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Sample records for semiconductor nanocrystals inmicrofluidic

  1. Synthesis and Manipulation of Semiconductor Nanocrystals inMicrofluidic Reactors

    SciTech Connect

    Chan, Emory Ming-Yue

    2006-01-01

    Microfluidic reactors are investigated as a mechanism tocontrol the growth of semiconductor nanocrystals and characterize thestructural evolution of colloidal quantum dots. Due to their shortdiffusion lengths, low thermal masses, and predictable fluid dynamics,microfluidic devices can be used to quickly and reproducibly alterreaction conditions such as concentration, temperature, and reactiontime, while allowing for rapid reagent mixing and productcharacterization. These features are particularly useful for colloidalnanocrystal reactions, which scale poorly and are difficult to controland characterize in bulk fluids. To demonstrate the capabilities ofnanoparticle microreactors, a size series of spherical CdSe nanocrystalswas synthesized at high temperature in a continuous-flow, microfabricatedglass reactor. Nanocrystal diameters are reproducibly controlled bysystematically altering reaction parameters such as the temperature,concentration, and reaction time. Microreactors with finer control overtemperature and reagent mixing were designed to synthesize nanoparticlesof different shapes, such as rods, tetrapods, and hollow shells. The twomajor challenges observed with continuous flow reactors are thedeposition of particles on channel walls and the broad distribution ofresidence times that result from laminar flow. To alleviate theseproblems, I designed and fabricated liquid-liquid segmented flowmicroreactors in which the reaction precursors are encapsulated inflowing droplets suspended in an immiscible carrier fluid. The synthesisof CdSe nanocrystals in such microreactors exhibited reduced depositionand residence time distributions while enabling the rapid screening aseries of samples isolated in nL droplets. Microfluidic reactors werealso designed to modify the composition of existing nanocrystals andcharacterize the kinetics of such reactions. The millisecond kinetics ofthe CdSe-to-Ag2Se nanocrystal cation exchange reaction are measured insitu with micro

  2. Electronic spectra of semiconductor nanocrystals

    SciTech Connect

    Alivisatos, A.P.

    1993-12-31

    Semiconductor nanocrystals smaller than the bulk exciton show substantial quantum confinement effects. Recent experiments including Stark effect, resonance Raman, valence band photoemission, and near edge X-ray adsorption will be used to put together a picture of the nanocrystal electronic states.

  3. Aqueous Based Semiconductor Nanocrystals.

    PubMed

    Jing, Lihong; Kershaw, Stephen V; Li, Yilin; Huang, Xiaodan; Li, Yingying; Rogach, Andrey L; Gao, Mingyuan

    2016-09-28

    This review summarizes traditional and recent nonconventional, bioinspired, methods for the aqueous synthesis of colloidal semiconductor quantum dots (QDs). The basic chemistry concepts are critically emphasized at the very beginning as these are strongly correlated with the selection of ligands and the optimal formation of aqueous QDs and their more sophisticated structures. The synergies of biomimetic and biosynthetic methods that can combine biospecific reactivity with the robust and strong optical responses of QDs have also resulted in new approaches to the synthesis of the nanoparticles themselves. A related new avenue is the recent extension of QD synthesis to form nanoparticles endowed with chiral optical properties. The optical characteristics of QD materials and their advanced forms such as core/shell heterostructures, alloys, and doped QDs are discussed: from the design considerations of optical band gap tuning, the control and reduction of the impact of surface traps, the consideration of charge carrier processes that affect emission and energy and charge transfer, to the impact and influence of lattice strain. We also describe the considerable progress in some selected QD applications such as in bioimaging and theranostics. The review concludes with future strategies and identification of key challenges that still need to be resolved in reaching very attractive, scalable, yet versatile aqueous syntheses that may widen the scope of commercial applications for semiconductor nanocrystals. PMID:27586892

  4. Semiconductor Nanocrystals for Biological Imaging

    SciTech Connect

    Fu, Aihua; Gu, Weiwei; Larabell, Carolyn; Alivisatos, A. Paul

    2005-06-28

    Conventional organic fluorophores suffer from poor photo stability, narrow absorption spectra and broad emission feature. Semiconductor nanocrystals, on the other hand, are highly photo-stable with broad absorption spectra and narrow size-tunable emission spectra. Recent advances in the synthesis of these materials have resulted in bright, sensitive, extremely photo-stable and biocompatible semiconductor fluorophores. Commercial availability facilitates their application in a variety of unprecedented biological experiments, including multiplexed cellular imaging, long-term in vitro and in vivo labeling, deep tissue structure mapping and single particle investigation of dynamic cellular processes. Semiconductor nanocrystals are one of the first examples of nanotechnology enabling a new class of biomedical applications.

  5. Semiconductor nanocrystal-based phagokinetic tracking

    DOEpatents

    Alivisatos, A Paul; Larabell, Carolyn A; Parak, Wolfgang J; Le Gros, Mark; Boudreau, Rosanne

    2014-11-18

    Methods for determining metabolic properties of living cells through the uptake of semiconductor nanocrystals by cells. Generally the methods require a layer of neutral or hydrophilic semiconductor nanocrystals and a layer of cells seeded onto a culture surface and changes in the layer of semiconductor nanocrystals are detected. The observed changes made to the layer of semiconductor nanocrystals can be correlated to such metabolic properties as metastatic potential, cell motility or migration.

  6. Photoemission studies of semiconductor nanocrystals

    SciTech Connect

    Hamad, K. S.; Roth, R.; Alivisatos, A. P.

    1997-04-01

    Semiconductor nanocrystals have been the focus of much attention in the last ten years due predominantly to their size dependent optical properties. Namely, the band gap of nanocrystals exhibits a shift to higher energy with decreasing size due to quantum confinement effects. Research in this field has employed primarily optical techniques to study nanocrystals, and in this respect this system has been investigated extensively. In addition, one is able to synthesize monodisperse, crystalline particles of CdS, CdSe, Si, InP, InAs, as well as CdS/HgS/CdS and CdSe/CdS composites. However, optical spectroscopies have proven ambiguous in determining the degree to which electronic excitations are interior or surface admixtures or giving a complete picture of the density of states. Photoemission is a useful technique for understanding the electronic structure of nanocrystals and the effects of quantum confinement, chemical environments of the nanocrystals, and surface coverages. Of particular interest to the authors is the surface composition and structure of these particles, for they have found that much of the behavior of nanocrystals is governed by their surface. Previously, the authors had performed x-ray photoelectron spectroscopy (XPS) on CdSe nanocrystals. XPS has proven to be a powerful tool in that it allows one to determine the composition of the nanocrystal surface.

  7. Mixed semiconductor nanocrystal compositions

    DOEpatents

    Maskaly, Garry R.; Schaller, Richard D.; Klimov, Victor I.

    2011-02-15

    Composition comprising one or more energy donors and one or more energy acceptors, wherein energy is transferred from the energy donor to the energy acceptor and wherein: the energy acceptor is a colloidal nanocrystal having a lower band gap energy than the energy donor; the energy donor and the energy acceptor are separated by a distance of 40 nm or less; wherein the average peak absorption energy of the acceptor is at least 20 meV greater than the average peak emission energy of the energy donor; and wherein the ratio of the number of energy donors to the number of energy acceptors is from about 2:1 to about 1000:1.

  8. Semiconductor-nanocrystal/conjugated polymer thin films

    DOEpatents

    Alivisatos, A. Paul; Dittmer, Janke J.; Huynh, Wendy U.; Milliron, Delia

    2010-08-17

    The invention described herein provides for thin films and methods of making comprising inorganic semiconductor-nanocrystals dispersed in semiconducting-polymers in high loading amounts. The invention also describes photovoltaic devices incorporating the thin films.

  9. Semiconductor-nanocrystal/conjugated polymer thin films

    DOEpatents

    Alivisatos, A. Paul; Dittmer, Janke J.; Huynh, Wendy U.; Milliron, Delia

    2014-06-17

    The invention described herein provides for thin films and methods of making comprising inorganic semiconductor-nanocrystals dispersed in semiconducting-polymers in high loading amounts. The invention also describes photovoltaic devices incorporating the thin films.

  10. Quantum theory of electroabsorption in semiconductor nanocrystals.

    PubMed

    Tepliakov, Nikita V; Leonov, Mikhail Yu; Baranov, Alexander V; Fedorov, Anatoly V; Rukhlenko, Ivan D

    2016-01-25

    We develop a simple quantum-mechanical theory of interband absorption by semiconductor nanocrystals exposed to a dc electric field. The theory is based on the model of noninteracting electrons and holes in an infinitely deep quantum well and describes all the major features of electroabsorption, including the Stark effect, the Franz-Keldysh effect, and the field-induced spectral broadening. It is applicable to nanocrystals of different shapes and dimensions (quantum dots, nanorods, and nanoplatelets), and will prove useful in modeling and design of electrooptical devices based on ensembles of semiconductor nanocrystals.

  11. Inorganic Chemistry Solutions to Semiconductor Nanocrystal Problems

    SciTech Connect

    Alvarado, Samuel R.; Guo, Yijun; Ruberu, T. Purnima A.; Tavasoli, Elham; Vela, Javier

    2014-03-15

    The optoelectronic and chemical properties of semiconductor nanocrystals heavily depend on their composition, size, shape and internal structure, surface functionality, etc. Available strategies to alter these properties through traditional colloidal syntheses and ligand exchange methods place a premium on specific reaction conditions and surfactant combinations. In this invited review, we apply a molecular-level understanding of chemical precursor reactivity to reliably control the morphology, composition and intimate architecture (core/shell vs. alloyed) of semiconductor nanocrystals. We also describe our work aimed at achieving highly selective, low-temperature photochemical methods for the synthesis of semiconductor–metal and semiconductor–metal oxide photocatalytic nanocomposites. In addition, we describe our work on surface modification of semiconductor nanocrystal quantum dots using new approaches and methods that bypass ligand exchange, retaining the nanocrystal's native ligands and original optical properties, as well as on spectroscopic methods of characterization useful in determining surface ligand organization and chemistry. Using recent examples from our group and collaborators, we demonstrate how these efforts have lead to faster, wider and more systematic application of semiconductor nanocrystal-based materials to biological imaging and tracking, and to photocatalysis of unconventional substrates. We believe techniques and methods borrowed from inorganic chemistry (including coordination, organometallic and solid state chemistry) have much to offer in reaching a better understanding of the synthesis, functionalization and real-life application of such exciting materials as semiconductor nanocrystals (quantum dots, rods, tetrapods, etc.).

  12. Phase transitions and doping in semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Sahu, Ayaskanta

    Colloidal semiconductor nanocrystals are a promising technological material because their size-dependent optical and electronic properties can be exploited for a diverse range of applications such as light-emitting diodes, bio-labels, transistors, and solar cells. For many of these applications, electrical current needs to be transported through the devices. However, while their solution processability makes these colloidal nanocrystals attractive candidates for device applications, the bulky surfactants that render these nanocrystals dispersible in common solvents block electrical current. Thus, in order to realize the full potential of colloidal semiconductor nanocrystals in the next-generation of solid-state devices, methods must be devised to make conductive films from these nanocrystals. One way to achieve this would be to add minute amounts of foreign impurity atoms (dopants) to increase their conductivity. Electronic doping in nanocrystals is still very much in its infancy with limited understanding of the underlying mechanisms that govern the doping process. This thesis introduces an innovative synthesis of doped nanocrystals and aims at expanding the fundamental understanding of charge transport in these doped nanocrystal films. The list of semiconductor nanocrystals that can be doped is large, and if one combines that with available dopants, an even larger set of materials with interesting properties and applications can be generated. In addition to doping, another promising route to increase conductivity in nanocrystal films is to use nanocrystals with high ionic conductivities. This thesis also examines this possibility by studying new phases of mixed ionic and electronic conductors at the nanoscale. Such a versatile approach may open new pathways for interesting fundamental research, and also lay the foundation for the creation of novel materials with important applications. In addition to their size-dependence, the intentional incorporation of

  13. Developing New Nanoprobes from Semiconductor Nanocrystals

    SciTech Connect

    Fu, Aihua

    2006-01-01

    In recent years, semiconductor nanocrystal quantum dots havegarnered the spotlight as an important new class of biological labelingtool. Withoptical properties superior to conventional organicfluorophores from many aspects, such as high photostability andmultiplexing capability, quantum dots have been applied in a variety ofadvanced imaging applications. This dissertation research goes along withlarge amount of research efforts in this field, while focusing on thedesign and development of new nanoprobes from semiconductor nanocrystalsthat are aimed for useful imaging or sensing applications not possiblewith quantum dots alone. Specifically speaking, two strategies have beenapplied. In one, we have taken advantage of the increasing capability ofmanipulating the shape of semiconductor nanocrystals by developingsemiconductor quantum rods as fluorescent biological labels. In theother, we have assembled quantum dots and gold nanocrystals into discretenanostructures using DNA. The background information and synthesis,surface manipulation, property characterization and applications of thesenew nanoprobes in a few biological experiments are detailed in thedissertation.

  14. Extracting hot carriers from photoexcited semiconductor nanocrystals

    SciTech Connect

    Zhu, Xiaoyang

    2014-12-10

    This research program addresses a fundamental question related to the use of nanomaterials in solar energy -- namely, whether semiconductor nanocrystals (NCs) can help surpass the efficiency limits, the so-called “Shockley-Queisser” limit, in conventional solar cells. In these cells, absorption of photons with energies above the semiconductor bandgap generates “hot” charge carriers that quickly “cool” to the band edges before they can be utilized to do work; this sets the solar cell efficiency at a limit of ~31%. If instead, all of the energy of the hot carriers could be captured, solar-to-electric power conversion efficiencies could be increased, theoretically, to as high as 66%. A potential route to capture this energy is to utilize semiconductor nanocrystals. In these materials, the quasi-continuous conduction and valence bands of the bulk semiconductor become discretized due to confinement of the charge carriers. Consequently, the energy spacing between the electronic levels can be much larger than the highest phonon frequency of the lattice, creating a “phonon bottleneck” wherein hot-carrier relaxation is possible via slower multiphonon emission. For example, hot-electron lifetimes as long as ~1 ns have been observed in NCs grown by molecular beam epitaxy. In colloidal NCs, long lifetimes have been demonstrated through careful design of the nanocrystal interfaces. Due to their ability to slow electronic relaxation, semiconductor NCs can in principle enable extraction of hot carriers before they cool to the band edges, leading to more efficient solar cells.

  15. Electronic displays using optically pumped luminescent semiconductor nanocrystals

    DOEpatents

    Weiss, Shimon; Schlamp, Michael C; Alivisatos, A. Paul

    2014-02-11

    A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

  16. Electronic displays using optically pumped luminescent semiconductor nanocrystals

    DOEpatents

    Weiss, Shimon; Schlam, Michael C; Alivisatos, A. Paul

    2014-03-25

    A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit tight of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

  17. Electronic displays using optically pumped luminescent semiconductor nanocrystals

    DOEpatents

    Weiss, Shimon; Schlamp, Michael C.; Alivisatos, A. Paul

    2010-04-13

    A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

  18. Electronic displays using optically pumped luminescent semiconductor nanocrystals

    DOEpatents

    Weiss, Shimon; Schlamp, Michael C.; Alivisatos, Paul A.

    2015-11-10

    A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit tight of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

  19. Electronic displays using optically pumped luminescent semiconductor nanocrystals

    SciTech Connect

    Weiss, Shimon; Schlamp, Michael C.; Alivisatos, A. Paul

    2015-06-23

    A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

  20. Electronic displays using optically pumped luminescent semiconductor nanocrystals

    DOEpatents

    Weiss, Shimon; Schlamp, Michael C.; Alivisatos, A. Paul

    2011-09-27

    A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

  1. Electronic displays using optically pumped luminescent semiconductor nanocrystals

    SciTech Connect

    Weiss, Shimon; Schlamp, Michael C.; Alivisatos, A. Paul

    2005-03-08

    A multicolor electronic display is based on an array of luminescent semiconductor nanocrystals. Nanocrystals which emit light of different colors are grouped into pixels. The nanocrystals are optically pumped to produce a multicolor display. Different sized nanocrystals are used to produce the different colors. A variety of pixel addressing systems can be used.

  2. The structure and morphology of semiconductor nanocrystals

    SciTech Connect

    Kadavanich, A V

    1997-11-01

    Colloidal semiconductor nanocrystals were studied using High Resolution Transmission Electron Microscopy (HRTEM). Organically capped nanocrystals were found to have faceted shapes consistent with Wulff polyhedra after the effects of capping ligands on surface energies were taken into account. The basic shape thus derived for wurtzite (WZ) structure CdSe nanocrystals capped by tri-octyl phosphine oxide (TOPO) was a truncated hexagonal prism, elongated alone the <001> axis with (100) and (002) facets. This structure has C{sub 3v} point group symmetry. The main defect in this structure is a stacking fault (a single layer of zinc blende type stacking), which does not significantly affect the shape (does not alter the point group).

  3. Synthesis and applications of heterostructured semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Khon, Elena

    Semiconductor nanocrystals (NCs) have been of great interest to researchers for several decades due to their unique optoelectronic properties. These nanoparticles are widely used for a variety of different applications. However, there are many unresolved issues that lower the efficiency and/or stability of devices which incorporate these NCs. Our research is dedicated to addressing these issues by identifying potential problems and resolving them, improving existing systems, generating new synthetic strategies, and/or building new devices. The general strategies for the synthesis of different nanocrystals were established in this work, one of which is the colloidal growth of gold domains onto CdS semiconductor nanocrystals. Control of shape and size was achieved simply by adjusting the temperature and the time of the reaction. Depending on the exact morphology of Au and CdS domains, fabricated nano-composites can undergo evaporation-induced self-assembly onto a substrate, which is very useful for building devices. CdS/Au heterostructures can assemble in two different ways: through end-to-end coupling of Au domains, resulting in the formation of one-dimensional chains; and via side-by-side packing of CdS nanorods, leading to the onset of two-dimensional superlattices. We investigated the nature of exciton-plasmon interactions in Au-tipped CdS nanorods using femtosecond transient absorption spectroscopy. The study demonstrated that the key optoelectronic properties of electrically coupled metal and semiconductor domains are significantly different from those observed in systems with weak inter-domain coupling. In particular, strongly-coupled nanocomposites promote mixing of electronic states at semiconductor-metal domain interfaces, which causes a significant suppression of both plasmon and exciton carrier excitations. Colloidal QDs are starting to replace organic molecules in many different applications, such as organic light emmiting diods (OLEDs), due to their

  4. Semiconductor nanocrystals photosensitize C60 crystals.

    PubMed

    Biebersdorf, Andreas; Dietmüller, Roland; Susha, Andrei S; Rogach, Andrey L; Poznyak, Sergey K; Talapin, Dmitri V; Weller, Horst; Klar, Thomas A; Feldmann, Jochen

    2006-07-01

    Semiconductor nanocrystals (SCNCs) made of CdSe, CdTe, and InP are used to photosensitize needlelike C(60) crystals. The photocurrent is increased by up to 3 orders of magnitude as compared with C(60) crystals without SCNCs. The photocurrent spectrum can be tuned precisely by the SCNC size and material, rendering the SCNC-functionalized C(60) crystals an excellent material for spectrally tuneable photodetectors. We explain the increased photocurrent as a result of photoexcited electrons transferring from the SCNCs to the C(60) crystals and causing photoconductivity, while the complementary holes remain trapped in the SCNCs.

  5. Enantioselective cellular uptake of chiral semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Martynenko, I. V.; Kuznetsova, V. A.; Litvinov, I. K.; Orlova, A. O.; Maslov, V. G.; Fedorov, A. V.; Dubavik, A.; Purcell-Milton, F.; Gun'ko, Yu K.; Baranov, A. V.

    2016-02-01

    The influence of the chirality of semiconductor nanocrystals, CdSe/ZnS quantum dots (QDs) capped with L- and D-cysteine, on the efficiency of their uptake by living Ehrlich Ascite carcinoma cells is studied by spectral- and time-resolved fluorescence microspectroscopy. We report an evident enantioselective process where cellular uptake of the L-Cys QDs is almost twice as effective as that of the D-Cys QDs. This finding paves the way for the creation of novel approaches to control the biological properties and behavior of nanomaterials in living cells.

  6. Doped semiconductor nanocrystal based fluorescent cellular imaging probes

    NASA Astrophysics Data System (ADS)

    Maity, Amit Ranjan; Palmal, Sharbari; Basiruddin, Sk; Karan, Niladri Sekhar; Sarkar, Suresh; Pradhan, Narayan; Jana, Nikhil R.

    2013-05-01

    Doped semiconductor nanocrystals such as Mn doped ZnS, Mn doped ZnSe and Cu doped InZnS, are considered as new classes of fluorescent biological probes with low toxicity. Although the synthesis in high quality of such nanomaterials is now well established, transforming them into functional fluorescent probes remains a challenge. Here we report a fluorescent cellular imaging probe made of high quality doped semiconductor nanocrystals. We have identified two different coating approaches suitable for transforming the as synthesized hydrophobic doped semiconductor nanocrystals into water-soluble functional nanoparticles. Following these approaches we have synthesized TAT-peptide- and folate-functionalized nanoparticles of 10-80 nm hydrodynamic diameter and used them as a fluorescent cell label. The results shows that doped semiconductor nanocrystals can be an attractive alternative for conventional cadmium based quantum dots with low toxicity.Doped semiconductor nanocrystals such as Mn doped ZnS, Mn doped ZnSe and Cu doped InZnS, are considered as new classes of fluorescent biological probes with low toxicity. Although the synthesis in high quality of such nanomaterials is now well established, transforming them into functional fluorescent probes remains a challenge. Here we report a fluorescent cellular imaging probe made of high quality doped semiconductor nanocrystals. We have identified two different coating approaches suitable for transforming the as synthesized hydrophobic doped semiconductor nanocrystals into water-soluble functional nanoparticles. Following these approaches we have synthesized TAT-peptide- and folate-functionalized nanoparticles of 10-80 nm hydrodynamic diameter and used them as a fluorescent cell label. The results shows that doped semiconductor nanocrystals can be an attractive alternative for conventional cadmium based quantum dots with low toxicity. Electronic supplementary information available: Characterization details of coating and

  7. Luminescent Colloidal Semiconductor Nanocrystals Containing Copper: Synthesis, Photophysics, and Applications.

    PubMed

    Knowles, Kathryn E; Hartstein, Kimberly H; Kilburn, Troy B; Marchioro, Arianna; Nelson, Heidi D; Whitham, Patrick J; Gamelin, Daniel R

    2016-09-28

    Copper-doped semiconductors are classic phosphor materials that have been used in a variety of applications for many decades. Colloidal copper-doped semiconductor nanocrystals have recently attracted a great deal of interest because they combine the solution processability and spectral tunability of colloidal nanocrystals with the unique photoluminescence properties of copper-doped semiconductor phosphors. Although ternary and quaternary semiconductors containing copper, such as CuInS2 and Cu2ZnSnS4, have been studied primarily in the context of their photovoltaic applications, when synthesized as colloidal nanocrystals, these materials have photoluminescence properties that are remarkably similar to those of copper-doped semiconductor nanocrystals. This review focuses on the luminescent properties of colloidal copper-doped, copper-based, and related copper-containing semiconductor nanocrystals. Fundamental investigations into the luminescence of copper-containing colloidal nanocrystals are reviewed in the context of the well-established luminescence mechanisms of bulk copper-doped semiconductors and copper(I) molecular coordination complexes. The use of colloidal copper-containing nanocrystals in applications that take advantage of their luminescent properties, such as bioimaging, solid-state lighting, and luminescent solar concentrators, is also discussed.

  8. Process for forming shaped group II-VI semiconductor nanocrystals, and product formed using process

    DOEpatents

    Alivisatos, A. Paul; Peng, Xiaogang; Manna, Liberato

    2001-01-01

    A process for the formation of shaped Group II-VI semiconductor nanocrystals comprises contacting the semiconductor nanocrystal precursors with a liquid media comprising a binary mixture of phosphorus-containing organic surfactants capable of promoting the growth of either spherical semiconductor nanocrystals or rod-like semiconductor nanocrystals, whereby the shape of the semiconductor nanocrystals formed in said binary mixture of surfactants is controlled by adjusting the ratio of the surfactants in the binary mixture.

  9. Process for forming shaped group III-V semiconductor nanocrystals, and product formed using process

    DOEpatents

    Alivisatos, A. Paul; Peng, Xiaogang; Manna, Liberato

    2001-01-01

    A process for the formation of shaped Group III-V semiconductor nanocrystals comprises contacting the semiconductor nanocrystal precursors with a liquid media comprising a binary mixture of phosphorus-containing organic surfactants capable of promoting the growth of either spherical semiconductor nanocrystals or rod-like semiconductor nanocrystals, whereby the shape of the semiconductor nanocrystals formed in said binary mixture of surfactants is controlled by adjusting the ratio of the surfactants in the binary mixture.

  10. Organo luminescent semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Jr., Marcel; Alivisatos, Paul

    2008-01-01

    A semiconductor nanocrystal compound is described capable of linking to an affinity molecule. The compound comprises (1) a semiconductor nanocrystal capable of emitting electromagnetic radiation and/or absorbing energy, and/or scattering or diffracting electromagnetic radiation--when excited by an electromagnetic radiation source or a particle beam; and (2) an affinity molecule linked to the semiconductor nanocrystal. The semiconductor nanocrystal is linked to an affinity molecule to form a semiconductor nanocrystal probe capable of bonding with a detectable substance. Exposure of the semiconductor nanocrystal to excitation energy will excite the semiconductor nanocrystal causing the emission of electromagnetic radiation. Further described are processes for respectively: making the luminescent semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and using the probe to determine the presence of a detectable substance in a material.

  11. Controlled Chemical Doping of Semiconductor Nanocrystals Using Redox Buffers

    SciTech Connect

    Engel, Jesse H.; Surendranath, Yogesh; Alivisatos, Paul

    2013-07-20

    Semiconductor nanocrystal solids are attractive materials for active layers in next-generation optoelectronic devices; however, their efficient implementation has been impeded by the lack of precise control over dopant concentrations. Herein we demonstrate a chemical strategy for the controlled doping of nanocrystal solids under equilibrium conditions. Exposing lead selenide nanocrystal thin films to solutions containing varying proportions of decamethylferrocene and decamethylferrocenium incrementally and reversibly increased the carrier concentration in the solid by 2 orders of magnitude from their native values. This application of redox buffers for controlled doping provides a new method for the precise control of the majority carrier concentration in porous semiconductor thin films.

  12. Radiative decay rates of impurity states in semiconductor nanocrystals

    SciTech Connect

    Turkov, Vadim K.; Baranov, Alexander V.; Fedorov, Anatoly V.; Rukhlenko, Ivan D.

    2015-10-15

    Doped semiconductor nanocrystals is a versatile material base for contemporary photonics and optoelectronics devices. Here, for the first time to the best of our knowledge, we theoretically calculate the radiative decay rates of the lowest-energy states of donor impurity in spherical nanocrystals made of four widely used semiconductors: ZnS, CdSe, Ge, and GaAs. The decay rates were shown to vary significantly with the nanocrystal radius, increasing by almost three orders of magnitude when the radius is reduced from 15 to 5 nm. Our results suggest that spontaneous emission may dominate the decay of impurity states at low temperatures, and should be taken into account in the design of advanced materials and devices based on doped semiconductor nanocrystals.

  13. Synthesis of Doped Semiconductor Nanocrystals and Conductive Coatings

    NASA Astrophysics Data System (ADS)

    Wills, Andrew Wilke

    Semiconductor nanocrystals are an intriguing class of materials because of their size-tunable properties. This makes them promising for future optoelectronic devices such as solar cells and light emitting diodes. Realization of these devices, however, requires precise control of the flow of electricity through the particles. In bulk semiconductors, this is achieved by using materials with few unintentional defects, then intentionally adding particular defects or dopants to alter the semiconductor's electronic properties. In contrast, the addition of electrically active dopants has scarcely been demonstrated in semiconductor nanocrystals, and charge transport is hindered by the barrier of electron hopping between particles. The goal of this thesis, therefore, is to discover new methods to control charge transport in nanocrystals. It divides into three major thrusts: 1) the investigation of the doping process in semiconductor nanocrystals, 2) the invention of new synthetic methods to incorporate electrically active dopants into semiconductor nanocrystals, and 3) the invention of a new nanocrystal surface coating that aids processing of nanocrystals into devices but can be removed to enhance charge transport between particles. The first objective is achieved by the comparison of four different precursors that have been used to dope Mn into nanocrystals. Experiments show that dimethylmanganese incorporates efficiently into ZnSe nanocrystals while other precursors are less efficient and sometimes lower the quality of the nanocrystals produced. The second goal is met by the application of a core-shell synthetic strategy to the incorporation of non-isovalent impurities (Al and In) into CdSe nanocrystals. By separating the three steps of nucleation, dopant binding, and growth, each step can be optimized so that doping is achieved and high quality particles are produced. Detailed characterization shows dopant incorporation and local environment, while transistor

  14. Metal-insulator transition in films of doped semiconductor nanocrystals.

    PubMed

    Chen, Ting; Reich, K V; Kramer, Nicolaas J; Fu, Han; Kortshagen, Uwe R; Shklovskii, B I

    2016-03-01

    To fully deploy the potential of semiconductor nanocrystal films as low-cost electronic materials, a better understanding of the amount of dopants required to make their conductivity metallic is needed. In bulk semiconductors, the critical concentration of electrons at the metal-insulator transition is described by the Mott criterion. Here, we theoretically derive the critical concentration nc for films of heavily doped nanocrystals devoid of ligands at their surface and in direct contact with each other. In the accompanying experiments, we investigate the conduction mechanism in films of phosphorus-doped, ligand-free silicon nanocrystals. At the largest electron concentration achieved in our samples, which is half the predicted nc, we find that the localization length of hopping electrons is close to three times the nanocrystals diameter, indicating that the film approaches the metal-insulator transition.

  15. Semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Marcel; Alivisatos, Paul

    2011-12-20

    A semiconductor nanocrystal compound and probe are described. The compound is capable of linking to one or more affinity molecules. The compound comprises (1) one or more semiconductor nanocrystals capable of, in response to exposure to a first energy, providing a second energy, and (2) one or more linking agents, having a first portion linked to the one or more semiconductor nanocrystals and a second portion capable of linking to one or more affinity molecules. One or more semiconductor nanocrystal compounds are linked to one or more affinity molecules to form a semiconductor nanocrystal probe capable of bonding with one or more detectable substances in a material being analyzed, and capable of, in response to exposure to a first energy, providing a second energy. Also described are processes for respectively: making the semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and treating materials with the probe.

  16. Semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Marcel; Alivisatos, Paul

    2012-10-16

    A semiconductor nanocrystal compound and probe are described. The compound is capable of linking to one or more affinity molecules. The compound comprises (1) one or more semiconductor nanocrystals capable of, in response to exposure to a first energy, providing a second energy, and (2) one or more linking agents, having a first portion linked to the one or more semiconductor nanocrystals and a second portion capable of linking to one or more affinity molecules. One or more semiconductor nanocrystal compounds are linked to one or more affinity molecules to form a semiconductor nanocrystal probe capable of bonding with one or more detectable substances in a material being analyzed, and capable of, in response to exposure to a first energy, providing a second energy. Also described are processes for respectively: making the semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and treating materials with the probe.

  17. Organo luminescent semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Jr., Marcel; Alivisatos, Paul

    2005-08-09

    A semiconductor nanocrystal compound is described capable of linking to an affinity molecule. The compound comprises (1) a semiconductor nanocrystal capable of emitting electromagnetic radiation and/or absorbing energy, and/or scattering or diffracting electromagnetic radiation--when excited by an electromagnetic radiation source or a particle beam; and (2) at least one linking agent, having a first portion linked to the semiconductor nanocrystal and a second portion capable of linking to an affinity molecule. The compound is linked to an affinity molecule to form a semiconductor nanocrystal probe capable of bonding with a detectable substance. Subsequent exposure to excitation energy will excite the semiconductor nanocrystal in the probe causing the emission of electromagnetic radiation. Further described are processes for respectively: making the luminescent semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and using the probe to determine the presence of a detectable substance in a material.

  18. Semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Marcel; Alivisatos, Paul

    2011-12-06

    A semiconductor nanocrystal compound and probe are described. The compound is capable of linking to one or more affinity molecules. The compound comprises (1) one or more semiconductor nanocrystals capable of, in response to exposure to a first energy, providing a second energy, and (2) one or more linking agents, having a first portion linked to the one or more semiconductor nanocrystals and a second portion capable of linking to one or more affinity molecules. One or more semiconductor nanocrystal compounds are linked to one or more affinity molecules to form a semiconductor nanocrystal probe capable of bonding with one or more detectable substances in a material being analyzed, and capable of, in response to exposure to a first energy, providing a second energy. Also described are processes for respectively: making the semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and treating materials with the probe.

  19. Organo luminescent semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Jr., Marcel; Alivisatos, Paul

    2002-01-01

    A semiconductor nanocrystal compound is described capable of linking to an affinity molecule. The compound comprises (1) a semiconductor nanocrystal capable of emitting electromagnetic radiation and/or absorbing energy, and/or scattering or diffracting electromagnetic radiation--when excited by an electromagnetic radiation source or a particle beam; and (2) at least one linking agent, having a first portion linked to the semiconductor nanocrystal and a second portion capable of linking to an affity molecule. The compound is linked to an affinity molecule to form a semiconductor nanocrystal probe capable of bonding with a detectable substance. Subsequent exposure to excitation energy will excite the semiconductor nanocrystal in he probe, causing the emission of electromagnetic radiation. Further described are processes for respectively: making the semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and using the probe to determine the presence of a detectable substance in a material.

  20. Organo luminescent semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Jr., Marcel; Alivisatos, Paul

    2004-03-02

    A semiconductor nanocrystal compound is described capable of linking to an affinity molecule. The compound comprises (1) a semiconductor nanocrystal capable of emitting electromagnetic radiation and/or absorbing energy, and/or scattering or diffracting electromagnetic radiation--when excited by an electromagnetic radiation source or a particle beam; and (2) at least one linking agent, having a first portion linked to the semiconductor nanocrystal and a second portion capable of linking to an affinity molecule. The compound is linked to an affinity molecule to form a semiconductor nanocrystal probe capable of bonding with a detectable substance. Subsequent exposure to excitation energy will excite the semiconductor nanocrystal in the probe, causing the emission of electromagnetic radiation. Further described are processes for respectively: making the semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and using the probe to determine the presence of a detectable substance in a material.

  1. Organo luminescent semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Jr., Marcel; Alivisatos, Paul

    2006-09-05

    A semiconductor nanocrystal compound is described capable of linking to an affinity molecule. The compound comprises (1) a semiconductor nanocrystal capable of emitting electromagnetic radiation and/or absorbing energy, and/or scattering or diffracting electromagnetic radiation--when excited by an electromagnetic radiation source or a particle beam; and (2) at least one linking agent, having a first portion linked to the semiconductor nanocrystal and a second portion capable of linking to an affinity molecule. The compound is linked to an affinity molecule to form a semiconductor nanocrystal probe capable of bonding with a detectable substance. subsequent exposure to excitation energy will excite the semiconductor nanocrystal in the probe causing the emission of electromagnetic radiation. Further described are processes for respectively: making the luminescent semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and using the probe to determine the presence of a detectable substance in a material.

  2. Semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Marcel; Alivisatos, Paul

    2014-01-28

    A semiconductor nanocrystal compound and probe are described. The compound is capable of linking to one or more affinity molecules. The compound comprises (1) one or more semiconductor nanocrystals capable of, in response to exposure to a first energy, providing a second energy, and (2) one or more linking agents, having a first portion linked to the one or more semiconductor nanocrystals and a second portion capable of linking to one or more affinity molecules. One or more semiconductor nanocrystal compounds are linked to one or more affinity molecules to form a semiconductor nanocrystal probe capable of bonding with one or more detectable substances in a material being analyzed, and capable of, in response to exposure to a first energy, providing a second energy. Also described are processes for respectively: making the semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and treating materials with the probe.

