Chemically Triggered Formation of Two-Dimensional Epitaxial Quantum Dot Superlattices.

PubMed

Walravens, Willem; De Roo, Jonathan; Drijvers, Emile; Ten Brinck, Stephanie; Solano, Eduardo; Dendooven, Jolien; Detavernier, Christophe; Infante, Ivan; Hens, Zeger

2016-07-26

Two dimensional superlattices of epitaxially connected quantum dots enable size-quantization effects to be combined with high charge carrier mobilities, an essential prerequisite for highly performing QD devices based on charge transport. Here, we demonstrate that surface active additives known to restore nanocrystal stoichiometry can trigger the formation of epitaxial superlattices of PbSe and PbS quantum dots. More specifically, we show that both chalcogen-adding (sodium sulfide) and lead oleate displacing (amines) additives induce small area epitaxial superlattices of PbSe quantum dots. In the latter case, the amine basicity is a sensitive handle to tune the superlattice symmetry, with strong and weak bases yielding pseudohexagonal or quasi-square lattices, respectively. Through density functional theory calculations and in situ titrations monitored by nuclear magnetic resonance spectroscopy, we link this observation to the concomitantly different coordination enthalpy and ligand displacement potency of the amine. Next to that, an initial ∼10% reduction of the initial ligand density prior to monolayer formation and addition of a mild, lead oleate displacing chemical trigger such as aniline proved key to induce square superlattices with long-range, square micrometer order; an effect that is the more pronounced the larger the quantum dots. Because the approach applies to PbS quantum dots as well, we conclude that it offers a reproducible and rational method for the formation of highly ordered epitaxial quantum dot superlattices.

Infra-red photoresponse of mesoscopic NiO-based solar cells sensitized with PbS quantum dot

PubMed Central

Raissi, Mahfoudh; Pellegrin, Yann; Jobic, Stéphane; Boujtita, Mohammed; Odobel, Fabrice

2016-01-01

Sensitized NiO based photocathode is a new field of investigation with increasing scientific interest in relation with the development of tandem dye-sensitized solar cells (photovoltaic) and dye-sensitized photoelectrosynthetic cells (solar fuel). We demonstrate herein that PbS quantum dots (QDs) represent promising inorganic sensitizers for NiO-based quantum dot-sensitized solar cells (QDSSCs). The solar cell sensitized with PbS quantum dot exhibits significantly higher photoconversion efficiency than solar cells sensitized with a classical and efficient molecular sensitizer (P1 dye = 4-(Bis-{4-[5-(2,2-dicyano-vinyl)-thiophene-2-yl]-phenyl}-amino)-benzoic acid). Furthermore, the system features an IPCE (Incident Photon-to-Current Efficiency) spectrum that spreads into the infra-red region, reaching operating wavelengths of 950 nm. The QDSSC photoelectrochemical device works with the complexes tris(4,4′-ditert-butyl-2,2′-bipyridine)cobalt(III/II) redox mediators, underscoring the formation of a long-lived charge-separated state. The electrochemical impedance spectrocopy measurements are consistent with a high packing of the QDs upon the NiO surface, the high density of which limits the access of the electrolyte and results in favorable light absorption cross-sections and a significant hole lifetime. These notable results highlight the potential of NiO-based photocathodes sensitized with quantum dots for accessing and exploiting the low-energy part of the solar spectrum in photovoltaic and photocatalysis applications. PMID:27125454

Charge Carrier Conduction Mechanism in PbS Quantum Dot Solar Cells: Electrochemical Impedance Spectroscopy Study.

PubMed

Wang, Haowei; Wang, Yishan; He, Bo; Li, Weile; Sulaman, Muhammad; Xu, Junfeng; Yang, Shengyi; Tang, Yi; Zou, Bingsuo

2016-07-20

With its properties of bandgap tunability, low cost, and substrate compatibility, colloidal quantum dots (CQDs) are becoming promising materials for optoelectronic applications. Additionally, solution-processed organic, inorganic, and hybrid ligand-exchange technologies have been widely used in PbS CQDs solar cells, and currently the maximum certified power conversion efficiency of 9.9% has been reported by passivation treatment of molecular iodine. Presently, there are still some challenges, and the basic physical mechanism of charge carriers in CQDs-based solar cells is not clear. Electrochemical impedance spectroscopy is a monitoring technology for current by changing the frequency of applied alternating current voltage, and it provides an insight into its electrical properties that cannot be measured by direct current testing facilities. In this work, we used EIS to analyze the recombination resistance, carrier lifetime, capacitance, and conductivity of two typical PbS CQD solar cells Au/PbS-TBAl/ZnO/ITO and Au/PbS-EDT/PbS-TBAl/ZnO/ITO, in this way, to better understand the charge carriers conduction mechanism behind in PbS CQD solar cells, and it provides a guide to design high-performance quantum-dots solar cells.

Measurement of Electronic States of PbS Nanocrystal Quantum Dots Using Scanning Tunneling Spectroscopy: The Role of Parity Selection Rules in Optical Absorption

NASA Astrophysics Data System (ADS)

Diaconescu, Bogdan; Padilha, Lazaro A.; Nagpal, Prashant; Swartzentruber, Brian S.; Klimov, Victor I.

2013-03-01

We study the structure of electronic states in individual PbS nanocrystal quantum dots by scanning tunneling spectroscopy (STS) using one-to-two monolayer nanocrystal films treated with 1, 2-ethanedithiols (EDT). Up to six individual valence and conduction band states are resolved for a range of quantum dot sizes. The measured states’ energies are in good agreement with calculations using the k·p four-band envelope function formalism. A comparison of STS and optical absorption spectra indicates that some of the absorption features can only be explained by asymmetric transitions involving the states of different symmetries (e.g., S and P or P and D), which points towards the relaxation of the parity selection rules in these nanostructures. STS measurements also reveal a midgap feature, which is likely similar to one observed in previous charge transport studies of EDT-treated quantum dot films.

Study of the back recombination processes of PbS quantum dots sensitized solar cells

NASA Astrophysics Data System (ADS)

Badawi, Ali; Al-Hosiny, N.; Merazga, Amar; Albaradi, Ateyyah M.; Abdallah, S.; Talaat, H.

2016-12-01

In this study, the back recombination processes of PbS quantum dots sensitized solar cells (QDSSCs) has been investigated. PbS QDs were adsorbed onto titania electrodes to act the role of sensitizers using successive ionic layer adsorption and reaction (SILAR) technique. The energy band gaps of the synthesized PbS QDs/titania are ranged from 1.64 eV (corresponding to 756 nm) to 3.12 eV (397 nm) matching the whole visible solar spectrum. The hyperbolic band model (HBM) was used to calculate PbS QDs size and it ranges from 1.76 to 3.44 nm. The photovoltaic parameters (open circuit voltage Voc, short circuit current density Jsc, fill factor FF and efficiency η) of the assembled PbS QDs sensitized solar cells (QDSSCs) were determined under a solar illumination of 100 mW/cm2 (AM 1.5 conditions). The open circuit voltage-decay (OCVD) rates of the assembled PbS QDSSCs were measured. The time constant (τ) for PbS QDSSCs (4 SILAR cycles) shows one order of magnitude larger than that of PbS QDSSCs (8 SILAR cycles) as a result of a decreased electron-hole back recombination.

Nongeminate Radiative Recombination of Free Charges in Cation-Exchanged PbS Quantum Dot Films

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marshall, Ashley R.; Beard, Matthew C.; Johnson, Justin C.

2016-06-01

Using photoluminescence (PL) spectroscopy we explore the radiative recombination pathways in PbS quantum dots (QDs) synthesized by two methods. We compare conventionally synthesized PbS from a PbO precursor to PbS synthesized using cation-exchange from CdS QDs. We show that strongly coupled films of PbS QDs from the cation-exchange luminesce with significant efficiency at room temperature. This is in stark contrast to conventional PbS QDs, which have exceedingly weak room temperature emission. Moreover, the power dependence of the emission is quadratic, indicating bimolecular radiative recombination that is reasonably competitive with trap-assisted recombination, a feature previously unreported in coupled PbS QD films.more » We interpret these results in terms of a greatly reduced defect concentration for cation-exchanged QDs that mitigates the influence of trap-assisted recombination. Cation-exchanged QDs have recently been employed in highly efficient and air-stable lead chalcogenide QD devices, and the reduced number of trap states inferred here may lead to improved current collection and higher open circuit voltage.« less

Nongeminate radiative recombination of free charges in cation-exchanged PbS quantum dot films

DOE Office of Scientific and Technical Information (OSTI.GOV)

Marshall, Ashley R.; Beard, Matthew C.; Johnson, Justin C.

2016-06-01

Using photoluminescence (PL) spectroscopy we explore the radiative recombination pathways in PbS quantum dots (QDs) synthesized by two methods. We compare conventionally synthesized PbS from a PbO precursor to PbS synthesized using cation-exchange from CdS QDs. We show that strongly coupled films of PbS QDs from the cation-exchange luminesce with significant efficiency at room temperature. This is in stark contrast to conventional PbS QDs, which have exceedingly weak room temperature emission. Moreover, the power dependence of the emission is quadratic, indicating bimolecular radiative recombination that is reasonably competitive with trap-assisted recombination, a feature previously unreported in coupled PbS QD films.more » We interpret these results in terms of a greatly reduced defect concentration for cation-exchanged QDs that mitigates the influence of trap-assisted recombination. Cation-exchanged QDs have recently been employed in highly efficient and air-stable lead chalcogenide QD devices, and the reduced number of trap states inferred here may lead to improved current collection and higher open circuit voltage.« less

XANES: observation of quantum confinement in the conduction band of colloidal PbS quantum dots

NASA Astrophysics Data System (ADS)

Demchenko, I. N.; Chernyshova, M.; He, X.; Minikayev, R.; Syryanyy, Y.; Derkachova, A.; Derkachov, G.; Stolte, W. C.; Piskorska-Hommel, E.; Reszka, A.; Liang, H.

2013-04-01

The presented investigations aimed at development of inexpensive method for synthesized materials suitable for utilization of solar energy. This important issue was addressed by focusing, mainly, on electronic local structure studies with supporting x-ray diffraction (XRD) and transmission electron microscopy (TEM) analysis of colloidal galena nano-particles (NPs) and quantum dots (QDs) synthesized using wet chemistry under microwave irradiation. Performed x-ray absorption near edge structure (XANES) analysis revealed an evidence of quantum confinement for the sample with QDs, where the bottom of the conduction band was shifted to higher energy. The QDs were found to be passivated with oxides at the surface. Existence of sulfate/sulfite and thiosulfate species in pure PbS and QDs, respectively, was identified.

Investigation of colloidal PbS quantum dot-based solar cells with near infrared emission.

PubMed

Lim, Sungoh; Kim, Yohan; Lee, Jeongno; Han, Chul Jong; Kang, Jungwon; Kim, Jiwan

2014-12-01

Colloidal quantum dots (QD)-based solar cells with near infrared (NIR) emission have been investigated. Lead sulfide (PbS) QDs, which have narrow band-gap and maximize the absorption of NIR spectrum, were chosen as active materials for efficient solar cells. The inverted structure of indium tin oxide/titanium dioxide/PbS QDs/poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate)/silver (ITO/TiO2/PbS QDs/ PSS/Ag) was applied for favorable electron and hole seperation from the PbS QD. Through the ligand exchange by 1,2-Ethanedithiol (EDT), the interparticle distance of the PbS QDs in thin film became closer and the performance of the PbS QD-based solar cells was improved. Our PbS QD-based inverted solar cells showed open circuit voltages (V(oc)) of 0.33 V, short circuit current density (J(sc)) of 10.89 mA/cm2, fill factor (FF) of 30%, and power conversion efficiency (PCE) of 1.11%. In our PbS QD-based multifunctional solar cell, the NIR light emission intensity was simply detected with photodiode system, which implies the potential of multi-functional diode device for various applications.

Synthetic Conditions for High-Accuracy Size Control of PbS Quantum Dots

DOE PAGES

Zhang, Jianbing; Crisp, Ryan W.; Gao, Jianbo; ...

2015-05-04

Decreasing the variability in quantum dot (QD) syntheses is desirable for better uniformity of samples for use in QD-based studies and applications. Here we report a highly reproducible linear relationship between the concentration of ligand (in this case oleic acid, OA) and the lowest energy exciton peak position (nm) of the resulting PbS QDs for various hot-injection temperatures. Thus, for a given injection temperature, the size of the PbS QD product is purely controlled by the amount of OA. We used this relationship to study PbS QD solar cells that are fabricated from the same size of PbS QDs butmore » synthesized using four different injection temperatures: 95, 120, 150, and 185 °C. We find that the power conversion efficiency does not depend on injection temperature but that the V oc is higher for QDs synthesized at lower temperatures while the J sc is improved in higher temperature QDs.« less

Electrochemical surface-enhanced Raman scattering measurement on ligand capped PbS quantum dots at gap of Au nanodimer

NASA Astrophysics Data System (ADS)

Li, Xiaowei; Minamimoto, Hiro; Murakoshi, Kei

2018-05-01

The vibrational characteristics of ligand-capped lead sulfide (PbS) quantum dots (QDs) were clarified via electrochemical surface-enhanced Raman spectroscopy (EC-SERS) using a hybridized system of gold (Au) nanodimers and PbS QDs under electrochemical potential control. Enhanced electromagnetic field caused by the coupling of QDs with plasmonic Au nanodimers allowed the characteristic behavior of the ligand oleic acid (OA) on the PbS QD surface to be detected under electrochemical potential control. Binding modes between the QDs and OA molecules were characterized using synchronous two-dimensional correlation spectra at distinct electrochemical potentials, confirming that the bidentate bridging mode was probably the most stable mode even under relatively negative potential polarization. Changes in binding modes and molecular orientations resulted in fluctuations in EC-SERS spectra. The present observations strongly recommend the validity of the QD-plasmonic nanostructure coupled system for sensitive molecular detection via EC-SERS.

‘Green’-synthesized near-infrared PbS quantum dots with silica-PEG dual-layer coating: ultrastable and biocompatible optical probes for in vivo animal imaging

NASA Astrophysics Data System (ADS)

Wang, D.; Qian, J.; Cai, F.; He, S.; Han, S.; Mu, Y.

2012-06-01

In this paper, PbS semiconductor quantum dots (QDs) with near-infrared (NIR) photoluminescence were synthesized in oleic acid and paraffin liquid mixture by using an easily handled and ‘green’ approach. Surface functionalization of the QDs was accomplished with a silica and polyethylene glycol (PEG) phospholipid dual-layer coating and the excellent chemical stability of the nanoparticles is demonstrated. We then successfully applied the ultrastable PbS QDs to in vivo sentinel lymph node (SLN) mapping of mice. Histological analyses were also carried out to ensure that the intravenously injected nanoparticles did not produce any toxicity to the organism of mice. These experimental results suggested that our ultrastable NIR PbS QDs can serve as biocompatible and efficient probes for in vivo optical bioimaging and has great potentials for disease diagnosis and clinical therapies in the future.

Effect of band-aligned double absorber layers on photovoltaic characteristics of chemical bath deposited PbS/CdS thin film solar cells.

PubMed

Ho Yeon, Deuk; Chandra Mohanty, Bhaskar; Lee, Seung Min; Soo Cho, Yong

2015-09-23

Here we report the highest energy conversion efficiency and good stability of PbS thin film-based depleted heterojunction solar cells, not involving PbS quantum dots. The PbS thin films were grown by the low cost chemical bath deposition (CBD) process at relatively low temperatures. Compared to the quantum dot solar cells which require critical and multistep complex procedures for surface passivation, the present approach, leveraging the facile modulation of the optoelectronic properties of the PbS films by the CBD process, offers a simpler route for optimization of PbS-based solar cells. Through an architectural modification, wherein two band-aligned junctions are stacked without any intervening layers, an enhancement of conversion efficiency by as much as 30% from 3.10 to 4.03% facilitated by absorption of a wider range of solar spectrum has been obtained. As an added advantage of the low band gap PbS stacked over a wide gap PbS, the devices show stability over a period of 10 days.

Tunability and Stability of Lead Sulfide Quantum Dots in Ferritin

NASA Astrophysics Data System (ADS)

Peterson, J. Ryan; Hansen, Kameron

Quantum dot solar cells have become one of the fastest growing solar cell technologies to date, and lead sulfide has proven to be an efficient absorber. However, one of the primary concerns in dye-sensitized quantum dot solar cell development is core degradation. We have synthesized lead sulfide quantum dots inside of the spherical protein ferritin in order to protect them from photocorrosion. We have studied the band gaps of these quantum dots and found them to be widely tunable inside ferritin just as they are outside the protein shell. In addition, we have examined their stability by measuring changes in photoluminescence as they are exposed to light over minutes and hours and found that the ferritin-enclosed PbS quantum dots have significantly better resistance to photocorrosion. Brigham Young University, National Science Foundation.

Size-dependent optical properties of colloidal PbS quantum dots.

PubMed

Moreels, Iwan; Lambert, Karel; Smeets, Dries; De Muynck, David; Nollet, Tom; Martins, José C; Vanhaecke, Frank; Vantomme, André; Delerue, Christophe; Allan, Guy; Hens, Zeger

2009-10-27

We quantitatively investigate the size-dependent optical properties of colloidal PbS nanocrystals or quantum dots (Qdots), by combining the Qdot absorbance spectra with detailed elemental analysis of the Qdot suspensions. At high energies, the molar extinction coefficient epsilon increases with the Qdot volume d(3) and agrees with theoretical calculations using the Maxwell-Garnett effective medium theory and bulk values for the Qdot dielectric function. This demonstrates that quantum confinement has no influence on epsilon in this spectral range, and it provides an accurate method to calculate the Qdot concentration. Around the band gap, epsilon only increases with d(1.3), and values are comparable to the epsilon of PbSe Qdots. The data are related to the oscillator strength f(if) of the band gap transition and results agree well with theoretical tight-binding calculations, predicting a linear dependence of f(if) on d. For both PbS and PbSe Qdots, the exciton lifetime tau is calculated from f(if). We find values ranging between 1 and 3 mus, in agreement with experimental literature data from time-resolved luminescence spectroscopy. Our results provide a thorough general framework to calculate and understand the optical properties of suspended colloidal quantum dots. Most importantly, it highlights the significance of the local field factor in these systems.

Enhanced interfacial contact between PbS and TiO2 layers in quantum dot solar cells using 2D-arrayed TiO2 hemisphere nanostructures

NASA Astrophysics Data System (ADS)

Lee, Wonseok; Ryu, Ilhwan; Lee, Haein; Yim, Sanggyu

2018-02-01

Two-dimensionally (2D) arrayed hemispherical nanostructures of TiO2 thin films were successfully fabricated using a simple procedure of spin-coating or dip-coating TiO2 nanoparticles onto 2D close-packed polystyrene (PS) nanospheres, followed by PS extraction. The nanostructured TiO2 film was then used as an n-type layer in a lead sulfide (PbS) colloidal quantum dot solar cell. The TiO2 nanostructure could provide significantly increased contacts with subsequently deposited PbS quantum dot layer. In addition, the periodically arrayed nanostructure could enhance optical absorption of the cell by redirecting the path of the incident light and increasing the path length passing though the active layer. As a result, the power conversion efficiency (PCE) reached 5.13%, which is approximately a 1.7-fold increase over that of the control cell without nanostructuring, 3.02%. This PCE enhancement can mainly be attributed to the increase of the short-circuit current density from 19.6 mA/cm2 to 30.6 mA/cm2, whereas the open-circuit voltage and fill factor values did not vary significantly.

Low temperature regulated growth of PbS quantum dots by wet chemical method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kumar, Hitanshu, E-mail: hitanshuminhas@gmail.com; Barman, P. B.; Singh, Ragini Raj

2015-08-28

Narrow size distribution with regulated synthesis of lead sulfide (PbS) quantum dots (QDs) was achieved through wet chemical method. Different concentrations of 2-mercaptoethanol (capping agent) were used for tailoring the QDs size. Transmission electron microscopy and X-ray diffraction studies revealed that the QDs have mean diameters between 6 to 15 nm. The optical absorption spectra were compared to the predictions of a theoretical model for the electronic structure. The theory agrees well with experiment for QDs larger than 7 nm, but for smaller dots there is some deviation from the theoretical predictions. Consequently, the produced particles are having monodispersity, good water solubility,more » stability and may be good arguments to be biologically compatible due to the use of 2-mercaptoethanol.« less

Fabrication of PbS quantum dots and their applications in solar cells based on ZnO nanorod arrays

NASA Astrophysics Data System (ADS)

Kumar, Dinesh; Chaudhary, Sujeet; Pandya, Dinesh K.

2018-05-01

An efficient, inexpensive and large area scalable approach based on sol-gel technique is presented to fabricate quantum dots (QDs) of PbS. Size of the QDs is tuned by the varying the bath concentrations in the range of 50-200 mM. Transmission electron microscopy (TEM) studies confirm the growth of spherically shaped ˜5.6 nm QDs at 50 mM bath concentration. The optical bandgap of the QDs is found to be ˜0.9 eV and corresponds to the size obtained from TEM studies. ZnO/PbS solar cells are fabricated by sensitizing the ZnO nanorods with PbS QDs. The fabricated solar cells demonstrate the highest open circuit voltage ˜200 mV and short circuit current density ˜0.81 µA/cm2.

High performance of PbSe/PbS core/shell quantum dot heterojunction solar cells: short circuit current enhancement without the loss of open circuit voltage by shell thickness control.

PubMed

Choi, Hyekyoung; Song, Jung Hoon; Jang, Jihoon; Mai, Xuan Dung; Kim, Sungwoo; Jeong, Sohee

2015-11-07

We fabricated heterojunction solar cells with PbSe/PbS core shell quantum dots and studied the precisely controlled PbS shell thickness dependency in terms of optical properties, electronic structure, and solar cell performances. When the PbS shell thickness increases, the short circuit current density (JSC) increases from 6.4 to 11.8 mA cm(-2) and the fill factor (FF) enhances from 30 to 49% while the open circuit voltage (VOC) remains unchanged at 0.46 V even with the decreased effective band gap. We found that the Fermi level and the valence band maximum level remain unchanged in both the PbSe core and PbSe/PbS core/shell with a less than 1 nm thick PbS shell as probed via ultraviolet photoelectron spectroscopy (UPS). The PbS shell reduces their surface trap density as confirmed by relative quantum yield measurements. Consequently, PbS shell formation on the PbSe core mitigates the trade-off relationship between the open circuit voltage and the short circuit current density. Finally, under the optimized conditions, the PbSe core with a 0.9 nm thick shell yielded a power conversion efficiency of 6.5% under AM 1.5.

Graphene and PbS quantum dot hybrid vertical phototransistor

NASA Astrophysics Data System (ADS)

Song, Xiaoxian; Zhang, Yating; Zhang, Haiting; Yu, Yu; Cao, Mingxuan; Che, Yongli; Dai, Haitao; Yang, Junbo; Ding, Xin; Yao, Jianquan

2017-04-01

A field-effect phototransistor based on a graphene and lead sulfide quantum dot (PbS QD) hybrid in which PbS QDs are embedded in a graphene matrix has been fabricated with a vertical architecture through a solution process. The n-type Si/SiO2 substrate (gate), Au/Ag nanowire transparent source electrode, active layer and Au drain electrode are vertically stacked in the device, which has a downscaled channel length of 250 nm. Photoinduced electrons in the PbS QDs leap into the conduction band and fill in the trap states, while the photoinduced holes left in the valence band transfer to the graphene and form the photocurrent under biases from which the photoconductive gain is evaluated. The graphene/QD-based vertical phototransistor shows a photoresponsivity of 2 × 103 A W-1, and specific detectivity up to 7 × 1012 Jones under 808 nm laser illumination with a light irradiance of 12 mW cm-2. The solution-processed vertical phototransistor provides a new facile method for optoelectronic device applications.

Chemical processing of three-dimensional graphene networks on transparent conducting electrodes for depleted-heterojunction quantum dot solar cells.

PubMed

Tavakoli, Mohammad Mahdi; Simchi, Abdolreza; Fan, Zhiyong; Aashuri, Hossein

2016-01-07

We present a novel chemical procedure to prepare three-dimensional graphene networks (3DGNs) as a transparent conductive film to enhance the photovoltaic performance of PbS quantum-dot (QD) solar cells. It is shown that 3DGN electrodes enhance electron extraction, yielding a 30% improvement in performance compared with the conventional device.

Silica coating of PbS quantum dots and their position control using a nanohole on Si substrate

NASA Astrophysics Data System (ADS)

Mukai, Kohki; Okumura, Isao; Nishizaki, Yuta; Yamashita, Shuzo; Niwa, Keisuke

2018-04-01

We succeeded in controlling the apparent size of a colloidal PbS quantum dot (QD) in the range of 20 to 140 nm by coating with silica and trapping the coated QDs in a nanohole prepared by scanning probe microscope lithography. Photoluminescence intensity was improved by controlling the process of adding the silica source material of tetraethoxysilane for the coating. Nanoholes of different sizes were formed on a single substrate by scanning probe oxidation with the combination of SF6 dry etching and KOH wet etching. QDs having an arbitrary energy structure can be arranged at an arbitrary position on the semiconductor substrate using this technique, which will aid in the fabrication of future nanosize solid devices such as quantum information circuits.

Fast current blinking in individual PbS and CdSe quantum dots.

PubMed

Maturova, Klara; Nanayakkara, Sanjini U; Luther, Joseph M; van de Lagemaat, Jao

2013-06-12

Fast current intermittency of the tunneling current through single semiconductor quantum dots was observed through time-resolved intermittent contact conductive atomic force microscopy in the dark and under illumination at room temperature. The current through a single dot switches on and off at time scales ranging from microseconds to seconds with power-law distributions for both the on and off times. On states are attributed to the resonant tunneling of charges from the electrically conductive AFM tip to the quantum dot, followed by transfer to the substrate, whereas off states are attributed to a Coulomb blockade effect in the quantum dots that shifts the energy levels out of resonance conditions due to the presence of the trapped charge, while at the same bias. The observation of current intermittency due to Coulomb blockade effects has important implications for the understanding of carrier transport through arrays of quantum dots.

Water-mediated green synthesis of PbS quantum dot and its glutathione and biotin conjugates for non-invasive live cell imaging

NASA Astrophysics Data System (ADS)

Vijaya Bharathi, M.; Maiti, Santanu; Sarkar, Bidisha; Ghosh, Kaustab; Paira, Priyankar

2018-03-01

This study addresses the cellular uptake of nanomaterials in the field of bio-applications. In the present study, we have synthesized water-soluble lead sulfide quantum dot (PbS QD) with glutathione and 3-MPA (mercaptopropionic acid) as the stabilizing ligand using a green approach. 3-MPA-capped QDs were further modified with streptavidin and then bound to biotin because of its high conjugation efficiency. Labelling and bio-imaging of cells with these bio-conjugated QDs were evaluated. The bright red fluorescence from these types of QDs in HeLa cells makes these materials suitable for deep tissue imaging.

Enhanced absorption with quantum dots, metal nanoparticles, and 2D materials

NASA Astrophysics Data System (ADS)

Simsek, Ergun; Mukherjee, Bablu; Guchhait, Asim; Chan, Yin Thai

2016-03-01

We fabricate and characterize mono- and few- layers of MoS2 and WSe2 on glass and SiO2/Si substrates. PbS quantum dots and/or Au nanoparticles are deposited on the fabricated thin metal dichalcogenide films by controlled drop casting and electron beam evaporation techniques. The reflection spectra of the fabricated structures are measured with a spatially resolved reflectometry setup. Both experimental and numerical results show that surface functionalization with metal nanoparticles can enhance atomically thin transition metal dichalcogenides' absorption and scattering capabilities, however semiconducting quantum dots do not create such effect.

Luminescence and transient lifetime studies for energy transfer of PbS QD films

NASA Astrophysics Data System (ADS)

Wang, Joanna S.; Ullrich, Bruno; Dass, Chandriker K.; Das, Anirban; Wai, Chien M.; Brown, Gail J.; Hendrickson, Joshua R.

2017-08-01

Quantum confined semiconductor materials in colloidal form have drawn great attention in scientific communities due to the size-tunability, which controls their optical properties. PbS quantum dots (QDs) are exciting candidates for quantum optics, particularly due to the control of the QD sizes during the synthetic process enabling the realization of precisely tunable emission properties in the near-infrared region. Differently sized pairs of PbS QDs were deposited onto glass substrates to form thin films using supercritical CO2 (sc-CO2) deposition and solvent deposition methods (SDM). The fluorescence and photoluminescence (PL) spectra obtained from these closely packed films prepared by the sc-CO2 method reveal effective Förster resonance energy transfer (FRET) between two different sized dots, while the films composed of three different QD sizes show an even more effective FRET from the smallest to the largest ones. Energy transfer can be observed more directly by temporally resolved PL decay of mixed dots. By means of transient lifetime measurements, a mixed PbS film with 3.1 and 4.7 nm QDs was studied for FRET by time correlated single photon counting. The PL peak of the 3.1 nm QDs is quenched with respect to the emission of the 4.7 nm QDs and decays faster, and the best fit for the lifetime (decay constant)-1 is a biexponential decay mode. The long wavelength decay (4.7 nm QDs) is best fit by a mono-exponential equation. More theoretical and experimental work is required for a thorough understanding of the radiative lifetimes of PbS QDs in mixed QD systems.

Reduced Carrier Recombination in PbS - CuInS2 Quantum Dot Solar Cells

PubMed Central

Sun, Zhenhua; Sitbon, Gary; Pons, Thomas; Bakulin, Artem A.; Chen, Zhuoying

2015-01-01

Energy loss due to carrier recombination is among the major factors limiting the performance of TiO2/PbS colloidal quantum dot (QD) heterojunction solar cells. In this work, enhanced photocurrent is achieved by incorporating another type of hole-transporting QDs, Zn-doped CuInS2 (Zn-CIS) QDs into the PbS QD matrix. Binary QD solar cells exhibit a reduced charge recombination associated with the spatial charge separation between these two types of QDs. A ~30% increase in short-circuit current density and a ~20% increase in power conversion efficiency are observed in binary QD solar cells compared to cells built from PbS QDs only. In agreement with the charge transfer process identified through ultrafast pump/probe spectroscopy between these two QD components, transient photovoltage characteristics of single-component and binary QDs solar cells reveal longer carrier recombination time constants associated with the incorporation of Zn-CIS QDs. This work presents a straightforward, solution-processed method based on the incorporation of another QDs in the PbS QD matrix to control the carrier dynamics in colloidal QD materials and enhance solar cell performance. PMID:26024021

Band-structure tailoring and surface passivation for highly efficient near-infrared responsive PbS quantum dot photovoltaics

NASA Astrophysics Data System (ADS)

Zhou, Ru; Niu, Haihong; Ji, Fengwei; Wan, Lei; Mao, Xiaoli; Guo, Huier; Xu, Jinzhang; Cao, Guozhong

2016-11-01

PbS is a promising light harvester for near-infrared (NIR) responsive quantum dot (QD) photovoltaics due to its narrow bulk band gap (0.41 eV) and large exciton Bohr radius (18 nm). However, the relatively low conduction band (CB) and high-density surface defects of PbS as two major drawbacks for its use in solar cells severely hamper the photovoltaic performance enhancement. In this work, a modified solution-based successive ionic layer adsorption and reaction (SILAR) utilizing mixed cationic precursors of Pb2+ and Cd2+ is explored, and such a scheme offers two benefits, band-structure tailoring and surface passivation. In-situ deposited CdS suppresses the excessive growth of PbS in the mesopores, thereby facilitating the favorable electron injection from PbS to TiO2 in view of the up-shifted CB level of QDs; the intimate interpenetration of two sulfides with each other leads to superior passivation of trap state defects on PbS, which suppresses the interfacial charge recombination. With the construction of photovoltaics based on such a hybrid (Pb,Cd)S/CdS configuration, impressive power conversion efficiency up to 4.08% has been reached, outperforming that of the conventional PbS/CdS pattern (2.95%). This work highlights the great importance of band-structure tailoring and surface passivation for constructing highly efficient PbS QD photovoltaics.

All-solution-processed PbS quantum dot solar modules.

PubMed

Jang, Jihoon; Shim, Hyung Cheoul; Ju, Yeonkyeong; Song, Jung Hoon; An, Hyejin; Yu, Jong-Su; Kwak, Sun-Woo; Lee, Taik-Min; Kim, Inyoung; Jeong, Sohee

2015-05-21

A rapid increase in power conversion efficiencies in colloidal quantum dot (QD) solar cells has been achieved recently with lead sulphide (PbS) QDs by adapting a heterojunction architecture, which consists of small-area devices associated with a vacuum-deposited buffer layer with metal electrodes. The preparation of QD solar modules by low-cost solution processes is required to further increase the power-to-cost ratio. Herein we demonstrate all-solution-processed flexible PbS QD solar modules with a layer-by-layer architecture comprising polyethylene terephthalate (PET) substrate/indium tin oxide (ITO)/titanium oxide (TiO2)/PbS QD/poly(3-hexylthiophene) (P3HT)/poly(3,4-ethylenedioxythiophene) : poly(styrene sulfonate) (PEDOT : PSS)/Ag, with an active area of up to 30 cm(2), exhibiting a power conversion efficiency (PCE) of 1.3% under AM 1.5 conditions (PCE of 2.2% for a 1 cm(2) unit cell). Our approach affords trade-offs between power and the active area of the photovoltaic devices, which results in a low-cost power source, and which is scalable to larger areas.

Electron-Electron and Electron-Phonon interactions effects on the tunnel electronic spectrum of PbS quantum dots

NASA Astrophysics Data System (ADS)

Wang, Hongyue; Lhuillier, Emmanuel; Yu, Qian; Mottaghizadeh, Alireza; Ulysse, Christian; Zimmers, Alexandre; Dubertret, Benoit; Aubin, Herve

2015-03-01

We present a tunnel spectroscopy study of the electronic spectrum of single PbS Quantum Dots (QDs) trapped between nanometer-spaced electrodes, measured at low temperature T=5 K. The carrier filling of the QD can be controlled either by the drain voltage in the shell filling regime or by a gate voltage. In the empty QD, the tunnel spectrum presents the expected signature of the 8x degenerated excited levels. In the drain controlled shell filling regime, the levels degeneracies are lifted by the global electrostatic Coulomb energy of the QD; in the gate controlled shell filling regime, the levels degeneracies are lifted by the intra-Coulomb interactions. In the charged quantum dot, electron-phonons interactions lead to the apparition of Franck-Condon side bands on the single excited levels and possibly Franck Condon blockade at low energy. The sharpening of excited levels at higher gate voltage suggests that the magnitude of electron-phonon interactions is decreased upon increasing the electron filling in the quantum dot. This work was supported by the French ANR Grants 10-BLAN-0409-01, 09-BLAN-0388-01, by the Region Ile-de-France in the framework of DIM Nano-K and by China Scholarship Council.

Exceeding Conventional Photovoltaic Efficiency Limits Using Colloidal Quantum Dots

NASA Astrophysics Data System (ADS)

Pach, Gregory F.

Colloidal quantum dots (QDs) are a widely investigated field of research due to their highly tunable nature in which the optical and electronic properties of the nanocrystal can be manipulated by merely changing the nanocrystal's size. Specifically, colloidal quantum dot solar cells (QDSCs) have become a promising candidate for future generation photovoltaic technology. Quantum dots exhibit multiple exciton generation (MEG) in which multiple electron-hole pairs are generated from a single high-energy photon. This process is not observed in bulk-like semiconductors and allows for QDSCs to achieve theoretical efficiency limits above the standard single-junction Shockley-Queisser limit. However, the fast expanding field of QDSC research has lacked standardization of synthetic techniques and device design. Therefore, we sought to detail methodology for synthesizing PbS and PbSe QDs as well as photovoltaic device fabrication techniques as a fast track toward constructing high-performance solar cells. We show that these protocols lead toward consistently achieving efficiencies above 8% for PbS QDSCs. Using the same methodology for building single-junction photovoltaic devices, we incorporated PbS QDs as a bottom cell into a monolithic tandem architecture along with solution-processed CdTe nanocrystals. Modeling shows that near-peak tandem device efficiencies can be achieved across a wide range of bottom cell band gaps, and therefore the highly tunable band gap of lead-chalcogenide QDs lends well towards a bottom cell in a tandem architecture. A fully functioning monolithic tandem device is realized through the development of a ZnTe/ZnO recombination layer that appropriately combines the two subcells in series. Multiple recent reports have shown nanocrystalline heterostructures to undergo the MEG process more efficiency than several other nanostrucutres, namely lead-chalcogenide QDs. The final section of my thesis expands upon a recent publication by Zhang et. al., which details the synthesis of PbS/CdS heterostructures in which the PbS and CdS domains exist on opposite sides of the nanocrystal and are termed "Janus particles". Transient absorption spectroscopy shows MEG quantum yields above unity very the thermodynamic limit of 2Eg for PbS/CdS Janus particles. We further explain a mechanism for enhanced MEG using photoluminescence studies.

Optical and electrical characterizations of a single step ion beam milling mesa devices of chloride passivated PbS colloidal quantum dots based film

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hechster, Elad, E-mail: elad.hechster@gmail.com; Sarusi, Gabby; Shapiro, Arthur

Colloidal Quantum Dots (CQDs) are of increasing interest, thanks to their quantum size effect that gives rise to their usage in various applications, such as biological tagging, solar cells and as the sensitizing layer of night vision devices. Here, we analyze the optical absorbance of chloride passivated PbS CQDs as well as revealing a correlation between their photoluminescence and sizes distribution, using theoretical models and experimental results from the literature. Next, we calculate the CQDs resistivity as a film. Although resistivity can be calculated from sheet resistance measurement using four point probes, such measurement is usually carried-out on the layer’smore » surface that in most cases has dangling bonds and surface states, which might affect the charges flow and modify the resistivity. Therefore; our approach, which was applied in this work, is to extract the actual resistivity from measurements that are performed along the film’s thickness (z-direction). For this intent, we fabricated gold capped PbS mesas devices using a single step Ion Beam Milling (IBM) process where we milled the gold and the PbS film continually, and then measured the vertical resistance. Knowing the mesas’ dimensions, we calculate the resistivity. To the best of our knowledge, no previous work has extracted, vertically, the resistivity of chloride passivated PbS CQDs using the above method.« less

Mode-locked Er-doped fiber laser based on PbS/CdS core/shell quantum dots as saturable absorber.

PubMed

Ming, Na; Tao, Shina; Yang, Wenqing; Chen, Qingyun; Sun, Ruyi; Wang, Chang; Wang, Shuyun; Man, Baoyuan; Zhang, Huanian

2018-04-02

Previously, PbS/CdS core/shell quantum dots with excellent optical properties have been widely used as light-harvesting materials in solar cell and biomarkers in bio-medicine. However, the nonlinear absorption characteristics of PbS/CdS core/shell quantum dots have been rarely investigated. In this work, PbS/CdS core/shell quantum dots were successfully employed as nonlinear saturable absorber (SA) for demonstrating a mode-locked Er-doped fiber laser. Based on a film-type SA, which was prepared by incorporating the quantum dots with the polyvinyl alcohol (PVA), mode-locked Er-doped operation with a pulse width of 54 ps and a maximum average output power of 2.71 mW at the repetition rate of 3.302 MHz was obtained. Our long-time stable results indicate that the CdS shell can effectively protect the PbS core from the effect of photo-oxidation and PbS/CdS core/shell quantum dots were efficient SA candidates for demonstrating pulse fiber lasers due to its tunable absorption peak and excellent saturable absorption properties.

Surface Traps in Colloidal Quantum Dots: A Combined Experimental and Theoretical Perspective.

PubMed

Giansante, Carlo; Infante, Ivan

2017-10-19

Surface traps are ubiquitous to nanoscopic semiconductor materials. Understanding their atomistic origin and manipulating them chemically have capital importance to design defect-free colloidal quantum dots and make a leap forward in the development of efficient optoelectronic devices. Recent advances in computing power established computational chemistry as a powerful tool to describe accurately complex chemical species and nowadays it became conceivable to model colloidal quantum dots with realistic sizes and shapes. In this Perspective, we combine the knowledge gathered in recent experimental findings with the computation of quantum dot electronic structures. We analyze three different systems: namely, CdSe, PbS, and CsPbI 3 as benchmark semiconductor nanocrystals showing how different types of trap states can form at their surface. In addition, we suggest experimental healing of such traps according to their chemical origin and nanocrystal composition.

Quantum Dot Solar Cell Fabrication Protocols

DOE PAGES

Chernomordik, Boris D.; Marshall, Ashley R.; Pach, Gregory F.; ...

2016-09-26

Colloidally synthesized quantum-confined semiconducting spherical nanocrystals, often referred to as quantum dots (QDs), offer a high degree of chemical, optical, and electronic tunability. As a result, there is an increasing interest in employing colloidal QDs for electronic and optical applications that is reflected in a growing number of publications. In this protocol we provide detailed procedures for the fabrication of QD solar cells specifically employing PbSe and PbS QDs. Here we include details that are learned through experience, beyond those in typical methodology sections, and include example pictures and videos to aid in fabricating QD solar cells. Although successful solarmore » cell fabrication is ultimately learned through experience, this protocol is intended to accelerate that process. The protocol developed here is intended to be a general starting point for developing PbS and PbSe QD test bed solar cells. We include steps for forming conductive QD films via dip coating as well as spin coating. Finally, we provide protocols that detail the synthesis of PbS and PbSe QDs through a unique cation exchange reaction and discuss how different QD synthetic routes could impact the resulting solar cell performance.« less

Quantum Dot Solar Cell Fabrication Protocols

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chernomordik, Boris D.; Marshall, Ashley R.; Pach, Gregory F.

Colloidally synthesized quantum-confined semiconducting spherical nanocrystals, often referred to as quantum dots (QDs), offer a high degree of chemical, optical, and electronic tunability. As a result, there is an increasing interest in employing colloidal QDs for electronic and optical applications that is reflected in a growing number of publications. In this protocol we provide detailed procedures for the fabrication of QD solar cells specifically employing PbSe and PbS QDs. Here we include details that are learned through experience, beyond those in typical methodology sections, and include example pictures and videos to aid in fabricating QD solar cells. Although successful solarmore » cell fabrication is ultimately learned through experience, this protocol is intended to accelerate that process. The protocol developed here is intended to be a general starting point for developing PbS and PbSe QD test bed solar cells. We include steps for forming conductive QD films via dip coating as well as spin coating. Finally, we provide protocols that detail the synthesis of PbS and PbSe QDs through a unique cation exchange reaction and discuss how different QD synthetic routes could impact the resulting solar cell performance.« less

High-performance PbS quantum dot vertical field-effect phototransistor using graphene as a transparent electrode

NASA Astrophysics Data System (ADS)

Che, Yongli; Zhang, Yating; Cao, Xiaolong; Song, Xiaoxian; Zhang, Haiting; Cao, Mingxuan; Dai, Haitao; Yang, Junbo; Zhang, Guizhong; Yao, Jianquan

2016-12-01

Solution processed photoactive PbS quantum dots (QDs) were used as channel in high-performance near-infrared vertical field-effect phototransistor (VFEpT) where monolayer graphene embedded as transparent electrode. In this vertical architecture, the PbS QD channel was sandwiched and naturally protected between the drain and source electrodes, which made the device ultrashort channel length (110 nm) simply the thickness of the channel layer. The VFEpT exhibited ambipolar operation with high mobilities of μe = 3.5 cm2/V s in n-channel operation and μh = 3.3 cm2/V s in p-channel operation at low operation voltages. By using the photoactive PbS QDs as channel material, the VFEpT exhibited good photoresponse properties with a responsivity of 4.2 × 102 A/W, an external quantum efficiency of 6.4 × 104% and a photodetectivity of 2.1 × 109 Jones at the light irradiance of 36 mW/cm2. Additionally, the VFEpT showed excellent on/off switching with good stability and reproducibility and fast response speed with a short rise time of 12 ms in n-channel operation and 10.6 ms in p-channel operation. These high mobilities, good photoresponse properties and simplistic fabrication of our VFEpTs provided a facile route to the high-performance inorganic photodetectors.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Park, Samuel; Baranov, Dmitry; Ryu, Jisu

Pump-probe polarization anisotropy measurements with 15 fs pulses are employed to investigate the electronic structure of PbS quantum dots. Here, the initial anisotropy at the bandgap is anomalously low (<0.1) and suggests large electronic couplings.

Passivation Using Molecular Halides Increases Quantum Dot Solar Cell Performance.

PubMed

Lan, Xinzheng; Voznyy, Oleksandr; Kiani, Amirreza; García de Arquer, F Pelayo; Abbas, Abdullah Saud; Kim, Gi-Hwan; Liu, Mengxia; Yang, Zhenyu; Walters, Grant; Xu, Jixian; Yuan, Mingjian; Ning, Zhijun; Fan, Fengjia; Kanjanaboos, Pongsakorn; Kramer, Illan; Zhitomirsky, David; Lee, Philip; Perelgut, Alexander; Hoogland, Sjoerd; Sargent, Edward H

2016-01-13

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. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Surface Traps in Colloidal Quantum Dots: A Combined Experimental and Theoretical Perspective

PubMed Central

2017-01-01

Surface traps are ubiquitous to nanoscopic semiconductor materials. Understanding their atomistic origin and manipulating them chemically have capital importance to design defect-free colloidal quantum dots and make a leap forward in the development of efficient optoelectronic devices. Recent advances in computing power established computational chemistry as a powerful tool to describe accurately complex chemical species and nowadays it became conceivable to model colloidal quantum dots with realistic sizes and shapes. In this Perspective, we combine the knowledge gathered in recent experimental findings with the computation of quantum dot electronic structures. We analyze three different systems: namely, CdSe, PbS, and CsPbI3 as benchmark semiconductor nanocrystals showing how different types of trap states can form at their surface. In addition, we suggest experimental healing of such traps according to their chemical origin and nanocrystal composition. PMID:28972763

Lead Sulfide Cathode for Quantum Dot Solar Cells: Electrosynthesis and Characterization

NASA Astrophysics Data System (ADS)

Van Le, Nghiem; Nguyen, Hoang Thai; Le, Hai Viet; Nguyen, Thoa Thi Phuong

2017-01-01

Deposition of lead sulfide (PbS) nanocrystalline thin films onto conducting fluorine-doped tin oxide (FTO) glass has been performed by cyclic voltammetry (CV) in 1.5 mM solution of lead nitrate and sodium thiosulfate at 100 mV s-1 scan rate in the potential range of -1.0 V to 0.0 V versus saturated calomel electrode. X-ray diffraction analysis and scanning electron microscopy revealed formation of cubic PbS crystals with size of 100 nm to 150 nm after 50 cycles. High electrocatalytic activity of the synthesized PbS film for the S2-/S n 2- redox couple, used as a mediator for quantum dot solar cells (QDSCs), was demonstrated by electrochemical impedance spectroscopy and CV measurements. The prepared PbS/FTO was used as a counterelectrode to fabricate PbS-QDSCs with a photoanode consisting of CdS/CdSe quantum dots adsorbed on mesoporous TiO2 film and a polysulfide solution electrolyte. The performance of the PbS-QDSC was compared with a QDSC with a platinum counterelectrode (Pt-QDSC). It was found that, using the same fabrication conditions, the performance of the PbS-QDSC was better than that of the Pt-QDSC. At 1 sun (100 mW cm-2) simulated light, average energy conversion efficiency of 2.14%, short-circuit current of 9.22 mA cm-2, open-circuit potential of 0.50 V, and fill factor of 0.47 were achieved by the fabricated PbS-QDSC.

Enhanced performance of solution-processed broadband photodiodes by epitaxially blending MAPbBr3 quantum dots and ternary PbSxSe1-x quantum dots as the active layer.

PubMed

Sulaman, Muhammad; Yang, Shengyi; Jiang, Yurong; Tang, Yi; Zou, Bingsuo

2017-12-15

Organic-inorganic hybrid photodetectors attract more and more interest, since they can combine the advantages of both organic and inorganic materials into one device, and broadband photodetectors are widely used in many scientific and industrial fields. In this work, we demonstrate the enhanced-performance solution-processed broadband photodiodes by epitaxially blending organo-lead halide perovskite (MAPbBr 3 ) colloidal quantum dots (CQDs) with ternary PbS x Se 1-x CQDs as the active layer. As a result, the interfacial features of the hetero-epitaxial nanocomposite MAPbBr 3 :PbS x Se 1-x enables the design and perception of functionalities that are not available for the single-phase constituents or layered devices. By combining the high electrical transport properties of MAPbBr 3 QDs with the highly radiative efficiency of PbS 0.4 Se 0.6 QDs, the photodiodes ITO/ZnO/PbS 0.4 Se 0.6 :MAPbBr 3 /Au exhibit a maximum photoresponsivity and specific detectivity of 21.48 A W -1 and 3.59 × 10 13 Jones, 22.16 A W -1 and 3.70 × 10 13 Jones at room temperature under 49.8 μW cm -2 532 nm laser and 62 μW cm -2 980 nm laser, respectively. This is higher than that of the layered photodiodes ITO/ZnO/PbS 0.4 Se 0.6 /MAPbBr 3 /Au, pure perovskite (MAPbBr 3 ) (or PbS 0.4 Se 0.6 ) QD-based photodiodes reported previously, and it is also better than the traditional inorganic semiconductor-based photodetectors. Our experimental results indicate that epitaxially-aligned nanocomposites (MAPbBr 3 :PbS x Se 1-x ) exhibit remarkable optoelectronic properties that are traceable to their atomic-scale crystalline coherence, and one can utilize the excellent photocarrier diffusion from PbS x Se 1-x into the perovskite to enhance the device performance from the UV-visible to infrared region.

Novel Photovoltaic Devices Using Ferroelectric Material and Colloidal Quantum Dots

NASA Astrophysics Data System (ADS)

Paik, Young Hun

As the global concern for the financial and environmental costs of traditional energy resources increases, research on renewable energy, most notably solar energy, has taken center stage. Many alternative photovoltaic (PV) technologies for 'the next generation solar cell' have been extensively studied to overcome the Shockley-Queisser 31% efficiency limit as well as tackle the efficiency vs. cost issues. This dissertation focuses on the novel photovoltaic mechanism for the next generation solar cells using two inorganic nanomaterials, nanocrystal quantum dots and ferroelectric nanoparticles. Lead zirconate titanate (PZT) materials are widely studied and easy to synthesize using solution based chemistry. One of the fascinating properties of the PZT material is a Bulk Photovoltaic effect (BPVE). This property has been spotlighted because it can produce very high open circuit voltage regardless of the electrical bandgap of the materials. However, the poor optical absorption of the PZT materials and the required high temperature to form the ferroelectric crystalline structure have been obstacles to fabricate efficient photovoltaic devices. Colloidal quantum dots also have fascinating optical and electrical properties such as tailored absorption spectrum, capability of the bandgap engineering due to the wide range of material selection and quantum confinement, and very efficient carrier dynamics called multiple exciton generations. In order to utilize these properties, many researchers have put numerous efforts in colloidal quantum dot photovoltaic research and there has been remarkable progress in the past decade. However, several drawbacks are still remaining to achieve highly efficient photovoltaic device. Traps created on the large surface area, low carrier mobility, and lower open circuit voltage while increasing the absorption of the solar spectrum is main issues of the nanocrystal based photovoltaic effect. To address these issues and to take the advantages of the two materials, this dissertation focused on material synthesis for low cost solution process for both materials, fabrication of various device structures and electrical/optical characterization to understand the underlying physics. We successfully demonstrated lead sulfide quantum dots (PbS QDs) and lead zirconate titanate nanoparticles (PZT NPs) in an aqueous solution and fabricated a photosensitive device. Solution based low-temperature process was used to fabricate a PbS QD and a PZT NP device. We exhibited a superior photoresponse and ferroelectric photovoltaic properties with the novel PZT NP device and studied the physics on domain wall effect and internal polarity effect. PZT NP was mainly investigated because PZT NP device is the first report as a photosensitive device with a successful property demonstration, as we know of. PZT's crystalline structure and the size of the nanocrystals were studied using X-ray diffraction and TEM (Transmission electron microscopy) respectively. We observed < 100 nm of PZT NPs and this result matched with DLS (dynamic light scattering) measurement. We fabricated ferroelectric devices using the PZT NPs for the various optical and electrical characterizations and verified ferroelectric properties including ferroelectric hysteresis loop. We also observed a typical ferroelectric photovoltaic effect from a PZT NP based device which was fabricated on an ITO substrate. We synthesized colloidal quantum dots (CQD) with the inexpensive soluble process. Fabricated PbS QD was used for the hybrid device with PZT thin films. J-V measured and the result shows superior open circuit voltage characteristics compared to conventional PbS QD PV devices, and resulting the improvement of the solar cell efficiency. This Ferroelectrics and Quantum Dots (FE-QDs) device also the first trial and the success as we know of.

All-solution-processed PbS quantum dot solar modules

NASA Astrophysics Data System (ADS)

Jang, Jihoon; Shim, Hyung Cheoul; Ju, Yeonkyeong; Song, Jung Hoon; An, Hyejin; Yu, Jong-Su; Kwak, Sun-Woo; Lee, Taik-Min; Kim, Inyoung; Jeong, Sohee

2015-05-01

A rapid increase in power conversion efficiencies in colloidal quantum dot (QD) solar cells has been achieved recently with lead sulphide (PbS) QDs by adapting a heterojunction architecture, which consists of small-area devices associated with a vacuum-deposited buffer layer with metal electrodes. The preparation of QD solar modules by low-cost solution processes is required to further increase the power-to-cost ratio. Herein we demonstrate all-solution-processed flexible PbS QD solar modules with a layer-by-layer architecture comprising polyethylene terephthalate (PET) substrate/indium tin oxide (ITO)/titanium oxide (TiO2)/PbS QD/poly(3-hexylthiophene) (P3HT)/poly(3,4-ethylenedioxythiophene) : poly(styrene sulfonate) (PEDOT : PSS)/Ag, with an active area of up to 30 cm2, exhibiting a power conversion efficiency (PCE) of 1.3% under AM 1.5 conditions (PCE of 2.2% for a 1 cm2 unit cell). Our approach affords trade-offs between power and the active area of the photovoltaic devices, which results in a low-cost power source, and which is scalable to larger areas.A rapid increase in power conversion efficiencies in colloidal quantum dot (QD) solar cells has been achieved recently with lead sulphide (PbS) QDs by adapting a heterojunction architecture, which consists of small-area devices associated with a vacuum-deposited buffer layer with metal electrodes. The preparation of QD solar modules by low-cost solution processes is required to further increase the power-to-cost ratio. Herein we demonstrate all-solution-processed flexible PbS QD solar modules with a layer-by-layer architecture comprising polyethylene terephthalate (PET) substrate/indium tin oxide (ITO)/titanium oxide (TiO2)/PbS QD/poly(3-hexylthiophene) (P3HT)/poly(3,4-ethylenedioxythiophene) : poly(styrene sulfonate) (PEDOT : PSS)/Ag, with an active area of up to 30 cm2, exhibiting a power conversion efficiency (PCE) of 1.3% under AM 1.5 conditions (PCE of 2.2% for a 1 cm2 unit cell). Our approach affords trade-offs between power and the active area of the photovoltaic devices, which results in a low-cost power source, and which is scalable to larger areas. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr01508a

Bright infrared quantum-dot light-emitting diodes through inter-dot spacing control.

PubMed

Sun, Liangfeng; Choi, Joshua J; Stachnik, David; Bartnik, Adam C; Hyun, Byung-Ryool; Malliaras, George G; Hanrath, Tobias; Wise, Frank W

2012-05-06

Infrared light-emitting diodes are currently fabricated from direct-gap semiconductors using epitaxy, which makes them expensive and difficult to integrate with other materials. Light-emitting diodes based on colloidal semiconductor quantum dots, on the other hand, can be solution-processed at low cost, and can be directly integrated with silicon. However, so far, exciton dissociation and recombination have not been well controlled in these devices, and this has limited their performance. Here, by tuning the distance between adjacent PbS quantum dots, we fabricate thin-film quantum-dot light-emitting diodes that operate at infrared wavelengths with radiances (6.4 W sr(-1) m(-2)) eight times higher and external quantum efficiencies (2.0%) two times higher than the highest values previously reported. The distance between adjacent dots is tuned over a range of 1.3 nm by varying the lengths of the linker molecules from three to eight CH(2) groups, which allows us to achieve the optimum balance between charge injection and radiative exciton recombination. The electroluminescent powers of the best devices are comparable to those produced by commercial InGaAsP light-emitting diodes. By varying the size of the quantum dots, we can tune the emission wavelengths between 800 and 1,850 nm.

Control of Energy Flow Dynamics between Tetracene Ligands and PbS Quantum Dots by Size Tuning and Ligand Coverage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kroupa, Daniel M.; Arias, Dylan H.; Blackburn, Jeffrey L.

We have prepared a series of samples with the ligand 6,13-bistri(iso-propyl)silylethynyl tetracene 2-carboxylic acid (TIPS-Tc-COOH) attached to PbS quantum dot (QD) samples of three different sizes in order to monitor and control the extent and time scales of energy flow after photoexcitation. Fast energy transfer (~1 ps) to the PbS QD occurs upon direct excitation of the ligand for all samples. The largest size QD maintains the microsecond exciton lifetime characteristic of the as-prepared oleate terminated PbS QDs. However, two smaller QD sizes with lowest exciton energies similar to or larger than the TIPS-Tc-COO- triplet energy undergo energy transfer betweenmore » QD core and ligand triplet on nanosecond to microsecond timescales. For the intermediate size QDs in particular, energy can be recycled many times between ligand and core, but the triplet remains the dominant excited species at long times, living for ~3 us for fully exchanged QDs and up to 30 us for partial ligand exchange, which is revealed as a method for controlling the triplet lifetime. A unique upconverted luminescence spectrum is observed that results from annihilation of triplets after exclusive excitation of the QD core.« less

Control of Energy Flow Dynamics between Tetracene Ligands and PbS Quantum Dots by Size Tuning and Ligand Coverage

DOE PAGES

Kroupa, Daniel M.; Arias, Dylan H.; Blackburn, Jeffrey L.; ...

2018-01-24

We have prepared a series of samples with the ligand 6,13-bistri(iso-propyl)silylethynyl tetracene 2-carboxylic acid (TIPS-Tc-COOH) attached to PbS quantum dot (QD) samples of three different sizes in order to monitor and control the extent and time scales of energy flow after photoexcitation. Fast energy transfer (~1 ps) to the PbS QD occurs upon direct excitation of the ligand for all samples. The largest size QD maintains the microsecond exciton lifetime characteristic of the as-prepared oleate terminated PbS QDs. However, two smaller QD sizes with lowest exciton energies similar to or larger than the TIPS-Tc-COO- triplet energy undergo energy transfer betweenmore » QD core and ligand triplet on nanosecond to microsecond timescales. For the intermediate size QDs in particular, energy can be recycled many times between ligand and core, but the triplet remains the dominant excited species at long times, living for ~3 us for fully exchanged QDs and up to 30 us for partial ligand exchange, which is revealed as a method for controlling the triplet lifetime. A unique upconverted luminescence spectrum is observed that results from annihilation of triplets after exclusive excitation of the QD core.« less

Detecting trap states in planar PbS colloidal quantum dot solar cells

PubMed Central

Jin, Zhiwen; Wang, Aiji; Zhou, Qing; Wang, Yinshu; Wang, Jizheng

2016-01-01

The recently developed planar architecture (ITO/ZnO/PbS-TBAI/PbS-EDT/Au) has greatly improved the power conversion efficiency of colloidal quantum dot photovoltaics (QDPVs). However, the performance is still far below the theoretical expectations and trap states in the PbS-TBAI film are believed to be the major origin, characterization and understanding of the traps are highly demanded to develop strategies for continued performance improvement. Here employing impedance spectroscopy we detect trap states in the planar PbS QDPVs. We determined a trap state of about 0.34 eV below the conduction band with a density of around 3.2 × 1016 cm−3 eV−1. Temperature dependent open-circuit voltage analysis, temperature dependent diode property analysis and temperature dependent build-in potential analysis consistently denotes an below-bandgap activation energy of about 1.17–1.20 eV. PMID:27845392

Broadening of Distribution of Trap States in PbS Quantum Dot Field-Effect Transistors with High-k Dielectrics

PubMed Central

2017-01-01

We perform a quantitative analysis of the trap density of states (trap DOS) in PbS quantum dot field-effect transistors (QD-FETs), which utilize several polymer gate insulators with a wide range of dielectric constants. With increasing gate dielectric constant, we observe increasing trap DOS close to the lowest unoccupied molecular orbital (LUMO) of the QDs. In addition, this increase is also consistently followed by broadening of the trap DOS. We rationalize that the increase and broadening of the spectral trap distribution originate from dipolar disorder as well as polaronic interactions, which are appearing at strong dielectric polarization. Interestingly, the increased polaron-induced traps do not show any negative effect on the charge carrier mobility in our QD devices at the highest applied gate voltage, giving the possibility to fabricate efficient low-voltage QD devices without suppressing carrier transport. PMID:28084725

Enhanced Performance of PbS-quantum-dot-sensitized Solar Cells via Optimizing Precursor Solution and Electrolytes

NASA Astrophysics Data System (ADS)

Tian, Jianjun; Shen, Ting; Liu, Xiaoguang; Fei, Chengbin; Lv, Lili; Cao, Guozhong

2016-03-01

This work reports a PbS-quantum-dot-sensitized solar cell (QDSC) with power conversion efficiency (PCE) of 4%. PbS quantum dots (QDs) were grown on mesoporous TiO2 film using a successive ion layer absorption and reaction (SILAR) method. The growth of QDs was found to be profoundly affected by the concentration of the precursor solution. At low concentrations, the rate-limiting factor of the crystal growth was the adsorption of the precursor ions, and the surface growth of the crystal became the limiting factor in the high concentration solution. The optimal concentration of precursor solution with respect to the quantity and size of synthesized QDs was 0.06 M. To further increase the performance of QDSCs, the 30% deionized water of polysulfide electrolyte was replaced with methanol to improve the wettability and permeability of electrolytes in the TiO2 film, which accelerated the redox couple diffusion in the electrolyte solution and improved charge transfer at the interfaces between photoanodes and electrolytes. The stability of PbS QDs in the electrolyte was also improved by methanol to reduce the charge recombination and prolong the electron lifetime. As a result, the PCE of QDSC was increased to 4.01%.

Enhanced Performance of PbS-quantum-dot-sensitized Solar Cells via Optimizing Precursor Solution and Electrolytes.

PubMed

Tian, Jianjun; Shen, Ting; Liu, Xiaoguang; Fei, Chengbin; Lv, Lili; Cao, Guozhong

2016-03-15

This work reports a PbS-quantum-dot-sensitized solar cell (QDSC) with power conversion efficiency (PCE) of 4%. PbS quantum dots (QDs) were grown on mesoporous TiO2 film using a successive ion layer absorption and reaction (SILAR) method. The growth of QDs was found to be profoundly affected by the concentration of the precursor solution. At low concentrations, the rate-limiting factor of the crystal growth was the adsorption of the precursor ions, and the surface growth of the crystal became the limiting factor in the high concentration solution. The optimal concentration of precursor solution with respect to the quantity and size of synthesized QDs was 0.06 M. To further increase the performance of QDSCs, the 30% deionized water of polysulfide electrolyte was replaced with methanol to improve the wettability and permeability of electrolytes in the TiO2 film, which accelerated the redox couple diffusion in the electrolyte solution and improved charge transfer at the interfaces between photoanodes and electrolytes. The stability of PbS QDs in the electrolyte was also improved by methanol to reduce the charge recombination and prolong the electron lifetime. As a result, the PCE of QDSC was increased to 4.01%.

Supersonically Spray-Coated Colloidal Quantum Dot Ink Solar Cells

DOE Office of Scientific and Technical Information (OSTI.GOV)

Choi, Hyekyoung; Lee, Jong-Gun; Mai, Xuan Dung

Controlling the thickness of quantum dot (QD) films is difficult using existing film formation techniques, which employ pre-ligand-exchanged PbS QD inks, because of several issues: 1) poor colloidal stability, 2) use of high-boiling-point solvents for QD dispersion, and 3) limitations associated with one-step deposition. Here in this paper, we suggest a new protocol for QD film deposition using electrical double-layered PbS QD inks, prepared by solution-phase ligand exchange using methyl ammonium lead iodide (MAPbI 3). The films are deposited by the supersonic spraying technique, which facilitates the rapid evaporation of the solvent and the subsequent deposition of the PbS QDmore » ink without requiring a post-deposition annealing treatment for solvent removal. The film thickness could be readily controlled by varying the number of spraying sweeps made across the substrate. This spray deposition process yields high-quality n-type QD films quickly (within 1 min) while minimizing the amount of the PbS QD ink used to less than 5 mg for one device (300-nm-thick absorbing layer, 2.5 x 2.5 cm 2). Further, the formation of an additional p-layer by treatment with mercaptopropionic acid allows for facile hole extraction from the QD films, resulting in a power conversion efficiency of 3.7% under 1.5 AM illumination.« less

Supersonically Spray-Coated Colloidal Quantum Dot Ink Solar Cells

DOE PAGES

Choi, Hyekyoung; Lee, Jong-Gun; Mai, Xuan Dung; ...

2017-04-04

Controlling the thickness of quantum dot (QD) films is difficult using existing film formation techniques, which employ pre-ligand-exchanged PbS QD inks, because of several issues: 1) poor colloidal stability, 2) use of high-boiling-point solvents for QD dispersion, and 3) limitations associated with one-step deposition. Here in this paper, we suggest a new protocol for QD film deposition using electrical double-layered PbS QD inks, prepared by solution-phase ligand exchange using methyl ammonium lead iodide (MAPbI 3). The films are deposited by the supersonic spraying technique, which facilitates the rapid evaporation of the solvent and the subsequent deposition of the PbS QDmore » ink without requiring a post-deposition annealing treatment for solvent removal. The film thickness could be readily controlled by varying the number of spraying sweeps made across the substrate. This spray deposition process yields high-quality n-type QD films quickly (within 1 min) while minimizing the amount of the PbS QD ink used to less than 5 mg for one device (300-nm-thick absorbing layer, 2.5 x 2.5 cm 2). Further, the formation of an additional p-layer by treatment with mercaptopropionic acid allows for facile hole extraction from the QD films, resulting in a power conversion efficiency of 3.7% under 1.5 AM illumination.« less

Enhancement of the photovoltaic performance in P3HT: PbS hybrid solar cells using small size PbS quantum dots

NASA Astrophysics Data System (ADS)

Firdaus, Yuliar; Vandenplas, Erwin; Justo, Yolanda; Gehlhaar, Robert; Cheyns, David; Hens, Zeger; Van der Auweraer, Mark

2014-09-01

Different approaches of surface modification of the quantum dots (QDs), namely, solution-phase (octylamine, octanethiol) and post-deposition (acetic acid, 1,4-benzenedithiol) ligand exchange were used in the fabrication of hybrid bulk heterojunction solar cell containing poly (3-hexylthiophene) (P3HT) and small (2.4 nm) PbS QDs. We show that replacing oleic acid by shorter chain ligands improves the figures of merit of the solar cells. This can possibly be attributed to a combination of a reduced thickness of the barrier for electron transfer and an optimized phase separation. The best results were obtained for post-deposition ligand exchange by 1,4-benzenedithiol, which improves the power conversion efficiency of solar cells based on a bulk heterojunction of lead sulfide (PbS) QDs and P3HT up to two orders of magnitude over previously reported hybrid cells based on a bulk heterojunction of P3HT:PbS QDs, where the QDs are capped by acetic acid ligands. The optimal performance was obtained for solar cells with 69 wt. % PbS QDs. Besides the ligand effects, the improvement was attributed to the formation of an energetically favorable bulk heterojunction with P3HT, when small size (2.4 nm) PbS QDs were used. Dark current density-voltage (J-V) measurements carried out on the device provided insight into the working mechanism: the comparison between the dark J-V characteristics of the bench mark system P3HT:PCBM and the P3HT:PbS blends allows us to conclude that a larger leakage current and a more efficient recombination are the major factors responsible for the larger losses in the hybrid system.

A filterless, visible-blind, narrow-band, and near-infrared photodetector with a gain

NASA Astrophysics Data System (ADS)

Shen, Liang; Zhang, Yang; Bai, Yang; Zheng, Xiaopeng; Wang, Qi; Huang, Jinsong

2016-06-01

In many applications of near-infrared (NIR) light detection, a band-pass filter is needed to exclude the noise caused by visible light. Here, we demonstrate a filterless, visible-blind, narrow-band NIR photodetector with a full-width at half-maximum of <50 nm for the response spectrum. These devices have a thick (>4 μm) nanocomposite absorbing layers made of polymer-fullerene:lead sulfide (PbS) quantum dots (QDs). The PbS QDs yield a photoconductive gain due to their hole-trapping effect, which effectively enhances both the responsivity and the visible rejection ratio of the external quantum efficiency by >10 fold compared to those without PbS QDs. Encouragingly, the inclusion of the PbS QDs does not increase the device noise. We directly measured a noise equivalent power (NEP) of 6.1 pW cm-2 at 890 nm, and a large linear dynamic range (LDR) over 11 orders of magnitude. The highly sensitive visible-blind NIR narrow-band photodetectors may find applications in biomedical engineering.

