Bright Silicon Nanocrystals from a Liquid Precursor: Quasi-Direct Recombination with High Quantum Yield

• Published in: ACS nano 2020-04, Vol.14 (4), p.3858-3867
• Main Authors: Pringle, Todd A, Hunter, Katharine I, Brumberg, Alexandra, Anderson, Kenneth J, Fagan, Jeffrey A, Thomas, Salim A, Petersen, Reed J, Sefannaser, Mahmud, Han, Yulun, Brown, Samuel L, Kilin, Dmitri S, Schaller, Richard D, Kortshagen, Uwe R, Boudjouk, Philip Raymond, Hobbie, Erik K
• Format: Article
• Language: English
• Subjects: INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; liquid silane; photoluminescence quantum yield; quantum confinement; silicon nanocrystals; surface effects
• ISSN: 1936-0851; 1936-086X
• DOI: 10.1021/acsnano.9b09614

Silicon nanocrystals (SiNCs) with bright bandgap photoluminescence (PL) are of current interest for a range of potential applications, from solar windows to biomedical contrast agents. Here, we use the liquid precursor cyclohexasilane (Si6H12) for the plasma synthesis of colloidal SiNCs with exemplary core emission. Through size separation executed in an oxygen-shielded environment, we achieve PL quantum yields (QYs) approaching 70% while exposing intrinsic constraints on efficient core emission from smaller SiNCs. Time-resolved PL spectra of these fractions in response to femtosecond pulsed excitation reveal a zero-phonon radiative channel that anticorrelates with QY, which we model using advanced computational methods applied to a 2 nm SiNC. Our results offer additional insight into the photophysical interplay of the nanocrystal surface, quasi-direct recombination, and efficient SiNC core PL.