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

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 (τesp) 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 τesp 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. Colloidal nanoplatelets are low‐cost analogs of quantum wells holding promise for spin‐based quantum technologies. The electron spin lifetimes for typical nanoplatelets are limited to a few picoseconds due to strong electron‐hole exchange interaction. Here through constructing type‐I CdSe/ZnS core/shell and type‐II CdSe/CdTe core/crown nanoplatelets to suppress the exchange interaction, an electron spin lifetime as long as 300 picoseconds is achieved at room temperature.