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By combining X-ray absorption fine structure and X-ray diffraction measurements with density functional and molecular dynamics simulations, we study the structure of a set of AgxBi1&minus, xS2 nanoparticles, a materials system of considerable current interest for photovoltaics. An apparent contradiction between the evidence provided by X-ray absorption and diffraction measurements is solved by means of the simulations. We find that disorder in the cation sublattice induces strong local distortions, leading to the appearance of short Ag&ndash, S bonds, the overall lattice symmetry remaining close to hexagonal.

Harnessing low energy photons is of paramount importance for multi-junction high efficiency solar cells as well as for thermo-photovoltaic applications. However, semiconductor absorbers with the bandgap lower than 0.8 eV have been limited to III-V (InGaAs) or IV (Ge) semiconductors that are characterized by high manufacturing costs and complicated lattice matching requirements in their growth and integration with higher bandgap cells. Here, we have developed solution processed low bandgap photovoltaic devices based on PbS colloidal quantum dots (CQDs) with a bandgap of 0.7 eV suited for both thermo-photovoltaics and low energy solar photon harvesting. By matching the spectral response of those cells to that of the infrared solar spectrum, we report a record high short circuit current (JSC) of 37 mA cm-2 under the full solar spectrum and 5.5 mA cm-2 when placed at the back of a silicon wafer resulting in power conversion efficiencies (PCEs) of 6.4% and 0.7%, respectively. Moreover, the device reached an above bandgap PCE of ∼6% as a thermo-photovoltaic cell recorded under a 1000 °C blackbody radiator.

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.

Two-terminal tandem cell architectures are believed to be an effective way to further improve the power conversion efficiency in solution processed photovoltaics. To design an efficient tandem solar cell, two key issues need to be considered. First, subcells with well-matched currents and complementary absorption characteristics are a prerequisite for high efficiency. Second, identifying the appropriate intermediate layer (IML) to connect the subcells is necessary to minimize the optical and electronic losses. PbS colloidal quantum dots (CQDs) are a notable choice for the subcells due to their low cost, solution processability, and remarkable wide range band gap tunability. Single-layer graphene (Gr) has been proposed to be a promising IML due to its high transparency and conductivity. Here, as a proof of concept, we demonstrate a solution-processed, two-terminal PbS CQDs tandem solar cell employing chemical vapor deposited Gr as the IML. In doing so, we report a PbS CQD cell comprising subcells with band...

Inverted Type-I quantum rings (QRs) are a recently developed class of nanostructure in which a lower bandgap material is laterally grown as a crown of same thickness around a higher bandgap nanoplatelet (NPL) core [l·2]· e.g. core/crown CdS/CdSe as shown in Fig. 1(a). For this work, we have colloidally synthesized 3 monolayer (ML) thick CdS/CdSe QR samples using seed-mediated method, by using 3ML CdS NPLs as the core seed [3]. Subsequently, continuous injection of Se precursor, elemental Se dissolved in octadecene (ODE), Cd precursor and Cd(CH3CO2)2 led to the growth of CdSe crown. The ring width was controlled by tuning the injection amount to regulate the extent of the lateral size of the crown coating. A TEM image of the 3ML CdS/CdSe QRs is shown in Fig. 1(b)· which suggests atomically flat lateral growth of CdSe on CdS NPLs, as it has larger average lateral size (30±10 nm) compared to the CdS core only NPLs. We have measured the photoluminescence (PL) and absorption spectra of CdS/CdSe QRs at different phases of crown growth. Fig. 1(c) shows the PL and absorption spectra for two contrasting cases having a (i) thin, and a (ii) thick CdSe crown. As the crown thickness increases, there is lesser extent of lateral confinement, and thus a red-shift in the PL peak position. Also the linewidth of the emission spectra narrows down as more CdSe is deposited in the crown. This is owing to the randomly dispersed CdSe islands of varying sizes formed around the CdS NPLs at the initial phase of the CdSe crown growth resulting in a normal distribution of energy levels. For a sufficiently thick CdSe crown, the electronic structure and optical properties of CdS/CdSe QR is identical to CdSe NPLs alone, characterized by narrower linewidths. Moreover, we have verified that the emission peak of the 3ML CdS/CdSe QRs is spectrally tunable between the peak emissions of 3ML CdS NPL core only (382 nm) and 3 ML CdSe NPL core only (462 nm). In terms of the absorption spectra, as we begin to grow the CdSe crown, there is a gradual emergence of the primary and secondary CdSe absorption peaks at 460 nm (electron-heavy hole) and 431 nm (electron-light hole) respectively, as can be seen in Fig. 1(c-ii). On the other hand, for thin CdSe crowns, these peaks are undeterminable, while the overlapping primary and secondary absorption peaks of CdS at 382 nm (electron-heavy hole) and 373 nm (electron-light hole) are more prominent, as can be seen in Fig. 1(c-i).