  3. Methods of use of semiconductor nanocrystal probes for treating a material

    DOEpatents

    Weiss, Shimon; Bruchez, Marcel; Alivisatos, Paul

    2007-04-27

    A semiconductor nanocrystal compound and probe are described. The compound is capable of linking to one or more affinity molecules. The compound comprises (1) one or more semiconductor nanocrystals capable of, in response to exposure to a first energy, providing a second energy, and (2) one or more linking agents, having a first portion linked to one or more semiconductor nanocrystals and a second portion capable of linking to one or more affinity molecules. One or more semiconductor nanocrystal compounds are linked to one or more affinity molecules to form a semiconductor nanocrystal probe capable of bonding with one or more detectable substances in a material being analyzed, and capable of, in response to exposure to a first energy, providing a second energy. Also described are processes for respectively: making the semiconductor nanocrystal compound; making the semiconductor nanocrystal probe; and treating materials with the probe.

  4. Level Anticrossing of Impurity States in Semiconductor Nanocrystals

    PubMed Central

    Baimuratov, Anvar S.; Rukhlenko, Ivan D.; Turkov, Vadim K.; Ponomareva, Irina O.; Leonov, Mikhail Yu.; Perova, Tatiana S.; Berwick, Kevin; Baranov, Alexander V.; Fedorov, Anatoly V.

    2014-01-01

    The size dependence of the quantized energies of elementary excitations is an essential feature of quantum nanostructures, underlying most of their applications in science and technology. Here we report on a fundamental property of impurity states in semiconductor nanocrystals that appears to have been overlooked—the anticrossing of energy levels exhibiting different size dependencies. We show that this property is inherent to the energy spectra of charge carriers whose spatial motion is simultaneously affected by the Coulomb potential of the impurity ion and the confining potential of the nanocrystal. The coupling of impurity states, which leads to the anticrossing, can be induced by interactions with elementary excitations residing inside the nanocrystal or an external electromagnetic field. We formulate physical conditions that allow a straightforward interpretation of level anticrossings in the nanocrystal energy spectrum and an accurate estimation of the states' coupling strength. PMID:25369911

  5. Nuclear magnetic relaxation studies of semiconductor nanocrystals and solids

    SciTech Connect

    Sachleben, J. R.

    1993-09-01

    Semiconductor nanocrystals, small biomolecules, and {sup 13}C enriched solids were studied through the relaxation in NMR spectra. Surface structure of semiconductor nanocrystals (CdS) was deduced from high resolution {sup 1}H and {sup 13}C liquid state spectra of thiophenol ligands on the nanocrystal surfaces. The surface coverage by thiophenol was found to be low, being 5.6 and 26% for nanocrystal radii of 11.8 and 19.2 {angstrom}. Internal motion is estimated to be slow with a correlation time > 10{sup {minus}8} s{sup {minus}1}. The surface thiophenol ligands react to form a dithiophenol when the nanocrystals were subjected to O{sub 2} and ultraviolet. A method for measuring {sup 14}N-{sup 1}H J-couplings is demonstrated on pyridine and the peptide oxytocin; selective 2D T{sub 1} and T{sub 2} experiments are presented for measuring relaxation times in crowded spectra with overlapping peaks in 1D, but relaxation effects interfere. Possibility of carbon-carbon cross relaxation in {sup 13}C enriched solids is demonstrated by experiments on zinc acetate and L-alanine.

  6. Nuclear magnetic relaxation studies of semiconductor nanocrystals and solids

    NASA Astrophysics Data System (ADS)

    Sachleben, J. R.

    1993-09-01

    Semiconductor nanocrystals, small biomolecules, and C-13 enriched solids were studied through the relaxation in NMR spectra. Surface structure of semiconductor nanocrystals (CdS) was deduced from high resolution H-1 and C-13 liquid state spectra of thiophenol ligands on the nanocrystal surfaces. The surface coverage by thiophenol was found to be low, being 5.6 and 26% for nanocrystal radii of 11.8 and 19.2 angstrom. Internal motion is estimated to be slow with a correlation time greater than 10(exp -8) s(exp -1). The surface thiophenol ligands react to form a dithiophenol when the nanocrystals were subjected to O2 and ultraviolet. A method for measuring (N-14)-(H-1) J-couplings is demonstrated on pyridine and the peptide oxytocin; selective 2D T(sub 1) and T(sub 2) experiments are presented for measuring relaxation times in crowded spectra with overlapping peaks in 1D, but relaxation effects interfere. Possibility of carbon-carbon cross relaxation in C-13 enriched solids is demonstrated by experiments on zinc acetate and L-alanine.

  7. Organic-Inorganic Composites of Semiconductor Nanocrystals for Efficient Excitonics.

    PubMed

    Guzelturk, Burak; Demir, Hilmi Volkan

    2015-06-18

    Nanocomposites of colloidal semiconductor nanocrystals integrated into conjugated polymers are the key to soft-material hybrid optoelectronics, combining advantages of both plastics and particles. Synergic combination of the favorable properties in the hybrids of colloidal nanocrystals and conjugated polymers offers enhanced performance and new functionalities in light-generation and light-harvesting applications, where controlling and mastering the excitonic interactions at the nanoscale are essential. In this Perspective, we highlight and critically consider the excitonic interactions in the organic-inorganic nanocomposites to achieve highly efficient exciton transfer through rational design of the nanocomposites. The use of strong excitonic interactions in optoelectronic devices can trigger efficiency breakthroughs in hybrid optoelectronics.

  8. Semiconductor-nanocrystals-based white light-emitting diodes.

    PubMed

    Dai, Quanqin; Duty, Chad E; Hu, Michael Z

    2010-08-01

    In response to the demands for energy and the concerns of global warming and climate change, energy efficient and environmentally friendly solid-state lighting, such as white light-emitting diodes (WLEDs), is considered to be the most promising and suitable light source. Because of their small size, high efficiency, and long lifetime, WLEDs based on colloidal semiconductor nanocrystals (or quantum dots) are emerging as a completely new technology platform for the development of flat-panel displays and solid-state lighting, exhibiting the potential to replace the conventionally used incandescent and fluorescent lamps. This replacement can cut the ever-increasing level of energy consumption, solve the problem of rapidly depleting fossil fuel reserves, and improve the quality of the global environment. In this review, the recent progress in semiconductor-nanocrystals-based WLEDs is highlighted, the different approaches for generating white light are compared, and the benefits and challenges of the solid-state lighting technology are discussed.

  9. Semiconductor Nanocrystals-Based White Light Emitting Diodes

    SciTech Connect

    Dai, Quanqin; Hu, Michael Z.; Duty, Chad E

    2010-01-01

    In response to the demands for energy and the concerns of global warming and climate change, energy efficient and environmentally friendly solid state lighting, such as white light emitting diodes (WLEDs), is considered to be the most promising and suitable light source. Because of their small size, high efficiency, and long lifetime, WLEDs based on colloidal semiconductor nanocrystals (or quantum dots) are emerging as a completely new technology platform for the development of flat-panel displays and solid state lighting, exhibiting the potential to replace the conventionally used incandescent and fluorescent lamps. This replacement could cut the ever-increasing energy consumption, solve the problem of rapidly depleting fossil fuel reserves, and improve the quality of the global environment. In this review, we highlight the recent progress in semiconductor nanocrystals-based WLEDs, compare different approaches for generating white light, and discuss the benefits and challenges of the solid state lighting technology.

  10. Semiconductor-Nanocrystals-Based White Light-Emitting Diodes

    SciTech Connect

    Dai, Quanqin; Duty, Chad E; Hu, Michael Z.

    2010-01-01

    In response to the demands for energy and the concerns of global warming and climate change, energy efficient and environmentally friendly solid-state lighting, such as white lightemitting diodes (WLEDs), is considered to be the most promising and suitable light source. Because of their small size, high efficiency, and long lifetime, WLEDs based on colloidal semiconductor nanocrystals (or quantum dots) are emerging as a completely new technology platform for the development of flat-panel displays and solid-state lighting, exhibiting the potential to replace the conventionally used incandescent and fluorescent lamps. This replacement can cut the ever-increasing level of energy consumption, solve the problem of rapidly depleting fossil fuel reserves, and improve the quality of the global environment. In this review, the recent progress in semiconductor-nanocrystals-based WLEDs is highlighted, the different approaches for generating white light are compared, and the benefits and challenges of the solid-state lighting technology are discussed.

  11. How many electrons make a semiconductor nanocrystal film metallic

    NASA Astrophysics Data System (ADS)

    Reich, Konstantin; Chen, Ting; Kramer, Nicolaas; Fu, Han; Kortshagen, Uwe; Shklovskii, Boris

    For films of semiconductor nanocrystals to achieve their potential as novel, low-cost electronic materials, a better understanding of their doping to tune their conductivity is required. So far, it not known how many dopants will turn a nanocrystal film from semiconducting to metallic. In bulk semiconductors, the critical concentration nM of electrons at the metal-insulator transition is described by the famous Mott criterion: nMaB3 ~= 0 . 02 , where aB is the effective Bohr radius. We show theoretically that in a dense NC film, where NCs touch each other by small facets, the concentration of electrons nc >>nM at the metal-insulator transition satisfies the condition: ncρ3 ~= 0 . 3 , where ρ is a radius of contact facets. In the accompanying experiments, we investigate the conduction mechanism in films of phosphorus-doped, ligand-free silicon nanocrystals. At the largest electron concentration achieved in our samples, which is half the predicted nc, we find that the localization length of hopping electrons is close to three times the nanocrystals diameter, indicating that the film approaches the metal-insulator transition. This work was supported primarily by the National Science Foundation through the University of Minnesota MRSEC under Award No. DMR-1420013.

  12. Semiconductor nanocrystals in photoconductive polymers: Charge generation and charge transport

    SciTech Connect

    Wang, Ying; Herron, Norman; Suna, A.

    1996-10-01

    A new class of photoconductive polymer composites, based on semiconductor nanocrystals (clusters) and carder-transporting polymers, have been developed. These materials are interesting for their potentials in laser printing, imaging, and photorefractives. We will describe material synthesis, charge transport and charge generation mechanisms. In particular, a model of field-dependent charge generation and separation in nonpolar media (e.g. polymers) will be discussed.

  13. Excited-State Dynamics in Colloidal Semiconductor Nanocrystals.

    PubMed

    Rabouw, Freddy T; de Mello Donega, Celso

    2016-10-01

    Colloidal semiconductor nanocrystals have attracted continuous worldwide interest over the last three decades owing to their remarkable and unique size- and shape-, dependent properties. The colloidal nature of these nanomaterials allows one to take full advantage of nanoscale effects to tailor their optoelectronic and physical-chemical properties, yielding materials that combine size-, shape-, and composition-dependent properties with easy surface manipulation and solution processing. These features have turned the study of colloidal semiconductor nanocrystals into a dynamic and multidisciplinary research field, with fascinating fundamental challenges and dazzling application prospects. This review focuses on the excited-state dynamics in these intriguing nanomaterials, covering a range of different relaxation mechanisms that span over 15 orders of magnitude, from a few femtoseconds to a few seconds after photoexcitation. In addition to reviewing the state of the art and highlighting the essential concepts in the field, we also discuss the relevance of the different relaxation processes to a number of potential applications, such as photovoltaics and LEDs. The fundamental physical and chemical principles needed to control and understand the properties of colloidal semiconductor nanocrystals are also addressed. PMID:27573500

  14. Preparation of III-V semiconductor nanocrystals

    DOEpatents

    Alivisatos, A. Paul; Olshavsky, Michael A.

    1996-01-01

    Nanometer-scale crystals of III-V semiconductors are disclosed, They are prepared by reacting a group III metal source with a group V anion source in a liquid phase at elevated temperature in the presence of a crystallite growth terminator such as pyridine or quinoline.

  15. Preparation of III-V semiconductor nanocrystals

    SciTech Connect

    Alivisatos, A.P.; Olshavsky, M.A.

    1996-04-09

    Nanometer-scale crystals of III-V semiconductors are disclosed. They are prepared by reacting a group III metal source with a group V anion source in a liquid phase at elevated temperature in the presence of a crystallite growth terminator such as pyridine or quinoline. 4 figs.

  16. Charge-controlled magnetism in colloidal doped semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Gamelin, Daniel

    2010-03-01

    Electrical control over the magnetic states of doped semiconductor nanostructures could enable new spin-based information processing technologies, but the relatively weak interactions between dopants and charge carriers have so far suggested that such gated magnetism will be limited to cryogenic temperatures. This talk will describe the observation of a large, reversible, room-temperature magnetic response to charge injection in free-standing colloidal ZnO nanocrystals doped with Mn(II) ions. Injected electrons are found to delocalize throughout the entire nanocrystal, and to activate new ferromagnetic Mn(II)-Mn(II) exchange interactions that are strong enough to overcome antiferromagnetic coupling between nearest-neighbor Mn(II) ions, making the full magnetic moments of all dopants observable upon charging. Removal of the electron causes the system to revert to its original form, allowing reversible charge-controlled manipulation of room-temperature nanocrystal magnetism. The physical properties of these charged, doped nanocrystals are directly analogous to those of bound magnetic poltroons (BMPs) postulated to underlie high-temperature ferromagnetic ordering in the bulk forms of this and related diluted magnetic oxides. This discovery of charge-controlled magnetism in free-standing colloidal nanocrystals that is large, reversible, and stable at room temperature presents new opportunities for fundamental studies and raises interesting possibilities for the development of spin-based information processing technologies from solution-processable semiconductor nanostructures. Related references: Ochsenbein, S. T.; Feng, Y.; Whitaker, K. M.; Badaeva, E.; Liu, W. K.; Li, X.; Gamelin, D. R., Nature Nanotechnology, 4, 681 (2009); Liu, W. K.; Whitaker, K. M.; Kittilstved, K. R.; Gamelin, D. R., J. Am. Chem. Soc., 128, 3910 (2006).

  17. Organo Luminescent semiconductor nanocrystal probes for biological applications and process for making and using such probes

    DOEpatents

    Weiss, Shimon; Bruchez, Jr., Marcel; Alivisatos, Paul

    1999-01-01

    A luminescent semiconductor nanocrystal compound is described which is capable of linking to an affinity molecule. The compound comprises (1) a semiconductor nanocrystal capable of emitting electromagnetic radiation (luminescing) in a narrow wavelength band and/or absorbing energy, and/or scattering or diffracting electromagnetic radiation--when excited by an electromagnetic radiation source (of narrow or broad bandwidth) or a particle beam; and (2) at least one linking agent, having a first portion linked to the semiconductor nanocrystal and a second portion capable of linking to an affinity molecule. The luminescent semiconductor nanocrystal compound is linked to an affinity molecule to form an organo luminescent semiconductor nanocrystal probe capable of bonding with a detectable substance in a material being analyzed, and capable of emitting electromagnetic radiation in a narrow wavelength band and/or absorbing, scattering, or diffracting energy when excited by an electromagnetic radiation source (of narrow or broad bandwidth) or a particle beam. The probe is stable to repeated exposure to light in the presence of oxygen and/or other radicals. Further described is a process for making the luminescent semiconductor nanocrystal compound and for making the organo luminescent semiconductor nanocrystal probe comprising the luminescent semiconductor nanocrystal compound linked to an affinity molecule capable of bonding to a detectable substance. A process is also described for using the probe to determine the presence of a detectable substance in a material.

  18. Dislocation-induced chirality of semiconductor nanocrystals.

    PubMed

    Baimuratov, Anvar S; Rukhlenko, Ivan D; Gun'ko, Yurii K; Baranov, Alexander V; Fedorov, Anatoly V

    2015-03-11

    Optical activity is a common natural phenomenon, which occurs in individual molecules, biomolecules, biological species, crystalline solids, liquid crystals, and various nanosized objects, leading to numerous important applications in almost every field of modern science and technology. Because this activity can hardly be altered, creation of artificial active media with controllable optical properties is of paramount importance. Here, for the first time to the best of our knowledge, we theoretically demonstrate that optical activity can be inherent to many semiconductor nanowires, as it is induced by chiral dislocations naturally developing during their growth. By assembling such nanowires in two- or three-dimensional periodic lattices, one can create optically active quantum supercrystals whose activity can be varied in many ways owing to the size quantization of the nanowires' energy spectra. We believe that this research is of particular importance for the future development of semiconducting nanomaterials and their applications in nanotechnology, chemistry, biology, and medicine.

  19. Building Structural Complexity in Semiconductor Nanocrystals through Chemical Transformations

    SciTech Connect

    Sadtler, Bryce F

    2009-05-01

    Methods are presented for synthesizing nanocrystal heterostructures comprised of two semiconductor materials epitaxially attached within individual nanostructures. The chemical transformation of cation exchange, where the cations within the lattice of an ionic nanocrystal are replaced with a different metal ion species, is used to alter the chemical composition at specific regions ofa nanocrystal. Partial cation exchange was performed in cadmium sulfide (CdS) nanorods of well-defined size and shape to examine the spatial organization of materials within the resulting nanocrystal heterostructures. The selectivity for cation exchange to take place at different facets of the nanocrystal plays an important role in determining the resulting morphology of the binary heterostructure. The exchange of copper (I) (Cu+) cations in CdS nanorods occurs preferentially at the ends of the nanorods. Theoretical modeling of epitaxial attachments between different facets of CdS and Cu2S indicate that the selectivity for cation exchange at the ends of the nanorods is a result of the low formation energy of the interfaces produced. During silver (I) (Ag+) cation exchange in CdS nanorods, non-selective nucleation of silver sulfide (Ag2S), followed by partial phase segregation leads to significant changes in the spatial arrangement of CdS and Ag2S regions at the exchange reaction proceeds through the nanocrystal. A well-ordered striped pattern of alternating CdS and Ag2S segments is found at intermediate fractions of exchange. The forces mediating this spontaneous process are a combination of Ostwald ripening to reduce the interfacial area along with a strain-induced repulsive interaction between Ag2S segments. To elucidate why Cu+ and Ag+ cation exchange with CdS nanorods produce different morphologies, models for epitaxial attachments between various facets of CdS with Cu2S or

  20. Engineered semiconductor nanocrystals with enhanced carrier multiplication yields

    NASA Astrophysics Data System (ADS)

    Klimov, Victor

    2014-03-01

    Carrier multiplication (CM) is a process whereby absorption of a single photon results in multiple electron-hole pairs (excitons). This process could benefit a number of solar-energy conversion technologies, most notably photocatalysis and photovoltaics. This presentation overviews recent progress in understanding the CM process in semiconductor nanocrystals, motivated by an outstanding challenge in this field - the lack of capability to predict the CM performance of nanocrystals based on their known photophysical properties or documented parameters of parental bulk solids. Here, we present a possible solution to this problem by showing that, using biexciton Auger lifetimes and intraband relaxation rates inferred from ultrafast spectroscopic studies, we can rationalize relative changes in CM yields as a function of nanocrystal composition, size and shape. Further, guided by this model, we demonstrate a two-fold enhancement in multiexciton yields in PbSe nanorods vs. quantum dots attributed to enhanced Coulomb interactions. We also explore the control of competing intra-band cooling for increasing multiexciton production. Specifically, we design a new type of hetero-structured PbSe/CdSe quantum dots with reduced rates of intra-band relaxation and demonstrate a four-fold boost in the multiexciton yield. These studies provide useful guidelines for future efforts to achieve the ultimate, energy-conservation-defined CM efficiencies.

  1. Mapping the exciton diffusion in semiconductor nanocrystal solids.

    PubMed

    Kholmicheva, Natalia; Moroz, Pavel; Bastola, Ebin; Razgoniaeva, Natalia; Bocanegra, Jesus; Shaughnessy, Martin; Porach, Zack; Khon, Dmitriy; Zamkov, Mikhail

    2015-03-24

    Colloidal nanocrystal solids represent an emerging class of functional materials that hold strong promise for device applications. The macroscopic properties of these disordered assemblies are determined by complex trajectories of exciton diffusion processes, which are still poorly understood. Owing to the lack of theoretical insight, experimental strategies for probing the exciton dynamics in quantum dot solids are in great demand. Here, we develop an experimental technique for mapping the motion of excitons in semiconductor nanocrystal films with a subdiffraction spatial sensitivity and a picosecond temporal resolution. This was accomplished by doping PbS nanocrystal solids with metal nanoparticles that force the exciton dissociation at known distances from their birth. The optical signature of the exciton motion was then inferred from the changes in the emission lifetime, which was mapped to the location of exciton quenching sites. By correlating the metal-metal interparticle distance in the film with corresponding changes in the emission lifetime, we could obtain important transport characteristics, including the exciton diffusion length, the number of predissociation hops, the rate of interparticle energy transfer, and the exciton diffusivity. The benefits of this approach to device applications were demonstrated through the use of two representative film morphologies featuring weak and strong interparticle coupling.

  2. X-ray and photoelectron spectroscopy of the structure, reactivity, and electronic structure of semiconductor nanocrystals

    SciTech Connect

    Hamad, K.S.

    2000-05-01

    Semiconductor nanocrystals are a system which has been the focus of interest due to their size dependent properties and their possible use in technological applications. Many chemical and physical properties vary systematically with the size of the nanocrystal and thus their study enables the investigation of scaling laws. Due to the increasing surface to volume ratio as size is decreased, the surfaces of nanocrystals are expected to have a large influence on their electronic, thermodynamic, and chemical behavior. In spite of their importance, nanocrystal surfaces are still relatively uncharacterized in terms of their structure, electronic properties, bonding, and reactivity. Investigation of nanocrystal surfaces is currently limited by what techniques to use, and which methods are suitable for nanocrystals is still being determined. This work presents experiments using x-ray and electronic spectroscopies to explore the structure, reactivity, and electronic properties of semiconductor (CdSe, InAs) nanocrystals and how they vary with size. Specifically, x-ray absorption near edge spectroscopy (XANES) in conjunction with multiple scattering simulations affords information about the structural disorder present at the surface of the nanocrystal. X-ray photoelectron spectroscopy (XPS) and ultra-violet photoelectron spectroscopy (UPS) probe the electronic structure in terms of hole screening, and also give information about band lineups when the nanocrystal is placed in electric contact with a substrate. XPS of the core levels of the nanocrystal as a function of photo-oxidation time yields kinetic data on the oxidation reaction occurring at the surface of the nanocrystal.

  3. Radiative and nonradiative rate fluctuations of single colloidal semiconductor nanocrystals.

    PubMed

    Biebricher, Andreas; Sauer, Markus; Tinnefeld, Philip

    2006-03-23

    Spectrally and time-resolved single-molecule fluorescence spectroscopy was used to investigate fluctuations of the photophysical characteristics of different types of semiconductor nanocrystals (NCs) at room temperature. Correlation of photoluminescence (PL) emission maxima, decay time, and intensity of individual NCs with millisecond time resolution reveals new sources of intensity fluctuations and photophysical properties. In particular, we demonstrate that independent of quenched states spectral diffusion is associated with changes of the radiative rate constant k(r) by means of the quantum-confined Stark effect. Correlation of the different photophysical parameters revealed an intrinsic nonradiative rate and enabled the disentangling of intrinsic and extrinsic nonradiative rate constants. Moreover, it allowed us to assess the PL quantum yield of single NCs. Finally, the presented technique was successfully applied to demonstrate that the addition of antiblinking reagents such as mercaptoethylamine accelerates the observed fluctuations between different photophysical states.

  4. The length distribution function of semiconductor filamentary nanocrystals

    NASA Astrophysics Data System (ADS)

    Dubrovskii, V. G.

    2016-07-01

    The length distribution function of semiconductor filamentary nanocrystals is analyzed based on the adsorption-diffusion growth model. It is demonstrated that the asymptotic distribution has a Gaussian shape. If the diffusion flux to the apex comes from the entire lateral surface, the average length increases exponentially with time, and the mean-square deviation is proportional to the average length (exponential growth regime). If the diffusion collection of adatoms is limited to the top of the crystal, the average length increases linearly and the mean-square deviation equals the square root of average length (linear Poisson growth regime). In real-world systems, transition from exponential to Poisson growth occurs at lengths of the order of the diffusion length of adatoms. The dispersion of the distribution is actually defined at the exponential stage. The general classification of length distributions of various crystals is given. It is demonstrated that self-induced GaN- and Ga-catalytic III-V filamentary nanocrystals should be more homogeneous than Au-catalytic ones.

  5. A novel approach for the fabrication of all-inorganic nanocrystal solids: Semiconductor matrix encapsulated nanocrystal arrays

    NASA Astrophysics Data System (ADS)

    Moroz, Pavel

    Growing fossil fuels consumption compels researchers to find new alternative pathways to produce energy. Along with new materials for the conversion of different types of energy into electricity innovative methods for efficient processing of energy sources are also introduced. The main criteria for the success of such materials and methods are the low cost and compelling performance. Among different types of materials semiconductor nanocrystals are considered as promising candidates for the role of the efficient and cheap absorbers for solar energy applications. In addition to the anticipated cost reduction, the integration of nanocrystals (NC) into device architectures is inspired by the possibility of tuning the energy of electrical charges in NCs via nanoparticle size. However, the stability of nanocrystals in photovoltaic devices is limited by the stability of organic ligands which passivate the surface of semiconductors to preserve quantum confinement. The present work introduces a new strategy for low-temperature processing of colloidal nanocrystals into all-inorganic films: semiconductor matrix encapsulated nanocrystal arrays (SMENA). This methodology goes beyond the traditional ligand-interlinking scheme and relies on the encapsulation of morphologically-defined nanocrystal arrays into a matrix of a wide-band gap semiconductor, which preserves optoelectronic properties of individual nanoparticles. Fabricated solids exhibit excellent thermal stability, which is attributed to the heteroepitaxial structure of nanocrystal-matrix interfaces. The main characteristics and properties of these solids were investigated and compared with ones of traditionally fabricated nanocrystal films using standard spectroscopic, optoelectronic and electronic techniques. As a proof of concept, we. We also characterized electron transport phenomena in different types of nanocrystal films using all-optical approach. By measuring excited carrier lifetimes in either ligand-linked or

  6. Second Harmonic Generation and Confined Acoustic Phonons in HighlyExcited Semiconductor Nanocrystals

    SciTech Connect

    Son, Dong Hee; Wittenberg, Joshua S.; Banin, Uri; Alivisatos, A.Paul

    2006-03-30

    The photo-induced enhancement of second harmonic generation, and the effect of nanocrystal shape and pump intensity on confined acoustic phonons in semiconductor nanocrystals, has been investigated with time-resolved scattering and absorption measurements. The second harmonic signal showed a sublinear increase of the second order susceptibility with respect to the pump pulse energy, indicating a reduction of the effective one-electron second-order nonlinearity with increasing electron-hole density in the nanocrystals. The coherent acoustic phonons in spherical and rod-shaped semiconductor nanocrystals were detected in a time-resolved absorption measurement. Both nanocrystal morphologies exhibited oscillatory modulation of the absorption cross section, the frequency of which corresponded to their coherent radial breathing modes. The amplitude of the oscillation also increased with the level of photoexcitation, suggesting an increase in the amplitude of the lattice displacement as well.

  7. Two-dimensional semiconductor nanocrystals: properties, templated formation, and magic-size nanocluster intermediates.

    PubMed

    Wang, Fudong; Wang, Yuanyuan; Liu, Yi-Hsin; Morrison, Paul J; Loomis, Richard A; Buhro, William E

    2015-01-20

    CONSPECTUS: Semiconductor nanocrystals having an extended length dimension and capable of efficiently transporting energy and charge would have useful applications in solar-energy conversion and other emerging technologies. Pseudocylindrical semiconductor nanowires and quantum wires are available that could potentially serve in this role. Sadly, however, their defective surfaces contain significant populations of surface trap sites that preclude efficient transport. The very large surface area of long wires is at least part of the problem. As electrons, holes, and excitons migrate along a nanowire or quantum wire, they are exposed to an extensive surface and to potentially large numbers of trap sites. A solution to this dilemma might be found by identifying "long" semiconductor nanocrystals of other morphologies that are better passivated. In this Account, we discuss a newly emerging family of flat semiconductor nanocrystals that have surprising characteristics. These thin, flat nanocrystals have up to micrometer-scale (orthogonal) lateral dimensions and thus very large surface areas. Even so, their typical photoluminescence efficiencies of 30% are astonishingly high and are 2 orders of magnitude higher than those typical of semiconductor quantum wires. The very sharp emission spectra of the pseudo-two-dimensional nanocrystals reflect a remarkable uniformity in their discrete thicknesses. Evidence that excitons are effectively delocalized and hence transported over the full dimensions of these nanocrystals has been obtained. The excellent optical properties of the flat semiconductor nanocrystals confirm that they are exceptionally well passivated. This Account summarizes the two synthetic methods that have been developed for the preparation of pseudo-two-dimensional semiconductor nanocrystals. A discussion of their structural features accounts for their discrete, uniform thicknesses and details the crystal-lattice expansions and contractions they exhibit. An

  8. Molecular Chemistry to the Fore: New Insights into the Fascinating World of Photoactive Colloidal Semiconductor Nanocrystals

    SciTech Connect

    Vela-Becerra, Javier

    2013-02-01

    Colloidal semiconductor nanocrystals possess unique properties that are unmatched by other chromophores such as organic dyes or transition-metal complexes. These versatile building blocks have generated much scientific interest and found applications in bioimaging, tracking, lighting, lasing, photovoltaics, photocatalysis, thermoelectrics, and spintronics. Despite these advances, important challenges remain, notably how to produce semiconductor nanostructures with predetermined architecture, how to produce metastable semiconductor nanostructures that are hard to isolate by conventional syntheses, and how to control the degree of surface loading or valence per nanocrystal. Molecular chemists are very familiar with these issues and can use their expertise to help solve these challenges. In this Perspective, we present our group’s recent work on bottom-up molecular control of nanoscale composition and morphology, low-temperature photochemical routes to semiconductor heterostructures and metastable phases, solar-to-chemical energy conversion with semiconductor-based photocatalysts, and controlled surface modification of colloidal semiconductors that bypasses ligand exchange.

  9. Structure-Dependent Spin Polarization in Polymorphic CdS:Y Semiconductor Nanocrystals.

    PubMed

    Wang, Pan; Xiao, Bingxin; Zhao, Rui; Ma, Yanzhang; Zhang, Mingzhe

    2016-03-01

    Searching for the polymorphic semiconductor nanocrystals would provide precise and insightful structure-spin polarization correlations and meaningful guidance for designing and synthesizing high spin-polarized spintronic materials. Herein, the high spin polarization is achieved in polymorphic CdS:Y semiconductor nanocrystals. The high-pressure polymorph of rock-salt CdS:Y nanocrystals has been recovered at ambient conditions synthesized by the wurtzite CdS:Y nanocrystals as starting material under 5.2 GPa and 300 °C conditions. The rock-salt CdS:Y polymorph displays more robust room-temperature ferromagnetism than wurtzite sample, which can reach the ferromagnetic level of conventional semiconductors doped with magnetic transition-metal ions, mainly due to the significantly enhanced spin configuration and defect states. Therefore, crystal structure directly governs the spin configuration, which determines the degree of spin polarization. This work can provide experimental and theoretical methods for designing the high spin-polarized semiconductor nanocrystals, which is important for applications in semiconductor spintronics. PMID:26905093

  10. Structure-Dependent Spin Polarization in Polymorphic CdS:Y Semiconductor Nanocrystals.

    PubMed

    Wang, Pan; Xiao, Bingxin; Zhao, Rui; Ma, Yanzhang; Zhang, Mingzhe

    2016-03-01

    Searching for the polymorphic semiconductor nanocrystals would provide precise and insightful structure-spin polarization correlations and meaningful guidance for designing and synthesizing high spin-polarized spintronic materials. Herein, the high spin polarization is achieved in polymorphic CdS:Y semiconductor nanocrystals. The high-pressure polymorph of rock-salt CdS:Y nanocrystals has been recovered at ambient conditions synthesized by the wurtzite CdS:Y nanocrystals as starting material under 5.2 GPa and 300 °C conditions. The rock-salt CdS:Y polymorph displays more robust room-temperature ferromagnetism than wurtzite sample, which can reach the ferromagnetic level of conventional semiconductors doped with magnetic transition-metal ions, mainly due to the significantly enhanced spin configuration and defect states. Therefore, crystal structure directly governs the spin configuration, which determines the degree of spin polarization. This work can provide experimental and theoretical methods for designing the high spin-polarized semiconductor nanocrystals, which is important for applications in semiconductor spintronics.

  11. Synthesis of Semiconductor Nanocrystals, Focusing on Nontoxic and Earth-Abundant Materials.

    PubMed

    Reiss, Peter; Carrière, Marie; Lincheneau, Christophe; Vaure, Louis; Tamang, Sudarsan

    2016-09-28

    We review the synthesis of semiconductor nanocrystals/colloidal quantum dots in organic solvents with special emphasis on earth-abundant and toxic heavy metal free compounds. Following the Introduction, section 2 defines the terms related to the toxicity of nanocrystals and gives a comprehensive overview on toxicity studies concerning all types of quantum dots. Section 3 aims at providing the reader with the basic concepts of nanocrystal synthesis. It starts with the concepts currently used to describe the nucleation and growth of monodisperse particles and next takes a closer look at the chemistry of the inorganic core and its interactions with surface ligands. Section 4 reviews in more detail the synthesis of different families of semiconductor nanocrystals, namely elemental group IV compounds (carbon nanodots, Si, Ge), III-V compounds (e.g., InP, InAs), and binary and multinary metal chalcogenides. Finally, the authors' view on the perspectives in this field is given. PMID:27391095

  12. Synthesis of Semiconductor Nanocrystals, Focusing on Nontoxic and Earth-Abundant Materials.

    PubMed

    Reiss, Peter; Carrière, Marie; Lincheneau, Christophe; Vaure, Louis; Tamang, Sudarsan

    2016-09-28

    We review the synthesis of semiconductor nanocrystals/colloidal quantum dots in organic solvents with special emphasis on earth-abundant and toxic heavy metal free compounds. Following the Introduction, section 2 defines the terms related to the toxicity of nanocrystals and gives a comprehensive overview on toxicity studies concerning all types of quantum dots. Section 3 aims at providing the reader with the basic concepts of nanocrystal synthesis. It starts with the concepts currently used to describe the nucleation and growth of monodisperse particles and next takes a closer look at the chemistry of the inorganic core and its interactions with surface ligands. Section 4 reviews in more detail the synthesis of different families of semiconductor nanocrystals, namely elemental group IV compounds (carbon nanodots, Si, Ge), III-V compounds (e.g., InP, InAs), and binary and multinary metal chalcogenides. Finally, the authors' view on the perspectives in this field is given.

  13. The role of confinement on the diffusion barriers in semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Chan, Tzu-Liang; Zayak, Alexey; Dalpian, Gustavo; Chelikowsky, James

    2009-03-01

    We find that quantum size effects not only play an important role in the electronic properties of defects in semiconductor nanocrystals, but also strongly affect the incorporation of defect atoms into the nanocrystals. In particular, using ab initio methods based on density functional theory, we predict that Mn defects will be energetically expelled to the surface of CdSe and ZnSe nanocrystals, and that the diffusion barrier of a Mn interstitial defect in a CdSe nanocrystal will be significantly lower than that in the bulk. This can be ascribed to the large surface to volume ratio of nanocrystals, which can effectively release the strain during diffusion. By calculating the vibrational spectrum of the CdSe nanocrystal, we estimated the diffusion rate within the nanocrystal. Our results suggest that energetics can play a role in the self purification of small CdSe and ZnSe nanocrystals, as diffusion of the defect atom can readily occur inside such small nanocrystals.

  14. Nanocrystal structures

    DOEpatents

    Eisler, Hans J.; Sundar, Vikram C.; Walsh, Michael E.; Klimov, Victor I.; Bawendi, Moungi G.; Smith, Henry I.

    2006-12-19

    A structure including a grating and a semiconductor nanocrystal layer on the grating, can be a laser. The semiconductor nanocrystal layer can include a plurality of semiconductor nanocrystals including a Group II–VI compound, the nanocrystals being distributed in a metal oxide matrix. The grating can have a periodicity from 200 nm to 500 nm.

  15. Nanocrystal structures

    SciTech Connect

    Eisler, Hans J.; Sundar, Vikram C.; Walsh, Michael E.; Klimov, Victor I.; Bawendi, Moungi G.; Smith, Henry I.

    2008-12-30

    A structure including a grating and a semiconductor nanocrystal layer on the grating, can be a laser. The semiconductor nanocrystal layer can include a plurality of semiconductor nanocrystals including a Group II-VI compound, the nanocrystals being distributed in a metal oxide matrix. The grating can have a periodicity from 200 nm to 500 nm.

