Alexandros Stavrinadis

Heterovalent cation substitutional doping for quantum dot homojunction solar cells

Colloidal quantum dots have emerged as a material platform for low-cost high-performance optoelectronics. At the heart of optoelectronic devices lies the formation of a junction, which requires the intimate contact of n-type and p-type semiconductors. Doping in bulk semiconductors has been largely deployed for many decades, yet electronically active doping in quantum dots has remained a challenge and the demonstration of robust functional optoelectronic devices had thus far been elusive. Here we report an optoelectronic device, a quantum dot homojunction solar cell, based on heterovalent cation substitution. We used PbS quantum dots as a reference material, which is a p-type semiconductor, and we employed Bi-doping to transform it into an n-type semiconductor. We then combined the two layers into a homojunction device operating as a solar cell robustly under ambient air conditions with power conversion efficiency of 2.7%.

SnS/PbS nanocrystal heterojunction photovoltaics.

We report advances in the growth, characterization and photovoltaic properties of SnS nanocrystals, with controlled < 10 nm size, and their inclusion into a lead chalcogenide solar cell. The SnS/PbS nanocrystalline film heterojunction is shown to display a type II band alignment, in which the direction of flow of the photocurrent depends on the order of the layers and not the relative work functions of the contacts. On placing the SnS layer next to the indium tin oxide (ITO) cathode we observe a dramatic increase in V(oc) to as much as 0.45 V. Our results suggest that SnS nanocrystal films can be used in multi-junction solar cells, that a SnS/PbS heterojunction on its own shows photovoltaic behaviour, and that a SnS layer in an ITO/SnS/PbS/Al device is acting to suppress the flow of an electron injection current.

Remote trap passivation in colloidal quantum dot bulk nano-heterojunctions and its effect in solution-processed solar cells

More-efficient charge collection and suppressed trap recombination in colloidal quantum dot (CQD) solar cells is achieved by means of a bulk nano-heterojunction (BNH) structure, in which p-type and n-type materials are blended on the nanometer scale. The improved performance of the BNH devices, compared with that of bilayer devices, is displayed in higher photocurrents and higher open-circuit voltages (resulting from a trap passivation mechanism).

Hybrid solution-processed bulk heterojunction solar cells based on bismuth sulfide nanocrystals

High efficiency organic and hybrid solar cells create demand for novel electron acceptor materials that possess appropriate energetic band levels and bandgap for efficient solar energy harnessing. We present hybrid bulk heterojunction devices based on P3HT and bismuth sulfide nanocrystals, a semiconductor based on environmentally friendly compounds, with a power conversion efficiency of 1% and NIR sensitization at 700 nm of 30%, among the highest ever reported for P3HT.

Colloidal synthesis of lead oxide nanocrystals for photovoltaics

Lead oxide nanocrystals are synthesised by injecting oxygen gas into an air and moisture free complex of Pb oleylamine and oleic acid in octadecene. Using various characterization methods including fabrication and testing of photovoltaic devices we explore the material properties and photovoltaic application of lead oxide nanocrystal films.

Strategies for the Controlled Electronic Doping of Colloidal Quantum Dot Solids

Over the last several years tremendous progress has been made in incorporating colloidal quantum dot (CQD) solids as photoactive components in optoelectronic devices. A large part of this progress is associated with significant advancements made in controlling the electronic doping of CQD solids. Today, a variety of strategies exists towards that purpose; this Minireview aims to survey the major published works in this subject. Additional attention is given to the many challenges associated with the task of doping CQDs, as well as to the realization of optoelectronic functionalities and applications upon successful light and heavy electronic doping of CQD solids.

