arXiv subjects

Guglielmo Lanzani

Publications and source records attributed to Guglielmo Lanzani.

26 records · Page 2Linked to original sources

arXiv2016

Photoinduced Absorption within Single-Walled Carbon Nanotube Systems

We study the photoabsorption properties of photoactive bulk polymer/ fullerene/nanotube heterojunctions in the near-infrared region. By combining pump-probe spectroscopy and linear response time-dependent density functional theory within the random phase approximation (TDDFT-RPA) we elucidate the excited state dynamics of the $E_{11}$ transition within (6,5) and (7,5) single-walled carbon nanotubes (SWNTs) and combined with poly(3-hexylthiophene-2,5-diyl) (P3HT) and [6,6]-phenyl-C$_{61}$-butyric acid methyl ester (PCBM) in P3HT/PCBM/SWNT blended samples. We find the presence of a photoinduced absorption (PA) peak is related mainly to the width of the photobleach (PB) peak and the charge carrier density of the SWNT system. For mixed SWNT samples, the PB peak is too broad to observe the PA peak, whereas within P3HT/PCBM/SWNT blended samples P3HT acts as a hole acceptor, narrowing the PB peak by exciton delocalization, which reveals a PA peak. Our results suggest that the PA peak originates from a widening of the band gap in the presence of excited electrons and holes. These results have important implications for the development of new organic photovoltaic heterojunctions including SWNTs.

cond-mat.mtrl-sci↗

arXiv2015

Molecular-Level Switching of Polymer/Nanocrystal Non-Covalent Interactions and Application in Hybrid Solar Cells

Hy brid composites obtained upon blending conjugated polymers and colloidal inorganic semiconductor nanocrystals are regarded as attractive photo-active materials for optoelectronic applications. Here we demonstrate that tailoring nanocrystal surface chemistry permits to exert control on non-covalent bonding and electronic interactions between organic and inorganic components. The pendant moieties of organic ligands at the nanocrystal surface do not merely confer colloidal stability while hindering charge separation and transport, but drastically impact morphology of hybrid composites during formation from blend solutions. The relevance of our approach to photovoltaic applications is demonstrated for composites based on poly(3-hexylthiophene) and Pbs nanocrystals, considered as inadequate before the submission of this manuscript, which enable the fabrication of hybrid solar cells displaying a power conversion efficiency that reaches 3 %. Upon (quasi)steady-state and time-resolved analisys of the photo-induced processes in the nanocomposites and their organic and inorganic components, we ascertained that electron transfer occurs at the hybrid interface yielding long-lived separated charge carriers, whereas interfacial hole transfer appears slow. Here we provide a reliable alternative aiming at gaining control over macroscopic optoelectronic properties of polymer/nanocrystal composites by acting at the molecular-level via ligands' pendant moieties, thus opening new possibilities towards efficient solution-processed hybrid solar cells.

cond-mat.mtrl-sci↗

arXiv2014

Charge photogeneration in few-layer MoS2

The two-dimensional semiconductor MoS2 in its mono- and few-layer form is expected to have a significant exciton binding energy of several 100 meV, leading to the consensus that excitons are the primary photoexcited species. Nevertheless, even single layers show a strong photovoltaic effect and work as the active material in high sensitivity photodetectors, thus indicating efficient charge carrier photogeneration (CPG). Here we use continuous wave photomodulation spectroscopy to identify the optical signature of long-lived charge carriers and femtosecond pump-probe spectroscopy to follow the CPG dynamics. We find that intitial photoexcitation yields a branching between excitons and charge carriers, followed by excitation energy dependent hot exciton dissociation as an additional CPG mechanism. Based on these findings, we make simple suggestions for the design of more efficient MoS2 photovoltaic and photodetector devices.

cond-mat.mtrl-sci↗

arXiv2014

Control of the chemiluminescence spectrum with porous Bragg mirrors

Tunable, battery free light emission is demonstrated in a solid state device that is compatible with lab on a chip technology and easily fabricated via solution processing techniques. A porous one dimensional (1D) photonic crystal (also called Bragg stack or mirror) is infiltrated by chemiluminescence rubrene-based reagents. The Bragg mirror has been designed to have the photonic band gap overlapping with the emission spectrum of rubrene. The chemiluminescence reaction occurs in the intrapores of the photonic crystal and the emission spectrum of the dye is modulated according to the photonic band gap position. This is a compact, powerless emitting source that can be exploited in disposable photonic chip for sensing and point of care applications.