  16. Hydrogen-Bonded Organic Semiconductor Micro- And Nanocrystals: From Colloidal Syntheses to (Opto-)Electronic Devices

    PubMed Central

    2014-01-01

    Organic pigments such as indigos, quinacridones, and phthalocyanines are widely produced industrially as colorants for everyday products as various as cosmetics and printing inks. Herein we introduce a general procedure to transform commercially available insoluble microcrystalline pigment powders into colloidal solutions of variously sized and shaped semiconductor micro- and nanocrystals. The synthesis is based on the transformation of the pigments into soluble dyes by introducing transient protecting groups on the secondary amine moieties, followed by controlled deprotection in solution. Three deprotection methods are demonstrated: thermal cleavage, acid-catalyzed deprotection, and amine-induced deprotection. During these processes, ligands are introduced to afford colloidal stability and to provide dedicated surface functionality and for size and shape control. The resulting micro- and nanocrystals exhibit a wide range of optical absorption and photoluminescence over spectral regions from the visible to the near-infrared. Due to excellent colloidal solubility offered by the ligands, the achieved organic nanocrystals are suitable for solution processing of (opto)electronic devices. As examples, phthalocyanine nanowire transistors as well as quinacridone nanocrystal photodetectors, with photoresponsivity values by far outperforming those of vacuum deposited reference samples, are demonstrated. The high responsivity is enabled by photoinduced charge transfer between the nanocrystals and the directly attached electron-accepting vitamin B2 ligands. The semiconducting nanocrystals described here offer a cheap, nontoxic, and environmentally friendly alternative to inorganic nanocrystals as well as a new paradigm for obtaining organic semiconductor materials from commercial colorants. PMID:25253644

  17. Characterization of CdSe-nanocrystals used in semiconductors for aerospace applications: Production and optical properties

    NASA Astrophysics Data System (ADS)

    Hegazy, Maroof A.; Abd El-Hameed, Afaf M.

    2014-06-01

    Semiconductor nanocrystals (NC’s) are the materials with dimensions less than 10 nm. When the dimensions of nanocrystals are reduced the bulk bohr diameter, the photo generated electron-hole pair becomes confined and nanocrystal exhibits size dependent upon optical properties. This work is focused on the studying of CdSe semiconductor nanocrystals. These nanocrystals are considered as one of the most widely studies semiconductors because of their size - tunable optical properties from the visible spectrum. CdSe-nanocrystals are produced and obtained throughout the experimental setup initiated at Nano-NRIAG Unit (NNU), which has been constructed and assembled at NRIAG institute. This unit has a specific characterization for preparing chemical compositions, which may be used for solar cell fabrications and space science technology. The materials prepared included cadmium oxide and selinid have sizes ranging between 2.27 nm and 3.75 nm. CdSe-nanocrystals are synthesized in “TOP/TOPO (tri-octyl phosphine/tri-octyl phosphine oxide). Diagnostic tools, include UV analysis, TEM microscope, and X-ray diffraction, which are considered for the analytical studies of the obtained materials. The results show that, in this size regime, the generated particles have unique optical properties, which is achieved from the UV analysis. Also, the TEM image analysis shows the size and shape of the produced particles. These studies are carried out to optimize the photoluminescent efficiency of these nanoparticles. Moreover, the data revealed that, the grain size of nanocrystals is dependent upon the growth time in turn, it leads to a change in the energy gap. Some applications of this class of materials are outlined.

  18. Multiple Exciton Generation in Semiconductor Nanocrystals: Toward Efficient Solar Energy Conversion

    SciTech Connect

    Beard, M. C.; Ellingson, R. J.

    2008-01-01

    Within the range of photon energies illuminating the Earth's surface, absorption of a photon by a conventional photovoltaic semiconductor device results in the production of a single electron-hole pair; energy of a photon in excess of the semiconductor's bandgap is efficiently converted to heat through interactions between the electron and hole with the crystal lattice. Recently, colloidal semiconductor nanocrystals and nanocrystal films have been shown to exhibit efficient multiple electron-hole pair generation from a single photon with energy greater than twice the effective band gap. This multiple carrier pair process, referred to as multiple exciton generation (MEG), represents one route to reducing the thermal loss in semiconductor solar cells and may lead to the development of low cost, high efficiency solar energy devices. We review the current experimental and theoretical understanding of MEG, and provide views to the near-term future for both fundamental research and the development of working devices which exploit MEG.

  19. Luminescence properties of II/VI semiconductor colloidal nanocrystals at collective and single scales

    NASA Astrophysics Data System (ADS)

    Vion, Céline; Barthou, Carlos; Coolen, Laurent; Bennaloul, Paul; Chinh, Vu Duc; Thuy Linh, Pham; Thi Bich, Vu; Thu Nga, Pham; Maître, Agnès

    2009-09-01

    Colloidal nanocrystals are crystalline spheres of semiconductors of a few nanometers, obtained by chemical synthesis. At this size scale, lower than Bohr radius of the exciton, emission properties are dominated by quantum confinement effects and depend crucially on the nanocrystal radius, which can be controlled by adjusting the synthesis parameters. Nanocrystals present high photostability and good quantum efficiency, even at room temperature. Their emission wavelength can be tuned over the whole visible range, making them very attractive solid state light sources which are already used in optoelectronic devices or for biological labeling. The luminescence properties of CdSe colloidal nanocrystals synthesized at the Institute of Materials Science in Hanoi are presented. At collective scale, the emission properties reveal the synthesis quality. Temperature effects from ambient to 4 K on spectra and decay rates will be presented and analyzed in terms of emitting level fine structure. The study of CdSe colloidal quantum dots at the single emitter scale is of great interest as it reveals properties which are hidden by collective studies, such as luminescence "blinking", a random switching from a fluorescent to a non fluorescent state, which is closely related to the crystalline defects of a nanocrystal and its interaction with its environment. We will present the blinking properties of the prepared nanocrystals, and relate them to the nanocrystals synthesis quality and shell quality.

  20. Optical properties of three-dimensional arrays of semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Kim, Bosang

    The major part of this thesis is devoted to interdot interactions in CdSe nanocrystal arrays at elevated pressure. Three-dimensional arrays of organically passivated CdSe nanocrystals were investigated under hydrostatic pressure using photoluminescence (PL) and absorption spectroscopies. Interdot separations were varied coarsely by varying the organic ligand on the nanocrystal and finely by applying hydrostatic pressure. The PL and absorption spectra of solutions and arrays of CdSe nanocrystals capped by tri-n-octylphosphine oxide (TOPO) or tri-n-butylphosphine oxide (TBPO) are the same up to 60 kbar. In contrast, there is a distinct difference between the pressure dependence of CdSe/pyridine dots in solution and arrays. This different dependence can be attributed to several factors, including possible carrier coupling between neighboring nanoparticles through the organic ligands capping the respective particles that would lead to a decrease in carrier confinement energy. The kinetics of solvent and organic ligand of CdSe nanocrystal arrays during the assembly were quantitatively investigated. Attenuated total reflection is shown to be a quantitative real-time probe of several important features of nanocrystal self-assembly by following the infrared absorption of the solvent and the organic ligands that passivate the nanocrystal surface. During the self-assembly of a 250 monolayer array of CdSe nanocrystals capped by pyridine, the pyridine solvent molecules evaporate in ˜30--40 min and the pyridine-capping molecules leave the array very slowly, apparently limited by diffusion, with ˜30 +/- 8% remaining after three days. The method of spin-assisted self-assembly was used to produce sub-micron thick films of CdSe nanocrystals. The uniformity was investigated with various spin rate and solvents; the films made from a hexane/octane mixture at a spin rate of 100 RPM with intermittent pauses resulted in the least fluctuations in film thickness. Using optical microscopy

  1. Conjugated polymers/semiconductor nanocrystals hybrid materials--preparation, electrical transport properties and applications.

    PubMed

    Reiss, Peter; Couderc, Elsa; De Girolamo, Julia; Pron, Adam

    2011-02-01

    This critical review discusses specific preparation and characterization methods applied to hybrid materials consisting of π-conjugated polymers (or oligomers) and semiconductor nanocrystals. These materials are of great importance in the quickly growing field of hybrid organic/inorganic electronics since they can serve as active components of photovoltaic cells, light emitting diodes, photodetectors and other devices. The electronic energy levels of the organic and inorganic components of the hybrid can be tuned individually and thin hybrid films can be processed using low cost solution based techniques. However, the interface between the hybrid components and the morphology of the hybrid directly influences the generation, separation and transport of charge carriers and those parameters are not easy to control. Therefore a large variety of different approaches for assembling the building blocks--conjugated polymers and semiconductor nanocrystals--has been developed. They range from their simple blending through various grafting procedures to methods exploiting specific non-covalent interactions between both components, induced by their tailor-made functionalization. In the first part of this review, we discuss the preparation of the building blocks (nanocrystals and polymers) and the strategies for their assembly into hybrid materials' thin films. In the second part, we focus on the charge carriers' generation and their transport within the hybrids. Finally, we summarize the performances of solar cells using conjugated polymer/semiconductor nanocrystals hybrids and give perspectives for future developments.

  2. Semiconductor nanocrystals covalently bound to solid inorganic surfaces using self-assembled monolayers

    DOEpatents

    Alivisatos, A. Paul; Colvin, Vicki L.

    1998-01-01

    Methods are described for attaching semiconductor nanocrystals to solid inorganic surfaces, using self-assembled bifunctional organic monolayers as bridge compounds. Two different techniques are presented. One relies on the formation of self-assembled monolayers on these surfaces. When exposed to solutions of nanocrystals, these bridge compounds bind the crystals and anchor them to the surface. The second technique attaches nanocrystals already coated with bridge compounds to the surfaces. Analyses indicate the presence of quantum confined clusters on the surfaces at the nanolayer level. These materials allow electron spectroscopies to be completed on condensed phase clusters, and represent a first step towards synthesis of an organized assembly of clusters. These new products are also disclosed.

  3. Semiconductor nanocrystals covalently bound to solid inorganic surfaces using self-assembled monolayers

    DOEpatents

    Alivisatos, A.P.; Colvin, V.L.

    1998-05-12

    Methods are described for attaching semiconductor nanocrystals to solid inorganic surfaces, using self-assembled bifunctional organic monolayers as bridge compounds. Two different techniques are presented. One relies on the formation of self-assembled monolayers on these surfaces. When exposed to solutions of nanocrystals, these bridge compounds bind the crystals and anchor them to the surface. The second technique attaches nanocrystals already coated with bridge compounds to the surfaces. Analyses indicate the presence of quantum confined clusters on the surfaces at the nanolayer level. These materials allow electron spectroscopies to be completed on condensed phase clusters, and represent a first step towards synthesis of an organized assembly of clusters. These new products are also disclosed. 10 figs.

  4. Can Tauc plot extrapolation be used for direct-band-gap semiconductor nanocrystals?

    SciTech Connect

    Feng, Y. Lin, S.; Huang, S.; Shrestha, S.; Conibeer, G.

    2015-03-28

    Despite that Tauc plot extrapolation has been widely adopted for extracting bandgap energies of semiconductors, there is a lack of theoretical support for applying it to nanocrystals. In this paper, direct-allowed optical transitions in semiconductor nanocrystals have been formulated based on a purely theoretical approach. This result reveals a size-dependant transition of the power factor used in Tauc plot, increasing from one half used in the 3D bulk case to one in the 0D case. This size-dependant intermediate value of power factor allows a better extrapolation of measured absorption data. Being a material characterization technique, the generalized Tauc extrapolation gives a more reasonable and accurate acquisition of the intrinsic bandgap, while the unjustified purpose of extrapolating any elevated bandgap caused by quantum confinement is shown to be incorrect.

  5. Improving the catalytic activity of semiconductor nanocrystals through selective domain etching.

    PubMed

    Khon, Elena; Lambright, Kelly; Khnayzer, Rony S; Moroz, Pavel; Perera, Dimuthu; Butaeva, Evgeniia; Lambright, Scott; Castellano, Felix N; Zamkov, Mikhail

    2013-05-01

    Colloidal chemistry offers an assortment of synthetic tools for tuning the shape of semiconductor nanocrystals. While many nanocrystal architectures can be obtained directly via colloidal growth, other nanoparticle morphologies require alternative processing strategies. Here, we show that chemical etching of colloidal nanoparticles can facilitate the realization of nanocrystal shapes that are topologically inaccessible by hot-injection techniques alone. The present methodology is demonstrated by synthesizing a two-component CdSe/CdS nanoparticle dimer, constructed in a way that both CdSe and CdS semiconductor domains are exposed to the external environment. This structural morphology is highly desirable for catalytic applications as it enables both reductive and oxidative reactions to occur simultaneously on dissimilar nanoparticle surfaces. Hydrogen production tests confirmed the improved catalytic activity of CdSe/CdS dimers, which was enhanced 3-4 times upon etching treatment. We expect that the demonstrated application of etching to shaping of colloidal heteronanocrystals can become a common methodology in the synthesis of charge-separating nanocrystals, leading to advanced nanoparticles architectures for applications in areas of photocatalysis, photovoltaics, and light detection.

  6. Photophysical Properties of II-VI Semiconductor Nanocrystals

    NASA Astrophysics Data System (ADS)

    Gong, Ke

    As it is well known, semiconductor nanocrystals (also called quantum dots, QDs) are being actively pursued for use in many different types of luminescent optical materials. These materials include the active media for luminescence downconversion in artificial lighting, lasers, luminescent solar concentrators and many other applications. Chapter 1 gives general introduction of QDs, which describe the basic physical properties and optical properties. Based on the experimental spectroscopic study, a semiquantitative method-effective mass model is employed to give theoretical prediction and guide. The following chapters will talks about several topics respectively. A predictive understanding of the radiative lifetimes is therefore a starting point for the understanding of the use of QDs for these applications. Absorption intensities and radiative lifetimes are fundamental properties of any luminescent material. Meantime, achievement of high efficiency with high working temperature and heterostructure fabrication with manipulation of lattice strain are not easy and need systematic investigation. To make accurate connections between extinction coefficients and radiative recombination rates, chapter 2 will consider three closely related aspects of the size dependent spectroscopy of II-VI QDs. First, it will consider the existing literature on cadmium selenide (CdSe) QD absorption spectra and extinction coefficients. From these results and fine structure considerations Boltzmann weighted radiative lifetimes are calculated. These lifetimes are compared to values measured on very high quality CdSe and CdSe coated with zinc selenide (ZnSe) shells. Second, analogous literature data are analyzed for cadmium telluride (CdTe) nanocrystals and compared to lifetimes measured for very high quality QDs. Furthermore, studies of the absorption and excitation spectra and measured radiative lifetimes for CdTe/CdSe Type-II core/shell QDs are reported. These results are also analyzed in

  7. Energy-transfer pumping of semiconductor nanocrystals using an epitaxial quantum well

    NASA Astrophysics Data System (ADS)

    Achermann, Marc; Petruska, Melissa A.; Kos, Simon; Smith, Darryl L.; Koleske, Daniel D.; Klimov, Victor I.

    2004-06-01

    As a result of quantum-confinement effects, the emission colour of semiconductor nanocrystals can be modified dramatically by simply changing their size. Such spectral tunability, together with large photoluminescence quantum yields and high photostability, make nanocrystals attractive for use in a variety of light-emitting technologies-for example, displays, fluorescence tagging, solid-state lighting and lasers. An important limitation for such applications, however, is the difficulty of achieving electrical pumping, largely due to the presence of an insulating organic capping layer on the nanocrystals. Here, we describe an approach for indirect injection of electron-hole pairs (the electron-hole radiative recombination gives rise to light emission) into nanocrystals by non-contact, non-radiative energy transfer from a proximal quantum well that can in principle be pumped either electrically or optically. Our theoretical and experimental results indicate that this transfer is fast enough to compete with electron-hole recombination in the quantum well, and results in greater than 50 per cent energy-transfer efficiencies in the tested structures. Furthermore, the measured energy-transfer rates are sufficiently large to provide pumping in the stimulated emission regime, indicating the feasibility of nanocrystal-based optical amplifiers and lasers based on this approach.

  8. Confined optical modes in small photonic molecules with semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Rakovich, Yu. P.; Gerlach, M.; Bradley, A. L.; Donegan, J. F.; Connolly, T. M.; Boland, J. J.; Przyjalgowski, M. A.; Ryder, A.; Gaponik, N.; Rogach, A. L.

    2004-12-01

    We report on the coherent coupling of whispering gallery modes (WGMs) in a photonic molecule formed from two melamine-formaldehyde spherical microcavities coated with a thin shell of light-emitting CdTe nanocrystals (NCs). Utilizing different excitation conditions, the splitting of the WGM resonances originating from bonding and antibonding branches of the photonic states is observed, and fine structure consisting of very sharp peaks resulting from lifting of the WGM degeneracy has been detected. Time-resolved measurements showed a slight increase in the spontaneous emission rate of NCs in a photonic molecule when compared to the spontaneous emission rate for NCs coating a single microsphere.

  9. Spontaneous emission from semiconductor nanocrystals in coupled spherical microcavities

    NASA Astrophysics Data System (ADS)

    Rakovich, Yu. P.; Gerlach, M.; Bradley, A. L.; Donegan, J. F.; Boland, J.; Connolly, T.; Przyjalgowski, M.; Ryder, A.; Gaponik, N.; Rogach, A. L.

    2005-02-01

    We report on the coherent coupling of whispering gallery modes (WGM) in a photonic molecule formed from two melamine-formaldehyde spherical microcavities coated with a thin shell of light-emitting CdTe nanocrystals (NCs). Utilizing different excitation conditions the splitting of the WGM resonances originating from bonding and anti-bonding branches of the photonic states is observed and fine structure consisting of very sharp peaks resulting from lifting of the WGM degeneracy has been detected. Time-resolved measurements showed a slight increase in the spontaneous emission rate of NCs in a photonic molecule when compared to the spontaneous emission rate for NCs coating a single microsphere.

  10. Electroluminescent devices formed using semiconductor nanocrystals as an electron transport media and method of making such electroluminescent devices

    DOEpatents

    Alivisatos, A. Paul; Colvin, Vickie

    1996-01-01

    An electroluminescent device is described, as well as a method of making same, wherein the device is characterized by a semiconductor nanocrystal electron transport layer capable of emitting visible light in response to a voltage applied to the device. The wavelength of the light emitted by the device may be changed by changing either the size or the type of semiconductor nanocrystals used in forming the electron transport layer. In a preferred embodiment the device is further characterized by the capability of emitting visible light of varying wavelengths in response to changes in the voltage applied to the device. The device comprises a hole processing structure capable of injecting and transporting holes, and usually comprising a hole injecting layer and a hole transporting layer; an electron transport layer in contact with the hole processing structure and comprising one or more layers of semiconductor nanocrystals; and an electron injecting layer in contact with the electron transport layer for injecting electrons into the electron transport layer. The capability of emitting visible light of various wavelengths is principally based on the variations in voltage applied thereto, but the type of semiconductor nanocrystals used and the size of the semiconductor nanocrystals in the layers of semiconductor nanometer crystals may also play a role in color change, in combination with the change in voltage.

  11. Enhanced Semiconductor Nanocrystal Conductance via Solution Grown Contacts

    SciTech Connect

    Sheldon, Matthew T.; Trudeau, Paul-Emile; Mokari, Taleb; Wang, Lin-Wang; Alivisatos, A. Paul

    2009-08-19

    We report a 100,000-fold increase in the conductance of individual CdSe nanorods when they are electrically contacted via direct solution phase growth of Au tips on the nanorod ends. Ensemble UV-Vis and X-Ray photoelectron spectroscopy indicate this enhancement does not result from alloying of the nanorod. Rather, low temperature tunneling and high temperature (250-400 K) thermionic emission across the junction at the Au contact reveal a 75percent lower interface barrier to conduction compared to a control sample. We correlate this barrier lowering with the electronic structure at the Au-CdSe interface. Our results emphasize the importance of nanocrystal surface structure for robust device performance and the advantage of this contact method.

  12. Charged two-exciton emission from a single semiconductor nanocrystal

    SciTech Connect

    Hu, Fengrui; Zhang, Qiang; Zhang, Chunfeng; Wang, Xiaoyong; Xiao, Min

    2015-03-30

    Here, we study the photoluminescence (PL) time trajectories of single CdSe/ZnS nanocrystals (NCs) as a function of the laser excitation power. At the low laser power, the PL intensity of a single NC switches between the “on” and “off” levels arising from the neutral and positively charged single excitons, respectively. With the increasing laser power, an intermediate “grey” level is formed due to the optical emission from a charged multiexciton state composed of two excitons and an extra electron. Both the inter-photon correlation and the PL decay measurements demonstrate that lifetime-indistinguishable photon pairs are emitted from this negatively charged two-exciton state.

  13. Active photonic devices based on colloidal semiconductor nanocrystals and organometallic halide perovskites

    NASA Astrophysics Data System (ADS)

    Suárez Alvarez, Isaac

    2016-10-01

    Semiconductor nanocrystals have arisen as outstanding materials to develop a new generation of optoelectronic devices. Their fabrication under simple and low cost colloidal chemistry methods results in cheap nanostructures able to provide a wide range of optical functionalities. Their attractive optical properties include a high absorption cross section below the band gap, a high quantum yield emission at room temperature, or the capability of tuning the band-gap with the size or the base material. In addition, their solution process nature enables an easy integration on several substrates and photonic structures. As a consequence, these nanoparticles have been extensively proposed to develop several photonic applications, such as detection of light, optical gain, generation of light or sensing. This manuscript reviews the great effort undertaken by the scientific community to construct active photonic devices based on these nanoparticles. The conditions to demonstrate stimulated emission are carefully studied by comparing the dependence of the optical properties of the nanocrystals with their size, shape and composition. In addition, this paper describes the design of different photonic architectures (waveguides and cavities) to enhance the generation of photoluminescence, and hence to reduce the threshold of optical gain. Finally, semiconductor nanocrystals are compared to organometallic halide perovskites, as this novel material has emerged as an alternative to colloidal nanoparticles.

  14. Low-dimensional semiconductor superlattices formed by geometric control over nanocrystal attachment.

    PubMed

    Evers, Wiel H; Goris, Bart; Bals, Sara; Casavola, Marianna; de Graaf, Joost; van Roij, René; Dijkstra, Marjolein; Vanmaekelbergh, Daniël

    2013-06-12

    Oriented attachment, the process in which nanometer-sized crystals fuse by atomic bonding of specific crystal facets, is expected to be more difficult to control than nanocrystal self-assembly that is driven by entropic factors or weak van der Waals attractions. Here, we present a study of oriented attachment of PbSe nanocrystals that counteract this tuition. The reaction was studied in a thin film of the suspension casted on an immiscible liquid at a given temperature. We report that attachment can be controlled such that it occurs with one type of facets exclusively. By control of the temperature and particle concentration we obtain one- or two-dimensional PbSe single crystals, the latter with a honeycomb or square superimposed periodicity in the nanometer range. We demonstrate the ability to convert these PbSe superstructures into other semiconductor compounds with the preservation of crystallinity and geometry.

  15. Universal size dependence of auger constants in direct- and indirect-gap semiconductor nanocrystals

    SciTech Connect

    Robel, Istvan; Schaller, Richard D; Klimov, Victor I; Gresback, Ryan; Kortshagen, Uwe

    2008-01-01

    Three-dimensional (3D) spatial confinement of electronic wave functions in semiconductor nanocrystals (NCs) results in a significant enhancement of multi-electron phenomena including non radiative Auger recombination. In this process, a conduction-band electron recombines with a valence-band hole by transferring the recombination energy to a third carrier. Significant interest in Auger recombination in NCs has been stimulated by recent studies ofNC lasing, and generation-III photovoltaics enabled by carrier multiplication because in both of these prospective applications Auger recombination represents a dominant carrier-loss mechanism. Here, we perform a side-by-side comparison of Auger recombination rates in NCs of several different compositions including Ge, PbSe, InAs, and CdSe. We observe that the only factor, which has a significant effect on the measured recombination rates, is the size of the NCs but not the details of the material's electronic structure. Most surprisingly, comparable rates are measured for nanocrystals of directand indirect-gap semiconductor NCs despite a dramatic four-to-five orders of magnitude difference in respective bulk-semiconductor Auger constants. This unusual observation can be explained by confinement-induced relaxation of momentum conservation, which smears out the difference between direct- and indirect-gap materials.

  16. A facile and green preparation of high-quality CdTe semiconductor nanocrystals at room temperature

    NASA Astrophysics Data System (ADS)

    Liu, Yan; Shen, Qihui; Yu, Dongdong; Shi, Weiguang; Li, Jixue; Zhou, Jianguang; Liu, Xiaoyang

    2008-06-01

    One chemical reagent, hydrazine hydrate, was discovered to accelerate the growth of semiconductor nanocrystals (cadmium telluride) instead of additional energy, which was applied to the synthesis of high-quality CdTe nanocrystals at room temperature and ambient conditions within several hours. Under this mild condition the mercapto stabilizers were not destroyed, and they guaranteed CdTe nanocrystal particle sizes with narrow and uniform distribution over the largest possible range. The CdTe nanocrystals (photoluminescence emission range of 530-660 nm) synthesized in this way had very good spectral properties; for instance, they showed high photoluminescence quantum yield of up to 60%. Furthermore, we have succeeded in detecting the living Borrelia burgdorferi of Lyme disease by its photoluminescence image using CdTe nanocrystals.

  17. Hybrid Solar Cells with Prescribed Nanoscale Morphologies Based onHyperbranched Semiconductor Nanocrystals

    SciTech Connect

    Gur, Ilan; Fromer, Neil A.; Chen, Chih-Ping; Kanaras, AntoniosG.; Alivisatos, A. Paul

    2006-09-09

    In recent years, the search to develop large-area solar cells at low cost has led to research on photovoltaic (PV) systems based on nanocomposites containing conjugated polymers. These composite films can be synthesized and processed at lower costs and with greater versatility than the solid state inorganic semiconductors that comprise today's solar cells. However, the best nanocomposite solar cells are based on a complex architecture, consisting of a fine blend of interpenetrating and percolating donor and acceptor materials. Cell performance is strongly dependent on blend morphology, and solution-based fabrication techniques often result in uncontrolled and irreproducible blends, whose composite morphologies are difficult to characterize accurately. Here we incorporate 3-dimensional hyper-branched colloidal semiconductor nanocrystals in solution-processed hybrid organic-inorganic solar cells, yielding reproducible and controlled nanoscale morphology.

  18. Design of metal/dielectric/nanocrystals core/shell/shell nano-structures for the fluorescence enhancement of cadmium-free semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Chevallier, Théo.; Le Blevennec, Gilles; Chandezon, Frédéric

    2015-10-01

    AgInS2-ZnS (ZAIS) quaternary semiconductors nanocrystals are versatile cadmium-free luminescent nanomaterials. Their broad emission spectrum and strong absorption make them ideal for the development of new white-LED devices taking advantage of nano-optical phenomena. We recently found strategies to increase the photoluminescence quantum yield of ZAIS nanocrystals up to 80%. In a second step toward high efficiency luminescent materials, we aim at increasing the net conversion efficiency of ZAIS nanocrystals by coupling them with metallic nano-antennae. Indeed, by grafting ZAIS nanocrystals onto carefully chosen metal/dielectric core/shell nanoparticles, both the absorption and emission processes can be tuned and enhanced. A finite-element simulation based on the discrete dipole approximation (DDA) was used to predict the nano-optical behavior of silver@oxide@ZAIS nanostructures. Desirable combinations of materials and geometry for the antennae were identified. A chemical method for the synthesis of the simulated nanostructures was developed. The coupling of ZAIS nanocrystals emission with the plasmonic structure is experimentally observed and is in accordance with our predictions.

  19. Size-dependent ligand layer dynamics in semiconductor nanocrystals probed by anisotropy measurements.

    PubMed

    Hadar, Ido; Abir, Tsafrir; Halivni, Shira; Faust, Adam; Banin, Uri

    2015-10-12

    Colloidal semiconductor nanocrystals (NC) have reached a high level of synthetic control allowing the tuning of their properties, and their use in various applications. However, the surface of NCs and in particular their size-dependent capping organic ligand behavior, which play an important role in the NC synthesis, dispersibility, and optoelectronic properties, is still not well understood. We study the size-dependent properties of the ligand shell on the surface of NCs, by embedding surface bound dyes as a probe within the ligand shell. The reorientation times for these dyes show a linear dependence on the NC surface curvature indicating size-dependent change in viscosity, which is related to a change in the density of the ligand layer because of the geometry of the surface, a unique feature of NCs. Understanding the properties of the ligand shell will allow rational design of the surface to achieve the desired properties, providing an additional important knob for tuning their functionality.

  20. Extended storage of multiple excitons in trap states of semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Xu, Qinfeng; Huang, Xiangnan; Hua, Zheng; Hu, Lian; Du, Lingxiao; Wu, Huizhen; Zhang, Chunfeng; Wang, Xiaoyong; Xiao, Min

    2016-02-01

    Owing to the Auger recombination effect, multiple excitons (MEs) in semiconductor nanocrystals (NCs) are dissipated nonradiatively at the sub-nanosecond time scale, which sets a stringent limit on the time window within which one can operate with them. Here, we show that this issue can be resolved by utilizing an intrinsic energy transfer system in CdSe NCs, where MEs created in the donor quantized states can be effectively extracted to the acceptor trap states. This was evidenced by the step-like increase in the intensity and the apparent decrease in the rise time of the trap-state photoluminescence with the elevated laser excitation power. With the radiative lifetime being tens of nanoseconds for the trap states, extended storage of MEs has been achieved and marks a crucial step towards flexible manipulations of their optoelectronic properties.

  1. The More Exotic Shapes of Semiconductor Nanocrystals: Emerging Applications in Bioimaging.

    PubMed

    Lim, Sung Jun; Smith, Andrew; Nie, Shuming

    2014-05-01

    Semiconductor nanocrystals are tiny fluorescent particles that have recently made a major impact in the biological and medical sciences by enabling high-sensitivity imaging of biomolecules, cells, and tissues. Spherical quantum dots are the prototypical material for these applications but recent synthetic advances have led to a diverse range of nanostructures with controllable sizes, shapes, and materials combinations that offer new dimensions of optical and structural tunability. Uniform anisotropic shapes with linearly polarized light emission allow optical imaging of particle orientation, planar structures have large flexible surfaces and ultra-narrow electronic transitions, and compact nanoparticles have enhanced diffusion in crowded biological environments. These properties are providing unique opportunities to probe basic biological processes, cellular structures, and organismal physiology. PMID:24982823

  2. General low-temperature reaction pathway from precursors to monomers before nucleation of compound semiconductor nanocrystals

    PubMed Central

    Yu, Kui; Liu, Xiangyang; Qi, Ting; Yang, Huaqing; Whitfield, Dennis M.; Y. Chen, Queena; Huisman, Erik J. C.; Hu, Changwei

    2016-01-01

    Little is known about the molecular pathway to monomers of semiconductor nanocrystals. Here we report a general reaction pathway, which is based on hydrogen-mediated ligand loss for the precursor conversion to ‘monomers' at low temperature before nucleation. We apply 31P nuclear magnetic resonance spectroscopy to monitor the key phosphorous-containing products that evolve from MXn+E=PPh2H+HY mixtures, where MXn, E=PPh2H, and HY are metal precursors, chalcogenide precursors, and additives, respectively. Surprisingly, the phosphorous-containing products detected can be categorized into two groups, Ph2P–Y and Ph2P(E)–Y. On the basis of our experimental and theoretical results, we propose two competing pathways to the formation of M2En monomers, each of which is accompanied by one of the two products. Our study unravels the pathway of precursor evolution into M2En monomers, the stoichiometry of which directly correlates with the atomic composition of the final compound nanocrystals. PMID:27531507

  3. Charge Blinking Statistics of Semiconductor Nanocrystals Revealed by Carbon Nanotube Single Charge Sensors.

    PubMed

    Zbydniewska, Ewa; Duzynska, Anna; Popoff, Michka; Hourlier, Djamila; Lenfant, Stéphane; Judek, Jaroslaw; Zdrojek, Mariusz; Mélin, Thierry

    2015-10-14

    We demonstrate the relation between the optical blinking of colloidal semiconductor nanocrystals (NCs) and their electrical charge blinking for which we provide the first experimental observation of power-law statistics. To show this, we harness the performance of CdSe/ZnS NCs coupled with carbon nanotube field-effect transistors (CNTFETs), which act as single charge-sensitive electrometers with submillisecond time resolution, at room temperature. A random telegraph signal (RTS) associated with the NC single-trap charging is observed and exhibits power-law temporal statistics (τ(-α), with α in the range of ∼1-3), and a Lorentzian current noise power spectrum with a well-defined 1/f(2) corner. The spectroscopic analysis of the NC-CNTFET devices is consistent with the charging of NC defect states with a charging energy of Ec ≥ 200 meV. These results pave the way for a deeper understanding of the physics and technology of nanocrystal-based optoelectronic devices.

  4. General low-temperature reaction pathway from precursors to monomers before nucleation of compound semiconductor nanocrystals.

    PubMed

    Yu, Kui; Liu, Xiangyang; Qi, Ting; Yang, Huaqing; Whitfield, Dennis M; Y Chen, Queena; Huisman, Erik J C; Hu, Changwei

    2016-01-01

    Little is known about the molecular pathway to monomers of semiconductor nanocrystals. Here we report a general reaction pathway, which is based on hydrogen-mediated ligand loss for the precursor conversion to 'monomers' at low temperature before nucleation. We apply (31)P nuclear magnetic resonance spectroscopy to monitor the key phosphorous-containing products that evolve from MXn+E=PPh2H+HY mixtures, where MXn, E=PPh2H, and HY are metal precursors, chalcogenide precursors, and additives, respectively. Surprisingly, the phosphorous-containing products detected can be categorized into two groups, Ph2P-Y and Ph2P(E)-Y. On the basis of our experimental and theoretical results, we propose two competing pathways to the formation of M2En monomers, each of which is accompanied by one of the two products. Our study unravels the pathway of precursor evolution into M2En monomers, the stoichiometry of which directly correlates with the atomic composition of the final compound nanocrystals. PMID:27531507

  5. Semiconductor nanocrystal-aptamer bioconjugate probes for specific prostate carcinoma cell targeting

    NASA Astrophysics Data System (ADS)

    Shieh, Felice; Lavery, Laura; Chu, Chitai T.; Richards-Kortum, Rebecca; Ellington, Andrew D.; Korgel, Brian A.

    2005-04-01

    Cancer of the prostate affects approximately 1 in 11 men. Current early screening for prostate cancer utilizes digital rectal examinations to detect anomalies in the prostate gland and blood test screenings for upregulated levels of prostate specific antigen (PSA). Many of these tests are invasive and can often be inconclusive as PSA levels may be heightened due to benign factors. Prostate specific membrane antigen (PSMA), a well-characterized integral membrane protein, is expressed in virtually all prostate cancers and often correlates with cancer aggressiveness. Therefore, it may be used as an indicator of cancer growth and metastases. PSMA-specific antibodies have been identified and conjugated to fluorescent markers for cancer cell targeting; however, both the antibodies and markers possess significant limitations in their pharmaceutical and diagnostic value. Here we report the use of semiconductor nanocrystals bioconjugated to PSMA-specific aptamer recognition molecules for prostate carcinoma cell targeting. The nanocrystal/aptamer bioconjugates are small biocompatible probes with the potential for color-tunability for multicolor imaging. Ongoing in vitro and in vivo research seeks to introduce these nanoparticle bioconjugates into medical diagnostics.