Photo-induced surface modification to improve the performance of lead sulfide quantum dot solar cell.

PubMed

Tulsani, Srikanth Reddy; Rath, Arup Kumar

2018-07-15

The solution-processed quantum dot (QD) solar cell technology has seen significant advancements in recent past to emerge as a potential contender for the next generation photovoltaic technology. In the development of high performance QD solar cell, the surface ligand chemistry has played the important role in controlling the doping type and doping density of QD solids. For instance, lead sulfide (PbS) QDs which is at the forefront of QD solar cell technology, can be made n-type or p-type respectively by using iodine or thiol as the surfactant. The advancements in surface ligand chemistry enable the formation of p-n homojunction of PbS QDs layers to attain high solar cell performances. It is shown here, however, that poor Fermi level alignment of thiol passivated p-type PbS QD hole transport layer with the n-type PbS QD light absorbing layer has rendered the photovoltaic devices from realizing their full potential. Here we develop a control surface oxidation technique using facile ultraviolet ozone treatment to increase the p-doping density in a controlled fashion for the thiol passivated PbS QD layer. This subtle surface modification tunes the Fermi energy level of the hole transport layer to deeper values to facilitate the carrier extraction and voltage generation in photovoltaic devices. In photovoltaic devices, the ultraviolet ozone treatment resulted in the average gain of 18% in the power conversion efficiency with the highest recorded efficiency of 8.98%. Copyright © 2018 Elsevier Inc. All rights reserved.

Open-Circuit Voltage Deficit, Radiative Sub-Bandgap States, and Prospects in Quantum Dot Solar Cells

PubMed Central

Chuang, Chia-Hao Marcus; Maurano, Andrea; Brandt, Riley E.; Hwang, Gyu Weon; Jean, Joel; Buonassisi, Tonio; Bulović, Vladimir; Bawendi, Moungi G.

2016-01-01

Quantum dot photovoltaics (QDPV) offer the potential for low-cost solar cells. To develop strategies for continued improvement in QDPVs, a better understanding of the factors that limit their performance is essential. Here, we study carrier recombination processes that limit the power conversion efficiency of PbS QDPVs. We demonstrate the presence of radiative sub-bandgap states and sub-bandgap state filling in operating devices by using photoluminescence (PL) and electroluminescence (EL) spectroscopy. These sub-bandgap states are most likely the origin of the high open-circuit-voltage (VOC) deficit and relatively limited carrier collection that have thus far been observed in QDPVs. Combining these results with our perspectives on recent progress in QDPV, we conclude that eliminating sub-bandgap states in PbS QD films has the potential to show a greater gain than may be attainable by optimization of interfaces between QDs and other materials. We suggest possible future directions that could guide the design of high-performance QDPVs. PMID:25927871

Combination of Cation Exchange and Quantized Ostwald Ripening for Controlling Size Distribution of Lead Chalcogenide Quantum Dots

DOE PAGES

Zhang, Changwang; Xia, Yong; Zhang, Zhiming; ...

2017-03-22

A new strategy for narrowing the size distribution of colloidal quantum dots (QDs) was developed by combining cation exchange and quantized Ostwald ripening. Medium-sized reactant CdS(e) QDs were subjected to cation exchange to form the target PbS(e) QDs, and then small reactant CdS(e) QDs were added which were converted to small PbS(e) dots via cation exchange. The small-sized ensemble of PbS(e) QDs dissolved completely rapidly and released a large amount of monomers, promoting the growth and size-focusing of the medium-sized ensemble of PbS(e) QDs. The addition of small reactant QDs can be repeated to continuously reduce the size distribution. Themore » new method was applied to synthesize PbSe and PbS QDs with extremely narrow size distributions and as a bonus they have hybrid surface passivation. In conclusion, the size distribution of prepared PbSe and PbS QDs are as low as 3.6% and 4.3%, respectively, leading to hexagonal close packing in monolayer and highly ordered three-dimensional superlattice.« less

Combination of Cation Exchange and Quantized Ostwald Ripening for Controlling Size Distribution of Lead Chalcogenide Quantum Dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Changwang; Xia, Yong; Zhang, Zhiming

A new strategy for narrowing the size distribution of colloidal quantum dots (QDs) was developed by combining cation exchange and quantized Ostwald ripening. Medium-sized reactant CdS(e) QDs were subjected to cation exchange to form the target PbS(e) QDs, and then small reactant CdS(e) QDs were added which were converted to small PbS(e) dots via cation exchange. The small-sized ensemble of PbS(e) QDs dissolved completely rapidly and released a large amount of monomers, promoting the growth and size-focusing of the medium-sized ensemble of PbS(e) QDs. The addition of small reactant QDs can be repeated to continuously reduce the size distribution. Themore » new method was applied to synthesize PbSe and PbS QDs with extremely narrow size distributions and as a bonus they have hybrid surface passivation. In conclusion, the size distribution of prepared PbSe and PbS QDs are as low as 3.6% and 4.3%, respectively, leading to hexagonal close packing in monolayer and highly ordered three-dimensional superlattice.« less

Ligand-dependent exciton dynamics and photovoltaic properties of PbS quantum dot heterojunction solar cells.

PubMed

Chang, Jin; Ogomi, Yuhei; Ding, Chao; Zhang, Yao Hong; Toyoda, Taro; Hayase, Shuzi; Katayama, Kenji; Shen, Qing

2017-03-01

The surface chemistry of colloidal quantum dots (QDs) plays an important role in determining the photoelectric properties of QD films and the corresponding quantum dot heterojunction solar cells (QDHSCs). To investigate the effects of the ligand structure on the photovoltaic performance and exciton dynamics of QDHSCs, PbS QDHSCs were fabricated by the solid state ligand exchange method with mercaptoalkanoic acid as the cross-linking ligand. Temperature-dependent photoluminescence and ultrafast transient absorption spectra show that the electronic coupling and charge transfer rate within QD ensembles were monotonically enhanced as the ligand length decreased. However, in practical QDHSCs, the second shortest ligand 3-mercaptopropionic acid (MPA) showed higher power conversion efficiency than the shortest ligand thioglycolic acid (TGA). This could be attributed to the difference in their surface trap states, supported by thermally stimulated current measurements. Moreover, compared with the non-conjugated ligand MPA, the conjugated ligand 4-mercaptobenzoic acid (MBA) introduces less trap states and has a similar charge transfer rate in QD ensembles, but has poor photovoltaic properties. This unexpected result could be contributed by the QD-ligand orbital mixing, leading to the charge transfer from QDs to ligands instead of charge transfer between adjacent QDs. This work highlights the significant effects of ligand structures on the photovoltaic properties and exciton dynamics of QDHSCs, which would shed light on the further development of QD-based photoelectric devices.

Giant photocurrent enhancement by transition metal doping in quantum dot sensitized solar cells

NASA Astrophysics Data System (ADS)

Rimal, Gaurab; Pimachev, Artem K.; Yost, Andrew J.; Poudyal, Uma; Maloney, Scott; Wang, Wenyong; Chien, TeYu; Dahnovsky, Yuri; Tang, Jinke

2016-09-01

A huge enhancement in the incident photon-to-current efficiency of PbS quantum dot (QD) sensitized solar cells by manganese doping is observed. In the presence of Mn dopants with relatively small concentration (4 at. %), the photoelectric current increases by an average of 300% (up to 700%). This effect cannot be explained by the light absorption mechanism because both the experimental and theoretical absorption spectra demonstrate several times decreases in the absorption coefficient. To explain such dramatic increase in the photocurrent we propose the electron tunneling mechanism from the LUMO of the QD excited state to the Zn2SnO4 (ZTO) semiconductor photoanode. This change is due to the presence of the Mn instead of Pb atom at the QD/ZTO interface. The ab initio calculations confirm this mechanism. This work proposes an alternative route for a significant improvement of the efficiency for quantum dot sensitized solar cells.

Enhanced performance of PbS-sensitized solar cells via controlled successive ionic-layer adsorption and reaction.

PubMed

Abbas, Muhammad A; Basit, Muhammad A; Park, Tae Joo; Bang, Jin Ho

2015-04-21

Despite the potential of PbS quantum dots (QDs) as sensitizers for quantum-dot-sensitized solar cells (QDSSCs), achieving a high photocurrent density over 30 mA cm(-2) remains a challenging task in PbS-sensitized solar cells. In contrast to previous attempts, where Hg(2+)-doping or multi-step post-treatment is necessary, we are capable of achieving a high photocurrent exceeding 30 mA cm(-2) simply by manipulating the successive ionic layer adsorption and reaction (SILAR) method. We show that controlling temperature at which SILAR is performed is critical to obtain a higher and more uniform coverage of PbS QDs over a mesoporous TiO2 film. The deposition of a CdS inter-layer between TiO2 and PbS is found to be an effective means of ensuring high photocurrent and stability. Not only does this modification improve the light absorption capability of the photoanode, but it also has a significant effect on charge recombination and electron injection efficiency at the PbS/TiO2 interface according to our in-depth study using electrochemical impedance spectroscopy (EIS). The implication of subtle changes in the interfacial events via modified SILAR conditions for PbS-sensitized solar cells is discussed.

Tandem Solar Cells from Solution-Processed CdTe and PbS Quantum Dots Using a ZnTe–ZnO Tunnel Junction

DOE PAGES

Crisp, Ryan W.; Pach, Gregory F.; Kurley, J. Matthew; ...

2017-01-10

Here, we developed a monolithic CdTe-PbS tandem solar cell architecture in which both the CdTe and PbS absorber layers are solution-processed from nanocrystal inks. Due to their tunable nature, PbS quantum dots (QDs), with a controllable band gap between 0.4 and ~1.6 eV, are a promising candidate for a bottom absorber layer in tandem photovoltaics. In the detailed balance limit, the ideal configuration of a CdTe (E g = 1.5 eV)-PbS tandem structure assumes infinite thickness of the absorber layers and requires the PbS band gap to be 0.75 eV to theoretically achieve a power conversion efficiency (PCE) of 45%.more » But, modeling shows that by allowing the thickness of the CdTe layer to vary, a tandem with efficiency over 40% is achievable using bottom cell band gaps ranging from 0.68 and 1.16 eV. In a first step toward developing this technology, we explore CdTe-PbS tandem devices by developing a ZnTe-ZnO tunnel junction, which appropriately combines the two subcells in series. Furthermore, we examine the basic characteristics of the solar cells as a function of layer thickness and bottom-cell band gap and demonstrate open-circuit voltages in excess of 1.1 V with matched short circuit current density of 10 mA/cm 2 in prototype devices.« less

Tandem Solar Cells from Solution-Processed CdTe and PbS Quantum Dots Using a ZnTe-ZnO Tunnel Junction.

PubMed

Crisp, Ryan W; Pach, Gregory F; Kurley, J Matthew; France, Ryan M; Reese, Matthew O; Nanayakkara, Sanjini U; MacLeod, Bradley A; Talapin, Dmitri V; Beard, Matthew C; Luther, Joseph M

2017-02-08

We developed a monolithic CdTe-PbS tandem solar cell architecture in which both the CdTe and PbS absorber layers are solution-processed from nanocrystal inks. Due to their tunable nature, PbS quantum dots (QDs), with a controllable band gap between 0.4 and ∼1.6 eV, are a promising candidate for a bottom absorber layer in tandem photovoltaics. In the detailed balance limit, the ideal configuration of a CdTe (E g = 1.5 eV)-PbS tandem structure assumes infinite thickness of the absorber layers and requires the PbS band gap to be 0.75 eV to theoretically achieve a power conversion efficiency (PCE) of 45%. However, modeling shows that by allowing the thickness of the CdTe layer to vary, a tandem with efficiency over 40% is achievable using bottom cell band gaps ranging from 0.68 and 1.16 eV. In a first step toward developing this technology, we explore CdTe-PbS tandem devices by developing a ZnTe-ZnO tunnel junction, which appropriately combines the two subcells in series. We examine the basic characteristics of the solar cells as a function of layer thickness and bottom-cell band gap and demonstrate open-circuit voltages in excess of 1.1 V with matched short circuit current density of 10 mA/cm 2 in prototype devices.

In Situ Passivation for Efficient PbS Quantum Dot Solar Cells by Precursor Engineering.

PubMed

Wang, Yongjie; Lu, Kunyuan; Han, Lu; Liu, Zeke; Shi, Guozheng; Fang, Honghua; Chen, Si; Wu, Tian; Yang, Fan; Gu, Mengfan; Zhou, Sijie; Ling, Xufeng; Tang, Xun; Zheng, Jiawei; Loi, Maria Antonietta; Ma, Wanli

2018-04-01

Current efforts on lead sulfide quantum dot (PbS QD) solar cells are mostly paid to the device architecture engineering and postsynthetic surface modification, while very rare work regarding the optimization of PbS synthesis is reported. Here, PbS QDs are successfully synthesized using PbO and PbAc 2  · 3H 2 O as the lead sources. QD solar cells based on PbAc-PbS have demonstrated a high power conversion efficiency (PCE) of 10.82% (and independently certificated values of 10.62%), which is significantly higher than the PCE of 9.39% for PbO-PbS QD based ones. For the first time, systematic investigations are carried out on the effect of lead precursor engineering on the device performance. It is revealed that acetate can act as an efficient capping ligands together with oleic acid, providing better surface coverage and replace some of the harmful hydroxyl (OH) ligands during the synthesis. Then the acetate on the surface can be exchanged by iodide and lead to desired passivation. This work demonstrates that the precursor engineering has great potential in performance improvement. It is also pointed out that the initial synthesis is an often neglected but critical stage and has abundant room for optimization to further improve the quality of the resultant QDs, leading to breakthrough efficiency. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The Physics of Ultracold Sr2 Molecules: Optical Production and Precision Measurement

NASA Astrophysics Data System (ADS)

Osborn, Christopher Butler

Colloidal quantum dots have desirable optical properties which can be exploited to realize a variety of photonic devices and functionalities. However, colloidal dots have not had a pervasive utility in photonic devices because of the absence of patterning methods. The electronic chip industry is highly successful due to the well-established lithographic procedures. In this thesis we borrow ideas from the semiconductor industry to develop lithographic techniques that can be used to pattern colloidal quantum dots while ensuring that the optical properties of the quantum dots are not affected by the process. In this thesis we have developed colloidal quantum dot based waveguide structures for amplification and switching applications for all-optical signal processing. We have also developed colloidal quantum dot based light emitting diodes. We successfully introduced CdSe/ZnS quantum dots into a UV curable photo-resist, which was then patterned to realize active devices. In addition, "passive" devices (devices without quantum dots) were integrated to "active" devices via waveguide couplers. Use of photo-resist devices offers two distinct advantages. First, they have low scattering loss and secondly, they allow good fiber to waveguide coupling efficiency due to the low refractive index which allows for large waveguide cross-sections while supporting single mode operation. Practical planar photonic devices and circuits incorporating both active and passive structures can now be realized, now that we have patterning capabilities of quantum dots while maintaining the original optical attributes of the system. In addition to the photo-resist host, we also explored the incorporation of colloidal quantum dots into a dielectric silicon dioxide and silicon nitride one-dimensional microcavity structures using low temperature plasma enhanced chemical vapor deposition. This material system can be used to realize microcavity light emitting diodes that can be realized on any substrate. As a proof of concept demonstration we show a 1550 nm emitting all-dielectric vertical cavity structure embedded with PbS quantum dots. Enhancement in spontaneous emission from the dots embedded in the microcavity is also demonstrated.

Quantum dot impregnated-chitosan film for heavy metal ion sensing and removal.

PubMed

Jaiswal, Amit; Ghsoh, Siddhartha Sankar; Chattopadhyay, Arun

2012-11-06

We report the use of biopolymer-stabilized ZnS quantum dots (Q-dots) for cation exchange reaction-based easy sensing and removal of heavy metal ions such as Hg(2+), Ag(+), and Pb(2+) in water. Chitosan-stabilized ZnS Q-dots were synthesized in aqueous medium and were observed to have been converted to HgS, Ag(2)S, and PbS Q-dots in the presence of corresponding ions. The transformed Q-dots showed characteristic color development, with Hg(2+) being exceptionally identifiable due to the visible bright yellow color formation, while brown coloration was observed in other metal ions. The cation exchange was driven by the difference in the solubility product of the reactant and the product Q-dots. The cation exchanged Q-dots preserved the morphology of the reactant Q-dots and displayed volume increase based on the bulk crystal lattice parameters. The band gap of the transformed Q-dots showed a major increase from the corresponding bulk band gap of the material, demonstrating the role of quantum confinement. Next, we fabricated ZnS Q-dot impregnated chitosan film which was used to remove heavy metal ions from contaminated water as measured using atomic absorption spectroscopy (AAS). The present system could suitably be used as a simple dipstick for elimination of heavy metal ion contamination in water.

Recombination Suppression in PbS Quantum Dot Heterojunction Solar Cells by Energy-Level Alignment in the Quantum Dot Active Layers.

PubMed

Ding, Chao; Zhang, Yaohong; Liu, Feng; Nakazawa, Naoki; Huang, Qingxun; Hayase, Shuzi; Ogomi, Yuhei; Toyoda, Taro; Wang, Ruixiang; Shen, Qing

2017-09-22

Using spatial energy-level gradient engineering with quantum dots (QDs) of different sizes to increase the generated carrier collection at the junction of a QD heterojunction solar cell (QDHSC) is a hopeful route for improving the energy-conversion efficiency. However, the results of current related research have shown that a variable band-gap structure in a QDHSC will create an appreciable increase, not in the illumination current density, but rather in the fill factor. In addition, there are a lack of studies on the mechanism of the effect of these graded structures on the photovoltaic performance of QDHSCs. This study presents the development of air atmosphere solution-processed TiO 2 /PbS QDs/Au QDHSCs by engineering the energy-level alignment (ELA) of the active layer via the use of a sorted order of differently sized QD layers (four QD sizes). In comparison to the ungraded device (without the ELA), the optimized graded architecture (containing the ELA) solar cells exhibited a great increase (21.4%) in short-circuit current density (J sc ). As a result, a J sc value greater than 30 mA/cm 2 has been realized in planar, thinner absorption layer (∼300 nm) PbS QDHSCs, and the open-circuit voltage (V oc ) and power-conversion efficiency (PCE) were also improved. Through characterization by the light intensity dependences of the J sc and V oc and transient photovoltage decay, we find that (i) the ELA structure, serving as an electron-blocking layer, reduces the interfacial recombination at the PbS/anode interface, and (ii) the ELA structure can drive more carriers toward the desirable collection electrode, and the additional carriers can fill the trap states, reducing the trap-assisted recombination in the PbS QDHSCs. This work has clearly elucidated the mechanism of the recombination suppression in the graded QDHSCs and demonstrated the effects of ELA structure on the improvement of J sc . The charge recombination mechanisms characterized in this work would be able to shed light on further improvements of QDHSCs, which could even benefit other types of solar cells.

Using p-type PbS Quantum Dots to Quench Photocurrent of Fullerene-Au NP@MoS2 Composite Structure for Ultrasensitive Photoelectrochemical Detection of ATP.

PubMed

Li, Meng-Jie; Zheng, Ying-Ning; Liang, Wen-Bin; Yuan, Ruo; Chai, Ya-Qin

2017-12-06

Ultrasensitive and rapid quantification of the universal energy currency adenosine triphosphate (ATP) is an extremely critical mission in clinical applications. In this work, a "signal-off" photoelectrochemical (PEC) biosensor was designed for ultrasensitive ATP detection based on a fullerene (C 60 )-decorated Au nanoparticle@MoS 2 (C 60 -Au NP@MoS 2 ) composite material as a signal indicator and a p-type PbS quantum dot (QD) as an efficient signal quencher. Modification of wide band gap C 60 with narrow band gap MoS 2 to form an ideal PEC signal indicator was proposed, which could significantly improve photocurrent conversion efficiency, leading to a desirable PEC signal. In the presence of p-type PbS QDs, the PEC signal of n-type C 60 -Au NP@MoS 2 was effectively quenched because p-type PbS QDs could compete with C 60 -Au NP@MoS 2 to consume light energy and electron donor. Besides, the conversion of a limited amount of target ATP into an amplified output PbS QD-labeled short DNA sequence (output S 1 ) was achieved via target-mediated aptazyme cycling amplification strategy, facilitating ultrasensitive ATP detection. The proposed signal-off PEC strategy exhibited a wide linear range from 1.00 × 10 -2 pM to 100 nM with a low detection limit of 3.30 fM. Importantly, this proposed strategy provides a promising platform to detect ATP at ultralow levels and has potential applications, including diagnosis of ATP-related diseases, monitoring of diseases progression and evaluation of prognosis.

Structure, transport and photoconductance of PbS quantum dot monolayers functionalized with a copper phthalocyanine derivative.

PubMed

André, A; Theurer, C; Lauth, J; Maiti, S; Hodas, M; Samadi Khoshkhoo, M; Kinge, S; Meixner, A J; Schreiber, F; Siebbeles, L D A; Braun, K; Scheele, M

2017-01-31

We simultaneously surface-functionalize PbS nanocrystals with Cu 4,4',4'',4'''-tetraaminophthalocyanine and assemble this hybrid material into macroscopic monolayers. Electron microscopy and X-ray scattering reveal a granular mesocrystalline structure with strong coherence between the atomic lattice and the superlattice of nanocrystals within each domain. Terahertz spectroscopy and field-effect transistor measurements indicate efficient coupling of holes throughout the hybrid thin film, in conjunction with a pronounced photoresponse. We demonstrate the potential of this material for optoelectronic applications by fabricating a light-effect transistor.

Improving the Performance of PbS Quantum Dot Solar Cells by Optimizing ZnO Window Layer

NASA Astrophysics Data System (ADS)

Yang, Xiaokun; Hu, Long; Deng, Hui; Qiao, Keke; Hu, Chao; Liu, Zhiyong; Yuan, Shengjie; Khan, Jahangeer; Li, Dengbing; Tang, Jiang; Song, Haisheng; Cheng, Chun

2017-04-01

Comparing with hot researches in absorber layer, window layer has attracted less attention in PbS quantum dot solar cells (QD SCs). Actually, the window layer plays a key role in exciton separation, charge drifting, and so on. Herein, ZnO window layer was systematically investigated for its roles in QD SCs performance. The physical mechanism of improved performance was also explored. It was found that the optimized ZnO films with appropriate thickness and doping concentration can balance the optical and electrical properties, and its energy band align well with the absorber layer for efficient charge extraction. Further characterizations demonstrated that the window layer optimization can help to reduce the surface defects, improve the heterojunction quality, as well as extend the depletion width. Compared with the control devices, the optimized devices have obtained an efficiency of 6.7% with an enhanced V oc of 18%, J sc of 21%, FF of 10%, and power conversion efficiency of 58%. The present work suggests a useful strategy to improve the device performance by optimizing the window layer besides the absorber layer.

Visualization of Current and Mapping of Elements in Quantum Dot Solar Cells

DOE PAGES

Niezgoda, J. Scott; Ng, Amy; Poplawsky, Jonathan D.; ...

2015-12-17

The delicate influence of properties such as high surface state density and organic-inorganic boundaries on the individual quantum dot electronic structure complicates pursuits toward forming quantitative models of quantum dot thin films ab initio. Our report describes the application of electron beam-induced current (EBIC) microscopy to depleted-heterojunction colloidal quantum dot photovoltaics (DH-CQD PVs), a technique which affords one a map of current production within the active layer of a PV device. The effects of QD sample size polydispersity as well as layer thickness in CQD active layers as they pertain to current production within these PVs are imaged and explained.more » The results from these experiments compare well with previous estimations, and confirm the ability of EBIC to function as a valuable empirical tool for the design and betterment of DH-CQD PVs. Lastly, extensive and unexpected PbS QD penetration into the mesoporous TiO 2 layer is observed through imaging of device cross sections by energy-dispersive X-ray spectroscopy combined with scanning transmission electron microscopy. Finally, the effects of this finding are discussed and corroborated with the EBIC studies on similar devices.« less

High reduction of interfacial charge recombination in colloidal quantum dot solar cells by metal oxide surface passivation.

PubMed

Chang, Jin; Kuga, Yuki; Mora-Seró, Iván; Toyoda, Taro; Ogomi, Yuhei; Hayase, Shuzi; Bisquert, Juan; Shen, Qing

2015-03-12

Bulk heterojunction (BHJ) solar cells based on colloidal QDs and metal oxide nanowires (NWs) possess unique and outstanding advantages in enhancing light harvesting and charge collection in comparison to planar architectures. However, the high surface area of the NW structure often brings about a large amount of recombination (especially interfacial recombination) and limits the open-circuit voltage in BHJ solar cells. This problem is solved here by passivating the surface of the metal oxide component in PbS colloidal quantum dot solar cells (CQDSCs). By coating thin TiO2 layers onto ZnO-NW surfaces, the open-circuit voltage and power conversion efficiency have been improved by over 40% in PbS CQDSCs. Characterization by transient photovoltage decay and impedance spectroscopy indicated that the interfacial recombination was significantly reduced by the surface passivation strategy. An efficiency as high as 6.13% was achieved through the passivation approach and optimization for the length of the ZnO-NW arrays (device active area: 16 mm2). All solar cells were tested in air, and exhibited excellent air storage stability (without any performance decline over more than 130 days). This work highlights the significance of metal oxide passivation in achieving high performance BHJ solar cells. The charge recombination mechanism uncovered in this work could shed light on the further improvement of PbS CQDSCs and/or other types of solar cells.

Stoichiometry control in quantum dots: a viable analog to impurity doping of bulk materials.

PubMed

Luther, Joseph M; Pietryga, Jeffrey M

2013-03-26

A growing body of research indicates that the stoichiometry of compound semiconductor quantum dots (QDs) may offer control over the materials' optoelectronic properties in ways that could be invaluable in electronic devices. Quantum dots have been characterized as having a stoichiometric bulk-like core with a highly reconstructed surface of a more flexible composition, consisting essentially of ligated, weakly bound ions. As such, many efforts toward stoichiometry-based control over material properties have focused on ligand manipulation. In this issue of ACS Nano, Murray and Kagan's groups instead demonstrate control of the conductive properties of QD arrays by altering the stoichiometry via atomic infusion using a thermal evaporation technique. In this work, PbSe and PbS QD films are made to show controlled n- or p-type behavior, which is key to developing optimized QD-based electronics. In this Perspective, we discuss recent developments and the future outlook in using stoichiometry as a tool to further manipulate QD material properties in this context.

Understanding chemically processed solar cells based on quantum dots

NASA Astrophysics Data System (ADS)

Malgras, Victor; Nattestad, Andrew; Kim, Jung Ho; Dou, Shi Xue; Yamauchi, Yusuke

2017-12-01

Photovoltaic energy conversion is one of the best alternatives to fossil fuel combustion. Petroleum resources are now close to depletion and their combustion is known to be responsible for the release of a considerable amount of greenhouse gases and carcinogenic airborne particles. Novel third-generation solar cells include a vast range of device designs and materials aiming to overcome the factors limiting the current technologies. Among them, quantum dot-based devices showed promising potential both as sensitizers and as colloidal nanoparticle films. A good example is the p-type PbS colloidal quantum dots (CQDs) forming a heterojunction with a n-type wide-band-gap semiconductor such as TiO2 or ZnO. The confinement in these nanostructures is also expected to result in marginal mechanisms, such as the collection of hot carriers and generation of multiple excitons, which would increase the theoretical conversion efficiency limit. Ultimately, this technology could also lead to the assembly of a tandem-type cell with CQD films absorbing in different regions of the solar spectrum.

Ambipolar Graphene-Quantum Dot Hybrid Vertical Photodetector with a Graphene Electrode.

PubMed

Che, Yongli; Zhang, Yating; Cao, Xiaolong; Zhang, Haiting; Song, Xiaoxian; Cao, Mingxuan; Yu, Yu; Dai, Haitao; Yang, Junbo; Zhang, Guizhong; Yao, Jianquan

2017-09-20

A strategy to fabricate an ambipolar near-infrared vertical photodetector (VPD) by sandwiching a photoactive material as a channel film between the bottom graphene and top metal electrodes was developed. The channel length in the vertical architecture was determined by the channel layer thickness, which can provide an ultrashort channel length without the need for a high-precision manufacturing process. The performance of VPDs with two types of semiconductor layers, a graphene-PbS quantum dot hybrid (GQDH) and PbS quantum dots (QDs), was measured. The GQDH VPD showed better photoelectric properties than the QD VPD because of the high mobility of graphene doped in the channel. The GQDH VPD exhibited excellent photoresponse properties with a responsivity of 1.6 × 10 4 A/W in the p-type regime and a fast response speed with a rise time of 8 ms. The simple manufacture and the promising photoresponse of the GQDH VPDs reveal that an easy and effective way to fabricate high-performance ambipolar photodetectors was developed.

3D superstructures with an orthorhombic lattice assembled by colloidal PbS quantum dots.

PubMed

Ushakova, Elena V; Cherevkov, Sergei A; Litvin, Aleksandr P; Parfenov, Peter S; Kasatkin, Igor A; Fedorov, Anatoly V; Gun'ko, Yurii K; Baranov, Alexander V

2018-05-03

We report a new type of metamaterial comprising a highly ordered 3D network of 3-7 nm lead sulfide quantum dots self-assembled in an organic matrix formed by amphiphilic ligands (oleic acid molecules). The obtained 3D superstructures possess an orthorhombic lattice with the distance between the nanocrystals as large as 10-40 nm. Analysis of self-assembly and destruction of the superstructures in time performed by a SAXS technique shows that their morphology depends on the quantity of amphiphilic ligands and width of the quantum dot size and its distribution. Formation of the superstructures is discussed in terms of a model describing the lyotropic crystal formation by micelles from three-phase mixtures. The results show that the organic molecules possessing surfactant properties and capable of forming micelles with nanoparticles as a micelle core can be utilized as building blocks for the creation of novel metamaterials based on a highly ordered 3D network of semiconductors, metals or magnetic nanoparticles.

Understanding chemically processed solar cells based on quantum dots.

PubMed

Malgras, Victor; Nattestad, Andrew; Kim, Jung Ho; Dou, Shi Xue; Yamauchi, Yusuke

2017-01-01

Photovoltaic energy conversion is one of the best alternatives to fossil fuel combustion. Petroleum resources are now close to depletion and their combustion is known to be responsible for the release of a considerable amount of greenhouse gases and carcinogenic airborne particles. Novel third-generation solar cells include a vast range of device designs and materials aiming to overcome the factors limiting the current technologies. Among them, quantum dot-based devices showed promising potential both as sensitizers and as colloidal nanoparticle films. A good example is the p-type PbS colloidal quantum dots (CQDs) forming a heterojunction with a n-type wide-band-gap semiconductor such as TiO 2 or ZnO. The confinement in these nanostructures is also expected to result in marginal mechanisms, such as the collection of hot carriers and generation of multiple excitons, which would increase the theoretical conversion efficiency limit. Ultimately, this technology could also lead to the assembly of a tandem-type cell with CQD films absorbing in different regions of the solar spectrum.

Chemical Control of Lead Sulfide Quantum Dot Shape, Self-Assembly, and Charge Transport

NASA Astrophysics Data System (ADS)

McPhail, Martin R.

Lead(II) sulfide quantum dots (PbS QDs) are a promising excitonic material for numerous application that require that control of fluxes of charge and energy at nanoscale interfaces, such as solar energy conversion, photo- and electrocatalysis, light emitting diodes, chemical sensing, single-electron logic elements, field effect transistors, and photovoltaics. PbS QDs are particularly suitable for photonics applications because they exhibit size-tunable band-edge absorption and fluorescence across the entire near-infrared spectrum, undergo efficient multi-exciton generation, exhibit a long radiative lifetime, and possess an eight-fold degenerate ground-state. The effective integration of PbS QDs into these applications requires a thorough understanding of how to control their synthesis, self-assembly, and charge transport phenomena. In this document, I describe a series of experiments to elucidate three levels of chemical control on the emergent properties of PbS QDs: (1) the role of surface chemistry in controlling PbS QD shape during solvothermal synthesis, (2) the role of QD shape and ligand functionalization in self-assembly at a liquid-air interface, and (3) the role of QD packing structure on steady-state conductivity and transient current dynamics. At the synthetic level (1), I show that the final shape and surface chemistry of PbS QDs is highly sensitive to the formation of organosulfur byproducts by commonly used sulfur reagents. The insight into PbS QD growth gained from this work is then developed to controllably tune PbS QD shape from cubic to octahedral to hexapodal while maintaining QD size. At the following level of QD self-assembly (2), I show how QD size and shape dictate packing geometry in extended 2D arrays and how this packing can be controllably interrupted in mixed monolayers. I also study the role of ligand structure on the reorganization of QD arrays at a liquid-air interface and find that the specific packing defects in QD arrays vary depending on exchange kinetics and ligand binding geometry. At the final level of emergent macroscopic properties (3), I show that while the size-dependent conductivity of quasi-2D PbS QD arrays can be explained by a simple diffusional hopping model that only accounts for nearest-neighbor interactions, the transient photocurrent dynamics are extremely sensitive to the morphology of the entire percolation network formed by the QDs.

Colloidal PbS nanocrystals integrated to Si-based photonics for applications at telecom wavelengths

NASA Astrophysics Data System (ADS)

Humer, M.; Guider, R.; Jantsch, W.; Fromherz, T.

2013-05-01

In the last decade, Si based photonics has made major advances in terms of design, fabrication, and device implementation. But due to Silicon's indirect bandgap, it still remains a challenge to create efficient Si-based light emitting devices. In order to overcome this problem, an approach is to develop hybrid systems integrating light-emitting materials into Si. A promising class of materials for this purpose is the class of semiconducting nanocrystal quantum dots (NCs) that are synthesized by colloidal chemistry. As their absorption and emission wavelength depends on the dot size, which can easily be controlled during synthesis, they are extremely attractive as building blocks for nanophotonic applications. For applications in telecom wavelength, Lead chalcogenide colloidal NCs are optimum materials due to their unique optical, electronic and nonlinear properties. In this work, we experimentally demonstrate the integration of PbS nanocrystals into Si-based photonic structures like slot waveguides and ring resonators as optically pumped emitters for room temperature applications. In order to create such hybrid structures, the NCs were dissolved into polymer resists and drop cast on top of the device. Upon optical pumping, intense photoluminescence emission from the resonating modes is recorded at the output of the waveguide with transmission quality factors up to 14000. The polymer host material was investigated with respect to its ability to stabilize the NC's photoluminescence emission against degradation under ambient conditions. The waveguide-ring coupling efficiency was also investigated as function of the NCs concentrations blended into the polymer matrix. The integration of colloidal quantum dots into Silicon photonic structures as demonstrated in this work is a very versatile technique and thus opens a large range of applications utilizing the linear and nonlinear optical properties of PbS NCs at telecom wavelengths.

Spin manipulation and spin-lattice interaction in magnetic colloidal quantum dots

NASA Astrophysics Data System (ADS)

Moro, Fabrizio; Turyanska, Lyudmila; Granwehr, Josef; Patanè, Amalia

2014-11-01

We report on the spin-lattice interaction and coherent manipulation of electron spins in Mn-doped colloidal PbS quantum dots (QDs) by electron spin resonance. We show that the phase memory time,TM , is limited by Mn-Mn dipolar interactions, hyperfine interactions of the protons (1H) on the QD capping ligands with Mn ions in their proximity (<1 nm), and surface phonons originating from thermal fluctuations of the capping ligands. In the low Mn concentration limit and at low temperature, we achieve a long phase memory time constant TM˜0.9 μ s , thus enabling the observation of Rabi oscillations. Our findings suggest routes to the rational design of magnetic colloidal QDs with phase memory times exceeding the current limits of relevance for the implementation of QDs as qubits in quantum information processing.

Design and development of novel linker for PbS quantum dots/TiO₂ mesoscopic solar cell.

PubMed

Etgar, Lioz; Park, Jinhyung; Barolo, Claudia; Nazeeruddin, Md K; Viscardi, Guido; Graetzel, Michael

2011-09-01

A novel bifunctional linker molecule, bis(4-mercaptophenyl)phosphinic acid, is designed to be used in a QDs solar cells. The linker anchors to TiO(2) mesoporous film through the phosphinic acid functional group and to the PbS QDs through the two thiol groups. The way of attachment of this new linker molecule in a photovoltaic PbS QDs/TiO(2) mesoporous device was studied by FTIR measurements. The photovoltaic performance of this new linker in a heterojunction PbS QDs solar cell show high V(oc) relative to QDs based solar cells, which will allow to receive high power conversion efficiency using this novel designed linker. This novel bifunctional linker molecule should pave the way for enhancing binding strength, and efficiency of QDs solar cells compared to the state-of-the-art linkers.

Controlled waveguide coupling for photon emission from colloidal PbS quantum dot using tunable microcavity made of optical polymer and silicon

NASA Astrophysics Data System (ADS)

Nozaka, Takahiro; Mukai, Kohki

2016-04-01

A tunable microcavity device composed of optical polymer and Si with a colloidal quantum dot (QD) is proposed as a single-photon source for planar optical circuit. Cavity size is controlled by electrostatic micromachine behavior with the air bridge structure to tune timing of photon injection into optical waveguide from QD. Three-dimensional positioning of a QD in the cavity structure is available using a nanohole on Si processed by scanning probe microscope lithography. We fabricated the prototype microcavity with PbS-QD-mixed polymenthyl methacrylate on a SOI (semiconductor-on-insulator) substrate to show the tunability of cavity size as the shift of emission peak wavelength of QD ensemble.

Optimization of carrier multiplication for more effcient solar cells: the case of Sn quantum dots.

PubMed

Allan, Guy; Delerue, Christophe

2011-09-27

We present calculations of impact ionization rates, carrier multiplication yields, and solar-power conversion efficiencies in solar cells based on quantum dots (QDs) of a semimetal, α-Sn. Using these results and previous ones on PbSe and PbS QDs, we discuss a strategy to select QDs with the highest carrier multiplication rate for more efficient solar cells. We suggest using QDs of materials with a close to zero band gap and a high multiplicity of the bands in order to favor the relaxation of photoexcited carriers by impact ionization. Even in that case, the improvement of the maximum solar-power conversion efficiency appears to be a challenging task. © 2011 American Chemical Society

Electrochemical immunoassay for the detection of IgM antibodies using polydopamine particles loaded with PbS quantum dots as labels.

PubMed

Ortega, Greter A; Zuaznabar-Gardona, Julio C; Reguera, Edilso

2018-09-30

Here, we report for the first time, an electrochemical immunoassay to detect IgM antibodies using lead sulfide quantum dots (PbS QDs) as electrochemical labels. In this sense, dendritic-like polydopamine particles loaded with PbS QDs were synthesized by the self-polymerization of dopamine in basic media in the presence of QDs (PbS@PDA) and further tagged with anti-IgM antibodies, dengue specific antigens, and streptavidin moieties. The analytical features of the sandwich immunoassay on ELISA microplate were carried out with the PbS@PDA-labeled anti-IgM as secondary antibody. The system was interrogated by acid dissolution of PbS@PDA, followed by differential pulse anodic stripping voltammetry in the presence of Bi(III) ions using carbon screen-printed electrodes. The results indicate that the voltammetric current increased with the increasing of the concentration of target IgM within a range of 0-0.5 mg mL -1 . The limit of detection of this electrochemical immunoassay was evaluated to 130 ng. The measures of satisfactory recoveries from 88.5% to 114% of spiked samples indicate that such a method has good specificity and is applicable to the quantification of IgM antibodies in complex biological samples. No significant differences at the 0.05 significance level were encountered in the analysis of IgM samples between the electrochemical immunoassay and a Bradford assay. Copyright © 2018 Elsevier B.V. All rights reserved.

Understanding chemically processed solar cells based on quantum dots

PubMed Central

Malgras, Victor; Nattestad, Andrew; Kim, Jung Ho; Dou, Shi Xue; Yamauchi, Yusuke

2017-01-01

Abstract Photovoltaic energy conversion is one of the best alternatives to fossil fuel combustion. Petroleum resources are now close to depletion and their combustion is known to be responsible for the release of a considerable amount of greenhouse gases and carcinogenic airborne particles. Novel third-generation solar cells include a vast range of device designs and materials aiming to overcome the factors limiting the current technologies. Among them, quantum dot-based devices showed promising potential both as sensitizers and as colloidal nanoparticle films. A good example is the p-type PbS colloidal quantum dots (CQDs) forming a heterojunction with a n-type wide-band-gap semiconductor such as TiO2 or ZnO. The confinement in these nanostructures is also expected to result in marginal mechanisms, such as the collection of hot carriers and generation of multiple excitons, which would increase the theoretical conversion efficiency limit. Ultimately, this technology could also lead to the assembly of a tandem-type cell with CQD films absorbing in different regions of the solar spectrum. PMID:28567179

An ultrasensitive quantum dots fluorescent polarization immunoassay based on the antibody modified Au nanoparticles amplifying for the detection of adenosine triphosphate.

PubMed

He, Yanlong; Tian, Jianniao; Hu, Kun; Zhang, Juanni; Chen, Sheng; Jiang, Yixuan; Zhao, Yanchun; Zhao, Shulin

2013-11-13

In this work, an ultrasensitive fluorescent polarization immunoassay (FPIA) method based on the quantum dot/aptamer/antibody/gold nanoparticles ensemble has been developed for the detection of adenosine triphosphate (ATP). DNA hybridization is formed when ATP is present in the PBS solution containing the DNA-conjugated quantum dots (QDs) and antibody-AuNPs. The substantial sensitivity improvement of the antibody-AuNPs-enhanced method is mainly attributed to the slower rotation of fluorescent unit when QDs-labeled oligonucleotides hybridize with antibody modified the gold nanoparticle. As a result, the fluorescent polarization (FP) values of the system increase significantly. Under the optimal conditions, a linear response with ATP concentration is ranged from 8×10(-12) M to 2.40×10(-4) M. The detection limit reached as low as 1.8 pM. The developed work provides a sensitive and selective immunoassay protocol for ATP detection, which could be applied in more bioanalytical systems. Crown Copyright © 2013. Published by Elsevier B.V. All rights reserved.

Study of Exciton Hopping Transport in PbS Colloidal Quantum Dot Thin Films Using Frequency- and Temperature-Scanned Photocarrier Radiometry

NASA Astrophysics Data System (ADS)

Hu, Lilei; Mandelis, Andreas; Melnikov, Alexander; Lan, Xinzheng; Hoogland, Sjoerd; Sargent, Edward H.

2017-01-01

Solution-processed colloidal quantum dots (CQDs) are promising materials for realizing low-cost, large-area, and flexible photovoltaic devices. The study of charge carrier transport in quantum dot solids is essential for understanding energy conversion mechanisms. Recently, solution-processed two-layer oleic-acid-capped PbS CQD solar cells with one layer treated with tetrabutylammonium iodide (TBAI) serving as the main light-absorbing layer and the other treated with 1,2-ethanedithiol (EDT) acting as an electron-blocking/hole-extraction layer were reported. These solar cells demonstrated a significant improvement in power conversion efficiency of 8.55% and long-term air stability. Coupled with photocarrier radiometry measurements, this work used a new trap-state mediated exciton hopping transport model, specifically for CQD thin films, to unveil and quantify exciton transport mechanisms through the extraction of hopping transport parameters including exciton lifetimes, hopping diffusivity, exciton detrapping time, and trap-state density. It is shown that PbS-TBAI has higher trap-state density than PbS-EDT that results in higher PbS-EDT exciton lifetimes. Hopping diffusivities of both CQD thin film types show similar temperature dependence, particularly higher temperatures yield higher hopping diffusivity. The higher diffusivity of PbS-TBAI compared with PbS-EDT indicates that PbS-TBAI is a much better photovoltaic material than PbS-EDT. Furthermore, PCR temperature spectra and deep-level photothermal spectroscopy provided additional insights to CQD surface trap states: PbS-TBAI thin films exhibit a single dominant trap level, while PbS-EDT films with lower trap-state densities show multiple trap levels.

Properties of POPC/POPE supported lipid bilayers modified with hydrophobic quantum dots on polyelectrolyte cushions.

PubMed

Kolasinska-Sojka, Marta; Wlodek, Magdalena; Szuwarzynski, Michal; Kereiche, Sami; Kovacik, Lubomir; Warszynski, Piotr

2017-10-01

The formation and properties of supported lipid bilayers (SLB) containing hydrophobic nanoparticles (NP) was studied in relation to underlying cushion obtained from selected polyelectrolyte multilayers. Lipid vesicles were formed from zwitterionic 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphocholine (POPC) and negatively charged 1-palmitoyl-2-oleoyl-sn-glycero-3-phosphoethanolamine (POPE) in phosphate buffer (PBS). As hydrophobic nanoparticles - quantum dots (QD) with size of 3.8nm (emission wavelength of 420nm) were used. Polyelectrolyte multilayers (PEM) were constructed by the sequential, i.e., layer-by-layer (LbL) adsorption of alternately charged polyelectrolytes from their solutions. Liposomes and Liposome-QDs complexes were studied with Transmission Cryo-Electron Microscopy (Cryo-TEM) to verify the quality of vesicles and the position of QD within lipid bilayer. Deposition of liposomes and liposomes with quantum dots on polyelectrolyte films was studied in situ using quartz crystal microbalance with dissipation (QCM-D) technique. The fluorescence emission spectra were analyzed for both: suspension of liposomes with nanoparticles and for supported lipid bilayers containing QD on PEM. It was demonstrated that quantum dots are located in the hydrophobic part of lipid bilayer. Moreover, we proved that such QD-modified liposomes formed supported lipid bilayers and their final structure depended on the type of underlying cushion. Copyright © 2017 Elsevier B.V. All rights reserved.

Efficient PbS/CdS co-sensitized solar cells based on TiO2 nanorod arrays

PubMed Central

2013-01-01

Narrow bandgap PbS nanoparticles, which may expand the light absorption range to the near-infrared region, were deposited on TiO2 nanorod arrays by successive ionic layer adsorption and reaction method to make a photoanode for quantum dot-sensitized solar cells (QDSCs). The thicknesses of PbS nanoparticles were optimized to enhance the photovoltaic performance of PbS QDSCs. A uniform CdS layer was directly coated on previously grown PbS-TiO2 photoanode to protect the PbS from the chemical attack of polysulfide electrolytes. A remarkable short-circuit photocurrent density (approximately 10.4 mA/cm2) for PbS/CdS co-sensitized solar cell was recorded while the photocurrent density of only PbS-sensitized solar cells was lower than 3 mA/cm2. The power conversion efficiency of the PbS/CdS co-sensitized solar cell reached 1.3%, which was beyond the arithmetic addition of the efficiencies of single constituents (PbS and CdS). These results indicate that the synergistic combination of PbS with CdS may provide a stable and effective sensitizer for practical solar cell applications. PMID:23394609

Improved current extraction from ZnO/PbS quantum dot heterojunction photovoltaics using a MoO3 interfacial layer.

PubMed

Brown, Patrick R; Lunt, Richard R; Zhao, Ni; Osedach, Timothy P; Wanger, Darcy D; Chang, Liang-Yi; Bawendi, Moungi G; Bulović, Vladimir

2011-07-13

The ability to engineer interfacial energy offsets in photovoltaic devices is one of the keys to their optimization. Here, we demonstrate that improvements in power conversion efficiency may be attained for ZnO/PbS heterojunction quantum dot photovoltaics through the incorporation of a MoO(3) interlayer between the PbS colloidal quantum dot film and the top-contact anode. Through a combination of current-voltage characterization, circuit modeling, Mott-Schottky analysis, and external quantum efficiency measurements performed with bottom- and top-illumination, these enhancements are shown to stem from the elimination of a reverse-bias Schottky diode present at the PbS/anode interface. The incorporation of the high-work-function MoO(3) layer pins the Fermi level of the top contact, effectively decoupling the device performance from the work function of the anode and resulting in a high open-circuit voltage (0.59 ± 0.01 V) for a range of different anode materials. Corresponding increases in short-circuit current and fill factor enable 1.5-fold, 2.3-fold, and 4.5-fold enhancements in photovoltaic device efficiency for gold, silver, and ITO anodes, respectively, and result in a power conversion efficiency of 3.5 ± 0.4% for a device employing a gold anode.

Automated four color CD4/CD8 analysis of leukocytes by scanning fluorescence microscopy using Quantum dots

NASA Astrophysics Data System (ADS)

Bocsi, Jozsef; Mittag, Anja; Varga, Viktor S.; Molnar, Bela; Tulassay, Zsolt; Sack, Ulrich; Lenz, Dominik; Tarnok, Attila

2006-02-01

Scanning Fluorescence Microscope (SFM) is a new technique for automated motorized microscopes to measure multiple fluorochrome labeled cells (Bocsi et al. Cytometry 2004, 61A:1). The ratio of CD4+/CD8+ cells is an important in immune diagnostics in immunodeficiency and HIV. Therefor a four-color staining protocol (DNA, CD3, CD4 and CD8) for automated SFM analysis of lymphocytes was developed. EDTA uncoagulated blood was stained with organic and inorganic (Quantum dots) fluorochromes in different combinations. Aliquots of samples were measured by Flow Cytometry (FCM) and SFM. By SFM specimens were scanned and digitized using four fluorescence filter sets. Automated cell detection (based on Hoechst 33342 fluorescence), CD3, CD4 and CD8 detection were performed, CD4/CD8 ratio was calculated. Fluorescence signals were well separable on SFM and FCM. Passing and Bablok regression of all CD4/CD8 ratios obtained by FCM and SFM (F(X)=0.0577+0.9378x) are in the 95% confidence interval. Cusum test did not show significant deviation from linearity (P>0.10). This comparison indicates that there is no systemic bias between the two different methods. In SFM analyses the inorganic Quantum dot staining was very stable in PBS in contrast to the organic fluorescent dyes, but bleached shortly after mounting with antioxidant and free radical scavenger mounting media. This shows the difficulty of combinations of organic dyes and Quantum dots. Slide based multi-fluorescence labeling system and automated SFM are applicable tools for the CD4/CD8 ratio determination in peripheral blood samples. Quantum Dots are stable inorganic fluorescence labels that may be used as reliable high resolution dyes for cell labeling.

Facile fabrication of CdSe/CdS quantum dots and their application on the screening of colorectal cancer

NASA Astrophysics Data System (ADS)

Cao, Hongfeng; Dong, Quanjin; Hu, Li; Tu, Shiliang; Chai, Rui; Dai, Qiaoqiong

2015-11-01

In this paper, a facile aqueous route to water-soluble CdSe/CdS quantum dots (QDs) under mild conditions has been developed. The samples were characterized by means of transmission electron microscopy, energy-dispersive X-ray spectroscopy, and photoluminescence (PL) spectroscopy. The PL property of the QDs can be controlled by adjusting the reaction time. The CdSe/CdS QDs after 48-h reaction with size of 5 nm have the strongest PL intensity located at 553 nm, and the highest quantum yield of 19.9 %. The obtained QDs were applied for the colorectal cancer screening. The QDs could be conjugated with antibody of aldo-keto reductase family 1, member B10 (AKR1B10) for the detection of AKR1B10. The AKR1B10 in PBS/5 % serum solution with concentration of 1 ng/mL could be well calibrated, and the limit of detection could be lower than 0.05 ng/mL.

TiO2/PbS/ZnS heterostructure for panchromatic quantum dot sensitized solar cells synthesized by wet chemical route

NASA Astrophysics Data System (ADS)

Bhat, T. S.; Mali, S. S.; Sheikh, A. D.; Korade, S. D.; Pawar, K. K.; Hong, C. K.; Kim, J. H.; Patil, P. S.

2017-11-01

So far we developed the efficient photoelectrodes which can harness the UV as well as the visible regime of the solar spectrum effectively. In order to exploit a maximum portion of solar spectrum, it is necessary to study the synergistic effect of a photoelectrode comprising UV and visible radiations absorbing materials. Present research work highlights the efforts to study the synchronized effect of TiO2 and PbS on the power conversion efficiency of quantum dot sensitized solar cell (QDSSC). A cascade structure of TiO2/PbS/ZnS QDSSC is achieved to enhance the photoconversion efficiency of TiO2/PbS system by incorporating a surface passivation layer of ZnS which avoids the recombination of charge carriers. A QDSSC is fabricated using a simple and cost-effective technique such as hydrothermally grown TiO2 nanorod arrays decorated with PbS and ZnS using successive ionic layer adsorption and reaction (SILAR) method. Synthesized electrode materials are characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), field emission scanning electron microscopy (FE-SEM), High resolution-transmission electron microscopy (TEM), STEM-EDS mapping, optical and solar cell performances. Phase formation of TiO2, PbS and ZnS get confirmed from the XPS study. FE-SEM images of the photoelectrode show uniform coverage of PbS QDs onto the TiO2 nanorods which increases with increasing number of SILAR cycles. The ZnS layer not only improves the charge transport but also reduces the photocorrosion of lead chalcogenides in the presence of a liquid electrolyte. Finally, the photoelectrochemical (PEC) study is carried out using an optimized photoanode comprising TiO2/PbS/ZnS assembly. Under AM 1.5G illumination the TiO2/PbS/ZnS QDSSC photoelectrode shows 4.08 mA/cm2 short circuit current density in a polysulfide electrolyte which is higher than that of a bare TiO2 nanorod array.

Computational Modeling of Photocatalysts for CO2 Conversion Applications

NASA Astrophysics Data System (ADS)

Tafen, De; Matranga, Christopher

2013-03-01

To make photocatalytic conversion approaches efficient, economically practical, and industrially scalable, catalysts capable of utilizing visible and near infrared photons need to be developed. Recently, a series of CdSe and PbS quantum dot-sensitized TiO2 heterostructures have been synthesized, characterized, and tested for reduction of CO2 under visible light. Following these experiments, we use density functional theory to model these heterostructured catalysts and investigate their CO2 catalytic activity. In particular, we study the nature of the heterostructure interface, charge transport/electron transfer, active sites and the electronic structures of these materials. The results will be presented and compared to experiments. The improvement of our understanding of the properties of these materials will aid not only the development of more robust, visible light active photocatalysts for carbon management applications, but also the development of quantum dot-sensitized semiconductor solar cells with high efficiencies in solar-to-electrical energy conversion.

Nanotetrapods: quantum dot hybrid for bulk heterojunction solar cells

PubMed Central

2013-01-01

Hybrid thin film solar cell based on all-inorganic nanoparticles is a new member in the family of photovoltaic devices. In this work, a novel and performance-efficient inorganic hybrid nanostructure with continuous charge transportation and collection channels is demonstrated by introducing CdTe nanotetropods (NTs) and CdSe quantum dots (QDs). Hybrid morphology is characterized, demonstrating an interpenetration and compacted contact of NTs and QDs. Electrical measurements show enhanced charge transfer at the hybrid bulk heterojunction interface of NTs and QDs after ligand exchange which accordingly improves the performance of solar cells. Photovoltaic and light response tests exhibit a combined optic-electric contribution from both CdTe NTs and CdSe QDs through a formation of interpercolation in morphology as well as a type II energy level distribution. The NT and QD hybrid bulk heterojunction is applicable and promising in other highly efficient photovoltaic materials such as PbS QDs. PMID:24139059

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

PubMed

Lan, Xinzheng; Voznyy, Oleksandr; García de Arquer, F Pelayo; Liu, Mengxia; Xu, Jixian; Proppe, Andrew H; Walters, Grant; Fan, Fengjia; Tan, Hairen; Liu, Min; Yang, Zhenyu; Hoogland, Sjoerd; Sargent, Edward H

2016-07-13

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.

Bioengineered II-VI semiconductor quantum dot-carboxymethylcellulose nanoconjugates as multifunctional fluorescent nanoprobes for bioimaging live cells

NASA Astrophysics Data System (ADS)

Mansur, Alexandra A. P.; Mansur, Herman S.; Mansur, Rafael L.; de Carvalho, Fernanda G.; Carvalho, Sandhra M.

2018-01-01

Colloidal semiconductor quantum dots (QDs) are light-emitting ultra-small nanoparticles, which have emerged as a new class of nanoprobes with unique optical properties for bioimaging and biomedical diagnostic. However, to be used for most biomedical applications the biocompatibility and water-solubility are mandatory that can achieved through surface modification forming QD-nanoconjugates. In this study, semiconductor II-VI quantum dots of type MX (M = Cd, Pb, Zn, X = S) were directly synthesized in aqueous media and at room temperature using carboxymethylcellulose sodium salt (CMC) behaving simultaneously as stabilizing and surface biofunctional ligand. These nanoconjugates were extensively characterized using UV-visible spectroscopy, photoluminescence spectroscopy, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, X-ray diffraction, transmission electron microscopy, dynamic light scattering and zeta potential. The results demonstrated that the biopolymer was effective on nucleating and stabilizing the colloidal nanocrystals of CdS, ZnS, and PbS with the average diameter ranging from 2.0 to 5.0 nm depending on the composition of the semiconductor core, which showed quantum-size confinement effect. These QD/polysaccharide conjugates showed luminescent activity from UV-visible to near-infrared range of the spectra under violet laser excitation. Moreover, the bioassays performed proved that these novel nanoconjugates were biocompatible and behaved as composition-dependent fluorescent nanoprobes for in vitro live cell bioimaging with very promising perspectives to be used in numerous biomedical applications and nanomedicine.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gao, Liang; Dong, Dongdong; Qiao, Keke

Wearable and sensitive photodetectors (PDs) have been demonstrated based on a blend film of PbS quantum dots (QDs) and QDs modified multiwalled carbon nanotubes (MWCNTs). Owing to the synergetic effect from high light sensitivity of PbS QDs and excellent conductive and mechanical properties of MWCNTs, the blend PDs show high sensitivity and flexibility performance: device responsivity and detectivity reach 583 mA/W and 3.25 × 10{sup 12 }Jones, respectively, and could stand large number (at least 10 000 cycles) and wide angle (up to 80°) bending. Furthermore, the wearable and sensitive PDs have been applied to measure the heart rate in both red and near infraredmore » (NIR) ranges. The presented PDs are expected to work as sensor candidates in integrated electronic skin.« less

Nanoscale Interfaces in Colloidal Quantum Dot Solar Cells: Physical Insights and Materials Engineering Strategies

NASA Astrophysics Data System (ADS)

Kemp, Kyle Wayne

With growing global energy demand there will be an increased need for sources of renewable energy such as solar cells. To make these photovoltaic technologies more competitive with conventional energy sources such as coal and natural gas requires further reduction in manufacturing costs that can be realized by solution processing and roll-to-roll printing. Colloidal quantum dots are a bandgap tunable, solution processible, semiconductor material which may offer a path forward to efficient, inexpensive photovoltaics. Despite impressive progress in performance with these materials, there remain limitations in photocarrier collection that must be overcome. This dissertation focuses on the characterization of charge recombination and transport in colloidal quantum dot photovoltaics, and the application of this knowledge to the development of new and better materials. Core-shell, PbS-CdS, quantum dots were investigated in an attempt to achieve better surface passivation and reduce electronic defects which can limit performance. Optimization of this material led to improved open circuit voltage, exceeding 0.6 V for the first time, and record published performance of 6% efficiency. Using temperature-dependent and transient photovoltage measurements we explored the significance of interface recombination on the operation of these devices. Careful engineering of the electrode using atomic layer deposition of ZnO helped lead to better TiO2 substrate materials and allowed us to realize a nearly two-fold reduction in recombination rate and an enhancement upwards of 50 mV in open circuit voltage. Carrier extraction efficiency was studied in these devices using intensity dependent current-voltage data of an operational solar cell. By developing an analytical model to describe recombination loss within the active layer of the device we were able to accurately determine transport lengths ranging up to 90 nm. Transient absorption and photoconductivity techniques were used to study charge dynamics by identifying states in these quantum dot materials which facilitate carrier transport. Thermal activation energies for transport of 60 meV or lower were measured for different PbS quantum dot bandgaps, representing a relatively small barrier for carrier transport. From these measurements a dark, quantum confined energy level was attributed to the electronic bandedge of these materials which serves to govern their optoelectronic behavior.

Crystal symmetry breaking and vacancies in colloidal lead chalcogenide quantum dots.

PubMed

Bertolotti, Federica; Dirin, Dmitry N; Ibáñez, Maria; Krumeich, Frank; Cervellino, Antonio; Frison, Ruggero; Voznyy, Oleksandr; Sargent, Edward H; Kovalenko, Maksym V; Guagliardi, Antonietta; Masciocchi, Norberto

2016-09-01

Size and shape tunability and low-cost solution processability make colloidal lead chalcogenide quantum dots (QDs) an emerging class of building blocks for innovative photovoltaic, thermoelectric and optoelectronic devices. Lead chalcogenide QDs are known to crystallize in the rock-salt structure, although with very different atomic order and stoichiometry in the core and surface regions; however, there exists no convincing prior identification of how extreme downsizing and surface-induced ligand effects influence structural distortion. Using forefront X-ray scattering techniques and density functional theory calculations, here we have identified that, at sizes below 8 nm, PbS and PbSe QDs undergo a lattice distortion with displacement of the Pb sublattice, driven by ligand-induced tensile strain. The resulting permanent electric dipoles may have implications on the oriented attachment of these QDs. Evidence is found for a Pb-deficient core and, in the as-synthesized QDs, for a rhombic dodecahedral shape with nonpolar {110} facets. On varying the nature of the surface ligands, differences in lattice strains are found.

Crystal symmetry breaking and vacancies in colloidal lead chalcogenide quantum dots

NASA Astrophysics Data System (ADS)

Bertolotti, Federica; Dirin, Dmitry N.; Ibáñez, Maria; Krumeich, Frank; Cervellino, Antonio; Frison, Ruggero; Voznyy, Oleksandr; Sargent, Edward H.; Kovalenko, Maksym V.; Guagliardi, Antonietta; Masciocchi, Norberto

2016-09-01

Size and shape tunability and low-cost solution processability make colloidal lead chalcogenide quantum dots (QDs) an emerging class of building blocks for innovative photovoltaic, thermoelectric and optoelectronic devices. Lead chalcogenide QDs are known to crystallize in the rock-salt structure, although with very different atomic order and stoichiometry in the core and surface regions; however, there exists no convincing prior identification of how extreme downsizing and surface-induced ligand effects influence structural distortion. Using forefront X-ray scattering techniques and density functional theory calculations, here we have identified that, at sizes below 8 nm, PbS and PbSe QDs undergo a lattice distortion with displacement of the Pb sublattice, driven by ligand-induced tensile strain. The resulting permanent electric dipoles may have implications on the oriented attachment of these QDs. Evidence is found for a Pb-deficient core and, in the as-synthesized QDs, for a rhombic dodecahedral shape with nonpolar {110} facets. On varying the nature of the surface ligands, differences in lattice strains are found.

Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification

DOE PAGES

Kroupa, Daniel M.; Vörös, Márton; Brawand, Nicholas P.; ...

2017-05-16

Band edge positions of semiconductors determine their functionality in many optoelectronic applications such as photovoltaics, photoelectrochemical cells and light emitting diodes. Here we show that band edge positions of lead sulfide (PbS) colloidal semiconductor nanocrystals, specifically quantum dots (QDs), can be tuned over 2.0 eV through surface chemistry modification. We achieved this remarkable control through the development of simple, robust and scalable solution-phase ligand exchange methods, which completely replace native ligands with functionalized cinnamate ligands, allowing for well-defined, highly tunable chemical systems. By combining experiments and ab initio simulations, we establish clear relationships between QD surface chemistry and the bandmore » edge positions of ligand/QD hybrid systems. We find that in addition to ligand dipole, inter-QD ligand shell inter-digitization contributes to the band edge shifts. As a result, we expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications.« less

Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kroupa, Daniel M.; Vörös, Márton; Brawand, Nicholas P.

Band edge positions of semiconductors determine their functionality in many optoelectronic applications such as photovoltaics, photoelectrochemical cells and light emitting diodes. Here we show that band edge positions of lead sulfide (PbS) colloidal semiconductor nanocrystals, specifically quantum dots (QDs), can be tuned over 2.0 eV through surface chemistry modification. We achieved this remarkable control through the development of simple, robust and scalable solution-phase ligand exchange methods, which completely replace native ligands with functionalized cinnamate ligands, allowing for well-defined, highly tunable chemical systems. By combining experiments and ab initio simulations, we establish clear relationships between QD surface chemistry and the bandmore » edge positions of ligand/QD hybrid systems. We find that in addition to ligand dipole, inter-QD ligand shell inter-digitization contributes to the band edge shifts. As a result, we expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications.« less

Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification

PubMed Central

Kroupa, Daniel M.; Vörös, Márton; Brawand, Nicholas P.; McNichols, Brett W.; Miller, Elisa M.; Gu, Jing; Nozik, Arthur J.; Sellinger, Alan; Galli, Giulia; Beard, Matthew C.

2017-01-01

Band edge positions of semiconductors determine their functionality in many optoelectronic applications such as photovoltaics, photoelectrochemical cells and light emitting diodes. Here we show that band edge positions of lead sulfide (PbS) colloidal semiconductor nanocrystals, specifically quantum dots (QDs), can be tuned over 2.0 eV through surface chemistry modification. We achieved this remarkable control through the development of simple, robust and scalable solution-phase ligand exchange methods, which completely replace native ligands with functionalized cinnamate ligands, allowing for well-defined, highly tunable chemical systems. By combining experiments and ab initio simulations, we establish clear relationships between QD surface chemistry and the band edge positions of ligand/QD hybrid systems. We find that in addition to ligand dipole, inter-QD ligand shell inter-digitization contributes to the band edge shifts. We expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications. PMID:28508866

An ultra-broadband perovskite-PbS quantum dot sensitized carbon nanotube photodetector.

PubMed

Ka, Ibrahima; Gerlein, Luis F; Asuo, Ivy M; Nechache, Riad; Cloutier, Sylvain G

2018-05-17

Organic-inorganic perovskites have been hailed as promising candidates for optoelectronic and photovoltaic devices, but their operation remains limited to the visible spectrum. Here, we combine single-wall carbon nanotubes, PbS quantum dots and a perovskite to synthesize hybrid devices suitable for operation in both the visible and near-infrared. The photodetectors thus fabricated show responsivities as high as 0.5 A W-1 and 0.35 A W-1 at 500 nm and at 1300 nm, respectively, with an applied bias of 1 V. Moreover, the incorporation of nanotubes within the perovskite matrix facilitates the carrier extraction, resulting in response time under 250 μs, a gain-bandwidth product of 0.1 MHz and detectivities of 1.4 × 1011 Jones and 0.9 × 1011 Jones at 500 nm and at 1300 nm, respectively. This unique approach opens new pathways for the development of low-cost, high-speed and broadband perovskite-based optoelectronic devices for large-scale manufacturing.

Tuning colloidal quantum dot band edge positions through solution-phase surface chemistry modification

NASA Astrophysics Data System (ADS)

Kroupa, Daniel M.; Vörös, Márton; Brawand, Nicholas P.; McNichols, Brett W.; Miller, Elisa M.; Gu, Jing; Nozik, Arthur J.; Sellinger, Alan; Galli, Giulia; Beard, Matthew C.

2017-05-01

Band edge positions of semiconductors determine their functionality in many optoelectronic applications such as photovoltaics, photoelectrochemical cells and light emitting diodes. Here we show that band edge positions of lead sulfide (PbS) colloidal semiconductor nanocrystals, specifically quantum dots (QDs), can be tuned over 2.0 eV through surface chemistry modification. We achieved this remarkable control through the development of simple, robust and scalable solution-phase ligand exchange methods, which completely replace native ligands with functionalized cinnamate ligands, allowing for well-defined, highly tunable chemical systems. By combining experiments and ab initio simulations, we establish clear relationships between QD surface chemistry and the band edge positions of ligand/QD hybrid systems. We find that in addition to ligand dipole, inter-QD ligand shell inter-digitization contributes to the band edge shifts. We expect that our established relationships and principles can help guide future optimization of functional organic/inorganic hybrid nanostructures for diverse optoelectronic applications.

Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%

DOE PAGES

Yan, Yong; Crisp, Ryan W.; Gu, Jing; ...

2017-04-03

Multiple exciton generation (MEG) in quantum dots (QDs) has the potential to greatly increase the power conversion efficiency in solar cells and in solar-fuel production. During the MEG process, two electron-hole pairs (excitons) are created from the absorption of one high-energy photon, bypassing hot-carrier cooling via phonon emission. Here we demonstrate that extra carriers produced via MEG can be used to drive a chemical reaction with quantum efficiency above 100%. We developed a lead sulfide (PbS) QD photoelectrochemical cell that is able to drive hydrogen evolution from aqueous Na 2S solution with a peak external quantum efficiency exceeding 100%. QDmore » photoelectrodes that were measured all demonstrated MEG when the incident photon energy was larger than 2.7 times the bandgap energy. Finally, our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.« less

Colossal photo-conductive gain in low temperature processed TiO2 films and their application in quantum dot solar cells

NASA Astrophysics Data System (ADS)

Mandal, Debranjan; Goswami, Prasenjit N.; Rath, Arup K.