Förster resonance energy transfer (FRET) interacted with localized surface plasmon (LSP) gives us the ability to overcome inadequate transfer of energy between donor and acceptor nanocrystals (NCs). In this paper, we show LSP-enhanced FRET in colloidal photosensors of NCs in operation, resulting in substantially enhanced photosensitivity. The proposed photosensitive device is a layered self-assembled colloidal platform consisting of separated monolayers of the donor and the acceptor colloidal NCs with an intermediate metal nanoparticle (MNP) layer made of gold interspaced by polyelectrolyte layers. Using LBL assembly, we fabricated and comparatively studied seven types of such NC-monolayer devices (containing only donor, only acceptor, Au MNP-donor, Au MNP-acceptor, donor-acceptor bilayer, donor-Au MNP-acceptor trilayer, and acceptor-Au MNP-donor reverse trilayer). In these structures, we revealed the effect of LSP-enhanced FRET and exciton interactions from the donor NCs layer to the acceptor NCs layer. Compared to a single acceptor NC device, we observed a significant extension in operating wavelength range and a substantial photosensitivity enhancement (2.91-fold) around the LSP resonance peak of Au MNPs in the LSP-enhanced FRET trilayer structure. Moreover, we present a theoretical model for the intercoupled donor-Au MNP-acceptor structure subject to the plasmon-mediated nonradiative energy transfer. The obtained numerical results are in excellent agreement with the systematic experimental studies done in our work. The potential to modify the energy transfer through mastering the exciton-plasmon interactions and its implication in devices make them attractive for applications in nanophotonic devices and sensors.

A new facile colloidal synthesis of CuBiS2 (CBS) nanocrystals with monodispersed size and good quality has been developed. The CBS nanocrystal films were deposited by solid-state ligand exchange and their field effect transistor and photoconductive characteristics were characterized. The prototype solar cell has presented a decent performance. The suitable bandgap and highly appealing photoresponsivity demonstrate the as-synthesized CBS nanocrystals as an alternative to existing Cd- and Pb-containing nanocrystals for optoelectronic and photovoltaic devices.

Colloidal quantum dots (QDs) offer advantageous properties as an optical gain media for lasers. Optical gain in the QDs has been shown in the whole visible spectrum, yet it has been intrinsically challenging to realize efficient amplified spontaneous emission (ASE) and lasing in the blue region of the visible spectrum. Here, we synthesize large-sized core/gradient shell CdZnS/ZnS QDs as an efficient optical gain media in the blue spectral range. In this Letter, we demonstrate for the first time that two-photon-absorption-pumped ASE from the blue-emitting QD is achievable with a threshold as low as 6 mJ/cm 2. Utilizing these QDs, we also report one-photon-absorption-pumped ASE at an ultralow threshold of ∼60 μJ/cm2, which is comparable to the state-of-the-art red-emitting QD-based gain media. This one-photon-pumped ASE threshold is an order of magnitude better than that of the previously reported best blue-emitting QD-based gain media. © 2014 American Chemical Society.

Date of Conference: 28 August - 1 September 2016 Conference Name: SPIE NanoScience Engineering, 2016 We studied the photoluminescence (PL)) from CdSe/CdMnS/CdS core/multi-shell colloidal nanoplatelets, a versatile platform to study the interplay of optical properties and nanomagnetism. The photoluminescence (PL) exhibits σ+ polarization in the applied magnetic field. Our measurement detects the presence of even a single magnetic monolayer shell. The PLL consists of a higher and a lower energy component; the latter exhibits a circular polarization peak. The time-resolved PL (trPL) shows a red shift as function of time delay. At early (later) times the trPL spectra coincide with the high (low) energy PL component. A model is proposed to interpret these results.

Here, colloidal quantum dots (QDs) are successfully incorporated into anthracene crystals. In the resulting systems of QDs-in-anthracene, exciton transfer from anthracene to QDs was observed and highly polarized emission from QDs was discovered.