  6. Measurement of accumulation of semiconductor nanocrystal quantum dots by pimephales promelas.

    PubMed

    Leigh, Kenton L; Bouldin, Jennifer L; Buchanan, Roger A

    2012-01-01

    As the production and use of nanomaterials increases, it is important to understand their environmental and biological fate. Because their unmatched chemical, physical, and optical properties make them useful in a wide variety of applications including biomedical imaging, photo-voltaics, and light emitting diodes, the use of semiconductor nanocrystals such as quantum dots (QDs) is increasing rapidly. Although QDs hold great potential in a wide variety of industrial and consumer applications, the environmental implications of these particles is largely unexplored. The nanocrystal core of many types of QDs contains the toxic metal cadmium (Cd), so possible release of Cd from the QD core is cause for concern. Because many types of QDs are miscible in water, QD interactions with aquatic organisms and their environment require more attention. In the present study we used fluorometry to measure time and dose dependent uptake, accumulation, and post-exposure clearance of accumulated QDs in the gut tract by the aquatic vertebrate Pimephales promelas. By using fluorometry, we were able to measure accumulated QD concentrations. To our knowledge, this is the first reported attempt to quantify accumulated QDs in an organism and is an important step in understanding the interactions among QDs in aquatic organisms and environments. PMID:22942867

  7. General low-temperature reaction pathway from precursors to monomers before nucleation of compound semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Yu, Kui; Liu, Xiangyang; Qi, Ting; Yang, Huaqing; Whitfield, Dennis M.; Y. Chen, Queena; Huisman, Erik J. C.; Hu, Changwei

    2016-08-01

    Little is known about the molecular pathway to monomers of semiconductor nanocrystals. Here we report a general reaction pathway, which is based on hydrogen-mediated ligand loss for the precursor conversion to `monomers' at low temperature before nucleation. We apply 31P nuclear magnetic resonance spectroscopy to monitor the key phosphorous-containing products that evolve from MXn+E=PPh2H+HY mixtures, where MXn, E=PPh2H, and HY are metal precursors, chalcogenide precursors, and additives, respectively. Surprisingly, the phosphorous-containing products detected can be categorized into two groups, Ph2P-Y and Ph2P(E)-Y. On the basis of our experimental and theoretical results, we propose two competing pathways to the formation of M2En monomers, each of which is accompanied by one of the two products. Our study unravels the pathway of precursor evolution into M2En monomers, the stoichiometry of which directly correlates with the atomic composition of the final compound nanocrystals.

  8. Charge Blinking Statistics of Semiconductor Nanocrystals Revealed by Carbon Nanotube Single Charge Sensors.

    PubMed

    Zbydniewska, Ewa; Duzynska, Anna; Popoff, Michka; Hourlier, Djamila; Lenfant, Stéphane; Judek, Jaroslaw; Zdrojek, Mariusz; Mélin, Thierry

    2015-10-14

    We demonstrate the relation between the optical blinking of colloidal semiconductor nanocrystals (NCs) and their electrical charge blinking for which we provide the first experimental observation of power-law statistics. To show this, we harness the performance of CdSe/ZnS NCs coupled with carbon nanotube field-effect transistors (CNTFETs), which act as single charge-sensitive electrometers with submillisecond time resolution, at room temperature. A random telegraph signal (RTS) associated with the NC single-trap charging is observed and exhibits power-law temporal statistics (τ(-α), with α in the range of ∼1-3), and a Lorentzian current noise power spectrum with a well-defined 1/f(2) corner. The spectroscopic analysis of the NC-CNTFET devices is consistent with the charging of NC defect states with a charging energy of Ec ≥ 200 meV. These results pave the way for a deeper understanding of the physics and technology of nanocrystal-based optoelectronic devices. PMID:26418364

  9. Direct measurement of lattice dynamics and optical phonon excitation in semiconductor nanocrystals using femtosecond stimulated Raman spectroscopy.

    PubMed

    Hannah, Daniel C; Brown, Kristen E; Young, Ryan M; Wasielewski, Michael R; Schatz, George C; Co, Dick T; Schaller, Richard D

    2013-09-01

    We report femtosecond stimulated Raman spectroscopy measurements of lattice dynamics in semiconductor nanocrystals and characterize longitudinal optical (LO) phonon production during confinement-enhanced, ultrafast intraband relaxation. Stimulated Raman signals from unexcited CdSe nanocrystals produce a spectral shape similar to spontaneous Raman signals. Upon photoexcitation, stimulated Raman amplitude decreases owing to experimentally resolved ultrafast phonon generation rates within the lattice. We find a ∼600  fs, particle-size-independent depletion time attributed to hole cooling, evidence of LO-to-acoustic down-conversion, and LO phonon mode softening. PMID:25166708

  10. Bioactivation and cell targeting of semiconductor CdSe/ZnS nanocrystals with phytochelatin-related peptides.

    PubMed

    Pinaud, Fabien; King, David; Moore, Hsiao-Ping; Weiss, Shimon

    2004-05-19

    Synthetic phytochelatin-related peptides are used as an organic coat on the surface of colloidal CdSe/ZnS semiconductor nanocrystals synthesized from hydrophobic coordinating trioctyl phosphine oxide (TOPO) solvents. The peptides are designed to bind to the nanocrystals via a C-terminal adhesive domain. This adhesive domain, composed of multiple repeats of cysteines pairs flanked by hydrophobic 3-cyclohexylalanines, is followed by a flexible hydrophilic linker domain to which various bio-affinity tags can be attached. This surface coating chemistry results in small, buffer soluble, monodisperse peptide-coated nanoparticles with high colloidal stability and ensemble photophysical properties similar to those of TOPO-coated nanocrystals. Various peptide coatings are used to modulate the nanocrystal surface properties and to bioactivate the nanoparticles. CdSe/ZnS nanocrystals coated with biotinylated peptides efficiently bind to streptavidin and are specifically targeted to GPI-anchored avidin-CD14 chimeric proteins expressed on the membranes of live HeLa cells. This peptide coating surface chemistry provides a novel approach for the production of biocompatible photoluminescent nanocrystal probes. PMID:15137777

  11. Bioinspired solar water splitting, sensitized solar cells, and ultraviolet sensor based on semiconductor nanocrystal antenna/graphene nanoassemblies

    NASA Astrophysics Data System (ADS)

    Chang, Haixin; Lv, Xiaojun; Zheng, Zijian; Wu, Hongkai

    2011-11-01

    Graphene, two-dimensional carbon crystal with only one atom thickness, provides a general platform for nanoscale even atomic scale optoelectronics and photonics. Graphene has many advantages for optoelectronics such as high conductivity, high electronic mobility, flexibility and transparency. However, graphene also has disadvantages such as low light absorption which are unfavorable for optoelectronic devices. On the other hand, many natural photonic systems provide wonderful solution to enhance light absorption for solar energy harvesting and conversion, such as chlorophyll in green plants. Herein, learning from nature, we described bioinspired photocatalytic solar-driven water splitting, sensitized solar cells and ultraviolet optoelectronic sensors enabled by introducing photosensitive semiconductor nanocrystal antenna to graphene for constructing a series of graphene/nanocrystal nanoassemblies. We have demonstrated that high performance optoelectronic devices can come true with the introducing of photosensitive nanocrystal antenna elements.

  12. Bioinspired solar water splitting, sensitized solar cells, and ultraviolet sensor based on semiconductor nanocrystal antenna/graphene nanoassemblies

    NASA Astrophysics Data System (ADS)

    Chang, Haixin; Lv, Xiaojun; Zheng, Zijian; Wu, Hongkai

    2012-02-01

    Graphene, two-dimensional carbon crystal with only one atom thickness, provides a general platform for nanoscale even atomic scale optoelectronics and photonics. Graphene has many advantages for optoelectronics such as high conductivity, high electronic mobility, flexibility and transparency. However, graphene also has disadvantages such as low light absorption which are unfavorable for optoelectronic devices. On the other hand, many natural photonic systems provide wonderful solution to enhance light absorption for solar energy harvesting and conversion, such as chlorophyll in green plants. Herein, learning from nature, we described bioinspired photocatalytic solar-driven water splitting, sensitized solar cells and ultraviolet optoelectronic sensors enabled by introducing photosensitive semiconductor nanocrystal antenna to graphene for constructing a series of graphene/nanocrystal nanoassemblies. We have demonstrated that high performance optoelectronic devices can come true with the introducing of photosensitive nanocrystal antenna elements.

  13. Challenge to the Charging Model of Semiconductor-Nanocrystal Fluorescence Intermittency from Off-State Quantum Yields and Multiexciton Blinking

    SciTech Connect

    Zhao, Jing; Nair, Gautham; Fisher, Brent R.; Bawendi, Moungi G.

    2010-04-16

    Semiconductor nanocrystals emit light intermittently; i.e., they “blink,” under steady illumination. The dark periods have been widely assumed to be due to photoluminescence (PL) quenching by an Auger-like process involving a single additional charge present in the nanocrystal. Our results challenge this long-standing assumption. Close examination of exciton PL intensity time traces of single CdSe(CdZnS) core(shell) nanocrystals reveals that the dark state PL quantum yield can be 10 times less than the biexciton PL quantum yield. In addition, we observe spectrally resolved multiexciton emission and find that it also blinks with an on/off ratio greater than 10:1 . These results directly contradict the predictions of the charging model.

  14. Synthesis, functionalization, and biological tagging applications of II-VI semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Wang, Jun

    Fluorescent labeling of biological molecules is a technique that is used widely for analytical purposes in biotechnology and bioengineering. It typically involves the use of an organic dye molecule linked to a moiety that selectively bonds a particular biological molecule, allowing the detection of the latter by the fluorescence of the dye molecule. Semiconductor nanocrystals or quantum dots have emerged as a new class of fluorescent markers with distinct advantages over the traditional organic dyes. Their attractive properties include narrow, symmetric, and bright emission, continuous excitation by any wavelength smaller than the emission wavelength, broad absorption spectrum, long lifetime, resistance to photobleaching, as well as excellent optical and chemical stability that allows their use in lengthy experiments. The focus of this thesis is the synthesis and surface functionalization of ZnSe quantum dots and (ZnSe)ZnS core-shell nanostructures, and their biological conjugation with DNA and protein. The ability to synthesize different populations of quantum dots with narrow emission spectra permits multiplexing, a property that is very important for simultaneous detection of several analytes, which would be very tedious and expensive if done sequentially. Highly luminescent ZnSe nanocrystals have been synthesized using a hot-injection colloidal method. The synthesis was performed in a stirred batch reactor containing liquid hexadecylamine at 310°C. The precursors were diethylzinc diluted in heptane and selenium powder mixed with trioctylphosphine. The mixture of reactants was injected into the batch reactor and the time of reaction was used to control the size and luminescence emission wavelength of the quantum dots. In order to optimize the process various parameters that can influence the photoluminescence property of quantum dots obtained were investigated, such as surfactant addition, temperature, precursor ratio, and mixing conditions. Capping of the Zn

  15. Interband Coulomb coupling in narrow-gap semiconductor nanocrystals: k .p theory

    NASA Astrophysics Data System (ADS)

    Azizi, Maryam; Machnikowski, Paweł

    2015-05-01

    We derive the matrix elements of Coulomb interaction between states with different numbers of electrons and holes in a semiconductor nanocrystal within the eight-band k .p theory. These matrix elements are responsible for multiple exciton generation which may contribute to the enhancement of the efficiency of solar cells. Our calculations are performed within the multiband envelope function formalism based on the states resulting from diagonalization of the eight-band k .p Hamiltonian. We study in detail and compare two contributions to the interband Coulomb coupling: the mesoscopic one, which involves only the envelope functions and relies on band mixing, and the microscopic one, which relies on the Bloch parts of the wave functions and is nonzero even between single-band states. We show that these two contributions are of a similar order of magnitude. We also study the statistical distribution of the magnitudes of the interband Coulomb matrix elements and show that the overall coupling to remote states decays according to a power law favorable for the convergence of numerical computations.

  16. From Light Impurity Doping to Complete Cation Exchange in Semiconductor Nanocrystals: The Role of Coulomb Interactions

    NASA Astrophysics Data System (ADS)

    Erwin, Steven; Ott, Florian; Norris, David

    2014-03-01

    Cation exchange is a reversible chemical reaction used to create new materials by replacing one type of cation with another, usually from solution. We have developed an atomistic model describing cation exchange in semiconductor nanocrystals. The model uses a small set of results obtained from DFT calculations for Ag-doped CdSe. From these we constructed a kinetic Monte Carlo model to address finite temperatures and time scales beyond the reach of DFT. Our simulations span a wide range of Ag concentrations, from light doping to full cation exchange. Thus our model provides a single conceptual framework in which these two phenomena can be understood as limiting endpoints. The results of the simulations are consistent with several experimentally observed aspects of both phenomena. An unexpected finding of our simulations is that the Coulomb interaction plays a central, but changing, role as the Ag concentration varies from light doping to fully cation exchanged. For example, if the Coulomb interaction is strongly screened then cation exchange is suppressed or stopped. When only moderately screened, Coulomb effects play an unanticipated but important role for both doping and cation exchange.

  17. Hopping conductivity and insulator-metal transition in films of touching semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Fu, Han; Reich, K. V.; Shklovskii, B. I.

    2016-03-01

    This paper is focused on the variable-range hopping of electrons in semiconductor nanocrystal (NC) films below the critical doping concentration nc at which it becomes metallic. The hopping conductivity is described by the Efros-Shklovskii law, which depends on the localization length of electrons. We study how the localization length grows with the doping concentration n in the film of touching NCs. For that we calculate the electron transfer matrix element t (n ) between neighboring NCs for two models when NCs touch by small facets or just one point. We study two sources of disorder: variations of NC diameters and random Coulomb potentials originating from random numbers of donors in NCs. We use the ratio of t (n ) to the disorder-induced NC level dispersion to find the localization length of electrons due to the multistep elastic co-tunneling process. We found three different phases at n

  18. Doped Semiconductor-Nanocrystal Emitters with Optimal Photoluminescence Decay Dynamics in Microsecond to Millisecond Range: Synthesis and Applications

    PubMed Central

    2015-01-01

    Transition metal doped semiconductor nanocrystals (d-dots) possess fundamentally different emission properties upon photo- or electroexcitation, which render them as unique emitters for special applications. However, in comparison with intrinsic semiconductor nanocrystals, the potential of d-dots has been barely realized, because many of their unique emission properties mostly rely on precise control of their photoluminescence (PL) decay dynamics. Results in this work revealed that it would be possible to obtain bright d-dots with nearly single-exponential PL decay dynamics. By tuning the number of Mn2+ ions per dot from ∼500 to 20 in Mn2+ doped ZnSe nanocrystals (Mn:ZnSe d-dots), the single-exponential PL decay lifetime was continuously tuned from ∼50 to 1000 μs. A synthetic scheme was further developed for uniform and epitaxial growth of thick ZnS shell, ∼7 monolayers. The resulting Mn:ZnSe/ZnS core/shell d-dots were found to be essential for necessary environmental durability of the PL properties, both steady-state and transient ones, for the d-dot emitters. These characteristics combined with intense absorption and high PL quantum yields (70 ± 5%) enabled greatly simplified schemes for various applications of PL lifetime multiplexing using Mn:ZnSe/ZnS core/shell d-dots. PMID:27163024

  19. Doped Semiconductor-Nanocrystal Emitters with Optimal Photoluminescence Decay Dynamics in Microsecond to Millisecond Range: Synthesis and Applications.

    PubMed

    Pu, Chaodan; Ma, Junliang; Qin, Haiyan; Yan, Ming; Fu, Tao; Niu, Yuan; Yang, Xiaoli; Huang, Yifan; Zhao, Fei; Peng, Xiaogang

    2016-01-27

    Transition metal doped semiconductor nanocrystals (d-dots) possess fundamentally different emission properties upon photo- or electroexcitation, which render them as unique emitters for special applications. However, in comparison with intrinsic semiconductor nanocrystals, the potential of d-dots has been barely realized, because many of their unique emission properties mostly rely on precise control of their photoluminescence (PL) decay dynamics. Results in this work revealed that it would be possible to obtain bright d-dots with nearly single-exponential PL decay dynamics. By tuning the number of Mn(2+) ions per dot from ∼500 to 20 in Mn(2+) doped ZnSe nanocrystals (Mn:ZnSe d-dots), the single-exponential PL decay lifetime was continuously tuned from ∼50 to 1000 μs. A synthetic scheme was further developed for uniform and epitaxial growth of thick ZnS shell, ∼7 monolayers. The resulting Mn:ZnSe/ZnS core/shell d-dots were found to be essential for necessary environmental durability of the PL properties, both steady-state and transient ones, for the d-dot emitters. These characteristics combined with intense absorption and high PL quantum yields (70 ± 5%) enabled greatly simplified schemes for various applications of PL lifetime multiplexing using Mn:ZnSe/ZnS core/shell d-dots. PMID:27163024

  20. Contact Radius and the Insulator-Metal Transition in Films Comprised of Touching Semiconductor Nanocrystals.

    PubMed

    Lanigan, Deanna; Thimsen, Elijah

    2016-07-26

    Nanocrystal assemblies are being explored for a number of optoelectronic applications such as transparent conductors, photovoltaic solar cells, and electrochromic windows. Majority carrier transport is important for these applications, yet it remains relatively poorly understood in films comprised of touching nanocrystals. Specifically, the underlying structural parameters expected to determine the transport mechanism have not been fully elucidated. In this report, we demonstrate experimentally that the contact radius, between touching heavily doped ZnO nanocrystals, controls the electron transport mechanism. Spherical nanocrystals are considered, which are connected by a circular area. The radius of this circular area is the contact radius. For nanocrystals that have local majority carrier concentration above the Mott transition, there is a critical contact radius. If the contact radius between nanocrystals is less than the critical value, then the transport mechanism is variable range hopping. If the contact radius is greater than the critical value, the films display behavior consistent with metallic electron transport. PMID:27398597

  1. Transient fluorescence of the off state in blinking CdSe/CdS/ZnS semiconductor nanocrystals is not governed by Auger recombination.

    PubMed

    Rosen, Shamir; Schwartz, Osip; Oron, Dan

    2010-04-16

    The observed intermittent light emission from colloidal semiconductor nanocrystals has long been associated with Auger recombination assisted quenching. We test this view by observing transient emission dynamics of CdSe/CdS/ZnS semiconductor nanocrystals using time-resolved photon counting. The size and intensity dependence of the observed decay dynamics seem inconsistent with those expected from Auger processes. Rather, the data suggest that in the "off" state the quantum dot cycles in a three-step process: photoexcitation, rapid trapping, and subsequent slow nonradiative decay.

  2. Electronic grade and flexible semiconductor film employing oriented attachment of colloidal ligand-free PbS and PbSe nanocrystals at room temperature

    NASA Astrophysics Data System (ADS)

    Shanker, G. Shiva; Swarnkar, Abhishek; Chatterjee, Arindom; Chakraborty, S.; Phukan, Manabjyoti; Parveen, Naziya; Biswas, Kanishka; Nag, Angshuman

    2015-05-01

    Electronic grade semiconductor films have been obtained via the sintering of solution processed PbS and PbSe nanocrystals at room temperature. Prior attempts to achieve similar films required the sintering of nanocrystals at higher temperatures (>350 °C), which inhibits the processing of such films on a flexible polymer substrate, and it is also expensive. We reduced the sintering temperature by employing two important strategies: (i) use of ligand-free nanocrystals and (ii) oriented attachment of nanocrystals. Colloidal ligand-free PbS and PbSe nanocrystals were synthesized at 70 °C with high yield (~70%). However, these nanocrystals start to agglomerate with time in formamide, and upon the removal of the solvation energy, nanocrystals undergo oriented attachment, forming larger elongated crystals. PbS and PbSe nanocrystal films made on both glass and flexible substrates at room temperature exhibit Ohmic behavior with optimum DC conductivities of 0.03 S m-1 and 0.08 S m-1, respectively. Mild annealing of the films at 150 °C increases the conductivity values to 1.1 S m-1 and 137 S m-1 for PbS and PbSe nanocrystal films, respectively. AC impedance was measured to distinguish the contributions from grain and grain boundaries to the charge transport mechanism. Charge transport properties remain similar after the repeated bending of the film on a flexible polymer substrate. Reasonably high thermoelectric Seebeck coefficients of 600 μV K-1 and 335 μV K-1 for PbS and PbSe nanocrystal pellets, respectively, were obtained at room temperature.Electronic grade semiconductor films have been obtained via the sintering of solution processed PbS and PbSe nanocrystals at room temperature. Prior attempts to achieve similar films required the sintering of nanocrystals at higher temperatures (>350 °C), which inhibits the processing of such films on a flexible polymer substrate, and it is also expensive. We reduced the sintering temperature by employing two important strategies

  3. General Strategy for Enhancing Electrochemiluminescence of Semiconductor Nanocrystals by Hydrogen Peroxide and Potassium Persulfate as Dual Coreactants.

    PubMed

    Dai, Pan-Pan; Yu, Tao; Shi, Hai-Wei; Xu, Jing-Juan; Chen, Hong-Yuan

    2015-12-15

    Semiconductor nanocrystals usually suffer from weak electrogenerated chemiluminescence (ECL) emissions compared with conventional organic emitters. In this work, we propose, for the first time, a very convenient but effective way to greatly enhance ECL emission of semiconductor TiO2 nanotubes (NTs) by H2O2 and K2S2O8 as dual coreactants, generating ECL emission ca. 6.3 and 107 times stronger than that of K2S2O8 or H2O2 as an individual coreactant, respectively. Scanning electron microscopy, X-ray diffraction, and electron paramagnetic resonance spectral studies were carried out to investigate the ECL enhancement mechanism. The ECL enhancement of TiO2 NTs by the K2S2O8-H2O2 system was supposed to originate from the coordination of H2O2 to the TiO2 surface and the synergy effect between H2O2 and K2S2O8 in the ECL process. The coordination of H2O2 to the surface of TiO2 could stabilize the electrogenerated coreactant-related radical OH(•) (hydroxyl radical), which could obviously promote the amount of sulfate radical anion (SO4(•-)) near the electrode surface by inducing decomposition of K2S2O8 into SO4(•-) or inhibiting the consumption of SO4(•-) by its reaction with H2O. The holes (h(+)) released from SO4(•-) were injected into the valence band of TiO2, resulting in more TiO2(+), which combined with the electrons coming from the conduction band with an enhanced light emission. Moreover, this enhancement effect was also applicable to ECL of a CdS nanocrystal film on a glass carbon electrode, with ca. 2.74- and 148.3-fold enhanced ECL intensity correspondingly, indicating wide applications in the development of semiconductor nanocrystal-based ECL biosensors. PMID:26564425

  4. Final Report for Nucleation and growth of semiconductor nanocrystals by solid-phase reaction

    SciTech Connect

    P. D. Persans; T. M. Hayes

    2005-12-12

    This final report describes the technical output of a scientific program aimed at understanding the formation and structure of II-VI nanocrystals formed by solid phase precipitation within a glass environment. The principle probes were optical absorption spectroscopy to determine crystallite sizes, Raman scattering to determine composition, and x-ray absorption spectroscopy to study the evolution of local reactant environments.

  5. Single-particle spectroscopy of I-III-VI semiconductor nanocrystals: spectral diffusion and suppression of blinking by two-color excitation

    NASA Astrophysics Data System (ADS)

    Sharma, Dharmendar Kumar; Hirata, Shuzo; Bujak, Lukasz; Biju, Vasudevanpillai; Kameyama, Tatsuya; Kishi, Marino; Torimoto, Tsukasa; Vacha, Martin

    2016-07-01

    Ternary I-III-VI semiconductor nanocrystals have been explored as non-toxic alternatives to II-VI semiconductors for optoelectronic and sensing applications, but large photoluminescence spectral width and moderate brightness restrict their practical use. Here, using single-particle photoluminescence spectroscopy on nanocrystals of (AgIn)xZn2(1-x)S2 we show that the photoluminescence band is inhomogeneously broadened and that size distribution is the dominant factor in the broadening. The residual homogeneous linewidth of individual nanocrystals reaches up to 75% of the ensemble spectral width. Single nanocrystals undergo spectral diffusion which also contributes to the inhomogeneous band. Excitation with two lasers with energies above and below the bandgap reveals coexistence of two emitting donor states within one particle. Spectral diffusion in such particles is due to temporal activation and deactivation of one such state. Filling of a trap state with a lower-energy laser enables optical modulation of photoluminescence intermittency (blinking) and leads to an almost two-fold increase in brightness.Ternary I-III-VI semiconductor nanocrystals have been explored as non-toxic alternatives to II-VI semiconductors for optoelectronic and sensing applications, but large photoluminescence spectral width and moderate brightness restrict their practical use. Here, using single-particle photoluminescence spectroscopy on nanocrystals of (AgIn)xZn2(1-x)S2 we show that the photoluminescence band is inhomogeneously broadened and that size distribution is the dominant factor in the broadening. The residual homogeneous linewidth of individual nanocrystals reaches up to 75% of the ensemble spectral width. Single nanocrystals undergo spectral diffusion which also contributes to the inhomogeneous band. Excitation with two lasers with energies above and below the bandgap reveals coexistence of two emitting donor states within one particle. Spectral diffusion in such particles is due

  6. Nanocrystal doped matrixes

    SciTech Connect

    Parce, J. Wallace; Bernatis, Paul; Dubrow, Robert; Freeman, William P.; Gamoras, Joel; Kan, Shihai; Meisel, Andreas; Qian, Baixin; Whiteford, Jeffery A.; Ziebarth, Jonathan

    2010-01-12

    Matrixes doped with semiconductor nanocrystals are provided. In certain embodiments, the semiconductor nanocrystals have a size and composition such that they absorb or emit light at particular wavelengths. The nanocrystals can comprise ligands that allow for mixing with various matrix materials, including polymers, such that a minimal portion of light is scattered by the matrixes. The matrixes of the present invention can also be utilized in refractive index matching applications. In other embodiments, semiconductor nanocrystals are embedded within matrixes to form a nanocrystal density gradient, thereby creating an effective refractive index gradient. The matrixes of the present invention can also be used as filters and antireflective coatings on optical devices and as down-converting layers. Processes for producing matrixes comprising semiconductor nanocrystals are also provided. Nanostructures having high quantum efficiency, small size, and/or a narrow size distribution are also described, as are methods of producing indium phosphide nanostructures and core-shell nanostructures with Group II-VI shells.

  7. Measuring and Predicting the Internal Structure of Semiconductor Nanocrystals through Raman Spectroscopy.

    PubMed

    Mukherjee, Prabuddha; Lim, Sung Jun; Wrobel, Tomasz P; Bhargava, Rohit; Smith, Andrew M

    2016-08-31

    Nanocrystals composed of mixed chemical domains have diverse properties that are driving their integration in next-generation electronics, light sources, and biosensors. However, the precise spatial distribution of elements within these particles is difficult to measure and control, yet profoundly impacts their quality and performance. Here we synthesized a unique series of 42 different quantum dot nanocrystals, composed of two chemical domains (CdS:CdSe), arranged in 7 alloy and (core)shell structural classes. Chemometric analyses of far-field Raman spectra accurately classified their internal structures from their vibrational signatures. These classifications provide direct insight into the elemental arrangement of the alloy as well as an independent prediction of fluorescence quantum yield. This nondestructive, rapid approach can be broadly applied to greatly enhance our capacity to measure, predict and monitor multicomponent nanomaterials for precise tuning of their structures and properties. PMID:27472011

  8. Carrier Multiplication in Semiconductor Nanocrystals: Theoretical Screening of Candidate Materials Based on Band-Structure Effects

    SciTech Connect

    Luo, J. W.; Franceschetti, A.; Zunger, A.

    2008-01-01

    Direct carrier multiplication (DCM) occurs when a highly excited electron-hole pair decays by transferring its excess energy to the electrons rather than to the lattice, possibly exciting additional electron-hole pairs. Atomistic electronic structure calculations have shown that DCM can be induced by electron-hole Coulomb interactions, in an impact-ionization-like process whose rate is proportional to the density of biexciton states {rho}{sub XX}. Here we introduce a DCM 'figure of merit' R{sub 2}(E) which is proportional to the ratio between the biexciton density of states {rho}{sub XX} and the single-exciton density of states {rho}{sub x}, restricted to single-exciton and biexciton states that are coupled by Coulomb interactions. Using R{sub 2}(E), we consider GaAs, InAs, InP, GaSb, InSb, CdSe, Ge, Si, and PbSe nanocrystals of different sizes. Although DCM can be affected by both quantum-confinement effects (reflecting the underly electronic structure of the confined dot-interior states) and surface effects, here we are interested to isolate the former. To this end the nanocrystal energy levels are obtained from the corresponding bulk band structure via the truncated crystal approximation. We find that PbSe, Si, GaAs, CdSe, and InP nanocrystals have larger DCM figure of merit than the other nanocrystals. Our calculations suggest that high DCM efficiency requires high degeneracy of the corresponding bulk band-edge states. Interestingly, by considering band structure effects we find that as the dot size increases the DCM critical energy E{sub 0} (the energy at which R{sub 2}(E) becomes {ge}1) is reduced, suggesting improved DCM. However, whether the normalized E{sub 0}/{var_epsilon}{sub g} increases or decreases as the dot size increases depends on dot material.

  9. Metal Oleate Induced Etching and Growth of Semiconductor Nanocrystals, Nanorods, and Their Heterostructures.

    PubMed

    Oh, Nuri; Shim, Moonsub

    2016-08-24

    Unexpected etching of nanocrystals, nanorods, and their heterostructures by one of the most commonly used metal precursors, metal oleates, is reported. Zn oleate is shown to etch CdS nanorods anisotropically, where the length decreases without a significant change in the diameter. Sodium oleate enhances the etch rate, whereas oleic acid alone does not cause etching, indicating the importance of the countercation on the rate of oleate induced etching. Subsequent addition of Se precursors to the partially etched nanorods in Zn oleate solution can lead to epitaxial growth of CdSe particles rather than the expected ZnSe growth, despite an excess amount of Zn precursors being present. The composition of this epitaxial growth can be varied from CdSe to ZnSe, depending on the amount of excess oleic acid or the reaction temperature. Similar tuning of composition can be observed when starting with collinear CdSe/CdS/CdSe rod/rod/rod heterostructures and spherical CdS (or CdSe/CdS core/shell) nanocrystals. Conversion of collinear rod/rod/rod structures to barbells and interesting rod growth from nearly spherical particles among other structures can also result due to the initial etching effect of metal oleates. These observations have important implications on our understanding of nanocrystal heterostructure synthesis and open up new routes to varying the composition and morphology of these materials. PMID:27485673

  10. The Effect of Exciton-Delocalizing Thiols on Intrinsic Dual Emitting Semiconductor Nanocrystals.

    PubMed

    Jethi, Lakshay; Mack, Timothy G; Krause, Michael M; Drake, Sebastian; Kambhampati, Patanjali

    2016-03-01

    The emissive properties of thiol-capped CdSe nanocrystals (NCs) with intrinsic dual emission are investigated through temperature-dependent photoluminescence (PL) measurements. We demonstrate the influence of thiols on the relative PL intensities of the core and surface emissive states, as well as on the observed Stokes shifts. A redshift of both the core and surface PL in comparison with phosphonate-capped NCs is consistent with recent work exploring the effect of thiols as excitonic hole-delocalizing ligands. This observation is consistent with prior reports suggesting that surface excitons originate from electrons bound to cadmium trap states. PMID:26752223

  11. Semiconductor nanocrystals functionalized with antimony telluride zintl ions for nanostructured thermoelectrics.

    PubMed

    Kovalenko, Maksym V; Spokoyny, Boris; Lee, Jong-Soo; Scheele, Marcus; Weber, Andrew; Perera, Susanthri; Landry, Daniel; Talapin, Dmitri V

    2010-05-19

    The energy efficiency of heat engines could be improved by the partial recovery of waste heat using thermoelectric (TE) generators. We show the possibility of designing nanostructured TE materials using colloidal inorganic nanocrystals functionalized with molecular antimony telluride complexes belonging to the family of Zintl ions. The unique advantage of using Zintl ions as the nanocrystal surface ligands is the possibility to convert them into crystalline metal chalcogenides, thus linking individual nanobuilding blocks into a macroscopic assembly of electronically coupled functional modules. This approach allows preserving the benefits of nanostructuring and quantum confinement while enabling facile charge transport through the interparticle boundaries. A developed methodology was applied for solution-based fabrication of nanostructured n- and p-type Bi(2-x)Sb(x)Te(3) alloys with tunable composition and PbTe-Sb(2)Te(3) nanocomposites with controlled grain size. Characterization of the TE properties of these materials showed that their Seebeck coefficients, electrical and thermal conductivities, and ZT values compared favorably with those of previously reported solution-processed TE materials.

  12. Protective ligand shells for luminescent SiO₂-coated alloyed semiconductor nanocrystals.

    PubMed

    Acebrón, María; Galisteo-López, Juan F; Granados, Daniel; López-Ogalla, Javier; Gallego, José M; Otero, Roberto; López, Cefe; Juárez, Beatriz H

    2015-04-01

    SiO2 encapsulation of alloyed CdSeZnS nanocrystals (NCs) shows differences in terms of optical properties and luminescence quantum yield, depending on the surface composition, size, and ligand content. In this work, emphasis has been placed on the fine control required to obtain luminescent SiO2 encapsulated NCs by studying the role of oleic acid (OA), stearic acid (SA), and dodecanethiol (DDT) ligands on the alloyed NCs. While the use of anchored DDT molecules is essential to preserve the optical properties, intercalated OA and SA play a critical role for SiO2 nucleation, as stated by (1)H NMR (including DOSY and NOESY) spectroscopy. These results emphasize the importance of surface chemistry in NCs; it is crucial to control their reactivity, and therefore their impact, in different applications, from optics to biomedicine.

  13. Role of electron carriers on local surface plasmon resonances in doped oxide semiconductor nanocrystals

    SciTech Connect

    Matsui, Hiroaki Tabata, Hitoshi; Furuta, Shinya

    2014-05-26

    Optical properties of carrier-dependent local surface plasmons (LSPs) were studied using dopant-controlled In{sub 2}O{sub 3}:Sn nanocrystals (NCs). From a systematic correlation between LSP excitations and electron carriers, electron-impurity scattering contributed towards plasmon damping as one of a factor that is absent in metal NCs. A threshold electron density (n{sub e}) from a damping dominated regime to a quenched damping regime appeared at around 10{sup 20} cm{sup −3}. The validity of Mie theory failed in ITO NCs with high n{sub e} greater than 10{sup 20} cm{sup −3} since the role of electron carriers could enhance LSPs with simultaneous damped plasmonic excitations, which is valuable information for optical applications.

  14. Nonlinear optical response of semiconductor-nanocrystals-embedded photonic band gap structure

    SciTech Connect

    Liao, Chen; Zhang, Huichao; Tang, Luping; Zhou, Zhiqiang; Lv, Changgui; Cui, Yiping; Zhang, Jiayu

    2014-04-28

    Colloidal CdSe/ZnS core/shell nanocrystals (NCs), which were dispersed in SiO{sub 2} sol, were utilized to fabricate a SiO{sub 2}:NCs/TiO{sub 2} all-dielectric photonic band gap (PBG) structure. The third-order nonlinear refractive index (n{sub 2}) of the PBG structure was nearly triple of that of the SiO{sub 2}:NCs film due to the local field enhancement in the PBG structure. The photoinduced change in refractive index (Δn) could shift the PBG band edge, so the PBG structure would show significant transmission modification, whose transmission change was ∼17 folds of that of the SiO{sub 2}:NCs film. Under excitation of a 30 GW/cm{sup 2} femtosecond laser beam, a transmission decrease of 80% was realized.

  15. Symmetry breaking in semiconductor nanocrystals via kinetic-controlled surface diffusion: a strategy for manipulating the junction structure.

    PubMed

    Wang, Xixi; Liu, Maochang; Chen, Yubin; Fu, Wenlong; Wang, Bin; Guo, Liejin

    2016-09-21

    The synthesis of semiconductor nanocrystals is usually limited to high-level symmetry, as constrained by the inherent, for example, face-centered cubic or hexagonal close-packed lattices of the crystals. Herein, we report a robust approach for breaking the symmetry of the CdS lattice and obtaining high-quality CdS ultrathin monopods, bipods, tripods, and tetrapods. The success relies on manipulating reaction kinetics by dropwise addition of a precursor solution, which permits deterministic control over the number of CdS monomers in the reaction solution. With rapid monomer supply by fast precursor injection, growth was restricted to only one {111} facet of the nascent CdS tetrahedron to produce an asymmetric ultrathin monopod (a zinc-blende tip with a wurtzite arm). Otherwise, growth monomers could access adjacent {111} facets through surface diffusion and thus lead to the switch of the growth pattern from asymmetric to symmetric to generate an ultrathin multipod (a zinc-blende tip/core with multi-wurtzite arms). These symmetry-controlled photocatalysts were characterized by a fine-tuned zinc blende-wurtzite intergrowth type-II homojunction. After evaluating their structure-dependent solar-hydrogen-production properties, the CdS ultrathin monopod with an appropriate length for controllable charge transportation showed the highest photocatalytic activity. PMID:27539367

  16. Nano-engineered electron–hole exchange interaction controls exciton dynamics in core–shell semiconductor nanocrystals

    PubMed Central

    Brovelli, S.; Schaller, R.D.; Crooker, S.A.; García-Santamaría, F.; Chen, Y.; Viswanatha, R.; Hollingsworth, J.A.; Htoon, H.; Klimov, V.I.