2017-03-01

Colloidal quantum dot (QD) solar cells have seen remarkable progress in recent past to reach the certified efficiency of 10.6%. Anatase titanium oxide (TiO2) is a widely studied n-type widow layer for the collection of photogenerated electrons in QD solar cells. Requirement of high temperature (˜500 °C) processing steps proved to be disadvantageous for its applications in flexible solar cells and roll to roll processing, and it also has adverse commercial implications. Here, we report that solar light exposure to low temperature processed (80 °C-150 °C) TiO2 and niobium doped TiO2 films leads to unprecedented enhancement in their electron densities and electron mobilities, which enables them to be used as efficient n-type layers in quantum dot solar cells. Such photoinduced high conducting states in these films show gradual decay over hours after the light bias is taken off and can be retrieved under solar illumination. On the contrary, TiO2 films processed at 500 °C show marginal photo induced enhancements in their characteristics. In bilayer configuration with PbS QDs, photovoltaic devices based on low temperature processed TiO2 films show improved performance over high temperature processed TiO2 films. The stability of photovoltaic devices also improved in low temperature processed TiO2 films under ambient working conditions.

Stability of polymer encapsulated quantum dots in cell culture media

NASA Astrophysics Data System (ADS)

Ojea-Jiménez, I.; Piella, J.; Nguyen, T.-L.; Bestetti, A.; Ryan, A. D.; Puntes, V.

2013-04-01

The unique optical properties of Quantum Dots have attracted a great interest to use these nanomaterials in diverse biological applications. The synthesis of QDs by methods from the literature permits one to obtain nanocrystals coated by hydrophobic alkyl coordinating ligands and soluble in most of the cases in organic solvents. The ideal biocompatible QD must be homogeneously dispersed and colloidally stable in aqueous solvents, exhibit pH and salt stability, show low levels of nonspecific binding to biological components, maintain a high quantum yield, and have a small hydrodynamic diameter. Polymer encapsulation represents an excellent scaffold on which to build additional biological function, allowing for a wide range of grafting approaches for biological ligands. As these QD are functionalized with poly(ethylene)glycol (PEG) derivatives on their surface, they show long term stability without any significant change in the optical properties, and they are also highly stable in the most common buffer solutions such as Phosphate Buffer Saline (PBS) or borate. However, as biological studies are normally done in more complex biological media which contain a mixture of amino acids, salts, glucose and vitamins, it is essential to determine the stability of our synthesized QDs under these conditions before tackling biological studies.

Carrier Multiplication in Quantum Dots within the Framework of Two Competing Energy Relaxation Mechanisms.

PubMed

Stewart, John T; Padilha, Lazaro A; Bae, Wan Ki; Koh, Weon-Kyu; Pietryga, Jeffrey M; Klimov, Victor I

2013-06-20

The realization of high-yield, low-threshold carrier multiplication (CM) in semiconductor quantum dots (QDs) is a promising step toward third-generation photovoltaics (PV). Recent studies of QD solar cells have shown that CM can indeed produce greater-than-unity quantum efficiencies in photon-to-charge-carrier conversion, establishing the relevance of this process to practical PV technologies. While being appreciable, the reported CM yields are still not high enough for a significant increase in the power conversion efficiency over traditional bulk materials. At present, the design of nanomaterials with improved CM is hindered by a poor understanding of the mechanism underlying this process. Here, we present a possible solution to this problem by introducing a model that treats CM as a competition between impact-ionization-like scattering and non-CM energy losses. Importantly, it allows for evaluation of expected CM yields from fairly straightforward measurements of Auger recombination (inverse of CM) and near-band-edge carrier cooling. The validation of this model via a comparative CM study of PbTe, PbSe, and PbS QDs suggests that it indeed represents a predictive capability, which might help in the development of nanomaterials with improved CM performance.

Metal-passivated PbS nanoparticles: fabrication and characterization.

PubMed

Tchaplyguine, M; Mikkelä, M-H; Mårsell, E; Polley, C; Mikkelsen, A; Zhang, W; Yartsev, A; Hetherington, C J D; Wallenberg, L R; Björneholm, O

2017-03-08

Organic-shell-free PbS nanoparticles have been produced in the size range relevant for quantum-dot solar cells (QDSCs) by a vapor aggregation method involving magnetron reactive sputtering. This method creates a beam of free 5-10 nm particles in a vacuum. The dimensions of the particles were estimated after their deposition on a substrate by imaging them using ex situ SEM and HRTEM electron microscopy. The particle structure and chemical composition could be deduced "on the fly", prior to deposition, using X-ray photoelectron spectroscopy (XPS) with tunable synchrotron radiation. Our XPS results suggest that under certain conditions it is possible to fabricate particles with a semiconductor core and 1 to 2 monolayer shells of metallic lead. For this case the absolute energy of the highest occupied molecular orbital (HOMO) in PbS has been determined to be (5.0 ± 0.5) eV below the vacuum level. For such particles deposited on a substrate HRTEM has confirmed the XPS-based conclusions on the crystalline PbS structure of the semiconductor core. Absorption spectroscopy on the deposited film has given a value of ∼1 eV for the lowest exciton. Together with the valence XPS results this has allowed us to reconstruct the energy level scheme of the particles. The results obtained are discussed in the context of the properties of PbS QDSCs.

Particle Size/ Grain Size Correlation and Mechanical Properties of Spark Plasma Sintered 8Y-ZrO2, MgAl2O4, and Al2O3 Based Composites

NASA Astrophysics Data System (ADS)

Karandikar, Keyur Kashinath

Solution-processed nanomaterials such as lead sulfide (PbS) colloidal quantum dots (CQDs) combine various manufacturing benefits and facile spectral tunability. However, the low mobility of CQD films limits its power conversion efficiency in photovoltaic cells. Here, I employ a novel femtosecond transient absorption (fs-TA) technique to determine the mobility of PbS CQD films that have undergone state of the art surface treatments. A significant mobility increase from 3 x 10-2 to 5 x 10 -1 cm2 V-1 s-1 was determined for iodide passivated and novel perovskite-shelled PbS CQDs, respectively. I performed, for the first time, temperature-dependent ultrafast carrier dynamics in perovskite-shelled CQDs using fs-TA, and determined an activation energy of 14 meV required for carrier hopping. Complementary studies that used time-of-flight measurements to determine the mobility in solar cell configuration corroborated the fs-TA method. Taken together, these results indicate a promising avenue toward improved CQD solar cells.

Enhanced performance of solution-processed broadband photodiodes by epitaxially blending MAPbBr3 quantum dots and ternary PbSxSe1-x quantum dots as the active layer

NASA Astrophysics Data System (ADS)

Sulaman, Muhammad; Yang, Shengyi; Jiang, Yurong; Tang, Yi; Zou, Bingsuo

2017-12-01

Organic-inorganic hybrid photodetectors attract more and more interest, since they can combine the advantages of both organic and inorganic materials into one device, and broadband photodetectors are widely used in many scientific and industrial fields. In this work, we demonstrate the enhanced-performance solution-processed broadband photodiodes by epitaxially blending organo-lead halide perovskite (MAPbBr3) colloidal quantum dots (CQDs) with ternary PbSxSe1-x CQDs as the active layer. As a result, the interfacial features of the hetero-epitaxial nanocomposite MAPbBr3:PbSxSe1-x enables the design and perception of functionalities that are not available for the single-phase constituents or layered devices. By combining the high electrical transport properties of MAPbBr3 QDs with the highly radiative efficiency of PbS0.4Se0.6 QDs, the photodiodes ITO/ZnO/PbS0.4Se0.6:MAPbBr3/Au exhibit a maximum photoresponsivity and specific detectivity of 21.48 A W-1 and 3.59 × 1013 Jones, 22.16 A W-1 and 3.70 × 1013 Jones at room temperature under 49.8 μW cm-2 532 nm laser and 62 μW cm-2 980 nm laser, respectively. This is higher than that of the layered photodiodes ITO/ZnO/PbS0.4Se0.6/MAPbBr3/Au, pure perovskite (MAPbBr3) (or PbS0.4Se0.6) QD-based photodiodes reported previously, and it is also better than the traditional inorganic semiconductor-based photodetectors. Our experimental results indicate that epitaxially-aligned nanocomposites (MAPbBr3:PbSxSe1-x) exhibit remarkable optoelectronic properties that are traceable to their atomic-scale crystalline coherence, and one can utilize the excellent photocarrier diffusion from PbSxSe1-x into the perovskite to enhance the device performance from the UV-visible to infrared region.

Highly Luminescent Phase-Stable CsPbI3 Perovskite Quantum Dots Achieving Near 100% Absolute Photoluminescence Quantum Yield.

PubMed

Liu, Feng; Zhang, Yaohong; Ding, Chao; Kobayashi, Syuusuke; Izuishi, Takuya; Nakazawa, Naoki; Toyoda, Taro; Ohta, Tsuyoshi; Hayase, Shuzi; Minemoto, Takashi; Yoshino, Kenji; Dai, Songyuan; Shen, Qing

2017-10-24

Perovskite quantum dots (QDs) as a new type of colloidal nanocrystals have gained significant attention for both fundamental research and commercial applications owing to their appealing optoelectronic properties and excellent chemical processability. For their wide range of potential applications, synthesizing colloidal QDs with high crystal quality is of crucial importance. However, like most common QD systems such as CdSe and PbS, those reported perovskite QDs still suffer from a certain density of trapping defects, giving rise to detrimental nonradiative recombination centers and thus quenching luminescence. In this paper, we show that a high room-temperature photoluminescence quantum yield of up to 100% can be obtained in CsPbI 3 perovskite QDs, signifying the achievement of almost complete elimination of the trapping defects. This is realized with our improved synthetic protocol that involves introducing organolead compound trioctylphosphine-PbI 2 (TOP-PbI 2 ) as the reactive precursor, which also leads to a significantly improved stability for the resulting CsPbI 3 QD solutions. Ultrafast kinetic analysis with time-resolved transient absorption spectroscopy evidence the negligible electron or hole-trapping pathways in our QDs, which explains such a high quantum efficiency. We expect the successful synthesis of the "ideal" perovskite QDs will exert profound influence on their applications to both QD-based light-harvesting and -emitting devices.

Direct Low-Temperature Growth of Single-Crystalline Anatase TiO2 Nanorod Arrays on Transparent Conducting Oxide Substrates for Use in PbS Quantum-Dot Solar Cells.

PubMed

Chung, Hyun Suk; Han, Gill Sang; Park, So Yeon; Shin, Hee-Won; Ahn, Tae Kyu; Jeong, Sohee; Cho, In Sun; Jung, Hyun Suk

2015-05-20

We report on the direct growth of anatase TiO2 nanorod arrays (A-NRs) on transparent conducting oxide (TCO) substrates that can be directly applied to various photovoltaic devices via a seed layer mediated epitaxial growth using a facile low-temperature hydrothermal method. We found that the crystallinity of the seed layer and the addition of an amine functional group play crucial roles in the A-NR growth process. The A-NRs exhibit a pure anatase phase with a high crystallinity and preferred growth orientation in the [001] direction. Importantly, for depleted heterojunction solar cells (TiO2/PbS), the A-NRs improve both electron transport and injection properties, thereby largely increasing the short-circuit current density and doubling their efficiency compared to TiO2 nanoparticle-based solar cells.

Optical Absorbance Enhancement in PbS QD/Cinnamate Ligand Complexes.

PubMed

Kroupa, Daniel M; Vörös, Márton; Brawand, Nicholas P; Bronstein, Noah; McNichols, Brett W; Castaneda, Chloe V; Nozik, Arthur J; Sellinger, Alan; Galli, Giulia; Beard, Matthew C

2018-06-08

We studied the optical absorption enhancement in colloidal suspensions of PbS quantum dots (QD) upon ligand exchange from oleate to a series of cinnamate ligands. By combining experiments and ab initio simulations, we elucidate physical parameters that govern the optical absorption enhancement. We find that, within the cinnamate/PbS QD system, the optical absorption enhancement scales linearly with the electronic gap of the ligand, indicating that the ligand/QD coupling occurs equally efficient between the QD and ligand HOMO and their respective LUMO levels. Disruption of the conjugation that connects the aromatic ring and its substituents to the QD core causes a reduction of the electronic coupling. Our results further support the notion that the ligand/QD complex should be considered as a distinct chemical system with emergent behavior rather than a QD core with ligands whose sole purpose is to passivate surface dangling bonds and prevent agglomeration.

Single step deposition of an interacting layer of a perovskite matrix with embedded quantum dots

NASA Astrophysics Data System (ADS)

Ngo, Thi Tuyen; Suarez, Isaac; Sanchez, Rafael S.; Martinez-Pastor, Juan P.; Mora-Sero, Ivan

2016-07-01

Hybrid lead halide perovskite (PS) derivatives have emerged as very promising materials for the development of optoelectronic devices in the last few years. At the same time, inorganic nanocrystals with quantum confinement (QDs) possess unique properties that make them suitable materials for the development of photovoltaics, imaging and lighting applications, among others. In this work, we report on a new methodology for the deposition of high quality, large grain size and pinhole free PS films (CH3NH3PbI3) with embedded PbS and PbS/CdS core/shell Quantum Dots (QDs). The strong interaction between both semiconductors is revealed by the formation of an exciplex state, which is monitored by photoluminescence and electroluminescence experiments. The radiative exciplex relaxation is centered in the near infrared region (NIR), ~1200 nm, which corresponds to lower energies than the corresponding band gap of both perovskite (PS) and QDs. Our approach allows the fabrication of multi-wavelength light emitting diodes (LEDs) based on a PS matrix with embedded QDs, which show considerably low turn-on potentials. The presence of the exciplex state of PS and QDs opens up a broad range of possibilities with important implications in both LEDs and solar cells.Hybrid lead halide perovskite (PS) derivatives have emerged as very promising materials for the development of optoelectronic devices in the last few years. At the same time, inorganic nanocrystals with quantum confinement (QDs) possess unique properties that make them suitable materials for the development of photovoltaics, imaging and lighting applications, among others. In this work, we report on a new methodology for the deposition of high quality, large grain size and pinhole free PS films (CH3NH3PbI3) with embedded PbS and PbS/CdS core/shell Quantum Dots (QDs). The strong interaction between both semiconductors is revealed by the formation of an exciplex state, which is monitored by photoluminescence and electroluminescence experiments. The radiative exciplex relaxation is centered in the near infrared region (NIR), ~1200 nm, which corresponds to lower energies than the corresponding band gap of both perovskite (PS) and QDs. Our approach allows the fabrication of multi-wavelength light emitting diodes (LEDs) based on a PS matrix with embedded QDs, which show considerably low turn-on potentials. The presence of the exciplex state of PS and QDs opens up a broad range of possibilities with important implications in both LEDs and solar cells. Electronic supplementary information (ESI) available. See DOI: 10.1039/c6nr04082a

Investigation of transport properties of ZnO/PbS heterojunction solar cells

NASA Astrophysics Data System (ADS)

Cheng, Yang; Whitaker, Michael D. C.; Whiteside, Vincent R.; Bumm, Lloyd A.; Sellers, Ian R.

Lead sulfide (PbS) and lead selenide (PbSe) colloidal quantum dots (CQDs) are considered as a potential candidate material for solar cell applications due to their large band gap tunability range (0.5 to 1.7 eV) and cost-effective solution based processing. A series of Glass/ITO/ZnO/PbS/MoO3/Au heterojunction solar cells were processed and analyzed. A stable (reproducible) 2% conversion efficiency under 1-sun is achieved based on the result of J - V measurements. Absorbance and external quantum efficiency (EQE) measurements clearly show photo-generated carrier extraction from PbS active layers in the solar cell. However, a non-ideal J - V behavior is observed in current-voltage measurements. This behavior may be attributed to a high density of trap states at the QD surface or defect states at the PbS/ZnO or ITO/ZnO interfaces. C-V and Impedance spectroscopy measurements are used to study this unusual behavior. These techniques could also help probe the transport properties and limitation of these heterojunction solar cells. This research is funded through NASA EPSCoR program Award # NNX13AN101A.

Impedance analysis of PbS colloidal quantum dot solar cells with different ZnO nanowire lengths

NASA Astrophysics Data System (ADS)

Fukuda, Takeshi; Takahashi, Akihiro; Wang, Haibin; Takahira, Kazuya; Kubo, Takaya; Segawa, Hiroshi

2018-03-01

The photoconversion efficiency of colloidal quantum dot (QD) solar cells has been markedly improved by optimizing the surface passivation and device structure, and details of device physics are now under investigation. In this study, we investigated the resistance and capacitance components at the ZnO/PbS-QD interface and inside a PbS-QD layer by measuring the impedance spectrum while the interface area was controlled by changing the ZnO nanowire length. By evaluating the dependence of optical intensity and DC bias voltage on the ZnO nanowire length, only the capacitance was observed to be influenced by the interface area, and this indicates that photoinduced carriers are generated at the surface of PbS-QD. In addition, since the capacitance is proportional to the surface area of the QD, the interface area can be evaluated from the capacitance. Finally, photovoltaic performance was observed to increase with increasing ZnO nanowire length owing to the large interface area, and this result is in good agreement with the capacitance measurement.

Highly Efficient Flexible Quantum Dot Solar Cells with Improved Electron Extraction Using MgZnO Nanocrystals.

PubMed

Zhang, Xiaoliang; Santra, Pralay Kanti; Tian, Lei; Johansson, Malin B; Rensmo, Håkan; Johansson, Erik M J

2017-08-22

Colloidal quantum dot (CQD) solar cells have high potential for realizing an efficient and lightweight energy supply for flexible or wearable electronic devices. To achieve highly efficient and flexible CQD solar cells, the electron transport layer (ETL), extracting electrons from the CQD solid layer, needs to be processed at a low-temperature and should also suppress interfacial recombination. Herein, a highly stable MgZnO nanocrystal (MZO-NC) layer is reported for efficient flexible PbS CQD solar cells. Solar cells fabricated with MZO-NC ETL give a high power conversion efficiency (PCE) of 10.4% and 9.4%, on glass and flexible plastic substrates, respectively. The reported flexible CQD solar cell has the record efficiency to date of flexible CQD solar cells. Detailed theoretical simulations and extensive characterizations reveal that the MZO-NCs significantly enhance charge extraction from CQD solids and diminish the charge accumulation at the ETL/CQD interface, suppressing charge interfacial recombination. These important results suggest that the low-temperature processed MZO-NCs are very promising for use in efficient flexible solar cells or other flexible optoelectronic devices.

Plasmon Enhanced Hetero-Junction Solar Cell

NASA Astrophysics Data System (ADS)

Long, Gen; Ching, Levine; Sadoqi, Mostafa; Xu, Huizhong

2015-03-01

Here we report a systematic study of plasmon-enhanced hetero-junction solar cells made of colloidal quantum dots (PbS) and nanowires (ZnO), with/without metal nanoparticles (Au). The structure of solar cell devices was characterized by AFM, SEM and profilometer, etc. The power conversion efficiencies of solar cell devices were characterized by solar simulator (OAI TriSOL, AM1.5G Class AAA). The enhancement in the photocurrent due to introduction of metal nanoparticles was obvious. We believe this is due to the plasmonic effect from the metal nanoparticles. The correlation between surface roughness, film uniformity and device performance was also studied.

Role of bond adaptability in the passivation of colloidal quantum dot solids.

PubMed

Thon, Susanna M; Ip, Alexander H; Voznyy, Oleksandr; Levina, Larissa; Kemp, Kyle W; Carey, Graham H; Masala, Silvia; Sargent, Edward H

2013-09-24

Colloidal quantum dot (CQD) solids are attractive materials for photovoltaic devices due to their low-cost solution-phase processing, high absorption cross sections, and their band gap tunability via the quantum size effect. Recent advances in CQD solar cell performance have relied on new surface passivation strategies. Specifically, cadmium cation passivation of surface chalcogen sites in PbS CQDs has been shown to contribute to lowered trap state densities and improved photovoltaic performance. Here we deploy a generalized solution-phase passivation strategy as a means to improving CQD surface management. We connect the effects of the choice of metal cation on solution-phase surface passivation, film-phase trap density of states, minority carrier mobility, and photovoltaic power conversion efficiency. We show that trap passivation and midgap density of states determine photovoltaic device performance and are strongly influenced by the choice of metal cation. Supported by density functional theory simulations, we propose a model for the role of cations, a picture wherein metals offering the shallowest electron affinities and the greatest adaptability in surface bonding configurations eliminate both deep and shallow traps effectively even in submonolayer amounts. This work illustrates the importance of materials choice in designing a flexible passivation strategy for optimum CQD device performance.

Visible-Light-Responsive Catalysts Using Quantum Dot-Modified TiO2 for Air and Water Purification

NASA Technical Reports Server (NTRS)

Coutts, Janelle L.; Hintze, Paul E.; Clausen, Christian; Richards, Jeffrey Todd

2014-01-01

Photocatalysis, the oxidation or reduction of contaminants by light-activated catalysts, utilizing titanium dioxide (TiO2) as the catalytic substrate has been widely studied for trace contaminant control in both air and water applications. The interest in this process is due primarily to its low energy consumption and capacity for catalyst regeneration. Titanium dioxide requires ultraviolet light for activation due to its relatively large band gap energy of 3.2 eV. Traditionally, Hg-vapor fluorescent light sources are used in PCO reactors; however, the use of mercury precludes the use of this PCO technology in a spaceflight environment due to concerns over crew Hg exposure. The development of a visible-light responsive (VLR) TiO2-based catalyst would eliminate the concerns over mercury contamination. Further, VLR development would allow for the use of ambient visible solar radiation or highly efficient LEDs, both of which would make PCO approaches more efficient, flexible, economical, and safe. Though VLR catalyst development has been an active area of research for the past two decades, there are few commercially available VLR catalysts. Those VLR catalysts that are commercially available do not have adequate catalytic activity, in the visible region, to make them competitive with those operating under UV irradiation. This study was initiated to develop more effective VLR catalysts through a novel method in which quantum dots (QD) consisting of narrow band gap semiconductors (e.g., CdS, CdSe, PbS, ZnSe, etc.) are coupled to TiO2 via two preparation methods: 1) photodeposition and 2) mechanical alloying using a high-speed ball mill. A library of catalysts was developed and screened for gas and aqueous phase applications using ethanol and 4-chlorophenol as the target contaminants, respectively. Both target compounds are well studied in photocatalytic systems and served as model contaminants for this research. Synthesized catalysts were compared in terms of preparation method, nature of the quantum dots, and dosage of quantum dots.

Visible Light Responsive Catalysts Using Quantum Dot-Modified Ti02 for Air and Water Purification

NASA Technical Reports Server (NTRS)

Coutts, Janelle L.; Levine, Lanfang H.; Richards, Jeffrey T.; Hintze, paul; Clausen, Christian

2012-01-01

The method of photocatalysis utilizing titanium dioxide, TiO2, as the catalyst has been widely studied for trace contaminant control for both air and water applications because of its low energy consumption and use of a regenerable catalyst. Titanium dioxide requires ultraviolet light for activation due to its band gap energy of 3.2 eV. Traditionally, Hg-vapor fluorescent light sources are used in PCO reactors and are a setback for the technology for space application due to the possibility of Hg contamination. The development of a visible light responsive (VLR) TiO2-based catalyst could lead to the use of solar energy in the visible region (approx.45% of the solar spectrum lies in the visible region; > 400 nm) or highly efficient LEDs (with wavelengths > 400 nm) to make PCO approaches more efficient, economical, and safe. Though VLR catalyst development has been an active area of research for the past two decades, there are few commercially available VLR catalysts; those that are available still have poor activity in the visible region compared to that in the UV region. Thus, this study was aimed at the further development of VLR catalysts by a new method - coupling of quantum dots (QD) of a narrow band gap semiconductor (e.g., CdS, CdSe, PbS, ZnSe, etc.) to the TiO2 by two preparation methods: 1) photodeposition and 2) mechanical alloying using a high-speed ball mill. A library of catalysts was developed and screened for gas and aqueous phase applications, using ethanol and 4-chlorophenol as the target contaminants, respectively. Both target compounds are well studied in photocatalytic systems serve as model contaminants for this research. Synthesized catalysts were compared in terms of preparation method, type of quantum dots, and dosage of quantum dots.

Plasmonically enhanced electromotive force of narrow bandgap PbS QD-based photovoltaics.

PubMed

Li, Xiaowei; McNaughter, Paul D; O'Brien, Paul; Minamimoto, Hiro; Murakoshi, Kei

2018-05-30

Electromotive force of photovoltaics is a key to define the output power density of photovoltaics. Multiple exciton generation (MEG) exhibited by semiconductor quantum dots (QDs) has great potential to enhance photovoltaic performance owing to the ability to generate more than one electron-hole pairs when absorbing a single photon. However, even in MEG-based photovoltaics, limitation of modifying the electromotive force exists due to the intrinsic electrochemical potential of the conduction band-edges of QDs. Here we report a pronouncedly improved photovoltaic performance by constructing a PbS QD-sensitized electrode that comprises plasmon-active Au nanoparticles embedded in a titanium dioxide thin film. Significant enhancement on electromotive force is characterized by the onset potential of photocurrent generation using MEG-effective PbS QDs with a narrow bandgap energy (Eg = 0.9 eV). By coupling with localized surface plasmon resonance (LSPR), such QDs exhibit improved photoresponses and the highest output power density over the other QDs with larger bandgap energies (Eg = 1.1 and 1.7 eV) under visible light irradiation. The wavelength-dependent onset potential and the output power density suggest effective electron injection owing to the enhanced density of electrons excited by energy overlapping between MEG and LSPR.

Semiconductor nanocrystals for novel optical applications

NASA Astrophysics Data System (ADS)

Moon, Jong-Sik

Inspired by the promise of enhanced spectral response, photorefractive polymeric composites photosensitized with semiconductor nanocrystals have emerged as an important class of materials. Here, we report on the photosensitization of photorefractive polymeric composites at visible wavelengths through the inclusion of narrow band-gap semiconductor nanocrystals composed of PbS. Through this approach, internal diffraction efficiencies in excess of 82%, two-beam-coupling gain coefficients in excess of 211 cm-1, and response times 34 ms have been observed, representing some of the best figures-of-merit reported on this class of materials. In addition to providing efficient photosensitization, however, extensive studies of these hybrid composites have indicated that the inclusion of nanocrystals also provides an enhancement in the charge-carrier mobility and subsequent reduction in the photorefractive response time. Through this approach with PbS as charge-carrier, unprecedented response times of 399 micros were observed, opening the door for video and other high-speed applications. It is further demonstrated that this improvement in response time occurs with little sacrifice in photorefractive efficiency and with internal diffraction efficiencies of 72% and two- beam-coupling gain coefficients of 500 cm-1 being measured. A thorough analysis of the experimental data is presented, supporting the hypothesized mechanism of the enhanced charge mobility without the accompaniment of superfluous traps. Finally, water soluble InP/ZnS and CdSe/ZnS quantum dots interacted with CPP and Herceptin to apply them as a bio-maker. Both of quantum dots showed the excellent potential for use in biomedical imaging and drug delivery applications. It is anticipated that these approaches can play a significant role in the eventual commercialization of these classes of materials.

Reaction mechanism of a PbS-on-ZnO heterostructure and enhanced photovoltaic diode performance with an interface-modulated heterojunction energy band structure.

PubMed

Li, Haili; Jiao, Shujie; Ren, Jinxian; Li, Hongtao; Gao, Shiyong; Wang, Jinzhong; Wang, Dongbo; Yu, Qingjiang; Zhang, Yong; Li, Lin

2016-02-07

A room temperature successive ionic layer adsorption and reaction (SILAR) method is introduced for fabricating quantum dots-on-wide bandgap semiconductors. Detailed exploration of how SILAR begins and proceeds is performed by analyzing changes in the electronic structure of related elements at interfaces by X-ray photoelectric spectroscopy, together with characterization of optical properties and X-ray diffraction. The distribution of PbS QDs on ZnO, which is critical for optoelectrical applications of PbS with a large dielectric constant, shows a close relationship with the dipping order. A successively deposited PbS QDs layer is obtained when the sample is first immersed in Na2S solution. This is reasonable because the initial formation of different chemical bonds on ZnO nanorods is closely related to dangling bonds and defect states on surfaces. Most importantly, dipping order also affects their optoelectrical characteristics greatly, which can be explained by the heterojunction energy band structure related to the interface. The formation mechanism for PbS QDs on ZnO is confirmed by the fact that the photovoltaic diode device performance is closely related to the dipping order. Our atomic-scale understanding emphasises the fundamental role of surface chemistry in the structure and tuning of optoelectrical properties, and consequently in devices.

Metal Halide Solid-State Surface Treatment for High Efficiency PbS and PbSe QD Solar Cells

PubMed Central

Crisp, Ryan W.; Kroupa, Daniel M.; Marshall, Ashley R.; Miller, Elisa M.; Zhang, Jianbing; Beard, Matthew C.; Luther, Joseph M.

2015-01-01

We developed a layer-by-layer method of preparing PbE (E = S or Se) quantum dot (QD) solar cells using metal halide (PbI2, PbCl2, CdI2, or CdCl2) salts dissolved in dimethylformamide to displace oleate surface ligands and form conductive QD solids. The resulting QD solids have a significant reduction in the carbon content compared to films treated with thiols and organic halides. We find that the PbI2 treatment is the most successful in removing alkyl surface ligands and also replaces most surface bound Cl- with I-. The treatment protocol results in PbS QD films exhibiting a deeper work function and band positions than other ligand exchanges reported previously. The method developed here produces solar cells that perform well even at film thicknesses approaching a micron, indicating improved carrier transport in the QD films. We demonstrate QD solar cells based on PbI2 with power conversion efficiencies above 7%. PMID:25910183

Metal halide solid-state surface treatment for high efficiency PbS and PbSe QD solar cells.

PubMed

Crisp, Ryan W; Kroupa, Daniel M; Marshall, Ashley R; Miller, Elisa M; Zhang, Jianbing; Beard, Matthew C; Luther, Joseph M

2015-04-24

We developed a layer-by-layer method of preparing PbE (E = S or Se) quantum dot (QD) solar cells using metal halide (PbI2, PbCl2, CdI2, or CdCl2) salts dissolved in dimethylformamide to displace oleate surface ligands and form conductive QD solids. The resulting QD solids have a significant reduction in the carbon content compared to films treated with thiols and organic halides. We find that the PbI2 treatment is the most successful in removing alkyl surface ligands and also replaces most surface bound Cl(-) with I(-). The treatment protocol results in PbS QD films exhibiting a deeper work function and band positions than other ligand exchanges reported previously. The method developed here produces solar cells that perform well even at film thicknesses approaching a micron, indicating improved carrier transport in the QD films. We demonstrate QD solar cells based on PbI2 with power conversion efficiencies above 7%.

Metal Halide Solid-State Surface Treatment for High Efficiency PbS and PbSe QD Solar Cells

DOE PAGES

Crisp, R. W.; Kroupa, D. M.; Marshall, A. R.; ...

2015-04-24

We developed a layer-by-layer method of preparing PbE (E = S or Se) quantum dot (QD) solar cells using metal halide (PbI 2, PbCl 2, CdI 2, or CdCl 2) salts dissolved in dimethylformamide to displace oleate surface ligands and form conductive QD solids. The resulting QD solids have a significant reduction in the carbon content compared to films treated with thiols and organic halides. We find that the PbI 2 treatment is the most successful in removing alkyl surface ligands and also replaces most surface bound Cl- with I-. The treatment protocol results in PbS QD films exhibiting amore » deeper work function and band positions than other ligand exchanges reported previously. The method developed here produces solar cells that perform well even at film thicknesses approaching a micron, indicating improved carrier transport in the QD films. We demonstrate QD solar cells based on PbI 2 with power conversion efficiencies above 7%.« less

Single molecule localization imaging of exosomes using blinking silicon quantum dots

NASA Astrophysics Data System (ADS)

Zong, Shenfei; Zong, Junzhu; Chen, Chen; Jiang, Xiaoyue; Zhang, Yizhi; Wang, Zhuyuan; Cui, Yiping

2018-02-01

Discovering new fluorophores, which are suitable for single molecule localization microscopy (SMLM) is important for promoting the applications of SMLM in biological or material sciences. Here, we found that silicon quantum dots (Si QDs) possess a fluorescence blinking behavior, making them an excellent candidate for SMLM. The Si QDs are fabricated using a facile microwave-assisted method. Blinking of Si QDs is confirmed by single particle fluorescence measurement and the spatial resolution achieved is about 30 nm. To explore the potential application of Si QDs as the nanoprobes for SMLM imaging, cell derived exosomes are chosen as the object owing to their small size (50-100 nm in diameter). Since CD63 is commonly presented on the membrane of exosomes, CD63 aptamers are attached to the surface of Si QDs to form nanoprobes which can specifically recognize exosomes. SMLM imaging shows that Si QDs based nanoprobes can indeed realize super resolved optical imaging of exosomes. More importantly, blinking of Si QDs is observed in water or PBS buffer with no need for special imaging buffers. Besides, considering that silicon is highly biocompatible, Si QDs should have minimal cytotoxicity. These features make Si QDs quite suitable for SMLM applications especially for live cell imaging.

Hybrid tandem quantum dot/organic photovoltaic cells with complementary near infrared absorption

NASA Astrophysics Data System (ADS)

Kim, Taesoo; Palmiano, Elenita; Liang, Ru-Ze; Hu, Hanlin; Murali, Banavoth; Kirmani, Ahmad R.; Firdaus, Yuliar; Gao, Yangqin; Sheikh, Arif; Yuan, Mingjian; Mohammed, Omar F.; Hoogland, Sjoerd; Beaujuge, Pierre M.; Sargent, Edward H.; Amassian, Aram

2017-05-01

Monolithically integrated hybrid tandem solar cells that effectively combine solution-processed colloidal quantum dot (CQD) and organic bulk heterojunction subcells to achieve tandem performance that surpasses the individual subcell efficiencies have not been demonstrated to date. In this work, we demonstrate hybrid tandem cells with a low bandgap PbS CQD subcell harvesting the visible and near-infrared photons and a polymer:fullerene—poly (diketopyrrolopyrrole-terthiophene) (PDPP3T):[6,6]-phenyl-C60-butyric acid methyl ester (PC61BM)—top cell absorbing effectively the red and near-infrared photons of the solar spectrum in a complementary fashion. The two subcells are connected in series via an interconnecting layer (ICL) composed of a metal oxide layer, a conjugated polyelectrolyte, and an ultrathin layer of Au. The ultrathin layer of Au forms nano-islands in the ICL, reducing the series resistance, increasing the shunt resistance, and enhancing the device fill-factor. The hybrid tandems reach a power conversion efficiency (PCE) of 7.9%, significantly higher than the PCE of the corresponding individual single cells, representing one of the highest efficiencies reported to date for hybrid tandem solar cells based on CQD and polymer subcells.

Thin-Film Quantum Dot Photodiode for Monolithic Infrared Image Sensors.

PubMed

Malinowski, Pawel E; Georgitzikis, Epimitheas; Maes, Jorick; Vamvaka, Ioanna; Frazzica, Fortunato; Van Olmen, Jan; De Moor, Piet; Heremans, Paul; Hens, Zeger; Cheyns, David

2017-12-10

Imaging in the infrared wavelength range has been fundamental in scientific, military and surveillance applications. Currently, it is a crucial enabler of new industries such as autonomous mobility (for obstacle detection), augmented reality (for eye tracking) and biometrics. Ubiquitous deployment of infrared cameras (on a scale similar to visible cameras) is however prevented by high manufacturing cost and low resolution related to the need of using image sensors based on flip-chip hybridization. One way to enable monolithic integration is by replacing expensive, small-scale III-V-based detector chips with narrow bandgap thin-films compatible with 8- and 12-inch full-wafer processing. This work describes a CMOS-compatible pixel stack based on lead sulfide quantum dots (PbS QD) with tunable absorption peak. Photodiode with a 150-nm thick absorber in an inverted architecture shows dark current of 10 -6 A/cm² at -2 V reverse bias and EQE above 20% at 1440 nm wavelength. Optical modeling for top illumination architecture can improve the contact transparency to 70%. Additional cooling (193 K) can improve the sensitivity to 60 dB. This stack can be integrated on a CMOS ROIC, enabling order-of-magnitude cost reduction for infrared sensors.

Development of Multifunctional Nanoparticles for Cancer Therapy Applications

NASA Astrophysics Data System (ADS)

Huth, Christopher

The focus of this thesis is the functionalization and tailoring of nanoparticle surfaces to perform specific objectives in a biological environment. The nanoparticles examined include carbon nanotubes (CNTs), superparamagnetic iron oxide nanoparticles and superparamagnetic iron oxide nanocomposites. The unique nanomaterials have been developed to address continued issues in cancer therapy, including cancer diagnosis and efficient drug delivery. CNT surfaces were modified by plasma polymerization, providing functional groups for conjugation. Luminescent amine labeled quantum dots were fixed to the surface of the CNTs to aid in cancer diagnosis by in vivo imaging. Mice, injected with the quantum dot functionalized carbon nanotubes, were imaged displaying the in vivo imaging capability. In addition, the drug loading and drug release capabilities were examined by incorporating the drug paclitaxel into PLGA-coated CNTs, which showed much higher cytotoxicity to PC-3MM2 human prostate carcinoma cells compared to CNTs without paclitaxel. Paclitaxel was loaded at 112.5 microg/mg of PLGA-coated CNTs. Iron oxide nanocomposites were functionalized with quantum dots for diagnosis applications. Because the nanocomposites contain iron oxide, the nanoparticle provides the opportunity for magnetic hyperthermia, creating a unique material for diagnosis and therapy. Mice, injected with the quantum dot functionalized iron oxide nanocomposites, were imaged displaying the in vivo imaging capability. The magnetic hyperthermic property of the quantum dot functionalized nanocomposites was observed with the attainment of temperatures above 50°C during exposure to an alternating magnetic field. Thermoresponsive nanoparticles were prepared by immobilizing a 2 - 3 nm thick phospholipid layer on the surface of superparamagnetic Fe3O 4 nanoparticles via high affinity avidin/biotin interactions. Morphological and physicochemical surface properties were assessed using TEM, confocal laser scanning microscopy, differential scanning calorimetry, and ATR-FTIR. The zeta potential of Fe3O4 colloids in phosphate buffered saline (PBS) decreased from -23.6 to -5.0 mV as a consequence of phospholipid immobilization. Hyperthermia-relevant temperatures greater than 40°C were achieved within 10--15 min using a 7-mT magnetic field alternating at a frequency of 1MHz. Loading of the surface-associated phospholipid layer with the hydrophobic dye dansylcadaverine was accomplished at an efficiency of 479 ng/mg Fe3O4. Release of this drug surrogate was temperature-dependent, resulting in a 2.5-fold greater release rate when nanoparticles were exposed to temperatures above the experimentally determined melting temperature of 39.7°C. In vitro cytotoxicity studies by release of the cytotoxic drug, doxorubicin, from the thermoresponsive nanoparticles was lastly intended. However, colloidal stability became an issue, prompting a thorough review of nanoparticle stabilization. Factors affecting stabilization, including dispersant, the nanoparticle, and the thermoresponsive coating, were characterized by dynamic light scattering and zeta potential. PBS was compared to two dispersants containing lower ionic concentrations, HBSS and HEPES, using the original iron oxide nanoparticles compared to an iron oxide nanocomposite. The nanocomposite in the HEPES buffer displayed the greatest stability with a zeta potential of -30.47 mV and particle size of 155.4 nm. Stabilization of the immobilized phospholipid bilayer was examined with and without incorporation of the cationic lipid stearylamine. Zeta potential (33.6 mV) and size (315 nm) data indicate that stearylamine incorporated DPPC coated nanoparticles provide better stability.

Microfluidic Technology: Uncovering the Mechanisms of Nanocrystal Nucleation and Growth.

PubMed

Lignos, Ioannis; Maceiczyk, Richard; deMello, Andrew J

2017-05-16

The controlled and reproducible formation of colloidal semiconductor nanocrystals (or quantum dots) is of central importance in nanoscale science and technology. The tunable size- and shape-dependent properties of such materials make them ideal candidates for the development of efficient and low-cost displays, solar cells, light-emitting devices, and catalysts. The formidable difficulties associated with the macroscale preparation of semiconductor nanocrystals (possessing bespoke optical and chemical properties) result from the fact that underlying reaction mechanisms are complex and that the reactive environment is difficult to control. Automated microfluidic reactors coupled with monitoring systems and optimization algorithms aim to elucidate complex reaction mechanisms that govern both nucleation and growth of nanocrystals. Such platforms are ideally suited for the efficient optimization of reaction parameters, assuring the reproducible synthesis of nanocrystals with user-defined properties. This Account aims to inform the nanomaterials community about how microfluidic technologies can supplement flask experimentation for the ensemble investigation of formation mechanisms and design of semiconductor nanocrystals. We present selected studies outlining the preparation of quantum dots using microfluidic systems with integrated analytics. Such microfluidic reaction systems leverage the ability to extract real-time information regarding optical, structural, and compositional characteristics of quantum dots during nucleation and growth stages. The Account further highlights our recent research activities focused on the development and application of droplet-based microfluidics with integrated optical detection systems for the efficient and rapid screening of reaction conditions and a better understanding of the mechanisms of quantum dot synthesis. We describe the features and operation of fully automated microfluidic reactors and their subsequent application to high-throughput parametric screening of metal chalcogenides (CdSe, PbS, PbSe, CdSeTe), ternary and core/shell heavy metal-free quantum dots (CuInS 2 , CuInS 2 /ZnS), and all-inorganic perovskite nanocrystals (CsPbX 3 , X = Cl, Br, I) syntheses. Critically, concurrent absorption and photoluminescence measurements on millisecond to second time scales allow the extraction of basic parameters governing nanocrystal formation. Moreover, experimental data obtained from such microfluidic platforms can be directly supported by theoretical models of nucleation and growth. To this end, we also describe the use of metamodeling algorithms able to accurately predict optimized conditions of CdSe synthesis using a minimal number of sample parameters. Importantly, we discuss future challenges that must be addressed before microfluidic technologies are in a position to be widely adopted for the on-demand formation of nanocrystals. From a technology perspective, these challenges include the development of novel engineering platforms for the formation of complex architectures, the integration of monitoring systems able to harvest photophysical and structural information, the incorporation of continuous purification systems, and the application of optimization algorithms to multicomponent quantum dot systems.

Detection of CdSe quantum dot photoluminescence for security label on paper

DOE Office of Scientific and Technical Information (OSTI.GOV)

Isnaeni,, E-mail: isnaeni@lipi.go.id; Sugiarto, Iyon Titok; Bilqis, Ratu

CdSe quantum dot has great potential in various applications especially for emitting devices. One example potential application of CdSe quantum dot is security label for anti-counterfeiting. In this work, we present a practical approach of security label on paper using one and two colors of colloidal CdSe quantum dot, which is used as stamping ink on various types of paper. Under ambient condition, quantum dot is almost invisible. The quantum dot security label can be revealed by detecting emission of quantum dot using photoluminescence and cnc machine. The recorded quantum dot emission intensity is then analyzed using home-made program tomore » reveal quantum dot pattern stamp having the word ’RAHASIA’. We found that security label using quantum dot works well on several types of paper. The quantum dot patterns can survive several days and further treatment is required to protect the quantum dot. Oxidation of quantum dot that occurred during this experiment reduced the emission intensity of quantum dot patterns.« less

Direct work function measurement by gas phase photoelectron spectroscopy and its application on PbS nanoparticles.

PubMed

Axnanda, Stephanus; Scheele, Marcus; Crumlin, Ethan; Mao, Baohua; Chang, Rui; Rani, Sana; Faiz, Mohamed; Wang, Suidong; Alivisatos, A Paul; Liu, Zhi

2013-01-01

Work function is a fundamental property of a material's surface. It is playing an ever more important role in engineering new energy materials and efficient energy devices, especially in the field of photovoltaic devices, catalysis, semiconductor heterojunctions, nanotechnology, and electrochemistry. Using ambient pressure X-ray photoelectron spectroscopy (APXPS), we have measured the binding energies of core level photoelectrons of Ar gas in the vicinity of several reference materials with known work functions (Au(111), Pt(111), graphite) and PbS nanoparticles. We demonstrate an unambiguously negative correlation between the work functions of reference samples and the binding energies of Ar 2p core level photoelectrons detected from the Ar gas near the sample surface region. Using this experimentally determined linear relationship between the surface work function and Ar gas core level photoelectron binding energy, we can measure the surface work function of different materials under different gas environments. To demonstrate the potential applications of this ambient pressure XPS technique in nanotechnology and solar energy research, we investigate the work functions of PbS nanoparticles with various capping ligands: methoxide, mercaptopropionic acid, and ethanedithiol. Significant Fermi level position changes are observed for PbS nanoparticles when the nanoparticle size and capping ligands are varied. The corresponding changes in the valence band maximum illustrate that an efficient quantum dot solar cell design has to take into account the electrochemical effect of the capping ligand as well.

Quantum Dots

NASA Astrophysics Data System (ADS)

Tartakovskii, Alexander

2012-07-01

Part I. Nanostructure Design and Structural Properties of Epitaxially Grown Quantum Dots and Nanowires: 1. Growth of III/V semiconductor quantum dots C. Schneider, S. Hofling and A. Forchel; 2. Single semiconductor quantum dots in nanowires: growth, optics, and devices M. E. Reimer, N. Akopian, M. Barkelid, G. Bulgarini, R. Heeres, M. Hocevar, B. J. Witek, E. Bakkers and V. Zwiller; 3. Atomic scale analysis of self-assembled quantum dots by cross-sectional scanning tunneling microscopy and atom probe tomography J. G. Keizer and P. M. Koenraad; Part II. Manipulation of Individual Quantum States in Quantum Dots Using Optical Techniques: 4. Studies of the hole spin in self-assembled quantum dots using optical techniques B. D. Gerardot and R. J. Warburton; 5. Resonance fluorescence from a single quantum dot A. N. Vamivakas, C. Matthiesen, Y. Zhao, C.-Y. Lu and M. Atature; 6. Coherent control of quantum dot excitons using ultra-fast optical techniques A. J. Ramsay and A. M. Fox; 7. Optical probing of holes in quantum dot molecules: structure, symmetry, and spin M. F. Doty and J. I. Climente; Part III. Optical Properties of Quantum Dots in Photonic Cavities and Plasmon-Coupled Dots: 8. Deterministic light-matter coupling using single quantum dots P. Senellart; 9. Quantum dots in photonic crystal cavities A. Faraon, D. Englund, I. Fushman, A. Majumdar and J. Vukovic; 10. Photon statistics in quantum dot micropillar emission M. Asmann and M. Bayer; 11. Nanoplasmonics with colloidal quantum dots V. Temnov and U. Woggon; Part IV. Quantum Dot Nano-Laboratory: Magnetic Ions and Nuclear Spins in a Dot: 12. Dynamics and optical control of an individual Mn spin in a quantum dot L. Besombes, C. Le Gall, H. Boukari and H. Mariette; 13. Optical spectroscopy of InAs/GaAs quantum dots doped with a single Mn atom O. Krebs and A. Lemaitre; 14. Nuclear spin effects in quantum dot optics B. Urbaszek, B. Eble, T. Amand and X. Marie; Part V. Electron Transport in Quantum Dots Fabricated by Lithographic Techniques: III-V Semiconductors and Carbon: 15. Electrically controlling single spin coherence in semiconductor nanostructures Y. Dovzhenko, K. Wang, M. D. Schroer and J. R. Petta; 16. Theory of electron and nuclear spins in III-V semiconductor and carbon-based dots H. Ribeiro and G. Burkard; 17. Graphene quantum dots: transport experiments and local imaging S. Schnez, J. Guettinger, F. Molitor, C. Stampfer, M. Huefner, T. Ihn and K. Ensslin; Part VI. Single Dots for Future Telecommunications Applications: 18. Electrically operated entangled light sources based on quantum dots R. M. Stevenson, A. J. Bennett and A. J. Shields; 19. Deterministic single quantum dot cavities at telecommunication wavelengths D. Dalacu, K. Mnaymneh, J. Lapointe, G. C. Aers, P. J. Poole, R. L. Williams and S. Hughes; Index.

Scalable quantum computer architecture with coupled donor-quantum dot qubits

DOEpatents

Schenkel, Thomas; Lo, Cheuk Chi; Weis, Christoph; Lyon, Stephen; Tyryshkin, Alexei; Bokor, Jeffrey

2014-08-26

A quantum bit computing architecture includes a plurality of single spin memory donor atoms embedded in a semiconductor layer, a plurality of quantum dots arranged with the semiconductor layer and aligned with the donor atoms, wherein a first voltage applied across at least one pair of the aligned quantum dot and donor atom controls a donor-quantum dot coupling. A method of performing quantum computing in a scalable architecture quantum computing apparatus includes arranging a pattern of single spin memory donor atoms in a semiconductor layer, forming a plurality of quantum dots arranged with the semiconductor layer and aligned with the donor atoms, applying a first voltage across at least one aligned pair of a quantum dot and donor atom to control a donor-quantum dot coupling, and applying a second voltage between one or more quantum dots to control a Heisenberg exchange J coupling between quantum dots and to cause transport of a single spin polarized electron between quantum dots.

TiO{sub 2} flower-like nanostructures decorated with CdS/PbS nanoparticles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Trenczek-Zajac, Anita, E-mail: anita.trenczek-zajac@agh.edu.pl; Kusior, Anna; Lacz, Agnieszka

Highlights: • TiO{sub 2} flower-like nanostructures were prepared with the use of Ti foil and 30% H{sub 2}O{sub 2}. • QDs of CdS and PbS were deposited using the SILAR method. • The SILAR method makes it possible to control the size of QDs. • Band gap energy of CdS was found to be 2.35 eV. • Sensitization of TiO{sub 2} with CdS or PbS improves the photoelectrochemical properties. - Abstract: Flower-like nanostructures of TiO{sub 2} were prepared by immersing Ti foil in 30% H{sub 2}O{sub 2} at 80 °C for times varying from 15 to 240 min. Upon annealingmore » at 450 °C in an Ar atmosphere, the received amorphous samples crystallized in an anatase structure with rutile as a minority phase. SEM images revealed that partially formed flowers were present at the surface of the prepared samples as early as after 15 min of immersion. The size of the individual flowers increased from 400–800 nm after 15 min of reaction to 2.5–6.0 μm after 240 min. It was also found that surface is very rough and surface development is considerable. After 45 min of immersion, the nanoflowers were sensitized with CdS and PbS quantum dots (QDs-CdS/QDs-PbS) deposited using the SILAR method from water- and methanol-based precursor solutions at different concentrations (0.001–0.1 M). QDs-CdS crystallized in the hawleyite structure, while QDs-PbS in the galena form. SEM analysis showed the tendency of quantum dots to agglomerate at high concentrations of the precursor in water-based solutions. QDs obtained from methanol-based solutions were uniformly distributed. The produced QDs-PbS were smaller than QDs-CdS. Based on the optical reflectance spectra, the band-gap energies of TiO{sub 2} nanostructures with and without QDs were calculated to be 3.32 eV for flower-like TiO{sub 2} nanostructures and 2.35 eV for QDs-CdS. The photoelectrochemical behaviour of nanoflowers was found to improve significantly after the deposition of QDs-CdS.« less

Thin-Film Quantum Dot Photodiode for Monolithic Infrared Image Sensors †

PubMed Central

Georgitzikis, Epimitheas; Vamvaka, Ioanna; Frazzica, Fortunato; Van Olmen, Jan; De Moor, Piet; Heremans, Paul; Hens, Zeger; Cheyns, David

2017-01-01

Imaging in the infrared wavelength range has been fundamental in scientific, military and surveillance applications. Currently, it is a crucial enabler of new industries such as autonomous mobility (for obstacle detection), augmented reality (for eye tracking) and biometrics. Ubiquitous deployment of infrared cameras (on a scale similar to visible cameras) is however prevented by high manufacturing cost and low resolution related to the need of using image sensors based on flip-chip hybridization. One way to enable monolithic integration is by replacing expensive, small-scale III–V-based detector chips with narrow bandgap thin-films compatible with 8- and 12-inch full-wafer processing. This work describes a CMOS-compatible pixel stack based on lead sulfide quantum dots (PbS QD) with tunable absorption peak. Photodiode with a 150-nm thick absorber in an inverted architecture shows dark current of 10−6 A/cm2 at −2 V reverse bias and EQE above 20% at 1440 nm wavelength. Optical modeling for top illumination architecture can improve the contact transparency to 70%. Additional cooling (193 K) can improve the sensitivity to 60 dB. This stack can be integrated on a CMOS ROIC, enabling order-of-magnitude cost reduction for infrared sensors. PMID:29232871

An All-Solution-Based Hybrid CMOS-Like Quantum Dot/Carbon Nanotube Inverter.

PubMed

Shulga, Artem G; Derenskyi, Vladimir; Salazar-Rios, Jorge Mario; Dirin, Dmitry N; Fritsch, Martin; Kovalenko, Maksym V; Scherf, Ullrich; Loi, Maria A

2017-09-01

The development of low-cost, flexible electronic devices is subordinated to the advancement in solution-based and low-temperature-processable semiconducting materials, such as colloidal quantum dots (QDs) and single-walled carbon nanotubes (SWCNTs). Here, excellent compatibility of QDs and SWCNTs as a complementary pair of semiconducting materials for fabrication of high-performance complementary metal-oxide-semiconductor (CMOS)-like inverters is demonstrated. The n-type field effect transistors (FETs) based on I - capped PbS QDs (V th = 0.2 V, on/off = 10 5 , S S-th = 114 mV dec -1 , µ e = 0.22 cm 2 V -1 s -1 ) and the p-type FETs with tailored parameters based on low-density random network of SWCNTs (V th = -0.2 V, on/off > 10 5 , S S-th = 63 mV dec -1 , µ h = 0.04 cm 2 V -1 s -1 ) are integrated on the same substrate in order to obtain high-performance hybrid inverters. The inverters operate in the sub-1 V range (0.9 V) and have high gain (76 V/V), large maximum-equal-criteria noise margins (80%), and peak power consumption of 3 nW, in combination with low hysteresis (10 mV). © 2017 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Intermediate-band photosensitive device with quantum dots having tunneling barrier embedded in organic matrix

DOEpatents

Forrest, Stephen R.

2008-08-19

A plurality of quantum dots each have a shell. The quantum dots are embedded in an organic matrix. At least the quantum dots and the organic matrix are photoconductive semiconductors. The shell of each quantum dot is arranged as a tunneling barrier to require a charge carrier (an electron or a hole) at a base of the tunneling barrier in the organic matrix to perform quantum mechanical tunneling to reach the respective quantum dot. A first quantum state in each quantum dot is between a lowest unoccupied molecular orbital (LUMO) and a highest occupied molecular orbital (HOMO) of the organic matrix. Wave functions of the first quantum state of the plurality of quantum dots may overlap to form an intermediate band.

Design and Synthesis of Antiblinking and Antibleaching Quantum Dots in Multiple Colors via Wave Function Confinement.

PubMed

Cao, Hujia; Ma, Junliang; Huang, Lin; Qin, Haiyan; Meng, Renyang; Li, Yang; Peng, Xiaogang

2016-12-07

Single-molecular spectroscopy reveals that photoluminescence (PL) of a single quantum dot blinks, randomly switching between bright and dim/dark states under constant photoexcitation, and quantum dots photobleach readily. These facts cast great doubts on potential applications of these promising emitters. After ∼20 years of efforts, synthesis of nonblinking quantum dots is still challenging, with nonblinking quantum dots only available in red-emitting window. Here we report synthesis of nonblinking quantum dots covering most part of the visible window using a new synthetic strategy, i.e., confining the excited-state wave functions of the core/shell quantum dots within the core quantum dot and its inner shells (≤ ∼5 monolayers). For the red-emitting ones, the new synthetic strategy yields nonblinking quantum dots with small sizes (∼8 nm in diameter) and improved nonblinking properties. These new nonblinking quantum dots are found to be antibleaching. Results further imply that the PL blinking and photobleaching of quantum dots are likely related to each other.

A non-genetic approach to labelling acute myeloid leukemia and bone marrow cells with quantum dots.

PubMed

Zheng, Yanwen; Tan, Dongming; Chen, Zheng; Hu, Chenxi; Mao, Zhengwei J; Singleton, Timothy P; Zeng, Yan; Shao, Xuejun; Yin, Bin

2014-06-01

The difficulty in manipulation of leukemia cells has long hindered the dissection of leukemia pathogenesis. We have introduced a non-genetic approach of marking blood cells, using quantum dots. We compared quantum dots complexed with different vehicles, including a peptide Tat, cationic polymer Turbofect and liposome. Quantum dots-Tat showed the highest efficiency of marking hematopoietic cells among the three vehicles. Quantum dots-Tat could also label a panel of leukemia cell lines at varied efficiencies. More uniform intracellular distributions of quantum dots in mouse bone marrow and leukemia cells were obtained with quantum dots-Tat, compared with the granule-like formation obtained with quantum dots-liposome. Our results suggest that quantum dots have provided a photostable and non-genetic approach that labels normal and malignant hematopoietic cells, in a cell type-, vehicle-, and quantum dot concentration-dependent manner. We expect for potential applications of quantum dots as an easy and fast marking tool assisting investigations of various types of blood cells in the future.

A modified gradient approach for the growth of low-density InAs quantum dot molecules by molecular beam epitaxy

NASA Astrophysics Data System (ADS)

Sharma, Nandlal; Reuter, Dirk

2017-11-01

Two vertically stacked quantum dots that are electronically coupled, so called quantum dot molecules, are of great interest for the realization of solid state building blocks for quantum communication networks. We present a modified gradient approach to realize InAs quantum dot molecules with a low areal density so that single quantum dot molecules can be optically addressed. The individual quantum dot layers were prepared by solid source molecular beam epitaxy depositing InAs on GaAs(100). The bottom quantum dot layer has been grown without substrate rotation resulting in an In-gradient across the surface, which translated into a density gradient with low quantum dot density in a certain region of the wafer. For the top quantum dot layer, separated from the bottom quantum dot layer by a 6 nm thick GaAs barrier, various InAs amounts were deposited without an In-gradient. In spite of the absence of an In-gradient, a pronounced density gradient is observed for the top quantum dots. Even for an In-amount slightly below the critical thickness for a single dot layer, a density gradient in the top quantum dot layer, which seems to reproduce the density gradient in the bottom layer, is observed. For more or less In, respectively, deviations from this behavior occur. We suggest that the obvious influence of the bottom quantum dot layer on the growth of the top quantum dots is due to the strain field induced by the buried dots.

Single molecule localization imaging of telomeres and centromeres using fluorescence in situ hybridization and semiconductor quantum dots.

PubMed

Wang, Le; Zong, Shenfei; Wang, Zhuyuan; Lu, Ju; Chen, Chen; Zhang, Ruohu; Cui, Yiping

2018-07-13

Single molecule localization microscopy (SMLM) is a powerful tool for imaging biological targets at the nanoscale. In this report, we present SMLM imaging of telomeres and centromeres using fluorescence in situ hybridization (FISH). The FISH probes were fabricated by decorating CdSSe/ZnS quantum dots (QDs) with telomere or centromere complementary DNA strands. SMLM imaging experiments using commercially available peptide nucleic acid (PNA) probes labeled with organic fluorophores were also conducted to demonstrate the advantages of using QDs FISH probes. Compared with the PNA probes, the QDs probes have the following merits. First, the fluorescence blinking of QDs can be realized in aqueous solution or PBS buffer without thiol, which is a key buffer component for organic fluorophores' blinking. Second, fluorescence blinking of the QDs probe needs only one excitation light (i.e. 405 nm). While fluorescence blinking of the organic fluorophores usually requires two illumination lights, that is, the activation light (i.e. 405 nm) and the imaging light. Third, the high quantum yield, multiple switching times and a good optical stability make the QDs more suitable for long-term imaging. The localization precision achieved in telomeres and centromeres imaging experiments is about 30 nm, which is far beyond the diffraction limit. SMLM has enabled new insights into telomeres or centromeres on the molecular level, and it is even possible to determine the length of telomere and become a potential technique for telomere-related investigation.

Single molecule localization imaging of telomeres and centromeres using fluorescence in situ hybridization and semiconductor quantum dots

NASA Astrophysics Data System (ADS)

Wang, Le; Zong, Shenfei; Wang, Zhuyuan; Lu, Ju; Chen, Chen; Zhang, Ruohu; Cui, Yiping

2018-07-01

Single molecule localization microscopy (SMLM) is a powerful tool for imaging biological targets at the nanoscale. In this report, we present SMLM imaging of telomeres and centromeres using fluorescence in situ hybridization (FISH). The FISH probes were fabricated by decorating CdSSe/ZnS quantum dots (QDs) with telomere or centromere complementary DNA strands. SMLM imaging experiments using commercially available peptide nucleic acid (PNA) probes labeled with organic fluorophores were also conducted to demonstrate the advantages of using QDs FISH probes. Compared with the PNA probes, the QDs probes have the following merits. First, the fluorescence blinking of QDs can be realized in aqueous solution or PBS buffer without thiol, which is a key buffer component for organic fluorophores’ blinking. Second, fluorescence blinking of the QDs probe needs only one excitation light (i.e. 405 nm). While fluorescence blinking of the organic fluorophores usually requires two illumination lights, that is, the activation light (i.e. 405 nm) and the imaging light. Third, the high quantum yield, multiple switching times and a good optical stability make the QDs more suitable for long-term imaging. The localization precision achieved in telomeres and centromeres imaging experiments is about 30 nm, which is far beyond the diffraction limit. SMLM has enabled new insights into telomeres or centromeres on the molecular level, and it is even possible to determine the length of telomere and become a potential technique for telomere-related investigation.

Interaction of Water-Soluble CdTe Quantum Dots with Bovine Serum Albumin

PubMed Central

2011-01-01

Semiconductor nanoparticles (quantum dots) are promising fluorescent markers, but it is very little known about interaction of quantum dots with biological molecules. In this study, interaction of CdTe quantum dots coated with thioglycolic acid (TGA) with bovine serum albumin was investigated. Steady state spectroscopy, atomic force microscopy, electron microscopy and dynamic light scattering methods were used. It was explored how bovine serum albumin affects stability and spectral properties of quantum dots in aqueous media. CdTe–TGA quantum dots in aqueous solution appeared to be not stable and precipitated. Interaction with bovine serum albumin significantly enhanced stability and photoluminescence quantum yield of quantum dots and prevented quantum dots from aggregating. PMID:27502633

Non-Markovian full counting statistics in quantum dot molecules

PubMed Central

Xue, Hai-Bin; Jiao, Hu-Jun; Liang, Jiu-Qing; Liu, Wu-Ming

2015-01-01

Full counting statistics of electron transport is a powerful diagnostic tool for probing the nature of quantum transport beyond what is obtainable from the average current or conductance measurement alone. In particular, the non-Markovian dynamics of quantum dot molecule plays an important role in the nonequilibrium electron tunneling processes. It is thus necessary to understand the non-Markovian full counting statistics in a quantum dot molecule. Here we study the non-Markovian full counting statistics in two typical quantum dot molecules, namely, serially coupled and side-coupled double quantum dots with high quantum coherence in a certain parameter regime. We demonstrate that the non-Markovian effect manifests itself through the quantum coherence of the quantum dot molecule system, and has a significant impact on the full counting statistics in the high quantum-coherent quantum dot molecule system, which depends on the coupling of the quantum dot molecule system with the source and drain electrodes. The results indicated that the influence of the non-Markovian effect on the full counting statistics of electron transport, which should be considered in a high quantum-coherent quantum dot molecule system, can provide a better understanding of electron transport through quantum dot molecules. PMID:25752245

Quantum Confined Semiconductors for High Efficiency Photovoltaics

NASA Astrophysics Data System (ADS)

Beard, Matthew

2014-03-01

Semiconductor nanostructures, where at least one dimension is small enough to produce quantum confinement effects, provide new pathways for controlling energy flow and therefore have the potential to increase the efficiency of the primary photon-to-free energy conversion step. In this discussion, I will present the current status of research efforts towards utilizing the unique properties of colloidal quantum dots (NCs confined in three dimensions) in prototype solar cells and demonstrate that these unique systems have the potential to bypass the Shockley-Queisser single-junction limit for solar photon conversion. The solar cells are constructed using a low temperature solution based deposition of PbS or PbSe QDs as the absorber layer. Different chemical treatments of the QD layer are employed in order to obtain good electrical communication while maintaining the quantum-confined properties of the QDs. We have characterized the transport and carrier dynamics using a transient absorption, time-resolved THz, and temperature-dependent photoluminescence. I will discuss the interplay between carrier generation, recombination, and mobility within the QD layers. A unique aspect of our devices is that the QDs exhibit multiple exciton generation with an efficiency that is ~ 2 to 3 times greater than the parental bulk semiconductor.

Synthesis and characterization of ZnO/ZnSe NWs/PbS QDs solar cell

NASA Astrophysics Data System (ADS)

Kamruzzaman, M.; Zapien, J. A.

2017-04-01

The capture of solar energy has gained the attention for the next generation solar cell. ZnO/ZnSe NW arrays were synthesized on an FTO glass substrate using a simple and facile hydrothermal and ion-exchange approaches. The lead sulfide (PbS) QDs was infiltrated into ZnO/ZnSe NWs via SILAR method for making inorganic quantum dot sensitized ZnO/ZnSe/PbS QDs solar cell. The surface morphology, structural, optical, and J-V characteristics have been investigated. The ZnO/ZnSe NW is a core-shell like structure, and the absorption edge shifted from the UV region (ZnO NWs) to the near infrared region for ZnO/ZnSe NWs/PbS QDs. For PbS QDs-sensitized solar cell, the obtained value of η = 1.1%, J sc = 20.60 mA/cm2, V oc = 155 mV, and FF = 34.7%, respectively. The photovoltaic performance of the device in this study is still inferior. However, it is the first report regarding to ZnO/ZnZe NWs/PbS QDs solar cell. The achieving high absorption and large short circuit current density may interest in further improvement of the device performance by suppressing surface defects, optimizing the quality of ZnO/ZnSe NWs and PbS QDs.

The impact of quantum dot filling on dual-band optical transitions via intermediate quantum states

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Jiang, E-mail: jiang.wu@ucl.ac.uk; Passmore, Brandon; Manasreh, M. O.

2015-08-28

InAs/GaAs quantum dot infrared photodetectors with different doping levels were investigated to understand the effect of quantum dot filling on both intraband and interband optical transitions. The electron filling of self-assembled InAs quantum dots was varied by direct doping of quantum dots with different concentrations. Photoresponse in the near infrared and middle wavelength infrared spectral region was observed from samples with low quantum dot filling. Although undoped quantum dots were favored for interband transitions with the absence of a second optical excitation in the near infrared region, doped quantum dots were preferred to improve intraband transitions in the middle wavelengthmore » infrared region. As a result, partial filling of quantum dot was required, to the extent of maintaining a low dark current, to enhance the dual-band photoresponse through the confined electron states.« less

Origins and optimization of entanglement in plasmonically coupled quantum dots

DOE PAGES

Otten, Matthew; Larson, Jeffrey; Min, Misun; ...

2016-08-11

In this paper, a system of two or more quantum dots interacting with a dissipative plasmonic nanostructure is investigated in detail by using a cavity quantum electrodynamics approach with a model Hamiltonian. We focus on determining and understanding system configurations that generate multiple bipartite quantum entanglements between the occupation states of the quantum dots. These configurations include allowing for the quantum dots to be asymmetrically coupled to the plasmonic system. Analytical solution of a simplified limit for an arbitrary number of quantum dots and numerical simulations and optimization for the two- and three-dot cases are used to develop guidelines formore » maximizing the bipartite entanglements. For any number of quantum dots, we show that through simple starting states and parameter guidelines, one quantum dot can be made to share a strong amount of bipartite entanglement with all other quantum dots in the system, while entangling all other pairs to a lesser degree.« less

Photovoltaic Performance of a Nanowire/Quantum Dot Hybrid Nanostructure Array Solar Cell.

PubMed

Wu, Yao; Yan, Xin; Zhang, Xia; Ren, Xiaomin

2018-02-23

An innovative solar cell based on a nanowire/quantum dot hybrid nanostructure array is designed and analyzed. By growing multilayer InAs quantum dots on the sidewalls of GaAs nanowires, not only the absorption spectrum of GaAs nanowires is extended by quantum dots but also the light absorption of quantum dots is dramatically enhanced due to the light-trapping effect of the nanowire array. By incorporating five layers of InAs quantum dots into a 500-nm high-GaAs nanowire array, the power conversion efficiency enhancement induced by the quantum dots is six times higher than the power conversion efficiency enhancement in thin-film solar cells which contain the same amount of quantum dots, indicating that the nanowire array structure can benefit the photovoltaic performance of quantum dot solar cells.

Photovoltaic Performance of a Nanowire/Quantum Dot Hybrid Nanostructure Array Solar Cell

NASA Astrophysics Data System (ADS)

Wu, Yao; Yan, Xin; Zhang, Xia; Ren, Xiaomin

2018-02-01

An innovative solar cell based on a nanowire/quantum dot hybrid nanostructure array is designed and analyzed. By growing multilayer InAs quantum dots on the sidewalls of GaAs nanowires, not only the absorption spectrum of GaAs nanowires is extended by quantum dots but also the light absorption of quantum dots is dramatically enhanced due to the light-trapping effect of the nanowire array. By incorporating five layers of InAs quantum dots into a 500-nm high-GaAs nanowire array, the power conversion efficiency enhancement induced by the quantum dots is six times higher than the power conversion efficiency enhancement in thin-film solar cells which contain the same amount of quantum dots, indicating that the nanowire array structure can benefit the photovoltaic performance of quantum dot solar cells.

