Mengxia Liu

Passivation Using Molecular Halides Increases Quantum Dot Solar Cell Performance.

A solution-based passivation scheme is developed featuring the use of molecular iodine and PbS colloidal quantum dots (CQDs). The improved passivation translates into a longer carrier diffusion length in the solid film. This allows thicker solar-cell devices to be built while preserving efficient charge collection, leading to a certified power conversion efficiency of 9.9%, which is a new record in CQD solar cells.

10.6% Certified Colloidal Quantum Dot Solar Cells via Solvent-Polarity-Engineered Halide Passivation

Colloidal quantum dot (CQD) solar cells are solution-processed photovoltaics with broad spectral absorption tunability. Major advances in their efficiency have been made via improved CQD surface passivation and device architectures with enhanced charge carrier collection. Herein, we demonstrate a new strategy to improve further the passivation of CQDs starting from the solution phase. A cosolvent system is employed to tune the solvent polarity in order to achieve the solvation of methylammonium iodide (MAI) and the dispersion of hydrophobic PbS CQDs simultaneously in a homogeneous phase, otherwise not achieved in a single solvent. This process enables MAI to access the CQDs to confer improved passivation. This, in turn, allows for efficient charge extraction from a thicker photoactive layer device, leading to a certified solar cell power conversion efficiency of 10.6%, a new certified record in CQD photovoltaics.

Hybrid organic–inorganic inks flatten the energy landscape in colloidal quantum dot solids

Bandtail states in disordered semiconductor materials result in losses in open-circuit voltage (Voc) and inhibit carrier transport in photovoltaics. For colloidal quantum dot (CQD) films that promise low-cost, large-area, air-stable photovoltaics, bandtails are determined by CQD synthetic polydispersity and inhomogeneous aggregation during the ligand-exchange process. Here we introduce a new method for the synthesis of solution-phase ligand-exchanged CQD inks that enable a flat energy landscape and an advantageously high packing density. In the solid state, these materials exhibit a sharper bandtail and reduced energy funnelling compared with the previous best CQD thin films for photovoltaics. Consequently, we demonstrate solar cells with higher Voc and more efficient charge injection into the electron acceptor, allowing the use of a closer-to-optimum bandgap to absorb more light. These enable the fabrication of CQD solar cells made via a solution-phase ligand exchange, with a certified power conversion efficiency of 11.28%. The devices are stable when stored in air, unencapsulated, for over 1,000 h.

High-Efficiency Colloidal Quantum Dot Photovoltaics via Robust Self-Assembled Monolayers

The optoelectronic tunability offered by colloidal quantum dots (CQDs) is attractive for photovoltaic applications but demands proper band alignment at electrodes for efficient charge extraction at minimal cost to voltage. With this goal in mind, self-assembled monolayers (SAMs) can be used to modify interface energy levels locally. However, to be effective SAMs must be made robust to treatment using the various solvents and ligands required for to fabricate high quality CQD solids. We report robust self-assembled monolayers (R-SAMs) that enable us to increase the efficiency of CQD photovoltaics. Only by developing a process for secure anchoring of aromatic SAMs, aided by deposition of the SAMs in a water-free deposition environment, were we able to provide an interface modification that was robust against the ensuing chemical treatments needed in the fabrication of CQD solids. The energy alignment at the rectifying interface was tailored by tuning the R-SAM for optimal alignment relative to the CQD quantum-confined electron energy levels. This resulted in a CQD PV record power conversion efficiency (PCE) of 10.7% with enhanced reproducibility relative to controls.

Double-Sided Junctions Enable High-Performance Colloidal-Quantum-Dot Photovoltaics

The latest advances in colloidal-quantum-dot material processing are combined with a double-sided junction architecture, which is done by efficiently incorporating indium ions in the ZnO eletrode. This platform allows the collection of all photogenerated carriers even at the maximum power point. The increased depletion width in the device facilitates full carrier collection, leading to a record 10.8% power conversion efficiency.

All-Quantum-Dot Infrared Light-Emitting Diodes

Colloidal quantum dots (CQDs) are promising candidates for infrared electroluminescent devices. To date, CQD-based light-emitting diodes (LEDs) have employed a CQD emission layer sandwiched between carrier transport layers built using organic materials and inorganic oxides. Herein, we report the infrared LEDs that use quantum-tuned materials for each of the hole-transporting, the electron-transporting, and the light-emitting layers. We successfully tailor the bandgap and band position of each CQD-based component to produce electroluminescent devices that exhibit emission that we tune from 1220 to 1622 nm. Devices emitting at 1350 nm achieve peak external quantum efficiency up to 1.6% with a low turn-on voltage of 1.2 V, surpassing previously reported all-inorganic CQD LEDs.