    2011-01-01

    A strong electron–hole exchange interaction (EI) in semiconductor nanocrystals (NCs) gives rise to a large (up to tens of meV) splitting between optically active ('bright') and optically passive ('dark') excitons. This dark–bright splitting has a significant effect on the optical properties of band-edge excitons and leads to a pronounced temperature and magnetic field dependence of radiative decay. Here we demonstrate a nanoengineering-based approach that provides control over EI while maintaining nearly constant emission energy. We show that the dark–bright splitting can be widely tuned by controlling the electron–hole spatial overlap in core–shell CdSe/CdS NCs with a variable shell width. In thick-shell samples, the EI energy reduces to <250 μeV, which yields a material that emits with a nearly constant rate over temperatures from 1.5 to 300 K and magnetic fields up to 7 T. The EI-manipulation strategies demonstrated here are general and can be applied to other nanostructures with variable electron–hole overlap. PMID:21505436

  17. Near-Infrared Photoluminescence Enhancement in Ge/CdS and Ge/ZnS Core/Shell Nanocrystals: Utilizing IV/II-VI Semiconductor Epitaxy

    SciTech Connect

    Guo, Yijun; Rowland, Clare E; Schaller, Richard D; Vela, Javier

    2014-08-26

    Ge nanocrystals have a large Bohr radius and a small, size-tunable band gap that may engender direct character via strain or doping. Colloidal Ge nanocrystals are particularly interesting in the development of near-infrared materials for applications in bioimaging, telecommunications and energy conversion. Epitaxial growth of a passivating shell is a common strategy employed in the synthesis of highly luminescent II–VI, III–V and IV–VI semiconductor quantum dots. Here, we use relatively unexplored IV/II–VI epitaxy as a way to enhance the photoluminescence and improve the optical stability of colloidal Ge nanocrystals. Selected on the basis of their relatively small lattice mismatch compared with crystalline Ge, we explore the growth of epitaxial CdS and ZnS shells using the successive ion layer adsorption and reaction method. Powder X-ray diffraction and electron microscopy techniques, including energy dispersive X-ray spectroscopy and selected area electron diffraction, clearly show the controllable growth of as many as 20 epitaxial monolayers of CdS atop Ge cores. In contrast, Ge etching and/or replacement by ZnS result in relatively small Ge/ZnS nanocrystals. The presence of an epitaxial II–VI shell greatly enhances the near-infrared photoluminescence and improves the photoluminescence stability of Ge. Ge/II–VI nanocrystals are reproducibly 1–3 orders of magnitude brighter than the brightest Ge cores. Ge/4.9CdS core/shells show the highest photoluminescence quantum yield and longest radiative recombination lifetime. Thiol ligand exchange easily results in near-infrared active, water-soluble Ge/II–VI nanocrystals. We expect this synthetic IV/II–VI epitaxial approach will lead to further studies into the optoelectronic behavior and practical applications of Si and Ge-based nanomaterials.

  18. Cryptography based on the absorption/emission features of multicolor semiconductor nanocrystal quantum dots.

    PubMed

    Zhou, Ming; Chang, Shoude; Grover, Chander

    2004-06-28

    Further to the optical coding based on fluorescent semiconductor quantum dots (QDs), a concept of using mixtures of multiple single-color QDs for creating highly secret cryptograms based on their absorption/emission properties was demonstrated. The key to readout of the optical codes is a group of excitation lights with the predetermined wavelengths programmed in a secret manner. The cryptograms can be printed on the surfaces of different objects such as valuable documents for security purposes.

  19. Carbon-shell-decorated p-semiconductor PbMoO4 nanocrystals for efficient and stable photocathode of photoelectrochemical water reduction

    NASA Astrophysics Data System (ADS)

    Wang, Ligang; Tang, Hanqin; Tian, Yang

    2016-07-01

    Photoelectrochemical (PEC) water splitting using semiconductors is a promising method for the future scalable production of renewable hydrogen fuels. The critical issues in PEC water splitting include the development of the photoelectrode materials with high efficiency and long-term stability, especially for p-type semiconductor photocathodes. Herein, we report the use of citric acid (CA) pyrolysis to prepare carbon-shell-decorated PbMoO4 (C@PbMoO4) nanocrystals via a simple solvothermal method. Different carbon shell thicknesses below 10 nm were generated by varying the amount of CA in the precursor solution. In contrast, without using CA, bare PbMoO4 nanocrystals were obtained. The PEC experiments showed that 2-nm carbon shell could preferably improve the water splitting performance of PbMoO4: the photocurrent density of 2-nm C@PbMoO4 is nearly 2-fold high as that of bare PbMoO4 at 0 V versus reversible hydrogen electrode (RHE). The surface charge transfer efficiency of 2-nm C@PbMoO4 in the PEC process was tested to increase from 83% to 90.4%, the charge separation efficiency enhanced 56%, and the PEC stability also greatly increased compared to those of the bare PbMoO4 nanocrystals. This strategy could be applied to other p-type semiconducting photocathodes for low-cost solar-fuel-generation devices.

  20. How Robust are Semiconductor Nanorods? Investigating the Stability and Chemical Decomposition Pathways of Photoactive Nanocrystals

    SciTech Connect

    Reichert, Malinda D; Lin, Chia-Cheng; Vela, Javier

    2014-07-08

    Anisotropic II–VI semiconductor nanostructures are important photoactive materials for various energy conversion and optical applications. However, aside from the many available surface chemistry studies and from their ubiquitous photodegradation under continuous illumination, the general chemical reactivity and thermal stability (phase and shape transformations) of these materials are poorly understood. Using CdSe and CdS nanorods as model systems, we have investigated the behavior of II–VI semiconductor nanorods against various conditions of extreme chemical and physical stress (acids, bases, oxidants, reductants, and heat). CdSe nanorods react rapidly with acids, becoming oxidized to Se or SeO2. In contrast, CdSe nanorods remain mostly unreactive when treated with bases or strong oxidants, although bases do partially etch the tips of the nanorods (along their axis). Roasting (heating in air) of CdSe nanorods results in rock-salt CdO, but neither CdSe nor CdO is easily reduced by hydrogen (H2). Another reductant, n-BuLi, reduces CdSe nanorods to metallic Cd. Variable temperature X-ray diffraction experiments show that axial annealing and selective axial melting of the nanorods precede particle coalescence. Furthermore, thermal analysis shows that the axial melting of II–VI nanorods is a ligand-dependent process. In agreement with chemical reactivity and thermal stability observations, silica-coating experiments show that the sharpest (most curved) II–VI surfaces are most active against heterogeneous nucleation of a silica shell. These results provide valuable insights into the fate and possible ways to enhance the stability and improve the use of II–VI semiconductor nanostructures in the fields of optics, magnetism, and energy conversion.

  1. Application of semiconductor fluorescent nanocrystals as optical probes for rapid early viral detection

    NASA Astrophysics Data System (ADS)

    Bentzen, Elizabeth L.; House, Frances; Tomlinson, Ian D.; Rosenthal, Sandra J.; Crowe, James E.; Wright, David D.

    2005-04-01

    Fluorescence is a tool widely employed in biological assays. Fluorescent semiconducting nanocrystals, quantum dots (QDs), are beginning to find their way into the tool box of many biologist, chemist and biochemist. These quantum dots are an attractive alternative to the traditional organic dyes due to their broad excitation spectra, narrow emission spectra and photostability. Non-specific binding is a frequently encountered problem with fluorescent labeling in biological assays. In these studies various cell lines were examined for non-specific binding to quantum dots. Evidence suggests that non-specific binding is related to cell type and, may be significantly reduced by functionalizing quantum dots with polyethyleneglycol ligands (PEG). In addition quantum dots were used to detect and monitor the progession of the viral glycoproteins ,F (fusion) and G (attachment), from Respiratory Syncytial Virus (RSV) in HEp-2 cells. RSV is the most common cause of lower respiratory tract infection in children worldwide and the most common cause of hospitalization of infants in the US. Antiviral therapy is available for treatment of RSV but is only effective if given within the first 48 hours of infection. Existing test methods require a virus level of at least 1000-fold of the amount needed for infection of most children and require several days to weeks to obtain results. The use of quantum dots may provide an early, rapid method for detection and provide insight into the trafficking of viral proteins during the course of infection.

  2. Mesoporous silica beads embedded with semiconductor quantum dots and iron oxide nanocrystals: dual-function microcarriers for optical encoding and magnetic separation.

    PubMed

    Sathe, Tushar R; Agrawal, Amit; Nie, Shuming

    2006-08-15

    Mesoporous beads are promising materials for embedding functional nanoparticles because of their nanometer-sized pores and large surface areas. Here we report the development of silica microbeads embedded with both semiconductor quantum dots (QD) and iron oxide (Fe3O4) nanocrystals as a new class of dual-function carriers for optical encoding and magnetic separation. The embedding (doping) process is carried out by either simultaneous or sequential addition of quantum dots and iron oxide (Fe3O4) nanocrystals in solution. The doping process is fast and quantitative, but the incorporated iron oxide strongly attenuates the signal intensity of QD fluorescence. We find that this attenuation is not due to conventional fluorescence quenching but is caused by the broad optical absorption spectrum of mixed-valence Fe3O4. For improved biocompatibility and reduced nonspecific binding, the encoded beads are further coated with amphiphilic polymers such as octylamine poly(acrylic acid). The results indicate that the polymer-coated beads are well suited for target capturing and enrichment, yielding magnetic separation efficiencies higher than 99%. By combining the multiplexing capability of QDs with the superparamagnetic properties of iron oxide nanocrystals, this class of encoded beads is expected to find broad applications in high-throughput and multiplexed biomolecular assays. PMID:16906704

  3. Silicon nanocrystal inks, films, and methods

    SciTech Connect

    Wheeler, Lance Michael; Kortshagen, Uwe Richard

    2015-09-01

    Silicon nanocrystal inks and films, and methods of making and using silicon nanocrystal inks and films, are disclosed herein. In certain embodiments the nanocrystal inks and films include halide-terminated (e.g., chloride-terminated) and/or halide and hydrogen-terminated nanocrystals of silicon or alloys thereof. Silicon nanocrystal inks and films can be used, for example, to prepare semiconductor devices.

  4. Design of a multi-coordinating polymer as a platform for functionalizing metal, metal oxide and semiconductor nanocrystals

    NASA Astrophysics Data System (ADS)

    Wang, Wentao; Ji, Xin; Kapur, Anshika; Mattoussi, Hedi

    2016-03-01

    We introduce a new set of amphiphilic polymers as multifunctional, metal-coordinating ligands adapted to surfacefunctionalize quantum dots (QDs), iron oxide nanoparticles (IONPs) and gold nanoparticles/nanorods (AuNPs/AuNRs). The ligand design relies on the introduction of several anchoring groups, hydrophilic moieties and reactive functionalities into a polymer chain, via one-step nucleophilic addition reaction. Such synthetic scheme also allows the insertion of target biomolecules during the ligand synthesis. This functionalization strategy yields nanocrystals that exhibit long-term colloidal stability over a broad range of biological conditions, such as pH changes and when mixed with growth media. When zwitterion groups are used as hydrophilic motifs, this provides compact nanocrystals that are compatible with conjugation to proteins via metal-polyhistidine self-assembly. In addition, we show that QDs ligated with these polymers can engage in energy or charge transfer interactions. Furthermore, nanocrystals coated with folic acid-modified polymers could promote the delivery of nanoparticle-conjugates into cancer cells via folate receptormediated endocytosis.

  5. LDRD-LW Final Report: 07-LW-041 "Magnetism in Semiconductor Nanocrystals: New Physics at the Nanoscale"

    SciTech Connect

    Meulenberg, R W; Lee, J I; McCall, S K

    2009-10-19

    The work conducted in this project was conducted with the aim of identifying and understanding the origin and mechanisms of magnetic behavior in undoped semiconductor nanocrystals (NCs), specifically those composed of CdSe. It was anticipated that the successful completion of this task would have the effect of addressing and resolving significant controversy over this topic in the literature. Meanwhile, application of the resultant knowledge was expected to permit manipulation of the magnetic properties, particularly the strength of any magnetic effects, which is of potential relevance in a range of advanced technologies. More specifically, the project was designed and research conducted with the goal of addressing the following series of questions: (1) How does the magnitude of the magnetism in CdSe NCs change with the organic molecules used to passivate their surface the NC size? i.e. Is the magnetism an intrinsic effect in the nanocrystalline CdSe (as observed for Au NCs) or a surface termination driven effect? (2) What is the chemical (elemental) nature of the magnetism? i.e. Are the magnetic effects associated with the Cd atoms or the Se atoms or both? (3) What is/are the underlying mechanism(s)? (4) How can the magnetism be controlled for further applications? To achieve this goal, several experimental/technical milestones were identified to be fulfilled during the course of the research: (A) The preparation of well characterized CdSe NCs with varying surface termination (B) Establishing the extent of the magnetism of these NCs using magnetometry (particularly using superconducting interference device [SQUID]) (C) Establishing the chemical nature of the magnetism using x-ray magnetic circular dichroism (XMCD) - the element specific nature of the technique allows identification of the element responsible for the magnetism (D) Identification of the effect of surface termination on the empty densities of states (DOS) using x-ray absorption spectroscopy (XAS

  6. Enhanced photophysical properties of plasmonic magnetic metal-alloyed semiconductor heterostructure nanocrystals: a case study for the Ag@Ni/Zn1-xMgxO system.

    PubMed

    Paul, Sumana; Ghosh, Sirshendu; Saha, Manas; De, S K

    2016-05-14

    Understanding the effect of homovalent cation alloying in wide band gap ZnO and the formation of metal-semiconductor heterostructures is very important for maximisation of the photophysical properties of ZnO. Nearly monodisperse ZnO nanopyramid and Mg alloyed ZnO nanostructures have been successfully synthesized by one pot decomposition of metal stearate by using oleylamine both as activating and capping agent. The solid solubility of Mg(ii) ions in ZnO is limited to ∼30% without phase segregation. An interesting morphology change is found on increasing Mg alloying: from nanopyramids to self-assembled nanoflowers. The morphology change is explained by the oriented attachment process. The introduction of Mg into the ZnO matrix increases the band gap of the materials and also generates new zinc interstitial (Zni) and oxygen vacancy related defects. Plasmonic magnetic Ag@Ni core-shell (Ag as core and Ni as shell) nanocrystals are used as a seed material to synthesize Ag@Ni/Zn1-xMgxO complex heterostructures. Epitaxial growth is established between Ag(111) and ZnO(110) planes in the heterostructure. An epitaxial metal-semiconductor interface is very crucial for complete electron-hole (e-h) separation and enhancement of the exciton lifetime. The alloyed semiconductor-metal heterostructure is observed to be highly photocatalytically active for dye degradation as well as photodetection. Incorporation of magnetic Ni(0) makes the photocatalyst superparamagnetic at room temperature which is found to be helpful for catalyst regeneration. PMID:27113320

  7. Enhanced photovoltaic performance of ultrathin Si solar cells via semiconductor nanocrystal sensitization: energy transfer vs. optical coupling effects

    NASA Astrophysics Data System (ADS)

    Hoang, Son; Ashraf, Ahsan; Eisaman, Matthew D.; Nykypanchuk, Dmytro; Nam, Chang-Yong

    2016-03-01

    Excitonic energy transfer (ET) offers exciting opportunities for advances in optoelectronic devices such as solar cells. While recent experimental attempts have demonstrated its potential in both organic and inorganic photovoltaics (PVs), what remains to be addressed is quantitative understanding of how different ET modes contribute to PV performance and how ET contribution is differentiated from the classical optical coupling (OC) effects. In this study, we implement an ET scheme using a PV device platform, comprising CdSe/ZnS nanocrystal energy donor and 500 nm-thick ultrathin Si acceptor layers, and present the quantitative mechanistic description of how different ET modes, distinguished from the OC effects, increase the light absorption and PV efficiency. We find that nanocrystal sensitization enhances the short circuit current of ultrathin Si solar cells by up to 35%, of which the efficient ET, primarily driven by a long-range radiative mode, contributes to 38% of the total current enhancement. These results not only confirm the positive impact of ET but also provide a guideline for rationally combining the ET and OC effects for improved light harvesting in PV and other optoelectronic devices.Excitonic energy transfer (ET) offers exciting opportunities for advances in optoelectronic devices such as solar cells. While recent experimental attempts have demonstrated its potential in both organic and inorganic photovoltaics (PVs), what remains to be addressed is quantitative understanding of how different ET modes contribute to PV performance and how ET contribution is differentiated from the classical optical coupling (OC) effects. In this study, we implement an ET scheme using a PV device platform, comprising CdSe/ZnS nanocrystal energy donor and 500 nm-thick ultrathin Si acceptor layers, and present the quantitative mechanistic description of how different ET modes, distinguished from the OC effects, increase the light absorption and PV efficiency. We find that

  8. Enhanced photovoltaic performance of ultrathin Si solar cells via semiconductor nanocrystal sensitization: Energy transfer vs. optical coupling effects

    DOE PAGESBeta

    Hoang, Son; Ashraf, Ahsan; Eisaman, Matthew D.; Nykypanchuk, Dmytro; Nam, Chang -Yong

    2015-12-07

    Excitonic energy transfer (ET) offers exciting opportunities for advances in optoelectronic devices such as solar cells. While recent experimental attempts have demonstrated its potential in both organic and inorganic photovoltaics (PVs), what remains to be addressed is quantitative understanding of how different ET modes contribute to PV performance and how ET contribution is differentiated from the classical optical coupling (OC) effects. In this study, we implement an ET scheme using a PV device platform, comprising CdSe/ZnS nanocrystal energy donor and 500 nm-thick ultrathin Si acceptor layers, and present the quantitative mechanistic description of how different ET modes, distinguished from themore » OC effects, increase the light absorption and PV efficiency. We find that nanocrystal sensitization enhances the short circuit current of ultrathin Si solar cells by up to 35%, of which the efficient ET, primarily driven by a long-range radiative mode, contributes to 38% of the total current enhancement. Lastly, these results not only confirm the positive impact of ET but also provide a guideline for rationally combining the ET and OC effects for improved light harvesting in PV and other optoelectronic devices.« less

  9. Enhanced photovoltaic performance of ultrathin Si solar cells via semiconductor nanocrystal sensitization: energy transfer vs. optical coupling effects.

    PubMed

    Hoang, Son; Ashraf, Ahsan; Eisaman, Matthew D; Nykypanchuk, Dmytro; Nam, Chang-Yong

    2016-03-21

    Excitonic energy transfer (ET) offers exciting opportunities for advances in optoelectronic devices such as solar cells. While recent experimental attempts have demonstrated its potential in both organic and inorganic photovoltaics (PVs), what remains to be addressed is quantitative understanding of how different ET modes contribute to PV performance and how ET contribution is differentiated from the classical optical coupling (OC) effects. In this study, we implement an ET scheme using a PV device platform, comprising CdSe/ZnS nanocrystal energy donor and 500 nm-thick ultrathin Si acceptor layers, and present the quantitative mechanistic description of how different ET modes, distinguished from the OC effects, increase the light absorption and PV efficiency. We find that nanocrystal sensitization enhances the short circuit current of ultrathin Si solar cells by up to 35%, of which the efficient ET, primarily driven by a long-range radiative mode, contributes to 38% of the total current enhancement. These results not only confirm the positive impact of ET but also provide a guideline for rationally combining the ET and OC effects for improved light harvesting in PV and other optoelectronic devices.

  10. Giant photoluminescence enhancement in SiC nanocrystals by resonant semiconductor exciton-metal surface plasmon coupling

    NASA Astrophysics Data System (ADS)

    Dai, Dejian; Dong, Zhenggao; Fan, Jiyang

    2013-01-01

    We report giant fluorescence enhancement in SiC nanocrystals (NCs) embedded in a sodium dodecyl sulfonate dielectric medium by proximately contacted Ag nanoparticles. The enhancement in integrated fluorescence intensity reaches an astonishing 176-fold under 360 nm excitation (53.3-fold enhancement in emission maximum intensity). Finite-element simulation indicates that the strong resonant coupling between the excited SiC NCs and localized surface plasmons of the Ag nanoparticles plays a dominant role in determining fluorescence enhancement. In contrast, the absorption enhancement caused by light concentration around the Ag nanoparticles makes only a slight contribution to the overall enhancement. Our result opens the possibility of applications of these highly enhanced fluorescent SiC NCs in diverse areas such as sensing, optoelectronics and life sciences.

  11. Giant photoluminescence enhancement in SiC nanocrystals by resonant semiconductor exciton-metal surface plasmon coupling.

    PubMed

    Dai, Dejian; Dong, Zhenggao; Fan, Jiyang

    2013-01-18

    We report giant fluorescence enhancement in SiC nanocrystals (NCs) embedded in a sodium dodecyl sulfonate dielectric medium by proximately contacted Ag nanoparticles. The enhancement in integrated fluorescence intensity reaches an astonishing 176-fold under 360 nm excitation (53.3-fold enhancement in emission maximum intensity). Finite-element simulation indicates that the strong resonant coupling between the excited SiC NCs and localized surface plasmons of the Ag nanoparticles plays a dominant role in determining fluorescence enhancement. In contrast, the absorption enhancement caused by light concentration around the Ag nanoparticles makes only a slight contribution to the overall enhancement. Our result opens the possibility of applications of these highly enhanced fluorescent SiC NCs in diverse areas such as sensing, optoelectronics and life sciences. PMID:23238520

  12. Determination of active doping in highly resistive boron doped silicon nanocrystals embedded in SiO2 by capacitance voltage measurement on inverted metal oxide semiconductor structure

    NASA Astrophysics Data System (ADS)

    Zhang, Tian; Puthen-Veettil, Binesh; Wu, Lingfeng; Jia, Xuguang; Lin, Ziyun; Yang, Terry Chien-Jen; Conibeer, Gavin; Perez-Wurfl, Ivan

    2015-10-01

    We investigate the Capacitance-Voltage (CV) measurement to study the electrically active boron doping in Si nanocrystals (ncSi) embedded in SiO2. The ncSi thin films with high resistivity (200-400 Ω cm) can be measured by using an inverted metal oxide semiconductor (MOS) structure (Al/ncSi (B)/SiO2/Si). This device structure eliminates the complications from the effects of lateral current flow and the high sheet resistance in standard lateral MOS structures. The characteristic MOS CV curves observed are consistent with the effective p-type doping. The CV modeling method is presented and used to evaluate the electrically active doping concentration. We find that the highly boron doped ncSi films have electrically active doping of 1018-1019 cm-3 despite their high resistivity. The saturation of doping at about 1.4 × 1019 cm-3 and the low doping efficiency less than 5% are observed and discussed. The calculated effective mobility is in the order of 10-3 cm2/V s, indicating strong impurity/defect scattering effect that hinders carriers transport.

  13. Determination of active doping in highly resistive boron doped silicon nanocrystals embedded in SiO{sub 2} by capacitance voltage measurement on inverted metal oxide semiconductor structure

    SciTech Connect

    Zhang, Tian Puthen-Veettil, Binesh; Wu, Lingfeng; Jia, Xuguang; Lin, Ziyun; Yang, Terry Chien-Jen; Conibeer, Gavin; Perez-Wurfl, Ivan

    2015-10-21

    We investigate the Capacitance-Voltage (CV) measurement to study the electrically active boron doping in Si nanocrystals (ncSi) embedded in SiO{sub 2}. The ncSi thin films with high resistivity (200–400 Ω cm) can be measured by using an inverted metal oxide semiconductor (MOS) structure (Al/ncSi (B)/SiO{sub 2}/Si). This device structure eliminates the complications from the effects of lateral current flow and the high sheet resistance in standard lateral MOS structures. The characteristic MOS CV curves observed are consistent with the effective p-type doping. The CV modeling method is presented and used to evaluate the electrically active doping concentration. We find that the highly boron doped ncSi films have electrically active doping of 10{sup 18}–10{sup 19 }cm{sup −3} despite their high resistivity. The saturation of doping at about 1.4 × 10{sup 19 }cm{sup −3} and the low doping efficiency less than 5% are observed and discussed. The calculated effective mobility is in the order of 10{sup −3} cm{sup 2}/V s, indicating strong impurity/defect scattering effect that hinders carriers transport.

  14. Sorting fluorescent nanocrystals with DNA

    SciTech Connect

    Gerion, Daniele; Parak, Wolfgang J.; Williams, Shara C.; Zanchet, Daniela; Micheel, Christine M.; Alivisatos, A. Paul

    2001-12-10

    Semiconductor nanocrystals with narrow and tunable fluorescence are covalently linked to oligonucleotides. These biocompounds retain the properties of both nanocrystals and DNA. Therefore, different sequences of DNA can be coded with nanocrystals and still preserve their ability to hybridize to their complements. We report the case where four different sequences of DNA are linked to four nanocrystal samples having different colors of emission in the range of 530-640 nm. When the DNA-nanocrystal conjugates are mixed together, it is possible to sort each type of nanoparticle using hybridization on a defined micrometer -size surface containing the complementary oligonucleotide. Detection of sorting requires only a single excitation source and an epifluorescence microscope. The possibility of directing fluorescent nanocrystals towards specific biological targets and detecting them, combined with their superior photo-stability compared to organic dyes, opens the way to improved biolabeling experiments, such as gene mapping on a nanometer scale or multicolor microarray analysis.

  15. Large-scale, solution-phase growth of semiconductor nanocrystals into ultralong one-dimensional arrays and study of their electrical properties

    NASA Astrophysics Data System (ADS)

    Ma, Yuchao; Xue, Mengmeng; Shi, Jiahua; Tan, Yiwei

    2014-05-01

    One-dimensional (1D) assemblies of semiconductor nanocrystals (NCs) represent an important kind of 1D nanomaterial system due to their potential for exploring novel and enhanced electronic and photonic performances of devices. Herein, we present mass fabrication of a series of 1D arrays of CdSe and PbSe NCs on a large length scale with ultralong, aligned Se nanowires (NWs) as both the reactant and structure-directing template. The 1D self-assembly patterns are the anchored growth of CdSe quantum dots (QDs) on the surface of Se NWs (i.e., 1D Se NWs/CdSe QDs core-shell heterostructure) and 1D aggregates of unsupported PbSe NCs formed by substantially increased collective particle-particle interactions. The size of CdSe QDs and shape of PbSe NCs in the 1D arrays can be effectively controlled by varying the synthetic conditions. Room temperature electrical measurements on the 1D Se/CdSe heterostructure field effect transistors (FETs) exhibit a pronounced improvement in the on/off ratio, device carrier mobility, and transconductance compared to the Se NW FETs fabricated in parallel. Furthermore, upon visible light excitation, the photocurrent from the Se/CdSe heterostructure FETs responses sharply (small time constant) and increases linearly with increasing the light intensity, indicating excellent photoconductive properties.One-dimensional (1D) assemblies of semiconductor nanocrystals (NCs) represent an important kind of 1D nanomaterial system due to their potential for exploring novel and enhanced electronic and photonic performances of devices. Herein, we present mass fabrication of a series of 1D arrays of CdSe and PbSe NCs on a large length scale with ultralong, aligned Se nanowires (NWs) as both the reactant and structure-directing template. The 1D self-assembly patterns are the anchored growth of CdSe quantum dots (QDs) on the surface of Se NWs (i.e., 1D Se NWs/CdSe QDs core-shell heterostructure) and 1D aggregates of unsupported PbSe NCs formed by substantially

  16. SEMICONDUCTOR DEVICES Density-controllable nonvolatile memory devices having metal nanocrystals through chemical synthesis and assembled by spin-coating technique

    NASA Astrophysics Data System (ADS)

    Guangli, Wang; Yubin, Chen; Yi, Shi; Lin, Pu; Lijia, Pan; Rong, Zhang; Youdou, Zheng

    2010-12-01

    A novel two-step method is employed, for the first time, to fabricate nonvolatile memory devices that have metal nanocrystals. First, size-averaged Au nanocrystals are synthesized chemically; second, they are assembled into memory devices by a spin-coating technique at room temperature. This attractive approach makes it possible to tailor the diameter and control the density of nanocrystals individually. In addition, processes at room temperature prevent Au diffusion, which is a main concern for the application of metal nanocrystal-based memory. The experimental results, both the morphology characterization and the electrical measurements, reveal that there is an optimum density of nanocrystal monolayer to balance between long data retention and a large hysteresis memory window. At the same time, density-controllable devices could also feed the preferential emphasis on either memory window or retention time. All these facts confirm the advantages and novelty of our two-step method.

  17. Composite material including nanocrystals and methods of making

    DOEpatents

    Bawendi, Moungi G.; Sundar, Vikram C.

    2010-04-06

    Temperature-sensing compositions can include an inorganic material, such as a semiconductor nanocrystal. The nanocrystal can be a dependable and accurate indicator of temperature. The intensity of emission of the nanocrystal varies with temperature and can be highly sensitive to surface temperature. The nanocrystals can be processed with a binder to form a matrix, which can be varied by altering the chemical nature of the surface of the nanocrystal. A nanocrystal with a compatibilizing outer layer can be incorporated into a coating formulation and retain its temperature sensitive emissive properties.

  18. Composite material including nanocrystals and methods of making

    DOEpatents

    Bawendi, Moungi G.; Sundar, Vikram C.

    2008-02-05

    Temperature-sensing compositions can include an inorganic material, such as a semiconductor nanocrystal. The nanocrystal can be a dependable and accurate indicator of temperature. The intensity of emission of the nanocrystal varies with temperature and can be highly sensitive to surface temperature. The nanocrystals can be processed with a binder to form a matrix, which can be varied by altering the chemical nature of the surface of the nanocrystal. A nanocrystal with a compatibilizing outer layer can be incorporated into a coating formulation and retain its temperature sensitive emissive properties

  19. Semiconductor nanowhiskers: Synthesis, properties, and applications

    SciTech Connect

    Dubrovskii, V. G. Cirlin, G. E. Ustinov, V. M.

    2009-12-15

    Recent results of studying the semiconductor's whisker nanocrystals are reviewed. Physical grounds of growing whisker nanocrystals using the mechanism vapor-liquid-crystal are given and the main epitaxial technologies of synthesis of whisker nanocrystals are described. Thermodynamic and kinetic factors controlling the morphological properties, composition, and crystal structure of whisker nanocrystals are considered in detail. The main theoretical models of the growth and structure of whisker nanocrystals are described. The data on physical properties of whisker nanocrystals and possibilities of their use in nanophotonics, nanoelectronics, and nanobiotechnology are presented.

  20. Modulation Spectroscopy of Semiconductor Nanocrystals

    NASA Astrophysics Data System (ADS)

    Stokes, Kevin L.

    1995-11-01

    The optical and electro-optical properties of nanometer-sized CdS_{X}Se _{1-X} crystallites embedded in a glass matrix are investigated. The goal of this study is to understand not only the effect of confinement on the electronic energy levels, but also the nature of the electron-hole excited states and their response to electric field. Electro- and photo- modulated absorption spectroscopies are the primary experimental tools. The electric-field response of CdS_ {0.44}Se_{0.56} nanoparticles in glass is studied as a function of particle size using electroabsorption spectroscopy. New transitions appear as confinement increases--up to six quantum-size levels can be observed in the data. The evolution of the transitions through many particle sizes provides evidence for mixing of the valence bands due to quantum confinement. Transitions involving electron-hole envelope functions with S-like symmetry are the most sensitive to electric field. The electromodulated absorption data were fit with a first-derivative lineshape function to separate the effects of the electric field on the energy level, width, and oscillator strength associated with each electron -hole state. The electroabsorption magnitude is a strong function of particle size and the modulation mechanisms also change with particle size. Frequency-, intensity- and temperature-dependent photoabsorption were used to study deep trap states in CdS_{0.44}Se_ {0.56} particles in glass. The photo -induced change in absorption consists of two components: (1) bleaching, due to phase-space filling of the lowest excited state and (2) a carrier-induced electric-field effect involving a long-lived trap state. The electroabsorption lineshape in the large (R = 6.2 nm) particles is found to be sensitive to the intensity of an additional pump beam. This effect is caused by the formation of two electron-hole pair states in the nanoparticle. One electron-hole pair is bound to a long-lived trap and the second electron-hole state behaves like a free exciton. The resulting electroabsorption spectrum is essentially the electric-field-induced change in the second (free) electron -hole state. Implications for the interpretation of electroabsorption lineshapes are discussed. No similar effect is observed in smaller particles.

  1. The dual role of sulfur-containing amino acids in the synthesis of IV-VI semiconductor nanocrystals: a mechanochemical approach.

    PubMed

    Baláž, Peter; Baláž, Matej; Caplovičová, Mária; Zorkovská, Anna; Caplovič, Lubomír; Psotka, Miroslav

    2014-01-01

    PbS@cystine nanocrystals were synthesized mechanochemically, with lead acetate and L-cystine being used as the lead and sulfur precursors, respectively. The resulting nanocrystals are 22-34 nm in size, well-faceted and octahedral in shape. Characterization by XRD, FT-IR, NMR, FE-SEM, EDS, TEM (HRTEM) and surface area measurement methods showed that the particles are single, defect-free crystals with a high crystallinity. Furthermore, the crystals were prepared using a solvent-free procedure that was performed under ambient temperature and atmospheric pressure. PMID:25406478

  2. Manipulation of structural and optical properties in charge-separating ZnTe/ZnSe chalcogenide core/shell semiconductor nanocrystals: Atomistic tight-binding theory

    NASA Astrophysics Data System (ADS)

    Sukkabot, Worasak

    2015-11-01

    The atomistic tight-binding theory (TB) is utilized to study the electronic structures and optical properties of type-II ZnTe/ZnSe chalcogenide core/shell nanocrystals. The purpose of the present study is to theoretically understand the atomistic impact of the ZnSe growth shell on the single-particle spectra, charge densities, optical band gaps, electron-hole overlaps and oscillation strengths. The sensitivity of ZnSe growth shell thickness in analyzing the electronic structures and optical properties of ZnTe/ZnSe core/shell nanocrystals reflects the charge separation of type-II band alignment. The comprehensive calculations of ZnTe/ZnSe core/shell nanocrystals are effectively manipulated by including and changing the ZnSe growth shell thickness. As a comparison, the atomistic tight-binding calculations demonstrate a reasonable agreement with effective mass approximation and experiment. Finally, the computations successfully discover the important factors of the growth shell on the natural behaviors of type-II ZnTe/ZnSe core/shell nanocrystals which affords a guideline to be implemented to the novel electronic cadmium-free nanodevices and the environmentally friendly applications.

  3. Biomolecular Assembly of Gold Nanocrystals

    SciTech Connect

    Micheel, Christine Marya

    2005-05-20

    Over the past ten years, methods have been developed to construct discrete nanostructures using nanocrystals and biomolecules. While these frequently consist of gold nanocrystals and DNA, semiconductor nanocrystals as well as antibodies and enzymes have also been used. One example of discrete nanostructures is dimers of gold nanocrystals linked together with complementary DNA. This type of nanostructure is also known as a nanocrystal molecule. Discrete nanostructures of this kind have a number of potential applications, from highly parallel self-assembly of electronics components and rapid read-out of DNA computations to biological imaging and a variety of bioassays. My research focused in three main areas. The first area, the refinement of electrophoresis as a purification and characterization method, included application of agarose gel electrophoresis to the purification of discrete gold nanocrystal/DNA conjugates and nanocrystal molecules, as well as development of a more detailed understanding of the hydrodynamic behavior of these materials in gels. The second area, the development of methods for quantitative analysis of transmission electron microscope data, used computer programs written to find pair correlations as well as higher order correlations. With these programs, it is possible to reliably locate and measure nanocrystal molecules in TEM images. The final area of research explored the use of DNA ligase in the formation of nanocrystal molecules. Synthesis of dimers of gold particles linked with a single strand of DNA possible through the use of DNA ligase opens the possibility for amplification of nanostructures in a manner similar to polymerase chain reaction. These three areas are discussed in the context of the work in the Alivisatos group, as well as the field as a whole.

  4. Incorporation of Cu Acceptors in ZnO Nanocrystals

    SciTech Connect

    Oo, W.M.H.; Mccluskey, Matthew D.; Huso, Jesse; Morrison, J.; Bergman, Leah; Engelhard, Mark H.; Saraf, Laxmikant V.

    2010-09-16

    Doping of semiconductor nanocrystals is an important problem in nanomaterials research. Using infrared (IR) and x-ray photoelectron spectroscopy (XPS), we have observed Cu acceptor dopants that were intentionally introduced into ZnO nanocrystals. The incorporation of Cu2+ dopants increased as the diameter of the nanocrystals was increased from ~3 to 5 nm. Etching the nanocrystals with acetic acid revealed a core-shell structure, where a 2-nm lightly doped core is surrounded by a heavily doped shell. These observations are consistent with the trapped dopant model, in which dopant atoms stick to the surface of the core and are overgrown by the nanocrystal material.

