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 (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.