1,721,010 research outputs found
Optical Nanostructures for Excitonic Devices
No full textUnrelenting advances in the field of nanoscience are fostering the progress in diverse research fields, ranging from light-emitting to medicine and diagnostics, from energy conversion to communication technologies. Besides representing the most paradigmatic example of nanoscience, semiconductor quantum dots (QDs) avowedly brought revolutions in many of the research fields mentioned above. Nowadays, some QDs-based devices and applications reported efficiencies almost as good as current state-of-the-art technologies. The founding concept of QDs is the application of quantum confinement effects on excitons, i.e., the main players of optical properties in bulk semiconductors. Among the wealth of ensuing properties, the size- and shape- tunability of the electronic excitations and increased coupling with light field aroused much interest. Also, the colloidal approach endows QDs with high processability and low cost, thereby encouraging their implementation in existing technologies and extending their impact to other fields. Howbeit, despite three decades of investigations, the bottom line has not been reached yet, and researchers are still delving deeper into the photophysics of these nanosystems. Though many of the low hanging fruit of QDs have been harvested, higher-lying ones seem to be even more succulent.
This thesis deals with the quest for highly performing nanostructures, as a prerequisite for some high impact optoelectronic applications, e.g., QD-Lasers and QD-Solar Cells. Within this framework, the struggle against fast Auger recombinations and trapping of either hot carriers or cold excitons was addressed mainly by sophisticated core/shell technologies. Thus, the first part of the thesis reports how tuning different shell parameters (e.g., the smoothness of the interface potential, the height of the confining potential, and the interfacial strain) it is possible to exert control on these detrimental recombination processes. Though often disregarded, even the role of organic capping ligand is reconsidered in promoting the outcoupling of QDs excited states and addressing their interaction. Besides the useful and technologically relevant advice gathered within these studies, the primary inheritance of the first part is the comprehensive photophysical scenario, portrayed by a phenomenological model that successfully describes many aspects of the exciton dynamics in QDs. This amount of knowledge was capitalized in the second part of this thesis, dealing with the quest for novel materials, potentially outpacing conventional CdSe-based QDs. Perovskite-based QDs reported promising results, whereas some pitfall in the conventional characterization of carbon-based QDs were discovered. The rationalization of both nature and dynamics of this materials is expected to expedite their development as alternative (and potentially superior) technologies concerning those studied in the first part
Replication Data for: Quo vadis, perovskite emitters?
No full textHalide perovskites hold great promise for next-generation printable optoelectronic devices. Within a decade of their debut in photovoltaics, these amazing materials proliferate beyond solar cells to applications such as light-emitting devices, lasers, radiation detectors, and memristors. Such versatility stems from perovskites’ favorable optoelectronic properties that are highly exceptional for a facile solution-processed system. Halide perovskite emitters have made significant inroads, in particular, perovskite light-emitting device (PeLED) efficiencies have risen from 20% within 5 years, and perovskite continuous-wave amplified spontaneous emission has also been demonstrated recently. This perspective distills the photophysical mechanisms underpinning the various approaches in enhancing their radiative efficiencies. Selected works are highlighted to detail the milestones and to chart the direction the field is heading. Challenges and opportunities for solid-state perovskite light-emitting devices are discussed. A clear understanding of their basic photophysics and structure-function relations holds the key to rationalizing strategies and streamlining efforts to realize high-efficiency PeLEDs and perovskite laser
Replication Data for: Hot Carriers Perspective on the Nature of Traps in Perovskites
No full textThe defects in lead halide perovskites are usually regarded benign to their optoelectronic properties but it remains a question to what extent. Here Righetto et al. quantify how hot carriers experience increased trapping rates at the defects, making them less benign and develop a strategy to passivate them
The central role of ligands in electron transfer from perovskite nanocrystals
No full textThe nanoscale miniaturization of hybrid organic-inorganic perovskite has given rise to new functionalities, but the full understanding of the multifaceted properties of perovskite nanostructures is still incomplete. Using a combination of optical and magnetic resonance (EPR) spectroscopies, we focused our investigation on the photoinduced electron transfer process taking place in perovskite nanocrystals blended with the fullerene derivative PCBM. In particular we analyzed the different effect of two types of nanocrystal ligands, namely octylamine and oleylamine, on the photoinduced processes. The electron transfer process resulted in efficient fluorescence quenching in a mixed solution and in the formation of charges (PCBM anions) detected by EPR in the blends. Both the optical and EPR techniques revealed a stronger effect when the shorter ligand is present. Finally, pulsed EPR demonstrated the stabilization of the photogenerated charges in proximity of perovskite nanocrystals
Bridging Energetics and Dynamics of Exciton Trapping in Core-Shell Quantum Dots
