Browsing by Author "Penzo, Erika"
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Item Light-Driven Permanent Charge Separation across a Hybrid Zero-Dimensional/Two-Dimensional Interface(2020-04) Kriegel, Ilka; Ghini, Michele; Bellani, Sepastiano; Zhang, Kehao; Jansons, Adam W.; Crockett, Brandon M.; Koskela, Kristopher M.; Barnard, Edward S.; Penzo, Erika; Hutchison, James E.; Robinson, Joshua A.; Manna, Liberato; Borys, Nicholas J.; Schuck, P. JamesWe report the first demonstration of light-driven permanent charge separation across an ultrathin solid-state zero-dimensional (0D)/2D hybrid interface by coupling photoactive Sn-doped In2O3 nanocrystals with monolayer MoS2, the latter serving as a hole collector. We demonstrate that the nanocrystals in this device-ready architecture act as local light-controlled charge sources by quasi-permanently donating ∼5 holes per nanocrystal to the monolayer MoS2. The amount of photoinduced contactless charge transfer to the monolayer MoS2 competes with what is reached in electrostatically gated devices. Thus, we have constructed a hybrid bilayer structure in which the electrons and holes are separated into two different solid-state materials. The temporal evolution of the local doping levels of the monolayer MoS2 follows a capacitive charging model with effective total capacitances in the femtofarad regime and areal capacitances in the μF cm–2 range. This analysis indicates that the 0D/2D hybrid system may be able to store light energy at densities of at least μJ cm–2, presenting new potential foundational building blocks for next-generation nanodevices that can remotely control local charge density, power miniaturized circuitry, and harvest and store optical energy.Item Light-Driven Permanent Charge Separation across a Hybrid Zero-Dimensional/Two-Dimensional Interface(2020-03) Kriegel, Ilka; Ghini, Michele; Bellani, Sebastiano; Zhang, Kehao; Jansons, Adam W.; Crockett, Brandon M.; Koskela, Kristopher M.; Barnard, Edward S.; Penzo, Erika; Hutchison, James E.; Robinson, Joshua A.; Manna, Liberato; Borys, Nicholas J.; Schuck, P. JamesWe report the first demonstration of light-driven permanent charge separation across an ultrathin solid-state zero-dimensional (0D)/2D hybrid interface by coupling photoactive Sn-doped In2O3 nanocrystals with monolayer MoS2, the latter serving as a hole collector. We demonstrate that the nanocrystals in this device-ready architecture act as local light-controlled charge sources by quasi-permanently donating ∼5 holes per nanocrystal to the monolayer MoS2. The amount of photoinduced contactless charge transfer to the monolayer MoS2 competes with what is reached in electrostatically gated devices. Thus, we have constructed a hybrid bilayer structure in which the electrons and holes are separated into two different solid-state materials. The temporal evolution of the local doping levels of the monolayer MoS2 follows a capacitive charging model with effective total capacitances in the femtofarad regime and areal capacitances in the μF cm–2 range. This analysis indicates that the 0D/2D hybrid system may be able to store light energy at densities of at least μJ cm–2, presenting new potential foundational building blocks for next-generation nanodevices that can remotely control local charge density, power miniaturized circuitry, and harvest and store optical energy.Item Long-Range Exciton Diffusion in Two-Dimensional Assemblies of Cesium Lead Bromide Perovskite Nanocrystals(2020-05) Penzo, Erika; Loiudice, Anna; Barnard, Edward S.; Borys, Nicholas J.; Jurow, Matthew J.; Lorenzon, Monica; Rajzbaum, Igor; Wong, Edward K.; Liu, Yi; Schwartzberg, Adam M.; Cabrini, Stefano; Whitelam, Stephen; Buonsanti, Raffaella; Weber-Bargioni, AlexanderFörster resonant energy transfer (FRET)-mediated exciton diffusion through artificial nanoscale building block assemblies could be used as an optoelectronic design element to transport energy. However, so far, nanocrystal (NC) systems supported only diffusion lengths of 30 nm, which are too small to be useful in devices. Here, we demonstrate a FRET-mediated exciton diffusion length of 200 nm with 0.5 cm2/s diffusivity through an ordered, two-dimensional assembly of cesium lead bromide perovskite nanocrystals (CsPbBr3 PNCs). Exciton diffusion was directly measured via steady-state and time-resolved photoluminescence (PL) microscopy, with physical modeling providing deeper insight into the transport process. This exceptionally efficient exciton transport is facilitated by PNCs’ high PL quantum yield, large absorption cross section, and high polarizability, together with minimal energetic and geometric disorder of the assembly. This FRET-mediated exciton diffusion length matches perovskites’ optical absorption depth, thus enabling the design of device architectures with improved performances and providing insight into the high conversion efficiencies of PNC-based optoelectronic devices.