Single-step colloidal quantum dot films for infrared solar harvesting

Semiconductors with bandgaps in the near- to mid-infrared can harvest solar light that is otherwise wasted by conventional single-junction solar cell architectures. In particular, colloidal quantum dots (CQDs) are promising materials since they are cost-effective, processed from solution, and have a bandgap that can be tuned into the infrared (IR) via the quantum size effect. These characteristics enable them to harvest the infrared portion of the solar spectrum to which silicon is transparent. To date, IR CQD solar cells have been made using a wasteful and complex sequential layer-by-layer process. Here, we demonstrate ∼1 eV bandgap solar-harvesting CQD films deposited in a single step. By engineering a fast-drying solvent mixture for metal iodide-capped CQDs, we deposited active layers greater than 200 nm in thickness having a mean roughness less than 1 nm. We integrated these films into infrared solar cells that are stable in air and exhibit power conversion efficiencies of 3.5% under illumination by t...

Pseudohalide-Exchanged Quantum Dot Solids Achieve Record Quantum Efficiency in Infrared Photovoltaics

Application of pseudohalogens in colloidal quantum dot (CQD) solar-cell active layers increases the solar-cell performance by reducing the trap densities and implementing thick CQD films. Pseudohalogens are polyatomic analogs of halogens, whose chemistry allows them to substitute halogen atoms by strong chemical interactions with the CQD surfaces. The pseudohalide thiocyanate anion is used to achieve a hybrid surface passivation. A fourfold reduced trap state density than in a control is observed by using a suite of field-effect transistor studies. This translates directly into the thickest CQD active layer ever reported, enabled by enhanced transport lengths in this new class of materials, and leads to the highest external quantum efficiency, 80% at the excitonic peak, compared with previous reports of CQD solar cells.

Nanoimprint-Transfer-Patterned Solids Enhance Light Absorption in Colloidal Quantum Dot Solar Cells

Colloidal quantum dot (CQD) materials are of interest in thin-film solar cells due to their size-tunable bandgap and low-cost solution-processing. However, CQD solar cells suffer from inefficient charge extraction over the film thicknesses required for complete absorption of solar light. Here we show a new strategy to enhance light absorption in CQD solar cells by nanostructuring the CQD film itself at the back interface. We use two-dimensional finite-difference time-domain (FDTD) simulations to study quantitatively the light absorption enhancement in nanostructured back interfaces in CQD solar cells. We implement this experimentally by demonstrating a nanoimprint-transfer-patterning (NTP) process for the fabrication of nanostructured CQD solids with highly ordered patterns. We show that this approach enables a boost in the power conversion efficiency in CQD solar cells primarily due to an increase in short-circuit current density as a result of enhanced absorption through light-trapping.

Broadband Epsilon-near-Zero Reflectors Enhance the Quantum Efficiency of Thin Solar Cells at Visible and Infrared Wavelengths

The engineering of broadband absorbers to harvest white light in thin-film semiconductors is a major challenge in developing renewable materials for energy harvesting. Many solution-processed materials with high manufacturability and low cost, such as semiconductor quantum dots, require the use of film structures with thicknesses on the order of 1 μm to absorb incoming photons completely. The electron transport lengths in these media, however, are 1 order of magnitude smaller than this length, hampering further progress with this platform. Herein, we show that, by engineering suitably disordered nanoplasmonic structures, we have created a new class of dispersionless epsilon-near-zero composite materials that efficiently harness white light. Our nanostructures localize light in the dielectric region outside the epsilon-near-zero material with characteristic lengths of 10-100 nm, resulting in an efficient system for harvesting broadband light when a thin absorptive film is deposited on top of the structure. By using a combination of theory and experiments, we demonstrate that ultrathin layers down to 50 nm of colloidal quantum dots deposited atop the epsilon-near-zero material show an increase in broadband absorption ranging from 200% to 500% compared to a planar structure of the same colloidal quantum-dot-absorber average thickness. When the epsilon-near-zero nanostructures were used in an energy-harvesting module, we observed a spectrally averaged 170% broadband increase in the external quantum efficiency of the device, measured at wavelengths between 400 and 1200 nm. Atomic force microscopy and photoluminescence excitation measurements demonstrate that the properties of these epsilon-near-zero structures apply to general metals and could be used to enhance the near-field absorption of semiconductor structures more widely. We have developed an inexpensive electrochemical deposition process that enables scaled-up production of this nanomaterial for large-scale energy-harvesting applications.