  5. Picosecond dynamics of photoexcited carriers in interacting silicon nanocrystals

    NASA Astrophysics Data System (ADS)

    Kořínek, Miroslav; Trojánek, František; Hiller, Daniel; Gutsch, Sebastian; Zacharias, Margit; Kübel, Christian; Malý, Petr

    2016-07-01

    The non-radiative Auger carrier recombination plays an important role in physics and the application of semiconductor nanocrystals. Here we report on the effect of inter-nanocrystal carrier interaction on Auger recombination. We prepared a special set of samples containing silicon nanocrystals embedded in silicon oxide with well-defined geometry. The picosecond carrier recombination rate measured by femtosecond pump and probe technique was found to be strongly dependent on the inter-nanocrystal separation. The observed decrease of the decay rate with nanocrystal separation on the nanometer scale is interpreted in terms of the wave function overlap appearing in the relevant matrix element describing the recombination process.

  6. Electronic states of lead salt nanocrystal and nanocrystal assemblies

    NASA Astrophysics Data System (ADS)

    Yang, Jun

    With the development of new synthetic methods, semiconductor nanocrystals of various morphologies and dimensions have been created. This changes their electro-optical properties, and brings new questions in understanding. At the same time, more and more research is now focused on nanocrystal assemblies, in particular nanocrystal superlattices with atomically coherent lattices, with the potential for various optoelectronic device applications. This thesis examines, in both theory and experiment, a number of nanocrystal systems, with the stress on dimensionality and morphology. In particular, in 1D and 2D systems, due to the anisotropic quantum connenment, the electrons and holes will form a tightly bond excitons, even at room temperature, in contrast to 0D and 3D systems, where either quantum connenment or coulomb interaction completely dominates. We'll also look into nanocrystal assemblies, both amorphous and atomically coherent, and study the effect of the inherent disorder in the structure on their electronic properties, with the goal of charge transportation through delocalized states. Last, we'll examine the ne structure in these nanocrystals.

  7. Size-Dependent Raman Shifts for nanocrystals

    PubMed Central

    Gao, Yukun; Zhao, Xinmei; Yin, Penggang; Gao, Faming

    2016-01-01

    Raman spectroscopy is a very sensitive tool for probing semiconductor nanocrystals. The underlying mechanism behind the size-dependent Raman shifts is still quite controversial. Here we offer a new theoretical method for the quantum confinement effects on the Raman spectra of semiconductor nanocrystals. We propose that the shift of Raman spectra in nanocrystals can result from two overlapping effects: the quantum effect shift and surface effect shift. The quantum effect shift is extracted from an extended Kubo formula, the surface effect shift is determined via the first principles calculations. Fairly good prediction of Raman shifts can be obtained without the use of any adjustable parameter. Closer analysis shows that the size-dependent Raman shifts in Si nanocrystals mainly result from the quantum effect shifts. For nanodiamond, the proportion of surface effect shift in Raman shift is up to about 40%. Such model can also provide a good baseline for using Raman spectroscopy as a tool to measure size. PMID:27102066

  8. Size-Dependent Raman Shifts for nanocrystals.

    PubMed

    Gao, Yukun; Zhao, Xinmei; Yin, Penggang; Gao, Faming

    2016-04-22

    Raman spectroscopy is a very sensitive tool for probing semiconductor nanocrystals. The underlying mechanism behind the size-dependent Raman shifts is still quite controversial. Here we offer a new theoretical method for the quantum confinement effects on the Raman spectra of semiconductor nanocrystals. We propose that the shift of Raman spectra in nanocrystals can result from two overlapping effects: the quantum effect shift and surface effect shift. The quantum effect shift is extracted from an extended Kubo formula, the surface effect shift is determined via the first principles calculations. Fairly good prediction of Raman shifts can be obtained without the use of any adjustable parameter. Closer analysis shows that the size-dependent Raman shifts in Si nanocrystals mainly result from the quantum effect shifts. For nanodiamond, the proportion of surface effect shift in Raman shift is up to about 40%. Such model can also provide a good baseline for using Raman spectroscopy as a tool to measure size.

  9. Artificial atoms on semiconductor surfaces

    PubMed Central

    Tisdale, W. A.; Zhu, X.-Y.

    2011-01-01

    Semiconductor nanocrystals are called artificial atoms because of their atom-like discrete electronic structure resulting from quantum confinement. Artificial atoms can also be assembled into artificial molecules or solids, thus, extending the toolbox for material design. We address the interaction of artificial atoms with bulk semiconductor surfaces. These interfaces are model systems for understanding the coupling between localized and delocalized electronic structures. In many perceived applications, such as nanoelectronics, optoelectronics, and solar energy conversion, interfacing semiconductor nanocrystals to bulk materials is a key ingredient. Here, we apply the well established theories of chemisorption and interfacial electron transfer as conceptual frameworks for understanding the adsorption of semiconductor nanocrystals on surfaces, paying particular attention to instances when the nonadiabatic Marcus picture breaks down. We illustrate these issues using recent examples from our laboratory. PMID:21097704

  10. Hybrid pn-junction solar cells based on layers of inorganic nanocrystals and organic semiconductors: optimization of layer thickness by considering the width of the depletion region.

    PubMed

    Saha, Sudip K; Guchhait, Asim; Pal, Amlan J

    2014-03-01

    We report the formation and characterization of hybrid pn-junction solar cells based on a layer of copper diffused silver indium disulfide (AgInS2@Cu) nanoparticles and another layer of copper phthalocyanine (CuPc) molecules. With copper diffusion in the nanocrystals, their optical absorption and hence the activity of the hybrid pn-junction solar cells was extended towards the near-IR region. To decrease the particle-to-particle separation for improved carrier transport through the inorganic layer, we replaced the long-chain ligands of copper-diffused nanocrystals in each monolayer with short-ones. Under illumination, the hybrid pn-junctions yielded a higher short-circuit current as compared to the combined contribution of the Schottky junctions based on the components. A wider depletion region at the interface between the two active layers in the pn-junction device as compared to that of the Schottky junctions has been considered to analyze the results. Capacitance-voltage characteristics under a dark condition supported such a hypothesis. We also determined the width of the depletion region in the two layers separately so that a pn-junction could be formed with a tailored thickness of the two materials. Such a "fully-depleted" device resulted in an improved photovoltaic performance, primarily due to lessening of the internal resistance of the hybrid pn-junction solar cells.

  11. Enhanced photovoltaic performance of ultrathin Si solar cells via semiconductor nanocrystal sensitization: Energy transfer vs. optical coupling effects

    SciTech Connect

    Hoang, Son; Ashraf, Ahsan; Eisaman, Matthew D.; Nykypanchuk, Dmytro; Nam, Chang -Yong

    2015-12-07

    Excitonic energy transfer (ET) offers exciting opportunities for advances in optoelectronic devices such as solar cells. While recent experimental attempts have demonstrated its potential in both organic and inorganic photovoltaics (PVs), what remains to be addressed is quantitative understanding of how different ET modes contribute to PV performance and how ET contribution is differentiated from the classical optical coupling (OC) effects. In this study, we implement an ET scheme using a PV device platform, comprising CdSe/ZnS nanocrystal energy donor and 500 nm-thick ultrathin Si acceptor layers, and present the quantitative mechanistic description of how different ET modes, distinguished from the OC effects, increase the light absorption and PV efficiency. We find that nanocrystal sensitization enhances the short circuit current of ultrathin Si solar cells by up to 35%, of which the efficient ET, primarily driven by a long-range radiative mode, contributes to 38% of the total current enhancement. Lastly, these results not only confirm the positive impact of ET but also provide a guideline for rationally combining the ET and OC effects for improved light harvesting in PV and other optoelectronic devices.

  12. Hybrid pn-junction solar cells based on layers of inorganic nanocrystals and organic semiconductors: optimization of layer thickness by considering the width of the depletion region.

    PubMed

    Saha, Sudip K; Guchhait, Asim; Pal, Amlan J

    2014-03-01

    We report the formation and characterization of hybrid pn-junction solar cells based on a layer of copper diffused silver indium disulfide (AgInS2@Cu) nanoparticles and another layer of copper phthalocyanine (CuPc) molecules. With copper diffusion in the nanocrystals, their optical absorption and hence the activity of the hybrid pn-junction solar cells was extended towards the near-IR region. To decrease the particle-to-particle separation for improved carrier transport through the inorganic layer, we replaced the long-chain ligands of copper-diffused nanocrystals in each monolayer with short-ones. Under illumination, the hybrid pn-junctions yielded a higher short-circuit current as compared to the combined contribution of the Schottky junctions based on the components. A wider depletion region at the interface between the two active layers in the pn-junction device as compared to that of the Schottky junctions has been considered to analyze the results. Capacitance-voltage characteristics under a dark condition supported such a hypothesis. We also determined the width of the depletion region in the two layers separately so that a pn-junction could be formed with a tailored thickness of the two materials. Such a "fully-depleted" device resulted in an improved photovoltaic performance, primarily due to lessening of the internal resistance of the hybrid pn-junction solar cells. PMID:24452695

  13. Synthesis and Doping of Silicon Nanocrystals for Versatile Nanocrystal Inks

    NASA Astrophysics Data System (ADS)

    Kramer, Nicolaas Johannes

    The impact of nanotechnology on our society is getting larger every year. Electronics are becoming smaller and more powerful, the "Internet of Things" is all around us, and data generation is increasing exponentially. None of this would have been possible without the developments in nanotechnology. Crystalline semiconductor nanoparticles (nanocrystals) are one of the latest developments in the field of nanotechnology. This thesis addresses three important challenges for the transition of silicon nanocrystals from the lab bench to the marketplace: A better understanding of the nanocrystal synthesis was obtained, the electronic properties of the nanocrystals were characterized and tuned, and novel silicon nanocrystal inks were formed and applied using simple coating technologies. Plasma synthesis of nanocrystals has numerous advantages over traditional solution-based synthesis methods. While the formation of nanoparticles in low pressure nonthermal plasmas is well known, the heating mechanism leading to their crystallization is poorly understood. A combination of comprehensive plasma characterization with a nanoparticle heating model presented here reveals the underlying plasma physics leading to crystallization. The model predicts that the nanoparticles reach temperatures as high as 900 K in the plasma as a result of heating reactions on the nanoparticle surface. These temperatures are well above the gas temperature and sufficient for complete nanoparticle crystallization. Moving the field of plasma nanoparticle synthesis to atmospheric pressures is important for lowering its cost and making the process attractive for industrial applications. The heating and charging model for silicon nanoparticles was adapted in Chapter 3 to study plasmas maintained over a wide range of pressures (10 -- 105 Pa). The model considers three collisionality regimes and determines the dominant contribution of each regime under various plasma conditions. Strong nanoparticle cooling at

  14. Aerosol printing of colloidal nanocrystals by aerodynamic focusing

    NASA Astrophysics Data System (ADS)

    Qi, Lejun

    Colloidal semiconductor nanocrystals, or quantum dots, have shown promise as the active material in electronic and optoelectronic applications, because of their high quantum yield, narrow spectral emission band, size-tunable bandgap, chemical stability, and easy processibility. Meanwhile, it is still challenging to print patterns of nanocrystal films with desired linewidth and thickness, which is a critical step in fabrication of nanocrystal-based devices. In this thesis, a direct-write method of colloidal semiconductor nanocrystals has been developed. Like other direct-write techniques, this aerosol based method simplifies printing process and reduces the manufacturing cost, as it avoids mask screening, lithography, and pre-patterning of the substrate. Moreover, the aerosol printing with aerodynamic lenses needs neither microscale nozzles nor sheath gases, and is able to incorporate into the vacuum systems currently used in microelectronic fabrication. This thesis research presents systematic efforts to develop an aerosol-based method to directly write patterns of semiconductor nanocrystals from colloidal dispersions by aerodynamic focusing. First, the synthesized colloidal nanocrystals in hexane were nebulized into compact and spherical agglomerates suspending in the carrier gas. The details about the impact dynamics of individual aerosolized nanocrystal agglomerates were investigated. As building blocks of printed nanocrystal films, the agglomerate exhibited cohesive and granular behaviors during impact deformation on the substrate. The strength of cohesion between nanocrystals in the agglomerates could be adjusted by tuning the number concentration of colloidal nanocrystal dispersion. Second, ultrathin films of nanocrystals were obtained by printing monodisperse nanocrystal agglomerates. As the result of the granular property of nanocrystal agglomerates, it was found that the thickness of deposited agglomerates strongly depended on the size of agglomerates. A

  15. The Surface Chemistry of Metal Chalcogenide Nanocrystals

    NASA Astrophysics Data System (ADS)

    Anderson, Nicholas Charles

    The surface chemistry of metal chalcogenide nanocrystals is explored through several interrelated analytical investigations. After a brief discussion of the nanocrystal history and applications, molecular orbital theory is used to describe the electronic properties of semiconductors, and how these materials behave on the nanoscale. Quantum confinement plays a major role in dictating the optical properties of metal chalcogenide nanocrystals, however surface states also have an equally significant contribution to the electronic properties of nanocrystals due to the high surface area to volume ratio of nanoscale semiconductors. Controlling surface chemistry is essential to functionalizing these materials for biological imaging and photovoltaic device applications. To better understand the surface chemistry of semiconducting nanocrystals, three competing surface chemistry models are presented: 1.) The TOPO model, 2.) the Non-stoichiometric model, and 3.) the Neutral Fragment model. Both the non-stoichiometric and neutral fragment models accurately describe the behavior of metal chalcogenide nanocrystals. These models rely on the covalent bond classification system, which divides ligands into three classes: 1.) X-type, 1-electron donating ligands that balance charge with excess metal at the nanocrystal surface, 2.) L-type, 2-electron donors that bind metal sites, and 3.) Z-type, 2-electron acceptors that bind chalcogenide sites. Each of these ligand classes is explored in detail to better understand the surface chemistry of metal chalcogenide nanocrystals. First, chloride-terminated, tri-n-butylphosphine (Bu 3P) bound CdSe nanocrystals were prepared by cleaving carboxylate ligands from CdSe nanocrystals with chlorotrimethylsilane in Bu3P solution. 1H and 31P{1H} nuclear magnetic resonance spectra of the isolated nanocrystals allowed assignment of distinct signals from several free and bound species, including surface-bound Bu3P and [Bu3P-H]+[Cl]- ligands as well as a Bu

  16. Multifunctional nanocrystals

    DOEpatents

    Klimov, Victor I.; Hollingsworth, Jennifer A.; Crooker, Scott A.; Kim, Hyungrak

    2010-06-22

    Multifunctional nanocomposites are provided including a core of either a magnetic material or an inorganic semiconductor, and, a shell of either a magnetic material or an inorganic semiconductor, wherein the core and the shell are of differing materials, such multifunctional nanocomposites having multifunctional properties including magnetic properties from the magnetic material and optical properties from the inorganic semiconductor material. Various applications of such multifunctional nanocomposites are also provided.

  17. Multifunctional nanocrystals

    SciTech Connect

    Klimov, Victor I.; Hollingsworth, Jennifer A.; Crooker, Scott A.; Kim, Hyungrak

    2007-08-28

    Multifunctional nanocomposites are provided including a core of either a magnetic material or an inorganic semiconductor, and, a shell of either a magnetic material or an inorganic semiconductor, wherein the core and the shell are of differing materials, such multifunctional nanocomposites having multifunctional properties including magnetic properties from the magnetic material and optical properties from the inorganic semiconductor material. Various applications of such multifunctional nanocomposites are also provided.

  18. Patterning nanocrystals using DNA

    SciTech Connect

    Williams, Shara Carol

    2003-09-01

    One of the goals of nanotechnology is to enable programmed self-assembly of patterns made of various materials with nanometer-sized control. This dissertation describes the results of experiments templating arrangements of gold and semiconductor nanocrystals using 2'-deoxyribonucleic acid (DNA). Previously, simple DNA-templated linear arrangements of two and three nanocrystals structures have been made.[1] Here, we have sought to assemble larger and more complex nanostructures. Gold-DNA conjugates with 50 to 100 bases self-assembled into planned arrangements using strands of DNA containing complementary base sequences. We used two methods to increase the complexity of the arrangements: using branched synthetic doublers within the DNA covalent backbone to create discrete nanocrystal groupings, and incorporating the nanocrystals into a previously developed DNA lattice structure [2][3] that self-assembles from tiles made of DNA double-crossover molecules to create ordered nanoparticle arrays. In the first project, the introduction of a covalently-branched synthetic doubler reagent into the backbone of DNA strands created a branched DNA ''trimer.'' This DNA trimer templated various structures that contained groupings of three and four gold nanoparticles, giving promising, but inconclusive transmission electron microscopy (TEM) results. Due to the presence of a variety of possible structures in the reaction mixtures, and due to the difficulty of isolating the desired structures, the TEM and gel electrophoresis results for larger structures having four particles, and for structures containing both 5 and 10 nm gold nanoparticles were inconclusive. Better results may come from using optical detection methods, or from improved sample preparation. In the second project, we worked toward making two-dimensional ordered arrays of nanocrystals. We replicated and improved upon previous results for making DNA lattices, increasing the size of the lattices to a length greater than

  19. Recent Progress in Photocatalysis Mediated by Colloidal II-VI Nanocrystals.

    PubMed

    Wilker, Molly B; Schnitzenbaumer, Kyle J; Dukovic, Gordana

    2012-12-01

    The use of photoexcited electrons and holes in semiconductor nanocrystals as reduction and oxidation reagents is an intriguing way of harvesting photon energy to drive chemical reactions. This review focuses on recent research efforts to understand and control the photocatalytic processes mediated by colloidal II-VI nanocrystalline materials, such as cadmium and zinc chalcogenides. First, we highlight how nanocrystal properties govern the rates and efficiencies of charge-transfer processes relevant to photocatalysis. We then describe the use of nanocrystal catalyst heterostructures for fuel-forming reactions, most commonly H2 generation. Finally, we review the use of nanocrystal photocatalysis as a synthetic tool for metal-semiconductor nano-heterostructures.

  20. Synthesis and investigation of optical properties of TOPO-capped CuInS{sub 2} semiconductor nanocrystal in the presence of different solvent

    SciTech Connect

    Asgary, Saeid; Mirabbaszadeh, Kavoos; Nayebi, Payman; Emadi, Hamid

    2014-03-01

    Graphical abstract: - Highlights: • TOPO-capped CuInS{sub 2} nanoparticles were synthesized by injection method. • Pure CuInS{sub 2} nanoparticle was obtained by injection in 200 °C. • The size, shape and optical properties of products were controlled. • Nanoparticles with size smaller than 10 nm and wurtzite phase was obtained. • The absorption and PL spectra of CuInS{sub 2} nanoparticles were tunable. - Abstract: In this work, synthesis of CuInS{sub 2} semiconductor nanoparticles by thermolysis of a mixed solution of CuAc, In(Ac){sub 3} and DDT in coordinating solvent and trioctylphosphine oxide (TOPO) as ligand was developed. CuInS{sub 2} nanoparticles with size of −10 nm and nanorods were obtained and optical properties controlled by adjusting the reaction parameters such as temperature and time. Also the shape of nanoparticles was controlled by various solvents elaborately. The as-prepared nanoparticles were characterized by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), Scanning electron microscopy (SEM), UV–vis absorption, and photoluminescence (PL) spectroscopy. With the use of different solvent different morphology obtained. In the presence of oleylamine/octadecene rectangle-like nanorods obtained while with the use of oleic acid sphere-like nanoparticles achieved.

  1. Lead sulphide nanocrystal photodetector technologies

    NASA Astrophysics Data System (ADS)

    Saran, Rinku; Curry, Richard J.

    2016-02-01

    Light detection is the underlying principle of many optoelectronic systems. For decades, semiconductors including silicon carbide, silicon, indium gallium arsenide and germanium have dominated the photodetector industry. They can show excellent photosensitivity but are limited by one or more aspects, such as high production cost, high-temperature processing, flexible substrate incompatibility, limited spectral range or a requirement for cryogenic cooling for efficient operation. Recently lead sulphide (PbS) nanocrystals have emerged as one of the most promising new materials for photodetector fabrication. They offer several advantages including low-cost manufacturing, solution processability, size-tunable spectral sensitivity and flexible substrate compatibility, and they have achieved figures of merit outperforming conventional photodetectors. We review the underlying concepts, breakthroughs and remaining challenges in photodetector technologies based on PbS nanocrystals.

  2. Plasmonic engineering of spontaneous emission from silicon nanocrystals

    PubMed Central

    Goffard, Julie; Gérard, Davy; Miska, Patrice; Baudrion, Anne-Laure; Deturche, Régis; Plain, Jérôme

    2013-01-01

    Silicon nanocrystals offer huge advantages compared to other semi-conductor quantum dots as they are made from an abundant, non-toxic material and are compatible with silicon devices. Besides, among a wealth of extraordinary properties ranging from catalysis to nanomedicine, metal nanoparticles are known to increase the radiative emission rate of semiconductor quantum dots. Here, we use gold nanoparticles to accelerate the emission of silicon nanocrystals. The resulting integrated hybrid emitter is 5-fold brighter than bare silicon nanocrystals. We also propose an in-depth analysis highlighting the role of the different physical parameters in the photoluminescence enhancement phenomenon. This result has important implications for the practical use of silicon nanocrystals in optoelectronic devices, for instance for the design of efficient down-shifting devices that could be integrated within future silicon solar cells. PMID:24037020

  3. Plasmonic engineering of spontaneous emission from silicon nanocrystals.

    PubMed

    Goffard, Julie; Gérard, Davy; Miska, Patrice; Baudrion, Anne-Laure; Deturche, Régis; Plain, Jérôme

    2013-01-01

    Silicon nanocrystals offer huge advantages compared to other semi-conductor quantum dots as they are made from an abundant, non-toxic material and are compatible with silicon devices. Besides, among a wealth of extraordinary properties ranging from catalysis to nanomedicine, metal nanoparticles are known to increase the radiative emission rate of semiconductor quantum dots. Here, we use gold nanoparticles to accelerate the emission of silicon nanocrystals. The resulting integrated hybrid emitter is 5-fold brighter than bare silicon nanocrystals. We also propose an in-depth analysis highlighting the role of the different physical parameters in the photoluminescence enhancement phenomenon. This result has important implications for the practical use of silicon nanocrystals in optoelectronic devices, for instance for the design of efficient down-shifting devices that could be integrated within future silicon solar cells.

  4. Potentiometric Titrations for Measuring the Capacitance of Colloidal Photodoped ZnO Nanocrystals.

    PubMed

    Brozek, Carl K; Hartstein, Kimberly H; Gamelin, Daniel R

    2016-08-24

    Colloidal semiconductor nanocrystals offer a unique opportunity to bridge molecular and bulk semiconductor redox phenomena. Here, potentiometric titration is demonstrated as a method for quantifying the Fermi levels and charging potentials of free-standing colloidal n-type ZnO nanocrystals possessing between 0 and 20 conduction-band electrons per nanocrystal, corresponding to carrier densities between 0 and 1.2 × 10(20) cm(-3). Potentiometric titration of colloidal semiconductor nanocrystals has not been described previously, and little precedent exists for analogous potentiometric titration of any soluble reductants involving so many electrons. Linear changes in Fermi level vs charge-carrier density are observed for each ensemble of nanocrystals, with slopes that depend on the nanocrystal size. Analysis indicates that the ensemble nanocrystal capacitance is governed by classical surface electrical double layers, showing no evidence of quantum contributions. Systematic shifts in the Fermi level are also observed with specific changes in the identity of the charge-compensating countercation. As a simple and contactless alternative to more common thin-film-based voltammetric techniques, potentiometric titration offers a powerful new approach for quantifying the redox properties of colloidal semiconductor nanocrystals.

  5. Potentiometric Titrations for Measuring the Capacitance of Colloidal Photodoped ZnO Nanocrystals.

    PubMed

    Brozek, Carl K; Hartstein, Kimberly H; Gamelin, Daniel R

    2016-08-24

    Colloidal semiconductor nanocrystals offer a unique opportunity to bridge molecular and bulk semiconductor redox phenomena. Here, potentiometric titration is demonstrated as a method for quantifying the Fermi levels and charging potentials of free-standing colloidal n-type ZnO nanocrystals possessing between 0 and 20 conduction-band electrons per nanocrystal, corresponding to carrier densities between 0 and 1.2 × 10(20) cm(-3). Potentiometric titration of colloidal semiconductor nanocrystals has not been described previously, and little precedent exists for analogous potentiometric titration of any soluble reductants involving so many electrons. Linear changes in Fermi level vs charge-carrier density are observed for each ensemble of nanocrystals, with slopes that depend on the nanocrystal size. Analysis indicates that the ensemble nanocrystal capacitance is governed by classical surface electrical double layers, showing no evidence of quantum contributions. Systematic shifts in the Fermi level are also observed with specific changes in the identity of the charge-compensating countercation. As a simple and contactless alternative to more common thin-film-based voltammetric techniques, potentiometric titration offers a powerful new approach for quantifying the redox properties of colloidal semiconductor nanocrystals. PMID:27444048

  6. From ligands to binding motifs and beyond; the enhanced versatility of nanocrystal surfaces.

    PubMed

    De Roo, J; De Keukeleere, K; Hens, Z; Van Driessche, I

    2016-09-14

    Surface chemistry bridges the gap between nanocrystal synthesis and their applications. In this respect, the discovery of complex ligand binding motifs on semiconductor quantum dots and metal oxide nanocrystals opens a gateway to new areas of research. The implications are far-reaching, from catalytic model systems to the performance of solar cells. PMID:27461488

  7. Growth of platinum nanocrystals

    SciTech Connect

    2009-01-01

    Movie showing the growth of platinum nanocrystals in a liquid cell observed in situ using the JEOL 3010 TEM at the National Center for Electron Microscopy. This is the first ever-real time movie showing nucleation and growth by monomer attachment or by smaller nanocrystals coalescing to form larger nanocrystals. All the nanocrystals end up being roughly the same shape and size. http://newscenter.lbl.gov/feature-stories/2009/08/04/growth-spurts/

  8. Field-effect electroluminescence in silicon nanocrystals.

    PubMed

    Walters, Robert J; Bourianoff, George I; Atwater, Harry A

    2005-02-01

    There is currently worldwide interest in developing silicon-based active optical components in order to leverage the infrastructure of silicon microelectronics technology for the fabrication of optoelectronic devices. Light emission in bulk silicon-based devices is constrained in wavelength to infrared emission, and in efficiency by the indirect bandgap of silicon. One promising strategy for overcoming these challenges is to make use of quantum-confined excitonic emission in silicon nanocrystals. A critical challenge for silicon nanocrystal devices based on nanocrystals embedded in silicon dioxide has been the development of a method for efficient electrical carrier injection. We report here a scheme for electrically pumping dense silicon nanocrystal arrays by a field-effect electroluminescence mechanism. In this excitation process, electrons and holes are both injected from the same semiconductor channel across a tunnelling barrier in a sequential programming process, in contrast to simultaneous carrier injection in conventional pn-junction light-emitting-diode structures. Light emission is strongly correlated with the injection of a second carrier into a nanocrystal that has been previously programmed with a charge of the opposite sign.

  9. Fabrication and electronic transport studies of single nanocrystal systems

    SciTech Connect

    Klein, D L

    1997-05-01

    Semiconductor and metallic nanocrystals exhibit interesting electronic transport behavior as a result of electrostatic and quantum mechanical confinement effects. These effects can be studied to learn about the nature of electronic states in these systems. This thesis describes several techniques for the electronic study of nanocrystals. The primary focus is the development of novel methods to attach leads to prefabricated nanocrystals. This is because, while nanocrystals can be readily synthesized from a variety of materials with excellent size control, means to make electrical contact to these nanocrystals are limited. The first approach that will be described uses scanning probe microscopy to first image and then electrically probe surfaces. It is found that electronic investigations of nanocrystals by this technique are complicated by tip-sample interactions and environmental factors such as salvation and capillary forces. Next, an atomic force microscope technique for the catalytic patterning of the surface of a self assembled monolayer is described. In principle, this nano-fabrication technique can be used to create electronic devices which are based upon complex arrangements of nanocrystals. Finally, the fabrication and electrical characterization of a nanocrystal-based single electron transistor is presented. This device is fabricated using a hybrid scheme which combines electron beam lithography and wet chemistry to bind single nanocrystals in tunneling contact between closely spaced metallic leads. In these devices, both Au and CdSe nanocrystals show Coulomb blockade effects with characteristic energies of several tens of meV. Additional structure is seen the transport behavior of CdSe nanocrystals as a result of its electronic structure.

  10. Low temperature thin films formed from nanocrystal precursors

    DOEpatents

    Alivisatos, A.P.; Goldstein, A.N.

    1993-11-16

    Nanocrystals of semiconductor compounds are produced. When they are applied as a contiguous layer onto a substrate and heated they fuse into a continuous layer at temperatures as much as 250, 500, 750 or even 1000 K below their bulk melting point. This allows continuous semiconductor films in the 0.25 to 25 nm thickness range to be formed with minimal thermal exposure. 9 figures.

  11. Low temperature thin films formed from nanocrystal precursors

    DOEpatents

    Alivisatos, A. Paul; Goldstein, Avery N.

    1993-01-01

    Nanocrystals of semiconductor compounds are produced. When they are applied as a contiguous layer onto a substrate and heated they fuse into a continuous layer at temperatures as much as 250, 500, 750 or even 1000.degree. K below their bulk melting point. This allows continuous semiconductor films in the 0.25 to 25 nm thickness range to be formed with minimal thermal exposure.

  12. Semiconductor nanorod liquid crystals

    SciTech Connect

    Li, Liang-shi; Walda, Joost; Manna, Liberato; Alivisatos, A. Paul

    2002-01-28

    Rodlike molecules form liquid crystalline phases with orientational order and positional disorder. The great majority of materials in which liquid crystalline phases have been observed are comprised of organic molecules or polymers, even though there has been continuing and growing interest in inorganic liquid crystals. Recent advances in the control of the sizes and shapes of inorganic nanocrystals allow for the formation of a broad class of new inorganic liquid crystals. Here we show the formation of liquid crystalline phases of CdSe semiconductor nanorods. These new liquid crystalline phases may have great importance for both application and fundamental study.

  13. Semiconductor structure

    NASA Technical Reports Server (NTRS)

    Hovel, Harold J. (Inventor); Woodall, Jerry M. (Inventor)

    1979-01-01

    A technique for fabricating a semiconductor heterostructure by growth of a ternary semiconductor on a binary semiconductor substrate from a melt of the ternary semiconductor containing less than saturation of at least one common ingredient of both the binary and ternary semiconductors wherein in a single temperature step the binary semiconductor substrate is etched, a p-n junction with specific device characteristics is produced in the binary semiconductor substrate by diffusion of a dopant from the melt and a region of the ternary semiconductor of precise conductivity type and thickness is grown by virtue of a change in the melt characteristics when the etched binary semiconductor enters the melt.

  14. Chelating ligands for nanocrystals' surface functionalization.

    PubMed

    Querner, Claudia; Reiss, Peter; Bleuse, Joël; Pron, Adam

    2004-09-22

    A new family of ligands for the surface functionalization of CdSe nanocrystals is proposed, namely alkyl or aryl derivatives of carbodithioic acids (R-C(S)SH). The main advantages of these new ligands are as follows: they nearly quantitatively exchange the initial surface ligands (TOPO) in very mild conditions; they significantly improve the resistance of nanocrystals against photooxidation because of their ability of strong chelate-type binding to metal atoms; their relatively simple preparation via Grignard intermediates facilitates the development of new bifunctional ligands containing, in addition to the anchoring carbodithioate group, a second function, which enables the grafting of molecules or macromolecules of interest on the nanocrystal surface. To give an example of this approach, we report, for the first time, the grafting of an electroactive oligomer from the polyaniline family-aniline tetramer-on CdSe nanocrystals after their functionalization with 4-formyldithiobenzoic acid. The grafting proceeds via a condensation reaction between the aldehyde group of the ligand and the terminal primary amine group of the tetramer. The resulting organic/inorganic hybrid exhibits complete extinction of the fluorescence of its constituents, indicating efficient charge or energy transfer between the organic and the inorganic semiconductors.

  15. Conjugated polymer/nanocrystal nanocomposites for renewable energy applications in photovoltaics and photocatalysis.

    PubMed

    Su, Yu-Wei; Lin, Wei-Hao; Hsu, Yung-Jung; Wei, Kung-Hwa

    2014-11-01

    Conjugated polymer/nanocrystal composites have attracted much attention for use in renewable energy applications because of their versatile and synergistic optical and electronic properties. Upon absorbing photons, charge separation occurs in the nanocrystals, generating electrons and holes for photocurrent flow or reduction/oxidation (redox) reactions under proper conditions. Incorporating these nanocrystals into conjugated polymers can complement the visible light absorption range of the polymers for photovoltaics applications or allow the polymers to sensitize or immobilize the nanocrystals for photocatalysis. Here, the current developments of conjugated polymer/nanocrystal nanocomposites for bulk heterojunction-type photovoltaics incorporating Cd- and Pb-based nanocrystals or quantum dots are reviewed. The effects of manipulating the organic ligands and the concentration of the nanocrystal precursor, critical factors that affect the shape and aggregation of the nanocrystals, are also discussed. In the conclusion, the mechanisms through which conjugated polymers can sensitize semiconductor nanocrystals (TiO2 , ZnO) to ensure efficient charge separation, as well as how they can support immobilized nanocrystals for use in photocatalysis, are addressed.

  16. Biomineralization: Nanocrystals by design

    NASA Astrophysics Data System (ADS)

    Shang, Li; Nienhaus, Gerd Ulrich

    2015-10-01

    Nanocrystals with precisely defined structures offer promise as components of advanced materials yet they are challenging to create. Now, a nanocrystal made up of seven cadmium and twelve chloride ions has been synthesized via a biotemplating approach that uses a de novo designed protein.

  17. Optical activity of chirally distorted nanocrystals

    NASA Astrophysics Data System (ADS)

    Tepliakov, Nikita V.; Baimuratov, Anvar S.; Baranov, Alexander V.; Fedorov, Anatoly V.; Rukhlenko, Ivan D.

    2016-05-01

    We develop a general theory of optical activity of semiconductor nanocrystals whose chirality is induced by a small perturbation of their otherwise achiral electronic subsystems. The optical activity is described using the quantum-mechanical expressions for the rotatory strengths and dissymmetry factors introduced by Rosenfeld. We show that the rotatory strengths of optically active transitions are decomposed on electric dipole and magnetic dipole contributions, which correspond to the electric dipole and magnetic dipole transitions between the unperturbed quantum states. Remarkably, while the two kinds of rotatory strengths are of the same order of magnitude, the corresponding dissymmetry factors can differ by a factor of 105. By maximizing the dissymmetry of magnetic dipole absorption one can significantly enhance the enantioselectivity in the interaction of semiconductor nanocrystals with circularly polarized light. This feature may advance chiral and analytical methods, which will benefit biophysics, chemistry, and pharmaceutical science. The developed theory is illustrated by an example of intraband transitions inside a semiconductor nanocuboid, whose rotatory strengths and dissymmetry factors are calculated analytically.