Solution-processed quantum wells, also known as colloidal nanoplatelets (NPLs), are emerging as promising materials for colloidal optoelectronics. In this work, we report the synthesis and characterization of CdSe/CdTe core/crown NPLs exhibiting a Type-II electronic structure and Type-II speci fic optical properties. Here, based on a core-seeded approach, the CdSe/CdTe core/crown NPLs were synthesized with well-controlled CdTe crown coatings. Uniform and epitaxial growth of CdTe crown region was verified by using structural characterization techniques including transmission electron microscopy (TEM) with quantitative EDX analysis and X-ray diffraction (XRD). Also the optical properties were systematically studied in these Type-II NPLs that reveal strongly red-shifted photoluminescence (up to ∼150 nm) along with 2 orders of magnitude longer fluorescence lifetimes (up to 190 ns) compared to the Type-I NPLs owing to spatially indirect excitons at the Type-II interface between the CdSe core and the CdTe crown regions. Photoluminescence excitation spectroscopy confirms that this strongly red-shifted emission actually arises from the CdSe/CdTe NPLs. In addition, temperature-dependent time-resolved fluorescence spectroscopy was performed to reveal the temperature-dependent fluorescence decay kinetics of the Type-II NPLs exhibiting interesting behavior. Also, water-soluble Type-II NPLs were achieved via ligand exchange of the CdSe/CdTe core/crown NPLs by using 3-mercaptopropionic acid (MPA), which allows for enhanced charge extraction efficiency owing to their shorter chain length and enables high quality film formation by layer-by-layer (LBL) assembly. With all of these appealing properties, the CdSe/CdTe core/crown heterostructures having Type-II electronic structure presented here are highly promising for light-harvesting applications. (Graph Presented). © 2015 American Chemical Society.

The synthesis and unique tunable optical properties of core/crown nanoplatelets having an inverted Type-I heterostructure are presented. Here, colloidal 2D CdS/CdSe heteronanoplatelets are grown with thickness of four monolayers using seed-mediated method. In this work, it is shown that the emission peak of the resulting CdS/CdSe heteronanoplatelets can be continuously spectrally tuned between the peak emission wavelengths of the core only CdS nanoplatelets (421 nm) and CdSe nanoplatelets (515 nm) having the same vertical thickness. In these inverted Type-I nanoplatelets, the unique continuous tunable emission is enabled by adjusting the lateral width of the CdSe crown, having a narrower bandgap, around the core CdS nanoplatelet, having a wider bandgap, as a result of the controlled lateral quantum confinement in the crown region additional to the pure vertical confinement. As a proof-of-concept demonstration, a white light generation is shown by using color conversion with these CdS/CdSe heteronanoplatelets having finely tuned thin crowns, resulting in a color rendering index of 80. The robust control of the electronic structure in such inverted Type-I heteronanoplatelets achieved by tailoring the lateral extent of the crown coating around the core template presents a new enabling pathway for bandgap engineering in solution-processed quantum wells. © 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

In this work, we report the manifestations of carrier-dopant exchange interactions in colloidal Mn2+-doped CdSe/CdS core/multishell quantum wells. The carrier-magnetic ion exchange interaction effects are tunable through wave function engineering. In our quantum well heterostructures, manganese was incorporated by growing a Cd0.985Mn0.015S monolayer shell on undoped CdSe nanoplatelets using the colloidal atomic layer deposition technique. Unlike previously synthesized Mn2+-doped colloidal nanostructures, the location of the Mn ions was controlled with atomic layer precision in our heterostructures. This is realized by controlling the spatial overlap between the carrier wave functions with the manganese ions by adjusting the location, composition, and number of the CdSe, Cd1-xMnxS, and CdS layers. The photoluminescence quantum yield of our magnetic heterostructures was found to be as high as 20% at room temperature with a narrow photoluminescence bandwidth of ∼22 nm. Our colloidal quantum wells, which exhibit magneto-optical properties analogous to those of epitaxially grown quantum wells, offer new opportunities for solution-processed spin-based semiconductor devices. © 2015 American Chemical Society.

In this work, centimeter-scale macrocrystals of nonpolar colloidal quantum dots (QDs) incorporated into anthracene were grown for the first time. The exciton transfer from the anthracene host to acceptor QDs was systematically investigated, and anisotropic emission from the isotropic QDs in the anthracene macrocrystals was discovered. Results showed a decreasing photoluminescence lifetime of the donor anthracene, indicating a strengthening energy transfer with increasing QD concentration in the macrocrystals. With the anisotropy study, QDs inside the anthracene host acquired a polarization ratio of ∼1.5 at 0° collection angle, and this increases to ∼2.5 at the collection angle of 60°. A proof-of-concept application of these excitonic macrocrystals as tunable color converters on light-emitting diodes was also demonstrated. © 2015 American Chemical Society.

An all-solution processed and all-colloidal laser is demonstrated using tailored CdSe/CdS core/shell quantum dots, which exhibit highly stable and low-threshold optical gain owing to substantially suppressed non-radiative Auger recombination. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.