Combined atomic force microscopy and photoluminescence imaging to select single InAs/GaAs quantum dots for quantum photonic devices.

PubMed

Sapienza, Luca; Liu, Jin; Song, Jin Dong; Fält, Stefan; Wegscheider, Werner; Badolato, Antonio; Srinivasan, Kartik

2017-07-24

We report on a combined photoluminescence imaging and atomic force microscopy study of single, isolated self-assembled InAs quantum dots. The motivation of this work is to determine an approach that allows to assess single quantum dots as candidates for quantum nanophotonic devices. By combining optical and scanning probe characterization techniques, we find that single quantum dots often appear in the vicinity of comparatively large topographic features. Despite this, the quantum dots generally do not exhibit significant differences in their non-resonantly pumped emission spectra in comparison to quantum dots appearing in defect-free regions, and this behavior is observed across multiple wafers produced in different growth chambers. Such large surface features are nevertheless a detriment to applications in which single quantum dots are embedded within nanofabricated photonic devices: they are likely to cause large spectral shifts in the wavelength of cavity modes designed to resonantly enhance the quantum dot emission, thereby resulting in a nominally perfectly-fabricated single quantum dot device failing to behave in accordance with design. We anticipate that the approach of screening quantum dots not only based on their optical properties, but also their surrounding surface topographies, will be necessary to improve the yield of single quantum dot nanophotonic devices.

Effect of organic materials used in the synthesis on the emission from CdSe quantum dots

NASA Astrophysics Data System (ADS)

Lee, Jae-Won; Yang, Ho-Soon; Hong, K. S.; Kim, S. M.

2013-12-01

Quantum-dot nanocrystals have particular optical properties due to the quantum confinement effect and the surface effect. This study focuses on the effect of surface conditions on the emission from quantum dots. The quantum dots prepared with 1-hexadecylamine (HDA) in the synthesis show strong emission while the quantum dots prepared without HDA show weak emission, as well as emission from surface energy traps. The comparison of the X-ray patterns of these two sets of quantum dots reveals that HDA forms a layer on the surface of quantum dot during the synthesis. This surface passivation with a layer of HDA reduces surface energy traps, therefore the emission from surface trap levels is suppressed in the quantum dots synthesized with HDA.

Energy structure and radiative lifetimes of InxGa1-xN /AlN quantum dots

NASA Astrophysics Data System (ADS)

Aleksandrov, Ivan A.; Zhuravlev, Konstantin S.

2018-01-01

We report calculations of the ground state transition energies and the radiative lifetimes in InxGa1-xN /AlN quantum dots with different size and indium content. The ground state transition energy and the radiative lifetime of the InxGa1-xN /AlN quantum dots can be varied over a wide range by changing the height of the quantum dot and the indium content. The sizes and compositions for quantum dots emitting in the wavelength range for fiber-optic telecommunications have been found. The radiative lifetime of the InxGa1-xN /AlN quantum dots increases with increase in quantum dot height at a constant indium content, and increases with increase in indium content at constant quantum dot height. For quantum dots with constant ground state transition energy the radiative lifetime decreases with increase in indium content.

Quantum dot-polymer conjugates for stable luminescent displays.

PubMed

Ghimire, Sushant; Sivadas, Anjaly; Yuyama, Ken-Ichi; Takano, Yuta; Francis, Raju; Biju, Vasudevanpillai

2018-05-23

The broad absorption of light in the UV-Vis-NIR region and the size-based tunable photoluminescence color of semiconductor quantum dots make these tiny crystals one of the most attractive antennae in solar cells and phosphors in electrooptical devices. One of the primary requirements for such real-world applications of quantum dots is their stable and uniform distribution in optically transparent matrices. In this work, we prepare transparent thin films of polymer-quantum dot conjugates, where CdSe/ZnS quantum dots are uniformly distributed at high densities in a chitosan-polystyrene copolymer (CS-g-PS) matrix. Here, quantum dots in an aqueous solution are conjugated to the copolymer by a phase transfer reaction. With the stable conjugation of quantum dots to the copolymer, we prevent undesired phase separation between the two and aggregation of quantum dots. Furthermore, the conjugate allows us to prepare transparent thin films in which quantum dots are uniformly distributed at high densities. The CS-g-PS copolymer helps us in not only preserving the photoluminescence properties of quantum dots in the film but also rendering excellent photostability to quantum dots at the ensemble and single particle levels, making the conjugate a promising material for photoluminescence-based devices.

Origins of low energy-transfer efficiency between patterned GaN quantum well and CdSe quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Xingsheng, E-mail: xsxu@semi.ac.cn

For hybrid light emitting devices (LEDs) consisting of GaN quantum wells and colloidal quantum dots, it is necessary to explore the physical mechanisms causing decreases in the quantum efficiencies and the energy transfer efficiency between a GaN quantum well and CdSe quantum dots. This study investigated the electro-luminescence for a hybrid LED consisting of colloidal quantum dots and a GaN quantum well patterned with photonic crystals. It was found that both the quantum efficiency of colloidal quantum dots on a GaN quantum well and the energy transfer efficiency between the patterned GaN quantum well and the colloidal quantum dots decreasedmore » with increases in the driving voltage or the driving time. Under high driving voltages, the decreases in the quantum efficiency of the colloidal quantum dots and the energy transfer efficiency can be attributed to Auger recombination, while those decreases under long driving time are due to photo-bleaching and Auger recombination.« less

[Effect of quantum dots CdSe/ZnS's concentration on its fluorescence].

PubMed

Jin, Min; Huang, Yu-hua; Luo, Ji-xiang

2015-02-01

The authors measured the absorption and the fluorescence spectra of the quantum dots CdSe/ZnS with 4 nm in size at different concentration with the use of the UV-Vis absorption spectroscopy and fluorescence spectrometer. The effect of quantum dots CdSe/ZnS's concentration on its fluorescence was especially studied and its physical mechanism was analyzed. It was observed that the optimal concentration of the quantum dots CdSe/ZnS for fluorescence is 2 micromole x L(-1). When the quantum dot's concentration is over 2 micromol x L(-1), the fluorescence is decreased with the increase in the concentration. While the quantum dot's concentration is less than 2 micromol x L(-1), the fluorescence is decreased with the decrease in the concentration. There are two main reasons: (1) fluorescence quenching and 2) the competition between absorption and fluorescence. When the quantum dot's concentration is over 2 micromol x L(-1), the distance between quantum dots is so close that the fluorescence quenching is induced. The closer the distance between quantum dots is, the more serious the fluorescence quenching is induced. Also, in this case, the absorption is so large that some of the quantum dots can not be excited because the incident light can not pass through the whole sample. As a result, the fluorescence is decreased with the increase in the quantum dot's concentration. As the quantum dot's concentration is below 2 micromol x L(-1), the distance between quantum dots is far enough that no more fluorescence quenching is induced. In this case, the fluorescence is determined by the particle number per unit volume. More particle number per unit volume produces more fluorescence. Therefore, the fluorescence is decreased with the decrease in the quantum dot's concentration.

Determining the exact number of dye molecules attached to colloidal CdSe/ZnS quantum dots in Förster resonant energy transfer assemblies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kaiser, Uwe; Jimenez de Aberasturi, Dorleta; Vázquez-González, Margarita

2015-01-14

Semiconductor quantum dots functionalized with organic dye molecules are important tools for biological sensor applications. Energy transfer between the quantum dot and the attached dyes can be utilized for sensing. Though important, the determination of the real number of dye molecules attached per quantum dot is rather difficult. In this work, a method will be presented to determine the number of ATTO-590 dye molecules attached to CdSe/ZnS quantum dots based on time resolved spectral analysis. The energy transfer from the excited quantum dot to the attached ATTO-590 dye leads to a reduced lifetime of the quantum dot's excitons. The highermore » the concentration of dye molecules, the shorter the excitonic lifetime becomes. However, the number of dye molecules attached per quantum dot will vary. Therefore, for correctly explaining the decay of the luminescence upon photoexcitation of the quantum dot, it is necessary to take into account the distribution of the number of dyes attached per quantum dot. A Poisson distribution of the ATTO-590 dye molecules not only leads to excellent agreement between experimental and theoretical decay curves but also additionally yields the average number of dye molecules attached per quantum dot. In this way, the number of dyes per quantum dot can be conveniently determined.« less

Elimination of Bimodal Size in InAs/GaAs Quantum Dots for Preparation of 1.3-μm Quantum Dot Lasers

NASA Astrophysics Data System (ADS)

Su, Xiang-Bin; Ding, Ying; Ma, Ben; Zhang, Ke-Lu; Chen, Ze-Sheng; Li, Jing-Lun; Cui, Xiao-Ran; Xu, Ying-Qiang; Ni, Hai-Qiao; Niu, Zhi-Chuan

2018-02-01

The device characteristics of semiconductor quantum dot lasers have been improved with progress in active layer structures. Self-assembly formed InAs quantum dots grown on GaAs had been intensively promoted in order to achieve quantum dot lasers with superior device performances. In the process of growing high-density InAs/GaAs quantum dots, bimodal size occurs due to large mismatch and other factors. The bimodal size in the InAs/GaAs quantum dot system is eliminated by the method of high-temperature annealing and optimized the in situ annealing temperature. The annealing temperature is taken as the key optimization parameters, and the optimal annealing temperature of 680 °C was obtained. In this process, quantum dot growth temperature, InAs deposition, and arsenic (As) pressure are optimized to improve quantum dot quality and emission wavelength. A 1.3-μm high-performance F-P quantum dot laser with a threshold current density of 110 A/cm2 was demonstrated.

Elimination of Bimodal Size in InAs/GaAs Quantum Dots for Preparation of 1.3-μm Quantum Dot Lasers.

PubMed

Su, Xiang-Bin; Ding, Ying; Ma, Ben; Zhang, Ke-Lu; Chen, Ze-Sheng; Li, Jing-Lun; Cui, Xiao-Ran; Xu, Ying-Qiang; Ni, Hai-Qiao; Niu, Zhi-Chuan

2018-02-21

The device characteristics of semiconductor quantum dot lasers have been improved with progress in active layer structures. Self-assembly formed InAs quantum dots grown on GaAs had been intensively promoted in order to achieve quantum dot lasers with superior device performances. In the process of growing high-density InAs/GaAs quantum dots, bimodal size occurs due to large mismatch and other factors. The bimodal size in the InAs/GaAs quantum dot system is eliminated by the method of high-temperature annealing and optimized the in situ annealing temperature. The annealing temperature is taken as the key optimization parameters, and the optimal annealing temperature of 680 °C was obtained. In this process, quantum dot growth temperature, InAs deposition, and arsenic (As) pressure are optimized to improve quantum dot quality and emission wavelength. A 1.3-μm high-performance F-P quantum dot laser with a threshold current density of 110 A/cm 2 was demonstrated.

Peptide-Decorated Tunable-Fluorescence Graphene Quantum Dots.

PubMed

Sapkota, Bedanga; Benabbas, Abdelkrim; Lin, Hao-Yu Greg; Liang, Wentao; Champion, Paul; Wanunu, Meni

2017-03-22

We report here the synthesis of graphene quantum dots with tunable size, surface chemistry, and fluorescence properties. In the size regime 15-35 nm, these quantum dots maintain strong visible light fluorescence (mean quantum yield of 0.64) and a high two-photon absorption (TPA) cross section (6500 Göppert-Mayer units). Furthermore, through noncovalent tailoring of the chemistry of these quantum dots, we obtain water-stable quantum dots. For example, quantum dots with lysine groups bind strongly to DNA in solution and inhibit polymerase-based DNA strand synthesis. Finally, by virtue of their mesoscopic size, the quantum dots exhibit good cell permeability into living epithelial cells, but they do not enter the cell nucleus.

Intracellular distribution of nontargeted quantum dots after natural uptake and microinjection

PubMed Central

Damalakiene, Leona; Karabanovas, Vitalijus; Bagdonas, Saulius; Valius, Mindaugas; Rotomskis, Ricardas

2013-01-01

Background: The purpose of this study was to elucidate the mechanism of natural uptake of nonfunctionalized quantum dots in comparison with microinjected quantum dots by focusing on their time-dependent accumulation and intracellular localization in different cell lines. Methods: The accumulation dynamics of nontargeted CdSe/ZnS carboxyl-coated quantum dots (emission peak 625 nm) was analyzed in NIH3T3, MCF-7, and HepG2 cells by applying the methods of confocal and steady-state fluorescence spectroscopy. Intracellular colocalization of the quantum dots was investigated by staining with Lysotracker®. Results: The uptake of quantum dots into cells was dramatically reduced at a low temperature (4°C), indicating that the process is energy-dependent. The uptake kinetics and imaging of intracellular localization of quantum dots revealed three accumulation stages of carboxyl-coated quantum dots at 37°C, ie, a plateau stage, growth stage, and a saturation stage, which comprised four morphological phases: adherence to the cell membrane; formation of granulated clusters spread throughout the cytoplasm; localization of granulated clusters in the perinuclear region; and formation of multivesicular body-like structures and their redistribution in the cytoplasm. Diverse quantum dots containing intracellular vesicles in the range of approximately 0.5–8 μm in diameter were observed in the cytoplasm, but none were found in the nucleus. Vesicles containing quantum dots formed multivesicular body-like structures in NIH3T3 cells after 24 hours of incubation, which were Lysotracker-negative in serum-free medium and Lysotracker-positive in complete medium. The microinjected quantum dots remained uniformly distributed in the cytosol for at least 24 hours. Conclusion: Natural uptake of quantum dots in cells occurs through three accumulation stages via a mechanism requiring energy. The sharp contrast of the intracellular distribution after microinjection of quantum dots in comparison with incubation as well as the limited transfer of quantum dots from vesicles into the cytosol and vice versa support the endocytotic origin of the natural uptake of quantum dots. Quantum dots with proteins adsorbed from the culture medium had a different fate in the final stage of accumulation from that of the protein-free quantum dots, implying different internalization pathways. PMID:23429995

Templated self-assembly of quantum dots from aqueous solution using protein scaffolds

NASA Astrophysics Data System (ADS)

Szuchmacher Blum, Amy; Soto, Carissa M.; Wilson, Charmaine D.; Whitley, Jessica L.; Moore, Martin H.; Sapsford, Kim E.; Lin, Tianwei; Chatterji, Anju; Johnson, John E.; Ratna, Banahalli R.

2006-10-01

Short, histidine-containing peptides can be conjugated to lysine-containing protein scaffolds to controllably attach quantum dots (QDs) to the scaffold, allowing for generic attachment of quantum dots to any protein without the use of specially engineered domains. This technique was used to bind quantum dots from aqueous solution to both chicken IgG and cowpea mosaic virus (CPMV), a 30 nm viral particle. These quantum dot protein assemblies were studied in detail. The IgG QD complexes were shown to retain binding specificity to their antigen after modification. The CPMV QD complexes have a local concentration of quantum dots greater than 3000 nmol ml-1, and show a 15% increase in fluorescence quantum yield over free quantum dots in solution.

On the advancement of quantum dot solar cell performance through enhanced charge carrier dynamics

NASA Astrophysics Data System (ADS)

Baker, David R.

The quantum dot solar cell is one of the few solar technologies which promises to compete with fossil fuels, but work is still needed to increase its performance. Electron transfer kinetics at interfaces and limitations of the redox couple within the cell, are responsible for lowering power conversion efficiency. Several techniques which are able to increase electron transfer within the working electrode and at the counter electrode/electrolyte interface are discussed in this dissertation. Trap sites on the surface of CdSe quantum dots are created when mercaptopropionic acid (MPA) is added to the suspension. The trap sites are emissive creating a loss pathway for photogenerated charges which will manifest as reduced photocurrent. MPA displaces amines on the surface of CdSe creating Se vacancies. Emission properties are controlled by the concentration of MPA. Because trap sites are generated, a more successful method to sensitize TiO2 films is the SILAR technique which directly grows quantum dots on the desired surface. Anodically etched TiO2 nanotubes yield photocurrents 20% greater than TiO2 nanoparticles because of longer electron diffusion lengths. Peak incident photon to charge carrier efficiencies of TiO2 nanotube samples show a doubling of photocurrent in the visible region compared to nanoparticles. The TiO2 substrates are sensitized with CdS by the SILAR process which is found to utilize both the inside and outside surfaces of the TiO2 nanotubes. Etched TiO2 nanotubes are removed from the underlying titanium foil in order to use spectroscopic techniques. Ultrafast transient absorption shows the extremely fast nature of charge injection from SILAR CdS into TiO 2 nanotubes. Surface area analysis of TiO2 nanotube powder gives an area of 77m2/g, a value 1.5 times larger than traditional TiO2 nanoparticles. By isolating the counter electrode with a salt bridge the effect of the polysulfide electrolyte is found to act as an electron scavenger on the working electrode. Though activity at the platinum counter electrode increases with the presence of polysulfides, the activity is too low to counteract scavenging at the working electrode. Cu2S, CoS and PbS electrochemically show promise as alternatives to platinum. Cu2S and CoS produce higher photocurrents and fill factors, greatly improving cell performance.

Atomistic theory of excitonic fine structure in InAs/InP nanowire quantum dot molecules

NASA Astrophysics Data System (ADS)

Świderski, M.; Zieliński, M.

2017-03-01

Nanowire quantum dots have peculiar electronic and optical properties. In this work we use atomistic tight binding to study excitonic spectra of artificial molecules formed by a double nanowire quantum dot. We demonstrate a key role of atomistic symmetry and nanowire substrate orientation rather than cylindrical shape symmetry of a nanowire and a molecule. In particular for [001 ] nanowire orientation we observe a nonvanishing bright exciton splitting for a quasimolecule formed by two cylindrical quantum dots of different heights. This effect is due to interdot coupling that effectively reduces the overall symmetry, whereas single uncoupled [001 ] quantum dots have zero fine structure splitting. We found that the same double quantum dot system grown on [111 ] nanowire reveals no excitonic fine structure for all considered quantum dot distances and individual quantum dot heights. Further we demonstrate a pronounced, by several orders of magnitude, increase of the dark exciton optical activity in a quantum dot molecule as compared to a single quantum dot. For [111 ] systems we also show spontaneous localization of single particle states in one of nominally identical quantum dots forming a molecule, which is mediated by strain and origins from the lack of the vertical inversion symmetry in [111 ] nanostructures of overall C3 v symmetry. Finally, we study lowering of symmetry due to alloy randomness that triggers nonzero excitonic fine structure and the dark exciton optical activity in realistic nanowire quantum dot molecules of intermixed composition.

Photon-assisted tunneling in an asymmetrically coupled triple quantum dot

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Bao-Chuan; Cao, Gang, E-mail: gcao@ustc.edu.cn; Chen, Bao-Bao

The gate-defined quantum dot is regarded as one of the basic structures required for scalable semiconductor quantum processors. Here, we demonstrate a structure that contains three quantum dots scaled in series. The electron number of each dot and the tunnel coupling between them can be tuned conveniently using splitting gates. We tune the quantum dot array asymmetrically such that the tunnel coupling between the right dot and the central dot is much larger than that between the left dot and the central dot. When driven by microwaves, the sidebands of the photon-assisted tunneling process appear not only in the left-to-centralmore » dot transition region but also in the left-to-right dot transition region. These sidebands are both attributed to the left-to-central transition for asymmetric coupling. Our result shows that there is a region of a triple quantum dot structure that remains indistinct when studied with a normal two-dimensional charge stability diagram; this will be helpful in future studies of the scalability of quantum dot systems.« less

Mid-Infrared Quantum-Dot Quantum Cascade Laser: A Theoretical Feasibility Study

DOE PAGES

Michael, Stephan; Chow, Weng; Schneider, Hans

2016-05-01

In the framework of a microscopic model for intersubband gain from electrically pumped quantum-dot structures we investigate electrically pumped quantum-dots as active material for a mid-infrared quantum cascade laser. Our previous calculations have indicated that these structures could operate with reduced threshold current densities while also achieving a modal gain comparable to that of quantum well active materials. We study the influence of two important quantum-dot material parameters, here, namely inhomogeneous broadening and quantum-dot sheet density, on the performance of a proposed quantum cascade laser design. In terms of achieving a positive modal net gain, a high quantum-dot density canmore » compensate for moderately high inhomogeneous broadening, but at a cost of increased threshold current density. By minimizing quantum-dot density with presently achievable inhomogeneous broadening and total losses, significantly lower threshold densities than those reported in quantum-well quantum-cascade lasers are predicted by our theory.« less

Chemical nature and structure of organic coating of quantum dots is crucial for their application in imaging diagnostics

PubMed Central

Bakalova, Rumiana; Zhelev, Zhivko; Kokuryo, Daisuke; Spasov, Lubomir; Aoki, Ichio; Saga, Tsuneo

2011-01-01

Background: One of the most attractive properties of quantum dots is their potential to extend the opportunities for fluorescent and multimodal imaging in vivo. The aim of the present study was to clarify whether the composition and structure of organic coating of nanoparticles are crucial for their application in vivo. Methods: We compared quantum dots coated with non-crosslinked amino-functionalized polyamidoamine (PAMAM) dendrimers, quantum dots encapsulated in crosslinked carboxyl-functionalized PAMAM dendrimers, and silica-shelled amino-functionalized quantum dots. A multimodal fluorescent and paramagnetic quantum dot probe was also developed and analyzed. The probes were applied intravenously in anesthetized animals for visualization of brain vasculature using two-photon excited fluorescent microscopy and visualization of tumors using fluorescent IVIS® imaging (Caliper Life Sciences, Hopkinton, MA) and magnetic resonance imaging. Results: Quantum dots coated with non-crosslinked dendrimers were cytotoxic. They induced side effects in vivo, including vasodilatation with a decrease in mean arterial blood pressure and heart rate. The quantum dots penetrated the vessels, which caused the quality of fluorescent imaging to deteriorate. Quantum dots encapsulated in crosslinked dendrimers had low cytotoxicity and were biocompatible. In concentrations <0.3 nmol quantum dots/kg bodyweight, these nanoparticles did not affect blood pressure and heart rate, and did not induce vasodilatation or vasoconstriction. PEGylation (PEG [polyethylene glycol]) was an indispensable step in development of a quantum dot probe for in vivo imaging, based on silica-shelled quantum dots. The non-PEGylated silica-shelled quantum dots possessed low colloidal stability in high-salt physiological fluids, accompanied by rapid aggregation in vivo. The conjugation of silica-shelled quantum dots with PEG1100 increased their stability and half-life in the circulation without significant enhancement of their size. In concentrations <2.5 nmol/kg bodyweight, these quantum dots did not affect the main physiological variables. It was possible to visualize capillaries, which makes this quantum dot probe appropriate for investigation of mediators of vasoconstriction, vasodilatation, and brain circulation in intact animals in vivo. The multimodal silica-shelled quantum dots allowed visualization of tumor tissue in an early stage of its development, using magnetic resonance imaging. Conclusion: The present study shows that the type and structure of organic/bioorganic shells of quantum dots determine their biocompatibility and are crucial for their application in imaging in vivo, due to the effects of the shell on the following properties: colloidal stability, solubility in physiological fluids, influence of the basic physiological parameters, and cytotoxicity. PMID:21980235

A reconfigurable gate architecture for Si/SiGe quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zajac, D. M.; Hazard, T. M.; Mi, X.

2015-06-01

We demonstrate a reconfigurable quantum dot gate architecture that incorporates two interchangeable transport channels. One channel is used to form quantum dots, and the other is used for charge sensing. The quantum dot transport channel can support either a single or a double quantum dot. We demonstrate few-electron occupation in a single quantum dot and extract charging energies as large as 6.6 meV. Magnetospectroscopy is used to measure valley splittings in the range of 35–70 μeV. By energizing two additional gates, we form a few-electron double quantum dot and demonstrate tunable tunnel coupling at the (1,0) to (0,1) interdot charge transition.

Reducing inhomogeneity in the dynamic properties of quantum dots via self-aligned plasmonic cavities

NASA Astrophysics Data System (ADS)

Demory, Brandon; Hill, Tyler A.; Teng, Chu-Hsiang; Deng, Hui; Ku, P. C.

2018-01-01

A plasmonic cavity is shown to greatly reduce the inhomogeneity of dynamic optical properties such as quantum efficiency and radiative lifetime of InGaN quantum dots. By using an open-top plasmonic cavity structure, which exhibits a large Purcell factor and antenna quantum efficiency, the resulting quantum efficiency distribution for the quantum dots narrows and is no longer limited by the quantum dot inhomogeneity. The standard deviation of the quantum efficiency can be reduced to 2% while maintaining the overall quantum efficiency at 70%, making InGaN quantum dots a viable candidate for high-speed quantum cryptography and random number generation applications.

Reducing inhomogeneity in the dynamic properties of quantum dots via self-aligned plasmonic cavities.

PubMed

Demory, Brandon; Hill, Tyler A; Teng, Chu-Hsiang; Deng, Hui; Ku, P C

2018-01-05

A plasmonic cavity is shown to greatly reduce the inhomogeneity of dynamic optical properties such as quantum efficiency and radiative lifetime of InGaN quantum dots. By using an open-top plasmonic cavity structure, which exhibits a large Purcell factor and antenna quantum efficiency, the resulting quantum efficiency distribution for the quantum dots narrows and is no longer limited by the quantum dot inhomogeneity. The standard deviation of the quantum efficiency can be reduced to 2% while maintaining the overall quantum efficiency at 70%, making InGaN quantum dots a viable candidate for high-speed quantum cryptography and random number generation applications.

Imaging and Manipulating Energy Transfer Among Quantum Dots at Individual Dot Resolution.

PubMed

Nguyen, Duc; Nguyen, Huy A; Lyding, Joseph W; Gruebele, Martin

2017-06-27

Many processes of interest in quantum dots involve charge or energy transfer from one dot to another. Energy transfer in films of quantum dots as well as between linked quantum dots has been demonstrated by luminescence shift, and the ultrafast time-dependence of energy transfer processes has been resolved. Bandgap variation among dots (energy disorder) and dot separation are known to play an important role in how energy diffuses. Thus, it would be very useful if energy transfer could be visualized directly on a dot-by-dot basis among small clusters or within films of quantum dots. To that effect, we report single molecule optical absorption detected by scanning tunneling microscopy (SMA-STM) to image energy pooling from donor into acceptor dots on a dot-by-dot basis. We show that we can manipulate groups of quantum dots by pruning away the dominant acceptor dot, and switching the energy transfer path to a different acceptor dot. Our experimental data agrees well with a simple Monte Carlo lattice model of energy transfer, similar to models in the literature, in which excitation energy is transferred preferentially from dots with a larger bandgap to dots with a smaller bandgap.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baart, T. A.; Vandersypen, L. M. K.; Kavli Institute of Nanoscience, Delft University of Technology, P.O. Box 5046, 2600 GA Delft

We report the computer-automated tuning of gate-defined semiconductor double quantum dots in GaAs heterostructures. We benchmark the algorithm by creating three double quantum dots inside a linear array of four quantum dots. The algorithm sets the correct gate voltages for all the gates to tune the double quantum dots into the single-electron regime. The algorithm only requires (1) prior knowledge of the gate design and (2) the pinch-off value of the single gate T that is shared by all the quantum dots. This work significantly alleviates the user effort required to tune multiple quantum dot devices.

Quantum Dots and Their Multimodal Applications: A Review

PubMed Central

Bera, Debasis; Qian, Lei; Tseng, Teng-Kuan; Holloway, Paul H.

2010-01-01

Semiconducting quantum dots, whose particle sizes are in the nanometer range, have very unusual properties. The quantum dots have band gaps that depend in a complicated fashion upon a number of factors, described in the article. Processing-structure-properties-performance relationships are reviewed for compound semiconducting quantum dots. Various methods for synthesizing these quantum dots are discussed, as well as their resulting properties. Quantum states and confinement of their excitons may shift their optical absorption and emission energies. Such effects are important for tuning their luminescence stimulated by photons (photoluminescence) or electric field (electroluminescence). In this article, decoupling of quantum effects on excitation and emission are described, along with the use of quantum dots as sensitizers in phosphors. In addition, we reviewed the multimodal applications of quantum dots, including in electroluminescence device, solar cell and biological imaging.

Interactions between N-acetyl-L-cysteine protected CdTe quantum dots and doxorubicin through spectroscopic method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Xiupei, E-mail: xiupeiyang@163.com; College of Chemistry and Chemical Engineering, China West Normal University, Nanchong 637000; Lin, Jia

2015-06-15

Highlights: • CdTe quantum dots with the diameter of 3–5 nm were synthesized in aqueous solution. • The modified CdTe quantum dots showed well fluorescence properties. • The interaction between the CdTe quantum dots and doxorubicin (DR) was investigated. - Abstract: N-acetyl-L-cysteine protected cadmium telluride quantum dots with a diameter of 3–5 nm were synthesized in aqueous solution. The interaction between N-acetyl-L-cysteine/cadmium telluride quantum dots and doxorubicin was investigated by ultraviolet–visible absorption and fluorescence spectroscopy at physiological conditions (pH 7.2, 37 °C). The results indicate that electron transfer has occurred between N-acetyl-L-cysteine/cadmium telluride quantum dots and doxorubicin under light illumination.more » The quantum dots react readily with doxorubicin to form a N-acetyl-L-cysteine/cadmium telluride-quantum dots/doxorubicin complex via electrostatic attraction between the −NH{sub 3}{sup +} moiety of doxorubicin and the −COO{sup −} moiety of N-acetyl-L-cysteine/cadmium telluride quantum dots. The interaction of N-acetyl-L-cysteine/cadmium telluride-quantum dots/doxorubicin complex with bovine serum albumin was studied as well, showing that the complex might induce the conformation change of bovine serum due to changes in microenvironment of bovine serum.« less

Photoluminescence of patterned CdSe quantum dot for anti-counterfeiting label on paper

NASA Astrophysics Data System (ADS)

Isnaeni, Yulianto, Nursidik; Suliyanti, Maria Margaretha

2016-03-01

We successfully developed a method utilizing colloidal CdSe nanocrystalline quantum dot for anti-counterfeiting label on a piece of glossy paper. We deposited numbers and lines patterns of toluene soluble CdSe quantum dot using rubber stamper on a glossy paper. The width of line pattern was about 1-2 mm with 1-2 mm separation between lines. It required less than one minute for deposited CdSe quantum dot on glossy paper to dry and become invisible by naked eyes. However, patterned quantum dot become visible using long-pass filter glasses upon excitation of UV lamp or blue laser. We characterized photoluminescence of line patterns of quantum dot, and we found that emission boundaries of line patterns were clearly observed. The error of line size and shape were mainly due to defect of the original stamper. The emission peak wavelength of CdSe quantum dot was 629 nm. The emission spectrum of deposited quantum dot has full width at half maximum (FWHM) of 30-40 nm. The spectra similarity between deposited quantum dot and the original quantum dot in solution proved that our stamping method can be simply applied on glossy paper without changing basic optical property of the quantum dot. Further development of this technique is potential for anti-counterfeiting label on very important documents or objects.

Synthesis and Characterization of Mercaptoacetic Acid Capped Cadmium Sulphide Quantum Dots.

PubMed

Wageh, S; Maize, Mai; Donia, A M; Al-Ghamdi, Ahmed A; Umar, Ahmad

2015-12-01

This paper reports the facile synthesis and detailed characterization of mercaptoacetic acid capped cadmium sulphide (CdS) quantum dots using various cadmium precursors. The mercaptoacetic acid capped CdS quantum dots were prepared by facile and simple wet chemical method and characterized by several techniques such as energy dispersive spectroscopy (EDS), X-ray diffraction, Fourier transform infrared (FTIR) spectroscopy, UV-vis. spectroscopy, photoluminescence spectroscopy, high-resolution transmission microscopy (HRTEM) and thremogravimetric analysis. The EDS studies revealed that the prepared quantum dots possess higher atomic percentage of sulfur compared to cadmium due to the coordination of thiolate to the quantum dots surfaces. The X-ray and absorption analyses exhibited that the size of quantum dots prepared by cadmium acetate is larger than the quantum dots prepared by cadmium chloride and cadmium nitrate. The increase in size can be attributed to the low stability constant of cadmium acetate in comparison with cadmium chloride and cadmium nitrate. The FTIR and thermogravimetric analysis showed that the nature of capping molecule on the surface of quantum dots are different depending on the cadmium precursors which affect the emission from CdS quantum dots. Photoemission spectroscopy revealed that the emission of quantum dots prepared by cadmium acetate has high intensity band edge emission along with low intensity trapping state emission. However the CdS quantum dots prepared by cadmium chloride and cadmium nitrate produced only trapping state emissions.

Suppression of low-frequency charge noise in gates-defined GaAs quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

You, Jie; Li, Hai-Ou, E-mail: haiouli@ustc.edu.cn, E-mail: gpguo@ustc.edu.cn; Wang, Ke

To reduce the charge noise of a modulation-doped GaAs/AlGaAs quantum dot, we have fabricated shallow-etched GaAs/AlGaAs quantum dots using the wet-etching method to study the effects of two-dimensional electron gas (2DEG) underneath the metallic gates. The low-frequency 1/f noise in the Coulomb blockade region of the shallow-etched quantum dot is compared with a non-etched quantum dot on the same wafer. The average values of the gate noise are approximately 0.5 μeV in the shallow-etched quantum dot and 3 μeV in the regular quantum dot. Our results show the quantum dot low-frequency charge noise can be suppressed by the removal ofmore » the 2DEG underneath the metallic gates, which provides an architecture for noise reduction.« less

[Imaging of surface cell antigens on the tumor sections of lymph nodes using fluorescence quantum dots].

PubMed

Rafalovskaia-Orlovskaia, E P; Gorgidze, L A; Gladkikh, A A; Tauger, S M; Vorob'ev, I A

2012-01-01

The usefulness of quantum dots for the immunofluorescent detection of surface antigens on the lymphoid cells has been studied. To optimize quantum dots detection we have upgraded fluorescent microscope that allows obtaining multiple images from different quantum dots from one section. Specimens stained with quantum dots remained stable over two weeks and practically did not bleach under mercury lamp illumination during tens of minutes. Direct conjugates of primary mouse monoclonal antibodies with quantum dots demonstrated high specificity and sufficient sensitivity in the case of double staining on the frozen sections. Because of the high stability of quantum dots' fluorescence, this method allows to analyze antigen coexpression on the lymphoid tissue sections for diagnostic purposes. The spillover of fluorescent signals from quantum dots into adjacent fluorescent channels, with maxima differing by 40 nm, did not exceed 8%, which makes the spectral compensation is practically unnecessary.

Carbon nanotube/metal-sulfide composite flexible electrodes for high-performance quantum dot-sensitized solar cells and supercapacitors

NASA Astrophysics Data System (ADS)

Muralee Gopi, Chandu V. V.; Ravi, Seenu; Rao, S. Srinivasa; Eswar Reddy, Araveeti; Kim, Hee-Je

2017-04-01

Carbon nanotubes (CNT) and metal sulfides have attracted considerable attention owing to their outstanding properties and multiple application areas, such as electrochemical energy conversion and energy storage. Here we describes a cost-effective and facile solution approach to the preparation of metal sulfides (PbS, CuS, CoS, and NiS) grown directly on CNTs, such as CNT/PbS, CNT/CuS, CNT/CoS, and CNT/NiS flexible electrodes for quantum dot-sensitized solar cells (QDSSCs) and supercapacitors (SCs). X-ray photoelectron spectroscopy, X-ray diffraction, and transmission electron microscopy confirmed that the CNT network was covered with high-purity metal sulfide compounds. QDSSCs equipped with the CNT/NiS counter electrode (CE) showed an impressive energy conversion efficiency (η) of 6.41% and remarkable stability. Interestingly, the assembled symmetric CNT/NiS-based polysulfide SC device exhibited a maximal energy density of 35.39 W h kg-1 and superior cycling durability with 98.39% retention after 1,000 cycles compared to the other CNT/metal-sulfides. The elevated performance of the composites was attributed mainly to the good conductivity, high surface area with mesoporous structures and stability of the CNTs and the high electrocatalytic activity of the metal sulfides. Overall, the designed composite CNT/metal-sulfide electrodes offer an important guideline for the development of next level energy conversion and energy storage devices.

Carbon nanotube/metal-sulfide composite flexible electrodes for high-performance quantum dot-sensitized solar cells and supercapacitors.

PubMed

Muralee Gopi, Chandu V V; Ravi, Seenu; Rao, S Srinivasa; Eswar Reddy, Araveeti; Kim, Hee-Je

2017-04-19

Carbon nanotubes (CNT) and metal sulfides have attracted considerable attention owing to their outstanding properties and multiple application areas, such as electrochemical energy conversion and energy storage. Here we describes a cost-effective and facile solution approach to the preparation of metal sulfides (PbS, CuS, CoS, and NiS) grown directly on CNTs, such as CNT/PbS, CNT/CuS, CNT/CoS, and CNT/NiS flexible electrodes for quantum dot-sensitized solar cells (QDSSCs) and supercapacitors (SCs). X-ray photoelectron spectroscopy, X-ray diffraction, and transmission electron microscopy confirmed that the CNT network was covered with high-purity metal sulfide compounds. QDSSCs equipped with the CNT/NiS counter electrode (CE) showed an impressive energy conversion efficiency (η) of 6.41% and remarkable stability. Interestingly, the assembled symmetric CNT/NiS-based polysulfide SC device exhibited a maximal energy density of 35.39 W h kg -1 and superior cycling durability with 98.39% retention after 1,000 cycles compared to the other CNT/metal-sulfides. The elevated performance of the composites was attributed mainly to the good conductivity, high surface area with mesoporous structures and stability of the CNTs and the high electrocatalytic activity of the metal sulfides. Overall, the designed composite CNT/metal-sulfide electrodes offer an important guideline for the development of next level energy conversion and energy storage devices.

Photojunction field-effect transistor based on a colloidal quantum dot absorber channel layer.

PubMed

Adinolfi, Valerio; Kramer, Illan J; Labelle, André J; Sutherland, Brandon R; Hoogland, S; Sargent, Edward H

2015-01-27

The performance of photodetectors is judged via high responsivity, fast speed of response, and low background current. Many previously reported photodetectors based on size-tuned colloidal quantum dots (CQDs) have relied either on photodiodes, which, since they are primary photocarrier devices, lack gain; or photoconductors, which provide gain but at the expense of slow response (due to delayed charge carrier escape from sensitizing centers) and an inherent dark current vs responsivity trade-off. Here we report a photojunction field-effect transistor (photoJFET), which provides gain while breaking prior photoconductors' response/speed/dark current trade-off. This is achieved by ensuring that, in the dark, the channel is fully depleted due to a rectifying junction between a deep-work-function transparent conductive top contact (MoO3) and a moderately n-type CQD film (iodine treated PbS CQDs). We characterize the rectifying behavior of the junction and the linearity of the channel characteristics under illumination, and we observe a 10 μs rise time, a record for a gain-providing, low-dark-current CQD photodetector. We prove, using an analytical model validated using experimental measurements, that for a given response time the device provides a two-orders-of-magnitude improvement in photocurrent-to-dark-current ratio compared to photoconductors. The photoJFET, which relies on a junction gate-effect, enriches the growing family of CQD photosensitive transistors.

Wave Function Engineering in CdSe/PbS Core/Shell Quantum Dots.

PubMed

Wieliczka, Brian M; Kaledin, Alexey L; Buhro, William E; Loomis, Richard A

2018-05-25

The synthesis of epitaxial CdSe/PbS core/shell quantum dots (QDs) is reported. The PbS shell grows in a rock salt structure on the zinc blende CdSe core, thereby creating a crystal structure mismatch through additive growth. Absorption and photoluminescence (PL) band edge features shift to lower energies with increasing shell thickness, but remain above the CdSe bulk band gap. Nevertheless, the profiles of the absorption spectra vary with shell growth, indicating that the overlap of the electron and hole wave functions is changing significantly. This leads to over an order of magnitude reduction of absorption near the band gap and a large, tunable energy shift, of up to 550 meV, between the onset of strong absorption and the band edge PL. While the bulk valence and conduction bands adopt an inverse type-I alignment, the observed spectroscopic behavior is consistent with a transition between quasi-type-I and quasi-type-II behavior depending on shell thickness. Three effective mass approximation models support this hypothesis and suggest that the large difference in effective masses between the core and shell results in hole localization in the CdSe core and a delocalization of the electron across the entire QD. These results show the tuning of wave functions and transition energies in CdSe/PbS nanoheterostructures with prospects for use in optoelectronic devices for luminescent solar concentration or multiexciton generation.

Unity quantum yield of photogenerated charges and band-like transport in quantum-dot solids.

PubMed

Talgorn, Elise; Gao, Yunan; Aerts, Michiel; Kunneman, Lucas T; Schins, Juleon M; Savenije, T J; van Huis, Marijn A; van der Zant, Herre S J; Houtepen, Arjan J; Siebbeles, Laurens D A

2011-09-25

Solid films of colloidal quantum dots show promise in the manufacture of photodetectors and solar cells. These devices require high yields of photogenerated charges and high carrier mobilities, which are difficult to achieve in quantum-dot films owing to a strong electron-hole interaction and quantum confinement. Here, we show that the quantum yield of photogenerated charges in strongly coupled PbSe quantum-dot films is unity over a large temperature range. At high photoexcitation density, a transition takes place from hopping between localized states to band-like transport. These strongly coupled quantum-dot films have electrical properties that approach those of crystalline bulk semiconductors, while retaining the size tunability and cheap processing properties of colloidal quantum dots.

Andreev molecules in semiconductor nanowire double quantum dots.

PubMed

Su, Zhaoen; Tacla, Alexandre B; Hocevar, Moïra; Car, Diana; Plissard, Sébastien R; Bakkers, Erik P A M; Daley, Andrew J; Pekker, David; Frolov, Sergey M

2017-09-19

Chains of quantum dots coupled to superconductors are promising for the realization of the Kitaev model of a topological superconductor. While individual superconducting quantum dots have been explored, control of longer chains requires understanding of interdot coupling. Here, double quantum dots are defined by gate voltages in indium antimonide nanowires. High transparency superconducting niobium titanium nitride contacts are made to each of the dots in order to induce superconductivity, as well as probe electron transport. Andreev bound states induced on each of dots hybridize to define Andreev molecular states. The evolution of these states is studied as a function of charge parity on the dots, and in magnetic field. The experiments are found in agreement with a numerical model.Quantum dots in a nanowire are one possible approach to creating a solid-state quantum simulator. Here, the authors demonstrate the coupling of electronic states in a double quantum dot to form Andreev molecule states; a potential building block for longer chains suitable for quantum simulation.

Boosting the efficiency of quantum dot sensitized solar cells through modulation of interfacial charge transfer.

PubMed

Kamat, Prashant V

2012-11-20

The demand for clean energy will require the design of nanostructure-based light-harvesting assemblies for the conversion of solar energy into chemical energy (solar fuels) and electrical energy (solar cells). Semiconductor nanocrystals serve as the building blocks for designing next generation solar cells, and metal chalcogenides (e.g., CdS, CdSe, PbS, and PbSe) are particularly useful for harnessing size-dependent optical and electronic properties in these nanostructures. This Account focuses on photoinduced electron transfer processes in quantum dot sensitized solar cells (QDSCs) and discusses strategies to overcome the limitations of various interfacial electron transfer processes. The heterojunction of two semiconductor nanocrystals with matched band energies (e.g., TiO(2) and CdSe) facilitates charge separation. The rate at which these separated charge carriers are driven toward opposing electrodes is a major factor that dictates the overall photocurrent generation efficiency. The hole transfer at the semiconductor remains a major bottleneck in QDSCs. For example, the rate constant for hole transfer is 2-3 orders of magnitude lower than the electron injection from excited CdSe into oxide (e.g., TiO(2)) semiconductor. Disparity between the electron and hole scavenging rate leads to further accumulation of holes within the CdSe QD and increases the rate of electron-hole recombination. To overcome the losses due to charge recombination processes at the interface, researchers need to accelerate electron and hole transport. The power conversion efficiency for liquid junction and solid state quantum dot solar cells, which is in the range of 5-6%, represents a significant advance toward effective utilization of nanomaterials for solar cells. The design of new semiconductor architectures could address many of the issues related to modulation of various charge transfer steps. With the resolution of those problems, the efficiencies of QDSCs could approach those of dye sensitized solar cells (DSSC) and organic photovoltaics.

Controlling the Photophysical Properties of Semiconductor Quantum Dot Arrays by Strategically Altering Their Surface Chemistry

NASA Astrophysics Data System (ADS)

Marshall, Ashley R.

Semiconductor quantum dots (QDs) are interesting materials that, after less than 40 years of research, are used in commercial products. QDs are now found in displays, such as Samsung televisions and the Kindle Fire, and have applications in lighting, bio-imaging, quantum computing, and photovoltaics. They offer a large range of desirable properties: a controllable band gap, solution processability, controlled energy levels, and are currently the best materials for multiple exciton generation. The tunable optoelectronic properties of QDs can be controlled using size, shape, composition, and surface treatments--as shown here. Due to the quasi-spherical shape of QDs the surface to volume ratio is high, i.e. many of the constituent atoms are found on the QD surface. This makes QDs highly sensitive to surface chemistry modifications. This thesis encompasses the effects of surface treatments for QDs of two semiconducting materials: lead chalcogenides and CsPbI3. Our group developed a new synthetic technique for lead chalcogenide QDs via the cation exchange of cadmium chalcogenides. An in-depth chemical analysis is paired with optical and electrical studies and we find that metal halide residue contributes to the oxidative stability and decreased trap state density in cation-exchanged PbS QDs. We exploit these properties to make air-stable QD photovoltaic devices from both PbS and PbSe QD materials. Beyond the effects of residual atoms left from the synthetic technique, I investigated how to controllably add atoms onto the surface of QDs. I found that by introducing metal halides as a post-treatment in an electronically coupled array I am able to control the performance parameters in QD photovoltaic devices. These treatments fully infiltrate the assembled film, even under short exposure times and allow me to add controlled quantities of surface atoms to study their effects on film properties and photovoltaic device performance. Finally, I sought to apply the knowledge of the lead chalcogenide QD surfaces to produce QD photovoltaics from a new material: CsPbI3. I fabricated the first perovskite QD photovoltaic devices and using similar treatment methods as the lead chalcogenide QD arrays, I am able to influence the photophysical properties of CsPbI3 QD arrays.

Charge reconfiguration in arrays of quantum dots

NASA Astrophysics Data System (ADS)

Bayer, Johannes C.; Wagner, Timo; Rugeramigabo, Eddy P.; Haug, Rolf J.

2017-12-01

Semiconductor quantum dots are potential building blocks for scalable qubit architectures. Efficient control over the exchange interaction and the possibility of coherently manipulating electron states are essential ingredients towards this goal. We studied experimentally the shuttling of electrons trapped in serial quantum dot arrays isolated from the reservoirs. The isolation hereby enables a high degree of control over the tunnel couplings between the quantum dots, while electrons can be transferred through the array by gate voltage variations. Model calculations are compared with our experimental results for double, triple, and quadruple quantum dot arrays. We are able to identify all transitions observed in our experiments, including cotunneling transitions between distant quantum dots. The shuttling of individual electrons between quantum dots along chosen paths is demonstrated.

Computation of energy states of hydrogenic quantum dot with two-electrons

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yakar, Y., E-mail: yuyakar@yahoo.com; Özmen, A., E-mail: aozmen@selcuk.edu.tr; Çakır, B., E-mail: bcakir@selcuk.edu.tr

2016-03-25

In this study we have investigated the electronic structure of the hydrogenic quantum dot with two electrons inside an impenetrable potential surface. The energy eigenvalues and wavefunctions of the ground and excited states of spherical quantum dot have been calculated by using the Quantum Genetic Algorithm (QGA) and Hartree-Fock Roothaan (HFR) method, and the energies are investigated as a function of dot radius. The results show that as dot radius increases, the energy of quantum dot decreases.

Fast synthesize ZnO quantum dots via ultrasonic method.

PubMed

Yang, Weimin; Zhang, Bing; Ding, Nan; Ding, Wenhao; Wang, Lixi; Yu, Mingxun; Zhang, Qitu

2016-05-01

Green emission ZnO quantum dots were synthesized by an ultrasonic sol-gel method. The ZnO quantum dots were synthesized in various ultrasonic temperature and time. Photoluminescence properties of these ZnO quantum dots were measured. Time-resolved photoluminescence decay spectra were also taken to discover the change of defects amount during the reaction. Both ultrasonic temperature and time could affect the type and amount of defects in ZnO quantum dots. Total defects of ZnO quantum dots decreased with the increasing of ultrasonic temperature and time. The dangling bonds defects disappeared faster than the optical defects. Types of optical defects first changed from oxygen interstitial defects to oxygen vacancy and zinc interstitial defects. Then transformed back to oxygen interstitial defects again. The sizes of ZnO quantum dots would be controlled by both ultrasonic temperature and time as well. That is, with the increasing of ultrasonic temperature and time, the sizes of ZnO quantum dots first decreased then increased. Moreover, concentrated raw materials solution brought larger sizes and more optical defects of ZnO quantum dots. Copyright © 2015 Elsevier B.V. All rights reserved.

Improved performance of CdSe/CdS/PbS co-sensitized solar cell with double-layered TiO2 films as photoanode

NASA Astrophysics Data System (ADS)

Zhang, Xiaolong; Lin, Yu; Wu, Jihuai; Jing, Jing; Fang, Biaopeng

2017-07-01

Improving the photovoltaic performance of CdSe/CdS/PbS co-sensitized double-layered TiO2 solar cells is reported. Double-layered TiO2 films with TiO2 microspheres as the light blocking layers were prepared. PbS, CdS and CdSe quantum dots (QDs) were assembled onto TiO2 photoanodes by simple successive ionic layer absorption and reaction (SILAR) to fabricate CdSe/CdS/PbS co-sensitized solar cells. An improved power conversion efficiency (PCE) of 5.11% was achieved for CdSe/CdS/PbS co-sensitized solar cells at one sun illumination (AM 1.5 G, 100 mW cm-2), which had an improvement of 22.6% over that of the CdSe/CdS co-sensitized solar cells (4.17%). This enhancement is mainly attributed to their better ability of the absorption of solar light with the existence of PbS QDs, the reduction of charge recombination of the excited electron and longer lifetime of electrons, which have been proved with the photovoltaic studies and electrochemical impedance spectroscopy (EIS).

Interparticle spacing and structural ordering in superlattice PbS nanocrystal solids undergoing ligand exchange

DOE PAGES

Weidman, Mark C.; Yager, Kevin G.; Tisdale, William A.

2014-12-12

Controlling the interparticle spacing in quantum dot (QD) thin films is the most readily accessible way to control transport rates between neighboring QDs and a critical component of device optimization. Here, we use X-ray scattering measurements to accurately measure the interparticle spacing in films of highly monodisperse lead sulfide (PbS) QDs that have undergone a variety of device-relevant ligand exchanges. We tabulate these values for use in simulations and data analysis. We find that monothiol and dithiol ligand species typically result in interparticle spacing values that are equal to the length of a single monothiol or dithiol ligand. Additionally, wemore » find that spin-coating a thick film of QDs followed by a long-duration ligand exchange results in a more complete ligand exchange than spin-coating many thin layers with short-duration ligand exchanges in between. The former method also preserves a remarkable degree of the long-range ordering that was present in the film prior to ligand exchange. These results shed light on ways to produce highly-ordered QD solids with compact and functional ligands, which could lead to enhanced interdot coupling and transport phenomena.« less

Formation of uniform high-density and small-size Ge/Si quantum dots by scanning pulsed laser annealing of pre-deposited Ge/Si film

DOE Office of Scientific and Technical Information (OSTI.GOV)

Qayyum, Hamza; Chen, Szu-yuan, E-mail: sychen@ltl.iams.sinica.edu.tw; Department of Physics, National Central University, Zhongli, Taoyuan 320, Taiwan

2016-05-15

The capability to fabricate Ge/Si quantum dots with small dot size and high dot density uniformly over a large area is crucial for many applications. In this work, we demonstrate that this can be achieved by scanning a pre-deposited Ge thin layer on Si substrate with a line-focused pulsed laser beam to induce formation of quantum dots. With suitable setting, Ge/Si quantum dots with a mean height of 2.9 nm, a mean diameter of 25 nm, and a dot density of 6×10{sup 10} cm{sup −2} could be formed over an area larger than 4 mm{sup 2}. The average size ofmore » the laser-induced quantum dots is smaller while their density is higher than that of quantum dots grown by using Stranski-Krastanov growth mode. Based on the dependence of the characteristics of quantum dots on the laser parameters, a model consisting of laser-induced strain, surface diffusion, and Ostwald ripening is proposed for the mechanism underlying the formation of the Ge/Si quantum dots. The technique demonstrated could be applicable to other materials besides Ge/Si.« less

Recent Progress Towards Quantum Dot Solar Cells with Enhanced Optical Absorption.

PubMed

Zheng, Zerui; Ji, Haining; Yu, Peng; Wang, Zhiming

2016-12-01

Quantum dot solar cells, as a promising candidate for the next generation solar cell technology, have received tremendous attention in the last 10 years. Some recent developments in epitaxy growth and device structures have opened up new avenues for practical quantum dot solar cells. Unfortunately, the performance of quantum dot solar cells is often plagued by marginal photon absorption. In this review, we focus on the recent progress made in enhancing optical absorption in quantum dot solar cells, including optimization of quantum dot growth, improving the solar cells structure, and engineering light trapping techniques.

Study of CdTe quantum dots grown using a two-step annealing method

NASA Astrophysics Data System (ADS)

Sharma, Kriti; Pandey, Praveen K.; Nagpal, Swati; Bhatnagar, P. K.; Mathur, P. C.

2006-02-01

High size dispersion, large average radius of quantum dot and low-volume ratio has been a major hurdle in the development of quantum dot based devices. In the present paper, we have grown CdTe quantum dots in a borosilicate glass matrix using a two-step annealing method. Results of optical characterization and the theoretical model of absorption spectra have shown that quantum dots grown using two-step annealing have lower average radius, lesser size dispersion, higher volume ratio and higher decrease in bulk free energy as compared to quantum dots grown conventionally.

Photoluminescence of patterned CdSe quantum dot for anti-counterfeiting label on paper

DOE Office of Scientific and Technical Information (OSTI.GOV)

Isnaeni,, E-mail: isnaeni@lipi.go.id; Yulianto, Nursidik; Suliyanti, Maria Margaretha

We successfully developed a method utilizing colloidal CdSe nanocrystalline quantum dot for anti-counterfeiting label on a piece of glossy paper. We deposited numbers and lines patterns of toluene soluble CdSe quantum dot using rubber stamper on a glossy paper. The width of line pattern was about 1-2 mm with 1-2 mm separation between lines. It required less than one minute for deposited CdSe quantum dot on glossy paper to dry and become invisible by naked eyes. However, patterned quantum dot become visible using long-pass filter glasses upon excitation of UV lamp or blue laser. We characterized photoluminescence of line patterns of quantummore » dot, and we found that emission boundaries of line patterns were clearly observed. The error of line size and shape were mainly due to defect of the original stamper. The emission peak wavelength of CdSe quantum dot was 629 nm. The emission spectrum of deposited quantum dot has full width at half maximum (FWHM) of 30-40 nm. The spectra similarity between deposited quantum dot and the original quantum dot in solution proved that our stamping method can be simply applied on glossy paper without changing basic optical property of the quantum dot. Further development of this technique is potential for anti-counterfeiting label on very important documents or objects.« less

Thermoelectric energy harvesting with quantum dots

NASA Astrophysics Data System (ADS)

Sothmann, Björn; Sánchez, Rafael; Jordan, Andrew N.

2015-01-01

We review recent theoretical work on thermoelectric energy harvesting in multi-terminal quantum-dot setups. We first discuss several examples of nanoscale heat engines based on Coulomb-coupled conductors. In particular, we focus on quantum dots in the Coulomb-blockade regime, chaotic cavities and resonant tunneling through quantum dots and wells. We then turn toward quantum-dot heat engines that are driven by bosonic degrees of freedom such as phonons, magnons and microwave photons. These systems provide interesting connections to spin caloritronics and circuit quantum electrodynamics.

Optically Driven Spin Based Quantum Dots for Quantum Computing - Research Area 6 Physics 6.3.2

DTIC Science & Technology

2015-12-15

quantum dots (SAQD) in Schottky diodes . Based on spins in these dots, a scalable architecture has been proposed [Adv. in Physics, 59, 703 (2010)] by us...housed in two coupled quantum dots with tunneling between them, as described above, may not be scalable but can serve as a node in a quantum network. The... tunneling -coupled two-electron spin ground states in the vertically coupled quantum dots for “universal computation” two spin qubits within the universe of

Studies of silicon quantum dots prepared at different substrate temperatures

NASA Astrophysics Data System (ADS)

Al-Agel, Faisal A.; Suleiman, Jamal; Khan, Shamshad A.

2017-03-01

In this research work, we have synthesized silicon quantum dots at different substrate temperatures 193, 153 and 123 K at a fixed working pressure 5 Torr. of Argon gas. The structural studies of these silicon quantum dots have been undertaken using X-ray diffraction, Field Emission Scanning Electron Microscopy (FESEM) and High Resolution Transmission Electron Microscopy (HRTEM). The optical and electrical properties have been studied using UV-visible spectroscopy, Fourier transform infrared (FTIR) spectroscopy, Fluorescence spectroscopy and I-V measurement system. X-ray diffraction pattern of Si quantum dots prepared at different temperatures show the amorphous nature except for the quantum dots synthesized at 193 K which shows polycrystalline nature. FESEM images of samples suggest that the size of quantum dots varies from 2 to 8 nm. On the basis of UV-visible spectroscopy measurements, a direct band gap has been observed for Si quantum dots. FTIR spectra suggest that as-grown Si quantum dots are partially oxidized which is due exposure of as-prepared samples to air after taking out from the chamber. PL spectra of the synthesized silicon quantum dots show an intense peak at 444 nm, which may be attributed to the formation of Si quantum dots. Temperature dependence of dc conductivity suggests that the dc conductivity enhances exponentially by raising the temperature. On the basis above properties i.e. direct band gap, high absorption coefficient and high conductivity, these silicon quantum dots will be useful for the fabrication of solar cells.

Plasma Reflection in Multigrain Layers of Narrow-Bandgap Semiconductors

NASA Astrophysics Data System (ADS)

Zhukov, N. D.; Shishkin, M. I.; Rokakh, A. G.

2018-04-01

Qualitatively similar spectral characteristics of plasma-resonance reflection in the region of 15-25 μm were obtained for layers of electrodeposited submicron particles of InSb, InAs, and GaAs and plates of these semiconductors ground with M1-grade diamond powder. The most narrow-bandgap semiconductor InSb (intrinsic absorption edge ˜7 μm) is characterized by an absorption band at 2.1-2.3 μm, which is interpreted in terms of the model of optical excitation of electrons coupled by the Coulomb interaction. The spectra of a multigrain layer of chemically deposited PbS nanoparticles (50-70 nm) exhibited absorption maxima at 7, 10, and 17 μm, which can be explained by electron transitions obeying the energy-quantization rules for quantum dots.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Michael, Stephan; Chow, Weng; Schneider, Hans

In the framework of a microscopic model for intersubband gain from electrically pumped quantum-dot structures we investigate electrically pumped quantum-dots as active material for a mid-infrared quantum cascade laser. Our previous calculations have indicated that these structures could operate with reduced threshold current densities while also achieving a modal gain comparable to that of quantum well active materials. We study the influence of two important quantum-dot material parameters, here, namely inhomogeneous broadening and quantum-dot sheet density, on the performance of a proposed quantum cascade laser design. In terms of achieving a positive modal net gain, a high quantum-dot density canmore » compensate for moderately high inhomogeneous broadening, but at a cost of increased threshold current density. By minimizing quantum-dot density with presently achievable inhomogeneous broadening and total losses, significantly lower threshold densities than those reported in quantum-well quantum-cascade lasers are predicted by our theory.« less

Phonon impact on optical control schemes of quantum dots: Role of quantum dot geometry and symmetry

NASA Astrophysics Data System (ADS)

Lüker, S.; Kuhn, T.; Reiter, D. E.

2017-12-01

Phonons strongly influence the optical control of semiconductor quantum dots. When modeling the electron-phonon interaction in several theoretical approaches, the quantum dot geometry is approximated by a spherical structure, though typical self-assembled quantum dots are strongly lens-shaped. By explicitly comparing simulations of a spherical and a lens-shaped dot using a well-established correlation expansion approach, we show that, indeed, lens-shaped dots can be exactly mapped to a spherical geometry when studying the phonon influence on the electronic system. We also give a recipe to reproduce spectral densities from more involved dots by rather simple spherical models. On the other hand, breaking the spherical symmetry has a pronounced impact on the spatiotemporal properties of the phonon dynamics. As an example we show that for a lens-shaped quantum dot, the phonon emission is strongly concentrated along the direction of the smallest axis of the dot, which is important for the use of phonons for the communication between different dots.

Green, Rapid, and Universal Preparation Approach of Graphene Quantum Dots under Ultraviolet Irradiation.

PubMed

Zhu, Jinli; Tang, Yanfeng; Wang, Gang; Mao, Jiarong; Liu, Zhiduo; Sun, Tongming; Wang, Miao; Chen, Da; Yang, Yucheng; Li, Jipeng; Deng, Yuan; Yang, Siwei

2017-04-26

It is of great significance and importance to explore a mild, clean, and highly efficient universal approach for the synthesis of graphene quantum dots. Herein, we introduced a new green, rapid, and universal preparation approach for graphene quantum dots via the free-radical polymerization of oxygen-containing aromatic compounds under ultraviolet irradiation. This approach had a high yield (86%), and the byproducts are only H 2 O and CO 2 . The obtained graphene quantum dots were well-crystallized and showed remarkable optical and biological properties. The colorful, different-sized graphene quantum dots can be used in fluorescent bioimaging in vitro and in vivo. This approach is suitable not only for the preparation of graphene quantum dots but also for heteroatom-doped graphene quantum dots.

Spectroscopy characterization and quantum yield determination of quantum dots

NASA Astrophysics Data System (ADS)

Contreras Ortiz, S. N.; Mejía Ospino, E.; Cabanzo, R.

2016-02-01

In this paper we show the characterization of two kinds of quantum dots: hydrophilic and hydrophobic, with core and core/shell respectively, using spectroscopy techniques such as UV-Vis, fluorescence and Raman. We determined the quantum yield in the quantum dots using the quinine sulphate as standard. This salt is commonly used because of its quantum yield (56%) and stability. For the CdTe excitation, we used a wavelength of 549nm and for the CdSe/ZnS excitation a wavelength of 527nm. The results show that CdSe/ZnS (49%) has better fluorescence, better quantum dots, and confirm the fluorescence result. The quantum dots have shown a good fluorescence performance, so this property will be used to replace dyes, with the advantage that quantum dots are less toxic than some dyes like the rhodamine. In addition, in this work we show different techniques to find the quantum dots emission: fluorescence spectrum, synchronous spectrum and Raman spectrum.

Carbon quantum dots and a method of making the same

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zidan, Ragaiy; Teprovich, Joseph A.; Washington, Aaron L.

The present invention is directed to a method of preparing a carbon quantum dot. The carbon quantum dot can be prepared from a carbon precursor, such as a fullerene, and a complex metal hydride. The present invention also discloses a carbon quantum dot made by reacting a carbon precursor with a complex metal hydride and a polymer containing a carbon quantum dot made by reacting a carbon precursor with a complex metal hydride.

Wavelength-tunable entangled photons from silicon-integrated III-V quantum dots.

PubMed

Chen, Yan; Zhang, Jiaxiang; Zopf, Michael; Jung, Kyubong; Zhang, Yang; Keil, Robert; Ding, Fei; Schmidt, Oliver G

2016-01-27

Many of the quantum information applications rely on indistinguishable sources of polarization-entangled photons. Semiconductor quantum dots are among the leading candidates for a deterministic entangled photon source; however, due to their random growth nature, it is impossible to find different quantum dots emitting entangled photons with identical wavelengths. The wavelength tunability has therefore become a fundamental requirement for a number of envisioned applications, for example, nesting different dots via the entanglement swapping and interfacing dots with cavities/atoms. Here we report the generation of wavelength-tunable entangled photons from on-chip integrated InAs/GaAs quantum dots. With a novel anisotropic strain engineering technique based on PMN-PT/silicon micro-electromechanical system, we can recover the quantum dot electronic symmetry at different exciton emission wavelengths. Together with a footprint of several hundred microns, our device facilitates the scalable integration of indistinguishable entangled photon sources on-chip, and therefore removes a major stumbling block to the quantum-dot-based solid-state quantum information platforms.

Size dependence in tunneling spectra of PbSe quantum-dot arrays.

PubMed

Ou, Y C; Cheng, S F; Jian, W B

2009-07-15

Interdot Coulomb interactions and collective Coulomb blockade were theoretically argued to be a newly important topic, and experimentally identified in semiconductor quantum dots, formed in the gate confined two-dimensional electron gas system. Developments of cluster science and colloidal synthesis accelerated the studies of electron transport in colloidal nanocrystal or quantum-dot solids. To study the interdot coupling, various sizes of two-dimensional arrays of colloidal PbSe quantum dots are self-assembled on flat gold surfaces for scanning tunneling microscopy and scanning tunneling spectroscopy measurements at both room and liquid-nitrogen temperatures. The tip-to-array, array-to-substrate, and interdot capacitances are evaluated and the tunneling spectra of quantum-dot arrays are analyzed by the theory of collective Coulomb blockade. The current-voltage of PbSe quantum-dot arrays conforms properly to a scaling power law function. In this study, the dependence of tunneling spectra on the sizes (numbers of quantum dots) of arrays is reported and the capacitive coupling between quantum dots in the arrays is explored.

InAs Colloidal Quantum Dots Synthesis via Aminopnictogen Precursor Chemistry.

PubMed

Grigel, Valeriia; Dupont, Dorian; De Nolf, Kim; Hens, Zeger; Tessier, Mickael D

2016-10-05

Despite their various potential applications, InAs colloidal quantum dots have attracted considerably less attention than more classical II-VI materials because of their complex syntheses that require hazardous precursors. Recently, amino-phosphine has been introduced as a cheap, easy-to-use and efficient phosphorus precursor to synthesize InP quantum dots. Here, we use aminopnictogen precursors to implement a similar approach for synthesizing InAs quantum dots. We develop a two-step method based on the combination of aminoarsine as the arsenic precursor and aminophosphine as the reducing agent. This results in state-of-the-art InAs quantum dots with respect to the size dispersion and band-gap range. Moreover, we present shell coating procedures that lead to the formation of InAs/ZnS(e) core/shell quantum dots that emit in the infrared region. This innovative synthesis approach can greatly facilitate the research on InAs quantum dots and may lead to synthesis protocols for a wide range of III-V quantum dots.

Improved dot size uniformity and luminescense of InAs quantum dots on InP substrate

NASA Technical Reports Server (NTRS)

Qiu, Y.; Uhl, D.

2002-01-01

InAs self-organized quantum dots have been grown in InGaAs quantum well on InP substrates by metalorganic vapor phase epitaxy. Atomic Force Microscopy confirmed of quantum dot formation with dot density of 3X10(sup 10) cm(sup -2). Improved dot size uniformity and strong room temperature photoluminescence up to 2 micron were observed after modifying the InGaAs well.

Zinc sulfide quantum dots for photocatalytic and sensing applications

NASA Astrophysics Data System (ADS)

Sergeev, Alexander A.; Leonov, Andrei A.; Zhuikova, Elena I.; Postnova, Irina V.; Voznesenskiy, Sergey S.

2017-09-01

Herein, we report the photocatalytic and sensing applications of pure and Mn-doped ZnS quantum dots. The quantum dots were prepared by a chemical precipitation in an aqueous solution in the presence of glutathione as a stabilizing agent. The synthesized quantum dots were used as effective photocatalyst for the degradation of methylene blue dye. Interestingly, fully degradation of methylene blue dye was achieved in 5 min using pure ZnS quantum dots. Further, the synthesized quantum dots were used as efficient sensing element for methane fluorescent sensor. Interfering studies confirmed that the developed sensor possesses very good sensitivity and selectivity towards methane.

The photosensitivity of carbon quantum dots/CuAlO2 films composites.

PubMed

Pan, Jiaqi; Sheng, Yingzhuo; Zhang, Jingxiang; Wei, Jumeng; Huang, Peng; Zhang, Xin; Feng, Boxue

2015-07-31

Carbon quantum dots/CuAlO2 films were prepared by a simple route through which CuAlO2 films prepared by sol-gel on crystal quartz substrates were composited with carbon quantum dots on their surface. The characterization results indicated that CuAlO2 films were well combined with carbon quantum dots. The photoconductivity of carbon quantum dots/CuAlO2 films was investigated under illumination and darkness switching, and was demonstrated to be significantly enhanced compared with CuAlO2 films. Through analysis, this enhancement of photoconductivity was attributed to the carbon quantum dots with unique up-converted photoluminescence behavior.

