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Naturally occurring van der Waals crystals have brought unprecedentedinterest to nanomaterial researchers in recent years. So far, more than 1800layered materials (LMs) have been identified but only a few insulating andnaturally occurring LMs were deeply investigated. Phyllosilicate minerals,which are a class of natural and abundant LMs, have been recently considered asa low-cost source of insulating nanomaterials. Within this family an almostbarely explored material emerges: phlogopite [KMg3(AlSi3)O10(OH)2]. Here wecarry out a high throughput characterization of this LM by employing severalexperimental techniques, corroborating the major findings with first-principlescalculations. We show that monolayers (1L) and few-layers of this material areair and temperature stable, as well as easily obtained by the standardmechanical exfoliation technique, have an atomically flat surface, and lowerbandgap than its bulk counterpart, an unusual trend in LMs. We alsosystematically study the basic properties of ultrathin phlogopite anddemonstrate that natural phlogopite presents iron impurities in its crystallattice, which decreases its bandgap from about 7 eV to 3.6 eV. Finally, wecombine phlogopite crystals with 1L-WS2 in ultrathin van der Waalsheterostructures and present a photoluminescence study, revealing a significantenhancement on the 1L-WS2 optical quality (i.e., higher recombinationefficiency through neutral excitons) similarly to that obtained on 1L-WS2/hBNheterostructures. Our proof-of-concept study shows that phlogopite should beregarded as a good and promising candidate for LM-based applications as alow-cost layered nanomaterial.

Exploring the structural and optoelectronic properties of natural insulating phlogopite in van der Waals heterostructures