Quantum Engineering of Landau Levels Using Isotopes in Graphene‐Like Graphite

ABSTRACT Landau levels are cornerstones of a wide range of quantum phenomena and applications. Understanding the impact of the gauge field, or pseudomagnetic field, on the electronic structure of 2D materials is critical for manipulating Landau electrodynamics. Although extensive theoretical and experimental studies have been carried out to probe pseudomagnetic field in graphene, most of them have been focused on the strain‐ and substrate‐engineering methods and magnetotransport properties. Here, we present using graphite as a unique material testbed for realizing isotope‐induced pseudomagnetic field. Using magneto‐Raman spectroscopy, we show that pure graphite and ‐doped graphite both exhibit graphene‐like Landau level transitions. Remarkably, we demonstrate that ‐doping leads to splitting of the Landau level transitions, a signature of pseudomagnetic field on the scale of 0.2 T. Moreover, the split Landau level transitions selectively couple with the G band phonon in distinct energy ranges. Our results highlight isotope doping as a feasible material engineering method of creating pseudomagnetic field and tuning magneto‐optical properties in 2D quantum materials.