The photosensitivity of carbon quantum dots/CuAlO2 films composites

NASA Astrophysics Data System (ADS)

Pan, Jiaqi; Sheng, Yingzhuo; Zhang, Jingxiang; Wei, Jumeng; Huang, Peng; Zhang, Xin; Feng, Boxue

2015-07-01

Carbon quantum dots/CuAlO2 films were prepared by a simple route through which CuAlO2 films prepared by sol-gel on crystal quartz substrates were composited with carbon quantum dots on their surface. The characterization results indicated that CuAlO2 films were well combined with carbon quantum dots. The photoconductivity of carbon quantum dots/CuAlO2 films was investigated under illumination and darkness switching, and was demonstrated to be significantly enhanced compared with CuAlO2 films. Through analysis, this enhancement of photoconductivity was attributed to the carbon quantum dots with unique up-converted photoluminescence behavior.

Effect of self assembled quantum dots on carrier mobility, with application to modeling the dark current in quantum dot infrared photodetectors

NASA Astrophysics Data System (ADS)

Youssef, Sarah; El-Batawy, Yasser M.; Abouelsaood, Ahmed A.

2016-09-01

A theoretical method for calculating the electron mobility in quantum dot infrared photodetectors is developed. The mobility calculation is based on a time-dependent, finite-difference solution of the Boltzmann transport equation in a bulk semiconductor material with randomly positioned conical quantum dots. The quantum dots act as scatterers of current carriers (conduction-band electrons in our case), resulting in limiting their mobility. In fact, carrier scattering by quantum dots is typically the dominant factor in determining the mobility in the active region of the quantum dot device. The calculated values of the mobility are used in a recently developed generalized drift-diffusion model for the dark current of the device [Ameen et al., J. Appl. Phys. 115, 063703 (2014)] in order to fix the overall current scale. The results of the model are verified by comparing the predicted dark current characteristics to those experimentally measured and reported for actual InAs/GaAs quantum dot infrared photodetectors. Finally, the effect of the several relevant device parameters, including the operating temperature and the quantum dot average density, is studied.

Investigation of trypsin-CdSe quantum dot interactions via spectroscopic methods and effects on enzymatic activity.

PubMed

Kaur, Gurvir; Tripathi, S K

2015-01-05

The paper presents the interactions between trypsin and water soluble cadmium selenide (CdSe) quantum dots investigated by spectrophotometric methods. CdSe quantum dots have strong ability to quench the intrinsic fluorescence of trypsin by a static quenching mechanism. The quenching has been studied at three different temperatures where the results revealed that electrostatic interactions exist between CdSe quantum dots and trypsin and are responsible to stabilize the complex. The Scatchard plot from quenching revealed 1 binding site for quantum dots by trypsin, the same has been confirmed by making isothermal titrations of quantum dots against trypsin. The distance between donor and acceptor for trypsin-CdSe quantum dot complexes is calculated to be 2.8 nm by energy transfer mechanisms. The intrinsic fluorescence of CdSe quantum dots has also been enhanced by the trypsin, and is linear for concentration of trypsin ranging 1-80 μl. All the observations evidence the formation of trypsin-CdSe quantum dot conjugates, where trypsin retains the enzymatic activity which in turn is temperature and pH dependent. Copyright © 2014 Elsevier B.V. All rights reserved.

Multi-Excitonic Quantum Dot Molecules

NASA Astrophysics Data System (ADS)

Scheibner, M.; Stinaff, E. A.; Doty, M. F.; Ware, M. E.; Bracker, A. S.; Gammon, D.; Ponomarev, I. V.; Reinecke, T. L.; Korenev, V. L.

2006-03-01

With the ability to create coupled pairs of quantum dots, the next step towards the realization of semiconductor based quantum information processing devices can be taken. However, so far little knowledge has been gained on these artificial molecules. Our photoluminescence experiments on single InAs/GaAs quantum dot molecules provide the systematics of coupled quantum dots by delineating the spectroscopic features of several key charge configurations in such quantum systems, including X, X^+,X^2+, XX, XX^+ (with X being the neutral exciton). We extract general rules which determine the formation of molecular states of coupled quantum dots. These include the fact that quantum dot molecules provide the possibility to realize various spin configurations and to switch the electron hole exchange interaction on and off by shifting charges inside the molecule. This knowledge will be valuable in developing implementations for quantum information processing.

Resonant tunneling spectroscopy of valley eigenstates on a donor-quantum dot coupled system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kobayashi, T., E-mail: t.kobayashi@unsw.edu.au; Heijden, J. van der; House, M. G.

We report on electronic transport measurements through a silicon double quantum dot consisting of a donor and a quantum dot. Transport spectra show resonant tunneling peaks involving different valley states, which illustrate the valley splitting in a quantum dot on a Si/SiO{sub 2} interface. The detailed gate bias dependence of double dot transport allows a first direct observation of the valley splitting in the quantum dot, which is controllable between 160 and 240 μeV with an electric field dependence 1.2 ± 0.2 meV/(MV/m). A large valley splitting is an essential requirement for implementing a physical electron spin qubit in a silicon quantum dot.

Arginine-glycine-aspartic acid-conjugated dendrimer-modified quantum dots for targeting and imaging melanoma.

PubMed

Li, Zhiming; Huang, Peng; Lin, Jing; He, Rong; Liu, Bing; Zhang, Xiaomin; Yang, Sen; Xi, Peng; Zhang, Xuejun; Ren, Qiushi; Cui, Daxiang

2010-08-01

Angiogenesis is essential for the development of malignant tumors and provides important targets for tumor diagnosis and therapy. Quantum dots have been broadly investigated for their potential application in cancer molecular imaging. In present work, CdSe quantum dots were synthesized, polyamidoamine dendrimers were used to modify surface of quantum dots and improve their solubility in water solution. Then, dendrimer-modified CdSe quantum dots were conjugated with arginine-glycine-aspartic acid (RGD) peptides. These prepared nanoprobes were injected into nude mice loaded with melanoma (A375) tumor xenografts via tail vessels, IVIS imaging system was used to image the targeting and bio-distribution of as-prepared nanoprobes. The dendrimer-modified quantum dots exhibit water-soluble, high quantum yield, and good biocompatibility. RGD-conjugated quantum dots can specifically target human umbilical vein endothelial cells (HUVEC) and A375 melanoma cells, as well as nude mice loaded with A735 melanoma cells. High-performance RGD-conjugated dendrimers modified quantum dot-based nanoprobes have great potential in application such as tumor diagnosis and therapy.

Photoluminescence Enhancement of Silole-Capped Silicon Quantum Dots Based on Förster Resonance Energy Transfer.

PubMed

Kim, Seongwoong; Kim, Sungsoo; Ko, Young Chun; Sohn, Honglae

2015-07-01

Photoluminescent porous silicon were prepared by an electrochemical etch of n-type silicon under the illumination with a 300 W tungsten filament bulb for the duration of etch. The red photoluminescence emitting at 650 nm with an excitation wavelength of 450 nm is due to the quantum confinement of silicon quantum dots in porous silicon. HO-terminated red luminescent PS was obtained by an electrochemical treatment of fresh PS with the current of 150 mA for 60 seconds in water and sodium chloride. As-prepared PS was sonicated, fractured, and centrifuged in toluene solution to obtain photoluminescence silicon quantum dots. Dichlorotetraphenylsilole exhibiting an emission band at 520 nm was reacted with HO-terminated silicon quantum dots to give a silole-capped silicon quantum dots. The optical characterization of silole-derivatized silicon quantum dots was investigated by UV-vis and fluorescence spectrometer. The fluorescence emission efficiency of silole-capped silicon quantum dots was increased by about 2.5 times due to F6rster resonance energy transfer from silole moiety to silicon quantum dots.

Reconfigurable quadruple quantum dots in a silicon nanowire transistor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Betz, A. C., E-mail: ab2106@cam.ac.uk; Broström, M.; Gonzalez-Zalba, M. F.

2016-05-16

We present a reconfigurable metal-oxide-semiconductor multi-gate transistor that can host a quadruple quantum dot in silicon. The device consists of an industrial quadruple-gate silicon nanowire field-effect transistor. Exploiting the corner effect, we study the versatility of the structure in the single quantum dot and the serial double quantum dot regimes and extract the relevant capacitance parameters. We address the fabrication variability of the quadruple-gate approach which, paired with improved silicon fabrication techniques, makes the corner state quantum dot approach a promising candidate for a scalable quantum information architecture.

A tunable few electron triple quantum dot

NASA Astrophysics Data System (ADS)

Gaudreau, L.; Kam, A.; Granger, G.; Studenikin, S. A.; Zawadzki, P.; Sachrajda, A. S.

2009-11-01

In this paper, we report on a tunable few electron lateral triple quantum dot design. The quantum dot potentials are arranged in series. The device is aimed at studies of triple quantum dot properties where knowing the exact number of electrons is important as well as quantum information applications involving electron spin qubits. We demonstrate tuning strategies for achieving required resonant conditions such as quadruple points where all three quantum dots are on resonance. We find that in such a device resonant conditions at specific configurations are accompanied by complex charge transfer behavior.

Growth of InAs Quantum Dots on GaAs (511)A Substrates: The Competition between Thermal Dynamics and Kinetics.

PubMed

Wen, Lei; Gao, Fangliang; Zhang, Shuguang; Li, Guoqiang

2016-08-01

The growth process of InAs quantum dots grown on GaAs (511)A substrates has been studied by atomic force microscopy. According to the atomic force microscopy studies for quantum dots grown with varying InAs coverage, a noncoherent nucleation of quantum dots is observed. Moreover, due to the long migration length of In atoms, the Ostwald ripening process is aggravated, resulting in the bad uniformity of InAs quantum dots on GaAs (511)A. In order to improve the uniformity of nucleation, the growth rate is increased. By studying the effects of increased growth rates on the growth of InAs quantum dots, it is found that the uniformity of InAs quantum dots is greatly improved as the growth rates increase to 0.14 ML s(-1) . However, as the growth rates increase further, the uniformity of InAs quantum dots becomes dual-mode, which can be attributed to the competition between Ostwald ripening and strain relaxation processes. The results in this work provide insights regarding the competition between thermal dynamical barriers and the growth kinetics in the growth of InAs quantum dots, and give guidance to improve the size uniformity of InAs quantum dots on (N11)A substrates. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantum-dot spin-photon entanglement via frequency downconversion to telecom wavelength.

PubMed

De Greve, Kristiaan; Yu, Leo; McMahon, Peter L; Pelc, Jason S; Natarajan, Chandra M; Kim, Na Young; Abe, Eisuke; Maier, Sebastian; Schneider, Christian; Kamp, Martin; Höfling, Sven; Hadfield, Robert H; Forchel, Alfred; Fejer, M M; Yamamoto, Yoshihisa

2012-11-15

Long-distance quantum teleportation and quantum repeater technologies require entanglement between a single matter quantum bit (qubit) and a telecommunications (telecom)-wavelength photonic qubit. Electron spins in III-V semiconductor quantum dots are among the matter qubits that allow for the fastest spin manipulation and photon emission, but entanglement between a single quantum-dot spin qubit and a flying (propagating) photonic qubit has yet to be demonstrated. Moreover, many quantum dots emit single photons at visible to near-infrared wavelengths, where silica fibre losses are so high that long-distance quantum communication protocols become difficult to implement. Here we demonstrate entanglement between an InAs quantum-dot electron spin qubit and a photonic qubit, by frequency downconversion of a spontaneously emitted photon from a singly charged quantum dot to a wavelength of 1,560 nanometres. The use of sub-10-picosecond pulses at a wavelength of 2.2 micrometres in the frequency downconversion process provides the necessary quantum erasure to eliminate which-path information in the photon energy. Together with previously demonstrated indistinguishable single-photon emission at high repetition rates, the present technique advances the III-V semiconductor quantum-dot spin system as a promising platform for long-distance quantum communication.

High quantum yield ZnO quantum dots synthesizing via an ultrasonication microreactor method.

PubMed

Yang, Weimin; Yang, Huafang; Ding, Wenhao; Zhang, Bing; Zhang, Le; Wang, Lixi; Yu, Mingxun; Zhang, Qitu

2016-11-01

Green emission ZnO quantum dots were synthesized by an ultrasonic microreactor. Ultrasonic radiation brought bubbles through ultrasonic cavitation. These bubbles built microreactor inside the microreactor. The photoluminescence properties of ZnO quantum dots synthesized with different flow rate, ultrasonic power and temperature were discussed. Flow rate, ultrasonic power and temperature would influence the type and quantity of defects in ZnO quantum dots. The sizes of ZnO quantum dots would be controlled by those conditions as well. Flow rate affected the reaction time. With the increasing of flow rate, the sizes of ZnO quantum dots decreased and the quantum yields first increased then decreased. Ultrasonic power changed the ultrasonic cavitation intensity, which affected the reaction energy and the separation of the solution. With the increasing of ultrasonic power, sizes of ZnO quantum dots first decreased then increased, while the quantum yields kept increasing. The effect of ultrasonic temperature on the photoluminescence properties of ZnO quantum dots was influenced by the flow rate. Different flow rate related to opposite changing trend. Moreover, the quantum yields of ZnO QDs synthesized by ultrasonic microreactor could reach 64.7%, which is higher than those synthesized only under ultrasonic radiation or only by microreactor. Copyright © 2016 Elsevier B.V. All rights reserved.

Using of Quantum Dots in Biology and Medicine.

PubMed

Pleskova, Svetlana; Mikheeva, Elza; Gornostaeva, Ekaterina

2018-01-01

Quantum dots are nanoparticles, which due to their unique physical and chemical (first of all optical) properties, are promising in biology and medicine. There are many ways for quantum dots synthesis, both in the form of nanoislands self-forming on the surfaces, which can be used as single-photon emitters in electronics for storing information, and in the form of colloidal quantum dots for diagnostic and therapeutic purposes in living systems. The paper describes the main methods of quantum dots synthesis and summarizes medical and biological ways of their use. The main emphasis is laid on the ways of quantum dots surface modification. Influence of the size and form of nanoparticles, charge on the surfaces of quantum dots, and cover type on the efficiency of internalization by cells and cell compartments is shown. The main mechanisms of penetration are considered.

Effect of the Semiconductor Quantum Dot Shell Structure on Fluorescence Quenching by Acridine Ligand

NASA Astrophysics Data System (ADS)

Linkov, P. A.; Vokhmintcev, K. V.; Samokhvalov, P. S.; Laronze-Cochard, M.; Sapi, J.; Nabiev, I. R.

2018-02-01

The main line of research in cancer treatment is the development of methods for early diagnosis and targeted drug delivery to cancer cells. Fluorescent semiconductor core/shell nanocrystals of quantum dots (e.g., CdSe/ZnS) conjugated with an anticancer drug, e.g., an acridine derivative, allow real-time tracking and control of the process of the drug delivery to tumors. However, linking of acridine derivatives to a quantum dot can be accompanied by quantum dot fluorescence quenching caused by electron transfer from the quantum dot to the organic molecule. In this work, it has been shown that the structure of the shell of the quantum dot plays the decisive role in the process of photoinduced charge transfer from the quantum dot to the acridine ligand, which is responsible for fluorescence quenching. It has been shown that multicomponent ZnS/CdS/ZnS shells of CdSe cores of quantum dots, which have a relatively small thickness, make it possible to significantly suppress a decrease in the quantum yield of fluorescence of quantum dots as compared to both the classical ZnS thin shell and superthick shells of the same composition. Thus, core/multicomponent shell CdSe/ZnS/CdS/ZnS quantum dots can be used as optimal fluorescent probes for the development of systems for diagnosis and treatment of cancer with the use of anticancer compounds based on acridine derivatives.

Photoluminescence kinetics slowdown in an ensemble of GaN/AlN quantum dots upon tunneling interaction with defects

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aleksandrov, I. A., E-mail: Aleksandrov@isp.nsc.ru; Mansurov, V. G.; Zhuravlev, K. S.

2016-08-15

The carrier recombination dynamics in an ensemble of GaN/AlN quantum dots is studied. The model proposed for describing this dynamics takes into account the transition of carriers between quantum dots and defects in a matrix. Comparison of the experimental and calculated photoluminescence decay curves shows that the interaction between quantum dots and defects slows down photoluminescence decay in the ensemble of GaN/AlN quantum dots.

Room-temperature lasing operation of a quantum-dot vertical-cavity surface-emitting laser

NASA Astrophysics Data System (ADS)

Saito, Hideaki; Nishi, Kenichi; Ogura, Ichiro; Sugou, Shigeo; Sugimoto, Yoshimasa

1996-11-01

Self-assembled growth of quantum dots by molecular-beam epitaxy is used to form the active region of a vertical-cavity surface-emitting laser (VCSEL). Ten layers of InGaAs quantum dots are stacked in order to increase the gain. This quantum-dot VCSEL has a continuous-wave operating current of 32 mA at room temperature. Emission spectra at various current injections demonstrate that the lasing action is associated with a higher-order transition in the quantum dots.

Influencing factors on the size uniformity of self-assembled SiGe quantum rings grown by molecular beam epitaxy.

PubMed

Cui, J; Lv, Y; Yang, X J; Fan, Y L; Zhong, Z; Jiang, Z M

2011-03-25

The size uniformity of self-assembled SiGe quantum rings, which are formed by capping SiGe quantum dots with a thin Si layer, is found to be greatly influenced by the growth temperature and the areal density of SiGe quantum dots. Higher growth temperature benefits the size uniformity of quantum dots, but results in low Ge concentration as well as asymmetric Ge distribution in the dots, which induces the subsequently formed quantum rings to be asymmetric in shape or even broken somewhere in the ridge of rings. Low growth temperature degrades the size uniformity of quantum dots, and thus that of quantum rings. A high areal density results in the expansion and coalescence of neighboring quantum dots to form a chain, rather than quantum rings. Uniform quantum rings with a size dispersion of 4.6% and an areal density of 7.8×10(8) cm(-2) are obtained at the optimized growth temperature of 640°C.

Graphene quantum dots as enhanced plant growth regulators: effects on coriander and garlic plants.

PubMed

Chakravarty, Disha; Erande, Manisha B; Late, Dattatray J

2015-10-01

We report investigations on the use of graphene quantum dots for growth enhancement in coriander (Coriandrum sativam L.) and garlic (Allium sativum) plants. The as-received seeds of coriander and garlic were treated with 0.2 mg mL(-1) of graphene quantum dots for 3 h before planting. Graphene quantum dots enhanced the growth rate in coriander and garlic plants, including leaves, roots, shoots, flowers and fruits, when the seeds were treated with graphene quantum dots. Our investigations open up the opportunity to use graphene quantum dots as plant growth regulators that can be used in a variety of other food plants for high yield. © 2015 Society of Chemical Industry.

Biocompatible Quantum Dots for Biological Applications

PubMed Central

Rosenthal, Sandra J.; Chang, Jerry C.; Kovtun, Oleg; McBride, James R.; Tomlinson, Ian D.

2011-01-01

Semiconductor quantum dots are quickly becoming a critical diagnostic tool for discerning cellular function at the molecular level. Their high brightness, long-lasting, sizetunable, and narrow luminescence set them apart from conventional fluorescence dyes. Quantum dots are being developed for a variety of biologically oriented applications, including fluorescent assays for drug discovery, disease detection, single protein tracking, and intracellular reporting. This review introduces the science behind quantum dots and describes how they are made biologically compatible. Several applications are also included, illustrating strategies toward target specificity, and are followed by a discussion on the limitations of quantum dot approaches. The article is concluded with a look at the future direction of quantum dots. PMID:21276935

Purification non-aqueous solution of quantum dots CdSe- CdS-ZnS from excess organic substance-stabilizer by use PE- HD membrane

NASA Astrophysics Data System (ADS)

Kosolapova, K.; Al-Alwani, A.; Gorbachev, I.; Glukhovskoy, E.

2015-11-01

Recently, a new simple method for the purification of CdSe-CdS-ZnS quantum dots by using membrane filtration, the filtration process, successfully separated the oleic acid from quantum dots through membranes purification after synthesis; purification of quantum dots is a very significant part of post synthetical treatment that determines the properties of the material. We explore the possibilities of the Langmuir-Blodgett technique to make such layers, using quantum dots as a model system. The Langmuir monolayer of quantum dots were then investigated the surface pressure-area isotherm. From isotherm, we found the surface pressure monolayer changed with time.

Phosphine-free synthesis and characterization of type-II ZnSe/CdS core-shell quantum dots

NASA Astrophysics Data System (ADS)

Ghasemzadeh, Roghayyeh; Armanmehr, Mohammad Hasan; Abedi, Mohammad; Fateh, Davood Sadeghi; Bahreini, Zaker

2018-01-01

A phosphine-free route for synthesis of type-II ZnSe/CdS core-shell quantum dots, using green, low cost and environmentally friendly reagents and phosphine-free solvents such as 1-octadecene (ODE) and liquid paraffin has been reported. Hot-injection technique has been used for the synthesis of ZnSe core quantum dots. The CdS shell quantum dots prepared by reaction of CdO precursor and S powder in 1-octadecene (ODE). The ZnSe/CdS core-shell quantum dots were synthesized via successive ion layer adsorption and reaction (SILAR) technique. The characterization of produced quantum dots were performed by absorption and fluorescence spectroscopy, X-ray diffraction (XRD) and energy dispersive X-ray spectroscopy (EDX) and transmission electron microscopy (TEM). The results showed the formation of type-II ZnSe/CdS core-shell quantum dots with FWHM 32 nm and uniform size distribution.

L-Cysteine Capped CdSe Quantum Dots Synthesized by Photochemical Route.

PubMed

Singh, Avinash; Kunwar, Amit; Rath, M C

2018-05-01

L-cysteine capped CdSe quantum dots were synthesized via photochemical route in aqueous solution under UV photo-irradiation. The as grown CdSe quantum dots exhibit broad fluorescence at room temperature. The CdSe quantum dots were found to be formed only through the reactions of the precursors, i.e., Cd(NH3)2+4 and SeSO2-3 with the photochemically generated 1-hydroxy-2-propyl radicals, (CH3)2COH radicals, which are formed through the process of H atom abstraction by the photoexcited acetone from 2-propanol. L-Cysteine was found to act as a suitable capping agent for the CdSe quantum dots and increases their biocompatability. Cytotoxicty effects of these quantum dots were evaluated in Chinese Hamster Ovary (CHO) epithelial cells, indicated a significant lower level for the L-cysteine capped CdSe quantum dots as compare to the bare ones.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Haw; Hsia, Chih-Hao

Novel Mn.sup.2+-doped quantum dots are provided. These Mn.sup.2+-doped quantum dots exhibit excellent temperature sensitivity in both organic solvents and water-based solutions. Methods of preparing the Mn.sup.2+-doped quantum dots are provided. The Mn.sup.2+-doped quantum dots may be prepared via a stepwise procedure using air-stable and inexpensive chemicals. The use of air-stable chemicals can significantly reduce the cost of synthesis, chemical storage, and the risk associated with handling flammable chemicals. Methods of temperature sensing using Mn.sup.2+-doped quantum dots are provided. The stepwise procedure provides the ability to tune the temperature-sensing properties to satisfy specific needs for temperature sensing applications. Water solubility maymore » be achieved by passivating the Mn.sup.2+-doped quantum dots, allowing the Mn.sup.2+-doped quantum dots to probe the fluctuations of local temperature in biological environments.« less

Three-terminal quantum-dot thermal management devices

NASA Astrophysics Data System (ADS)

Zhang, Yanchao; Zhang, Xin; Ye, Zhuolin; Lin, Guoxing; Chen, Jincan

2017-04-01

We theoretically demonstrate that the heat flows can be manipulated by designing a three-terminal quantum-dot system consisting of three Coulomb-coupled quantum dots connected to respective reservoirs. In this structure, the electron transport between the quantum dots is forbidden, but the heat transport is allowed by the Coulomb interaction to transmit heat between the reservoirs with a temperature difference. We show that such a system is capable of performing thermal management operations, such as heat flow swap, thermal switch, and heat path selector. An important thermal rectifier, i.e., a thermal diode, can be implemented separately in two different paths. The asymmetric configuration of a quantum-dot system is a necessary condition for thermal management operations in practical applications. These results should have important implications in providing the design principle for quantum-dot thermal management devices and may open up potential applications for the thermal management of quantum-dot systems at the nanoscale.

Functional Carbon Quantum Dots: A Versatile Platform for Chemosensing and Biosensing.

PubMed

Feng, Hui; Qian, Zhaosheng

2018-05-01

Carbon quantum dot has emerged as a new promising fluorescent nanomaterial due to its excellent optical properties, outstanding biocompatibility and accessible fabrication methods, and has shown huge application perspective in a variety of areas, especially in chemosensing and biosensing applications. In this personal account, we give a brief overview of carbon quantum dots from its origin and preparation methods, present some advance on fluorescence origin of carbon quantum dots, and focus on development of chemosensors and biosensors based on functional carbon quantum dots. Comprehensive advances on functional carbon quantum dots as a versatile platform for sensing from our group are included and summarized as well as some typical examples from the other groups. The biosensing applications of functional carbon quantum dots are highlighted from selective assays of enzyme activity to fluorescent identification of cancer cells and bacteria. © 2018 The Chemical Society of Japan & Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Negative exchange interactions in coupled few-electron quantum dots

NASA Astrophysics Data System (ADS)

Deng, Kuangyin; Calderon-Vargas, F. A.; Mayhall, Nicholas J.; Barnes, Edwin

2018-06-01

It has been experimentally shown that negative exchange interactions can arise in a linear three-dot system when a two-electron double quantum dot is exchange coupled to a larger quantum dot containing on the order of one hundred electrons. The origin of this negative exchange can be traced to the larger quantum dot exhibiting a spin tripletlike rather than singletlike ground state. Here we show using a microscopic model based on the configuration interaction (CI) method that both tripletlike and singletlike ground states are realized depending on the number of electrons. In the case of only four electrons, a full CI calculation reveals that tripletlike ground states occur for sufficiently large dots. These results hold for symmetric and asymmetric quantum dots in both Si and GaAs, showing that negative exchange interactions are robust in few-electron double quantum dots and do not require large numbers of electrons.

A 2 × 2 quantum dot array with controllable inter-dot tunnel couplings

NASA Astrophysics Data System (ADS)

Mukhopadhyay, Uditendu; Dehollain, Juan Pablo; Reichl, Christian; Wegscheider, Werner; Vandersypen, Lieven M. K.

2018-04-01

The interaction between electrons in arrays of electrostatically defined quantum dots is naturally described by a Fermi-Hubbard Hamiltonian. Moreover, the high degree of tunability of these systems makes them a powerful platform to simulate different regimes of the Hubbard model. However, most quantum dot array implementations have been limited to one-dimensional linear arrays. In this letter, we present a square lattice unit cell of 2 × 2 quantum dots defined electrostatically in an AlGaAs/GaAs heterostructure using a double-layer gate technique. We probe the properties of the array using nearby quantum dots operated as charge sensors. We show that we can deterministically and dynamically control the charge occupation in each quantum dot in the single- to few-electron regime. Additionally, we achieve simultaneous individual control of the nearest-neighbor tunnel couplings over a range of 0-40 μeV. Finally, we demonstrate fast (˜1 μs) single-shot readout of the spin state of electrons in the dots through spin-to-charge conversion via Pauli spin blockade. These advances pave the way for analog quantum simulations in two dimensions, not previously accessible in quantum dot systems.

Charge transport in quantum dot organic solar cells with Si quantum dots sandwiched between poly(3-hexylthiophene) (P3HT) absorber and bathocuproine (BCP) transport layers

NASA Astrophysics Data System (ADS)

Verma, Upendra Kumar; Kumar, Brijesh

2017-10-01

We have modeled a multilayer quantum dot organic solar cell that explores the current-voltage characteristic of the solar cell whose characteristics can be tuned by varying the fabrication parameters of the quantum dots (QDs). The modeled device consists of a hole transport layer (HTL) which doubles up as photon absorbing layer, several quantum dot layers, and an electron transport layer (ETL). The conduction of charge carriers in HTL and ETL has been modeled by the drift-diffusion transport mechanism. The conduction and recombination in the quantum dot layers are described by a system of coupled rate equations incorporating tunneling and bimolecular recombination. Analysis of QD-solar cells shows improved device performance compared to the similar bilayer and trilayer device structures without QDs. Keeping other design parameters constant, solar cell characteristics can be controlled by the quantum dot layers. Bimolecular recombination coefficient of quantum dots is a prime factor which controls the open circuit voltage (VOC) without any significant reduction in short circuit current (JSC).

Photon antibunching from a single quantum-dot-microcavity system in the strong coupling regime.

PubMed

Press, David; Götzinger, Stephan; Reitzenstein, Stephan; Hofmann, Carolin; Löffler, Andreas; Kamp, Martin; Forchel, Alfred; Yamamoto, Yoshihisa

2007-03-16

We observe antibunching in the photons emitted from a strongly coupled single quantum dot and pillar microcavity in resonance. When the quantum dot was spectrally detuned from the cavity mode, the cavity emission remained antibunched, and also anticorrelated from the quantum dot emission. Resonant pumping of the selected quantum dot via an excited state enabled these observations by eliminating the background emitters that are usually coupled to the cavity. This device demonstrates an on-demand single-photon source operating in the strong coupling regime, with a Purcell factor of 61+/-7 and quantum efficiency of 97%.

A Nanowire-Based Plasmonic Quantum Dot Laser.

PubMed

Ho, Jinfa; Tatebayashi, Jun; Sergent, Sylvain; Fong, Chee Fai; Ota, Yasutomo; Iwamoto, Satoshi; Arakawa, Yasuhiko

2016-04-13

Quantum dots enable strong carrier confinement and exhibit a delta-function like density of states, offering significant improvements to laser performance and high-temperature stability when used as a gain medium. However, quantum dot lasers have been limited to photonic cavities that are diffraction-limited and further miniaturization to meet the demands of nanophotonic-electronic integration applications is challenging based on existing designs. Here we introduce the first quantum dot-based plasmonic laser to reduce the cross-sectional area of nanowire quantum dot lasers below the cutoff limit of photonic modes while maintaining the length in the order of the lasing wavelength. Metal organic chemical vapor deposition grown GaAs-AlGaAs core-shell nanowires containing InGaAs quantum dot stacks are placed directly on a silver film, and lasing was observed from single nanowires originating from the InGaAs quantum dot emission into the low-loss higher order plasmonic mode. Lasing threshold pump fluences as low as ∼120 μJ/cm(2) was observed at 7 K, and lasing was observed up to 125 K. Temperature stability from the quantum dot gain, leading to a high characteristic temperature was demonstrated. These results indicate that high-performance, miniaturized quantum dot lasers can be realized with plasmonics.

Coherently-enabled environmental control of optics and energy transfer pathways of hybrid quantum dot-metallic nanoparticle systems.

PubMed

Hatef, Ali; Sadeghi, Seyed M; Fortin-Deschênes, Simon; Boulais, Etienne; Meunier, Michel

2013-03-11

It is well-known that optical properties of semiconductor quantum dots can be controlled using optical cavities or near fields of localized surface plasmon resonances (LSPRs) of metallic nanoparticles. In this paper we study the optics, energy transfer pathways, and exciton states of quantum dots when they are influenced by the near fields associated with plasmonic meta-resonances. Such resonances are formed via coherent coupling of excitons and LSPRs when the quantum dots are close to metallic nanorods and driven by a laser beam. Our results suggest an unprecedented sensitivity to the refractive index of the environment, causing significant spectral changes in the Förster resonance energy transfer from the quantum dots to the nanorods and in exciton transition energies. We demonstrate that when a quantum dot-metallic nanorod system is close to its plasmonic meta-resonance, we can adjust the refractive index to: (i) control the frequency range where the energy transfer from the quantum dot to the metallic nanorod is inhibited, (ii) manipulate the exciton transition energy shift of the quantum dot, and (iii) disengage the quantum dot from the metallic nanoparticle and laser field. Our results show that near meta-resonances the spectral forms of energy transfer and exciton energy shifts are strongly correlated to each other.

Facilitated preparation of bioconjugatable zwitterionic quantum dots using dual-lipid encapsulation.

PubMed

Shrake, Robert; Demillo, Violeta G; Ahmadiantehrani, Mojtaba; Zhu, Xiaoshan; Publicover, Nelson G; Hunter, Kenneth W

2015-01-01

Zwitterionic quantum dots prepared through incorporated zwitterionic ligands on quantum dot surfaces, are being paid significant attention in biomedical applications because of their excellent colloidal stability across a wide pH and ionic strength range, antifouling surface, good biocompatibility, etc. In this work, we report a dual-lipid encapsulation approach to prepare bioconjugatable zwitterionic quantum dots using amidosulfobetaine-16 lipids, dipalmitoyl-sn-glycero-3-phosphoethanolamine lipids with functional head groups, and CuInS2/ZnS quantum dots in a tetrahydrofuran/methanol/water solvent system with sonication. Amidosulfobetaine-16 is a zwitterionic lipid and dipalmitoyl-sn-glycero-3-phosphoethanolamine, with its functional head, provides bioconjugation capability. Under sonication, tetrahydrofuran/methanol containing amidosulfobetaine-16, dipalmitoyl-sn-glycero-3-phosphoethanolamine, and hydrophobic quantum dots are dispersed in water to form droplets. Highly water-soluble tetrahydrofuran/methanol in droplets is further displaced by water, which induces the lipid self-assembling on hydrophobic surface of quantum dots and thus forms water soluble zwitterionic quantum dots. The prepared zwitterionic quantum dots maintain colloidal stability in aqueous solutions with high salinity and over a wide pH range. They are also able to be conjugated with biomolecules for bioassay with minimal nonspecific binding. Copyright © 2014 Elsevier Inc. All rights reserved.

In vivo cation exchange in quantum dots for tumor-specific imaging.

PubMed

Liu, Xiangyou; Braun, Gary B; Qin, Mingde; Ruoslahti, Erkki; Sugahara, Kazuki N

2017-08-24

In vivo tumor imaging with nanoprobes suffers from poor tumor specificity. Here, we introduce a nanosystem, which allows selective background quenching to gain exceptionally tumor-specific signals. The system uses near-infrared quantum dots and a membrane-impermeable etchant, which serves as a cation donor. The etchant rapidly quenches the quantum dots through cation exchange (ionic etching), and facilitates renal clearance of metal ions released from the quantum dots. The quantum dots are intravenously delivered into orthotopic breast and pancreas tumors in mice by using the tumor-penetrating iRGD peptide. Subsequent etching quenches excess quantum dots, leaving a highly tumor-specific signal provided by the intact quantum dots remaining in the extravascular tumor cells and fibroblasts. No toxicity is noted. The system also facilitates the detection of peritoneal tumors with high specificity upon intraperitoneal tumor targeting and selective etching of excess untargeted quantum dots. In vivo cation exchange may be a promising strategy to enhance specificity of tumor imaging.The imaging of tumors in vivo using nanoprobes has been challenging due to the lack of sufficient tumor specificity. Here, the authors develop a tumor-specific quantum dot system that permits in vivo cation exchange to achieve selective background quenching and high tumor-specific imaging.

Synthesis of Cd-free InP/ZnS Quantum Dots Suitable for Biomedical Applications.

PubMed

Ellis, Matthew A; Grandinetti, Giovanna; Fichter, Katye M; Fichter, Kathryn M

2016-02-06

Fluorescent nanocrystals, specifically quantum dots, have been a useful tool for many biomedical applications. For successful use in biological systems, quantum dots should be highly fluorescent and small/monodisperse in size. While commonly used cadmium-based quantum dots possess these qualities, they are potentially toxic due to the possible release of Cd(2+) ions through nanoparticle degradation. Indium-based quantum dots, specifically InP/ZnS, have recently been explored as a viable alternative to cadmium-based quantum dots due to their relatively similar fluorescence characteristics and size. The synthesis presented here uses standard hot-injection techniques for effective nanoparticle growth; however, nanoparticle properties such as size, emission wavelength, and emission intensity can drastically change due to small changes in the reaction conditions. Therefore, reaction conditions such temperature, reaction duration, and precursor concentration should be maintained precisely to yield reproducible products. Because quantum dots are not inherently soluble in aqueous solutions, they must also undergo surface modification to impart solubility in water. In this protocol, an amphiphilic polymer is used to interact with both hydrophobic ligands on the quantum dot surface and bulk solvent water molecules. Here, a detailed protocol is provided for the synthesis of highly fluorescent InP/ZnS quantum dots that are suitable for use in biomedical applications.

Synthesis of Cd-free InP/ZnS Quantum Dots Suitable for Biomedical Applications

PubMed Central

Ellis, Matthew A.; Grandinetti, Giovanna; Fichter, Katye M.

2016-01-01

Fluorescent nanocrystals, specifically quantum dots, have been a useful tool for many biomedical applications. For successful use in biological systems, quantum dots should be highly fluorescent and small/monodisperse in size. While commonly used cadmium-based quantum dots possess these qualities, they are potentially toxic due to the possible release of Cd2+ ions through nanoparticle degradation. Indium-based quantum dots, specifically InP/ZnS, have recently been explored as a viable alternative to cadmium-based quantum dots due to their relatively similar fluorescence characteristics and size. The synthesis presented here uses standard hot-injection techniques for effective nanoparticle growth; however, nanoparticle properties such as size, emission wavelength, and emission intensity can drastically change due to small changes in the reaction conditions. Therefore, reaction conditions such temperature, reaction duration, and precursor concentration should be maintained precisely to yield reproducible products. Because quantum dots are not inherently soluble in aqueous solutions, they must also undergo surface modification to impart solubility in water. In this protocol, an amphiphilic polymer is used to interact with both hydrophobic ligands on the quantum dot surface and bulk solvent water molecules. Here, a detailed protocol is provided for the synthesis of highly fluorescent InP/ZnS quantum dots that are suitable for use in biomedical applications. PMID:26891282

Internalization of targeted quantum dots by brain capillary endothelial cells in vivo.

PubMed

Paris-Robidas, Sarah; Brouard, Danny; Emond, Vincent; Parent, Martin; Calon, Frédéric

2016-04-01

Receptors located on brain capillary endothelial cells forming the blood-brain barrier are the target of most brain drug delivery approaches. Yet, direct subcellular evidence of vectorized transport of nanoformulations into the brain is lacking. To resolve this question, quantum dots were conjugated to monoclonal antibodies (Ri7) targeting the murine transferrin receptor. Specific transferrin receptor-mediated endocytosis of Ri7-quantum dots was first confirmed in N2A and bEnd5 cells. After intravenous injection in mice, Ri7-quantum dots exhibited a fourfold higher volume of distribution in brain tissues, compared to controls. Immunofluorescence analysis showed that Ri7-quantum dots were sequestered throughout the cerebral vasculature 30 min, 1 h, and 4 h post injection, with a decline of signal intensity after 24 h. Transmission electron microscopic studies confirmed that Ri7-quantum dots were massively internalized by brain capillary endothelial cells, averaging 37 ± 4 Ri7-quantum dots/cell 1 h after injection. Most quantum dots within brain capillary endothelial cells were observed in small vesicles (58%), with a smaller proportion detected in tubular structures or in multivesicular bodies. Parenchymal penetration of Ri7-quantum dots was extremely low and comparable to control IgG. Our results show that systemically administered Ri7-quantum dots complexes undergo extensive endocytosis by brain capillary endothelial cells and open the door for novel therapeutic approaches based on brain endothelial cell drug delivery. © The Author(s) 2015.

Different valence Sn doping - A simple way to detect oxygen concentration variation of ZnO quantum dots synthesized under ultrasonic irradiation.

PubMed

Yang, Weimin; Zhang, Bing; Zhang, Qitu; Wang, Lixi; Song, Bo; Wu, Fan; Wong, C P

2017-09-01

An ultrasonic method is employed to synthesize the Sn doped Zn 0.95 Sn 0.05 O quantum dots with green light emission. Sn 2+ and Sn 4+ ions are used to create different optical defects inside Zn 0.95 Sn 0.05 O quantum dots and the changing trend of oxygen concentration under different ultrasonic irradiation power are investigated. The photoluminescence spectra are employed to characterize the optical defects of Zn 0.95 Sn 0.05 O quantum dots. The UV-vis spectra are used to study the band gap of Zn 0.95 Sn 0.05 O quantum dots, which is influenced by their sizes. The results indicate that ultrasonic power would influence the size of Zn 0.95 Sn 0.05 O quantum dots as well as the type and quantity of defects in ZnO quantum dots. Changing trends in size of Sn 2+ and Sn 4+ doped Zn 0.95 Sn 0.05 O quantum dots are quite similar with each other, while the changing trends in optical defects types and concentration of Sn 2+ and Sn 4+ doped Zn 0.95 Sn 0.05 O quantum dots are different. The difference of the optical defects concentration changing between Sn 2+ doped Zn 0.95 Sn 0.05 O quantum dots (V O defects) and Sn 4+ doped Zn 0.95 Sn 0.05 O quantum dots (O Zn and O i defects) shows that the formation process of ZnO under ultrasonic irradiation wiped oxygen out. Copyright © 2017 Elsevier B.V. All rights reserved.

Probing the structural dependency of photoinduced properties of colloidal quantum dots using metal-oxide photo-active substrates.

PubMed

Patty, Kira; Sadeghi, Seyed M; Campbell, Quinn; Hamilton, Nathan; West, Robert G; Mao, Chuanbin

2014-09-21

We used photoactive substrates consisting of about 1 nm coating of a metal oxide on glass substrates to investigate the impact of the structures of colloidal quantum dots on their photophysical and photochemical properties. We showed during irradiation these substrates can interact uniquely with such quantum dots, inducing distinct forms of photo-induced processes when they have different cores, shells, or ligands. In particular, our results showed that for certain types of core-shell quantum dot structures an ultrathin layer of a metal oxide can reduce suppression of quantum efficiency of the quantum dots happening when they undergo extensive photo-oxidation. This suggests the possibility of shrinking the sizes of quantum dots without significant enhancement of their non-radiative decay rates. We show that such quantum dots are not influenced significantly by Coulomb blockade or photoionization, while those without a shell can undergo a large amount of photo-induced fluorescence enhancement via such blockade when they are in touch with the metal oxide.

Probing the structural dependency of photoinduced properties of colloidal quantum dots using metal-oxide photo-active substrates

PubMed Central

Patty, Kira; Sadeghi, Seyed M.; Campbell, Quinn; Hamilton, Nathan; West, Robert G.; Mao, Chuanbin

2014-01-01

We used photoactive substrates consisting of about 1 nm coating of a metal oxide on glass substrates to investigate the impact of the structures of colloidal quantum dots on their photophysical and photochemical properties. We showed during irradiation these substrates can interact uniquely with such quantum dots, inducing distinct forms of photo-induced processes when they have different cores, shells, or ligands. In particular, our results showed that for certain types of core-shell quantum dot structures an ultrathin layer of a metal oxide can reduce suppression of quantum efficiency of the quantum dots happening when they undergo extensive photo-oxidation. This suggests the possibility of shrinking the sizes of quantum dots without significant enhancement of their non-radiative decay rates. We show that such quantum dots are not influenced significantly by Coulomb blockade or photoionization, while those without a shell can undergo a large amount of photo-induced fluorescence enhancement via such blockade when they are in touch with the metal oxide. PMID:25316953

Photosensitization of ZnO nanowires with CdSe quantum dots for photovoltaic devices.

PubMed

Leschkies, Kurtis S; Divakar, Ramachandran; Basu, Joysurya; Enache-Pommer, Emil; Boercker, Janice E; Carter, C Barry; Kortshagen, Uwe R; Norris, David J; Aydil, Eray S

2007-06-01

We combine CdSe semiconductor nanocrystals (or quantum dots) and single-crystal ZnO nanowires to demonstrate a new type of quantum-dot-sensitized solar cell. An array of ZnO nanowires was grown vertically from a fluorine-doped tin oxide conducting substrate. CdSe quantum dots, capped with mercaptopropionic acid, were attached to the surface of the nanowires. When illuminated with visible light, the excited CdSe quantum dots injected electrons across the quantum dot-nanowire interface. The morphology of the nanowires then provided the photoinjected electrons with a direct electrical pathway to the photoanode. With a liquid electrolyte as the hole transport medium, quantum-dot-sensitized nanowire solar cells exhibited short-circuit currents ranging from 1 to 2 mA/cm2 and open-circuit voltages of 0.5-0.6 V when illuminated with 100 mW/cm2 simulated AM1.5 spectrum. Internal quantum efficiencies as high as 50-60% were also obtained.

Spectroscopy of Single AlInAs Quantum Dots

NASA Astrophysics Data System (ADS)

Derebezov, I. A.; Gaisler, A. V.; Gaisler, V. A.; Dmitriev, D. V.; Toropov, A. I.; Kozhukhov, A. S.; Shcheglov, D. V.; Latyshev, A. V.; Aseev, A. L.

2018-03-01

A system of quantum dots based on Al x In1- x As/Al y Ga1- y As solid solutions is investigated. The use of Al x In1- x As wide-gap solid solutions as the basis of quantum dots substantially extends the spectral emission range to the short-wavelength region, including the wavelength region near 770 nm, which is of interest for the development of aerospace systems of quantum cryptography. The optical characteristics of Al x In1- x As single quantum dots grown by the Stranski-Krastanov mechanism were studied by cryogenic microphotoluminescence. The statistics of the emission of single quantum dot excitons was studied using a Hanbury Brown-Twiss interferometer. The pair photon correlation function indicates the sub-Poissonian nature of the emission statistics, which directly confirms the possibility of developing single-photon emitters based on Al x In1- x As quantum dots. The fine structure of quantum dot exciton states was investigated at wavelengths near 770 nm. The splitting of the exciton states is found to be similar to the natural width of exciton lines, which is of great interest for the development of entangled photon pair emitters based on Al x In1- x As quantum dots.

Entanglement in a quantum neural network based on quantum dots

NASA Astrophysics Data System (ADS)

Altaisky, M. V.; Zolnikova, N. N.; Kaputkina, N. E.; Krylov, V. A.; Lozovik, Yu E.; Dattani, N. S.

2017-05-01

We studied the quantum correlations between the nodes in a quantum neural network built of an array of quantum dots with dipole-dipole interaction. By means of the quasiadiabatic path integral simulation of the density matrix evolution in a presence of the common phonon bath we have shown the coherence in such system can survive up to the liquid nitrogen temperature of 77 K and above. The quantum correlations between quantum dots are studied by means of calculation of the entanglement of formation in a pair of quantum dots with the typical dot size of a few nanometers and interdot distance of the same order. We have shown that the proposed quantum neural network can keep the mixture of entangled states of QD pairs up to the above mentioned high temperatures.

Transient Evolutional Dynamics of Quantum-Dot Molecular Phase Coherence for Sensitive Optical Switching

NASA Astrophysics Data System (ADS)

Shen, Jian Qi; Gu, Jing

2018-04-01

Atomic phase coherence (quantum interference) in a multilevel atomic gas exhibits a number of interesting phenomena. Such an atomic quantum coherence effect can be generalized to a quantum-dot molecular dielectric. Two quantum dots form a quantum-dot molecule, which can be described by a three-level Λ-configuration model { |0> ,|1> ,|2> } , i.e., the ground state of the molecule is the lower level |0> and the highly degenerate electronic states in the two quantum dots are the two upper levels |1> ,|2> . The electromagnetic characteristics due to the |0>-|1> transition can be controllably manipulated by a tunable gate voltage (control field) that drives the |2>-|1> transition. When the gate voltage is switched on, the quantum-dot molecular state can evolve from one steady state (i.e., |0>-|1> two-level dressed state) to another steady state (i.e., three-level coherent-population-trapping state). In this process, the electromagnetic characteristics of a quantum-dot molecular dielectric, which is modified by the gate voltage, will also evolve. In this study, the transient evolutional behavior of the susceptibility of a quantum-dot molecular thin film and its reflection spectrum are treated by using the density matrix formulation of the multilevel systems. The present field-tunable and frequency-sensitive electromagnetic characteristics of a quantum-dot molecular thin film, which are sensitive to the applied gate voltage, can be utilized to design optical switching devices.

Quantum Dots in a Polymer Composite: A Convenient Particle-in-a-Box Laboratory Experiment

ERIC Educational Resources Information Center

Rice, Charles V.; Giffin, Guinevere A.

2008-01-01

Semiconductor quantum dots are at the forefront of materials science chemistry with applications in biological imaging and photovoltaic technologies. We have developed a simple laboratory experiment to measure the quantum-dot size from fluorescence spectra. A major roadblock of quantum-dot based exercises is the particle synthesis and handling;…

The influence of bio-conjugation on photoluminescence of CdSe/ZnS quantum dots

NASA Astrophysics Data System (ADS)

Torchynska, Tetyana V.; Vorobiev, Yuri V.; Makhniy, Victor P.; Horley, Paul P.

2014-11-01

We report a considerable blue shift in the luminescence spectra of CdSe/ZnS quantum dots conjugated to anti-interleukin-10 antibodies. This phenomenon can be explained theoretically by accounting for bio-conjugation as a process causing electrostatic interaction between a quantum dot and an antibody, which reduces effective volume of the dot core. To solve the Schrödinger equation for an exciton confined in the quantum dot, we use mirror boundary conditions that were successfully tested for different geometries of quantum wells.

Single photon emission from charged excitons in CdTe/ZnTe quantum dots

NASA Astrophysics Data System (ADS)

Belyaev, K. G.; Rakhlin, M. V.; Sorokin, S. V.; Klimko, G. V.; Gronin, S. V.; Sedova, I. V.; Mukhin, I. S.; Ivanov, S. V.; Toropov, A. A.

2017-11-01

We report on micro-photoluminescence studies of individual self-organized CdTe/ZnTe quantum dots intended for single-photon-source applications in a visible spectral range. The quantum dots surface density below 1010 per cm2 was achieved by using a thermally activated regime of molecular beam epitaxy that allowed fabrication of etched mesa-structures containing only a few emitting quantum dots. The single photon emission with the autocorrelation function g(2)(0)<0.2 was detected and identified as recombination of charged excitons in the individual quantum dot.

Enhanced hot-carrier cooling and ultrafast spectral diffusion in strongly coupled PbSe quantum-dot solids.

PubMed

Gao, Yunan; Talgorn, Elise; Aerts, Michiel; Trinh, M Tuan; Schins, Juleon M; Houtepen, Arjan J; Siebbeles, Laurens D A

2011-12-14

PbSe quantum-dot solids are of great interest for low cost and efficient photodetectors and solar cells. We have prepared PbSe quantum-dot solids with high charge carrier mobilities using layer-by-layer dip-coating with 1,2-ethanediamine as substitute capping ligands. Here we present a time and energy resolved transient absorption spectroscopy study on the kinetics of photogenerated charge carriers, focusing on 0-5 ps after photoexcitation. We compare the observed carrier kinetics to those for quantum dots in dispersion and show that the intraband carrier cooling is significantly faster in quantum-dot solids. In addition we find that carriers diffuse from higher to lower energy sites in the quantum-dot solid within several picoseconds.

Synthesis and Properties of Water-Soluble Blue-Emitting Mn-Alloyed CdTe Quantum Dots

NASA Astrophysics Data System (ADS)

Tynkevych, Olena; Karavan, Volodymyr; Vorona, Igor; Filonenko, Svitlana; Khalavka, Yuriy

2018-05-01

In this work, we prepared CdTe quantum dots, and series of Cd1-xMnxTe-alloyed quantum dots with narrow size distribution by an ion-exchange reaction in water solution. We found that the photoluminescence peaks are shifted to higher energies with the increasing Mn2+ content. So far, this is the first report of blue-emitting CdTe-based quantum dots. By means of cyclic voltammetry, we detected features of electrochemical activity of manganese energy levels formed inside the Cd1-xMnxTe-alloyed quantum dot band gap. This allowed us to estimate their energy position. We also demonstrate paramagnetic behavior for Cd1-xMnxTe-alloyed quantum dots which confirmed the successful ion-exchange reaction.

Silicon Quantum Dots with Counted Antimony Donor Implants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Singh, Meenakshi; Pacheco, Jose L.; Perry, Daniel Lee

2015-10-01

Deterministic control over the location and number of donors is crucial to donor spin quantum bits (qubits) in semiconductor based quantum computing. A focused ion beam is used to implant close to quantum dots. Ion detectors are integrated next to the quantum dots to sense the implants. The numbers of ions implanted can be counted to a precision of a single ion. Regular coulomb blockade is observed from the quantum dots. Charge offsets indicative of donor ionization, are observed in devices with counted implants.

Demonstration of quantum entanglement between a single electron spin confined to an InAs quantum dot and a photon.

PubMed

Schaibley, J R; Burgers, A P; McCracken, G A; Duan, L-M; Berman, P R; Steel, D G; Bracker, A S; Gammon, D; Sham, L J

2013-04-19

The electron spin state of a singly charged semiconductor quantum dot has been shown to form a suitable single qubit for quantum computing architectures with fast gate times. A key challenge in realizing a useful quantum dot quantum computing architecture lies in demonstrating the ability to scale the system to many qubits. In this Letter, we report an all optical experimental demonstration of quantum entanglement between a single electron spin confined to a single charged semiconductor quantum dot and the polarization state of a photon spontaneously emitted from the quantum dot's excited state. We obtain a lower bound on the fidelity of entanglement of 0.59±0.04, which is 84% of the maximum achievable given the timing resolution of available single photon detectors. In future applications, such as measurement-based spin-spin entanglement which does not require sub-nanosecond timing resolution, we estimate that this system would enable near ideal performance. The inferred (usable) entanglement generation rate is 3×10(3) s(-1). This spin-photon entanglement is the first step to a scalable quantum dot quantum computing architecture relying on photon (flying) qubits to mediate entanglement between distant nodes of a quantum dot network.

Nanofabrication of Gate-defined GaAs/AlGaAs Lateral Quantum Dots

PubMed Central

Bureau-Oxton, Chloé; Camirand Lemyre, Julien; Pioro-Ladrière, Michel

2013-01-01

A quantum computer is a computer composed of quantum bits (qubits) that takes advantage of quantum effects, such as superposition of states and entanglement, to solve certain problems exponentially faster than with the best known algorithms on a classical computer. Gate-defined lateral quantum dots on GaAs/AlGaAs are one of many avenues explored for the implementation of a qubit. When properly fabricated, such a device is able to trap a small number of electrons in a certain region of space. The spin states of these electrons can then be used to implement the logical 0 and 1 of the quantum bit. Given the nanometer scale of these quantum dots, cleanroom facilities offering specialized equipment- such as scanning electron microscopes and e-beam evaporators- are required for their fabrication. Great care must be taken throughout the fabrication process to maintain cleanliness of the sample surface and to avoid damaging the fragile gates of the structure. This paper presents the detailed fabrication protocol of gate-defined lateral quantum dots from the wafer to a working device. Characterization methods and representative results are also briefly discussed. Although this paper concentrates on double quantum dots, the fabrication process remains the same for single or triple dots or even arrays of quantum dots. Moreover, the protocol can be adapted to fabricate lateral quantum dots on other substrates, such as Si/SiGe. PMID:24300661

Strain-induced formation of fourfold symmetric SiGe quantum dot molecules.

PubMed

Zinovyev, V A; Dvurechenskii, A V; Kuchinskaya, P A; Armbrister, V A

2013-12-27

The strain field distribution at the surface of a multilayer structure with disklike SiGe nanomounds formed by heteroepitaxy is exploited to arrange the symmetric quantum dot molecules typically consisting of four elongated quantum dots ordered along the [010] and [100] directions. The morphological transition from fourfold quantum dot molecules to continuous fortresslike quantum rings with an increasing amount of deposited Ge is revealed. We examine key mechanisms underlying the formation of lateral quantum dot molecules by using scanning tunneling microscopy and numerical calculations of the strain energy distribution on the top of disklike SiGe nanomounds. Experimental data are well described by a simple thermodynamic model based on the accurate evaluation of the strain dependent part of the surface chemical potential. The spatial arrangement of quantum dots inside molecules is attributed to the effect of elastic property anisotropy.

Nanosecond-timescale spin transfer using individual electrons in a quadruple-quantum-dot device

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baart, T. A.; Jovanovic, N.; Vandersypen, L. M. K.

2016-07-25

The ability to coherently transport electron-spin states between different sites of gate-defined semiconductor quantum dots is an essential ingredient for a quantum-dot-based quantum computer. Previous shuttles using electrostatic gating were too slow to move an electron within the spin dephasing time across an array. Here, we report a nanosecond-timescale spin transfer of individual electrons across a quadruple-quantum-dot device. Utilizing enhanced relaxation rates at a so-called hot spot, we can upper bound the shuttle time to at most 150 ns. While actual shuttle times are likely shorter, 150 ns is already fast enough to preserve spin coherence in, e.g., silicon based quantum dots.more » This work therefore realizes an important prerequisite for coherent spin transfer in quantum dot arrays.« less

Antiresonance and decoupling in electronic transport through parallel-coupled quantum-dot structures with laterally-coupled Majorana zero modes

NASA Astrophysics Data System (ADS)

Zhang, Ya-Jing; Zhang, Lian-Lian; Jiang, Cui; Gong, Wei-Jiang

2018-02-01

We theoretically investigate the electronic transport through a parallel-coupled multi-quantum-dot system, in which the terminal dots of a one-dimensional quantum-dot chain are embodied in the two arms of an Aharonov-Bohm interferometer. It is found that in the structures of odd(even) dots, all their even(odd) molecular states have opportunities to decouple from the leads, and in this process antiresonance occurs which are accordant with the odd(even)-numbered eigenenergies of the sub-molecule without terminal dots. Next when Majorana zero modes are introduced to couple laterally to the terminal dots, the antiresonance and decoupling phenomena still co-exist in the quantum transport process. Such a result can be helpful in understanding the special influence of Majorana zero mode on the electronic transport through quantum-dot systems.

Optical Fiber Sensing Using Quantum Dots

PubMed Central

Jorge, Pedro; Martins, Manuel António; Trindade, Tito; Santos, José Luís; Farahi, Faramarz

2007-01-01

Recent advances in the application of semiconductor nanocrystals, or quantum dots, as biochemical sensors are reviewed. Quantum dots have unique optical properties that make them promising alternatives to traditional dyes in many luminescence based bioanalytical techniques. An overview of the more relevant progresses in the application of quantum dots as biochemical probes is addressed. Special focus will be given to configurations where the sensing dots are incorporated in solid membranes and immobilized in optical fibers or planar waveguide platforms. PMID:28903308

The role of surface ligands in determining the electronic properties of quantum dot solids and their impact on photovoltaic figure of merits.

PubMed

Goswami, Prasenjit N; Mandal, Debranjan; Rath, Arup K

2018-01-18

Surface chemistry plays a crucial role in determining the electronic properties of quantum dot solids and may well be the key to mitigate loss processes involved in quantum dot solar cells. Surface ligands help to maintain the shape and size of the individual dots in solid films, to preserve the clean energy band gap of the individual particles and to control charge carrier conduction across solid films, in turn regulating their performance in photovoltaic applications. In this report, we show that the changes in size, shape and functional groups of small chain organic ligands enable us to modulate mobility, dielectric constant and carrier doping density of lead sulfide quantum dot solids. Furthermore, we correlate these results with performance, stability and recombination processes in the respective photovoltaic devices. Our results highlight the critical role of surface chemistry in the electronic properties of quantum dots. The role of the size, functionality and the surface coverage of the ligands in determining charge transport properties and the stability of quantum dot solids have been discussed. Our findings, when applied in designing new ligands with higher mobility and improved passivation of quantum dot solids, can have important implications for the development of high-performance quantum dot solar cells.

Record Charge Carrier Diffusion Length in Colloidal Quantum Dot Solids via Mutual Dot-To-Dot Surface Passivation.

PubMed

Carey, Graham H; Levina, Larissa; Comin, Riccardo; Voznyy, Oleksandr; Sargent, Edward H

2015-06-03

Through a combination of chemical and mutual dot-to-dot surface passivation, high-quality colloidal quantum dot solids are fabricated. The joint passivation techniques lead to a record diffusion length for colloidal quantum dots of 230 ± 20 nm. The technique is applied to create thick photovoltaic devices that exhibit high current density without losing fill factor. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

First principles study of edge carboxylated graphene quantum dots

NASA Astrophysics Data System (ADS)

Abdelsalam, Hazem; Elhaes, Hanan; Ibrahim, Medhat A.

2018-05-01

The structure stability and electronic properties of edge carboxylated hexagonal and triangular graphene quantum dots are investigated using density functional theory. The calculated binding energies show that the hexagonal clusters with armchair edges have the highest stability among all the quantum dots. The binding energy of carboxylated graphene quantum dots increases by increasing the number of carboxyl groups. Our study shows that the total dipole moment significantly increases by adding COOH with the highest value observed in triangular clusters. The edge states in triangular graphene quantum dots with zigzag edges produce completely different energy spectrum from other dots: (a) the energy gap in triangular zigzag is very small as compared to other clusters and (b) the highest occupied molecular orbital is localized at the edges which is in contrast to other clusters where it is distributed over the cluster surface. The enhanced reactivity and the controllable energy gap by shape and edge termination make graphene quantum dots ideal for various nanodevice applications such as sensors. The infrared spectra are presented to confirm the stability of the quantum dots.

Small GSH-Capped CuInS2 Quantum Dots: MPA-Assisted Aqueous Phase Transfer and Bioimaging Applications.

PubMed

Zhao, Chuanzhen; Bai, Zelong; Liu, Xiangyou; Zhang, Yijia; Zou, Bingsuo; Zhong, Haizheng

2015-08-19

An efficient ligand exchange strategy for aqueous phase transfer of hydrophobic CuInS2/ZnS quantum dots was developed by employing glutathione (GSH) and mercaptopropionic acid (MPA) as the ligands. The whole process takes less than 20 min and can be scaled up to gram amount. The material characterizations show that the final aqueous soluble samples are solely capped with GSH on the surface. Importantly, these GSH-capped CuInS2/ZnS quantum dots have small size (hydrodynamic diameter <10 nm), moderate fluorescent properties (up to 34%) as well as high stability in aqueous solutions (stable for more than three months in 4 °C without any significant fluorescence quenching). Moreover, this ligand exchange strategy is also versatile for the aqueous phase transfer of other hydrophobic quantum dots, for instance, CuInSe2 and CdSe/ZnS quantum dots. We further demonstrated that GSH-capped quantum dots could be suitable fluorescence markers to penetrate cell membrane and image the cells. In addition, the GSH-capped CuInS2 quantum dots also have potential use in other fields such as photocatalysis and quantum dots sensitized solar cells.

The Stanford Nanocharacterization Laboratory (SNL) and Recent Applications of an Aberration-Corrected Environmental Transmission Electron Microscope

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zschech, Ehrenfried; Sinclair, Robert; Kempen, Paul Joseph

2014-04-30

Here, this article describes the establishment, over a period of 10 years or so, of a multi-user, institution-wide facility for the characterization of materials and devices at the nanoscale. Emphasis is placed on the type of equipment that we have found to be most useful for our users, and the business strategy that maintains its operations. A central component of our facility is an aberration-corrected environmental transmission electron microscope and its application is summarized in the studies of plasmon energies of silver nanoparticles, the band gap of PbS quantum dots, atomic site occupancy near grain boundaries in yttria stabilized zirconia,more » the lithiation of silicon nanoparticles, in situ observations on carbon nanotube oxidation and the electron tomography of varicella zoster virus nucleocapsids.« less

Carbon nanotube/metal-sulfide composite flexible electrodes for high-performance quantum dot-sensitized solar cells and supercapacitors

PubMed Central

Muralee Gopi, Chandu V. V.; Ravi, Seenu; Rao, S. Srinivasa; Eswar Reddy, Araveeti; Kim, Hee-Je

2017-01-01

Carbon nanotubes (CNT) and metal sulfides have attracted considerable attention owing to their outstanding properties and multiple application areas, such as electrochemical energy conversion and energy storage. Here we describes a cost-effective and facile solution approach to the preparation of metal sulfides (PbS, CuS, CoS, and NiS) grown directly on CNTs, such as CNT/PbS, CNT/CuS, CNT/CoS, and CNT/NiS flexible electrodes for quantum dot-sensitized solar cells (QDSSCs) and supercapacitors (SCs). X-ray photoelectron spectroscopy, X-ray diffraction, and transmission electron microscopy confirmed that the CNT network was covered with high-purity metal sulfide compounds. QDSSCs equipped with the CNT/NiS counter electrode (CE) showed an impressive energy conversion efficiency (η) of 6.41% and remarkable stability. Interestingly, the assembled symmetric CNT/NiS-based polysulfide SC device exhibited a maximal energy density of 35.39 W h kg−1 and superior cycling durability with 98.39% retention after 1,000 cycles compared to the other CNT/metal-sulfides. The elevated performance of the composites was attributed mainly to the good conductivity, high surface area with mesoporous structures and stability of the CNTs and the high electrocatalytic activity of the metal sulfides. Overall, the designed composite CNT/metal-sulfide electrodes offer an important guideline for the development of next level energy conversion and energy storage devices. PMID:28422182

Accelerating FRET between Near-Infrared Emitting Quantum Dots Using a Molecular J-Aggregate as an Exciton Bridge.

PubMed

Wang, Chen; Weiss, Emily A

2017-09-13

Fast energy transfer (EnT) among quantum dots (QDs) with near-infrared (NIR) emission is essential for fully exploiting their light harvesting and photon downconversion (multiexciton generation) abilities. This paper demonstrates a relayed EnT mechanism that accelerates the migration of NIR excitons between PbS QDs by a factor of 20 from that of one-step EnT through a polyelectrolyte and even a factor of ∼2 from that of one-step EnT between QDs in direct contact, by employing a J-aggregate (J-agg) of a cyanine dye as an exciton bridge. The donor QDs, acceptor QDs, and J-agg are electrostatically assembled into a sandwich structure with layer-by-layer deposition. Estimates of EnT rate and yield from transient and steady-state absorption and photoluminescence spectroscopies show that the rate-limiting step in the relay is EnT from the donor QD to the J-agg, while EnT from the J-agg to the acceptor QD occurs in <10 ps. A comparison of this system to the analogous solution-phase system suggests that the overall donor-to-acceptor EnT yield in the relay (18%) can be improved by depositing the J-agg with more intermolecular order. This work demonstrates the viability of relayed EnT through a molecular bridge as a strategy for accelerating long-distance exciton migration in assemblies of QDs, in particular in the near-infrared.

Quantum dot immunoassays in renewable surface column and 96-well plate formats for the fluorescence detection of Botulinum neurotoxin using high-affinity antibodies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Warner, Marvin G.; Grate, Jay W.; Tyler, Abby J.

2009-09-01

A fluorescence sandwich immunoassay using high affinity antibodies and quantum dot (QD) reporters has been developed for detection of botulinum toxin serotype A (BoNT/A). For the development of the assay, a nontoxic recombinant fragment of the holotoxin (BoNT/A-HC-fragment) has been used as a structurally valid simulant for the full toxin molecule. The antibodies used, AR4 and RAZ1, bind to nonoverlapping epitopes present on both the full toxin and on the recombinant fragment. In one format, the immunoassay is carried out in a 96-well plate with detection in a standard plate reader. Detection down to 31 pM of the BoNT/Hc-fragment wasmore » demonstrated with a total incubation time of 3 hours, using AR4 as the capture antibody and QD-coupled RAZ1 as the reporter. In a second format, the AR4 capture antibody was coupled to Sepharose beads, and the immunochemical reactions were carried out in microcentrifuge tubes with an incubation time of 1 hour. These beads were subsequently captured and concentrated in a rotating rod “renewable surface” flow cell as part of a sequential injection fluidic system. This flow cell was equipped with a fiber optic system for fluorescence measurements. In PBS buffer solution matrix, the BoNT/A-HC-fragment was detected to concentrations as low as 5 pM using the fluidic measurement approach.« less

Self-assembled InN quantum dots on side facets of GaN nanowires

NASA Astrophysics Data System (ADS)

Bi, Zhaoxia; Ek, Martin; Stankevic, Tomas; Colvin, Jovana; Hjort, Martin; Lindgren, David; Lenrick, Filip; Johansson, Jonas; Wallenberg, L. Reine; Timm, Rainer; Feidenhans'l, Robert; Mikkelsen, Anders; Borgström, Magnus T.; Gustafsson, Anders; Ohlsson, B. Jonas; Monemar, Bo; Samuelson, Lars

2018-04-01

Self-assembled, atomic diffusion controlled growth of InN quantum dots was realized on the side facets of dislocation-free and c-oriented GaN nanowires having a hexagonal cross-section. The nanowires were synthesized by selective area metal organic vapor phase epitaxy. A 3 Å thick InN wetting layer was observed after growth, on top of which the InN quantum dots formed, indicating self-assembly in the Stranski-Krastanow growth mode. We found that the InN quantum dots can be tuned to nucleate either preferentially at the edges between GaN nanowire side facets, or directly on the side facets by tuning the adatom migration by controlling the precursor supersaturation and growth temperature. Structural characterization by transmission electron microscopy and reciprocal space mapping show that the InN quantum dots are close to be fully relaxed (residual strain below 1%) and that the c-planes of the InN quantum dots are tilted with respect to the GaN core. The strain relaxes mainly by the formation of misfit dislocations, observed with a periodicity of 3.2 nm at the InN and GaN hetero-interface. The misfit dislocations introduce I1 type stacking faults (…ABABCBC…) in the InN quantum dots. Photoluminescence investigations of the InN quantum dots show that the emissions shift to higher energy with reduced quantum dot size, which we attribute to increased quantum confinement.

Enhancement of emission efficiency of colloidal CdSe quantum dots on silicon substrate via an ultra-thin layer of aluminum oxide.