cond-mat.mtrl-sci↗

arXiv2014

High energetic excitons in carbon nanotubes directly probe charge-carriers

Theory predicts peculiar features for excited-state dynamics in one dimension (1D) that are difficult to be observed experimentally. Single-walled carbon nanotubes (SWNTs) are an excellent approximation to 1D quantum confinement, due to their very high aspect ratio and low density of defects. Here we use ultrafast optical spectroscopy to probe photogenerated charge-carriers in (6,5) semiconducting SWNTs. We identify the transient energy shift of the highly polarizable S33 transition as a sensitive fingerprint of charge-carriers in SWNTs. By measuring the coherent phonon amplitude profile we obtain a precise estimate of the Stark-shift and discuss the binding energy of the S33 excitonic transition. From this, we infer that charge-carriers are formed instantaneously with sizable quantum yield even upon pumping the first exciton, S11. The decay of the photogenerated charge-carrier population is well described by a model for geminate recombination in 1D, suggesting an initial charge carrier separation of the same order of the exciton correlation length.

cond-mat.mes-hall↗

arXiv2014

Fast Ultrahigh-Density Writing of Low Conductivity Patterns on Semiconducting Polymers

The exceptional interest in improving the limitations of data storage, molecular electronics, and optoelectronics has promoted the development of an ever increasing number of techniques used to pattern polymers at micro and nanoscale. Most of them rely on Atomic Force Microscopy to thermally or electrostatically induce mass transport, thereby creating topographic features. Here we show that the mechanical interaction of the tip of the Atomic Force Microscope with the surface of a class of conjugate polymers produces a local increase of molecular disorder, inducing a localized lowering of the semiconductor conductivity, not associated to detectable modifications in the surface topography. This phenomenon allows for the swift production of low conductivity patterns on the polymer surface at an unprecedented speed exceeding 20 $μm s^{-1}$; paths have a resolution in the order of the tip size (20 nm) and are detected by a Conducting-Atomic Force Microscopy tip in the conductivity maps.

cond-mat.mtrl-sci↗

arXiv2013

Plasmonics in heavily-doped semiconductor nanocrystals

Heavily-doped semiconductor nanocrystals characterized by a tunable plasmonic band have been gaining increasing attention recently. Herein, we introduce this type of materials focusing on their structural and photo physical properties. Beside their continuous-wave plasmonic response, depicted both theoretically and experimentally, we also review recent results on their transient, ultrafast response. This was successfully interpreted by adapting models of the ultrafast response of gold nanoparticles.

cond-mat.mes-hall↗

arXiv2012

A hybrid bio-organic interface for neuronal photo-activation

Interfacing artificial functional materials and living neuronal tissues is at the forefront of bio-nano-technology. Attempts have been so far based onto microscale processing of metals and inorganic semiconductors as electrodes or photoactive layers in biased devices. More recently, also nanomaterials properties have been investigated. In spite of extensive research however, the communication between biological tissues and artificial sensors is still a challenge. Constraints consist in the complexity of the fabrication processes (i.e. metal and semiconductor lithography), the mechanical properties (e.g. flexibility and mechanical invasiveness) and chemical influence (e.g. inflammatory reactions). In addition, electrodes have fixed geometries that limit the location in space of the stimulus and often electrical currents are detrimental for the overall system. To this respect organic soft matter offers a chance in terms of biological affinity and mechanical properties. In particular conjugated polymers have appealing optoelectronic features which could lead to a new generation of neuronal communication and photo-manipulation techniques. So far conjugated polymers have being only tested as coatings of electrodes for neuronal activity recording. Here we report an up-scale of their use: the successful interfacing of an organic semiconductor to a network of cultured primary neurons, through optical excitation. This allows to a new paradigm for the optical stimulation of neurons which could have important implications for the development of an artificial retina based on organic photodetectors.

cond-mat.soft↗