductivity (AHC) only for SQA along $\hat{x}$ and $\hat{y}$, $ε$-FeOOH enables a unique piezo-anomalous Hall effect where one can switch on the AHC at a lower pressure and change its direction at a higher pressure.