PubMed

Patty, K; Sadeghi, S M; Nejat, A; Mao, C-B

2014-04-18

We demonstrate that an ultra-thin layer of aluminum oxide can significantly enhance the emission efficiency of colloidal quantum dots on a Si substrate. For an ensemble of single quantum dots, our results show that this super brightening process can increase the fluorescence of CdSe quantum dots, forming well-resolved spectra, while in the absence of this layer the emission remains mostly at the noise level. We demonstrate that this process can be further enhanced with irradiation of the quantum dots, suggesting a significant photo-induced fluorescence enhancement via considerable suppression of non-radiative decay channels of the quantum dots. We study the impact of the Al oxide thickness on Si and interdot interactions, and discuss the results in terms of photo-induced catalytic properties of the Al oxide and the effects of such an oxide on the Coulomb blockade responsible for suppression of photo-ionization of the quantum dots.

Electrochemical Study and Applications of Selective Electrodeposition of Silver on Quantum Dots.

PubMed

Martín-Yerga, Daniel; Rama, Estefanía Costa; Costa-García, Agustín

2016-04-05

In this work, selective electrodeposition of silver on quantum dots is described. The particular characteristics of the nanostructured silver thus obtained are studied by electrochemical and microscopic techniques. On one hand, quantum dots were found to catalyze the silver electrodeposition, and on the other hand, a strong adsorption between electrodeposited silver and quantum dots was observed, indicated by two silver stripping processes. Nucleation of silver nanoparticles followed different mechanisms depending on the surface (carbon or quantum dots). Voltammetric and confocal microscopy studies showed the great influence of electrodeposition time on surface coating, and high-resolution transmission electron microscopy (HRTEM) imaging confirmed the initial formation of Janus-like Ag@QD nanoparticles in this process. By use of moderate electrodeposition conditions such as 50 μM silver, -0.1 V, and 60 s, the silver was deposited only on quantum dots, allowing the generation of localized nanostructured electrode surfaces. This methodology can also be employed for sensing applications, showing a promising ultrasensitive electrochemical method for quantum dot detection.

Rhizopus stolonifer mediated biosynthesis of biocompatible cadmium chalcogenide quantum dots.

PubMed

Mareeswari, P; Brijitta, J; Harikrishna Etti, S; Meganathan, C; Kaliaraj, Gobi Saravanan

2016-12-01

We report an efficient method to biosynthesize biocompatible cadmium telluride and cadmium sulphide quantum dots from the fungus Rhizopus stolonifer. The suspension of the quantum dots exhibited purple and greenish-blue luminescence respectively upon UV light illumination. Photoluminescence spectroscopy, X-ray diffraction, and transmission electron microscopy confirms the formation of the quantum dots. From the photoluminescence spectrum the emission maxima is found to be 424 and 476nm respectively. The X-ray diffraction of the quantum dots matches with results reported in literature. The 3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide assay for cell viability evaluation carried out on 3-days transfer, inoculum 3×10 5 cells, embryonic fibroblast cells lines shows that more than 80% of the cells are viable even after 48h, indicating the biocompatible nature of the quantum dots. A good contrast in imaging has been obtained upon incorporating the quantum dots in human breast adenocarcinoma Michigan Cancer Foundation-7 cell lines. Copyright © 2016 Elsevier Inc. All rights reserved.

Designing artificial 2D crystals with site and size controlled quantum dots.

PubMed

Xie, Xuejun; Kang, Jiahao; Cao, Wei; Chu, Jae Hwan; Gong, Yongji; Ajayan, Pulickel M; Banerjee, Kaustav

2017-08-30

Ordered arrays of quantum dots in two-dimensional (2D) materials would make promising optical materials, but their assembly could prove challenging. Here we demonstrate a scalable, site and size controlled fabrication of quantum dots in monolayer molybdenum disulfide (MoS 2 ), and quantum dot arrays with nanometer-scale spatial density by focused electron beam irradiation induced local 2H to 1T phase change in MoS 2 . By designing the quantum dots in a 2D superlattice, we show that new energy bands form where the new band gap can be controlled by the size and pitch of the quantum dots in the superlattice. The band gap can be tuned from 1.81 eV to 1.42 eV without loss of its photoluminescence performance, which provides new directions for fabricating lasers with designed wavelengths. Our work constitutes a photoresist-free, top-down method to create large-area quantum dot arrays with nanometer-scale spatial density that allow the quantum dots to interfere with each other and create artificial crystals. This technique opens up new pathways for fabricating light emitting devices with 2D materials at desired wavelengths. This demonstration can also enable the assembly of large scale quantum information systems and open up new avenues for the design of artificial 2D materials.

Quantum Dots in Diagnostics and Detection: Principles and Paradigms

PubMed Central

Pisanic, T. R.; Zhang, Y.; Wang, T. H.

2014-01-01

Quantum dots are semiconductor nanocrystals that exhibit exceptional optical and electrical behaviors not found in their bulk counterparts. Following seminal work in the development of water-soluble quantum dots in the late 1990's, researchers have sought to develop interesting and novel ways of exploiting the extraordinary properties of quantum dots for biomedical applications. Since that time, over 10,000 articles have been published related to the use of quantum dots in biomedicine, many of which regard their use in detection and diagnostic bioassays. This review presents a didactic overview of fundamental physical phenomena associated with quantum dots and paradigm examples of how these phenomena can and have been readily exploited for manifold uses in nanobiotechnology with a specific focus on their implementation in in vitro diagnostic assays and biodetection. PMID:24770716

Fabrication of nanoscale heterostructures comprised of graphene-encapsulated gold nanoparticles and semiconducting quantum dots for photocatalysis.

PubMed

Li, Yuan; Chopra, Nitin

2015-05-21

Patterned growth of multilayer graphene shell encapsulated gold nanoparticles (GNPs) and their covalent linking with inorganic quantum dots are demonstrated. GNPs were grown using a xylene chemical vapor deposition process, where the surface oxidized gold nanoparticles catalyze the multilayer graphene shell growth in a single step process. The graphene shell encapsulating gold nanoparticles could be further functionalized with carboxylic groups, which were covalently linked to amine-terminated quantum dots resulting in GNP-quantum dot heterostructures. The compositions, morphologies, crystallinity, and surface functionalization of GNPs and their heterostructures with quantum dots were evaluated using microscopic, spectroscopic, and analytical methods. Furthermore, optical properties of the derived architectures were studied using both experimental methods and simulations. Finally, GNP-quantum dot heterostructures were studied for photocatalytic degradation of phenol.

Synthesis and Properties of Water-Soluble Blue-Emitting Mn-Alloyed CdTe Quantum Dots.

PubMed

Tynkevych, Olena; Karavan, Volodymyr; Vorona, Igor; Filonenko, Svitlana; Khalavka, Yuriy

2018-05-02

In this work, we prepared CdTe quantum dots, and series of Cd 1-x Mn x Te-alloyed quantum dots with narrow size distribution by an ion-exchange reaction in water solution. We found that the photoluminescence peaks are shifted to higher energies with the increasing Mn 2+ content. So far, this is the first report of blue-emitting CdTe-based quantum dots. By means of cyclic voltammetry, we detected features of electrochemical activity of manganese energy levels formed inside the Cd 1-x Mn x Te-alloyed quantum dot band gap. This allowed us to estimate their energy position. We also demonstrate paramagnetic behavior for Cd 1-x Mn x Te-alloyed quantum dots which confirmed the successful ion-exchange reaction.

Nanoscale patterning of colloidal quantum dots on transparent and metallic planar surfaces.

PubMed

Park, Yeonsang; Roh, Young-Geun; Kim, Un Jeong; Chung, Dae-Young; Suh, Hwansoo; Kim, Jineun; Cheon, Sangmo; Lee, Jaesoong; Kim, Tae-Ho; Cho, Kyung-Sang; Lee, Chang-Won

2012-09-07

The patterning of colloidal quantum dots with nanometer resolution is essential for their application in photonics and plasmonics. Several patterning approaches, such as the use of polymer composites, molecular lock-and-key methods, inkjet printing and microcontact printing of quantum dots have been recently developed. Herein, we present a simple method of patterning colloidal quantum dots for photonic nanostructures such as straight lines, rings and dot patterns either on transparent or metallic substrates. Sub-10 nm width of the patterned line could be achieved with a well-defined sidewall profile. Using this method, we demonstrate a surface plasmon launcher from a quantum dot cluster in the visible spectrum.

Probing the structural dependency of photoinduced properties of colloidal quantum dots using metal-oxide photo-active substrates

DOE Office of Scientific and Technical Information (OSTI.GOV)

Patty, Kira; Campbell, Quinn; Hamilton, Nathan

We used photoactive substrates consisting of about 1 nm coating of a metal oxide on glass substrates to investigate the impact of the structures of colloidal quantum dots on their photophysical and photochemical properties. We showed during irradiation these substrates can interact uniquely with such quantum dots, inducing distinct forms of photo-induced processes when they have different cores, shells, or ligands. In particular, our results showed that for certain types of core-shell quantum dot structures an ultrathin layer of a metal oxide can reduce suppression of quantum efficiency of the quantum dots happening when they undergo extensive photo-oxidation. This suggestsmore » the possibility of shrinking the sizes of quantum dots without significant enhancement of their non-radiative decay rates. We show that such quantum dots are not influenced significantly by Coulomb blockade or photoionization, while those without a shell can undergo a large amount of photo-induced fluorescence enhancement via such blockade when they are in touch with the metal oxide.« less

The thermoelectric efficiency of quantum dots in indium arsenide/indium phosphide nanowires

NASA Astrophysics Data System (ADS)

Hoffmann, Eric A.

State of the art semiconductor materials engineering provides the possibility to fabricate devices on the lower end of the mesoscopic scale and confine only a handful of electrons to a region of space. When the thermal energy is reduced below the energetic quantum level spacing, the confined electrons assume energy levels akin to the core-shell structure of natural atoms. Such "artificial atoms", also known as quantum dots, can be loaded with electrons, one-by-one, and subsequently unloaded using source and drain electrical contacts. As such, quantum dots are uniquely tunable platforms for performing quantum transport and quantum control experiments. Voltage-biased electron transport through quantum dots has been studied extensively. Far less attention has been given to thermoelectric effects in quantum dots, that is, electron transport induced by a temperature gradient. This dissertation focuses on the efficiency of direct thermal-to-electric energy conversion in InAs/InP quantum dots embedded in nanowires. The efficiency of thermoelectric heat engines is bounded by the same maximum efficiency as cyclic heat engines; namely, by Carnot efficiency. The efficiency of bulk thermoelectric materials suffers from their inability to transport charge carriers selectively based on energy. Owing to their three-dimensional momentum quantization, quantum dots operate as electron energy filters---a property which can be harnessed to minimize entropy production and therefore maximize efficiency. This research was motivated by the possibility to realize experimentally a thermodynamic heat engine operating with near-Carnot efficiency using the unique behavior of quantum dots. To this end, a microscopic heating scheme for the application of a temperature difference across a quantum dot was developed in conjunction with a novel quantum-dot thermometry technique used for quantifying the magnitude of the applied temperature difference. While pursuing high-efficiency thermoelectric performance, many mesoscopic thermoelectric effects were observed and studied, including Coulomb-blockade thermovoltage oscillations, thermoelectric power generation, and strong nonlinear behavior. In the end, a quantum-dot-based thermoelectric heat engine was achieved and demonstrated an electronic efficiency of up to 95% Carnot efficiency.

Optical signatures of coupled quantum dots.

PubMed

Stinaff, E A; Scheibner, M; Bracker, A S; Ponomarev, I V; Korenev, V L; Ware, M E; Doty, M F; Reinecke, T L; Gammon, D

2006-02-03

An asymmetric pair of coupled InAs quantum dots is tuned into resonance by applying an electric field so that a single hole forms a coherent molecular wave function. The optical spectrum shows a rich pattern of level anticrossings and crossings that can be understood as a superposition of charge and spin configurations of the two dots. Coulomb interactions shift the molecular resonance of the optically excited state (charged exciton) with respect to the ground state (single charge), enabling light-induced coupling of the quantum dots. This result demonstrates the possibility of optically coupling quantum dots for application in quantum information processing.

Optical Signatures of Coupled Quantum Dots

NASA Astrophysics Data System (ADS)

Stinaff, E. A.; Scheibner, M.; Bracker, A. S.; Ponomarev, I. V.; Korenev, V. L.; Ware, M. E.; Doty, M. F.; Reinecke, T. L.; Gammon, D.

2006-02-01

An asymmetric pair of coupled InAs quantum dots is tuned into resonance by applying an electric field so that a single hole forms a coherent molecular wave function. The optical spectrum shows a rich pattern of level anticrossings and crossings that can be understood as a superposition of charge and spin configurations of the two dots. Coulomb interactions shift the molecular resonance of the optically excited state (charged exciton) with respect to the ground state (single charge), enabling light-induced coupling of the quantum dots. This result demonstrates the possibility of optically coupling quantum dots for application in quantum information processing.

Spectrum Tunable Quantum Dot-In-A-Well Infrared Detector Arrays for Thermal Imaging

DTIC Science & Technology

2008-09-01

Spectrum tunable quantum dot-in-a- well infrared detector arrays for thermal imaging Jonathan R. Andrews1, Sergio R. Restaino1, Scott W. Teare2...Materials at the University of New Mexico has been investigating quantum dot and quantum well detectors for thermal infrared imaging applications...SEP 2008 2. REPORT TYPE 3. DATES COVERED 00-00-2008 to 00-00-2008 4. TITLE AND SUBTITLE Spectrum tunable quantum dot-in-a- well infrared

Downconversion quantum interface for a single quantum dot spin and 1550-nm single-photon channel.

PubMed

Pelc, Jason S; Yu, Leo; De Greve, Kristiaan; McMahon, Peter L; Natarajan, Chandra M; Esfandyarpour, Vahid; Maier, Sebastian; Schneider, Christian; Kamp, Martin; Höfling, Sven; Hadfield, Robert H; Forchel, Alfred; Yamamoto, Yoshihisa; Fejer, M M

2012-12-03

Long-distance quantum communication networks require appropriate interfaces between matter qubit-based nodes and low-loss photonic quantum channels. We implement a downconversion quantum interface, where the single photons emitted from a semiconductor quantum dot at 910 nm are downconverted to 1560 nm using a fiber-coupled periodically poled lithium niobate waveguide and a 2.2-μm pulsed pump laser. The single-photon character of the quantum dot emission is preserved during the downconversion process: we measure a cross-correlation g(2)(τ = 0) = 0.17 using resonant excitation of the quantum dot. We show that the downconversion interface is fully compatible with coherent optical control of the quantum dot electron spin through the observation of Rabi oscillations in the downconverted photon counts. These results represent a critical step towards a long-distance hybrid quantum network in which subsystems operating at different wavelengths are connected through quantum frequency conversion devices and 1.5-μm quantum channels.

Measurement back-action: Listening with quantum dots

NASA Astrophysics Data System (ADS)

Ladd, Thaddeus D.

2012-07-01

Single electrons in quantum dots can be disturbed by the apparatus used to measure them. The disturbance can be mediated by incoherent phonons -- literally, noise. Engineering acoustic interference could negate these deleterious effects and bring quantum dots closer to becoming a robust quantum technology.

Effect of temperature on the single-particle ground-state energy of a polar quantum dot with Gaussian confinement

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jahan, Luhluh K., E-mail: luhluhjahan@gmail.com; Chatterjee, Ashok

2016-05-23

The temperature and size dependence of the ground-state energy of a polaron in a Gaussian quantum dot have been investigated by using a variational technique. It is found that the ground-state energy increases with increasing temperature and decreases with the size of the quantum dot. Also, it is found that the ground-state energy is larger for a three-dimensional quantum dot as compared to a two-dimensional dot.

Magneto-optical absorption in semiconducting spherical quantum dots: Influence of the dot-size, confining potential, and magnetic field

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kushwaha, Manvir S.

2014-12-15

Semiconducting quantum dots – more fancifully dubbed artificial atoms – are quasi-zero dimensional, tiny, man-made systems with charge carriers completely confined in all three dimensions. The scientific quest behind the synthesis of quantum dots is to create and control future electronic and optical nanostructures engineered through tailoring size, shape, and composition. The complete confinement – or the lack of any degree of freedom for the electrons (and/or holes) – in quantum dots limits the exploration of spatially localized elementary excitations such as plasmons to direct rather than reciprocal space. Here we embark on a thorough investigation of the magneto-optical absorptionmore » in semiconducting spherical quantum dots characterized by a confining harmonic potential and an applied magnetic field in the symmetric gauge. This is done within the framework of Bohm-Pines’ random-phase approximation that enables us to derive and discuss the full Dyson equation that takes proper account of the Coulomb interactions. As an application of our theoretical strategy, we compute various single-particle and many-particle phenomena such as the Fock-Darwin spectrum; Fermi energy; magneto-optical transitions; probability distribution; and the magneto-optical absorption in the quantum dots. It is observed that the role of an applied magnetic field on the absorption spectrum is comparable to that of a confining potential. Increasing (decreasing) the strength of the magnetic field or the confining potential is found to be analogous to shrinking (expanding) the size of the quantum dots: resulting into a blue (red) shift in the absorption spectrum. The Fermi energy diminishes with both increasing magnetic-field and dot-size; and exhibits saw-tooth-like oscillations at large values of field or dot-size. Unlike laterally confined quantum dots, both (upper and lower) magneto-optical transitions survive even in the extreme instances. However, the intra-Landau level transitions are seen to be forbidden. The spherical quantum dots have an edge over the strictly two-dimensional quantum dots in that the additional (magnetic) quantum number makes the physics richer (but complex). A deeper grasp of the Coulomb blockade, quantum coherence, and entanglement can lead to a better insight into promising applications involving lasers, detectors, storage devices, and quantum computing.« less

Quantum Dots Investigated for Solar Cells

NASA Technical Reports Server (NTRS)

Bailey, Sheila G.; Castro, Stephanie L.; Raffaelle, Ryne P.; Hepp, Aloysius F.

2001-01-01

The NASA Glenn Research Center has been investigating the synthesis of quantum dots of CdSe and CuInS2 for use in intermediate-bandgap solar cells. Using quantum dots in a solar cell to create an intermediate band will allow the harvesting of a much larger portion of the available solar spectrum. Theoretical studies predict a potential efficiency of 63.2 percent, which is approximately a factor of 2 better than any state-of-the-art devices available today. This technology is also applicable to thin-film devices--where it offers a potential four-fold increase in power-to-weight ratio over the state of the art. Intermediate-bandgap solar cells require that quantum dots be sandwiched in an intrinsic region between the photovoltaic solar cell's ordinary p- and n-type regions (see the preceding figure). The quantum dots form the intermediate band of discrete states that allow sub-bandgap energies to be absorbed. However, when the current is extracted, it is limited by the bandgap, not the individual photon energies. The energy states of the quantum dot can be controlled by controlling the size of the dot. Ironically, the ground-state energy levels are inversely proportional to the size of the quantum dots. We have prepared a variety of quantum dots using the typical organometallic synthesis routes pioneered by Ba Wendi et al., in the early 1990's. The most studied quantum dots prepared by this method have been of CdSe. To produce these dots, researchers inject a syringe of the desired organometallic precursors into heated triocytlphosphine oxide (TOPO) that has been vigorously stirred under an inert atmosphere (see the following figure). The solution immediately begins to change from colorless to yellow, then orange and red/brown, as the quantum dots increase in size. When the desired size is reached, the heat is removed from the flask. Quantum dots of different sizes can be identified by placing them under a "black light" and observing the various color differences in their fluorescence (see the photograph).

Self-organized formation of quantum dots of a material on a substrate

DOEpatents

Zhang, Zhenyu; Wendelken, John F.; Chang, Ming-Che; Pai, Woei Wu

2001-01-01

Systems and methods are described for fabricating arrays of quantum dots. A method for making a quantum dot device, includes: forming clusters of atoms on a substrate; and charging the clusters of atoms such that the clusters of atoms repel one another. The systems and methods provide advantages because the quantum dots can be ordered with regard to spacing and/or size.

Blinking correlation in nanocrystal quantum dots probed with novel laser scanning confocal microscopy methods

NASA Astrophysics Data System (ADS)

Hefti, Ryan Alf

Semiconductor quantum dots have a vast array of applications: as fluorescent labels in biological systems, as physical or chemical sensors, as components in photovoltaic technology, and in display devices. An attribute of nearly every quantum dot is its blinking, or fluorescence intermittency, which tends to be a disadvantage in most applications. Despite the fact that blinking has been a nearly universal phenomenon among all types of fluorescent constructs, it is more prevalent in quantum dots than in traditional fluorophores. Furthermore, no unanimously accepted model of quantum dot blinking yet exists. The work encompassed by this dissertation began with an in-depth study of molecular motor protein dynamics in a variety of environments using two specially developed techniques, both of which feature applicability to live cell systems. Parked-beam confocal microscopy was utilized to increase temporal resolution of molecular motor motion dynamics by an order of magnitude over other popular methods. The second technique, fast-scanning confocal microscopy (FSCM), was used for long range observation of motor proteins. While using FSCM on motor protein assays, we discovered an unusual phenomenon. Single quantum dots seemingly communicated with neighboring quantum dots, indicated by a distinct correlation in their blinking patterns. In order to explain this novel correlation phenomenon, the majority of blinking models developed thus far would suggest a dipole-dipole interaction or a Coulomb interaction between singly charged quantum dots. However, our results indicate that the interaction energy is higher than supported by current models, thereby prompting a renewed examination. We propose that the blinking correlation we observed is due to a Coulomb interaction on the order of 3-4 elementary charges per quantum dot and that multiple charging of individual quantum dots may be required to plunge them into a non-emissive state. As a result of charging, charge carriers are displaced into a wide distribution of trap sites in the surrounding matrix, resulting in the expected power-law probability distribution of off times ubiquitous in quantum dots. Our discovery also implies that quantum dot blinking can be controlled, advocating the creation of switchable nanoscale emitters.

Quantum Entanglement of Quantum Dot Spin Using Flying Qubits

DTIC Science & Technology

2015-05-01

QUANTUM ENTANGLEMENT OF QUANTUM DOT SPIN USING FLYING QUBITS UNIVERSITY OF MICHIGAN MAY 2015 FINAL TECHNICAL REPORT APPROVED FOR PUBLIC RELEASE...To) SEP 2012 – DEC 2014 4. TITLE AND SUBTITLE QUANTUM ENTANGLEMENT OF QUANTUM DOT SPIN USING FLYING QUBITS 5a. CONTRACT NUMBER FA8750-12-2-0333...been to advance the frontier of quantum entangled semiconductor electrons using ultrafast optical techniques. The approach is based on

Studies of quantum dots in the quantum Hall regime

NASA Astrophysics Data System (ADS)

Goldmann, Eyal

We present two studies of quantum dots in the quantum Hall regime. In the first study, presented in Chapter 3, we investigate the edge reconstruction phenomenon believed to occur when the quantum dot filling fraction is n≲1 . Our approach involves the examination of large dots (≤40 electrons) using a partial diagonalization technique in which the occupancies of the deep interior orbitals are frozen. To interpret the results of this calculation, we evaluate the overlap between the diagonalized ground state and a set of trial wavefunctions which we call projected necklace (PN) states. A PN state is simply the angular momentum projection of a maximum density droplet surrounded by a ring of localized electrons. Our calculations reveal that PN states have up to 99% overlap with the diagonalized ground states, and are lower in energy than the states identified in Chamon and Wen's study of the edge reconstruction. In the second study, presented in Chapter 4, we investigate quantum dots in the fractional quantum Hall regime using a Hartree formulation of composite fermion theory. We find that under appropriate conditions, the chemical potential of the dots oscillates periodically with B due to the transfer of composite fermions between quasi-Landau bands. This effect is analogous the addition spectrum oscillations which occur in quantum dots in the integer quantum Hall regime. Period f0 oscillations are found in sharply confined dots with filling factors nu = 2/5 and nu = 2/3. Period 3 f0 oscillations are found in a parabolically confined nu = 2/5 dot. More generally, we argue that the oscillation period of dots with band pinning should vary continuously with B, whereas the period of dots without band pinning is f0 .

MWP phase shifters integrated in PbS-SU8 waveguides.

PubMed

Hervás, Javier; Suárez, Isaac; Pérez, Joaquín; Cantó, Pedro J Rodríguez; Abargues, Rafael; Martínez-Pastor, Juan P; Sales, Salvador; Capmany, José

2015-06-01

We present new kind of microwave phase shifters (MPS) based on dispersion of PbS colloidal quantum dots (QDs) in commercially available photoresist SU8 after a ligand exchange process. Ridge PbS-SU8 waveguides are implemented by integration of the nanocomposite in a silicon platform. When these waveguides are pumped at wavelengths below the band-gap of the PbS QDs, a phase shift in an optically conveyed (at 1550 nm) microwave signal is produced. The strong light confinement produced in the ridge waveguides allows an improvement of the phase shift as compared to the case of planar structures. Moreover, a novel ridge bilayer waveguide composed by a PbS-SU8 nanocomposite and a SU8 passive layer is proposed to decrease the propagation losses of the pump beam and in consequence to improve the microwave phase shift up to 36.5° at 25 GHz. Experimental results are reproduced by a theoretical model based on the slow light effect produced in a semiconductor waveguide due to the coherent population oscillations. The resulting device shows potential benefits respect to the current MPS technologies since it allows a fast tunability of the phase shift and a high level of integration due to its small size.

Quantum dot nanoparticle conjugation, characterization, and applications in neuroscience

NASA Astrophysics Data System (ADS)

Pathak, Smita

Quantum dot are semiconducting nanoparticles that have been used for decades in a variety of applications such as solar cells, LEDs and medical imaging. Their use in the last area, however, has been extremely limited despite their potential as revolutionary new biological labeling tools. Quantum dots are much brighter and more stable than conventional fluorophores, making them optimal for high resolution imaging and long term studies. Prior work in this area involves synthesizing and chemically conjugating quantum dots to molecules of interest in-house. However this method is both time consuming and prone to human error. Additionally, non-specific binding and nanoparticle aggregation currently prevent researchers from utilizing this system to its fullest capacity. Another critical issue that has not been addressed is determining the number of ligands bound to nanoparticles, which is crucial for proper interpretation of results. In this work, methods to label fixed cells using two types of chemically modified quantum dots are studied. Reproducible non-specific artifact labeling is consistently demonstrated if antibody-quantum dot conditions are less than optimal. In order to explain this, antibodies bound to quantum dots were characterized and quantified. While other groups have qualitatively characterized antibody functionalized quantum dots using TEM, AFM, UV spectroscopy and gel electrophoresis, and in some cases have reported calculated estimates of the putative number of total antibodies bound to quantum dots, no quantitative experimental results had been reported prior to this work. The chemical functionalization and characterization of quantum dot nanocrystals achieved in this work elucidates binding mechanisms of ligands to nanoparticles and allows researchers to not only translate our tools to studies in their own areas of interest but also derive quantitative results from these studies. This research brings ease of use and increased reliability to nanoparticles in medical imaging.

Characterizing and engineering tunable spin functionality inside indium arsenide/gallium arsenide quantum dot molecules

NASA Astrophysics Data System (ADS)

Liu, Weiwen

The continual downsizing of the basic functional units used in the electronics industry has motivated the study of the quantum computation and related topics. To overcome the limitations of classical physics and engineering, some unique quantum mechanical features, especially entanglement and superpositions have begun to be considered as important properties for future bits. Including these quantum mechanical features is attractive because the ability to utilize quantum mechanics can dramatically enhance computational power. Among the various ways of constructing the basic building blocks for quantum computation, we are particularly interested in using spins inside epitaxially grown InAs/GaAs quantum dot molecules as quantum bits (qubits). The ability to design and engineer nanostructures with tailored quantum properties is critical to engineering quantum computers and other novel electro-optical devices and is one of the key challenges for scaling up new ideas for device application. In this thesis, we will focus on how the structure and composition of quantum dot molecules can be used to control spin properties and charge interactions. Tunable spin and charge properties can enable new, more scalable, methods of initializing and manipulating quantum information. In this thesis, we demonstrate one method to enable electric-field tunability of Zeeman splitting for a single electron spin inside a quantum dot molecules by using heterostructure engineering techniques to modify the barrier that separates quantum dots. We describe how these structural changes to the quantum dot molecules also change charge interactions and propose ways to use this effect to enable accurate measurement of coulomb interactions and possibly charge occupancy inside these complicated quantum dot molecules.

Single-electron-occupation metal-oxide-semiconductor quantum dots formed from efficient poly-silicon gate layout

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carroll, Malcolm S.; rochette, sophie; Rudolph, Martin

We introduce a silicon metal-oxide-semiconductor quantum dot structure that achieves dot-reservoir tunnel coupling control without a dedicated barrier gate. The elementary structure consists of two accumulation gates separated spatially by a gap, one gate accumulating a reservoir and the other a quantum dot. Control of the tunnel rate between the dot and the reservoir across the gap is demonstrated in the single electron regime by varying the reservoir accumulation gate voltage while compensating with the dot accumulation gate voltage. The method is then applied to a quantum dot connected in series to source and drain reservoirs, enabling transport down tomore » the single electron regime. Finally, tuning of the valley splitting with the dot accumulation gate voltage is observed. This split accumulation gate structure creates silicon quantum dots of similar characteristics to other realizations but with less electrodes, in a single gate stack subtractive fabrication process that is fully compatible with silicon foundry manufacturing.« less

The emission wavelength dependent photoluminescence lifetime of the N-doped graphene quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Deng, Xingxia; School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210; University of Chinese Academy of Sciences, Beijing 100049

2015-12-14

Aromatic nitrogen doped graphene quantum dots were investigated by steady-state and time-resolved photoluminescence (PL) techniques. The PL lifetime was found to be dependent on the emission wavelength and coincident with the PL spectrum, which is different from most semiconductor quantum dots and fluorescent dyes. This result shows the synergy and competition between the quantum confinement effect and edge functional groups, which may have the potential to guide the synthesis and expand the applications of graphene quantum dots.

A Quantum Dot with Spin-Orbit Interaction--Analytical Solution

ERIC Educational Resources Information Center

Basu, B.; Roy, B.

2009-01-01

The practical applicability of a semiconductor quantum dot with spin-orbit interaction gives an impetus to study analytical solutions to one- and two-electron quantum dots with or without a magnetic field.

Clinical Potential of Quantum Dots

PubMed Central

Iga, Arthur M.; Robertson, John H. P.; Winslet, Marc C.; Seifalian, Alexander M.

2007-01-01

Advances in nanotechnology have led to the development of novel fluorescent probes called quantum dots. Quantum dots have revolutionalized the processes of tagging molecules within research settings and are improving sentinel lymph node mapping and identification in vivo studies. As the unique physical and chemical properties of these fluorescent probes are being unraveled, new potential methods of early cancer detection, rapid spread and therapeutic management, that is, photodynamic therapy are being explored. Encouraging results of optical and real time identification of sentinel lymph nodes and lymph flow using quantum dots in vivo models are emerging. Quantum dots have also superseded many of the limitations of organic fluorophores and are a promising alternative as a research tool. In this review, we examine the promising clinical potential of quantum dots, their hindrances for clinical use and the current progress in abrogating their inherent toxicity. PMID:18317518

Synthesis of quantum dots

DOEpatents

McDaniel, Hunter

2017-10-17

Common approaches to synthesizing alloyed quantum dots employ high-cost, air-sensitive phosphine complexes as the selenium precursor. Disclosed quantum dot synthesis embodiments avoid these hazardous and air-sensitive selenium precursors. Certain embodiments utilize a combination comprising a thiol and an amine that together reduce and complex the elemental selenium to form a highly reactive selenium precursor at room temperature. The same combination of thiol and amine acts as the reaction solvent, stabilizing ligand, and sulfur source in the synthesis of quantum dot cores. A non-injection approach may also be used. The optical properties of the quantum dots synthesized by this new approach can be finely tuned for a variety of applications by controlling size and/or composition of size and composition. Further, using the same approach, a shell can be grown around a quantum dot core that improves stability, luminescence efficiency, and may reduce toxicity.

Cadmium sulfide quantum dots induce oxidative stress and behavioral impairments in the marine clam Scrobicularia plana.

PubMed

Buffet, Pierre-Emmanuel; Zalouk-Vergnoux, Aurore; Poirier, Laurence; Lopes, Christelle; Risso-de-Faverney, Christine; Guibbolini, Marielle; Gilliland, Douglas; Perrein-Ettajani, Hanane; Valsami-Jones, Eugenia; Mouneyrac, Catherine

2015-07-01

Cadmium sulfide (CdS) quantum dots have a number of current applications in electronics and solar cells and significant future potential in medicine. The aim of the present study was to examine the toxic effects of CdS quantum dots on the marine clam Scrobicularia plana exposed for 14 d to these nanomaterials (10 µg Cd L(-1) ) in natural seawater and to compare them with soluble Cd. Measurement of labile Cd released from CdS quantum dots showed that 52% of CdS quantum dots remained in the nanoparticulate form. Clams accumulated the same levels of Cd regardless of the form in which it was delivered (soluble Cd vs CdS quantum dots). However, significant changes in biochemical responses were observed in clams exposed to CdS quantum dots compared with soluble Cd. Increased activities of catalase and glutathione-S-transferase were significantly higher in clams exposed in seawater to Cd as the nanoparticulate versus the soluble form, suggesting a specific nano effect. The behavior of S. plana in sediment showed impairments of foot movements only in the case of exposure to CdS quantum dots. The results show that oxidative stress and behavior biomarkers are sensitive predictors of CdS quantum dots toxicity in S. plana. Such responses, appearing well before changes might occur at the population level, demonstrate the usefulness of this model species and type of biomarker in the assessment of nanoparticle contamination in estuarine ecosystems. © 2015 SETAC.

Quantum dot-linked immunosorbent assay (QLISA) using orientation-directed antibodies.

PubMed

Suzuki, Miho; Udaka, Hikari; Fukuda, Takeshi

2017-09-05

An approach similar to the enzyme-linked immunosorbent assay (ELISA), with the advantage of saving time and effort but exhibiting high performance, was developed using orientation-directed half-part antibodies immobilized on CdSe/ZnS quantum dots. ELISA is a widely accepted assay used to detect the presence of a target substance. However, it takes time to quantify the target with specificity and sensitivity owing to signal amplification. In this study, CdSe/ZnS quantum dots are introduced as bright and photobleaching-tolerant fluorescent materials. Since hydrophilic surface coating of quantum dots rendered biocompatibility and functional groups for chemical reactions, the quantum dots were modified with half-sized antibodies after partial reduction. The half-sized antibody could be bound to a quantum dot through a unique thiol site to properly display the recognition domain for the core process of ELISA, which is an antigen-antibody interaction. The reducing conditions were investigated to generate efficient conjugates of quantum dots and half-sized antibodies. This was applied to IL-6 detection, as the quantification of IL-6 is significant owing to its close relationships with various biomedical phenomena that cause different diseases. An ELISA-like assay with CdSe/ZnS quantum dot institution (QLISA; Quantum dot-linked immunosorbent assay) was developed to detect 0.05ng/mL IL-6, which makes it sufficiently sensitive as an immunosorbent assay. Copyright © 2017 Elsevier B.V. All rights reserved.

Quantum strain sensor with a topological insulator HgTe quantum dot

PubMed Central

Korkusinski, Marek; Hawrylak, Pawel

2014-01-01

We present a theory of electronic properties of HgTe quantum dot and propose a strain sensor based on a strain-driven transition from a HgTe quantum dot with inverted bandstructure and robust topologically protected quantum edge states to a normal state without edge states in the energy gap. The presence or absence of edge states leads to large on/off ratio of conductivity across the quantum dot, tunable by adjusting the number of conduction channels in the source-drain voltage window. The electronic properties of a HgTe quantum dot as a function of size and applied strain are described using eight-band Luttinger and Bir-Pikus Hamiltonians, with surface states identified with chirality of Luttinger spinors and obtained through extensive numerical diagonalization of the Hamiltonian. PMID:24811674

Polarization of the photoluminescence of quantum dots incorporated into quantum wires

DOE Office of Scientific and Technical Information (OSTI.GOV)

Platonov, A. V., E-mail: alexei.platonov@mail.ioffe.ru; Kochereshko, V. P.; Kats, V. N.

The photoluminescence spectra of individual quantum dots incorporated into a quantum wire are studied. From the behavior of the spectra in a magnetic field, it is possible to estimate the exciton binding energy in a quantum dot incorporated into a quantum wire. It is found that the exciton photoluminescence signal emitted from a quantum dot along the direction of the nanowire axis is linearly polarized. At the same time, the photoluminescence signal propagating in the direction orthogonal to the nanowire axis is practically unpolarized. The experimentally observed effect is attributed to the nonaxial arrangement of the dot in the wiremore » under conditions of a huge increase in the exciton binding energy due to the effect of the image potential on the exciton.« less

Growing High-Quality InAs Quantum Dots for Infrared Lasers

NASA Technical Reports Server (NTRS)

Qiu, Yueming; Uhl, David

2004-01-01

An improved method of growing high-quality InAs quantum dots embedded in lattice-matched InGaAs quantum wells on InP substrates has been developed. InAs/InGaAs/InP quantum dot semiconductor lasers fabricated by this method are capable of operating at room temperature at wavelengths greater than or equal to 1.8 mm. Previously, InAs quantum dot lasers based on InP substrates have been reported only at low temperature of 77 K at a wavelength of 1.9 micrometers. In the present method, as in the prior method, one utilizes metalorganic vapor phase epitaxy to grow the aforementioned semiconductor structures. The development of the present method was prompted in part by the observation that when InAs quantum dots are deposited on an InGaAs layer, some of the InAs in the InGaAs layer becomes segregated from the layer and contributes to the formation of the InAs quantum dots. As a result, the quantum dots become highly nonuniform; some even exceed a critical thickness, beyond which they relax. In the present method, one covers the InGaAs layer with a thin layer of GaAs before depositing the InAs quantum dots. The purpose and effect of this thin GaAs layer is to suppress the segregation of InAs from the InGaAs layer, thereby enabling the InAs quantum dots to become nearly uniform (see figure). Devices fabricated by this method have shown near-room-temperature performance.

Local Gate Control of a Carbon Nanotube Double Quantum Dot

DTIC Science & Technology

2016-04-04

Nanotube Double Quantum Dot N. Mason,*† M. J. Biercuk,* C. M. Marcus† We have measured carbon nanotube quantum dots with multiple electro- static gates and...computation. Carbon nanotubes have been considered lead- ing candidates for nanoscale electronic applica- tions (1, 2). Previous measurements of nano- tube...electronics have shown electron confine- ment (quantum dot) effects such as single- electron charging and energy-level quantization (3–5). Nanotube

Understanding/Modelling of Thermal and Radiation Benefits of Quantum Dot Solar Cells

DTIC Science & Technology

2008-07-11

GaAs solar cells have been investigated. Strain compensation is a key step in realizing high- efficiency quantum dots solar cells (QDSC). InAs...factor. A strong correlation between the temperature dependent quantum dot electroluminescence peak emission wavelength and the sub-GaAs bandgap...increased efficiency and radiation resistance devices. The incorporation of quantum dots (QDs) into traditional single or multi-junction crystalline solar

Water-soluble luminescent quantum dots and biomolecular conjugates thereof and related compositions and methods of use

DOEpatents

Nie, Shuming; Chan, Warren C. W.; Emory, Stephen

2007-03-20

The present invention provides a water-soluble luminescent quantum dot, a biomolecular conjugate thereof and a composition comprising such a quantum dot or conjugate. Additionally, the present invention provides a method of obtaining a luminescent quantum dot, a method of making a biomolecular conjugate thereof, and methods of using a biomolecular conjugate for ultrasensitive nonisotopic detection in vitro and in vivo.

Water-soluble luminescent quantum dots and biomolecular conjugates thereof and related compositions and method of use

DOEpatents

Nie, Shuming; Chan, Warren C. W.; Emory, Steven R.

2002-01-01

The present invention provides a water-soluble luminescent quantum dot, a biomolecular conjugate thereof and a composition comprising such a quantum dot or conjugate. Additionally, the present invention provides a method of obtaining a luminescent quantum dot, a method of making a biomolecular conjugate thereof, and methods of using a biomolecular conjugate for ultrasensitive nonisotopic detection in vitro and in vivo.

In situ electron-beam polymerization stabilized quantum dot micelles.

PubMed

Travert-Branger, Nathalie; Dubois, Fabien; Renault, Jean-Philippe; Pin, Serge; Mahler, Benoit; Gravel, Edmond; Dubertret, Benoit; Doris, Eric

2011-04-19

A polymerizable amphiphile polymer containing PEG was synthesized and used to encapsulate quantum dots in micelles. The quantum dot micelles were then polymerized using a "clean" electron beam process that did not require any post-irradiation purification. Fluorescence spectroscopy revealed that the polymerized micelles provided an organic coating that preserved the quantum dot fluorescence better than nonpolymerized micelles, even under harsh conditions. © 2011 American Chemical Society

Ultralow Noise Monolithic Quantum Dot Photonic Oscillators

DTIC Science & Technology

2013-10-28

HBCU/MI) ULTRALOW NOISE MONOLITHIC QUANTUM DOT PHOTONIC OSCILLATORS LUKE LESTER UNIVERSITY OF NEW MEXICO 10/28/2013 Final Report DISTRIBUTION A...TELEPHONE NUMBER (Include area code) 24-10-2013 Final 01-06-2010 to 31-05-2013 Ultralow Noise Monolithic Quantum Dot Photonic Oscillators FA9550-10-1-0276...277-7647 Reset Grant Title: ULTRALOW NOISE MONOLITHIC QUANTUM DOT PHOTONIC OSCILLATORS Grant/Contract Number: FA9550-10-1-0276 Final Performance

Ligand removal and photo-activation of CsPbBr3 quantum dots for enhanced optoelectronic devices.

PubMed

Moyen, Eric; Kanwat, Anil; Cho, Sinyoung; Jun, Haeyeon; Aad, Roy; Jang, Jin

2018-05-10

Perovskite quantum dots have recently emerged as a promising light source for optoelectronic applications. However, integrating them into devices while preserving their outstanding optical properties remains challenging. Due to their ionic nature, perovskite quantum dots are extremely sensitive and degrade on applying the simplest processes. To maintain their colloidal stability, they are surrounded by organic ligands; these prevent efficient charge carrier injection in devices and have to be removed. Here we report on a simple method, where a moderate thermal process followed by exposure to UV in air can efficiently remove ligands and increase the photo-luminescence of the room temperature synthesized perovskite quantum dot thin films. Annealing is accompanied by a red shift of the emission wavelength, usually attributed to the coalescence and irreversible degradation of the quantum dots. We show that it is actually related to the relaxation of the quantum dots upon the ligand removal, without the creation of non-radiative recombining defects. The quantum dot surface, as devoid of ligands, is subsequently photo-oxidized and smoothened upon exposure to UV in air, which drastically enhances their photo-luminescence. This adequate combination of treatments improves by more than an order of magnitude the performances of perovskite quantum dot light emitting diodes.

Scanning gate imaging of two coupled quantum dots in single-walled carbon nanotubes.

PubMed

Zhou, Xin; Hedberg, James; Miyahara, Yoichi; Grutter, Peter; Ishibashi, Koji

2014-12-12

Two coupled single wall carbon nanotube quantum dots in a multiple quantum dot system were characterized by using a low temperature scanning gate microscopy (SGM) technique, at a temperature of 170 mK. The locations of single wall carbon nanotube quantum dots were identified by taking the conductance images of a single wall carbon nanotube contacted by two metallic electrodes. The single electron transport through single wall carbon nanotube multiple quantum dots has been observed by varying either the position or voltage bias of a conductive atomic force microscopy tip. Clear hexagonal patterns were observed in the region of the conductance images where only two sets of overlapping conductance rings are visible. The values of coupling capacitance over the total capacitance of the two dots, C(m)/C(1(2)) have been extracted to be 0.21 ∼ 0.27 and 0.23 ∼ 0.28, respectively. In addition, the interdot coupling (conductance peak splitting) has also been confirmed in both conductance image measurement and current-voltage curves. The results show that a SGM technique enables spectroscopic investigation of coupled quantum dots even in the presence of unexpected multiple quantum dots.

Optimization of digital image processing to determine quantum dots' height and density from atomic force microscopy.

PubMed

Ruiz, J E; Paciornik, S; Pinto, L D; Ptak, F; Pires, M P; Souza, P L

2018-01-01

An optimized method of digital image processing to interpret quantum dots' height measurements obtained by atomic force microscopy is presented. The method was developed by combining well-known digital image processing techniques and particle recognition algorithms. The properties of quantum dot structures strongly depend on dots' height, among other features. Determination of their height is sensitive to small variations in their digital image processing parameters, which can generate misleading results. Comparing the results obtained with two image processing techniques - a conventional method and the new method proposed herein - with the data obtained by determining the height of quantum dots one by one within a fixed area, showed that the optimized method leads to more accurate results. Moreover, the log-normal distribution, which is often used to represent natural processes, shows a better fit to the quantum dots' height histogram obtained with the proposed method. Finally, the quantum dots' height obtained were used to calculate the predicted photoluminescence peak energies which were compared with the experimental data. Again, a better match was observed when using the proposed method to evaluate the quantum dots' height. Copyright © 2017 Elsevier B.V. All rights reserved.

State-conditional coherent charge qubit oscillations in a Si/SiGe quadruple quantum dot

NASA Astrophysics Data System (ADS)

Ward, Daniel R.; Kim, Dohun; Savage, Donald E.; Lagally, Max G.; Foote, Ryan H.; Friesen, Mark; Coppersmith, Susan N.; Eriksson, Mark A.

2016-10-01

Universal quantum computation requires high-fidelity single-qubit rotations and controlled two-qubit gates. Along with high-fidelity single-qubit gates, strong efforts have been made in developing robust two-qubit logic gates in electrically gated quantum dot systems to realise a compact and nanofabrication-compatible architecture. Here we perform measurements of state-conditional coherent oscillations of a charge qubit. Using a quadruple quantum dot formed in a Si/SiGe heterostructure, we show the first demonstration of coherent two-axis control of a double quantum dot charge qubit in undoped Si/SiGe, performing Larmor and Ramsey oscillation measurements. We extract the strength of the capacitive coupling between a pair of double quantum dots by measuring the detuning energy shift (≈75 μeV) of one double dot depending on the excess charge configuration of the other double dot. We further demonstrate that the strong capacitive coupling allows fast, state-conditional Landau-Zener-Stückelberg oscillations with a conditional π phase flip time of about 80 ps, showing a promising pathway towards multi-qubit entanglement and control in semiconductor quantum dots.

Fabrication of quantum dots in undoped Si/Si 0.8Ge 0.2 heterostructures using a single metal-gate layer

DOE PAGES

Lu, T. M.; Gamble, J. K.; Muller, R. P.; ...

2016-08-01

Enhancement-mode Si/SiGe electron quantum dots have been pursued extensively by many groups for their potential in quantum computing. Most of the reported dot designs utilize multiple metal-gate layers and use Si/SiGe heterostructures with Ge concentration close to 30%. Here, we report the fabrication and low-temperature characterization of quantum dots in the Si/Si 0.8Ge 0.2 heterostructures using only one metal-gate layer. We find that the threshold voltage of a channel narrower than 1 μm increases as the width decreases. The higher threshold can be attributed to the combination of quantum confinement and disorder. We also find that the lower Ge ratiomore » used here leads to a narrower operational gate bias range. The higher threshold combined with the limited gate bias range constrains the device design of lithographic quantum dots. We incorporate such considerations in our device design and demonstrate a quantum dot that can be tuned from a single dot to a double dot. Furthermore, the device uses only a single metal-gate layer, greatly simplifying device design and fabrication.« less

State-conditional coherent charge qubit oscillations in a Si/SiGe quadruple quantum dot

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ward, Daniel R.; Kim, Dohun; Savage, Donald E.

Universal quantum computation requires high-fidelity single-qubit rotations and controlled two-qubit gates. Along with high-fidelity single-qubit gates, strong efforts have been made in developing robust two-qubit logic gates in electrically gated quantum dot systems to realise a compact and nanofabrication-compatible architecture. Here we perform measurements of state-conditional coherent oscillations of a charge qubit. Using a quadruple quantum dot formed in a Si/SiGe heterostructure, we show the first demonstration of coherent two-axis control of a double quantum dot charge qubit in undoped Si/SiGe, performing Larmor and Ramsey oscillation measurements. We extract the strength of the capacitive coupling between a pair of doublemore » quantum dots by measuring the detuning energy shift (≈75 μeV) of one double dot depending on the excess charge configuration of the other double dot. Finally, we further demonstrate that the strong capacitive coupling allows fast, state-conditional Landau–Zener–Stückelberg oscillations with a conditional π phase flip time of about 80 ps, showing a promising pathway towards multi-qubit entanglement and control in semiconductor quantum dots.« less

State-conditional coherent charge qubit oscillations in a Si/SiGe quadruple quantum dot

DOE PAGES

Ward, Daniel R.; Kim, Dohun; Savage, Donald E.; ...

2016-10-18

Universal quantum computation requires high-fidelity single-qubit rotations and controlled two-qubit gates. Along with high-fidelity single-qubit gates, strong efforts have been made in developing robust two-qubit logic gates in electrically gated quantum dot systems to realise a compact and nanofabrication-compatible architecture. Here we perform measurements of state-conditional coherent oscillations of a charge qubit. Using a quadruple quantum dot formed in a Si/SiGe heterostructure, we show the first demonstration of coherent two-axis control of a double quantum dot charge qubit in undoped Si/SiGe, performing Larmor and Ramsey oscillation measurements. We extract the strength of the capacitive coupling between a pair of doublemore » quantum dots by measuring the detuning energy shift (≈75 μeV) of one double dot depending on the excess charge configuration of the other double dot. Finally, we further demonstrate that the strong capacitive coupling allows fast, state-conditional Landau–Zener–Stückelberg oscillations with a conditional π phase flip time of about 80 ps, showing a promising pathway towards multi-qubit entanglement and control in semiconductor quantum dots.« less

Fabrication of (In,Ga)As quantum-dot chains on GaAs(100)

NASA Astrophysics Data System (ADS)

Wang, Z. M.; Holmes, K.; Mazur, Yu. I.; Salamo, G. J.

2004-03-01

Nanostructure evolution during the growth of multilayers of In0.5Ga0.5As/GaAs (100) by molecular-beam epitaxy is investigated to control the formation of lines of quantum dots called quantum-dot chains. It is found that the dot chains can be substantially increased in length by the introduction of growth interruptions during the initial stages of growth of the GaAs spacer layer. Quantum-dot chains that are longer than 5 μm are obtained by adjusting the In0.5Ga0.5As coverage and growth interruptions. The growth procedure is also used to create a template to form InAs dots into chains with a predictable dot density. The resulting dot chains offer the possibility to engineer carrier interaction among dots for novel physical phenomena and potential devices.

Holographic assembly of semiconductor CdSe quantum dots in polymer for volume Bragg grating structures with diffraction efficiency near 100%

NASA Astrophysics Data System (ADS)

Liu, Xiangming; Tomita, Yasuo; Oshima, Juro; Chikama, Katsumi; Matsubara, Koutatsu; Nakashima, Takuya; Kawai, Tsuyoshi

2009-12-01

We report on the fabrication of centimeter-size transmission Bragg gratings in semiconductor CdSe quantum dots dispersed 50 μm thick photopolymer films. This was done by holographic assembly of CdSe quantum dots in a photopolymerizable monomer blend. Periodic patterning of CdSe quantum dots in polymer was confirmed by a fluorescence microscope and confocal Raman imaging. The diffraction efficiency from the grating of 1 μm spacing was near 100% in the green with 0.34 vol % CdSe quantum dots, giving the refractive index modulation as large as 5.1×10-3.

Three-State Quantum Dot Gate FETs Using ZnS-ZnMgS Lattice-Matched Gate Insulator on Silicon

NASA Astrophysics Data System (ADS)

Karmakar, Supriya; Suarez, Ernesto; Jain, Faquir C.

2011-08-01

This paper presents the three-state behavior of quantum dot gate field-effect transistors (FETs). GeO x -cladded Ge quantum dots (QDs) are site-specifically self-assembled over lattice-matched ZnS-ZnMgS high- κ gate insulator layers grown by metalorganic chemical vapor deposition (MOCVD) on silicon substrates. A model of three-state behavior manifested in the transfer characteristics due to the quantum dot gate is also presented. The model is based on the transfer of carriers from the inversion channel to two layers of cladded GeO x -Ge quantum dots.

Realizing Rec. 2020 color gamut with quantum dot displays.

PubMed

Zhu, Ruidong; Luo, Zhenyue; Chen, Haiwei; Dong, Yajie; Wu, Shin-Tson

2015-09-07

We analyze how to realize Rec. 2020 wide color gamut with quantum dots. For photoluminescence, our simulation indicates that we are able to achieve over 97% of the Rec. 2020 standard with quantum dots by optimizing the emission spectra and redesigning the color filters. For electroluminescence, by optimizing the emission spectra of quantum dots is adequate to render over 97% of the Rec. 2020 standard. We also analyze the efficiency and angular performance of these devices, and then compare results with LCDs using green and red phosphors-based LED backlight. Our results indicate that quantum dot display is an outstanding candidate for achieving wide color gamut and high optical efficiency.

Synthetic Developments of Nontoxic Quantum Dots.

PubMed

Das, Adita; Snee, Preston T

2016-03-03

Semiconductor nanocrystals, or quantum dots (QDs), are candidates for biological sensing, photovoltaics, and catalysis due to their unique photophysical properties. The most studied QDs are composed of heavy metals like cadmium and lead. However, this engenders concerns over heavy metal toxicity. To address this issue, numerous studies have explored the development of nontoxic (or more accurately less toxic) quantum dots. In this Review, we select three major classes of nontoxic quantum dots composed of carbon, silicon and Group I-III-VI elements and discuss the myriad of synthetic strategies and surface modification methods to synthesize quantum dots composed of these material systems. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Current Application of Quantum Dots (QD) in Cancer Therapy: A Review.

PubMed

Babu, Lavanya Thilak; Paira, Priyankar

2017-01-01

Semiconductor quantum dots proved themselves as efficient fluorescent probes in cancer detection and treatment. Their size, high stability, non-photobleaching and water solubility made them a unique fluorophore in place of conventional organic dyes. Newly emerged theranostic drug delivery system using quantum dots helped us in better understanding of the drug delivery mechanism inside the cells. Surface modified Quantum dots and their applications became wide in bioimaging, immunohistochemistry, tracking intracellular drug and intracellular molecules target. We have highlighted various applications of quantum dots in cancer treatment, drug delivery, flow cytometry, and theranostics. Copyright© Bentham Science Publishers; For any queries, please email at epub@benthamscience.org.

Semiconductor quantum dot super-emitters: spontaneous emission enhancement combined with suppression of defect environment using metal-oxide plasmonic metafilms

NASA Astrophysics Data System (ADS)

Sadeghi, Seyed M.; Wing, Waylin J.; Gutha, Rithvik R.; Sharp, Christina

2018-01-01

We demonstrate that a metal-oxide plasmonic metafilm consisting of a Si/Al oxide junction in the vicinity of a thin gold layer can quarantine excitons in colloidal semiconductor quantum dots against their defect environments. This process happens while the plasmon fields of the gold layer enhance spontaneous emission decay rates of the quantum dots. We study the emission dynamics of such quantum dots when the distance between the Si/Al oxide junction and the gold thin layer is varied. The results show that for distances less than a critical value the lifetime of the quantum dots can be elongated while they experience intense plasmon fields. This suggests that the metal-oxide metafilm can keep photo-excited electrons in the cores of the quantum dots, suppressing their migration to the surface defect sites. This leads to suppression of Auger recombination, offering quantum dot super-emitters with emission that is enhanced not only by the plasmon fields (Purcell effect), but also by strong suppression of the non-radiative decay caused by the defect sites.

Biological sensing and control of emission dynamics of quantum dot bioconjugates using arrays of long metallic nanorods.

PubMed

Sadeghi, Seyed M; Gutha, Rithvik R; Wing, Waylin J; Sharp, Christina; Capps, Lucas; Mao, Chuanbin

2017-01-01

We study biological sensing using plasmonic and photonic-plasmonic resonances of arrays of ultralong metallic nanorods and analyze the impact of these resonances on emission dynamics of quantum dot bioconjugates. We demonstrate that the LSPRs and plasmonic lattice modes of such array can be used to detect a single self-assembled monolayer of alkanethiol at the visible (550 nm) and near infrared (770 nm) range with well resolved shifts. We study adsorption of streptavidin-quantum dot conjugates to this monolayer, demonstrating that formation of nearly two dimensional arrays of quantum dots with limited emission blinking can lead to extra well-defined wavelength shifts in these modes. Using spectrally-resolved lifetime measurements we study the emission dynamics of such quantum dot bioconjugates within their monodispersed size distribution. We show that, despite their close vicinity to the nanorods, the rate of energy transfer from these quantum dots to nanorods is rather weak, while the plasmon field enhancement can be strong. Our results reveal that the nanorods present a strongly wavelength or size-dependent non-radiative decay channel to the quantum dot bioconjugates.

Fabrication and characterization of silicon quantum dots in Si-rich silicon carbide films.

PubMed

Chang, Geng-Rong; Ma, Fei; Ma, Dayan; Xu, Kewei

2011-12-01

Amorphous Si-rich silicon carbide films were prepared by magnetron co-sputtering and subsequently annealed at 900-1100 degrees C. After annealing at 1100 degrees C, this configuration of silicon quantum dots embedded in amorphous silicon carbide formed. X-ray photoelectron spectroscopy was used to study the chemical modulation of the films. The formation and orientation of silicon quantum dots were characterized by glancing angle X-ray diffraction, which shows that the ratio of silicon and carbon significantly influences the species of quantum dots. High-resolution transmission electron microscopy investigations directly demonstrated that the formation of silicon quantum dots is heavily dependent on the annealing temperatures and the ratio of silicon and carbide. Only the temperature of about 1100 degrees C is enough for the formation of high-density and small-size silicon quantum dots due to phase separation and thermal crystallization. Deconvolution of the first order Raman spectra shows the existence of a lower frequency peak in the range 500-505 cm(-1) corresponding to silicon quantum dots with different atom ratio of silicon and carbon.

A Transfer Hamiltonian Model for Devices Based on Quantum Dot Arrays

PubMed Central

Illera, S.; Prades, J. D.; Cirera, A.; Cornet, A.

2015-01-01

We present a model of electron transport through a random distribution of interacting quantum dots embedded in a dielectric matrix to simulate realistic devices. The method underlying the model depends only on fundamental parameters of the system and it is based on the Transfer Hamiltonian approach. A set of noncoherent rate equations can be written and the interaction between the quantum dots and between the quantum dots and the electrodes is introduced by transition rates and capacitive couplings. A realistic modelization of the capacitive couplings, the transmission coefficients, the electron/hole tunneling currents, and the density of states of each quantum dot have been taken into account. The effects of the local potential are computed within the self-consistent field regime. While the description of the theoretical framework is kept as general as possible, two specific prototypical devices, an arbitrary array of quantum dots embedded in a matrix insulator and a transistor device based on quantum dots, are used to illustrate the kind of unique insight that numerical simulations based on the theory are able to provide. PMID:25879055

Luminescent behavior of cadmium sulfide quantum dots for gallic acid estimation

NASA Astrophysics Data System (ADS)

Singh, Suman; Garg, Sourav; Chahal, Jitender; Raheja, Khushboo; Singh, Deepak; Singla, M. L.

2013-03-01

Thioglycolic acid capped cadmium sulfide (CdS/T) quantum dots have been synthesized using wet chemistry and their optical behavior has been investigated using UV-visible absorption and fluorescence spectroscopy. The role of the capping agent, sulfide source concentration, pH and temperature has been studied and discussed. Studies showed that alkaline pH leads to a decrease in the size of quantum dots and reflux temperature above 70 °C resulted in red-shift of emission spectra which is due to narrowing of the bandgap. Further, to reduce the toxicity and photochemical instability of quantum dots, the quantum dots have been functionalized with polyethylene glycol (PEG), which resulted in a 20% enhancement of the fluorescence intensity. The application potential of CdS/T-PEG quantum dots was further studied using gallic acid as a model compound. The sensing is based on fluorescence quenching of quantum dots in the presence of gallic acid, and this study showed linearity in the range from 1.3 × 10-8 to 46.5 × 10-8 mM, with a detection limit of 3.6 × 10-8 mM.

A transfer hamiltonian model for devices based on quantum dot arrays.

PubMed

Illera, S; Prades, J D; Cirera, A; Cornet, A

2015-01-01

We present a model of electron transport through a random distribution of interacting quantum dots embedded in a dielectric matrix to simulate realistic devices. The method underlying the model depends only on fundamental parameters of the system and it is based on the Transfer Hamiltonian approach. A set of noncoherent rate equations can be written and the interaction between the quantum dots and between the quantum dots and the electrodes is introduced by transition rates and capacitive couplings. A realistic modelization of the capacitive couplings, the transmission coefficients, the electron/hole tunneling currents, and the density of states of each quantum dot have been taken into account. The effects of the local potential are computed within the self-consistent field regime. While the description of the theoretical framework is kept as general as possible, two specific prototypical devices, an arbitrary array of quantum dots embedded in a matrix insulator and a transistor device based on quantum dots, are used to illustrate the kind of unique insight that numerical simulations based on the theory are able to provide.

Four-Wave Mixing Spectroscopy of Quantum Dot Molecules

NASA Astrophysics Data System (ADS)

Sitek, A.; Machnikowski, P.

2007-08-01

We study theoretically the nonlinear four-wave mixing response of an ensemble of coupled pairs of quantum dots (quantum dot molecules). We discuss the shape of the echo signal depending on the parameters of the ensemble: the statistics of transition energies and the degree of size correlations between the dots forming the molecules.

Impact of heavy hole-light hole coupling on optical selection rules in GaAs quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Belhadj, T.; Amand, T.; Kunz, S.

2010-08-02

We report strong heavy hole-light hole mixing in GaAs quantum dots grown by droplet epitaxy. Using the neutral and charged exciton emission as a monitor we observe the direct consequence of quantum dot symmetry reduction in this strain free system. By fitting the polar diagram of the emission with simple analytical expressions obtained from k{center_dot}p theory we are able to extract the mixing that arises from the heavy-light hole coupling due to the geometrical asymmetry of the quantum dot.

Production of three-dimensional quantum dot lattice of Ge/Si core-shell quantum dots and Si/Ge layers in an alumina glass matrix.

PubMed

Buljan, M; Radić, N; Sancho-Paramon, J; Janicki, V; Grenzer, J; Bogdanović-Radović, I; Siketić, Z; Ivanda, M; Utrobičić, A; Hübner, R; Weidauer, R; Valeš, V; Endres, J; Car, T; Jerčinović, M; Roško, J; Bernstorff, S; Holy, V

2015-02-13

We report on the formation of Ge/Si quantum dots with core/shell structure that are arranged in a three-dimensional body centered tetragonal quantum dot lattice in an amorphous alumina matrix. The material is prepared by magnetron sputtering deposition of Al2O3/Ge/Si multilayer. The inversion of Ge and Si in the deposition sequence results in the formation of thin Si/Ge layers instead of the dots. Both materials show an atomically sharp interface between the Ge and Si parts of the dots and layers. They have an amorphous internal structure that can be crystallized by an annealing treatment. The light absorption properties of these complex materials are significantly different compared to films that form quantum dot lattices of the pure Ge, Si or a solid solution of GeSi. They show a strong narrow absorption peak that characterizes a type II confinement in accordance with theoretical predictions. The prepared materials are promising for application in quantum dot solar cells.

Trap elimination and reduction of size dispersion due to aging in CdS x Se1- x quantum dots

NASA Astrophysics Data System (ADS)

Verma, Abhishek; Nagpal, Swati; Pandey, Praveen K.; Bhatnagar, P. K.; Mathur, P. C.

2007-12-01

Quantum Dots of CdS x Se1- x embedded in borosilicate glass matrix have been grown using Double-Step annealing method. Optical characterization of the quantum dots has been done through the combinative analysis of optical absorption and photoluminescence spectroscopy at room temperature. Decreasing trend of photoluminescence intensity with aging has been observed and is attributed to trap elimination. The changes in particle size, size distribution, number of quantum dots, volume fraction, trap related phenomenon and Gibbs free energy of quantum dots, has been explained on the basis of the diffusion-controlled growth process, which continues with passage of time. For a typical case, it was found that after 24 months of aging, the average radii increased from 3.05 to 3.12 nm with the increase in number of quantum dots by 190% and the size-dispersion decreased from 10.8% to 9.9%. For this sample, the initial size range of the quantum dots was 2.85 to 3.18 nm. After that no significant change was found in these parameters for the next 12 months. This shows that the system attains almost a stable nature after 24 months of aging. It was also observed that the size-dispersion in quantum dots reduces with the increase in annealing duration, but at the cost of quantum confinement effect. Therefore, a trade off optimization has to be done between the size-dispersion and the quantum confinement.

Luminescent Quantum Dots as Ultrasensitive Biological Labels

NASA Astrophysics Data System (ADS)

Nie, Shuming

2000-03-01

Highly luminescent semiconductor quantum dots have been covalently coupled to biological molecules for use in ultrasensitive biological detection. This new class of luminescent labels is considerably brighter and more resistant againt photobleaching in comparison with organic dyes. Quantum dots labeled with the protein transferrin undergo receptor-mediated endocytosis (RME) in cultured HeLa cells, and those dots that were conjugated to immunomolecules recognize specific antibodies or antigens. In addition, we show that DNA functionalized quantum dots can be used to target specific genes by hybridization. We expect that quantum dot bioconjugates will have a broad range of biological applications, such as ligand-receptor interactions, real-time monitoring of molecular trafficking inside living cells, multicolor fluorescence in-situ hybridization (FISH), high-sensitivity detection in miniaturized devices (e.g., DNA chips), and fluorescent tagging of combinatorial chemical libraries. A potential clinical application is the use of quantum dots for ultrasensitive viral RNA detection, in which as low as 100 copies of hepatitis C and HIV viruses per ml blood should be detected.

Aptamer-Modified Semiconductor Quantum Dots for Biosensing Applications

PubMed Central

Wen, Lin; Qiu, Liping; Wu, Yongxiang; Hu, Xiaoxiao; Zhang, Xiaobing

2017-01-01

Semiconductor quantum dots have attracted extensive interest in the biosensing area because of their properties, such as narrow and symmetric emission with tunable colors, high quantum yield, high stability and controllable morphology. The introduction of various reactive functional groups on the surface of semiconductor quantum dots allows one to conjugate a spectrum of ligands, antibodies, peptides, or nucleic acids for broader and smarter applications. Among these ligands, aptamers exhibit many advantages including small size, high chemical stability, simple synthesis with high batch-to-batch consistency and convenient modification. More importantly, it is easy to introduce nucleic acid amplification strategies and/or nanomaterials to improve the sensitivity of aptamer-based sensing systems. Therefore, the combination of semiconductor quantum dots and aptamers brings more opportunities in bioanalysis. Here we summarize recent advances on aptamer-functionalized semiconductor quantum dots in biosensing applications. Firstly, we discuss the properties and structure of semiconductor quantum dots and aptamers. Then, the applications of biosensors based on aptamer-modified semiconductor quantum dots by different signal transducing mechanisms, including optical, electrochemical and electrogenerated chemiluminescence approaches, is discussed. Finally, our perspectives on the challenges and opportunities in this promising field are provided. PMID:28788080

Aptamer-Modified Semiconductor Quantum Dots for Biosensing Applications.

PubMed

Wen, Lin; Qiu, Liping; Wu, Yongxiang; Hu, Xiaoxiao; Zhang, Xiaobing

2017-07-28

Semiconductor quantum dots have attracted extensive interest in the biosensing area because of their properties, such as narrow and symmetric emission with tunable colors, high quantum yield, high stability and controllable morphology. The introduction of various reactive functional groups on the surface of semiconductor quantum dots allows one to conjugate a spectrum of ligands, antibodies, peptides, or nucleic acids for broader and smarter applications. Among these ligands, aptamers exhibit many advantages including small size, high chemical stability, simple synthesis with high batch-to-batch consistency and convenient modification. More importantly, it is easy to introduce nucleic acid amplification strategies and/or nanomaterials to improve the sensitivity of aptamer-based sensing systems. Therefore, the combination of semiconductor quantum dots and aptamers brings more opportunities in bioanalysis. Here we summarize recent advances on aptamer-functionalized semiconductor quantum dots in biosensing applications. Firstly, we discuss the properties and structure of semiconductor quantum dots and aptamers. Then, the applications of biosensors based on aptamer-modified semiconductor quantum dots by different signal transducing mechanisms, including optical, electrochemical and electrogenerated chemiluminescence approaches, is discussed. Finally, our perspectives on the challenges and opportunities in this promising field are provided.

Increased InAs quantum dot size and density using bismuth as a surfactant

NASA Astrophysics Data System (ADS)

Dasika, Vaishno D.; Krivoy, E. M.; Nair, H. P.; Maddox, S. J.; Park, K. W.; Jung, D.; Lee, M. L.; Yu, E. T.; Bank, S. R.