Trap-state suppression and improved charge transport in PbS quantum dot solar cells with synergistic mixed ligand treatments

The power conversion efficiency of colloidal PbS-quantum-dot (QD)-based solar cells is significantly hampered by lower-than-expected open circuit voltage (VOC ). The VOC deficit is considerably higher in QD-based solar cells compared to other types of existing solar cells due to in-gap trap-induced bulk recombination of photogenerated carriers. Here, this study reports a ligand exchange procedure based on a mixture of zinc iodide and 3-mercaptopropyonic acid to reduce the VOC deficit without compromising the high current density. This layer-by-layer solid state ligand exchange treatment enhances the photovoltaic performance from 6.62 to 9.92% with a significant improvement in VOC from 0.58 to 0.66 V. This study further employs optoelectronic characterization, X-ray photoelectron spectroscopy, and photoluminescence spectroscopy to understand the origin of VOC improvement. The mixed-ligand treatment reduces the sub-bandgap traps and significantly reduces bulk recombination in the devices.

The Influence of Doping on the Optoelectronic Properties of PbS Colloidal Quantum Dot Solids

We report on an extensive spectroscopic investigation of the impact of substitutional doping on the optoelectronic properties of PbS colloidal quantum dot (CQD) solids. N-doping is provided by Bi incorporation during CQD synthesis as well as post-synthetically via cation exchange reactions. The spectroscopic data indicate a systematic quenching of the excitonic absorption and luminescence and the appearance of two dopant-induced contributions at lower energies to the CQD free exciton. Temperature-dependent photoluminescence indicates the presence of temperature-activated detrapping and trapping processes of photoexcitations for the films doped during and after synthesis, respectively. The data are consistent with a preferential incorporation of the dopants at the QDs surface in the case of the cation-exchange treated films versus a more uniform doping profile in the case of in-situ Bi incorporation during synthesis. Time-resolved experiments indicate the presence of fast dopant- and excitation-dependent recombination channels attributed to Auger recombination of negatively charged excitons, formed due to excess of dopant electrons. The data indicate that apart from dopant compensation and filling of dopant induced trap states, a fraction of the Bi ionized electrons feeds the QD core states resulting in n-doping of the semiconductor, confirming reported work on devices based on such doped CQD material.

Reducing Interface Recombination through Mixed Nanocrystal Interlayers in PbS Quantum Dot Solar Cells

The performance of ZnO/PbS colloidal quantum dot (CQD)-based heterojunction solar cells is hindered by charge carrier recombination at the heterojunction interface. Reducing interfacial recombination can improve charge collection and the photocurrent of the device. Here we report the use of a mixed nanocrystal (MNC) buffer layer comprising zinc oxide nanocrystals and lead sulfide quantum dots at the respective heterojunction interface. Remote trap passivation of the PbS CQDs taking place within this MNC layer reduces interfacial recombination and electron back transfer which in turn improves charge collection efficiency. Upon the addition of the MNC layer, the overall power conversion efficiency increases from 9.11 to 10.16% and Short-circuit current density (JSC) increases from 23.54 to 25.23 mA/cm2. Optoelectronic characterization of the solar cells confirms that the effects underlying device improvement are reduced trap density and improved charge collection efficiency due to the presence of the MNC buffer layer.

Infrared Solution‐Processed Quantum Dot Solar Cells Reaching External Quantum Efficiency of 80% at 1.35 µm and Jsc in Excess of 34 mA cm−2

Developing low-cost photovoltaic absorbers that can harvest the short-wave infrared (SWIR) part of the solar spectrum, which remains unharnessed by current Si-based and perovskite photovoltaic technologies, is a prerequisite for making high-efficiency, low-cost tandem solar cells. Here, infrared PbS colloidal quantum dot (CQD) solar cells employing a hybrid inorganic-organic ligand exchange process that results in an external quantum efficiency of 80% at 1.35 µm are reported, leading to a short-circuit current density of 34 mA cm-2 and a power conversion efficiency (PCE) up to 7.9%, which is a current record for SWIR CQD solar cells. When this cell is placed at the back of an MAPbI3 perovskite film, it delivers an extra 3.3% PCE by harnessing light beyond 750 nm.