  18. The influence of dopant distribution on the optoelectronic properties of tin-doped indium oxide nanocrystals and nanocrystal films

    NASA Astrophysics Data System (ADS)

    Lounis, Sebastien Dahmane

    Colloidally prepared nanocrystals of transparent conducting oxide (TCO) semiconductors have emerged in the past decade as an exciting new class of plasmonic materials. In recent years, there has been tremendous progress in developing synthetic methods for the growth of these nanocrystals, basic characterization of their properties, and their successful integration into optoelectronic and electrochemical devices. However, many fundamental questions remain about the physics of localized surface plasmon resonance (LSPR) in these materials, and how their optoelectronic properties derive from their underlying structural properties. In particular, the influence of the concentration and distribution of dopant ions and compensating defects on the optoelectronic properties of TCO nanocrystals has seen little investigation. Indium tin oxide (ITO) is the most widely studied and commercially deployed TCO. Herein we investigate the role of the distribution of tin dopants on the optoelectronic properties of colloidally prepared ITO nanocrystals. Owing to a high free electron density, ITO nanocrystals display strong LSPR absorption in the near infrared. Depending on the particular organic ligands used, they are soluble in various solvents and can readily be integrated into densely packed nanocrystal films with high conductivities. Using a combination of spectroscopic techniques, modeling and simulation of the optical properties of the nanocrystals using the Drude model, and transport measurements, it is demonstrated herein that the radial distribution of tin dopants has a strong effect on the optoelectronic properties of ITO nanocrystals. ITO nanocrystals were synthesized in both surface-segregated and uniformly distributed dopant profiles. Temperature dependent measurements of optical absorbance were first combined with Drude modeling to extract the internal electrical properties of the ITO nanocrystals, demonstrating that they are well-behaved degenerately doped semiconductors

  19. Prospects of nanoscience with nanocrystals

    SciTech Connect

    Kovalenko, Maksym V.; Manna, Liberato; Cabot, Andreu; Hens, Zeger; Talapin, Dmitri V.; Kagan, Cherie R.; Klimov, Victor I.; Rogach, Andrey L.; Reiss, Peter; Milliron, Delia J.; Guyot-Sionnnest, Philippe; Konstantatos, Gerasimos; Parak, Wolfgang J.; Hyeon, Taeghwan; Korgel, Brian A.; Murray, Christopher B.; Heiss, Wolfgang

    2015-01-22

    Colloidal nanocrystals (NCs, i.e., crystalline nanoparticles) have become an important class of materials with great potential for applications ranging from medicine to electronic and optoelectronic devices. Today's strong research focus on NCs has been prompted by the tremendous progress in their synthesis. Impressively narrow size distributions of just a few percent, rational shape-engineering, compositional modulation, electronic doping, and tailored surface chemistries are now feasible for a broad range of inorganic compounds. Furthermore, the performance of inorganic NC-based photovoltaic and lightemitting devices has become competitive to other state-of-the-art materials. Semiconductor NCs hold unique promise for near- and mid-infrared technologies, where very few semiconductor materials are available. On a purely fundamental side, new insights into NC growth, chemical transformations, and self-organization can be gained from rapidly progressing in situ characterization and direct imaging techniques. New phenomena are constantly being discovered in the photophysics of NCs and in the electronic properties of NC solids. In our Nano Focus, we review the state of the art in research on colloidal NCs focusing on the most recent works published in the last 2 years.

  20. Prospects of nanoscience with nanocrystals

    DOE PAGESBeta

    Kovalenko, Maksym V.; Manna, Liberato; Cabot, Andreu; Hens, Zeger; Talapin, Dmitri V.; Kagan, Cherie R.; Klimov, Victor I.; Rogach, Andrey L.; Reiss, Peter; Milliron, Delia J.; et al

    2015-01-22

    Colloidal nanocrystals (NCs, i.e., crystalline nanoparticles) have become an important class of materials with great potential for applications ranging from medicine to electronic and optoelectronic devices. Today's strong research focus on NCs has been prompted by the tremendous progress in their synthesis. Impressively narrow size distributions of just a few percent, rational shape-engineering, compositional modulation, electronic doping, and tailored surface chemistries are now feasible for a broad range of inorganic compounds. Furthermore, the performance of inorganic NC-based photovoltaic and lightemitting devices has become competitive to other state-of-the-art materials. Semiconductor NCs hold unique promise for near- and mid-infrared technologies, where verymore » few semiconductor materials are available. On a purely fundamental side, new insights into NC growth, chemical transformations, and self-organization can be gained from rapidly progressing in situ characterization and direct imaging techniques. New phenomena are constantly being discovered in the photophysics of NCs and in the electronic properties of NC solids. In our Nano Focus, we review the state of the art in research on colloidal NCs focusing on the most recent works published in the last 2 years.« less

  1. Frequency upconverted lasing of nanocrystal quantum dots in microbeads

    NASA Astrophysics Data System (ADS)

    Zhang, Chunfeng; Zhang, Fan; Cheng, An; Kimball, Brian; Wang, Andrew Y.; Xu, Jian

    2009-11-01

    Stable, frequency upconverted lasing of semiconductor nanocrystal quantum dots was demonstrated in silica microbeads under two-photon pumping conditions. Upon infrared excitation, the stimulated emission of the nanocrystal-doped microbeads exhibits sharp peaks at λ ˜610 nm with narrow line widths of ≤1 nm. The lasing action has been attributed to the biexciton gain coupled to the whispering gallery modes in spherical cavities, as confirmed by time-resolved photoluminescence spectra. The lasing lifetime characterized in term of pulse numbers (˜106 pulses) was two orders of magnitude longer than that of the dye salt-based two-photon lasers.

  2. Passivation effects in B doped self-assembled Si nanocrystals

    SciTech Connect

    Puthen Veettil, B. Wu, Lingfeng; Jia, Xuguang; Lin, Ziyun; Zhang, Tian; Yang, Terry; Johnson, Craig; Conibeer, Gavin; Perez-Würfl, Ivan; McCamey, Dane

    2014-12-01

    Doping of semiconductor nanocrystals has enabled their widespread technological application in optoelectronics and micro/nano-electronics. In this work, boron-doped self-assembled silicon nanocrystal samples have been grown and characterised using Electron Spin Resonance and photoluminescence spectroscopy. The passivation effects of boron on the interface dangling bonds have been investigated. Addition of boron dopants is found to compensate the active dangling bonds at the interface, and this is confirmed by an increase in photoluminescence intensity. Further addition of dopants is found to reduce the photoluminescence intensity by decreasing the minority carrier lifetime as a result of the increased number of non-radiative processes.

  3. Recent Progress in Photocatalysis Mediated by Colloidal II-VI Nanocrystals

    PubMed Central

    Wilker, Molly B; Schnitzenbaumer, Kyle J; Dukovic, Gordana

    2012-01-01

    The use of photoexcited electrons and holes in semiconductor nanocrystals as reduction and oxidation reagents is an intriguing way of harvesting photon energy to drive chemical reactions. This review focuses on recent research efforts to understand and control the photocatalytic processes mediated by colloidal II-VI nanocrystalline materials, such as cadmium and zinc chalcogenides. First, we highlight how nanocrystal properties govern the rates and efficiencies of charge-transfer processes relevant to photocatalysis. We then describe the use of nanocrystal catalyst heterostructures for fuel-forming reactions, most commonly H2 generation. Finally, we review the use of nanocrystal photocatalysis as a synthetic tool for metal–semiconductor nano-heterostructures. PMID:24115781

  4. On Ultrasmall Nanocrystals

    PubMed Central

    McBride, James R.; Dukes, Albert D.; Schreuder, Michael A.; Rosenthal, Sandra J.

    2010-01-01

    Ultrasmall nanocrystals are a growing sub-class of traditional nanocrystals that exhibit new properties at diameters typically below 2 nm. In this review, we define what constitutes an ultrasmall nanoparticle while distinguishing between ultrasmall and magic-size nanoparticles. After a brief overview of ultrasmall nanoparticles, including ultrasmall gold clusters, our recent work is presented covering the optical properties, structure, and application of ultrasmall CdSe nanocrystals. This unique material has potential application in solid state lighting due to its balanced white emission. This section is followed by a discussion on the blurring boundary between what can be considered a nanoparticle and a molecule. PMID:21132106

  5. Pyramidal and Chiral Groupings of Gold Nanocrystals Assembled Using DNA Scaffolds

    SciTech Connect

    Mastroianni, Alexander; Claridge, Shelley; Alivisatos, A. Paul

    2009-03-30

    Nanostructures constructed from metal and semiconductor nanocrystals conjugated to, and organized by DNA are an emerging class of material with collective optical properties. We created discrete pyramids of DNA with gold nanocrystals at the tips. By taking small angle X-ray scattering (SAXS) measurments from solutions of these pyramids we confirmed that this pyramidal geometry creates structures which are more rigid in solution than linear DNA. We then took advantage of the tetrahedral symmetry to demonstrate construction of chiral nanostructures.

  6. Red spectral shift and enhanced quantum efficiency in phonon-free photoluminescence from silicon nanocrystals.

    PubMed

    de Boer, W D A M; Timmerman, D; Dohnalová, K; Yassievich, I N; Zhang, H; Buma, W J; Gregorkiewicz, T

    2010-12-01

    Crystalline silicon is the most important semiconductor material in the electronics industry. However, silicon has poor optical properties because of its indirect bandgap, which prevents the efficient emission and absorption of light. The energy structure of silicon can be manipulated through quantum confinement effects, and the excitonic emission from silicon nanocrystals increases in intensity and shifts to shorter wavelengths (a blueshift) as the size of the nanocrystals is reduced. Here we report experimental evidence for a short-lived visible band in the photoluminescence spectrum of silicon nanocrystals that increases in intensity and shifts to longer wavelengths (a redshift) with smaller nanocrystal sizes. This higher intensity indicates an increased quantum efficiency, which for 2.5-nm-diameter nanocrystals is enhanced by three orders of magnitude compared to bulk silicon. We assign this band to the radiative recombination of non-equilibrium electron-hole pairs in a process that does not involve phonons.

  7. Solution based synthesis of simple fcc Si nano-crystals under ambient conditions.

    PubMed

    Balcı, Mustafa H; Sæterli, Ragnhild; Maria, Jerome; Lindgren, Mikael; Holmestad, Randi; Grande, Tor; Einarsrud, Mari-Ann

    2013-02-28

    We demonstrate for the first time that simple face-centered cubic (fcc) silicon nano-crystals can be produced by a solution based bottom-up synthesis route under ambient conditions. Simple fcc Si nano-crystals (2-7 nm) were prepared at room temperature by using sodium cyclopentadienide as a reducing agent for silicon tetrachloride. Photoluminescence emission at 550 nm was observed for the fcc silicon nano-crystals upon excitation at 340 nm, indicating that fcc Si nano-crystals were exhibiting direct bandgap like semiconductor properties with very fast radiative recombination rates. The new synthesis route makes possible the production and study of simple fcc polymorphs of Si nano-crystals with an easy alteration of surface termination groups.

  8. Formation of Si nanocrystals utilizing a Au nanoscale island etching mask

    SciTech Connect

    Kang, Y.M.; Lee, S.J.; Kim, D.Y. . E-mail: dykim@dongguk.edu; Kim, T.W.; Woo, Y.-D.; Wang, K.L.

    2005-01-04

    Si nanocrystals were formed by using a Au nanoscale island etching mask. A high-resolution transmission electron microscopy image showed that the Si nanocrystals were created on a SiO{sub x} layer, and the luminescence peak related to Si nanocrystals was observed in the cathodoluminescence spectrum. Capacitance-voltage measurements demonstrate a metal-insulator-semiconductor behavior with a flatband voltage shift for the Al/SiO{sub 2}/nanocrystalline Si/SiO{sub 2}/p-Si structures, indicative of the existence of the Si nanocrystals embedded into the SiO{sub x} layer. These results indicate that Si nanocrystals embedded into the SiO{sub x} layer can be formed by using a Au island etching mask.

  9. Hypervalent surface interactions for colloidal stability and doping of silicon nanocrystals

    PubMed Central

    Wheeler, Lance M.; Neale, Nathan R.; Chen, Ting; Kortshagen, Uwe R.

    2013-01-01

    Colloidal semiconductor nanocrystals have attracted attention for cost-effective, solution-based deposition of quantum-confined thin films for optoelectronics. However, two significant challenges must be addressed before practical nanocrystal-based devices can be realized. The first is coping with the ligands that terminate the nanocrystal surfaces. Though ligands provide the colloidal stability needed to cast thin films from solution, these ligands dramatically hinder charge carrier transport in the resulting film. Second, after a conductive film is achieved, doping has proven difficult for further control of the optoelectronic properties of the film. Here we report the ability to confront both of these challenges by exploiting the ability of silicon to engage in hypervalent interactions with hard donor molecules. For the first time, we demonstrate the significant potential of applying the interaction to the nanocrystal surface. In this study, hypervalent interactions are shown to provide colloidal stability as well as doping of silicon nanocrystals. PMID:23893292

  10. Nanocrystal dispersed amorphous alloys

    NASA Technical Reports Server (NTRS)

    Perepezko, John H. (Inventor); Allen, Donald R. (Inventor); Foley, James C. (Inventor)

    2001-01-01

    Compositions and methods for obtaining nanocrystal dispersed amorphous alloys are described. A composition includes an amorphous matrix forming element (e.g., Al or Fe); at least one transition metal element; and at least one crystallizing agent that is insoluble in the resulting amorphous matrix. During devitrification, the crystallizing agent causes the formation of a high density nanocrystal dispersion. The compositions and methods provide advantages in that materials with superior properties are provided.

  11. Nanocrystal-Powered Nanomotor

    SciTech Connect

    Regan, B.C.; Aloni, S.; Jensen, K.; Ritchie, R.O.; Zettl, A.

    2005-07-05

    We have constructed and operated a nanoscale linear motorpowered by a single metal nanocrystal ram sandwiched between mechanicallever arms. Low-level electrical voltages applied to the carbon nanotubelever arms cause the nanocrystal to grow or shrink in a controlledmanner. The length of the ram is adjustable from 0 to more than 150 nm,with extension speeds exceeding 1900 nm/s. The thermodynamic principlesgoverning motor operation resemble those driving frost heave, a naturalsolid-state linear motor.

  12. 2009 Clusters, Nanocrystals & Nanostructures GRC

    SciTech Connect

    Lai-Sheng Wang

    2009-07-19

    For over thirty years, this Gordon Conference has been the premiere meeting for the field of cluster science, which studies the phenomena that arise when matter becomes small. During its history, participants have witnessed the discovery and development of many novel materials, including C60, carbon nanotubes, semiconductor and metal nanocrystals, and nanowires. In addition to addressing fundamental scientific questions related to these materials, the meeting has always included a discussion of their potential applications. Consequently, this conference has played a critical role in the birth and growth of nanoscience and engineering. The goal of the 2009 Gordon Conference is to continue the forward-looking tradition of this meeting and discuss the most recent advances in the field of clusters, nanocrystals, and nanostructures. As in past meetings, this will include new topics that broaden the field. In particular, a special emphasis will be placed on nanomaterials related to the efficient use, generation, or conversion of energy. For example, we anticipate presentations related to batteries, catalysts, photovoltaics, and thermoelectrics. In addition, we expect to address the controversy surrounding carrier multiplication with a session in which recent results addressing this phenomenon will be discussed and debated. The atmosphere of the conference, which emphasizes the presentation of unpublished results and lengthy discussion periods, ensures that attendees will enjoy a valuable and stimulating experience. Because only a limited number of participants are allowed to attend this conference, and oversubscription is anticipated, we encourage all interested researchers from academia, industry, and government institutions to apply as early as possible. An invitation is not required. We also encourage all attendees to submit their latest results for presentation at the poster sessions. We anticipate that several posters will be selected for 'hot topic' oral

  13. Defect Chemistry and Plasmon Physics of Colloidal Metal Oxide Nanocrystals

    SciTech Connect

    Lounis, SD; Runnerstrorm, EL; Llordes, A; Milliron, DJ

    2014-05-01

    Plasmonic nanocrystals of highly doped metal oxides have seen rapid development in the past decade and represent a class of materials with unique optoelectronic properties. In this Perspective, we discuss doping mechanisms in metal oxides and the accompanying physics of free carrier scattering, both of which have implications in determining the properties of localized surface plasmon resonances (LSPRs) in these nanocrystals. The balance between activation and compensation of dopants limits the free carrier concentration of the most common metal oxides, placing a ceiling on the LSPR frequency. Furthermore, because of ionized impurity scattering of the oscillating plasma by dopant ions, scattering must be treated in a fundamentally different way in semiconductor metal oxide materials when compared with conventional metals. Though these effects are well-understood in bulk metal oxides, further study is needed to understand their manifestation in nanocrystals and corresponding impact on plasmonic properties, and to develop materials that surpass current limitations in free carrier concentration.

  14. Photocatalytic Applications of Colloidal Heterostructured Nanocrystals: What's Next?

    PubMed

    Razgoniaeva, Natalia; Moroz, Pavel; Lambright, Scott; Zamkov, Mikhail

    2015-11-01

    Recent progress in the colloidal synthesis of inorganic nanocrystals has led to the realization of complex, multidomain nanoparticle morphologies that give rise to advanced optoelectronic properties. Such nanocomposites are particularly appealing for photocatalytic applications where tunable absorption, extensive charge separation, and large surface-to-volume ratios are important. To date, heterostructured nanocrystals featuring a metal catalyst and a semiconductor "chromophore" component have shown compelling efficiencies in photoreduction reactions, including sacrificial hydrogen production. Time-resolved optical studies have attributed their success to a near-complete separation of photoinduced charges across dissimilar nanoparticle domains. The spectroscopy approach has also identified the key performance-limiting factors of nanocrystal catalysts that arise from inefficient extraction of photoinduced charges to catalytic sites. Along these lines, the main scope of present-day efforts targets the improvement of interstitial charge transfer pathways across the chromophore-catalyst assembly through the design of high-quality stoichiometric interfaces.

  15. A quantitative model for charge carrier transport, trapping and recombination in nanocrystal-based solar cells

    PubMed Central

    Bozyigit, Deniz; Lin, Weyde M. M.; Yazdani, Nuri; Yarema, Olesya; Wood, Vanessa

    2015-01-01

    Improving devices incorporating solution-processed nanocrystal-based semiconductors requires a better understanding of charge transport in these complex, inorganic–organic materials. Here we perform a systematic study on PbS nanocrystal-based diodes using temperature-dependent current–voltage characterization and thermal admittance spectroscopy to develop a model for charge transport that is applicable to different nanocrystal-solids and device architectures. Our analysis confirms that charge transport occurs in states that derive from the quantum-confined electronic levels of the individual nanocrystals and is governed by diffusion-controlled trap-assisted recombination. The current is limited not by the Schottky effect, but by Fermi-level pinning because of trap states that is independent of the electrode–nanocrystal interface. Our model successfully explains the non-trivial trends in charge transport as a function of nanocrystal size and the origins of the trade-offs facing the optimization of nanocrystal-based solar cells. We use the insights from our charge transport model to formulate design guidelines for engineering higher-performance nanocrystal-based devices. PMID:25625647

  16. A quantitative model for charge carrier transport, trapping and recombination in nanocrystal-based solar cells

    NASA Astrophysics Data System (ADS)

    Bozyigit, Deniz; Lin, Weyde M. M.; Yazdani, Nuri; Yarema, Olesya; Wood, Vanessa

    2015-01-01

    Improving devices incorporating solution-processed nanocrystal-based semiconductors requires a better understanding of charge transport in these complex, inorganic-organic materials. Here we perform a systematic study on PbS nanocrystal-based diodes using temperature-dependent current-voltage characterization and thermal admittance spectroscopy to develop a model for charge transport that is applicable to different nanocrystal-solids and device architectures. Our analysis confirms that charge transport occurs in states that derive from the quantum-confined electronic levels of the individual nanocrystals and is governed by diffusion-controlled trap-assisted recombination. The current is limited not by the Schottky effect, but by Fermi-level pinning because of trap states that is independent of the electrode-nanocrystal interface. Our model successfully explains the non-trivial trends in charge transport as a function of nanocrystal size and the origins of the trade-offs facing the optimization of nanocrystal-based solar cells. We use the insights from our charge transport model to formulate design guidelines for engineering higher-performance nanocrystal-based devices.

  17. A Chemical Approach to 3-D Lithographic Patterning of Si and GeNanocrystals

    SciTech Connect

    Sharp, I.D.; Xu, Q.; Yi, D.O.; Liao, C.Y.; Ager III, J.W.; Beeman, J.W.; Yu, K.M.; Robinson, J.T.; Dubon, O.D.; Chrzan, D.C.; Haller, E.E.

    2005-12-12

    Ion implantation into silica followed by thermal annealingis an established growth method for Si and Ge nanocrystals. Wedemonstrate that growth of Group IV semiconductor nanocrystals can besuppressed by co-implantation of oxygen prior to annealing. For Sinanocrystals, at low Si/O dose ratios, oxygen co-implantation leads to areduction of the average nanocrystal size and a blue-shift of thephotoluminescence emission energy. For both Si and Ge nanocrystals, atlarger Si/O or Ge/O dose ratios, the implanted specie is oxidized andnanocrystals do not form. This chemical deactivation was utilized toachieve patterned growth of Si and Ge nanocrystals. Si was implanted intoa thin SiO2 film on a Si substrate followed by oxygen implantationthrough an electron beam lithographically defined stencil mask. Thermalannealing of the co-implanted structure yields two-dimensionallypatterned growth of Si nanocrystals under the masked regions. We applieda previously developed process to obtain exposed nanocrystals byselective HF etching of the silica matrix to these patterned structures.Atomic force microscopy (AFM) of etched structures revealed that exposednanocrystals are not laterally displaced from their original positionsduring the etching process. Therefore, this process provides a means ofachieving patterned structures of exposed nanocrystals. The possibilitiesfor scaling this chemical-based lithography process to smaller featuresand for extending it to 3-D patterning is discussed.

  18. Nanocrystal Solar Cells

    SciTech Connect

    Gur, Ilan

    2006-01-01

    This dissertation presents the results of a research agenda aimed at improving integration and stability in nanocrystal-based solar cells through advances in active materials and device architectures. The introduction of 3-dimensional nanocrystals illustrates the potential for improving transport and percolation in hybrid solar cells and enables novel fabrication methods for optimizing integration in these systems. Fabricating cells by sequential deposition allows for solution-based assembly of hybrid composites with controlled and well-characterized dispersion and electrode contact. Hyperbranched nanocrystals emerge as a nearly ideal building block for hybrid cells, allowing the controlled morphologies targeted by templated approaches to be achieved in an easily fabricated solution-cast device. In addition to offering practical benefits to device processing, these approaches offer fundamental insight into the operation of hybrid solar cells, shedding light on key phenomena such as the roles of electrode-contact and percolation behavior in these cells. Finally, all-inorganic nanocrystal solar cells are presented as a wholly new cell concept, illustrating that donor-acceptor charge transfer and directed carrier diffusion can be utilized in a system with no organic components, and that nanocrystals may act as building blocks for efficient, stable, and low-cost thin-film solar cells.

  19. A Silicon Nanocrystal Schottky Junction Solar Cell produced from Colloidal Silicon Nanocrystals.

    PubMed

    Liu, Chin-Yi; Kortshagen, Uwe R

    2010-05-20

    Solution-processed semiconductors are seen as a promising route to reducing the cost of the photovoltaic device manufacture. We are reporting a single-layer Schottky photovoltaic device that was fabricated by spin-coating intrinsic silicon nanocrystals (Si NCs) from colloidal suspension. The thin-film formation process was based on Si NCs without any ligand attachment, exchange, or removal reactions. The Schottky junction device showed a photovoltaic response with a power conversion efficiency of 0.02%, a fill factor of 0.26, short circuit-current density of 0.148 mA/cm2, and open-circuit voltage of 0.51 V.

  20. Femtosecond chirp-free studies of energy relaxation in semiconductor quantum dots: Search for a phonon bottleneck

    SciTech Connect

    Klimov, V.; McBranch, D.

    1997-08-01

    Contrary to the predictions of phonon bottleneck theories, we observe very fast subpicosecond energy relaxation in strongly confined semiconductor nanocrystals with electron level spacing as large as 20 LO phonon energies.

  1. Designer Nanocrystal Materials for Photovoltaics

    NASA Astrophysics Data System (ADS)

    Kagan, Cherie

    Advances in synthetic methods allow a wide range of semiconductor nanocrystals (NCs) to be tailored in size and shape and to be used as building blocks in the design of NC solids. However, the long, insulating ligands commonly employed in the synthesis of colloidal NCs inhibit strong interparticle coupling and charge transport once NCs are assembled into the solids state as NC arrays. We will describe the range of short, compact ligand chemistries we employ to exchange the long, insulating ligands used in synthesis and to increase interparticle coupling. These ligand exchange processes can have a dramatic influence on NC surface chemistry as well as NC organization in the solids, showing examples of short-range order. Synergistically, we use 1) thermal evaporation and diffusion and 2) wet-chemical methods to introduce extrinsic impurities and non-stoichiometry to passivate surface traps and dope NC solids. NC coupling and doping provide control over the density of states and the carrier type, concentration, mobility, and lifetime, which we characterize by a range of electronic and spectroscopic techniques. We will describe the importance of engineering device interfaces to design NC materials for solar photovoltaics.

  2. Synthesis of nanocrystals and nanocrystal self-assembly

    NASA Astrophysics Data System (ADS)

    Chen, Zhuoying

    nanocrystals is presented. Different surfactants of amines, carboxylic acids, and alcohols were used to study the effect of size and morphological control over the nanocrystals. Techniques including X-ray diffraction, transmission electron microscopy, selected area electron diffraction, and high-resolution electron microscopy are used to examine crystallinity and morphology. Chapter 3. By investigating the self-assembly of cadmium selenide-gold (CdSe-Au) nanoparticle mixtures by transmission electron microscopy after solvent evaporation, the effect of solvents in the formation process of CdSe-Au binary nanoparticle superlattices (BNSLs) was studied. 1-dodecanethiol was found to be critical in generating conditions necessary for superlattice formation, prior to the other factors that likely determine structure, highlighting the dual role of this organic polar molecule as both ligand and high boiling point/crystallization solvent. The influence of thiol was investigated under various concentrations (and also compared with other less polar solvents) in order to determine optimized conditions for self-assembly, for which relatively large (> 1 mum2) areas of superlattices could be routinely formed. Depending on appropriate selection of the radius ratio, AuCu or CaCu 5 binary superlattices of CdSe-Au nanoparticles were generated. Chapter 4. The preparation of binary nanoparticle superlattices obtained by self-assembly of two different semiconductor quantum dots is presented. Such a system is a means to include two discretized, quantum-confined, and complimentary semiconductor units in close proximity, which might exhibit interesting charge transport properties for applications such as solar cells. From a range of possible structures predicted, we observe an exclusive preference for the formation of Cuboctahedral AB13 (Cuboctahedral modification of NaZn13) and AB5 (isostructural with CaCu5) structures in the system of 8.1 nm CdTe and 4.4 nm CdSe nanoparticles. To understand further

  3. Polytypic Nanocrystals of Cu-Based Ternary Chalcogenides: Colloidal Synthesis and Photoelectrochemical Properties.

    PubMed

    Wu, Liang; Chen, Shi-You; Fan, Feng-Jia; Zhuang, Tao-Tao; Dai, Chen-Min; Yu, Shu-Hong

    2016-05-01

    Heterocrystalline polytype nanostructured semiconductors have been attracting more and more attention in recent years due to their novel structures and special interfaces. Up to now, controlled polytypic nanostructures are mostly realized in II-VI and III-V semiconductors. Herein, we report the synthesis and photoelectrochemical properties of Cu-based ternary I-III-VI2 chalcogenide polytypic nanocrystals, with a focus on polytypic CuInS2 (CIS), CuInSe2 (CISe), and CuIn(S0.5Se0.5)2 alloy nanocrystals. Each obtained polytypic nanocrystal is constructed with a wurtzite hexagonal column and a zinc blende/chalcopyrite cusp, regardless of the S/Se ratio. The growth mechanisms of polytypic CIS and CISe nanocrystals have been studied by time-dependent experiments. The polytypic nanocrystals are solution-deposited on indium-tin oxide glass substrate and used as a photoelectrode, thus showing stable photoelectrochemical activity in aqueous solution. Density functional theory calculation was used to study the electronic structure and the band gap alignment. This versatile synthetic method provides a new route for synthesis of novel polytypic nanostructured semiconductors with unique properties. PMID:27063512

  4. Oxide Nanocrystal Model Catalysts.

    PubMed

    Huang, Weixin

    2016-03-15

    Model catalysts with uniform and well-defined surface structures have been extensively employed to explore structure-property relationships of powder catalysts. Traditional oxide model catalysts are based on oxide single crystals and single crystal thin films, and the surface chemistry and catalysis are studied under ultrahigh-vacuum conditions. However, the acquired fundamental understandings often suffer from the "materials gap" and "pressure gap" when they are extended to the real world of powder catalysts working at atmospheric or higher pressures. Recent advances in colloidal synthesis have realized controlled synthesis of catalytic oxide nanocrystals with uniform and well-defined morphologies. These oxide nanocrystals consist of a novel type of oxide model catalyst whose surface chemistry and catalysis can be studied under the same conditions as working oxide catalysts. In this Account, the emerging concept of oxide nanocrystal model catalysts is demonstrated using our investigations of surface chemistry and catalysis of uniform and well-defined cuprous oxide nanocrystals and ceria nanocrystals. Cu2O cubes enclosed with the {100} crystal planes, Cu2O octahedra enclosed with the {111} crystal planes, and Cu2O rhombic dodecahedra enclosed with the {110} crystal planes exhibit distinct morphology-dependent surface reactivities and catalytic properties that can be well correlated with the surface compositions and structures of exposed crystal planes. Among these types of Cu2O nanocrystals, the octahedra are most reactive and catalytically active due to the presence of coordination-unsaturated (1-fold-coordinated) Cu on the exposed {111} crystal planes. The crystal-plane-controlled surface restructuring and catalytic activity of Cu2O nanocrystals were observed in CO oxidation with excess oxygen. In the propylene oxidation reaction with O2, 1-fold-coordinated Cu on Cu2O(111), 3-fold-coordinated O on Cu2O(110), and 2-fold-coordinated O on Cu2O(100) were identified

  5. Germanium and Silicon Nanocrystal Thin-Film Field-Effect Transistors from Solution

    SciTech Connect

    Holman, Zachary C.; Liu, Chin-Yi; Kortshagen, Uwe R.

    2010-07-09

    Germanium and silicon have lagged behind more popular II-VI and IV-VI semiconductor materials in the emerging field of semiconductor nanocrystal thin film devices. We report germanium and silicon nanocrystal field-effect transistors fabricated by synthesizing nanocrystals in a plasma, transferring them into solution, and casting thin films. Germanium devices show n-type, ambipolar, or p-type behavior depending on annealing temperature with electron and hole mobilities as large as 0.02 and 0.006 cm2 V-1 s-1, respectively. Silicon devices exhibit n-type behavior without any postdeposition treatment, but are plagued by poor film morphology.

  6. Nickel and nickel oxide nanocrystals selectively grafting on multiwalled carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Prabhu, Yendrapati Taraka; Rao, Kalagadda Venkateswara; Kumari, Bandla Siva; Sai, Vemula Sesha; Pavani, Tambur

    2015-01-01

    Nickel and nickel oxide nanocrystals in their pure phase are carefully embellished by a facial method on oxygen-functionalized multi-walled carbon nanotubes (O-MWCNTs) using nickel nitrate (NN) was effectively accomplished for the first time by calcining them in hydrogen, nitrogen and air, respectively, at suitable temperatures. Nickel and nickel oxide nanocrystals impregnated O-MWCNTs were examined for its structure and morphology by various techniques, such as powder X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy and field emission scanning electron microscopy. The nanocrystals on the O-MWCNTs were determined of 15-20 nm size. Decorated nanocrystals on CNT's have potential applications in semiconductor industries.

  7. Atomistic understanding of cation exchange in PbS nanocrystals using simulations with pseudoligands

    NASA Astrophysics Data System (ADS)

    Fan, Zhaochuan; Lin, Li-Chiang; Buijs, Wim; Vlugt, Thijs J. H.; van Huis, Marijn A.

    2016-05-01

    Cation exchange is a powerful tool for the synthesis of nanostructures such as core-shell nanocrystals, however, the underlying mechanism is poorly understood. Interactions of cations with ligands and solvent molecules are systematically ignored in simulations. Here, we introduce the concept of pseudoligands to incorporate cation-ligand-solvent interactions in molecular dynamics. This leads to excellent agreement with experimental data on cation exchange of PbS nanocrystals, whereby Pb ions are partially replaced by Cd ions from solution. The temperature and the ligand-type control the exchange rate and equilibrium composition of cations in the nanocrystal. Our simulations reveal that Pb ions are kicked out by exchanged Cd interstitials and migrate through interstitial sites, aided by local relaxations at core-shell interfaces and point defects. We also predict that high-pressure conditions facilitate strongly enhanced cation exchange reactions at elevated temperatures. Our approach is easily extendable to other semiconductor compounds and to other families of nanocrystals.

  8. Real-time magnetic resonance imaging and quantification of lipoprotein metabolism in vivo using nanocrystals

    NASA Astrophysics Data System (ADS)

    Bruns, Oliver T.; Ittrich, Harald; Peldschus, Kersten; Kaul, Michael G.; Tromsdorf, Ulrich I.; Lauterwasser, Joachim; Nikolic, Marija S.; Mollwitz, Birgit; Merkel, Martin; Bigall, Nadja C.; Sapra, Sameer; Reimer, Rudolph; Hohenberg, Heinz; Weller, Horst; Eychmüller, Alexander; Adam, Gerhard; Beisiegel, Ulrike; Heeren, Joerg

    2009-03-01

    Semiconductor quantum dots and superparamagnetic iron oxide nanocrystals have physical properties that are well suited for biomedical imaging. Previously, we have shown that iron oxide nanocrystals embedded within the lipid core of micelles show optimized characteristics for quantitative imaging. Here, we embed quantum dots and superparamagnetic iron oxide nanocrystals in the core of lipoproteins-micelles that transport lipids and other hydrophobic substances in the blood-and show that it is possible to image and quantify the kinetics of lipoprotein metabolism in vivo using fluorescence and dynamic magnetic resonance imaging. The lipoproteins were taken up by liver cells in wild-type mice and displayed defective clearance in knock-out mice lacking a lipoprotein receptor or its ligand, indicating that the nanocrystals did not influence the specificity of the metabolic process. Using this strategy it is possible to study the clearance of lipoproteins in metabolic disorders and to improve the contrast in clinical imaging.

  9. Hybrid Molecule-Nanocrystal Photon Upconversion Across the Visible and Near-Infrared.

    PubMed

    Huang, Zhiyuan; Li, Xin; Mahboub, Melika; Hanson, Kerry M; Nichols, Valerie M; Le, Hoang; Tang, Ming L; Bardeen, Christopher J

    2015-08-12

    The ability to upconvert two low energy photons into one high energy photon has potential applications in solar energy, biological imaging, and data storage. In this Letter, CdSe and PbSe semiconductor nanocrystals are combined with molecular emitters (diphenylanthracene and rubrene) to upconvert photons in both the visible and the near-infrared spectral regions. Absorption of low energy photons by the nanocrystals is followed by energy transfer to the molecular triplet states, which then undergo triplet-triplet annihilation to create high energy singlet states that emit upconverted light. By using conjugated organic ligands on the CdSe nanocrystals to form an energy cascade, the upconversion process could be enhanced by up to 3 orders of magnitude. The use of different combinations of nanocrystals and emitters shows that this platform has great flexibility in the choice of both excitation and emission wavelengths.

  10. Hybrid Molecule-Nanocrystal Photon Upconversion Across the Visible and Near-Infrared.

    PubMed

    Huang, Zhiyuan; Li, Xin; Mahboub, Melika; Hanson, Kerry M; Nichols, Valerie M; Le, Hoang; Tang, Ming L; Bardeen, Christopher J

    2015-08-12

    The ability to upconvert two low energy photons into one high energy photon has potential applications in solar energy, biological imaging, and data storage. In this Letter, CdSe and PbSe semiconductor nanocrystals are combined with molecular emitters (diphenylanthracene and rubrene) to upconvert photons in both the visible and the near-infrared spectral regions. Absorption of low energy photons by the nanocrystals is followed by energy transfer to the molecular triplet states, which then undergo triplet-triplet annihilation to create high energy singlet states that emit upconverted light. By using conjugated organic ligands on the CdSe nanocrystals to form an energy cascade, the upconversion process could be enhanced by up to 3 orders of magnitude. The use of different combinations of nanocrystals and emitters shows that this platform has great flexibility in the choice of both excitation and emission wavelengths. PMID:26161875

  11. Multiple Exciton Generation in Colloidal Silicon Nanocrystals

    SciTech Connect

    Beard, M. C.; Knutsen, K. P.; Yu, P.; Luther, J. M.; Song, Q.; Metzger, W. K.; Ellingson, R. J.; Nozik, A. M.