2014-12-01

We have investigated the growth of self-assembled InAs quantum dots using bismuth as a surfactant to control the dot size and density. We find that the bismuth surfactant increases the quantum dot density, size, and uniformity, enabling the extension of the emission wavelength with increasing InAs deposition without a concomitant reduction in dot density. We show that these effects are due to bismuth acting as a reactive surfactant to kinetically suppress the surface adatom mobility. This mechanism for controlling quantum dot density and size has the potential to extend the operating wavelength and enhance the performance of various optoelectronic devices.

Laser location and manipulation of a single quantum tunneling channel in an InAs quantum dot.

PubMed

Makarovsky, O; Vdovin, E E; Patané, A; Eaves, L; Makhonin, M N; Tartakovskii, A I; Hopkinson, M

2012-03-16

We use a femtowatt focused laser beam to locate and manipulate a single quantum tunneling channel associated with an individual InAs quantum dot within an ensemble of dots. The intensity of the directed laser beam tunes the tunneling current through the targeted dot with an effective optical gain of 10(7) and modifies the curvature of the dot's confining potential and the spatial extent of its ground state electron eigenfunction. These observations are explained by the effect of photocreated hole charges which become bound close to the targeted dot, thus acting as an optically induced gate electrode.

Ultrafast electronic dynamics in unipolar n-doped indium gallium arsenide/gallium arsenide self-assembled quantum dots

NASA Astrophysics Data System (ADS)

Wu, Zong-Kwei J.

2006-12-01

Photodetectors based on intraband infrared absorption in the quantum dots have demonstrated improved performance over its quantum well counterpart by lower dark current, relative temperature insensitivity, and its ability for normal incidence operation. Various scattering processes, including phonon emission/absorption and carrier-carrier scattering, are critical in understanding device operation on the fundamental level. In previous studies, our group has investigated carrier dynamics in both low- and high-density regime. Ultrafast electron-hole scattering and the predicted phonon bottleneck effect in intrinsic quantum dots have been observed. Further examination on electron dynamics in unipolar structures is presented in this thesis. We used n-doped quantum dot in mid-infrared photodetector device structure to study the electron dynamics in unipolar structure. Differential transmission spectroscopy with mid-infrared intraband pump and optical interband probe was implemented to measure the electron dynamics directly without creating extra electron-hole pair, Electron relaxation after excitation was measured under various density and temperature conditions. Rapid capture into quantum dot within ˜ 10 ps was observed due to Auger-type electron-electron scattering. Intradot relaxation from the quantum dot excited state to the ground state was also observed on the time scale of 100 ps. With highly doped electron density in the structure, the inter-sublevel relaxation is dominated by Auger-type electron-electron scattering and the phonon bottleneck effect is circumvented. Nanosecond-scale recovery in larger-sized quantum dots was observed, not intrinsic to electron dynamics but due to band-bending and built-in voltage drift. An ensemble Monte Carlo simulation was also established to model the dynamics in quantum dots and in goad agreement with the experimental results. We presented a comprehensive picture of electron dynamics in the unipolar quantum dot structure. Although the phonon bottleneck is circumvented with high doped electron density, relaxation processes in unipolar quantum dots have been measured with time scales longer than that of bipolar systems. The results explain the operation principles of the quantum dot infrared photodetector on a microscopic level and provide basic understanding for future applications and designs.

Demonstration of Quantum Entanglement between a Single Electron Spin Confined to an InAs Quantum Dot and a Photon

NASA Astrophysics Data System (ADS)

Schaibley, J. R.; Burgers, A. P.; McCracken, G. A.; Duan, L.-M.; Berman, P. R.; Steel, D. G.; Bracker, A. S.; Gammon, D.; Sham, L. J.

2013-04-01

The electron spin state of a singly charged semiconductor quantum dot has been shown to form a suitable single qubit for quantum computing architectures with fast gate times. A key challenge in realizing a useful quantum dot quantum computing architecture lies in demonstrating the ability to scale the system to many qubits. In this Letter, we report an all optical experimental demonstration of quantum entanglement between a single electron spin confined to a single charged semiconductor quantum dot and the polarization state of a photon spontaneously emitted from the quantum dot’s excited state. We obtain a lower bound on the fidelity of entanglement of 0.59±0.04, which is 84% of the maximum achievable given the timing resolution of available single photon detectors. In future applications, such as measurement-based spin-spin entanglement which does not require sub-nanosecond timing resolution, we estimate that this system would enable near ideal performance. The inferred (usable) entanglement generation rate is 3×103s-1. This spin-photon entanglement is the first step to a scalable quantum dot quantum computing architecture relying on photon (flying) qubits to mediate entanglement between distant nodes of a quantum dot network.

Unbound states in quantum heterostructures

PubMed Central

Bastard, G

2006-01-01

We report in this review on the electronic continuum states of semiconductor Quantum Wells and Quantum Dots and highlight the decisive part played by the virtual bound states in the optical properties of these structures. The two particles continuum states of Quantum Dots control the decoherence of the excited electron – hole states. The part played by Auger scattering in Quantum Dots is also discussed.

Quantum-dot temperature profiles during laser irradiation for semiconductor-doped glasses

NASA Astrophysics Data System (ADS)

Nagpal, Swati

2002-12-01

Temperature profiles around laser irradiated CdX (X=S, Se, and Te) quantum dots in borosilicate glasses were theoretically modeled. Initially the quantum dots heat up rapidly, followed by a gradual increase of temperature. Also it is found that larger dots reach higher temperatures for the same pulse characteristics. After the pulse is turned off, the dots initially cool rapidly, followed by a gradual decrease in temperature.

A Phosphine-Free Route to Size-Adjustable CdSe and CdSe/CdS Core-Shell Quantum Dots for White-Light-Emitting Diodes.

PubMed

Zhang, Yugang; Li, Guopeng; Zhang, Ting; Song, Zihang; Wang, Hui; Zhang, Zhongping; Jiang, Yang

2018-03-01

The selenium dioxide was used as the precursor to synthesize wide-size-ranged CdSe quantum dots (2.4-5.7 nm) via hot-injection route. The CdSe quantum dots are featured with high crystalline, monodisperse, zinc blende structure and wide emission region (530-635 nm). In order to improve the stability and quantum yield, a phosphine-free single-molecular precursor approach is used to obtain CdSe/CdS core/shell quantum dots. The CdSe/CdS quantum dots are highly fluorescent with quantum yield up to 65%, and persist the good monodispersity and high crystallinity. Moreover, the quantum dots white light-emitting-diodes are fabricated by using the resultant red emission core/shell quantum dots and Y3Al5O12:Ce3+ yellow phosphors as color-conversion layers on a blue InGaN chip. The prepared light-emitting-diodes show good performance with CIE-1931 coordinated of (0.3583, 0.3349), an Ra of 92.9, and a Tc of 4410 K at 20 mA, which indicate that the combination of red-emission QDs and yellow phophors as a promising approach to obtain warm WLEDs with good color rendering.

Spatially selective assembly of quantum dot light emitters in an LED using engineered peptides.

PubMed

Demir, Hilmi Volkan; Seker, Urartu Ozgur Safak; Zengin, Gulis; Mutlugun, Evren; Sari, Emre; Tamerler, Candan; Sarikaya, Mehmet

2011-04-26

Semiconductor nanocrystal quantum dots are utilized in numerous applications in nano- and biotechnology. In device applications, where several different material components are involved, quantum dots typically need to be assembled at explicit locations for enhanced functionality. Conventional approaches cannot meet these requirements where assembly of nanocrystals is usually material-nonspecific, thereby limiting the control of their spatial distribution. Here we demonstrate directed self-assembly of quantum dot emitters at material-specific locations in a color-conversion LED containing several material components including a metal, a dielectric, and a semiconductor. We achieve a spatially selective immobilization of quantum dot emitters by using the unique material selectivity characteristics provided by the engineered solid-binding peptides as smart linkers. Peptide-decorated quantum dots exhibited several orders of magnitude higher photoluminescence compared to the control groups, thus, potentially opening up novel ways to advance these photonic platforms in applications ranging from chemical to biodetection.

Temperature Sensitivity of Water-Soluble CdTe and CdSe/ZnS Quantum Dots Incorporated into Biopolymer Submicron Particles

NASA Astrophysics Data System (ADS)

Slyusarenko, N. V.; Gerasimova, M. A.; Slabko, V. V.; Slyusareva, E. A.

2017-07-01

Polymer particles with sizes 0.3-0.4 μm are synthesized based on chitosan and chondroitin sulfate with incorporated CdTe (core) and CdSe/ZnS (core-shell) quantum dots. Their morphological and spectral properties are investigated by the methods of dynamic scattering, electron microscopy, and absorption and luminescence spectroscopy at temperatures from 10 to 80°C. Spectral effects associated with a change in temperature (a red shift and a decrease in the amplitude of the photoluminescence spectrum) can be explained by the temperature expansion of the quantum dots and activation of surface traps. It is shown that the temperature sensitivity of spectra of the quantum dots incorporated into the biopolymer particles is not less than in water. To develop an optical temperature sensor, the core quantum dots are more preferable than the core-shell quantum dots.

The Effect of Temperature on Photoluminescence Enhancement of Quantum Dots in Brain Slices.

PubMed

Zhao, Fei; Kim, Jongsung

2017-04-01

In this paper, we investigated the effect of temperature on photoluminescence of quantum dots immobilized on the surface of an optical fiber in a rat brain slice. The optical fiber was silanized with 3-aminopropyl trimethoxysilane (APTMS), following which quantum dots with carboxyl functional group were immobilized on the optical fiber via amide bond formation. The effect of temperature on the fluorescence intensity of the quantum dots in rat brain slices was studied. This report shows that the fluorescence intensity of quantum dots increases with the increase of temperature of the brain slice. The fluorescence enhancement phenomenon appears to take place via electron transfer related to pH increase. With the gradual increase of temperature, the fluorescence intensity of quantum dots in solution decreased, while that in the brain slice increased. This enhanced thermal performance of QDs in brain slice makes suggestion for the study of QDs-based brain temperature sensors.

What are the reasons for low use of graphene quantum dots in immunosensing of cancer biomarkers?

PubMed

Hasanzadeh, Mohammad; Shadjou, Nasrin

2017-02-01

Graphene quantum dots-based immunosensors have recently gained importance for detecting antigens and biomarkers responsible for cancer diagnosis. This paper reports a literature survey of the applications of graphene quantum dots for sensing cancer biomarkers. The survey sought to explore three questions: (1) Do graphene quantum dots improve immunosensing technology? (2) If so, can graphene quantum dots have a critical, positive impact on construction of immuno-devices? And (3) What is the reason for some troubles in the application of this technology? The number of published papers in the field seems positively answer the first two questions. However additional efforts must be made to move from the bench to the real diagnosis. Some approaches to improve the analytical performance of graphene quantum dots-based immunosensors through their figures of merit have been also discussed. Copyright © 2016 Elsevier B.V. All rights reserved.

3D super-resolution imaging with blinking quantum dots

PubMed Central

Wang, Yong; Fruhwirth, Gilbert; Cai, En; Ng, Tony; Selvin, Paul R.

2013-01-01

Quantum dots are promising candidates for single molecule imaging due to their exceptional photophysical properties, including their intense brightness and resistance to photobleaching. They are also notorious for their blinking. Here we report a novel way to take advantage of quantum dot blinking to develop an imaging technique in three-dimensions with nanometric resolution. We first applied this method to simulated images of quantum dots, and then to quantum dots immobilized on microspheres. We achieved imaging resolutions (FWHM) of 8–17 nm in the x-y plane and 58 nm (on coverslip) or 81 nm (deep in solution) in the z-direction, approximately 3–7 times better than what has been achieved previously with quantum dots. This approach was applied to resolve the 3D distribution of epidermal growth factor receptor (EGFR) molecules at, and inside of, the plasma membrane of resting basal breast cancer cells. PMID:24093439

Influence of surface states of CuInS2 quantum dots in quantum dots sensitized photo-electrodes

NASA Astrophysics Data System (ADS)

Peng, Zhuoyin; Liu, Yueli; Wu, Lei; Zhao, Yinghan; Chen, Keqiang; Chen, Wen

2016-12-01

Surface states are significant factor for the enhancement of electrochemical performance in CuInS2 quantum dot sensitized photo-electrodes. DDT, OLA, MPA, and S2- ligand capped CuInS2 quantum dot sensitized photo-electrodes are prepared by thermolysis, solvethermal and ligand-exchange processes, respectively, and their optical properties and photoelectrochemical properties are investigated. The S2- ligand enhances the UV-vis absorption and electron-hole separation property as well as the excellent charge transfer performance of the photo-electrodes, which is attributed to the fact that the atomic S2- ligand for the interfacial region of quantum dots may improve the electron transfer rate. These S2--capped CuInS2 quantum dot sensitized photo-electrodes exhibit the excellent photoelectrochemical efficiency and IPCE peak value, which is higher than that of the samples with DDT, OLA and MPA ligands.

Intermediate-band photosensitive device with quantum dots embedded in energy fence barrier

DOEpatents

Forrest, Stephen R.; Wei, Guodan

2010-07-06

A plurality of layers of a first semiconductor material and a plurality of dots-in-a-fence barriers disposed in a stack between a first electrode and a second electrode. Each dots-in-a-fence barrier consists essentially of a plurality of quantum dots of a second semiconductor material embedded between and in direct contact with two layers of a third semiconductor material. Wave functions of the quantum dots overlap as at least one intermediate band. The layers of the third semiconductor material are arranged as tunneling barriers to require a first electron and/or a first hole in a layer of the first material to perform quantum mechanical tunneling to reach the second material within a respective quantum dot, and to require a second electron and/or a second hole in a layer of the first semiconductor material to perform quantum mechanical tunneling to reach another layer of the first semiconductor material.

In-situ laser nano-patterning for ordered InAs/GaAs(001) quantum dot growth

NASA Astrophysics Data System (ADS)

Zhang, Wei; Shi, Zhenwu; Huo, Dayun; Guo, Xiaoxiang; Zhang, Feng; Chen, Linsen; Wang, Qinhua; Zhang, Baoshun; Peng, Changsi

2018-04-01

A study of in-situ laser interference nano-patterning on InGaAs wetting layers was carried out during InAs/GaAs (001) quantum dot molecular beam epitaxy growth. Periodic nano-islands with heights of a few atomic layers were obtained via four-beam laser interference irradiation on the InGaAs wetting layer at an InAs coverage of 0.9 monolayer. The quantum dots nucleated preferentially at edges of nano-islands upon subsequent deposition of InAs on the patterned surface. When the nano-islands are sufficiently small, the patterned substrate could be spontaneously re-flattened and an ordered quantum dot array could be produced on the smooth surface. This letter discusses the mechanisms of nano-patterning and ordered quantum dot nucleation in detail. This study provides a potential technique leading to site-controlled, high-quality quantum dot fabrication.

Plasmon-resonance-enhanced visible-light photocatalytic activity of Ag quantum dots/TiO2 microspheres for methyl orange degradation

NASA Astrophysics Data System (ADS)

Yu, Xin; Shang, Liwei; Wang, Dongjun; An, Li; Li, Zhonghua; Liu, Jiawen; Shen, Jun

2018-06-01

We successfully prepared Ag quantum dots modified TiO2 microspheres by facile solvothermal and calcination method. The as-prepared Ag quantum dots/TiO2 microspheres were characterized by scanning electron microscope, transmission electron microscope, X-ray diffraction, X-ray photoelectron spectroscopy and UV-vis diffuse reflectance spectroscopy. The Ag quantum dots/TiO2 photocatalyst showed excellent visible light absorption and efficient photocatalytic activity for methyl orange degradation. And the sample with the molar ratio of 0.05 (Ag to Ti) showed the best visible light photocatalytic activity for methyl orange degradation, mainly because of the surface plasmon resonance (SPR) effects of Ag quantum dots to generate electron and hole pairs for enhanced visible light photocatalysis. Finally, possible visible light photocatalytic mechanism of Ag quantum dots/TiO2 microspheres for methyl orange degradation was proposed in detail.

Dicke states in multiple quantum dots

NASA Astrophysics Data System (ADS)

Sitek, Anna; Manolescu, Andrei

2013-10-01

We present a theoretical study of the collective optical effects which can occur in groups of three and four quantum dots. We define conditions for stable subradiant (dark) states, rapidly decaying super-radiant states, and spontaneous trapping of excitation. Each quantum dot is treated like a two-level system. The quantum dots are, however, realistic, meaning that they may have different transition energies and dipole moments. The dots interact via a short-range coupling which allows excitation transfer across the dots, but conserves the total population of the system. We calculate the time evolution of single-exciton and biexciton states using the Lindblad equation. In the steady state the individual populations of each dot may have permanent oscillations with frequencies given by the energy separation between the subradiant eigenstates.

Effects of multiple organic ligands on size uniformity and optical properties of ZnSe quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Archana, J., E-mail: archana.jayaram@yahoo.com; Navaneethan, M.; Hayakawa, Y.

2012-08-15

Highlights: ► Highly monodispersed ZnSe quantum dots have been synthesized by wet chemical route. ► Strong quantum confinement effect have been observed in ∼ 4 nm ZnSe quantum dots. ► Enhanced ultraviolet near band emission have been obtained using long chain polymer. -- Abstract: The effects of multi-ligands on the formation and optical transitions of ZnSe quantum dots have been investigated. The dots are synthesized using 3-mercapto-1,2-propanediol and polyvinylpyrrolidone ligands, and have been characterized by X-ray diffraction, transmission electron microscopy (TEM), UV–visible absorption spectroscopy, photoluminescence spectroscopy, and Fourier transform infrared spectroscopy. TEM reveals high monodispersion with an average size ofmore » 4 nm. Polymer-stabilized, organic ligand-passivated ZnSe quantum dots exhibit strong UV emission at 326 nm and strong quantum confinement in the UV–visible absorption spectrum. Uniform size and suppressed surface trap emission are observed when the polymer ligand is used. The possible growth mechanism is discussed.« less

Purcell effect in triangular plasmonic nanopatch antennas with three-layer colloidal quantum dots

NASA Astrophysics Data System (ADS)

Eliseev, S. P.; Kurochkin, N. S.; Vergeles, S. S.; Sychev, V. V.; Chubich, D. A.; Argyrakis, P.; Kolymagin, D. A.; Vitukhnovskii, A. G.

2017-05-01

A model describing a plasmonic nanopatch antenna based on triangular silver nanoprisms and multilayer cadmium chalcogenide quantum dots is introduced. Electromagnetic-field distributions in nanopatch antennas with different orientations of the quantum-dot dipoles are calculated for the first time with the finite element method for numerical electrodynamics simulations. The energy flux through the surface of an emitting quantum dot is calculated for the configurations with the dot in free space, on an aluminum substrate, and in a nanopatch antenna. It is shown that the radiative part of the Purcell factor is as large as 1.7 × 102 The calculated photoluminescence lifetimes of a CdSe/CdS/ZnS colloidal quantum dot in a nanopatch antenna based on a silver nanoprism agree well with the experimental results.

[Spectral Analysis of CdZnSe Ternary Quantum Dots Sensitized TiO2 Tubes and Its Application in Visible-Light Photocatalysis].

PubMed

Han, Zhi-zhong; Ren, Li-li; Pan, Hai-bo; Li, Chun-yan; Chen, Jing-hua; Chen, Jian-zhong

2015-11-01

In this work, cadmium nitrate hexahydrate [Cd(NO₃)₂ · 6H₂O] is as a source of cadmium, zinc nitrate [Zn(NO₃)₂] as a source of zinc source, and NaHSe as a source of selenium which was prepared through reducing the elemental selenium with sodium borohydride (NaBH₄). Then water-soluble Cd₁₋xZnxSe ternary quantum dots with different component were prepared by colloid chemistry. The as-prepared Cd₁₋xZnx Se ternary quantum dots exhibit stable fluorescent property in aqueous solution, and can still maintain good dispersivity at room temperature for four months. Powder X-ray diffraction (XRD) and high resolution transmission electron microscope (HRTEM) were used to analyze crystal structure and morphology of the prepared Cd₁₋xZnxSe. It is found that the as-prepared ternary quantum dots are cubic phase, show as sphere, and the average of particle size is approximate 4 nm. The spectral properties and energy band structure of the as-prepared ternary quantum dots were modulated through changing the atom ratio of elements Zn and Cd. Compared with binary quantum dots CdSe and ZnSe, the ultraviolet-visible (UV-Visible) absorption spectrum and fluorescence (FL) emission spectrum of ternary quantum dots are both red-shift. The composites (Cd₀.₅ Zn₀.₅ Se@TNTs) of Cd₀.₅ Zn₀.₅ Se ternary quantum dots and TiO₂ nanotubes (TNTs) were prepared by directly immerging TNTs into quantum dots dispersive solution for 5 hours. TEM image shows that the Cd₀.₅ Zn₀.₅ Se ternary quantum dots were closely combined to nanotube surface. The infrared spectra show that the Ti-Se bond was formed between Cd₀.₅ Zn₀.₅ Se ternary quantum dots and TiO₂ nanotubes, which improve the stability of the composite. Compared to pristine TNTs, UV-Visible absorption spectrum of the composites is significantly enhanced in the visible region of light. And the absorption band edge of Cd₀.₅Zn₀.₅ Se@TNTs red-shift from 400 to 700 nm. The recombination of the photogenerated electron-hole pairs was restrained with the as-prepared ternary quantum dots. Therefore, the visible-light photocatalytic efficiency was greatly improved. After visible-light irradiation for 60 min, the degradation of Cd₀.₅ Zn₀.₅ Se@TNTs photocatalysts for RhB is nearly 100%, which is about 3. 3 times of that of pristine TNTs and 2. 5 times of that of pure Cd₀.₅ Zn₀.₅ Se ternary quantum dots, respectively.

Mode locking of electron spin coherences in singly charged quantum dots.

PubMed

Greilich, A; Yakovlev, D R; Shabaev, A; Efros, Al L; Yugova, I A; Oulton, R; Stavarache, V; Reuter, D; Wieck, A; Bayer, M

2006-07-21

The fast dephasing of electron spins in an ensemble of quantum dots is detrimental for applications in quantum information processing. We show here that dephasing can be overcome by using a periodic train of light pulses to synchronize the phases of the precessing spins, and we demonstrate this effect in an ensemble of singly charged (In,Ga)As/GaAs quantum dots. This mode locking leads to constructive interference of contributions to Faraday rotation and presents potential applications based on robust quantum coherence within an ensemble of dots.

Cubic GaN quantum dots embedded in zinc-blende AlN microdisks

NASA Astrophysics Data System (ADS)

Bürger, M.; Kemper, R. M.; Bader, C. A.; Ruth, M.; Declair, S.; Meier, C.; Förstner, J.; As, D. J.

2013-09-01

Microresonators containing quantum dots find application in devices like single photon emitters for quantum information technology as well as low threshold laser devices. We demonstrate the fabrication of 60 nm thin zinc-blende AlN microdisks including cubic GaN quantum dots using dry chemical etching techniques. Scanning electron microscopy analysis reveals the morphology with smooth surfaces of the microdisks. Micro-photoluminescence measurements exhibit optically active quantum dots. Furthermore this is the first report of resonator modes in the emission spectrum of a cubic AlN microdisk.

Peptide-coated semiconductor quantum dots and their applications in biological imaging of single molecules in live cells and organisms

NASA Astrophysics Data System (ADS)

Pinaud, Fabien Florent

2007-12-01

A new surface chemistry has been developed for the solubilization and biofunctionalization of inorganic semiconductor nanocrystals fluorescent probes, also known as quantum dots. This chemistry is based on the surface coating of quantum dots with custom-designed polycysteine peptides and yields water-soluble, small, monodispersed and colloidally stable probes that remain bright and photostable in complex biological milieus. This peptide coating strategy was successfully tested on several types of core and core-shell quantum dots emitting from the visible (e.g. CdSe/ZnS) to the NIR spectrum range (e.g. CdTe/CdSe/ZnS). By taking advantage of the versatile physico-chemical properties of peptides, a peptide "toolkit" was designed and employed to impart several biological functions to individual quantum dots and control their biochemical activity at the nanometer scale. These biofunctionalized peptide-coated quantum dots were exploited in very diverse biological applications. Near-infrared emitting quantum dot probes were engineered with optimized blood circulation and biodistribution properties for in vivo animal imaging. Visible emitting quantum dots were used for single molecule tracking of raft-associated GPI-anchored proteins in live cells. This last application revealed the presence of discrete and non-caveolar lipid microdomains capable of impeding free lateral diffusions in the plasma membrane of Hela cells. Imaging and tracking of peptide-coated quantum dots provided the first direct evidence that microdomains having the composition and behavior expected for lipid rafts can induce molecular compartmentalization in the membrane of living cells.

Two-electrons quantum dot in plasmas under the external fields

NASA Astrophysics Data System (ADS)

Bahar, M. K.; Soylu, A.

2018-02-01

In this study, for the first time, the combined effects of the external electric field, magnetic field, and confinement frequency on energies of two-electron parabolic quantum dots in Debye and quantum plasmas modeled by more general exponential cosine screened Coulomb (MGECSC) potential are investigated by numerically solving the Schrödinger equation using the asymptotic iteration method. The MGECSC potential includes four different potential forms when considering different sets of the parameters in potential. Since the plasma is an important experimental argument for quantum dots, the influence of plasmas modeled by the MGECSC potential on quantum dots is probed. The confinement frequency of quantum dots and the external fields created significant quantum restrictions on quantum dot. In this study, as well as discussion of the functionalities of the quantum restrictions for experimental applications, the parameters are also compared with each other in terms of influence and behaviour. In this manner, the motivation points of this study are summarized as follows: Which parameter can be alternative to which parameter, in terms of experimental applications? Which parameters exhibit similar behaviour? What is the role of plasmas on the corresponding behaviours? In the light of these research studies, it can be said that obtained results and performed discussions would be important in experimental and theoretical research related to plasma physics and/or quantum dots.

Photoconductive gain and quantum efficiency of remotely doped Ge/Si quantum dot photodetectors

NASA Astrophysics Data System (ADS)

Yakimov, A. I.; Kirienko, V. V.; Armbrister, V. A.; Bloshkin, A. A.; Dvurechenskii, A. V.; Shklyaev, A. A.

2016-10-01

We study the effect of quantum dot charging on the mid-infrared photocurrent, optical gain, hole capture probability, and absorption quantum efficiency in remotely delta-doped Ge/Si quantum dot photodetectors. The dot occupation with holes is controlled by varying dot and doping densities. From our investigations of samples doped to contain from about one to nine holes per dot we observe an over 10 times gain enhancement and similar suppression of the hole capture probability with increased carrier population. The data are explained by quenching the capture process and increasing the photoexcited hole lifetime due to formation of the repulsive Coulomb potential of the extra holes inside the quantum dots. The normal incidence quantum efficiency is found to be strongly asymmetric with respect to applied bias polarity. Based on the polarization-dependent absorption measurements it is concluded that, at a positive voltage, when holes move toward the nearest δ-doping plane, photocurrent is originated from the bound-to-continuum transitions of holes between the ground state confined in Ge dots and the extended states of the Si matrix. At a negative bias polarity, the photoresponse is caused by optical excitation to a quasibound state confined near the valence band edge with subsequent tunneling to the Si valence band. In a latter case, the possibility of hole transfer into continuum states arises from the electric field generated by charge distributed between quantum dots and delta-doping planes.

Synthesis of Cesium Lead Halide Perovskite Quantum Dots

ERIC Educational Resources Information Center

Shekhirev, Mikhail; Goza, John; Teeter, Jacob D.; Lipatov, Alexey; Sinitskii, Alexander

2017-01-01

Synthesis of quantum dots is a valuable experiment for demonstration and discussion of quantum phenomena in undergraduate chemistry curricula. Recently, a new class of all-inorganic perovskite quantum dots (QDs) with a formula of CsPbX[subscript 3] (X = Cl, Br, I) was presented and attracted tremendous attention. Here we adapt the synthesis of…

Quantum soldering of individual quantum dots.

PubMed

Roy, Xavier; Schenck, Christine L; Ahn, Seokhoon; Lalancette, Roger A; Venkataraman, Latha; Nuckolls, Colin; Steigerwald, Michael L

2012-12-07

Making contact to a quantum dot: Single quantum-dot electronic circuits are fabricated by wiring atomically precise metal chalcogenide clusters with conjugated molecular connectors. These wired clusters can couple electronically to nanoscale electrodes and be tuned to control the charge-transfer characteristics (see picture). Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Surface treatment of nanocrystal quantum dots after film deposition

DOEpatents

Sykora, Milan; Koposov, Alexey; Fuke, Nobuhiro

2015-02-03

Provided are methods of surface treatment of nanocrystal quantum dots after film deposition so as to exchange the native ligands of the quantum dots for exchange ligands that result in improvement in charge extraction from the nanocrystals.

Polarized quantum dot emission in electrohydrodynamic jet printed photonic crystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

See, Gloria G.; Xu, Lu; Nuzzo, Ralph G.

2015-08-03

Tailored optical output, such as color purity and efficient optical intensity, are critical considerations for displays, particularly in mobile applications. To this end, we demonstrate a replica molded photonic crystal structure with embedded quantum dots. Electrohydrodynamic jet printing is used to control the position of the quantum dots within the device structure. This results in significantly less waste of the quantum dot material than application through drop-casting or spin coating. In addition, the targeted placement of the quantum dots minimizes any emission outside of the resonant enhancement field, which enables an 8× output enhancement and highly polarized emission from themore » photonic crystal structure.« less

Comparative photoluminescence study of close-packed and colloidal InP/ZnS quantum dots

NASA Astrophysics Data System (ADS)

Thuy, Ung Thi Dieu; Thuy, Pham Thi; Liem, Nguyen Quang; Li, Liang; Reiss, Peter

2010-02-01

This letter reports on the comparative photoluminescence study of InP/ZnS quantum dots in the close-packed solid state and in colloidal solution. The steady-state photoluminescence spectrum of the close-packed InP/ZnS quantum dots peaks at a longer wavelength than that of the colloidal ones. Time-resolved photoluminescence shows that the close-packed quantum dots possess a shorter luminescence decay time and strongly increased spectral shift with the time delayed from the excitation moment in comparison with the colloidal ones. The observed behavior is discussed on the basis of energy transfer enabled by the short interparticle distance between the close-packed quantum dots.

Complete Coherent Control of a Quantum Dot Strongly Coupled to a Nanocavity.

PubMed

Dory, Constantin; Fischer, Kevin A; Müller, Kai; Lagoudakis, Konstantinos G; Sarmiento, Tomas; Rundquist, Armand; Zhang, Jingyuan L; Kelaita, Yousif; Vučković, Jelena

2016-04-26

Strongly coupled quantum dot-cavity systems provide a non-linear configuration of hybridized light-matter states with promising quantum-optical applications. Here, we investigate the coherent interaction between strong laser pulses and quantum dot-cavity polaritons. Resonant excitation of polaritonic states and their interaction with phonons allow us to observe coherent Rabi oscillations and Ramsey fringes. Furthermore, we demonstrate complete coherent control of a quantum dot-photonic crystal cavity based quantum-bit. By controlling the excitation power and phase in a two-pulse excitation scheme we achieve access to the full Bloch sphere. Quantum-optical simulations are in good agreement with our experiments and provide insight into the decoherence mechanisms.

Complete Coherent Control of a Quantum Dot Strongly Coupled to a Nanocavity

NASA Astrophysics Data System (ADS)

Dory, Constantin; Fischer, Kevin A.; Müller, Kai; Lagoudakis, Konstantinos G.; Sarmiento, Tomas; Rundquist, Armand; Zhang, Jingyuan L.; Kelaita, Yousif; Vučković, Jelena

2016-04-01

Strongly coupled quantum dot-cavity systems provide a non-linear configuration of hybridized light-matter states with promising quantum-optical applications. Here, we investigate the coherent interaction between strong laser pulses and quantum dot-cavity polaritons. Resonant excitation of polaritonic states and their interaction with phonons allow us to observe coherent Rabi oscillations and Ramsey fringes. Furthermore, we demonstrate complete coherent control of a quantum dot-photonic crystal cavity based quantum-bit. By controlling the excitation power and phase in a two-pulse excitation scheme we achieve access to the full Bloch sphere. Quantum-optical simulations are in good agreement with our experiments and provide insight into the decoherence mechanisms.

Facile synthetic method for pristine graphene quantum dots and graphene oxide quantum dots: origin of blue and green luminescence.

PubMed

Liu, Fei; Jang, Min-Ho; Ha, Hyun Dong; Kim, Je-Hyung; Cho, Yong-Hoon; Seo, Tae Seok

2013-07-19

Pristine graphene quantum dots and graphene oxide quantum dots are synthesized by chemical exfoliation from the graphite nanoparticles with high uniformity in terms of shape (circle), size (less than 4 nm), and thickness (monolayer). The origin of the blue and green photoluminescence of GQDs and GOQDs is attributed to intrinsic and extrinsic energy states, respectively. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Semiconductor quantum dot scintillation under gamma-ray irradiation.

PubMed

Létant, S E; Wang, T-F

2006-12-01

We recently demonstrated the ability of semiconductor quantum dots to convert alpha radiation into visible photons. In this letter, we report on the scintillation of quantum dots under gamma irradiation and compare the energy resolution of the 59 keV line of americium-241 obtained with our quantum dot-glass nanocomposite to that of a standard sodium iodide scintillator. A factor 2 improvement is demonstrated experimentally and interpreted theoretically using a combination of energy-loss and photon-transport models.

Excitonic quantum interference in a quantum dot chain with rings.

PubMed

Hong, Suc-Kyoung; Nam, Seog Woo; Yeon, Kyu-Hwang

2008-04-16

We demonstrate excitonic quantum interference in a closely spaced quantum dot chain with nanorings. In the resonant dipole-dipole interaction model with direct diagonalization method, we have found a peculiar feature that the excitation of specified quantum dots in the chain is completely inhibited, depending on the orientational configuration of the transition dipole moments and specified initial preparation of the excitation. In practice, these excited states facilitating quantum interference can provide a conceptual basis for quantum interference devices of excitonic hopping.

A triple quantum dot based nano-electromechanical memory device

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pozner, R.; Lifshitz, E.; Solid State Institute, Technion-Israel Institute of Technology, Haifa 32000

Colloidal quantum dots (CQDs) are free-standing nano-structures with chemically tunable electronic properties. This tunability offers intriguing possibilities for nano-electromechanical devices. In this work, we consider a nano-electromechanical nonvolatile memory (NVM) device incorporating a triple quantum dot (TQD) cluster. The device operation is based on a bias induced motion of a floating quantum dot (FQD) located between two bound quantum dots (BQDs). The mechanical motion is used for switching between two stable states, “ON” and “OFF” states, where ligand-mediated effective interdot forces between the BQDs and the FQD serve to hold the FQD in each stable position under zero bias. Consideringmore » realistic microscopic parameters, our quantum-classical theoretical treatment of the TQD reveals the characteristics of the NVM.« less

Transport through an impurity tunnel coupled to a Si/SiGe quantum dot

DOE PAGES

Foote, Ryan H.; Ward, Daniel R.; Prance, J. R.; ...

2015-09-11

Achieving controllable coupling of dopants in silicon is crucial for operating donor-based qubit devices, but it is difficult because of the small size of donor-bound electron wavefunctions. Here in this paper, we report the characterization of a quantum dot coupled to a localized electronic state and present evidence of controllable coupling between the quantum dot and the localized state. A set of measurements of transport through the device enable the determination that the most likely location of the localized state is consistent with a location in the quantum well near the edge of the quantum dot. Finally, our results aremore » consistent with a gate-voltage controllable tunnel coupling, which is an important building block for hybrid donor and gate-defined quantum dot devices.« less

Color-selective photodetection from intermediate colloidal quantum dots buried in amorphous-oxide semiconductors.

PubMed

Cho, Kyung-Sang; Heo, Keun; Baik, Chan-Wook; Choi, Jun Young; Jeong, Heejeong; Hwang, Sungwoo; Lee, Sang Yeol

2017-10-10

We report color-selective photodetection from intermediate, monolayered, quantum dots buried in between amorphous-oxide semiconductors. The proposed active channel in phototransistors is a hybrid configuration of oxide-quantum dot-oxide layers, where the gate-tunable electrical property of silicon-doped, indium-zinc-oxide layers is incorporated with the color-selective properties of quantum dots. A remarkably high detectivity (8.1 × 10 13 Jones) is obtained, along with three major findings: fast charge separation in monolayered quantum dots; efficient charge transport through high-mobility oxide layers (20 cm 2  V -1  s -1 ); and gate-tunable drain-current modulation. Particularly, the fast charge separation rate of 3.3 ns -1 measured with time-resolved photoluminescence is attributed to the intermediate quantum dots buried in oxide layers. These results facilitate the realization of efficient color-selective detection exhibiting a photoconductive gain of 10 7 , obtained using a room-temperature deposition of oxide layers and a solution process of quantum dots. This work offers promising opportunities in emerging applications for color detection with sensitivity, transparency, and flexibility.The development of highly sensitive photodetectors is important for image sensing and optical communication applications. Cho et al., report ultra-sensitive photodetectors based on monolayered quantum dots buried in between amorphous-oxide semiconductors and demonstrate color-detecting logic gates.

Influence of the quantum dot geometry on p -shell transitions in differently charged quantum dots

NASA Astrophysics Data System (ADS)

Holtkemper, M.; Reiter, D. E.; Kuhn, T.

2018-02-01

Absorption spectra of neutral, negatively, and positively charged semiconductor quantum dots are studied theoretically. We provide an overview of the main energetic structure around the p -shell transitions, including the influence of nearby nominally dark states. Based on the envelope function approximation, we treat the four-band Luttinger theory as well as the direct and short-range exchange Coulomb interactions within a configuration interaction approach. The quantum dot confinement is approximated by an anisotropic harmonic potential. We present a detailed investigation of state mixing and correlations mediated by the individual interactions. Differences and similarities between the differently charged quantum dots are highlighted. Especially large differences between negatively and positively charged quantum dots become evident. We present a visualization of energetic shifts and state mixtures due to changes in size, in-plane asymmetry, and aspect ratio. Thereby we provide a better understanding of the experimentally hard to access question of quantum dot geometry effects. Our findings show a method to determine the in-plane asymmetry from photoluminescence excitation spectra. Furthermore, we supply basic knowledge for tailoring the strength of certain state mixtures or the energetic order of particular excited states via changes of the shape of the quantum dot. Such knowledge builds the basis to find the optimal QD geometry for possible applications and experiments using excited states.

On the size and temperature dependence of the energy gap in cadmium-selenide quantum dots embedded in fluorophosphate glasses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lipatova, Zh. O., E-mail: zluka-yo@mail.ru; Kolobkova, E. V.; Babkina, A. N.

2017-03-15

The temperature and size dependences of the energy gap in CdSe quantum dots with diameters of 2.4, 4.0, and 5.2 nm embedded in fluorophosphate glasses are investigated. It is shown that the temperature coefficient of the band gap dE{sub g}/dT in the quantum dots differs from the bulk value and depends strictly on the dot size. It is found that, furthermore, the energy of each transition in these quantum dots is characterized by an individual temperature coefficient dE/dT.

Theoretical study of polarization dependence of carrier-induced refractive index change of quantum dot.

PubMed

Miao, Qingyuan; Yang, Ziyi; Dong, Jianji; He, Ping-An; Huang, Dexiu

2018-02-05

The influences of dot material component, barrier material component, aspect ratio and carrier density on the refractive index changes of TE mode and TM mode of columnar quantum dot are analyzed, and a multiparameter adjustment method is proposed to realize low polarization dependence of refractive index change. Then the quantum dots with low polarization dependence of refractive index change (<1.5%) within C-band (1530 nm - 1565 nm) are designed, and it shows that quantum dots with different material parameters are anticipated to have similar characteristics of low polarization dependence.

Electrostatically defined silicon quantum dots with counted antimony donor implants

DOE Office of Scientific and Technical Information (OSTI.GOV)

Singh, M., E-mail: msingh@sandia.gov; Luhman, D. R.; Lilly, M. P.

2016-02-08

Deterministic control over the location and number of donors is crucial to donor spin quantum bits (qubits) in semiconductor based quantum computing. In this work, a focused ion beam is used to implant antimony donors in 100 nm × 150 nm windows straddling quantum dots. Ion detectors are integrated next to the quantum dots to sense the implants. The numbers of donors implanted can be counted to a precision of a single ion. In low-temperature transport measurements, regular Coulomb blockade is observed from the quantum dots. Charge offsets indicative of donor ionization are also observed in devices with counted donor implants.

Effects of Shannon entropy and electric field on polaron in RbCl triangular quantum dot

NASA Astrophysics Data System (ADS)

M, Tiotsop; A, J. Fotue; S, C. Kenfack; N, Issofa; H, Fotsin; L, C. Fai

2016-04-01

In this paper, the time evolution of the quantum mechanical state of a polaron is examined using the Pekar type variational method on the condition of the electric-LO-phonon strong-coupling and polar angle in RbCl triangular quantum dot. We obtain the eigenenergies, and the eigenfunctions of the ground state, and the first excited state respectively. This system in a quantum dot can be treated as a two-level quantum system qubit and the numerical calculations are performed. The effects of Shannon entropy and electric field on the polaron in the RbCl triangular quantum dot are also studied.

Hybrid plasmonic systems: from optical transparencies to strong coupling and entanglement

NASA Astrophysics Data System (ADS)

Gray, Stephen K.

2018-02-01

Classical electrodynamics and quantum mechanical models of quantum dots and molecules interacting with plasmonic systems are discussed. Calculations show that just one quantum dot interacting with a plasmonic system can lead to interesting optical effects, including optical transparencies and more general Fano resonance features that can be tailored with ultrafast laser pulses. Such effects can occur in the limit of moderate coupling between quantum dot and plasmonic system. The approach to the strong coupling regime is also discussed. In cases with two or more quantum dots within a plasmonic system, the possibility of quantum entanglement mediated through the dissipative plasmonic structure arises.

Electrostatically defined silicon quantum dots with counted antimony donor implants

NASA Astrophysics Data System (ADS)

Singh, M.; Pacheco, J. L.; Perry, D.; Garratt, E.; Ten Eyck, G.; Bishop, N. C.; Wendt, J. R.; Manginell, R. P.; Dominguez, J.; Pluym, T.; Luhman, D. R.; Bielejec, E.; Lilly, M. P.; Carroll, M. S.

2016-02-01

Deterministic control over the location and number of donors is crucial to donor spin quantum bits (qubits) in semiconductor based quantum computing. In this work, a focused ion beam is used to implant antimony donors in 100 nm × 150 nm windows straddling quantum dots. Ion detectors are integrated next to the quantum dots to sense the implants. The numbers of donors implanted can be counted to a precision of a single ion. In low-temperature transport measurements, regular Coulomb blockade is observed from the quantum dots. Charge offsets indicative of donor ionization are also observed in devices with counted donor implants.

Growth of group II-VI semiconductor quantum dots with strong quantum confinement and low size dispersion

NASA Astrophysics Data System (ADS)

Pandey, Praveen K.; Sharma, Kriti; Nagpal, Swati; Bhatnagar, P. K.; Mathur, P. C.

2003-11-01

CdTe quantum dots embedded in glass matrix are grown using two-step annealing method. The results for the optical transmission characterization are analysed and compared with the results obtained from CdTe quantum dots grown using conventional single-step annealing method. A theoretical model for the absorption spectra is used to quantitatively estimate the size dispersion in the two cases. In the present work, it is established that the quantum dots grown using two-step annealing method have stronger quantum confinement, reduced size dispersion and higher volume ratio as compared to the single-step annealed samples. (

Control of spontaneous emission of quantum dots using correlated effects of metal oxides and dielectric materials

NASA Astrophysics Data System (ADS)

Sadeghi, S. M.; Wing, W. J.; Gutha, R. R.; Capps, L.

2017-03-01

We study the emission dynamics of semiconductor quantum dots in the presence of the correlated impact of metal oxides and dielectric materials. For this we used layered material structures consisting of a base substrate, a dielectric layer, and an ultrathin layer of a metal oxide. After depositing colloidal CdSe/ZnS quantum dots on the top of the metal oxide, we used spectral and time-resolved techniques to show that, depending on the type and thickness of the dielectric material, the metal oxide can characteristically change the interplay between intrinsic excitons, defect states, and the environment, offering new material properties. Our results show that aluminum oxide, in particular, can strongly change the impact of amorphous silicon on the emission dynamics of quantum dots by balancing the intrinsic near band emission and fast trapping of carriers. In such a system the silicon/aluminum oxide charge barrier can lead to large variation of the radiative lifetime of quantum dots and control of the photo-ejection rate of electrons in quantum dots. The results provide unique techniques to investigate and modify physical properties of dielectrics and manage optical and electrical properties of quantum dots.

On the origin of stretched exponential (Kohlrausch) relaxation kinetics in the room temperature luminescence decay of colloidal quantum dots.

PubMed

Bodunov, E N; Antonov, Yu A; Simões Gamboa, A L

2017-03-21

The non-exponential room temperature luminescence decay of colloidal quantum dots is often well described by a stretched exponential function. However, the physical meaning of the parameters of the function is not clear in the majority of cases reported in the literature. In this work, the room temperature stretched exponential luminescence decay of colloidal quantum dots is investigated theoretically in an attempt to identify the underlying physical mechanisms associated with the parameters of the function. Three classes of non-radiative transition processes between the excited and ground states of colloidal quantum dots are discussed: long-range resonance energy transfer, multiphonon relaxation, and contact quenching without diffusion. It is shown that multiphonon relaxation cannot explain a stretched exponential functional form of the luminescence decay while such dynamics of relaxation can be understood in terms of long-range resonance energy transfer to acceptors (molecules, quantum dots, or anharmonic molecular vibrations) in the environment of the quantum dots acting as energy-donors or by contact quenching by acceptors (surface traps or molecules) distributed statistically on the surface of the quantum dots. These non-radiative transition processes are assigned to different ranges of the stretching parameter β.

Comparison of the Optical Properties of Graphene and Alkyl-terminated Si and Ge Quantum Dots.

PubMed

de Weerd, Chris; Shin, Yonghun; Marino, Emanuele; Kim, Joosung; Lee, Hyoyoung; Saeed, Saba; Gregorkiewicz, Tom

2017-10-31

Semiconductor quantum dots are widely investigated due to their size dependent energy structure. In particular, colloidal quantum dots represent a promising nanomaterial for optoelectronic devices, such as photodetectors and solar cells, but also luminescent markers for biotechnology, among other applications. Ideal materials for these applications should feature efficient radiative recombination and absorption transitions, altogether with spectral tunability over a wide range. Group IV semiconductor quantum dots can fulfill these requirements and serve as an alternative to the commonly used direct bandgap materials containing toxic and/or rare elements. Here, we present optical properties of butyl-terminated Si and Ge quantum dots and compare them to those of graphene quantum dots, finding them remarkably similar. We investigate their time-resolved photoluminescence emission as well as the photoluminescence excitation and linear absorption spectra. We contemplate that their emission characteristics indicate a (semi-) resonant activation of the emitting channel; the photoluminescence excitation shows characteristics similar to those of a molecule. The optical density is consistent with band-to-band absorption processes originating from core-related states. Hence, these observations strongly indicate a different microscopic origin for absorption and radiative recombination in the three investigated quantum dot systems.

Control of spontaneous emission of quantum dots using correlated effects of metal oxides and dielectric materials.

PubMed

Sadeghi, S M; Wing, W J; Gutha, R R; Capps, L

2017-03-03

We study the emission dynamics of semiconductor quantum dots in the presence of the correlated impact of metal oxides and dielectric materials. For this we used layered material structures consisting of a base substrate, a dielectric layer, and an ultrathin layer of a metal oxide. After depositing colloidal CdSe/ZnS quantum dots on the top of the metal oxide, we used spectral and time-resolved techniques to show that, depending on the type and thickness of the dielectric material, the metal oxide can characteristically change the interplay between intrinsic excitons, defect states, and the environment, offering new material properties. Our results show that aluminum oxide, in particular, can strongly change the impact of amorphous silicon on the emission dynamics of quantum dots by balancing the intrinsic near band emission and fast trapping of carriers. In such a system the silicon/aluminum oxide charge barrier can lead to large variation of the radiative lifetime of quantum dots and control of the photo-ejection rate of electrons in quantum dots. The results provide unique techniques to investigate and modify physical properties of dielectrics and manage optical and electrical properties of quantum dots.

Cadmium-containing nanoparticles: Perspectives on pharmacology and toxicology of quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rzigalinski, Beverly A.; Strobl, Jeannine S.

2009-08-01

The field of nanotechnology is rapidly expanding with the development of novel nanopharmaceuticals that have potential for revolutionizing medical treatment. The rapid pace of expansion in this field has exceeded the pace of pharmacological and toxicological research on the effects of nanoparticles in the biological environment. The development of cadmium-containing nanoparticles, known as quantum dots, show great promise for treatment and diagnosis of cancer and targeted drug delivery, due to their size-tunable fluorescence and ease of functionalization for tissue targeting. However, information on pharmacology and toxicology of quantum dots needs much further development, making it difficult to assess the risksmore » associated with this new nanotechnology. Further, nanotechnology poses yet another risk for toxic cadmium, which will now enter the biological realm in nano-form. In this review, we discuss cadmium-containing quantum dots and their physicochemical properties at the nano-scale. We summarize the existing work on pharmacology and toxicology of cadmium-containing quantum dots and discuss perspectives in their utility in disease treatment. Finally, we identify critical gaps in our knowledge of cadmium quantum dot toxicity, and how these gaps need to be assessed to enable quantum dot nanotechnology to transit safely from bench to bedside.« less

Excitonic complexes in single zinc-blende GaN/AlN quantum dots grown by droplet epitaxy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sergent, S.; Kako, S.; Bürger, M.

2014-10-06

We study by microphotoluminescence the optical properties of single zinc-blende GaN/AlN quantum dots grown by droplet epitaxy. We show evidences of both excitonic and multiexcitonic recombinations in individual quantum dots with radiative lifetimes shorter than 287 ± 8 ps. Owing to large band offsets and a large exciton binding energy, the excitonic recombinations of single zinc-blende GaN/AlN quantum dots can be observed up to 300 K.

Mode-locking of an InAs Quantum Dot Based Vertical External Cavity Surface Emitting Laser Using Atomic Layer Graphene

DTIC Science & Technology

2015-07-16

SECURITY CLASSIFICATION OF: The InAs quantum dot (QD) grown on GaAs substrates represents a highly performance active region in the 1 - 1.3 µm...2015 Approved for Public Release; Distribution Unlimited Final Report: Mode-locking of an InAs Quantum Dot Based Vertical External Cavity Surface...ABSTRACT Final Report: Mode-locking of an InAs Quantum Dot Based Vertical External Cavity Surface Emitting Laser Using Atomic Layer Graphene Report

Study of strain boundary conditions and GaAs buffer sizes in InGaAs quantum dots

NASA Technical Reports Server (NTRS)

Oyafuso, F.; Klimeck, G.; Boykin, T. B.; Bowen, R. C.; Allmen, P. von

2003-01-01

NEMO 3-D has been developed for the simulation of electronic structure in self-assembled InGaAs quantum dots on GaAs substrates. Typical self-assembled quantum dots in that material system contain about 0.5 to 1 million atoms. Effects of strain by the surrounding GaAs buffer modify the electronic structure inside the quantum dot significantly and a large GaAs buffer must be included in the strain and electronic structure.

Spin fine structure of optically excited quantum dot molecules

NASA Astrophysics Data System (ADS)

Scheibner, M.; Doty, M. F.; Ponomarev, I. V.; Bracker, A. S.; Stinaff, E. A.; Korenev, V. L.; Reinecke, T. L.; Gammon, D.

2007-06-01

The interaction between spins in coupled quantum dots is revealed in distinct fine structure patterns in the measured optical spectra of InAs/GaAs double quantum dot molecules containing zero, one, or two excess holes. The fine structure is explained well in terms of a uniquely molecular interplay of spin-exchange interactions, Pauli exclusion, and orbital tunneling. This knowledge is critical for converting quantum dot molecule tunneling into a means of optically coupling not just orbitals but also spins.

Quantum Dots Microstructured Optical Fiber for X-Ray Detection

NASA Technical Reports Server (NTRS)

DeHaven, Stan; Williams, Phillip; Burke, Eric

2015-01-01

Microstructured optical fibers containing quantum dots scintillation material comprised of zinc sulfide nanocrystals doped with magnesium sulfide are presented. These quantum dots are applied inside the microstructured optical fibers using capillary action. The x-ray photon counts of these fibers are compared to the output of a collimated CdTe solid state detector over an energy range from 10 to 40 keV. The results of the fiber light output and associated effects of an acrylate coating and the quantum dot application technique are discussed.

Near-infrared quantum dots for HER2 localization and imaging of cancer cells.

PubMed

Rizvi, Sarwat B; Rouhi, Sepideh; Taniguchi, Shohei; Yang, Shi Yu; Green, Mark; Keshtgar, Mo; Seifalian, Alexander M

2014-01-01

Quantum dots are fluorescent nanoparticles with unique photophysical properties that allow them to be used as diagnostic, therapeutic, and theranostic agents, particularly in medical and surgical oncology. Near-infrared-emitting quantum dots can be visualized in deep tissues because the biological window is transparent to these wavelengths. Their small sizes and free surface reactive groups that can be conjugated to biomolecules make them ideal probes for in vivo cancer localization, targeted chemotherapy, and image-guided cancer surgery. The human epidermal growth factor receptor 2 gene (HER2/neu) is overexpressed in 25%-30% of breast cancers. The current methods of detection for HER2 status, including immunohistochemistry and fluorescence in situ hybridization, are used ex vivo and cannot be used in vivo. In this paper, we demonstrate the application of near-infrared-emitting quantum dots for HER2 localization in fixed and live cancer cells as a first step prior to their in vivo application. Near-infrared-emitting quantum dots were characterized and their in vitro toxicity was established using three cancer cell lines, ie, HepG2, SK-BR-3 (HER2-overexpressing), and MCF7 (HER2-underexpressing). Mouse antihuman anti-HER2 monoclonal antibody was conjugated to the near-infrared-emitting quantum dots. In vitro toxicity studies showed biocompatibility of SK-BR-3 and MCF7 cell lines with near-infrared-emitting quantum dots at a concentration of 60 μg/mL after one hour and 24 hours of exposure. Near-infrared-emitting quantum dot antiHER2-antibody bioconjugates successfully localized HER2 receptors on SK-BR-3 cells. Near-infrared-emitting quantum dot bioconjugates can be used for rapid localization of HER2 receptors and can potentially be used for targeted therapy as well as image-guided surgery.

Tuning Single Quantum Dot Emission with a Micromirror.

PubMed

Yuan, Gangcheng; Gómez, Daniel; Kirkwood, Nicholas; Mulvaney, Paul

2018-02-14

The photoluminescence of single quantum dots fluctuates between bright (on) and dark (off) states, also termed fluorescence intermittency or blinking. This blinking limits the performance of quantum dot-based devices such as light-emitting diodes and solar cells. However, the origins of the blinking remain unresolved. Here, we use a movable gold micromirror to determine both the quantum yield of the bright state and the orientation of the excited state dipole of single quantum dots. We observe that the quantum yield of the bright state is close to unity for these single QDs. Furthermore, we also study the effect of a micromirror on blinking, and then evaluate excitation efficiency, biexciton quantum yield, and detection efficiency. The mirror does not modify the off-time statistics, but it does change the density of optical states available to the quantum dot and hence the on times. The duration of the on times can be lengthened due to an increase in the radiative recombination rate.

Highly indistinguishable and strongly entangled photons from symmetric GaAs quantum dots.

PubMed

Huber, Daniel; Reindl, Marcus; Huo, Yongheng; Huang, Huiying; Wildmann, Johannes S; Schmidt, Oliver G; Rastelli, Armando; Trotta, Rinaldo

2017-05-26

The development of scalable sources of non-classical light is fundamental to unlocking the technological potential of quantum photonics. Semiconductor quantum dots are emerging as near-optimal sources of indistinguishable single photons. However, their performance as sources of entangled-photon pairs are still modest compared to parametric down converters. Photons emitted from conventional Stranski-Krastanov InGaAs quantum dots have shown non-optimal levels of entanglement and indistinguishability. For quantum networks, both criteria must be met simultaneously. Here, we show that this is possible with a system that has received limited attention so far: GaAs quantum dots. They can emit triggered polarization-entangled photons with high purity (g (2) (0) = 0.002±0.002), high indistinguishability (0.93±0.07 for 2 ns pulse separation) and high entanglement fidelity (0.94±0.01). Our results show that GaAs might be the material of choice for quantum-dot entanglement sources in future quantum technologies.

Highly indistinguishable and strongly entangled photons from symmetric GaAs quantum dots

PubMed Central

Huber, Daniel; Reindl, Marcus; Huo, Yongheng; Huang, Huiying; Wildmann, Johannes S.; Schmidt, Oliver G.; Rastelli, Armando; Trotta, Rinaldo

2017-01-01

The development of scalable sources of non-classical light is fundamental to unlocking the technological potential of quantum photonics. Semiconductor quantum dots are emerging as near-optimal sources of indistinguishable single photons. However, their performance as sources of entangled-photon pairs are still modest compared to parametric down converters. Photons emitted from conventional Stranski–Krastanov InGaAs quantum dots have shown non-optimal levels of entanglement and indistinguishability. For quantum networks, both criteria must be met simultaneously. Here, we show that this is possible with a system that has received limited attention so far: GaAs quantum dots. They can emit triggered polarization-entangled photons with high purity (g(2)(0) = 0.002±0.002), high indistinguishability (0.93±0.07 for 2 ns pulse separation) and high entanglement fidelity (0.94±0.01). Our results show that GaAs might be the material of choice for quantum-dot entanglement sources in future quantum technologies. PMID:28548081

Role of surface states and defects in the ultrafast nonlinear optical properties of CuS quantum dots

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mary, K. A. Ann; Unnikrishnan, N. V., E-mail: nvu100@yahoo.com; Philip, Reji

2014-07-01

We report facile preparation of water dispersible CuS quantum dots (2–4 nm) and nanoparticles (5–11 nm) through a nontoxic, green, one-pot synthesis method. Optical and microstructural studies indicate the presence of surface states and defects (dislocations, stacking faults, and twins) in the quantum dots. The smaller crystallite size and quantum dot formation have significant effects on the high energy excitonic and low energy plasmonic absorption bands. Effective two-photon absorption coefficients measured using 100 fs laser pulses employing open-aperture Z-scan in the plasmonic region of 800 nm reveal that CuS quantum dots are better ultrafast optical limiters compared to CuS nanoparticles.

Measuring the complex admittance and tunneling rate of a germanium hut wire hole quantum dot

NASA Astrophysics Data System (ADS)

Li, Yan; Li, Shu-Xiao; Gao, Fei; Li, Hai-Ou; Xu, Gang; Wang, Ke; Liu, He; Cao, Gang; Xiao, Ming; Wang, Ting; Zhang, Jian-Jun; Guo, Guo-Ping

2018-05-01

We investigate the microwave reflectometry of an on-chip reflection line cavity coupled to a Ge hut wire hole quantum dot. The amplitude and phase responses of the cavity can be used to measure the complex admittance and evaluate the tunneling rate of the quantum dot, even in the region where transport signal through the quantum dot is too small to be measured by conventional direct transport means. The experimental observations are found to be in good agreement with a theoretical model of the hybrid system based on cavity frequency shift and linewidth shift. Our experimental results take the first step towards fast and sensitive readout of charge and spin states in Ge hut wire hole quantum dot.

Polarization control of quantum dot emission by chiral photonic crystal slabs

NASA Astrophysics Data System (ADS)

Lobanov, Sergey V.; Weiss, Thomas; Gippius, Nikolay A.; Tikhodeev, Sergei G.; Kulakovskii, Vladimir D.; Konishi, Kuniaki; Kuwata-Gonokami, Makoto

2015-04-01

We investigate theoretically the polarization properties of the quantum dot's optical emission from chiral photonic crystal structures made of achiral materials in the absence of external magnetic field at room temperature. The mirror symmetry of the local electromagnetic field is broken in this system due to the decreased symmetry of the chiral modulated layer. As a result, the radiation of randomly polarized quantum dots normal to the structure becomes partially circularly polarized. The sign and degree of circular polarization are determined by the geometry of the chiral modulated structure and depend on the radiation frequency. A degree of circular polarization up to 99% can be achieved for randomly distributed quantum dots, and can be close to 100% for some single quantum dots.

Comparison of two quantum dots for bioluminescence resonance energy transfer based on nucleic acid detection

NASA Astrophysics Data System (ADS)

Zhang, Daohong

2017-05-01

The performance of two commercially available quantum dots, quantum dot 605 (Qd605) and quantum dot 625 (Qd625), was tested and compared in the sensing system developed by our group previously. The sandwich format sensing system employed Renilla luciferase (Rluc) and quantum dots (Qds), could report the presence of targets with increasing bioluminescent resonance energy transfer (BRET) signal. The best spacing between the Rluc and Qds probes were 15 nucleotides. Both of Qd605 and Qd625 sensing system could quantify nucleic acid targets through 1-min hybridization from 0.2 picomoles. However, the Qd625 system showed higher BRET signal and better selectivity. Therefore, Qd625 is a better choice in this system compared to Qd605.

Carrier multiplication and charge transport in artificial quantum-dot solids probed by ultrafast photocurrent spectroscopy (Conference Presentation)

NASA Astrophysics Data System (ADS)

Klimov, Victor I.

2017-05-01

Understanding and controlling carrier transport and recombination dynamics in colloidal quantum dot films is key to their application in electronic and optoelectronic devices. Towards this end, we have conducted transient photocurrent measurements to monitor transport through quantum confined band edge states in lead selenide quantum dots films as a function of pump fluence, temperature, electrical bias, and surface treatment. Room temperature dynamics reveal two distinct timescales of intra-dot geminate processes followed by non-geminate inter-dot processes. The non-geminate kinetics is well described by the recombination of holes with photoinjected and pre-existing electrons residing in mid-gap states. We find the mobility of the quantum-confined states shows no temperature dependence down to 6 K, indicating a tunneling mechanism of early time photoconductance. We present evidence of the importance of the exciton fine structure in controlling the low temperature photoconductance, whereby the nanoscale enhanced exchange interaction between electrons and holes in quantum dots introduces a barrier to charge separation. Finally, side-by-side comparison of photocurrent transients using excitation with low- and high-photon energies (1.5 vs. 3.0 eV) reveals clear signatures of carrier multiplication (CM), that is, generation of multiple excitons by single photons. Based on photocurrent measurements of quantum dot solids and optical measurements of solution based samples, we conclude that the CM efficiency is unaffected by strong inter-dot coupling. Therefore, the results of previous numerous spectroscopic CM studies conducted on dilute quantum dot suspensions should, in principle, be reproducible in electronically coupled QD films used in devices.

Multi-million atom electronic structure calculations for quantum dots

NASA Astrophysics Data System (ADS)

Usman, Muhammad

Quantum dots grown by self-assembly process are typically constructed by 50,000 to 5,000,000 structural atoms which confine a small, countable number of extra electrons or holes in a space that is comparable in size to the electron wavelength. Under such conditions quantum dots can be interpreted as artificial atoms with the potential to be custom tailored to new functionality. In the past decade or so, these nanostructures have attracted significant experimental and theoretical attention in the field of nanoscience. The new and tunable optical and electrical properties of these artificial atoms have been proposed in a variety of different fields, for example in communication and computing systems, medical and quantum computing applications. Predictive and quantitative modeling and simulation of these structures can help to narrow down the vast design space to a range that is experimentally affordable and move this part of nanoscience to nano-Technology. Modeling of such quantum dots pose a formidable challenge to theoretical physicists because: (1) Strain originating from the lattice mismatch of the materials penetrates deep inside the buffer surrounding the quantum dots and require large scale (multi-million atom) simulations to correctly capture its effect on the electronic structure, (2) The interface roughness, the alloy randomness, and the atomistic granularity require the calculation of electronic structure at the atomistic scale. Most of the current or past theoretical calculations are based on continuum approach such as effective mass approximation or k.p modeling capturing either no or one of the above mentioned effects, thus missing some of the essential physics. The Objectives of this thesis are: (1) to model and simulate the experimental quantum dot topologies at the atomistic scale; (2) to theoretically explore the essential physics i.e. long range strain, linear and quadratic piezoelectricity, interband optical transition strengths, quantum confined stark shift, coherent coupling of electronic states in a quantum dot molecule etc.; (3) to assess the potential use of the quantum dots in real device implementation and to provide physical insight to the experimentalists. Full three dimensional strain and electronic structure simulations of quantum dot structures containing multi-million atoms are done using NEMO 3-D. Both single and vertically stacked quantum dot structures are analyzed in detail. The results show that the strain and the piezoelectricity significantly impact the electronic structure of these devices. This work shows that the InAs quantum dots when placed in the InGaAs quantum well red shifts the emission wavelength. Such InAs/GaAs-based optical devices can be used for optical-fiber based communication systems at longer wavelengths (1.3um -- 1.5um). Our atomistic simulations of InAs/InGaAs/GaAs quantum dots quantitatively match with the experiment and give the critical insight of the physics involved in these structures. A single quantum dot molecule is studied for coherent quantum coupling of electronic states under the influence of static electric field applied in the growth direction. Such nanostructures can be used in the implementation of quantum information technologies. A close quantitative match with the experimental optical measurements allowed us to get a physical insight into the complex physics of quantum tunnel couplings of electronic states as the device operation switches between atomic and molecular regimes. Another important aspect is to design the quantum dots for a desired isotropic polarization of the optical emissions. Both single and coupled quantum dots are studied for TE/TM ratio engineering. The atomistic study provides a detailed physical analysis of these computationally expensive large nanostructures and serves as a guide for the experimentalists for the design of the polarization independent devices for the optical communication systems.

Optical Spectroscopy Of Charged Quantum Dot Molecules

NASA Astrophysics Data System (ADS)

Scheibner, M.; Bracker, A. S.; Stinaff, E. A.; Doty, M. F.; Gammon, D.; Ponomarev, I. V.; Reinecke, T. L.; Korenev, V. L.

2007-04-01

Coupling between two closely spaced quantum dots is observed by means of photoluminescence spectroscopy. Hole coupling is realized by rational crystal growth and heterostructure design. We identify molecular resonances of different excitonic charge states, including the important case of a doubly charged quantum dot molecule.

Non-blinking quantum dot with a plasmonic nanoshell resonator

NASA Astrophysics Data System (ADS)

Ji, Botao; Giovanelli, Emerson; Habert, Benjamin; Spinicelli, Piernicola; Nasilowski, Michel; Xu, Xiangzhen; Lequeux, Nicolas; Hugonin, Jean-Paul; Marquier, Francois; Greffet, Jean-Jacques; Dubertret, Benoit

2015-02-01

Colloidal semiconductor quantum dots are fluorescent nanocrystals exhibiting exceptional optical properties, but their emission intensity strongly depends on their charging state and local environment. This leads to blinking at the single-particle level or even complete fluorescence quenching, and limits the applications of quantum dots as fluorescent particles. Here, we show that a single quantum dot encapsulated in a silica shell coated with a continuous gold nanoshell provides a system with a stable and Poissonian emission at room temperature that is preserved regardless of drastic changes in the local environment. This novel hybrid quantum dot/silica/gold structure behaves as a plasmonic resonator with a strong Purcell factor, in very good agreement with simulations. The gold nanoshell also acts as a shield that protects the quantum dot fluorescence and enhances its resistance to high-power photoexcitation or high-energy electron beams. This plasmonic fluorescent resonator opens the way to a new family of plasmonic nanoemitters with robust optical properties.

CdS/CdSe co-sensitized SnO2 photoelectrodes for quantum dots sensitized solar cells

NASA Astrophysics Data System (ADS)

Lin, Yibing; Lin, Yu; Meng, Yongming; Tu, Yongguang; Zhang, Xiaolong

2015-07-01

SnO2 nanoparticles were synthesized by hydrothermal method and applied to photo-electrodes of quantum dots-sensitized solar cells (QDSSCs). After sensitizing SnO2 films via CdS quantum dots, CdSe quantum dots was decorated on the surface of CdS/SnO2 photo-electrodes to further improve the power conversion efficiency. CdS and CdSe quantum dots were deposited by successive ionic layer absorption and reaction method (SILAR) and chemical bath deposition method (CBD) respectively. Scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray diffraction (XRD) were used to identify the surface profile and crystal structure of SnO2 photo-electrodes before and after deposited quantum dots. After CdSe co-sensitized process, an overall power conversion efficiency of 1.78% was obtained in CdSe/CdS/SnO2 QDSSC, which showed 66.4% improvement than that of CdS/SnO2 QDSSC.

Two-photon absorption and efficient encapsulation of near-infrared-emitting CdSexTe1-x quantum dots

NASA Astrophysics Data System (ADS)

Szeremeta, Janusz; Lamch, Lukasz; Wawrzynczyk, Dominika; Wilk, Kazimiera A.; Samoc, Marek; Nyk, Marcin

2015-07-01

Hydrophobic CdSexTe1-x quantum dots with near infrared emission in the 700-750 nm range were synthesized by a wet chemistry technique. Their nonlinear optical properties were studied using Z-scan technique with a tunable femtosecond laser system. The peak value of the two-photon absorption cross section was found to be ∼2400 GM at 1400 nm. To demonstrate a possible way of utilizing the CdSexTe1-x quantum dots in aqueous environment we describe here a convenient method of preparation of Brij 58® micellar systems loaded with the quantum dots. The obtained nanoconstructs were characterized using optical spectroscopy, TEM and DLS. The micelles colloidal stability, and the influence of the encapsulation process on the spectroscopic properties of the quantum dots are discussed. In particular, we have observed a 60 nm blue-shift of the emission maxima upon loading quantum dots inside the micelles.

