Programmed
alloying within a van der Waals (vdW) semiconductor
monolayer (ML) is achieved by metalorganic vapor-phase epitaxy. Specifically,
two versions of on-ML alloying are demonstrated by precise controls
of time-lapse vapor pressures during the single-crystalline WS2x
Se2(1–x) ML growth, where the alloying degree, x, is either
continuously or discretely directed on the MLs in the entire range
of 0 ≤ x ≤ 1. With this, on-ML band
gap modulation is accomplished in the forms of either graded or discrete
intra-ML junctions, leading to atomically thin multispectral photodetectors
by a spatially resolved manner at the nanoscales.