title: Direct observation of rapid discrete spectral dynamics in single colloidal CdSe-CdS core-shell quantum dots.
abstract: We measure the anomalous spectral diffusion of single colloidal quantum dots over eight temporal decades simultaneously by combining single-molecule spectroscopy and photon-correlation Fourier spectroscopy. Our technique distinguishes between discrete and continuous dynamics and directly reveals that the quasicontinuous spectral diffusion observed using conventional spectroscopy is composed of rapid, discrete spectral jumps. Despite their multiple time scales, these dynamics can be captured by a single mechanism whose parameters vary widely between dots and over time in individual dots.
authors.affiliation: Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, USA.
authors.forename: Andrew P
authors.initials: AP
authors.lastname: Beyler
authors.forename: Lisa F
authors.initials: LF
authors.lastname: Marshall
authors.forename: Jian
authors.initials: J
authors.lastname: Cui
authors.forename: Xavier
authors.initials: X
authors.lastname: Brokmann
authors.forename: Moungi G
authors.initials: MG
authors.lastname: Bawendi
mesh_terms: D019187:Cadmium Compounds / Q000737:chemistry*; D003102:Colloids / Q000737:chemistry*; D004058:Diffusion; D005583:Fourier Analysis; D008956:Models, Chemical; D045663:Quantum Dots; D018036:Selenium Compounds / Q000737:chemistry*; D013057:Spectrum Analysis / Q000379:methods; D013440:Sulfides / Q000737:chemistry*
chemical_list: D019187:Cadmium Compounds; D003102:Colloids; D018036:Selenium Compounds; D013440:Sulfides; C034939:cadmium sulfide; C058667:cadmium selenide