Graphene quantum dots with nitrogen-doped content dependence for highly efficient dual-modality photodynamic antimicrobial therapy and bioimaging.

PubMed

Kuo, Wen-Shuo; Chen, Hua-Han; Chen, Shih-Yao; Chang, Chia-Yuan; Chen, Pei-Chi; Hou, Yung-I; Shao, Yu-Ting; Kao, Hui-Fang; Lilian Hsu, Chih-Li; Chen, Yi-Chun; Chen, Shean-Jen; Wu, Shang-Rung; Wang, Jiu-Yao

2017-03-01

Reactive oxygen species is the main contributor to photodynamic therapy. The results of this study show that a nitrogen-doped graphene quantum dot, serving as a photosensitizer, was capable of generating a higher amount of reactive oxygen species than a nitrogen-free graphene quantum dot in photodynamic therapy when photoexcited for only 3 min of 670 nm laser exposure (0.1 W cm -2 ), indicating highly improved antimicrobial effects. In addition, we found that higher nitrogen-bonding compositions of graphene quantum dots more efficiently performed photodynamic therapy actions than did the lower compositions that underwent identical treatments. Furthermore, the intrinsically emitted luminescence from nitrogen-doped graphene quantum dots and high photostability simultaneously enabled it to act as a promising contrast probe for tracking and localizing bacteria in biomedical imaging. Thus, the dual modality of nitrogen-doped graphene quantum dots presents possibilities for future clinical applications, and in particular multidrug resistant bacteria. Copyright © 2016 Elsevier Ltd. All rights reserved.

Quantum Dot-Based Luminescent Oxygen Channeling Assay for Potential Application in Homogeneous Bioassays.

PubMed

Zhuang, Si-Hui; Guo, Xin-Xin; Wu, Ying-Song; Chen, Zhen-Hua; Chen, Yao; Ren, Zhi-Qi; Liu, Tian-Cai

2016-01-01

The unique photoproperties of quantum dots are promising for potential application in bioassays. In the present study, quantum dots were applied to a luminescent oxygen channeling assay. The reaction system developed in this study was based on interaction of biotin with streptavidin. Carboxyl-modified polystyrene microspheres doped with quantum dots were biotinylated and used as acceptors. Photosensitizer-doped carboxyl-modified polystyrene microspheres were conjugated with streptavidin and used as donors. The results indicated that the singlet oxygen that was released from the donor beads diffused into the acceptor beads. The acceptor beads were then exited via thioxene, and were subsequently fluoresced. To avoid generating false positives, a high concentration (0.01 mg/mL) of quantum dots is required for application in homogeneous immunoassays. Compared to a conventional luminescent oxygen channeling assay, this quantum dots-based technique requires less time, and would be easier to automate and miniaturize because it requires no washing to remove excess labels.

Quantum dot in interacting environments

NASA Astrophysics Data System (ADS)

Rylands, Colin; Andrei, Natan

2018-04-01

A quantum impurity attached to an interacting quantum wire gives rise to an array of new phenomena. Using the Bethe Ansatz we solve exactly models describing two geometries of a quantum dot coupled to an interacting quantum wire: a quantum dot that is (i) side coupled and (ii) embedded in a Luttinger liquid. We find the eigenstates and determine the spectrum through the Bethe Ansatz equations. Using this we derive exact expressions for the ground-state dot occupation. The thermodynamics are then studied using the thermodynamics Bethe Ansatz equations. It is shown that at low energies the dot becomes fully hybridized and acts as a backscattering impurity or tunnel junction depending on the geometry and furthermore that the two geometries are related by changing the sign of the interactions. Although remaining strongly coupled for all values of the interaction in the wire, there exists competition between the tunneling and backscattering leading to a suppression or enhancement of the dot occupation depending on the sign of the bulk interactions.

Enhanced Photon Extraction from a Nanowire Quantum Dot Using a Bottom-Up Photonic Shell

NASA Astrophysics Data System (ADS)

Jeannin, Mathieu; Cremel, Thibault; Häyrynen, Teppo; Gregersen, Niels; Bellet-Amalric, Edith; Nogues, Gilles; Kheng, Kuntheak

2017-11-01

Semiconductor nanowires offer the possibility to grow high-quality quantum-dot heterostructures, and, in particular, CdSe quantum dots inserted in ZnSe nanowires have demonstrated the ability to emit single photons up to room temperature. In this paper, we demonstrate a bottom-up approach to fabricate a photonic fiberlike structure around such nanowire quantum dots by depositing an oxide shell using atomic-layer deposition. Simulations suggest that the intensity collected in our NA =0.6 microscope objective can be increased by a factor 7 with respect to the bare nanowire case. Combining microphotoluminescence, decay time measurements, and numerical simulations, we obtain a fourfold increase in the collected photoluminescence from the quantum dot. We show that this improvement is due to an increase of the quantum-dot emission rate and a redirection of the emitted light. Our ex situ fabrication technique allows a precise and reproducible fabrication on a large scale. Its improved extraction efficiency is compared to state-of-the-art top-down devices.

Selective contacts drive charge extraction in quantum dot solids via asymmetry in carrier transfer kinetics.

PubMed

Mora-Sero, Ivan; Bertoluzzi, Luca; Gonzalez-Pedro, Victoria; Gimenez, Sixto; Fabregat-Santiago, Francisco; Kemp, Kyle W; Sargent, Edward H; Bisquert, Juan

2013-01-01

Colloidal quantum dot solar cells achieve spectrally selective optical absorption in a thin layer of solution-processed, size-effect tuned, nanoparticles. The best devices built to date have relied heavily on drift-based transport due to the action of an electric field in a depletion region that extends throughout the thickness of the quantum dot layer. Here we study for the first time the behaviour of the best-performing class of colloidal quantum dot films in the absence of an electric field, by screening using an electrolyte. We find that the action of selective contacts on photovoltage sign and amplitude can be retained, implying that the contacts operate by kinetic preferences of charge transfer for either electrons or holes. We develop a theoretical model to explain these experimental findings. The work is the first to present a switch in the photovoltage in colloidal quantum dot solar cells by purposefully formed selective contacts, opening the way to new strategies in the engineering of colloidal quantum dot solar cells.

Interplay of morphology, composition, and optical properties of InP-based quantum dots emitting at the 1.55 μ m telecom wavelength

NASA Astrophysics Data System (ADS)

Carmesin, C.; Schowalter, M.; Lorke, M.; Mourad, D.; Grieb, T.; Müller-Caspary, K.; Yacob, M.; Reithmaier, J. P.; Benyoucef, M.; Rosenauer, A.; Jahnke, F.

2017-12-01

Results for the development and detailed analysis of self-organized InAs/InAlGaAs/InP quantum dots suitable for single-photon emission at the 1.55 μ m telecom wavelength are reported. The structural and compositional properties of the system are obtained from high-resolution scanning transmission electron microscopy of individual quantum dots. The system is composed of almost pure InAs quantum dots embedded in quaternary InAlGaAs barrier material, which is lattice matched to the InP substrate. When using the measured results for a representative quantum-dot geometry as well as experimentally reconstructed alloy concentrations, a combination of strain-field and electronic-state calculations is able to reproduce the quantum-dot emission wavelength in agreement with the experimentally determined photoluminescence spectrum. The inhomogeneous broadening of the latter can be related to calculated variations of the emission wavelength for the experimentally deduced In-concentration fluctuations and size variations.

Demonstration of the lack of cytotoxicity of unmodified and folic acid modified graphene oxide quantum dots, and their application to fluorescence lifetime imaging of HaCaT cells.

PubMed

Goreham, Renee V; Schroeder, Kathryn L; Holmes, Amy; Bradley, Siobhan J; Nann, Thomas

2018-01-24

The authors describe the synthesis of water-soluble and fluorescent graphene oxide quantum dots via acid exfoliation of graphite nanoparticles. The resultant graphene oxide quantum dots (GoQDs) were then modified with folic acid. Folic acid receptors are overexpressed in cancer cells and hence can bind to functionalized graphene oxide quantum dots. On excitation at 305 nm, the GoQDs display green fluorescence with a peak wavelength at ~520 nm. The modified GoQDs are non-toxic to macrophage cells even after prolonged exposure and high concentrations. Fluorescence lifetime imaging and multiphoton microscopy was used (in combination) to image HeCaT cells exposed to GoQDs, resulting in a superior method for bioimaging. Graphical abstract Schematic representation of graphene oxide quantum dots, folic acid modified graphene oxide quantum dots (red), and the use of fluorescence lifetime to discriminate against green auto-fluorescence of HeCaT cells.

Effect of a low-temperature-grown GaAs layer on InAs quantum-dot photoluminescence

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kosarev, A. N.; Chaldyshev, V. V., E-mail: chald.gvg@mail.ioffe.ru; Preobrazhenskii, V. V.

2016-11-15

The photoluminescence of InAs semiconductor quantum dots overgrown by GaAs in the low-temperature mode (LT-GaAs) using various spacer layers or without them is studied. Spacer layers are thin GaAs or AlAs layers grown at temperatures normal for molecular-beam epitaxy (MBE). Direct overgrowth leads to photoluminescence disappearance. When using a thin GaAs spacer layer, the photoluminescence from InAs quantum dots is partially recovered; however, its intensity appears lower by two orders of magnitude than in the reference sample in which the quantum-dot array is overgrown at normal temperature. The use of wider-gap AlAs as a spacer-layer material leads to the enhancementmore » of photoluminescence from InAs quantum dots, but it is still more than ten times lower than that of reference-sample emission. A model taking into account carrier generation by light, diffusion and tunneling from quantum dots to the LT-GaAs layer is constructed.« less

Modeling and simulation of InGaN/GaN quantum dots solar cell

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aissat, A., E-mail: sakre23@yahoo.fr; LASICOMLaboratory, Faculty of Sciences, University of Blida 1; Benyettou, F.

2016-07-25

Currently, quantum dots have attracted attention in the field of optoelectronics, and are used to overcome the limits of a conventional solar cell. Here, an In{sub 0.25}Ga{sub 0.75}N/GaN Quantum Dots Solar Cell has been modeled and simulated using Silvaco Atlas. Our results show that the short circuit current increases with the insertion of the InGaN quantum dots inside the intrinsic region of a GaN pin solar cell. In contrary, the open circuit voltage decreases. A relative optimization of the conversion efficiency of 54.77% was achieved comparing a 5-layers In{sub 0.25}Ga{sub 0.75}N/GaN quantum dots with pin solar cell. The conversion efficiencymore » begins to decline beyond 5-layers quantum dots introduced. Indium composition of 10 % improves relatively the efficiency about 42.58% and a temperature of 285 K gives better conversion efficiency of 13.14%.« less

Generation and control of polarization-entangled photons from GaAs island quantum dots by an electric field.

PubMed

Ghali, Mohsen; Ohtani, Keita; Ohno, Yuzo; Ohno, Hideo

2012-02-07

Semiconductor quantum dots are potential sources for generating polarization-entangled photons efficiently. The main prerequisite for such generation based on biexciton-exciton cascaded emission is to control the exciton fine-structure splitting. Among various techniques investigated for this purpose, an electric field is a promising means to facilitate the integration into optoelectronic devices. Here we demonstrate the generation of polarization-entangled photons from single GaAs quantum dots by an electric field. In contrast to previous studies, which were limited to In(Ga)As quantum dots, GaAs island quantum dots formed by a thickness fluctuation were used because they exhibit a larger oscillator strength and emit light with a shorter wavelength. A forward voltage was applied to a Schottky diode to control the fine-structure splitting. We observed a decrease and suppression in the fine-structure splitting of the studied single quantum dot with the field, which enabled us to generate polarization-entangled photons with a high fidelity of 0.72 ± 0.05.

DNA nanosensor based on biocompatible graphene quantum dots and carbon nanotubes.

PubMed

Qian, Zhao Sheng; Shan, Xiao Yue; Chai, Lu Jing; Ma, Juan Juan; Chen, Jian Rong; Feng, Hui

2014-10-15

An ultrasensitive nanosensor based on fluorescence resonance energy transfer (FRET) between biocompatible graphene quantum dots and carbon nanotubes for DNA detection was reported. We take advantage of good biocompatibility and strong fluorescence of graphene quantum dots, base pairing specificity of DNA and unique fluorescence resonance energy transfer between graphene quantum dots and carbon nanotubes to achieve the analysis of low concentrations of DNA. Graphene quantum dots with high quantum yield up to 0.20 were prepared and served as the fluorophore of DNA probe. FRET process between graphene quantum dots-labeled probe and oxidized carbon nanotubes is easily achieved due to their efficient self-assembly through specific π-π interaction. This nanosensor can distinguish complementary and mismatched nucleic acid sequences with high sensitivity and good reproducibility. The detection method based on this nanosensor possesses a broad linear span of up to 133.0 nM and ultralow detection limit of 0.4 nM. The constructed nanosensor is expected to be highly biocompatible because of all its components with excellent biocompatibility. Copyright © 2014 Elsevier B.V. All rights reserved.

GaAs/GaP quantum dots: Ensemble of direct and indirect heterostructures with room temperature optical emission

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dadgostar, S.; Mogilatenko, A.; Masselink, W. T.

2016-03-07

We describe the optical emission and the carrier dynamics of an ensemble of self-assembled GaAs quantum dots embedded in GaP(001). The QD formation is driven by the 3.6% lattice mismatch between GaAs and GaP in the Stranski-Krastanow mode after deposition of more than 1.2 monolayers of GaAs. The quantum dots have an areal density between 6 and 7.6 × 10{sup 10} per cm{sup −2} and multimodal size distribution. The luminescence spectra show two peaks in the range of 1.7 and 2.1 eV. The samples with larger quantum dots have red emission and show less thermal quenching compared with the samples with smaller QDs.more » The large QDs luminescence up to room temperature. We attribute the high energy emission to indirect carrier recombination in the thin quantum wells or small strained quantum dots, whereas the low energy red emission is due to the direct electron-hole recombination in the relaxed quantum dots.« less

Exciton shelves for charge and energy transport in third-generation quantum-dot devices

NASA Astrophysics Data System (ADS)

Goodman, Samuel; Singh, Vivek; Noh, Hyunwoo; Casamada, Josep; Chatterjee, Anushree; Cha, Jennifer; Nagpal, Prashant

2014-03-01

Quantum dots are semiconductor nanocrystallites with size-dependent quantum-confined energy levels. While they have been intensively investigated to utilize hot-carriers for photovoltaic applications, to bridge the mismatch between incident solar photons and finite bandgap of semiconductor photocells, efficient charge or exciton transport in quantum-dot films has proven challenging. Here we show development of new coupled conjugated molecular wires with ``exciton shelves'', or different energy levels, matched with the multiple energy levels of quantum dots. Using single nanoparticle and ensemble device measurements we show successful extraction and transport of both bandedge and high-energy charge carriers, and energy transport of excitons. We demonstrate using measurements of electronic density of states, that careful matching of energy states of quantum-dot with molecular wires is important, and any mismatch can generate midgap states leading to charge recombination and reduced efficiency. Therefore, these exciton-shelves and quantum dots can lead to development of next-generation photovoltaic and photodetection devices using simultaneous transport of bandedge and hot-carriers or energy transport of excitons in these nanostructured solution-processed films.

Hyper-branched CdTe nanostructures based on the self-assembling of quantum dots and their optical properties.

PubMed

Pan, Ling-Yun; Pan, Gen-Cai; Zhang, Yong-Lai; Gao, Bing-Rong; Dai, Zhen-Wen

2013-02-01

As the priority of interconnects and active components in nanoscale optical and electronic devices, three-dimensional hyper-branched nanostructures came into focus of research. Recently, a novel crystallization route, named as "nonclassical crystallization," has been reported for three-dimensional nanostructuring. In this process, Quantum dots are used as building blocks for the construction of the whole hyper-branched structures instead of ions or single-molecules in conventional crystallization. The specialty of these nanostructures is the inheritability of pristine quantum dots' physical integrity because of their polycrystalline structures, such as quantum confinement effect and thus the luminescence. Moreover, since a longer diffusion length could exist in polycrystalline nanostructures due to the dramatically decreased distance between pristine quantum dots, the exciton-exciton interaction would be different with well dispersed quantum dots and single crystal nanostructures. This may be a benefit for electron transport in solar cell application. Therefore, it is very necessary to investigate the exciton-exciton interaction in such kind of polycrystalline nanostructures and their optical properites for solar cell application. In this research, we report a novel CdTe hyper-branched nanostructures based on self-assembly of CdTe quantum dots. Each branch shows polycrystalline with pristine quantum dots as the building units. Both steady state and time-resolved spectroscopy were performed to investigate the properties of carrier transport. Steady state optical properties of pristine quantum dots are well inherited by formed structures. While a suppressed multi-exciton recombination rate was observed. This result supports the percolation of carriers through the branches' network.

Rashba effect in an asymmetric quantum dot in a magnetic field

NASA Astrophysics Data System (ADS)

Bandyopadhyay, S.; Cahay, M.

2002-12-01

We derive an expression for the total spin-splitting energy in an asymmetric quantum dot with ferromagnetic contacts, subjected to a transverse electric field. Such a structure has been shown by one of us to act as a spintronic quantum gate with in-built qubit readers and writers (Phys. Rev. B61, 13813 (2000)). The ferromagnetic contacts result in a magnetic field that causes a Zeeman splitting of the electronic states in the quantum dot. We show that this Zeeman splitting can be finely tuned with a transverse electric field as a result of nonvanishing Rashba spin-orbit coupling in an asymmetric quantum dot. This feature is critical for implementing a quantum gate.

Double quantum dot memristor

NASA Astrophysics Data System (ADS)

Li, Ying; Holloway, Gregory W.; Benjamin, Simon C.; Briggs, G. Andrew D.; Baugh, Jonathan; Mol, Jan A.

2017-08-01

Memristive systems are generalizations of memristors, which are resistors with memory. In this paper, we present a quantum description of quantum dot memristive systems. Using this model we propose and experimentally demonstrate a simple and practical scheme for realizing memristive systems with quantum dots. The approach harnesses a phenomenon that is commonly seen as a bane of nanoelectronics, i.e., switching of a trapped charge in the vicinity of the device. We show that quantum dot memristive systems have hysteresis current-voltage characteristics and quantum jump-induced stochastic behavior. While our experiment requires low temperatures, the same setup could, in principle, be realized with a suitable single-molecule transistor and operated at or near room temperature.

Quantum control and process tomography of a semiconductor quantum dot hybrid qubit.

PubMed

Kim, Dohun; Shi, Zhan; Simmons, C B; Ward, D R; Prance, J R; Koh, Teck Seng; Gamble, John King; Savage, D E; Lagally, M G; Friesen, Mark; Coppersmith, S N; Eriksson, Mark A

2014-07-03

The similarities between gated quantum dots and the transistors in modern microelectronics--in fabrication methods, physical structure and voltage scales for manipulation--have led to great interest in the development of quantum bits (qubits) in semiconductor quantum dots. Although quantum dot spin qubits have demonstrated long coherence times, their manipulation is often slower than desired for important future applications, such as factoring. Furthermore, scalability and manufacturability are enhanced when qubits are as simple as possible. Previous work has increased the speed of spin qubit rotations by making use of integrated micromagnets, dynamic pumping of nuclear spins or the addition of a third quantum dot. Here we demonstrate a qubit that is a hybrid of spin and charge. It is simple, requiring neither nuclear-state preparation nor micromagnets. Unlike previous double-dot qubits, the hybrid qubit enables fast rotations about two axes of the Bloch sphere. We demonstrate full control on the Bloch sphere with π-rotation times of less than 100 picoseconds in two orthogonal directions, which is more than an order of magnitude faster than any other double-dot qubit. The speed arises from the qubit's charge-like characteristics, and its spin-like features result in resistance to decoherence over a wide range of gate voltages. We achieve full process tomography in our electrically controlled semiconductor quantum dot qubit, extracting high fidelities of 85 per cent for X rotations (transitions between qubit states) and 94 per cent for Z rotations (phase accumulation between qubit states).

Short term inhalation toxicity of a liquid aerosol of glutaraldehyde-coated CdS/Cd(OH)2 core shell quantum dots in rats.

PubMed

Ma-Hock, L; Farias, P M A; Hofmann, T; Andrade, A C D S; Silva, J N; Arnaud, T M S; Wohlleben, W; Strauss, V; Treumann, S; Chaves, C R; Gröters, S; Landsiedel, R; van Ravenzwaay, B

2014-02-10

Quantum dots exhibit extraordinary optical and mechanical properties, and the number of their applications is increasing. In order to investigate a possible effect of coating on the inhalation toxicity of previously tested non-coated CdS/Cd(OH)2 quantum dots and translocation of these very small particles from the lungs, rats were exposed to coated quantum dots or CdCl2 aerosol (since Cd(2+) was present as impurity), 6h/d for 5 consecutive days. Cd content was determined in organs and excreta after the end of exposure and three weeks thereafter. Toxicity was determined by examination of broncho-alveolar lavage fluid and microscopic evaluation of the entire respiratory tract. There was no evidence for translocation of particles from the respiratory tract. Evidence of a minimal inflammatory process was observed by examination of broncho-alveolar lavage fluid. Microscopically, minimal to mild epithelial alteration was seen in the larynx. The effects observed with coated quantum dots, non-coated quantum dots and CdCl2 were comparable, indicating that quantum dots elicited no significant effects beyond the toxicity of the Cd(2+) ion itself. Compared to other compounds with larger particle size tested at similarly low concentrations, quantum dots caused much less pronounced toxicological effects. Therefore, the present data show that small particle sizes with corresponding high surfaces are not the only factor triggering the toxic response or translocation. Copyright © 2013 Elsevier Ireland Ltd. All rights reserved.

Adding GaAs Monolayers to InAs Quantum-Dot Lasers on (001) InP

NASA Technical Reports Server (NTRS)

Qiu, Yueming; Chacon, Rebecca; Uhl, David; Yang, Rui

2005-01-01

In a modification of the basic configuration of InAs quantum-dot semiconductor lasers on (001)lnP substrate, a thin layer (typically 1 to 2 monolayer thick) of GaAs is incorporated into the active region. This modification enhances laser performance: In particular, whereas it has been necessary to cool the unmodified devices to temperatures of about 80 K in order to obtain lasing at long wavelengths, the modified devices can lase at wavelengths of about 1.7 microns or more near room temperature. InAs quantum dots self-assemble, as a consequence of the lattice mismatch, during epitaxial deposition of InAs on ln0.53Ga0.47As/lnP. In the unmodified devices, the quantum dots as thus formed are typically nonuniform in size. Strainenergy relaxation in very large quantum dots can lead to poor laser performance, especially at wavelengths near 2 microns, for which large quantum dots are needed. In the modified devices, the thin layers of GaAs added to the active regions constitute potential-energy barriers that electrons can only penetrate by quantum tunneling and thus reduce the hot carrier effects. Also, the insertion of thin GaAs layer is shown to reduce the degree of nonuniformity of sizes of the quantum dots. In the fabrication of a batch of modified InAs quantum-dot lasers, the thin additional layer of GaAs is deposited as an interfacial layer in an InGaAs quantum well on (001) InP substrate. The device as described thus far is sandwiched between InGaAsPy waveguide layers, then further sandwiched between InP cladding layers, then further sandwiched between heavily Zn-doped (p-type) InGaAs contact layer.

Magnetically Defined Qubits on 3D Topological Insulators

NASA Astrophysics Data System (ADS)

Ferreira, Gerson J.; Loss, Daniel

2014-03-01

We explore potentials that break time-reversal symmetry to confine the surface states of 3D topological insulators into quantum wires and quantum dots. A magnetic domain wall on a ferromagnet insulator cap layer provides interfacial states predicted to show the quantum anomalous Hall effect. Here, we show that confinement can also occur at magnetic domain heterostructures, with states extended in the inner domain, as well as interfacial QAHE states at the surrounding domain walls. The proposed geometry allows the isolation of the wire and dot from spurious circumventing surface states. For the quantum dots, we find that highly spin-polarized quantized QAHE states at the dot edge constitute a promising candidate for quantum computing qubits. See [Ferreira and Loss, Phys. Rev. Lett. 111, 106802 (2013)]. We explore potentials that break time-reversal symmetry to confine the surface states of 3D topological insulators into quantum wires and quantum dots. A magnetic domain wall on a ferromagnet insulator cap layer provides interfacial states predicted to show the quantum anomalous Hall effect. Here, we show that confinement can also occur at magnetic domain heterostructures, with states extended in the inner domain, as well as interfacial QAHE states at the surrounding domain walls. The proposed geometry allows the isolation of the wire and dot from spurious circumventing surface states. For the quantum dots, we find that highly spin-polarized quantized QAHE states at the dot edge constitute a promising candidate for quantum computing qubits. See [Ferreira and Loss, Phys. Rev. Lett. 111, 106802 (2013)]. We acknowledge support from the Swiss NSF, NCCR Nanoscience, NCCR QSIT, and the Brazillian Research Support Center Initiative (NAP Q-NANO) from Pró-Reitoria de Pesquisa (PRP/USP).

RKKY interaction in a chirally coupled double quantum dot system

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heine, A. W.; Tutuc, D.; Haug, R. J.

2013-12-04

The competition between the Kondo effect and the Ruderman-Kittel-Kasuya-Yoshida (RKKY) interaction is investigated in a double quantum dots system, coupled via a central open conducting region. A perpendicular magnetic field induces the formation of Landau Levels which in turn give rise to the so-called Kondo chessboard pattern in the transport through the quantum dots. The two quantum dots become therefore chirally coupled via the edge channels formed in the open conducting area. In regions where both quantum dots exhibit Kondo transport the presence of the RKKY exchange interaction is probed by an analysis of the temperature dependence. The thus obtainedmore » Kondo temperature of one dot shows an abrupt increase at the onset of Kondo transport in the other, independent of the magnetic field polarity, i.e. edge state chirality in the central region.« less

Bright Single InAsP Quantum Dots at Telecom Wavelengths in Position-Controlled InP Nanowires: The Role of the Photonic Waveguide

NASA Astrophysics Data System (ADS)

Haffouz, Sofiane; Zeuner, Katharina D.; Dalacu, Dan; Poole, Philip J.; Lapointe, Jean; Poitras, Daniel; Mnaymneh, Khaled; Wu, Xiaohua; Couillard, Martin; Korkusinski, Marek; Schöll, Eva; Jöns, Klaus D.; Zwiller, Valery; Williams, Robin L.

2018-05-01

We report on the site-selected growth of bright single InAsP quantum dots embedded within InP photonic nanowire waveguides emitting at telecom wavelengths. We demonstrate a dramatic dependence of the emission rate on both the emission wavelength and the nanowire diameter. With an appropriately designed waveguide, tailored to the emission wavelength of the dot, an increase in count rate by nearly two orders of magnitude (0.4kcps to 35kcps) is obtained for quantum dots emitting in the telecom O-band. Using emission-wavelength-optimised waveguides, we demonstrate bright, narrow linewidth emission from single InAsP quantum dots with an unprecedented tuning range from 880nm to 1550nm. These results pave the way towards efficient single photon sources at telecom wavelengths using deterministically grown InAsP/InP nanowire quantum dots.

Spin-based quantum computation in multielectron quantum dots

NASA Astrophysics Data System (ADS)

Hu, Xuedong; Das Sarma, S.

2001-10-01

In a quantum computer the hardware and software are intrinsically connected because the quantum Hamiltonian (or more precisely its time development) is the code that runs the computer. We demonstrate this subtle and crucial relationship by considering the example of electron-spin-based solid-state quantum computer in semiconductor quantum dots. We show that multielectron quantum dots with one valence electron in the outermost shell do not behave simply as an effective single-spin system unless special conditions are satisfied. Our work compellingly demonstrates that a delicate synergy between theory and experiment (between software and hardware) is essential for constructing a quantum computer.

Electrical control of single hole spins in nanowire quantum dots.

PubMed

Pribiag, V S; Nadj-Perge, S; Frolov, S M; van den Berg, J W G; van Weperen, I; Plissard, S R; Bakkers, E P A M; Kouwenhoven, L P

2013-03-01

The development of viable quantum computation devices will require the ability to preserve the coherence of quantum bits (qubits). Single electron spins in semiconductor quantum dots are a versatile platform for quantum information processing, but controlling decoherence remains a considerable challenge. Hole spins in III-V semiconductors have unique properties, such as a strong spin-orbit interaction and weak coupling to nuclear spins, and therefore, have the potential for enhanced spin control and longer coherence times. A weaker hyperfine interaction has previously been reported in self-assembled quantum dots using quantum optics techniques, but the development of hole-spin-based electronic devices in conventional III-V heterostructures has been limited by fabrication challenges. Here, we show that gate-tunable hole quantum dots can be formed in InSb nanowires and used to demonstrate Pauli spin blockade and electrical control of single hole spins. The devices are fully tunable between hole and electron quantum dots, which allows the hyperfine interaction strengths, g-factors and spin blockade anisotropies to be compared directly in the two regimes.

Quantum dot quantum cascade infrared photodetector

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Xue-Jiao; Zhai, Shen-Qiang; Zhuo, Ning

2014-04-28

We demonstrate an InAs quantum dot quantum cascade infrared photodetector operating at room temperature with a peak detection wavelength of 4.3 μm. The detector shows sensitive photoresponse for normal-incidence light, which is attributed to an intraband transition of the quantum dots and the following transfer of excited electrons on a cascade of quantum levels. The InAs quantum dots for the infrared absorption were formed by making use of self-assembled quantum dots in the Stranski–Krastanov growth mode and two-step strain-compensation design based on InAs/GaAs/InGaAs/InAlAs heterostructure, while the following extraction quantum stairs formed by LO-phonon energy are based on a strain-compensated InGaAs/InAlAs chirpedmore » superlattice. Johnson noise limited detectivities of 3.64 × 10{sup 11} and 4.83 × 10{sup 6} Jones at zero bias were obtained at 80 K and room temperature, respectively. Due to the low dark current and distinct photoresponse up to room temperature, this device can form high temperature imaging.« less

Optically programmable electron spin memory using semiconductor quantum dots.

PubMed

Kroutvar, Miro; Ducommun, Yann; Heiss, Dominik; Bichler, Max; Schuh, Dieter; Abstreiter, Gerhard; Finley, Jonathan J

2004-11-04

The spin of a single electron subject to a static magnetic field provides a natural two-level system that is suitable for use as a quantum bit, the fundamental logical unit in a quantum computer. Semiconductor quantum dots fabricated by strain driven self-assembly are particularly attractive for the realization of spin quantum bits, as they can be controllably positioned, electronically coupled and embedded into active devices. It has been predicted that the atomic-like electronic structure of such quantum dots suppresses coupling of the spin to the solid-state quantum dot environment, thus protecting the 'spin' quantum information against decoherence. Here we demonstrate a single electron spin memory device in which the electron spin can be programmed by frequency selective optical excitation. We use the device to prepare single electron spins in semiconductor quantum dots with a well defined orientation, and directly measure the intrinsic spin flip time and its dependence on magnetic field. A very long spin lifetime is obtained, with a lower limit of about 20 milliseconds at a magnetic field of 4 tesla and at 1 kelvin.

Inter-dot strain field effect on the optoelectronic properties of realistic InP lateral quantum-dot molecules

DOE Office of Scientific and Technical Information (OSTI.GOV)

Barettin, Daniele, E-mail: Daniele.Barettin@uniroma2.it; Auf der Maur, Matthias; De Angelis, Roberta

2015-03-07

We report on numerical simulations of InP surface lateral quantum-dot molecules on In{sub 0.48}Ga{sub 0.52 }P buffer, using a model strictly derived by experimental results by extrapolation of the molecules shape from atomic force microscopy images. Our study has been inspired by the comparison of a photoluminescence spectrum of a high-density InP surface quantum dot sample with a numerical ensemble average given by a weighted sum of simulated single quantum-dot spectra. A lack of experimental optical response from the smaller dots of the sample is found to be due to strong inter-dot strain fields, which influence the optoelectronic properties of lateralmore » quantum-dot molecules. Continuum electromechanical, k{sup →}·p{sup →} bandstructure, and optical calculations are presented for two different molecules, the first composed of two dots of nearly identical dimensions (homonuclear), the second of two dots with rather different sizes (heteronuclear). We show that in the homonuclear molecule the hydrostatic strain raises a potential barrier for the electrons in the connection zone between the dots, while conversely the holes do not experience any barrier, which considerably increases the coupling. Results for the heteronuclear molecule show instead that its dots do not appear as two separate and distinguishable structures, but as a single large dot, and no optical emission is observed in the range of higher energies where the smaller dot is supposed to emit. We believe that in samples of such a high density the smaller dots result as practically incorporated into bigger molecular structures, an effect strongly enforced by the inter-dot strain fields, and consequently it is not possible to experimentally obtain a separate optical emission from the smaller dots.« less

Inter-dot strain field effect on the optoelectronic properties of realistic InP lateral quantum-dot molecules

NASA Astrophysics Data System (ADS)

Barettin, Daniele; Auf der Maur, Matthias; De Angelis, Roberta; Prosposito, Paolo; Casalboni, Mauro; Pecchia, Alessandro

2015-03-01

We report on numerical simulations of InP surface lateral quantum-dot molecules on In0.48Ga0.52P buffer, using a model strictly derived by experimental results by extrapolation of the molecules shape from atomic force microscopy images. Our study has been inspired by the comparison of a photoluminescence spectrum of a high-density InP surface quantum dot sample with a numerical ensemble average given by a weighted sum of simulated single quantum-dot spectra. A lack of experimental optical response from the smaller dots of the sample is found to be due to strong inter-dot strain fields, which influence the optoelectronic properties of lateral quantum-dot molecules. Continuum electromechanical, k →.p → bandstructure, and optical calculations are presented for two different molecules, the first composed of two dots of nearly identical dimensions (homonuclear), the second of two dots with rather different sizes (heteronuclear). We show that in the homonuclear molecule the hydrostatic strain raises a potential barrier for the electrons in the connection zone between the dots, while conversely the holes do not experience any barrier, which considerably increases the coupling. Results for the heteronuclear molecule show instead that its dots do not appear as two separate and distinguishable structures, but as a single large dot, and no optical emission is observed in the range of higher energies where the smaller dot is supposed to emit. We believe that in samples of such a high density the smaller dots result as practically incorporated into bigger molecular structures, an effect strongly enforced by the inter-dot strain fields, and consequently it is not possible to experimentally obtain a separate optical emission from the smaller dots.

A real-time spectrum acquisition system design based on quantum dots-quantum well detector

NASA Astrophysics Data System (ADS)

Zhang, S. H.; Guo, F. M.

2016-01-01

In this paper, we studied the structure characteristics of quantum dots-quantum well photodetector with response wavelength range from 400 nm to 1000 nm. It has the characteristics of high sensitivity, low dark current and the high conductance gain. According to the properties of the quantum dots-quantum well photodetectors, we designed a new type of capacitive transimpedence amplifier (CTIA) readout circuit structure with the advantages of adjustable gain, wide bandwidth and high driving ability. We have implemented the chip packaging between CTIA-CDS structure readout circuit and quantum dots detector and tested the readout response characteristics. According to the timing signals requirements of our readout circuit, we designed a real-time spectral data acquisition system based on FPGA and ARM. Parallel processing mode of programmable devices makes the system has high sensitivity and high transmission rate. In addition, we realized blind pixel compensation and smoothing filter algorithm processing to the real time spectrum data by using C++. Through the fluorescence spectrum measurement of carbon quantum dots and the signal acquisition system and computer software system to realize the collection of the spectrum signal processing and analysis, we verified the excellent characteristics of detector. It meets the design requirements of quantum dot spectrum acquisition system with the characteristics of short integration time, real-time and portability.

Investigation of Quantum Dot Lasers

DTIC Science & Technology

2004-08-09

Accomplishments: • Introduction Since the first demonstration of room-temperature operation of self-assembled quantum-dot (QD) lasers about a...regions (JGaAs), wetting layer (JWL), and Auger recombination in the dots ( JAug ). for the present 1.3µm dots, the temperature invariant measured

Late Quaternary to Holocene Geology, Geomorphology and Glacial History of Dawson Creek and Surrounding area, Northeast British Columbia, Canada

NASA Astrophysics Data System (ADS)

Henry, Edward Trowbridge

Semiconductor quantum dots in silicon demonstrate exceptionally long spin lifetimes as qubits and are therefore promising candidates for quantum information processing. However, control and readout techniques for these devices have thus far employed low frequency electrons, in contrast to high speed temperature readout techniques used in other qubit architectures, and coupling between multiple quantum dot qubits has not been satisfactorily addressed. This dissertation presents the design and characterization of a semiconductor charge qubit based on double quantum dot in silicon with an integrated microwave resonator for control and readout. The 6 GHz resonator is designed to achieve strong coupling with the quantum dot qubit, allowing the use of circuit QED control and readout techniques which have not previously been applicable to semiconductor qubits. To achieve this coupling, this document demonstrates successful operation of a novel silicon double quantum dot design with a single active metallic layer and a coplanar stripline resonator with a bias tee for dc excitation. Experiments presented here demonstrate quantum localization and measurement of both electrons on the quantum dot and photons in the resonator. Further, it is shown that the resonator-qubit coupling in these devices is sufficient to reach the strong coupling regime of circuit QED. The details of a measurement setup capable of performing simultaneous low noise measurements of the resonator and quantum dot structure are also presented here. The ultimate aim of this research is to integrate the long coherence times observed in electron spins in silicon with the sophisticated readout architectures available in circuit QED based quantum information systems. This would allow superconducting qubits to be coupled directly to semiconductor qubits to create hybrid quantum systems with separate quantum memory and processing components.

Temperature independent infrared responsivity of a quantum dot quantum cascade photodetector

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Feng-Jiao; Zhuo, Ning; Liu, Shu-Man, E-mail: liusm@semi.ac.cn

2016-06-20

We demonstrate a quantum dot quantum cascade photodetector with a hybrid active region of InAs quantum dots and an InGaAs quantum well, which exhibited a temperature independent response at 4.5 μm. The normal incident responsivity reached 10.3 mA/W at 120 K and maintained a value of 9 mA/W up to 260 K. It exhibited a specific detectivity above 10{sup 11} cm Hz{sup 1/2} W{sup −1} at 77 K, which remained at 10{sup 8} cm Hz{sup 1/2} W{sup −1} at 260 K. We ascribe the device's good thermal stability of infrared response to the three-dimensional quantum confinement of the InAs quantum dots incorporated in the active region.

Density of Trap States and Auger-mediated Electron Trapping in CdTe Quantum-Dot Solids.

PubMed

Boehme, Simon C; Azpiroz, Jon Mikel; Aulin, Yaroslav V; Grozema, Ferdinand C; Vanmaekelbergh, Daniël; Siebbeles, Laurens D A; Infante, Ivan; Houtepen, Arjan J

2015-05-13

Charge trapping is an ubiquitous process in colloidal quantum-dot solids and a major limitation to the efficiency of quantum dot based devices such as solar cells, LEDs, and thermoelectrics. Although empirical approaches led to a reduction of trapping and thereby efficiency enhancements, the exact chemical nature of the trapping mechanism remains largely unidentified. In this study, we determine the density of trap states in CdTe quantum-dot solids both experimentally, using a combination of electrochemical control of the Fermi level with ultrafast transient absorption and time-resolved photoluminescence spectroscopy, and theoretically, via density functional theory calculations. We find a high density of very efficient electron traps centered ∼0.42 eV above the valence band. Electrochemical filling of these traps increases the electron lifetime and the photoluminescence quantum yield by more than an order of magnitude. The trapping rate constant for holes is an order of magnitude lower that for electrons. These observations can be explained by Auger-mediated electron trapping. From density functional theory calculations we infer that the traps are formed by dicoordinated Te atoms at the quantum dot surface. The combination of our unique experimental determination of the density of trap states with the theoretical modeling of the quantum dot surface allows us to identify the trapping mechanism and chemical reaction at play during charge trapping in these quantum dots.

A comparison between semi-spheroid- and dome-shaped quantum dots coupled to wetting layer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shahzadeh, Mohammadreza; Sabaeian, Mohammad, E-mail: Sabaeian@scu.ac.ir

2014-06-15

During the epitaxial growth method, self-assembled semi-spheroid-shaped quantum dots (QDs) are formed on the wetting layer (WL). However for sake of simplicity, researchers sometimes assume semi-spheroid-shaped QDs to be dome-shaped (hemisphere). In this work, a detailed and comprehensive study on the difference between electronic and transition properties of dome- and semi-spheroid-shaped quantum dots is presented. We will explain why the P-to-S intersubband transition behaves the way it does. The calculated results for intersubband P-to-S transition properties of quantum dots show two different trends for dome-shaped and semi-spheroid-shaped quantum dots. The results are interpreted using the probability of finding electron insidemore » the dome/spheroid region, with emphasis on the effects of wetting layer. It is shown that dome-shaped and semi-spheroid-shaped quantum dots feature different electronic and transition properties, arising from the difference in lateral dimensions between dome- and semi-spheroid-shaped QDs. Moreover, an analogy is presented between the bound S-states in the quantum dots and a simple 3D quantum mechanical particle in a box, and effective sizes are calculated. The results of this work will benefit researchers to present more realistic models of coupled QD/WL systems and explain their properties more precisely.« less

Growth and optical characteristics of InAs quantum dot structures with tunnel injection quantum wells for 1.55 μ m high-speed lasers

NASA Astrophysics Data System (ADS)

Bauer, Sven; Sichkovskyi, Vitalii; Reithmaier, Johann Peter

2018-06-01

InP based lattice matched tunnel injection structures consisting of a InGaAs quantum well, InAlGaAs barrier and InAs quantum dots designed to emit at 1.55 μ m were grown by molecular beam epitaxy and investigated by photoluminescence spectroscopy and atomic force microscopy. The strong influence of quantum well and barrier thicknesses on the samples emission properties at low and room temperatures was investigated. The phenomenon of a decreased photoluminescence linewidth of tunnel injection structures compared to a reference InAs quantum dots sample could be explained by the selection of the emitting dots through the tunneling process. Morphological investigations have not revealed any effect of the injector well on the dot formation and their size distribution. The optimum TI structure design could be defined.

Gate-controlled electromechanical backaction induced by a quantum dot

NASA Astrophysics Data System (ADS)

Okazaki, Yuma; Mahboob, Imran; Onomitsu, Koji; Sasaki, Satoshi; Yamaguchi, Hiroshi

2016-04-01

Semiconductor-based quantum structures integrated into mechanical resonators have emerged as a unique platform for generating entanglement between macroscopic phononic and mesocopic electronic degrees of freedom. A key challenge to realizing this is the ability to create and control the coupling between two vastly dissimilar systems. Here, such coupling is demonstrated in a hybrid device composed of a gate-defined quantum dot integrated into a piezoelectricity-based mechanical resonator enabling milli-Kelvin phonon states to be detected via charge fluctuations in the quantum dot. Conversely, the single electron transport in the quantum dot can induce a backaction onto the mechanics where appropriate bias of the quantum dot can enable damping and even current-driven amplification of the mechanical motion. Such electron transport induced control of the mechanical resonator dynamics paves the way towards a new class of hybrid semiconductor devices including a current injected phonon laser and an on-demand single phonon emitter.

Room-temperature lasing in a single nanowire with quantum dots

NASA Astrophysics Data System (ADS)

Tatebayashi, Jun; Kako, Satoshi; Ho, Jinfa; Ota, Yasutomo; Iwamoto, Satoshi; Arakawa, Yasuhiko

2015-08-01

Semiconductor nanowire lasers are promising as ultrasmall, highly efficient coherent light emitters in the fields of nanophotonics, nano-optics and nanobiotechnology. Although there have been several demonstrations of nanowire lasers using homogeneous bulk gain materials or multi-quantum-wells/disks, it is crucial to incorporate lower-dimensional quantum nanostructures into the nanowire to achieve superior device performance in relation to threshold current, differential gain, modulation bandwidth and temperature sensitivity. The quantum dot is a useful and essential nanostructure that can meet these requirements. However, difficulties in forming stacks of quantum dots in a single nanowire hamper the realization of lasing operation. Here, we demonstrate room-temperature lasing of a single nanowire containing 50 quantum dots by properly designing the nanowire cavity and tailoring the emission energy of each dot to enhance the optical gain. Our demonstration paves the way toward ultrasmall lasers with extremely low power consumption for integrated photonic systems.

CdSe quantum dot internalization by Bacillus subtilis and Escherichia coli

NASA Technical Reports Server (NTRS)

Kloepfer, Jeremiah A.; Mielke, Randall E.; Nadeau, Jay L.

2004-01-01

Biological labeling has been demonstrated with CdSe quantum dots in a variety of animal cells, but bacteria are harder to label because of their cell walls. We discuss the challenges of using minimally coated, bare CdSe quantum dots as luminescent internal labels for bacteria.

The diamagnetic susceptibility of a donor in a semiconductor core shell quantum dot

NASA Astrophysics Data System (ADS)

Sudharshan, M. S.; Subhash, P.; Shaik, Nagoor Babu; Kalpana, P.; Jayakumar, K.; Reuben, A. Merwyn Jasper D.

2015-06-01

The effect of Aluminium concentration, shell thickness and size of the core shell Quantum Dot on the Diamagnetic Susceptibility of a donor in the Core Shell Quantum Dot is calculated in the effective mass approximation using the variational method. The results are presented and discussed.

Morphological evolution of Ge/Si(001) quantum dot rings formed at the rim of wet-etched pits.

PubMed

Grydlik, Martyna; Brehm, Moritz; Schäffler, Friedrich

2012-10-30

We demonstrate the formation of Ge quantum dots in ring-like arrangements around predefined {111}-faceted pits in the Si(001) substrate. We report on the complex morphological evolution of the single quantum dots contributing to the rings by means of atomic force microscopy and demonstrate that by careful adjustment of the epitaxial growth parameters, such rings containing densely squeezed islands can be grown with large spatial distances of up to 5 μm without additional nucleation of randomly distributed quantum dots between the rings.

Multiphoton microscopy of transdermal quantum dot delivery using two photon polymerization-fabricated polymer microneedles

PubMed Central

Gittard, Shaun D; Miller, Philip R; Boehm, Ryan D; Ovsianikov, Aleksandr; Chichkov, Boris N; Heiser, Jeremy; Gordon, John; Monteiro-Riviere, Nancy A; Narayan, Roger J

2010-01-01

Due to their ability to serve as fluorophores and drug delivery vehicles, quantum dots are a powerful tool for theranostics-based clinical applications. In this study, microneedle devices for transdermal drug delivery were fabricated by means of two-photon polymerization of an acrylate-based polymer. We examined proliferation of cells on this polymer using neonatal human epidermal keratinocytes and human dermal fibroblasts. The microneedle device was used to inject quantum dots into porcine skin; imaging of the quantum dots was performed using multiphoton microscopy. PMID:21413181

Synthesis, characterization and cells and tissues imaging of carbon quantum dots

NASA Astrophysics Data System (ADS)

Wang, Jing; Li, Qilong; Zhou, JingE.; Wang, Yiting; Yu, Lei; Peng, Hui; Zhu, Jianzhong

2017-10-01

Compare to other quantum dots, carbon quantum dots have its own incomparable advantages, such as low cell toxicity, favorable biocompatibility, cheap production cost, mild reaction conditions, easy to large-scale synthesis and functionalization. In this thesis, we took citric acid monohydrate and diethylene glycol bis (3-aMinopropyl) ether as materials, used decomposition method to acquire carbon quantum dots (CQDs) which can emission blue fluorescence under ultraviolet excitation. In the aspect of application, we achieved the biological imaging of CQDs in vivo and in vitro.

A fabrication guide for planar silicon quantum dot heterostructures

NASA Astrophysics Data System (ADS)

Spruijtenburg, Paul C.; Amitonov, Sergey V.; van der Wiel, Wilfred G.; Zwanenburg, Floris A.

2018-04-01

We describe important considerations to create top-down fabricated planar quantum dots in silicon, often not discussed in detail in literature. The subtle interplay between intrinsic material properties, interfaces and fabrication processes plays a crucial role in the formation of electrostatically defined quantum dots. Processes such as oxidation, physical vapor deposition and atomic-layer deposition must be tailored in order to prevent unwanted side effects such as defects, disorder and dewetting. In two directly related manuscripts written in parallel we use techniques described in this work to create depletion-mode quantum dots in intrinsic silicon, and low-disorder silicon quantum dots defined with palladium gates. While we discuss three different planar gate structures, the general principles also apply to 0D and 1D systems, such as self-assembled islands and nanowires.

Specific features of electroluminescence in heterostructures with InSb quantum dots in an InAs matrix

DOE Office of Scientific and Technical Information (OSTI.GOV)

Parkhomenko, Ya. A.; Ivanov, E. V.; Moiseev, K. D., E-mail: mkd@iropt2.ioffe.rssi.ru

2013-11-15

The electrical and electroluminescence properties of a single narrow-gap heterostructure based on a p-n junction in indium arsenide, containing a single layer of InSb quantum dots in the InAs matrix, are studied. The presence of quantum dots has a significant effect on the shape of the reverse branch of the current-voltage characteristic of the heterostructure. Under reverse bias, the room-temperature electroluminescence spectra of the heterostructure with quantum dots, in addition to a negative-luminescence band with a maximum at the wavelength {lambda} = 3.5 {mu}m, contained a positive-luminescence emission band at 3.8 {mu}m, caused by radiative transitions involving localized states ofmore » quantum dots at the type-II InSb/InAs heterointerface.« less

Quantum dots grown in the InSb/GaSb system by liquid-phase epitaxy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Parkhomenko, Ya. A.; Dement’ev, P. A.; Moiseev, K. D., E-mail: mkd@iropt2.ioffe.rssi.ru

2016-07-15

The first results of the liquid-phase epitaxial growth of quantum dots in the InSb/GaSb system and atomic-force microscopy data on the structural characteristics of the quantum dots are reported. It is shown that the surface density, shape, and size of nanoislands depend on the deposition temperature and the chemical properties of the matrix surface. Arrays of InSb quantum dots on GaSb (001) substrates are produced in the temperature range T = 450–465°C. The average dimensions of the quantum dots correspond to a height of h = 3 nm and a base dimension of D = 30 nm; the surface densitymore » is 3 × 10{sup 9} cm{sup –2}.« less

Resonant electronic excitation energy transfer by Dexter mechanism in the quantum dot system

NASA Astrophysics Data System (ADS)

Samosvat, D. M.; Chikalova-Luzina, O. P.; Vyatkin, V. M.; Zegrya, G. G.

2016-11-01

In present work the energy transfer between quantum dots by the exchange (Dexter) mechanism is analysed. The interdot Coulomb interaction is taken into consideration. It is assumed that the quantum dot-donor and the quantum dot-acceptor are made from the same compound A3B5 and embedded in the matrix of other material creating potential barriers for electron and holes. The dependences of the energy transfer rate on the quantum-dot system parameters are found using the Kane model that provides the most adequate description spectra of semiconductors A3B5. Numerical calculations show that the rate of the energy transfer by Dexter mechanism is comparable to the rate of the energy transfer by electrostatic mechanism at the distances approaching to the contact ones.

Quantum Dots in the Therapy: Current Trends and Perspectives.

PubMed

Pohanka, Miroslav

2017-01-01

Quantum dots are an emerging nanomaterial with broad use in technical disciplines; however, their application in the field of biomedicine becomes also relevant and significant possibilities have appeared since the discovery in 1980s. The current review is focused on the therapeutic applications of quantum dots which become an emerging use of the particles. They are introduced as potent carriers of drugs and as a material well suited for the diagnosis of disparate pathologies like visualization of cancer cells or pathogenic microorganisms. Quantum dots toxicity and modifications for the toxicity reduction are discussed here as well. Survey of actual papers and patents in the field of quantum dots use in the biomedicine is provided. Copyright© Bentham Science Publishers; For any queries, please email at epub@benthamscience.org.

Berry phase jumps and giant nonreciprocity in Dirac quantum dots

NASA Astrophysics Data System (ADS)

Rodriguez-Nieva, Joaquin F.; Levitov, Leonid S.

2016-12-01

We predict that a strong nonreciprocity in the resonance spectra of Dirac quantum dots can be induced by the Berry phase. The nonreciprocity arises in relatively weak magnetic fields and is manifest in anomalously large field-induced splittings of quantum dot resonances which are degenerate at B =0 due to time-reversal symmetry. This exotic behavior, which is governed by field-induced jumps in the Berry phase of confined electronic states, is unique to quantum dots in Dirac materials and is absent in conventional quantum dots. The effect is strong for gapless Dirac particles and can overwhelm the B -induced orbital and Zeeman splittings. A finite Dirac mass suppresses the effect. The nonreciprocity, predicted for generic two-dimensional Dirac materials, is accessible through Faraday and Kerr optical rotation measurements and scanning tunneling spectroscopy.

Resonance fluorescence revival in a voltage-controlled semiconductor quantum dot

NASA Astrophysics Data System (ADS)

Reigue, Antoine; Lemaître, Aristide; Gomez Carbonell, Carmen; Ulysse, Christian; Merghem, Kamel; Guilet, Stéphane; Hostein, Richard; Voliotis, Valia

2018-02-01

We demonstrate systematic resonance fluorescence recovery with near-unity emission efficiency in single quantum dots embedded in a charge-tunable device in a wave-guiding geometry. The quantum dot charge state is controlled by a gate voltage, through carrier tunneling from a close-lying Fermi sea, stabilizing the resonantly photocreated electron-hole pair. The electric field cancels out the charging/discharging mechanisms from nearby traps toward the quantum dots, responsible for the usually observed inhibition of the resonant fluorescence. Fourier transform spectroscopy as a function of the applied voltage shows a strong increase in the coherence time though not reaching the radiative limit. These charge controlled quantum dots can act as quasi-perfect deterministic single-photon emitters, with one laser pulse converted into one emitted single photon.

Compact and highly stable quantum dots through optimized aqueous phase transfer

NASA Astrophysics Data System (ADS)

Tamang, Sudarsan; Beaune, Grégory; Poillot, Cathy; De Waard, Michel; Texier-Nogues, Isabelle; Reiss, Peter

2011-03-01

A large number of different approaches for the aqueous phase transfer of quantum dots have been proposed. Surface ligand exchange with small hydrophilic thiols, such as L-cysteine, yields the lowest particle hydrodynamic diameter. However, cysteine is prone to dimer formation, which limits colloidal stability. We demonstrate that precise pH control during aqueous phase transfer dramatically increases the colloidal stability of InP/ZnS quantum dots. Various bifunctional thiols have been applied. The formation of disulfides, strongly diminishing the fluorescence QY has been prevented through addition of appropriate reducing agents. Bright InP/ZnS quantum dots with a hydrodynamic diameter <10 nm and long-term stability have been obtained. Finally we present in vitro studies of the quantum dots functionalized with the cell-penetrating peptide maurocalcine.

Time-resolved photoluminescence measurements of InP/ZnS quantum dots

NASA Astrophysics Data System (ADS)

Thi Thuy, Pham; Thi Dieu Thuy, Ung; Chi, Tran Thi Kim; Phuong, Le Quang; Liem, Nguyen Quang; Li, Liang; Reiss, Peter

2009-09-01

This paper reports the results on the time-resolved photoluminescence study of InP/ZnS core/shell quantum dots. The ZnS shell played a decisive role to passivate imperfections on the surface of InP quantum dots, consequently giving rise to a strong enhancement of the photoluminescence from the InP core. Under appropriate excitation conditions, not only the emission from the InP core but also that from the ZnS shell was observed. The emission peak in InP core quantum dots varied as a function of quantum dots size, ranging in the 600 - 700 nm region; while the ZnS shell showed emission in the blue region around 470 nm, which is interpreted as resulting from defects in ZnS.

Green biosynthesis of biocompatible CdSe quantum dots in living Escherichia coli cells

NASA Astrophysics Data System (ADS)

Yan, Zhengyu; Qian, Jing; Gu, Yueqing; Su, Yilong; Ai, Xiaoxia; Wu, Shengmei

2014-03-01

A green and efficient biosynthesis method to prepare fluorescence-tunable biocompatible cadmium selenide quantum dots using Escherichia coli cells as biological matrix was proposed. Decisive factors in biosynthesis of cadmium selenide quantum dots in a designed route in Escherichia coli cells were elaborately investigated, including the influence of the biological matrix growth stage, the working concentration of inorganic reactants, and the co-incubation duration of inorganic metals to biomatrix. Ultraviolet-visible, photoluminescence, and inverted fluorescence microscope analysis confirmed the unique optical properties of the biosynthesized cadmium selenide quantum dots. The size distribution of the nanocrystals extracted from cells and the location of nanocrystals foci in vivo were also detected seriously by transmission electron microscopy. A surface protein capping layer outside the nanocrystals was confirmed by Fourier transform infrared spectroscopy measurements, which were supposed to contribute to reducing cytotoxicity and maintain a high viability of cells when incubating with quantum dots at concentrations as high as 2 μM. Cell morphology observation indicated an effective labeling of living cells by the biosynthesized quantum dots after a 48 h co-incubation. The present work demonstrated an economical and environmentally friendly approach to fabricating highly fluorescent quantum dots which were expected to be an excellent fluorescent dye for broad bio-imaging and labeling.

Quantitative characterization of nanoparticle agglomeration within biological media

NASA Astrophysics Data System (ADS)

Hondow, Nicole; Brydson, Rik; Wang, Peiyi; Holton, Mark D.; Brown, M. Rowan; Rees, Paul; Summers, Huw D.; Brown, Andy

2012-07-01

Quantitative analysis of nanoparticle dispersion state within biological media is essential to understanding cellular uptake and the roles of diffusion, sedimentation, and endocytosis in determining nanoparticle dose. The dispersion of polymer-coated CdTe/ZnS quantum dots in water and cell growth medium with and without fetal bovine serum was analyzed by transmission electron microscopy (TEM) and dynamic light scattering (DLS) techniques. Characterization by TEM of samples prepared by plunge freezing the blotted solutions into liquid ethane was sensitive to the dispersion state of the quantum dots and enabled measurement of agglomerate size distributions even in the presence of serum proteins where DLS failed. In addition, TEM showed a reduced packing fraction of quantum dots per agglomerate when dispersed in biological media and serum compared to just water, highlighting the effect of interactions between the media, serum proteins, and the quantum dots. The identification of a heterogeneous distribution of quantum dots and quantum dot agglomerates in cell growth medium and serum by TEM will enable correlation with the previously reported optical metrology of in vitro cellular uptake of this quantum dot dispersion. In this paper, we present a comparative study of TEM and DLS and show that plunge-freeze TEM provides a robust assessment of nanoparticle agglomeration state.

Folic acid-CdTe quantum dot conjugates and their applications for cancer cell targeting

DOE Office of Scientific and Technical Information (OSTI.GOV)

Suriamoorthy, Preethi; Zhang, Xing; Hao, Guiyang

2010-12-01

In this study, we report the preparation,luminescence, and targeting properties of folic acid- CdTe quantum dot conjugates. Water-soluble CdTe quantum dots were synthesized and conjugated with folic acid using 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide-N-hydroxysuccinimide chemistry. The in-fluence of folic acid on the luminescence properties of CdTe quantum dots was investigated, and no energy transfer between them was observed. To investigate the efficiency of folic acid-CdTe nanoconjugates for tumor targeting, pure CdTe quantum dots and folic acid-coated CdTe quantum dots were incubated with human naso- pharyngeal epidermal carcinoma cell line with positive expressing folic acid receptors (KB cells) and lung cancer cells without expressionmore » of folic acid receptors (A549 cells). For the cancer cells with positive folate receptors (KB cells), the uptake for CdTe quantum dots is very low, but for folic acid-CdTe nanoconjugates, the uptake is very high. For the lung cancer cells without folate receptors (A549 cells), the uptake for folic acid- CdTe nanoconjugates is also very low. The results indicate that folic acid is an effective targeting molecule for tumor cells with overexpressed folate receptors.« less

Functionalization of Cadmium Selenide Quantum Dots with Poly(ethylene glycol): Ligand Exchange, Surface Coverage, and Dispersion Stability.

PubMed

Wenger, Whitney Nowak; Bates, Frank S; Aydil, Eray S

2017-08-22

Semiconductor quantum dots synthesized using rapid mixing of precursors by injection into a hot solution of solvents and surfactants have surface ligands that sterically stabilize the dispersions in nonpolar solvents. Often, these ligands are exchanged to disperse the quantum dots in polar solvents, but quantitative studies of quantum dot surfaces before and after ligand exchange are scarce. We studied exchanging trioctylphosphine (TOP) and trioctylphosphine oxide (TOPO) ligands on as-synthesized CdSe quantum dots dispersed in hexane with a 2000 g/mol thiolated poly(ethylene glycol) (PEG) polymer. Using infrared spectroscopy we quantify the absolute surface concentration of TOP/TOPO and PEG ligands per unit area before and after ligand exchange. While 50-85% of the TOP/TOPO ligands are removed upon ligand exchange, only a few are replaced with PEG. Surprisingly, the remaining TOP/TOPO ligands outnumber the PEG ligands, but these few PEG ligands are sufficient to disperse the quantum dots in polar solvents such as chloroform, tetrahydrofuran, and water. Moreover, as-synthesized quantum dots once easily dispersed in hexane are no longer dispersible in nonpolar solvents after ligand exchange. A subtle coverage-dependent balance between attractive PEG-solvent interactions and repulsive TOP/TOPO-solvent interactions determines the dispersion stability.

Magnetic field effect on the energy levels of an exciton in a GaAs quantum dot: Application for excitonic lasers.

PubMed

Jahan, K Luhluh; Boda, A; Shankar, I V; Raju, Ch Narasimha; Chatterjee, Ashok

2018-03-22

The problem of an exciton trapped in a Gaussian quantum dot (QD) of GaAs is studied in both two and three dimensions in the presence of an external magnetic field using the Ritz variational method, the 1/N expansion method and the shifted 1/N expansion method. The ground state energy and the binding energy of the exciton are obtained as a function of the quantum dot size, confinement strength and the magnetic field and compared with those available in the literature. While the variational method gives the upper bound to the ground state energy, the 1/N expansion method gives the lower bound. The results obtained from the shifted 1/N expansion method are shown to match very well with those obtained from the exact diagonalization technique. The variation of the exciton size and the oscillator strength of the exciton are also studied as a function of the size of the quantum dot. The excited states of the exciton are computed using the shifted 1/N expansion method and it is suggested that a given number of stable excitonic bound states can be realized in a quantum dot by tuning the quantum dot parameters. This can open up the possibility of having quantum dot lasers using excitonic states.

Cavity-Mediated Coherent Coupling between Distant Quantum Dots

NASA Astrophysics Data System (ADS)

Nicolí, Giorgio; Ferguson, Michael Sven; Rössler, Clemens; Wolfertz, Alexander; Blatter, Gianni; Ihn, Thomas; Ensslin, Klaus; Reichl, Christian; Wegscheider, Werner; Zilberberg, Oded

2018-06-01

Scalable architectures for quantum information technologies require one to selectively couple long-distance qubits while suppressing environmental noise and cross talk. In semiconductor materials, the coherent coupling of a single spin on a quantum dot to a cavity hosting fermionic modes offers a new solution to this technological challenge. Here, we demonstrate coherent coupling between two spatially separated quantum dots using an electronic cavity design that takes advantage of whispering-gallery modes in a two-dimensional electron gas. The cavity-mediated, long-distance coupling effectively minimizes undesirable direct cross talk between the dots and defines a scalable architecture for all-electronic semiconductor-based quantum information processing.

Physics of lateral triple quantum-dot molecules with controlled electron numbers.

PubMed

Hsieh, Chang-Yu; Shim, Yun-Pil; Korkusinski, Marek; Hawrylak, Pawel

2012-11-01

We review the recent progress in theory and experiments with lateral triple quantum dots with controlled electron numbers down to one electron in each dot. The theory covers electronic and spin properties as a function of topology, number of electrons, gate voltage and external magnetic field. The orbital Hund's rules and Nagaoka ferromagnetism, magnetic frustration and chirality, interplay of quantum interference and electron-electron interactions and geometrical phases are described and related to charging and transport spectroscopy. Fabrication techniques and recent experiments are covered, as well as potential applications of triple quantum-dot molecule in coherent control, spin manipulation and quantum computation.

Temperature dependence of spectral linewidth of InAs/InP quantum dot distributed feedback lasers

NASA Astrophysics Data System (ADS)

Duan, J.; Huang, H.; Schires, K.; Poole, P. J.; Wang, C.; Grillot, F.

2018-02-01

In this paper, we investigate the temperature dependence of spectral linewidth of InAs/InP quantum dot distributed feedback lasers. In comparison with their quantum well counterparts, results show that quantum dot lasers have spectral linewidths rather insensitive to the temperature with minimum values below 200 kHz in the range of 283K to 303K. The experimental results are also well confirmed by numerical simulations. Overall, this work shows that quantum dot lasers are excellent candidates for various applications such as coherent communication systems, high-resolution spectroscopy, high purity photonic microwave generation and on-chip atomic clocks.

Suppressed Kondo effect and Kosterlitz-Thouless-type phase transition induced by level difference in a triple dot device

NASA Astrophysics Data System (ADS)

Xiong, Yong-Chen; Huang, Hai-Ming; Zhao, Wen-Lei; Laref, Amel

2017-10-01

Quantum dot system provides an ideal platform for quantum information processing, within which to demonstrate the quantum states is one of the most important issue for quantum simulation and quantum computation. In this paper, we report a peculiar electron state in a parallel triple dot device where the Ruderman-Kittel-Kasuya-Yosida interaction is invalid when the level differences of the dots sweep into appropriate regime. This extraordinary tendency then results in an antiferromagnetic spin coupling between two of the dots and may lead to zero or full conductance, relying deeply on the relation of the two level spacings. e.g. when the level differences are kept equal, the Kondo effect is totally suppressed although the dots are triply occupied, since in this case a local inter-dot transport loop is found to play an important role in the transmission coefficient. By contrast, when the differences are retained symmetric, the Kondo peak reaches nearly to its unitary limit, owing to that the inter-dot transport process is significantly suppressed. To approach these problems, voltage controllable quantum phase transitions of Kosterlitz-Thouless type and first order are shown, and possible pictures related to the many-body effect and the effective Kondo model are given.

Direct photonic coupling of a semiconductor quantum dot and a trapped ion.

PubMed

Meyer, H M; Stockill, R; Steiner, M; Le Gall, C; Matthiesen, C; Clarke, E; Ludwig, A; Reichel, J; Atatüre, M; Köhl, M

2015-03-27

Coupling individual quantum systems lies at the heart of building scalable quantum networks. Here, we report the first direct photonic coupling between a semiconductor quantum dot and a trapped ion and we demonstrate that single photons generated by a quantum dot controllably change the internal state of a Yb^{+} ion. We ameliorate the effect of the 60-fold mismatch of the radiative linewidths with coherent photon generation and a high-finesse fiber-based optical cavity enhancing the coupling between the single photon and the ion. The transfer of information presented here via the classical correlations between the σ_{z} projection of the quantum-dot spin and the internal state of the ion provides a promising step towards quantum-state transfer in a hybrid photonic network.

Generation of heralded entanglement between distant quantum dot hole spins

NASA Astrophysics Data System (ADS)

Delteil, Aymeric

Entanglement plays a central role in fundamental tests of quantum mechanics as well as in the burgeoning field of quantum information processing. Particularly in the context of quantum networks and communication, some of the major challenges are the efficient generation of entanglement between stationary (spin) and propagating (photon) qubits, the transfer of information from flying to stationary qubits, and the efficient generation of entanglement between distant stationary (spin) qubits. In this talk, I will present such experimental implementations achieved in our team with semiconductor self-assembled quantum dots.Not only are self-assembled quantum dots good single-photon emitters, but they can host an electron or a hole whose spin serves as a quantum memory, and then present spin-dependent optical selection rules leading to an efficient spin-photon quantum interface. Moreover InGaAs quantum dots grown on GaAs substrate can profit from the maturity of III-V semiconductor technology and can be embedded in semiconductor structures like photonic cavities and Schottky diodes.I will report on the realization of heralded quantum entanglement between two semiconductor quantum dot hole spins separated by more than five meters. The entanglement generation scheme relies on single photon interference of Raman scattered light from both dots. A single photon detection projects the system into a maximally entangled state. We developed a delayed two-photon interference scheme that allows for efficient verification of quantum correlations. Moreover the efficient spin-photon interface provided by self-assembled quantum dots allows us to reach an unprecedented rate of 2300 entangled spin pairs per second, which represents an improvement of four orders of magnitude as compared to prior experiments carried out in other systems.Our results extend previous demonstrations in single trapped ions or neutral atoms, in atom ensembles and nitrogen vacancy centers to the domain of artificial atoms in semiconductor nanostructures that allow for on-chip integration of electronic and photonic elements. This work lays the groundwork for the realization of quantum repeaters and quantum networks on a chip.