Layered silicon nanosheets (SiNSs)
have attracted considerable
attention owing to their unique combination of chemical and physical
properties, which makes them an exciting candidate for next-generation
on-chip light sources and lasers. Despite over 150 years of research
on SiNSs, the effects of the CaSi2 precursor quality on
SiNSs have not been studied. Here, we report a comparison of CaSi2 (and SiNSs derived therefrom) synthesized from two reaction
pathways: (1) melting Ca and Si (elemental melting, or EM-CaSi2) and (2) the less-explored reaction between CaH2 and Si (hydride synthesis, or HS-CaSi2). We demonstrate
that both reaction pathways lead to CaSi2, but the HS-CaSi2 pathway requires only a single step without the need to melt
the CaSi2 product and at a temperature below the peritectic
decomposition of CaSi2. We find that the EM-CaSi2 exhibits grains that lay flat against the substrate, whereas the
HS-CaSi2 has little preferred orientation. We deintercalated
both EM- and HS-CaSi2 with HCl at −35 °C to
yield hydrogen-terminated SiNSs. We characterized the SiNSs and found
that the HS-SiNSs and EM-SiNSs exhibit properties that are nearly
identical, with the exception that the morphology of the precursor
is imparted to the SiNSs. These results provide the community with
a one-step method to synthesize CaSi2 and demonstrate that
the morphology of CaSi2 and SiNSs can be controlled with
different synthetic techniques.