Nucleation and Growth of Bipyramidal Yb:LiYF4 Nanocrystals─Growing Up in a Hot Environment

Lanthanide-doped LiYF4 (Ln:YLF) is commonly used for a broad variety of optical applications, such as lasing, photon upconversion and optical refrigeration. When synthesized as nanocrystals (NCs), this material is also of interest for biological applications and fundamental physical studies. Until now, it was unclear how Ln:YLF NCs grow from...

Tuning the Driving Force for Charge Transfer in Perovskite-Chromophore Systems

Understanding the interplay between the kinetics and energetics of photophysical processes in perovskite-chromophore hybrid systems is crucial for realizing their potential in optoelectronics, photocatalysis, and light-harvesting applications. By combining steady-state optical characterizations and transient absorption spectroscopy, we have...

Size-Dependent Optical Properties of InP Colloidal Quantum Dots

Indium phosphide colloidal quantum dots (CQDs) are the main alternative for toxic and restricted Cd based CQDs for lighting and display applications. Here we systematically report on the size-dependent optical absorption, ensemble, and single particle photoluminescence (PL) and biexciton lifetimes of core-only InP CQDs. This systematic study...

Zero-Threshold Optical Gain in Electrochemically Doped Nanoplatelets and the Physics behind It

Colloidal nanoplatelets (NPLs) are promising materials for lasing applications. The properties are usually discussed in the framework of 2D materials, where strong excitonic effects dominate the optical properties near the band edge. At the same time, NPLs have finite lateral dimensions such that NPLs are not true extended 2D structures. Here...

The Fine-Structure Constant as a Ruler for the Band-Edge Light Absorption Strength of Bulk and Quantum-Confined Semiconductors

Low-dimensional semiconductors have found numerous applications in optoelectronics. However, a quantitative comparison of the absorption strength of low-dimensional versus bulk semiconductors has remained elusive. Here, we report generality in the band-edge light absorptance of semiconductors, independent of their dimensions. First, we...

Quantitative Electrochemical Control over Optical Gain in Quantum-Dot Solids

Solution-processed quantum dot (QD) lasers are one of the holy grails of nanoscience. They are not yet commercialized because the lasing threshold is too high: one needs >1 exciton per QD, which is difficult to achieve because of fast nonradiative Auger recombination. The threshold can, however, be reduced by electronic doping of the QDs,...

On the Stability of Permanent Electrochemical Doping of Quantum Dot, Fullerene, and Conductive Polymer Films in Frozen Electrolytes for Use in Semiconductor Devices

Semiconductor films that allow facile ion transport can be electronically doped via electrochemistry, where the amount of injected charge can be controlled by the potential applied. To apply electrochemical doping to the design of semiconductor devices, the injected charge has to be stabilized to avoid unintentional relaxation back to the...

Hot-electron transfer in quantum-dot heterojunction films

Thermalization losses limit the photon-to-power conversion of solar cells at the high-energy side of the solar spectrum, as electrons quickly lose their energy relaxing to the band edge. Hot-electron transfer could reduce these losses. Here, we demonstrate fast and efficient hot-electron transfer between lead selenide and cadmium selenide...

Selective antimony reduction initiating the nucleation and growth of InSb quantum dots

Indium antimonide (InSb) quantum dots (QDs) have unique and interesting photophysical properties, but widespread experimentation with InSb QDs is lacking due to the difficulty in synthesizing this material. The key experimental challenge in fabricating InSb QDs is preparing a suitable Sb-precursor in the correct oxidation state that reacts...

Asymmetric Optical Transitions Determine the Onset of Carrier Multiplication in Lead Chalcogenide Quantum Confined and Bulk Crystals

Carrier multiplication is a process in which one absorbed photon excites two or more electrons. This is of great promise to increase the efficiency of photovoltaic devices. Until now, the factors that determine the onset energy of carrier multiplication have not been convincingly explained. We show experimentally that the onset of carrier...

The Role of Dopant Ions on Charge Injection and Transport in Electrochemically Doped Quantum Dot Films

Control over the charge density is very important for implementation of colloidal semiconductor nanocrystals into various optoelectronic applications. A promising approach to dope nanocrystal assemblies is charge injection by electrochemistry, in which the charge compensating electrolyte ions can be regarded as external dopant ions. To gain...

Tuning and Probing the Distribution of Cu⁺ and Cu²⁺ Trap States Responsible for Broad-Band Photoluminescence in CuInS₂ Nanocrystals

The processes that govern radiative recombination in ternary CuInS₂ (CIS) nanocrystals (NCs) have been heavily debated, but recently, several research groups have come to the same conclusion that a photoexcited electron recombines with a localized hole on a Cu-related trap state. Furthermore, it has been observed that single CIS...

Switching between Plasmonic and Fluorescent Copper Sulfide Nanocrystals

Control over the doping density in copper sulfide nanocrystals is of great importance and determines its use in optoelectronic applications such as NIR optical switches and photovoltaic devices. Here, we demonstrate that we can reversibly control the hole carrier density (varying from >10²² cm^-3 to intrinsic) in...

Transport Properties of a Two-Dimensional PbSe Square Superstructure in an Electrolyte-Gated Transistor

Self-assembled nanocrystal solids show promise as a versatile platform for novel optoelectronic materials. Superlattices composed of a single layer of lead-chalcogenide and cadmium-chalcogenide nanocrystals with epitaxial connections between the nanocrystals, present outstanding questions to the community regarding their predicted band...

In Situ Spectroelectrochemical Determination of Energy Levels and Energy Level Offsets in Quantum-Dot Heterojunctions

Charge transfer in semiconductor heterojunctions is largely governed by the offset in the energy levels of the constituent materials. Unfortunately, literature values for such energy level offsets vary widely and are usually based on energy levels of the individual materials rather than of actual heterojunctions. Here we present a new method...