Quantum-Dots-on-Silicon
Hybrids: Towards Energy Transfer Based
Nanostructured
Photovoltaics.
Yuri
Gartstein
Department of Physics, The
Energy transfer (ET) based hybrids comprise
components with a clear separation of the functionalities: one component of the
nanostructure is chosen for its strong light-matter
interaction while the other for its high charge-carrier mobilities. Conceptually
reminiscent of photosynthesis, solar light is envisioned to be harvested in the
well absorbing component followed by exciton diffusion and ET across the
interface with the subsequent separation and transport of charge carriers
entirely within the high-mobility semiconductor component. The crucial energy
exchange between the components is enabled by the strong near-field
electromagnetic interactions. The excitonic sensitization is particularly
appealing for crystalline silicon as it would eliminate the weak solar light
absorption in the indirect band-gap Si as a defining design factor thus
possibly leading to ultrathin silicon devices.
In this talk I will discuss recent
progress of our collaborative team from Departments of Physics and Materials
Science and Engineering in studying ET from photoexcited colloidal quantum dots
(QDs) into Si substrates. The quantitative analysis
of the time-resolved photoluminescence reveals that this ET can be highly
efficient over a broad range of wavelengths including into ultrathin (~ 100 nm)
Si nano membranes. It is demonstrated that ET occurs by means of both
non-radiative (NRET) and radiative (RET) mechanisms exhibiting different
distance and wavelength dependences. While NRET corresponds to the direct
production of electron-hole pairs in Si, in the RET process the QD excitons
preferentially decay into photonic modes propagating within Si (waveguiding modes
in thin layers).We find that our systems make an interesting “case study”
for the general problem of modification of radiative lifetimes of
electric-dipole emitters by polarizable environments. As a further step towards
exploration and utilization of optically thick QD assemblies, we provide
evidence for the concept of directed ET by analyzing energy relaxation pathways
through QD-size-gradient bilayer structures on Si substrates.
This research has been supported by
grants from NSF (DMR-1207123) and DOE/BES (DE-SC0010697).
Host: Prof. V. Podzorov