Full text linkThe widespread application of quantum dots greatly profits from their broad absorption band. However, the variable nature of excitations within these bands is expected to result in undesired excitation energy dependence of steady state emission properties. We demonstrate the different role played by hot and cold carrier trapping in determining fluorescence quantum yields. Our analysis relates the energetic parameters with the available knowledge on the dynamics of charge trapping. It turns out that detrapping processes play a pivotal role in determining steady state emission properties. We studied excitation dependent photoluminescence quantum yields (PLQY) in different CdSe/CdxZn1–xS (x = 0, 0.5, and 1) quantum dots to identify best performing heterostructures in terms of shell thickness and composition. Our rationalization of the observed behavior is focused on the modulation of trapping and detrapping rates. The combination of experimental results and PLQY kinetics modeling reveals the need to consider hot-carrier trapping, supporting recent dynamics observations. This work provides a deeper insight into the trapping process in quantum dots, relating its energetics and dynamics
Going Beyond Counting First Authors in Author Co-citation Analysis
Full text linkThe present study examines one of the fundamental aspects of author co-citation analysis (ACA) - the way co-citation
counts are defined. Co-citation counting provides the data on which all subsequent statistical analyses and mappings
are based, and we compare ACA results based on two different types of co-citation counting - the traditional type that
only counts the first one among a cited work's authors on the one hand and a non-traditional type that takes into
account the first 5 authors of a cited work on the other hand. Results indicate that the picture produced through this non-traditional author co-citation counting contains more coherent author groups and is therefore considerably clearer. However, this picture represents fewer specialties in the research field being studied than that produced through the traditional first-author co-citation counting when the same number of top-ranked authors is selected and analyzed. Reasons for these effects are discussed
Boosting carbon quantum dots/fullerene electron transfer via surface group engineering
No full textThe design of novel nanostructures with tailored opto-electronic properties is a crucial step for thirdgeneration
photovoltaics, and the development of cheap and environmentally compatible materials is
still a challenge. Carbon quantum dots (CQDs) emerged as promising candidates but usually a low
processability and poor electron-donor properties hampered their photovoltaic applications. We tackle
these issues through the synthesis and photophysical characterization of N-doped CQDs functionalized
with different thiophene-containing groups. Functionalization was aimed at enhancing the electron
donating properties of the carbon dots and improving the solubility in nonpolar solvents. The increased
solubility in organic solvents allowed us to investigate the photoinduced interactions of the functionalized
carbon dots with the fullerene derivative PCBM in solution and in solid blends. The investigation was
carried out by cyclic voltammetry, photoluminescence spectroscopy and electron paramagnetic
resonance (EPR). The remarkable oxidation potential shift of the functionalized carbon dots with respect
to the pristine materials and the HOMO–LUMO energies strongly suggest them as good electron donors
towards PCBM. The electron transfer process between CQDs and PCBM resulted in efficient fluorescence
quenching in solution and in total quenching in solid blends. By using EPR spectroscopy in the solid
blends, we demonstrated the efficient electron transfer by observing the photoinduced formation of a
PCBM radical anion in the presence of functionalized CQDs. Time-resolved EPR allowed us to identify
differences in the charge transport efficiency for different CQD:PCBM blends. The enhanced processability
of CQDs with PCBM and the promising charge-generation and separation properties pave the way to the
development of ‘‘all-carbon’’ photovoltaic devices
Variations on the Author
Full text link“Variations on the Author” discusses two of Eduardo Coutinho’s recent films (Um Dia na Vida, from 2010, and Últimas Conversas, posthumously released in 2015) and their contribution to the general question of documentary authorship. The director’s filmography is characterized by a consistent yet self-effacing form of authorial self-inscription: Coutinho often features as an interviewer that rather than express opinions propels discourses; an interviewer that is good at listening. This mode of self-inscription characterizes him as an author who is not expressive but who is nonetheless markedly present on the screen. In Um Dia na Vida, however, Coutinho is completely absent form the image, while Últimas Conversas, on the contrary, includes a confessional prologue that moves the director from the margins to the center of his films. This article examines the ways in which these works stand out in the filmography of a director who offers new insights into the notion of cinematic authorship
Appropriate Similarity Measures for Author Cocitation Analysis
Full text linkWe provide a number of new insights into the methodological discussion about author cocitation analysis. We first argue that the use of the Pearson correlation for measuring the similarity between authors’ cocitation profiles is not very satisfactory. We then discuss what kind of similarity measures may be used as an alternative to the Pearson correlation. We consider three similarity measures in particular. One is the well-known cosine. The other two similarity measures have not been used before in the bibliometric literature. Finally, we show by means of an example that our findings have a high practical relevance.information science;Pearson correlation;cosine;similarity measure;author cocitation analysis
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