Dielectric and Wavefunction Engineering of Electron Spin Lifetime in Colloidal Nanoplatelet Heterostructures

Abstract Colloidal semiconductor nanoplatelets (NPLs) have emerged as low‐cost and free‐standing alternates of traditional quantum wells. The giant heavy‐ and light‐hole splitting in NPLs allows for efficient optical spin injection. However, the electron spin lifetimes for prototypical CdSe NPLs are within a few picoseconds, likely limited by strong electron‐hole exchange in these quantum‐ and dielectric‐confined materials. Here how this hurdle can be overcome with engineered NPL‐heterostructures is demonstrated. By constructing type‐I CdSe/ZnS core/shell NPLs, dielectric screening inside the core is strongly enhanced, prolonging the electron spin polarization time (τ_esp) to over 30 ps (or 60 ps electron spin‐flip time). Alternatively, by growing type‐II CdSe/CdTe core/crown NPLs to spatially separate electron and hole wavefunctions, the electron‐hole exchange is strongly suppressed, resulting in τ_esp as long as 300 ps at room temperature. This study not only exemplifies how the well‐established synthetic chemistry of colloidal heterostructures can aid in spin dynamics control but also establishes the feasibility of room‐temperature coherent spin manipulation in colloidal NPLs.