    2007-01-01

    Multiple exciton generation (MEG) is a process whereby multiple electron-hole pairs, or excitons, are produced upon absorption of a single photon in semiconductor nanocrystals (NCs) and represents a promising route to increased solar conversion efficiencies in single-junction photovoltaic cells. We report for the first time MEG yields in colloidal Si NCs using ultrafast transient absorption spectroscopy. We find the threshold photon energy for MEG in 9.5 nm diameter Si NCs (effective band gap {identical_to} Eg = 1.20 eV) to be 2.4 {+-} 0.1E{sub g} and find an exciton-production quantum yield of 2.6 {+-} 0.2 excitons per absorbed photon at 3.4E{sub g}. While MEG has been previously reported in direct-gap semiconductor NCs of PbSe, PbS, PbTe, CdSe, and InAs, this represents the first report of MEG within indirect-gap semiconductor NCs. Furthermore, MEG is found in relatively large Si NCs (diameter equal to about twice the Bohr radius) such that the confinement energy is not large enough to produce a large blue-shift of the band gap (only 80 meV), but the Coulomb interaction is sufficiently enhanced to produce efficient MEG. Our findings are of particular importance because Si dominates the photovoltaic solar cell industry, presents no problems regarding abundance and accessibility within the Earth's crust, and poses no significant environmental problems regarding toxicity.

  12. Analytical modeling of localized surface plasmon resonance in heterostructure copper sulfide nanocrystals

    SciTech Connect

    Caldwell, Andrew H.; Ha, Don-Hyung; Robinson, Richard D.; Ding, Xiaoyue

    2014-10-28

    Localized surface plasmon resonance (LSPR) in semiconductor nanocrystals is a relatively new field of investigation that promises greater tunability of plasmonic properties compared to metal nanoparticles. A novel process by which the LSPR in semiconductor nanocrystals can be altered is through heterostructure formation arising from solution-based cation exchange. Herein, we describe the development of an analytical model of LSPR in heterostructure copper sulfide-zinc sulfide nanocrystals synthesized via a cation exchange reaction between copper sulfide (Cu{sub 1.81}S) nanocrystals and Zn ions. The cation exchange reaction produces dual-interface, heterostructure nanocrystals in which the geometry of the copper sulfide phase can be tuned from a sphere to a thin disk separating symmetrically-grown sulfide (ZnS) grains. Drude model electronic conduction and Mie-Gans theory are applied to describe how the LSPR wavelength changes during cation exchange, taking into account the morphology evolution and changes to the local permittivity. The results of the modeling indicate that the presence of the ZnS grains has a significant effect on the out-of-plane LSPR mode. By comparing the results of the model to previous studies on solid-solid phase transformations of copper sulfide in these nanocrystals during cation exchange, we show that the carrier concentration is independent of the copper vacancy concentration dictated by its atomic phase. The evolution of the effective carrier concentration calculated from the model suggests that the out-of-plane resonance mode is dominant. The classical model was compared to a simplified quantum mechanical model which suggested that quantum mechanical effects become significant when the characteristic size is less than ∼8 nm. Overall, we find that the analytical models are not accurate for these heterostructured semiconductor nanocrystals, indicating the need for new model development for this emerging field.

  13. Structural, transport and optical properties of (La0.6Pr0.4)0.65Ca0.35MnO3 nanocrystals: a wide band-gap magnetic semiconductor.

    PubMed

    Kumar, Satyam; Dwivedi, G D; Kumar, Shiv; Mathur, R B; Saxena, U; Ghosh, A K; Joshi, Amish G; Yang, H D; Chatterjee, Sandip

    2015-02-21

    (La0.6Pr0.4)0.65Ca0.35MnO3 system has been synthesized via a sol-gel route at different sintering temperatures. Structural, transport and optical measurements have been carried out to investigate (La0.6Pr0.4)0.65Ca0.35MnO3 nanoparticles. Raman spectra show that Jahn-Teller distortion has been decreased due to the presence of Ca and Pr in A-site. Magnetic measurements provide a Curie temperature around 200 K and saturation magnetization (MS) of about 3.43μB/Mn at 5 K. X-ray photoemission spectroscopy study suggests that Mn exists in a dual oxidation state (Mn(3+) and Mn(4+)). Resistivity measurements suggest that charge-ordered states of Mn(3+) and Mn(4+), which might be influenced by the presence of Pr, have enhanced insulating behavior in (La0.6Pr0.4)0.65Ca0.35MnO3. Band gap estimated from UV-Vis spectroscopy measurements comes in the range of wide band gap semiconductors (∼3.5 eV); this makes (La0.6Pr0.4)0.65Ca0.35MnO3 a potential candidate for device application. PMID:25567084

  14. Suppressed carrier scattering in CdS-encapsulated PbS nanocrystal films.

    PubMed

    Moroz, Pavel; Kholmicheva, Natalia; Mellott, Bryan; Liyanage, Geethika; Rijal, Upendra; Bastola, Ebin; Huband, Kyla; Khon, Elena; McBride, Keith; Zamkov, Mikhail

    2013-08-27

    One of the key challenges facing the realization of functional nanocrystal devices concerns the development of techniques for depositing colloidal nanocrystals into electrically coupled nanoparticle solids. This work compares several alternative strategies for the assembly of such films using an all-optical approach to the characterization of electron transport phenomena. By measuring excited carrier lifetimes in either ligand-linked or matrix-encapsulated PbS nanocrystal films containing a tunable fraction of insulating ZnS domains, we uniquely distinguish the dynamics of charge scattering on defects from other processes of exciton dissociation. The measured times are subsequently used to estimate the diffusion length and the carrier mobility for each film type within the hopping transport regime. It is demonstrated that nanocrystal films encapsulated into semiconductor matrices exhibit a lower probability of charge scattering than that of nanocrystal solids cross-linked with either 3-mercaptopropionic acid or 1,2-ethanedithiol molecular linkers. The suppression of carrier scattering in matrix-encapsulated nanocrystal films is attributed to a relatively low density of surface defects at nanocrystal/matrix interfaces.

  15. Semiconductor sensors

    NASA Technical Reports Server (NTRS)

    Gatos, Harry C. (Inventor); Lagowski, Jacek (Inventor)

    1977-01-01

    A semiconductor sensor adapted to detect with a high degree of sensitivity small magnitudes of a mechanical force, presence of traces of a gas or light. The sensor includes a high energy gap (i.e., .about. 1.0 electron volts) semiconductor wafer. Mechanical force is measured by employing a non-centrosymmetric material for the semiconductor. Distortion of the semiconductor by the force creates a contact potential difference (cpd) at the semiconductor surface, and this cpd is determined to give a measure of the force. When such a semiconductor is subjected to illumination with an energy less than the energy gap of the semiconductors, such illumination also creates a cpd at the surface. Detection of this cpd is employed to sense the illumination itself or, in a variation of the system, to detect a gas. When either a gas or light is to be detected and a crystal of a non-centrosymmetric material is employed, the presence of gas or light, in appropriate circumstances, results in a strain within the crystal which distorts the same and the distortion provides a mechanism for qualitative and quantitative evaluation of the gas or the light, as the case may be.

  16. Research Update: Comparison of salt- and molecular-based iodine treatments of PbS nanocrystal solids for solar cells

    SciTech Connect

    Jähnig, Fabian; Bozyigit, Deniz; Yarema, Olesya; Wood, Vanessa

    2015-02-01

    Molecular- and salt-based chemical treatments are believed to passivate electronic trap states in nanocrystal-based semiconductors, which are considered promising for solar cells but suffer from high carrier recombination. Here, we compare the chemical, optical, and electronic properties of PbS nanocrystal-based solids treated with molecular iodine and tetrabutylammonium iodide. Surprisingly, both treatments increase—rather than decrease—the number density of trap states; however, the increase does not directly influence solar cell performance. We explain the origins of the observed impact on solar cell performance and the potential in using different chemical treatments to tune charge carrier dynamics in nanocrystal-solids.

  17. New self-assembled nanocrystal micelles for biolabels and biosensors.

    SciTech Connect

    Tallant, David Robert; Wilson, Michael C. (University of New Mexico, Albuquerque, NM); Leve, Erik W. (University of New Mexico, Albuquerque, NM); Fan, Hongyou; Brinker, C. Jeffrey; Gabaldon, John (University of New Mexico, Albuquerque, NM); Scullin, Chessa (University of New Mexico, Albuquerque, NM)

    2005-12-01

    The ability of semiconductor nanocrystals (NCs) to display multiple (size-specific) colors simultaneously during a single, long term excitation holds great promise for their use in fluorescent bio-imaging. The main challenges of using nanocrystals as biolabels are achieving biocompatibility, low non-specific adsorption, and no aggregation. In addition, functional groups that can be used to further couple and conjugate with biospecies (proteins, DNAs, antibodies, etc.) are required. In this project, we invented a new route to the synthesis of water-soluble and biocompatible NCs. Our approach is to encapsulate as-synthesized, monosized, hydrophobic NCs within the hydrophobic cores of micelles composed of a mixture of surfactants and phospholipids containing head groups functionalized with polyethylene glycol (-PEG), -COOH, and NH{sub 2} groups. PEG provided biocompatibility and the other groups were used for further biofunctionalization. The resulting water-soluble metal and semiconductor NC-micelles preserve the optical properties of the original hydrophobic NCs. Semiconductor NCs emit the same color; they exhibit equal photoluminescence (PL) intensity under long-time laser irradiation (one week) ; and they exhibit the same PL lifetime (30-ns). The results from transmission electron microscopy and confocal fluorescent imaging indicate that water-soluble semiconductor NC-micelles are biocompatible and exhibit no aggregation in cells. We have extended the surfactant/lipid encapsulation techniques to synthesize water-soluble magnetic NC-micelles. Transmission electron microscopy results suggest that water-soluble magnetic NC-micelles exhibit no aggregation. The resulting NC-micelles preserve the magnetic properties of the original hydrophobic magnetic NCs. Viability studies conducted using yeast cells suggest that the magnetic nanocrystal-micelles are biocompatible. We have demonstrated, for the first time, that using external oscillating magnetic fields to manipulate

  18. Size-dependent properties of semiconductor nanostructures

    NASA Astrophysics Data System (ADS)

    Kwak, Hyun Wook

    Doping is crucial to many potential applications of nanometer-sized semiconductors. Since their properties are strongly affected by both doping and quantum size effect, it is important to understand how dopants will influence its media under strong quantum confinement. In this dissertation, we will discuss the role of quantum confinement in the properties of nanometer-sized semiconductors doped with impurities. It is well-known that electronic and optical properties of nanometer-sized semiconductors can vary with size. We present size-dependent properties of lithium doped silicon and zinc oxide nanocrystals as examples. With the help of first-principles methods based on real space approach, we find that not only the size itself but also the chemical nature of the impurity is important to determine the properties of nanometer-sized semiconductors. We will also discuss size-induced magnetism in semiconductor nanostructures doped with non-magnetic impurities. From recent studies, it has been proposed that magnetic semiconductors can be designed by using non-magnetic defects, e.g., through the introduction of an extrinsic impurity atom that does not exhibit magnetism by itself. We examine this idea with silicon and zinc oxide nanostructures doped with impurities. We find that quantum size effect may induce magnetism in doped nanostructures. The evidence of the size-dependent magnetic properties offers a new perspective for the design of semiconductor-based spintronic materials.

  19. Silicon nanocrystal-noble metal hybrid nanoparticles.

    PubMed

    Sugimoto, H; Fujii, M; Imakita, K

    2016-06-01

    We report a novel and facile self-limiting synthesis route of silicon nanocrystal (Si NC)-based colloidally stable semiconductor-metal (gold, silver and platinum) hybrid nanoparticles (NPs). For the formation of hybrid NPs, we employ ligand-free colloidal Si NCs with heavily boron (B) and phosphorus (P) doped shells. By simply mixing B and P codoped colloidal Si NCs with metal salts, hybrid NPs consisting of metal cores and Si NC shells are spontaneously formed. We demonstrate the synthesis of highly uniform and size controllable hybrid NPs. It is shown that codoped Si NCs act as a reducing agent for metal salts and also as a protecting layer to stop metal NP growth. The process is thus self-limiting. The development of a variety of Si NC-based hybrid NPs is a promising first step for the design of biocompatible multifunctional NPs with broad material choices for biosensing, bioimaging and solar energy conversion. PMID:27121127

  20. Suppression of auger recombination in ""giant"" core/shell nanocrystals

    SciTech Connect

    Garcia Santamaria, Florencio; Vela, Javier; Schaller, Richard D; Hollingsworth, Jennifer A; Klimov, Victor I; Chen, Yongfen

    2009-01-01

    Many potential applications of semiconductor nanocrystals are hindered by nonradiative Auger recombination wherein the electron-hole (exciton) recombination energy is transferred to a third charge carrier. This process severely limits the lifetime and bandwidth of optical gain, leads to large nonradiative losses in light emitting diodes and photovoltaic cells, and is believed to be responsible for intermittency ('blinking') of emission from single nanocrystals. The development of nanostructures in which Auger recombination is suppressed has been a longstanding goal in colloidal nanocrystal research. Here, we demonstrate that such suppression is possible using so-called 'giant' nanocrystals that consist of a small CdSe core and a thick CdS shell. These nanostructures exhibit a very long biexciton lifetime ({approx}10 ns) that is likely dominated by radiative decay instead of non-radiative Auger recombination. As a result of suppressed Auger recombination, even high-order multiexcitons exhibit high emission efficiencies, which allows us to demonstrate optical amplification with an extraordinarily large bandwidth (>500 me V) and record low excitation thresholds.

  1. Nanocrystal waveguide (NOW) laser

    DOEpatents

    Simpson, John T.; Simpson, Marcus L.; Withrow, Stephen P.; White, Clark W.; Jaiswal, Supriya L.

    2005-02-08

    A solid state laser includes an optical waveguide and a laser cavity including at least one subwavelength mirror disposed in or on the optical waveguide. A plurality of photoluminescent nanocrystals are disposed in the laser cavity. The reflective subwavelength mirror can be a pair of subwavelength resonant gratings (SWG), a pair of photonic crystal structures (PC), or a distributed feedback structure. In the case of a pair of mirrors, a PC which is substantially transmissive at an operating wavelength of the laser can be disposed in the laser cavity between the subwavelength mirrors to improve the mode structure, coherence and overall efficiency of the laser. A method for forming a solid state laser includes the steps of providing an optical waveguide, creating a laser cavity in the optical waveguide by disposing at least one subwavelength mirror on or in the waveguide, and positioning a plurality of photoluminescent nanocrystals in the laser cavity.

  2. Photodoping of Colloidal Nanocrystals

    NASA Astrophysics Data System (ADS)

    Cohn, Alicia W.

    This dissertation addresses various aspects of photodoping colloidal nanocrystals. Photodoped ZnO nanocrystals were found to be versatile tuneable reducers using both quantum confinement and band-gap engineering with Mg2+ doping to change the conduction band potential. Using photoluminescence of the visible trap and magnetic circular dichroism spectroscopy of Mg2+ and Mn2+ co-doped ZnO, Mg2+ was shown to change the potential of both the conduction and valence band in a ratio of 0.68:0.32. The hole scavenging reaction using ethanol as the hole scavenger was investigated using continuous-wave and time resolved photoluminescence of the visible trap state of ZnO. The reaction was found to occur between the valence band hole and with a rate of > 15 ps-1. Quenching of the ZnO visible trap luminescence upon photodoping was shown to be due to trap/electron Auger process while the concomitant enhancement of the UV band-gap emission was hypothesized to be due to a reduction in non-radiative processes due to extra electrons in the conduction-band. The trap/electron Auger process in ZnO nanocrystals was further characterized by a size-dependence and shown to scale with R2. Another previously unknown Auger size dependence was measured in CdSe/ZnS trions and shown to scale with R4.3.

  3. Electronic transport of N-type semiconductor nanocrystalline solids

    NASA Astrophysics Data System (ADS)

    Yu, Dong

    2005-07-01

    A bottleneck limiting the widespread applications of semiconductor nanocrystalline solids on optoelectronic devices such as photovoltaic cells, light emitting devices and quantum dots lasers is their poor conductivity. In this thesis, we show that the conductivity of thin films of CdSe nanocrystals is increased by many orders of magnitude when n-doped either by potassium or electrochemistry. Around half-filling of the first electronic shell, a peak in the conductivity is observed indicating shell to shell transport. Introducing conjugated ligands between nanocrystals increases the conductivities to ˜10-2 S cm. NaOH treatment of the thin films leads to a large carrier mobility and a semiconductor nanocrystals field effect transistor is produced. The temperature and electrical field dependent conductivity of n-type CdSe nanocrystal thin films is then investigated. The low field conductivity follows exp(-(T*/T)-1/2 ) and high field conductivity follows exp(-(E*/ E)-1/2). The complete behavior is very well described by the variable range hopping theory with a Coulomb gap. Finally, n-type colloidal CdSe nanocrystalline solids show large positive magnetoresistance at low temperatures (0.3K--4K). We attempted to dope Manganese (II) ions in nanocrystals, which might show interesting negative magnetoresistance. However, they still show similar positive magnetoresistance probably due to the difficulty of Mn doping. At ˜0.3K the resistance is increased by ˜150% at 10 Tesla.

  4. Tuning Equilibrium Compositions in Colloidal Cd1-xMnxSe Nanocrystals Using Diffusion Doping and Cation Exchange.

    PubMed

    Barrows, Charles J; Chakraborty, Pradip; Kornowske, Lindsey M; Gamelin, Daniel R

    2016-01-26

    The physical properties of semiconductor nanocrystals can be tuned dramatically via composition control. Here, we report a detailed investigation of the synthesis of high-quality colloidal Cd1-xMnxSe nanocrystals by diffusion doping of preformed CdSe nanocrystals. Until recently, Cd1-xMnxSe nanocrystals proved elusive because of kinetic incompatibilities between Mn(2+) and Cd(2+) chemistries. Diffusion doping allows Cd1-xMnxSe nanocrystals to be prepared under thermodynamic rather than kinetic control, allowing access to broader composition ranges. We now investigate this chemistry as a model system for understanding the characteristics of nanocrystal diffusion doping more deeply. From the present work, a Se(2-)-limited reaction regime is identified, in which Mn(2+) diffusion into CdSe nanocrystals is gated by added Se(2-), and equilibrium compositions are proportional to the amount of added Se(2-). At large added Se(2-) concentrations, a solubility-limited regime is also identified, in which x = xmax = ∼0.31, independent of the amount of added Se(2-). We further demonstrate that Mn(2+) in-diffusion can be reversed by cation exchange with Cd(2+) under exactly the same reaction conditions, purifying Cd1-xMnxSe nanocrystals back to CdSe nanocrystals with fine tunability. These chemistries offer exceptional composition control in Cd1-xMnxSe NCs, providing opportunities for fundamental studies of impurity diffusion in nanocrystals and for development of compositionally tuned nanocrystals with diverse applications ranging from solar energy conversion to spin-based photonics. PMID:26643033

  5. Ultrahigh resolution multicolor colocalization of single fluorescent nanocrystals

    SciTech Connect

    Michalet, X.; Lacoste, T.D.; Pinaud, F.; Chemla, D.S.; Alivisatos, A.P.; Weiss, S.

    2000-12-20

    A new method for in vitro and possibly in vivo ultrahigh-resolution colocalization and distance measurement between biomolecules is described, based on semiconductor nanocrystal probes. This ruler bridges the gap between FRET and far-field (or near-field scanning optical microscope) imaging and has a dynamic range from few nanometers to tens of micrometers. The ruler is based on a stage-scanning confocal microscope that allows the simultaneous excitation and localization of the excitation point-spread-function (PSF) of various colors nanocrystals while maintaining perfect registry between the channels. Fit of the observed diffraction and photophysics-limited images of the PSFs with a two-dimensional Gaussian allows one to determine their position with nanometer accuracy. This new high-resolution tool opens new windows in various molecular, cell biology and biotechnology applications.

  6. Nanocrystal/sol-gel nanocomposites

    DOEpatents

    Petruska, Melissa A.; Klimov, Victor L.

    2012-06-12

    The present invention is directed to solid composites including colloidal nanocrystals within a sol-gel host or matrix and to processes of forming such solid composites. The present invention is further directed to alcohol soluble colloidal nanocrystals useful in formation of sol-gel based solid composites

  7. Nanocrystal/sol-gel nanocomposites

    DOEpatents

    Petruska, Melissa A.; Klimov, Victor L.

    2007-06-05

    The present invention is directed to solid composites including colloidal nanocrystals within a sol-gel host or matrix and to processes of forming such solid composites. The present invention is further directed to alcohol soluble colloidal nanocrystals useful in formation of sol-gel based solid composites.

  8. Method of synthesizing pyrite nanocrystals

    SciTech Connect

    Wadia, Cyrus; Wu, Yue

    2013-04-23

    A method of synthesizing pyrite nanocrystals is disclosed which in one embodiment includes forming a solution of iron (III) diethyl dithiophosphate and tetra-alkyl-ammonium halide in water. The solution is heated under pressure. Pyrite nanocrystal particles are then recovered from the solution.

  9. Surface modification of cellulose nanocrystals

    NASA Astrophysics Data System (ADS)

    Eyley, Samuel; Thielemans, Wim

    2014-06-01

    Chemical modification of cellulose nanocrystals is an increasingly popular topic in the literature. This review analyses the type of cellulose nanocrystal modification reactions that have been published in the literature thus far and looks at the steps that have been taken towards analysing the products of the nanocrystal modifications. The main categories of reactions carried out on cellulose nanocrystals are oxidations, esterifications, amidations, carbamations and etherifications. More recently nucleophilic substitutions have been used to introduce more complex functionality to cellulose nanocrystals. Multi-step modifications are also considered. This review emphasizes quantification of modification at the nanocrystal surface in terms of degree of substitution and the validity of conclusions drawn from different analysis techniques in this area. The mechanisms of the modification reactions are presented and considered with respect to the effect on the outcome of the reactions. While great strides have been made in the quality of analytical data published in the field of cellulose nanocrystal modification, there is still vast scope for improvement, both in data quality and the quality of analysis of data. Given the difficulty of surface analysis, cross-checking of results from different analysis techniques is fundamental for the development of reliable cellulose nanocrystal modification techniques.

  10. Mechanical Properties of Nanocrystal Supercrystals

    SciTech Connect

    Tam, Enrico; Podsiadlo, Paul; Shevchenko, Elena; Ogletree, D. Frank; Delplancke-Ogletree, Marie-Paule; Ashby, Paul D.

    2009-12-30

    Colloidal nanocrystals attract significant interest due to their potential applications in electronic, magnetic, and optical devices. Nanocrystal supercrystals (NCSCs) are particularly appealing for their well ordered structure and homogeneity. The interactions between organic ligands that passivate the inorganic nanocrystal cores critically influence their self-organization into supercrystals, By investigating the mechanical properties of supercrystals, we can directly characterize the particle-particle interactions in a well-defined geometry, and gain insight into both the self-assembly process and the potential applications of nanocrystal supercrystals. Here we report nanoindentation studies of well ordered lead-sulfide (Pbs) nanocrystal supercrystals. Their modulus and hardness were found to be similar to soft polymers at 1.7 GPa and 70 MPa respectively and the fractures toughness was 39 KPa/m1/2, revealing the extremely brittle nature of these materials.

  11. Germanium Nanocrystals Embedded in Sapphire

    SciTech Connect

    Xu, Q.; Sharp, I.D.; Liao, C.Y.; Yi, D.O.; Ager III, J.W.; Beeman, J.W.; Yu, K.M.; Chrzan, D.C.; Haller, E.E.

    2005-04-15

    {sup 74}Ge nanocrystals are formed in a sapphire matrix by ion implantation followed by damage. Embedded nanocrystals experience large compressive stress relative to bulk, as embedded in sapphire melt very close to the bulk melting point (Tm = 936 C) whereas experience considerably lower stresses. Also, in situ TEM reveals that nanocrystals ion-beam-synthesized nanocrystals embedded in silica are observed to be spherical and measured by Raman spectroscopy of the zone center optical phonon. In contrast, reveals that the nanocrystals are faceted and have a bi-modal size distribution. Notably, the matrix remains crystalline despite the large implantation dose and corresponding thermal annealing. Transmission electron microscopy (TEM) of as-grown samples those embedded in silica exhibit a significant melting point hysteresis around T{sub m}.

  12. Nanocrystal/sol-gel nanocomposites

    DOEpatents

    Klimov, Victor L.; Petruska, Melissa A.

    2010-05-25

    The present invention is directed to a process for preparing a solid composite having colloidal nanocrystals dispersed within a sol-gel matrix, the process including admixing colloidal nanocrystals with an amphiphilic polymer including hydrophilic groups selected from the group consisting of --COOH, --OH, --SO.sub.3H, --NH.sub.2, and --PO.sub.3H.sub.2 within a solvent to form an alcohol-soluble colloidal nanocrystal-polymer complex, admixing the alcohol-soluble colloidal nanocrystal-polymer complex and a sol-gel precursor material, and, forming the solid composite from the admixture. The present invention is also directed to the resultant solid composites and to the alcohol-soluble colloidal nanocrystal-polymer complexes.

  13. Structural investigation of CdSSe-nanocrystals synthesized by ion-beam-implantation

    NASA Astrophysics Data System (ADS)

    Huber, P.; Karl, H.; Lindner, J. K. N.; Stritzker, B.

    2006-01-01

    II-VI semiconductor nanoparticle systems can be prepared by keV high-dose ion implantation and subsequent thermal annealing. The ternay Cd-S-Se system offers an additional degree of freedom to adjust materials properties, as Se and S are completely miscible on the Se sublattice. X-ray diffraction analysis indicates, that hexagonal CdSxSe1-x nanocrystals are formed after rapid thermal annealing. Peak positions are evaluated using Vegard's law. Material loss is monitored quantitatively by Rutherford backscattering spectroscopy (RBS). Cross-sectional TEM images are revealing strong influence of the composition on the nanocrystal structural evolution.

  14. Luminescence in quantum-confined cadmium selenide nanocrystals and nanorods in external electric fields

    SciTech Connect

    Gurinovich, L. I. Lutich, A. A.; Stupak, A. P.; Prislopsky, S. Ya.; Rusakov, E. K.; Artemyev, M. V.; Gaponenko, S. V.; Demir, H. V.

    2009-08-15

    It is found that the absorption and luminescence spectra of CdSe nanocrystals and nanorods depend on the external electric field. It is shown that the external electric field quenches the P-polarized photoluminescence of CdSe nanorods to a degree higher than the degree of field-induced quenching of the S-polarized photoluminescence. It is established that the nanocrystals are more sensitive to the external electric field than the nanorods. The effect of the external electric field on the luminescence properties of the semiconductor nanorods is discussed.

  15. Tuning the Magnetic Properties of Metal Oxide Nanocrystal Heterostructures by Cation Exchange

    PubMed Central

    2013-01-01

    For three types of colloidal magnetic nanocrystals, we demonstrate that postsynthetic cation exchange enables tuning of the nanocrystal’s magnetic properties and achieving characteristics not obtainable by conventional synthetic routes. While the cation exchange procedure, performed in solution phase approach, was restricted so far to chalcogenide based semiconductor nanocrystals, here ferrite-based nanocrystals were subjected to a Fe2+ to Co2+ cation exchange procedure. This allows tracing of the compositional modifications by systematic and detailed magnetic characterization. In homogeneous magnetite nanocrystals and in gold/magnetite core shell nanocrystals the cation exchange increases the coercivity field, the remanence magnetization, as well as the superparamagnetic blocking temperature. For core/shell nanoheterostructures a selective doping of either the shell or predominantly of the core with Co2+ is demonstrated. By applying the cation exchange to FeO/CoFe2O4 core/shell nanocrystals the Neél temperature of the core material is increased and exchange-bias effects are enhanced so that vertical shifts of the hysteresis loops are obtained which are superior to those in any other system. PMID:23362940

  16. A general and robust strategy for the synthesis of nearly monodisperse colloidal nanocrystals

    NASA Astrophysics Data System (ADS)

    Pang, Xinchang; Zhao, Lei; Han, Wei; Xin, Xukai; Lin, Zhiqun

    2013-06-01

    Colloidal nanocrystals exhibit a wide range of size- and shape-dependent properties and have found application in myriad fields, incuding optics, electronics, mechanics, drug delivery and catalysis, to name but a few. Synthetic protocols that enable the simple and convenient production of colloidal nanocrystals with controlled size, shape and composition are therefore of key general importance. Current strategies include organic solution-phase synthesis, thermolysis of organometallic precursors, sol-gel processes, hydrothermal reactions and biomimetic and dendrimer templating. Often, however, these procedures require stringent experimental conditions, are difficult to generalize, or necessitate tedious multistep reactions and purification. Recently, linear amphiphilic block co-polymer micelles have been used as templates to synthesize functional nanocrystals, but the thermodynamic instability of these micelles limits the scope of this approach. Here, we report a general strategy for crafting a large variety of functional nanocrystals with precisely controlled dimensions, compositions and architectures by using star-like block co-polymers as nanoreactors. This new class of co-polymers forms unimolecular micelles that are structurally stable, therefore overcoming the intrinsic instability of linear block co-polymer micelles. Our approach enables the facile synthesis of organic solvent- and water-soluble nearly monodisperse nanocrystals with desired composition and architecture, including core-shell and hollow nanostructures. We demonstrate the generality of our approach by describing, as examples, the synthesis of various sizes and architectures of metallic, ferroelectric, magnetic, semiconductor and luminescent colloidal nanocrystals.

  17. Modifying growth of perylene diimide nanocrystals with poly(3-hexyl thiophene) as additives

    NASA Astrophysics Data System (ADS)

    Bu, Laju; Hayward, Ryan

    2014-03-01

    The shape, size, and crystallinity of organic semiconductors play vital roles in their applications in optoelectronics. Various methods to control crystallization of organic semiconductors, including thermal/solvent annealing, addition of poor solvents, and chemical structure modification, have been applied to improve the performance of organic photovoltaics. While soluble additives controlled crystallization are commonly found in biomineralization, pharmaceutics, and food science, they have rarely been applied to organic semiconductors. Here, we show that a p-type polymer, P3HT, serves as a soluble additive in crystallization of a n-type semiconductor, perylene diimide (PDI), by preferentially adsorbing on lateral crystal faces, which reduce lateral growth of PDI crystals relative to longitudinal growth, yielding extended 1-D nanofibers. Upon subsequent crystallization of P3HT, the PDI nanofibers serve as efficient nucleation sties, resulting in shish-kebab like p/n heterostuctures. Using ultrasound to enhance nucleation of PDI crystals, variations in P3HT molecular weight and concentration, and sonication temperature, allow PDI nanocrystal size and uniformity to be tuned. The uniform PDI nanocrystals can act as seeds to crystallize additional PDI to get segmented nanocrystals.

  18. Hybrid bulk heterojunction solar cells based on low band gap polymers and CdSe nanocrystals

    NASA Astrophysics Data System (ADS)

    Dayneko, Sergey; Tameev, Alexey; Tedoradze, Marine; Martynov, Igor; Linkov, Pavel; Samokhvalov, Pavel; Nabiev, Igor; Chistyakov, Alexander

    2014-03-01

    Solar energy converters based on organic semiconductors are inexpensive, can be layered onto flexible surfaces, and show great promise for photovoltaics. In bulk heterojunction polymer solar cells, charges are separated at the interface of two materials, an electron donor and an electron acceptor. Typically, only the donor effectively absorbs light. Therefore, the use of an acceptor with a wide absorption spectrum and high extinction coefficient and charge mobility should increase the efficiency of bulk heterojunction polymer solar cells. Semiconductor nanocrystals (quantum dots and rods) are good candidate acceptors for these solar cells. Recently, most progress in the development of bulk heterojunction polymer solar cells was achieved using PCBM, a traditional fullerene acceptor, and two low band gap polymers, poly[N- 9'-heptadecanyl-2,7-carbazole-alt-5,5-(4',7'-di-2-thienyl-2',1',3'-benzothiadiazole)] (PCDTBT) and poly4,8-bis[(2- ethylhexyl)oxy]benzo[1,2-b:4,5-b']dithiophene-2,6-diyl][3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3,4-b] thiophenediyl (PTB7). Therefore, the possibility of combining these polymers with semiconductor nanocrystals deserves consideration. Here, we present the first comparison of solar cells based on PCDTBT and PTB7 where CdSe quantum dots serve as acceptors. We have found that PTB7-based cells are more efficient than PCDTBT-based ones. The efficiency also strongly depends on the nanocrystal size. An increase in the QD diameter from 5 to 10 nm causes a more than fourfold increase in the cell efficiency. This is determined by the relationship between the nanoparticle size and energy spectrum, its pattern clearly demonstrating how the mutual positions of the donor and acceptor levels affect the solar cell efficiency. These results will help to develop novel, improved nanohybrid components of solar cells based on organic semiconductors and semiconductor nanocrystals.

  19. Si nanocrystals and nanocrystal interfaces studied by positron annihilation

    NASA Astrophysics Data System (ADS)

    Kujala, J.; Slotte, J.; Tuomisto, F.; Hiller, D.; Zacharias, M.

    2016-10-01

    Si nanocrystals embedded in a SiO 2 matrix were studied with positron annihilation and photoluminescence spectroscopies. Analysis of the S- and W-parameters for the sample annealed at 800 °C reveals a positron trap at the interface between the amorphous nanodots and the surrounding matrix. Another trap state is observed in the 1150 °C heat treated samples where nanodots are in a crystalline form. Positrons are most likely trapped to defects related to dangling bonds at the surface of the nanocrystals. Passivation of the samples results on one hand in the decrease of the S-parameter implying a decrease in the open volume of the interface state and, on the other hand, in the strengthening of the positron annihilation signal from the interface. The intensity of the photoluminescence signal increases with the formation of the nanocrystals. Passivation of samples strengthens the photoluminescence signal, further indicating a successful deactivation of luminescence quenching at the nanocrystal surface. Strengthening of the positron annihilation signal and an increase in the photoluminescence intensity in passivated silicon nanocrystals suggests that the positron trap at the interface does not contribute to a significant extent to the exciton recombination in the nanocrystals.

  20. Observation of size dependence in multicolor upconversion in single Yb3+, Er3+ Codoped NaYF4 nanocrystals.

    PubMed

    Schietinger, Stefan; Menezes, Leonardo de S; Lauritzen, Björn; Benson, Oliver

    2009-06-01

    In this Letter we report on the investigation of the upconversion emission of single NaYF(4) nanocrystals codoped with Yb(3+) and Er(3+). Single nanocrystals on a coverslip are excited with continuous wave laser light at 973 nm in a confocal setup and the upconversion fluorescence is analyzed with a spectrometer. With the help of an atomic force microscope the size of the nanocrystals is simultaneously determined. A strong size-dependence of the spectral properties of the upconversion signal of individual nanocrystals is observed. We attribute this to a differing number of available phonons in the individual crystals for multiphonon relaxation processes, depending on their size. We believe that this result provides a new strategy in the synthesis of upconversion nanoparticles with different spectral properties by changing only their size as it is well-known from the case of semiconductor quantum dots.

  1. Tailoring indium oxide nanocrystal synthesis conditions for air-stable high-performance solution-processed thin-film transistors.

    PubMed

    Swisher, Sarah L; Volkman, Steven K; Subramanian, Vivek

    2015-05-20

    Semiconducting metal oxides (ZnO, SnO2, In2O3, and combinations thereof) are a uniquely interesting family of materials because of their high carrier mobilities in the amorphous and generally disordered states, and solution-processed routes to these materials are of particular interest to the printed electronics community. Colloidal nanocrystal routes to these materials are particularly interesting, because nanocrystals may be formulated with tunable surface properties into stable inks, and printed to form devices in an additive manner. We report our investigation of an In2O3 nanocrystal synthesis for high-performance solution-deposited semiconductor layers for thin-film transistors (TFTs). We studied the effects of various synthesis parameters on the nanocrystals themselves, and how those changes ultimately impacted the performance of TFTs. Using a sintered film of solution-deposited In2O3 nanocrystals as the TFT channel material, we fabricated devices that exhibit field effect mobility of 10 cm(2)/(V s) and an on/off current ratio greater than 1 × 10(6). These results outperform previous air-stable nanocrystal TFTs, and demonstrate the suitability of colloidal nanocrystal inks for high-performance printed electronics.

  2. Tailoring indium oxide nanocrystal synthesis conditions for air-stable high-performance solution-processed thin-film transistors.

    PubMed

    Swisher, Sarah L; Volkman, Steven K; Subramanian, Vivek

    2015-05-20

    Semiconducting metal oxides (ZnO, SnO2, In2O3, and combinations thereof) are a uniquely interesting family of materials because of their high carrier mobilities in the amorphous and generally disordered states, and solution-processed routes to these materials are of particular interest to the printed electronics community. Colloidal nanocrystal routes to these materials are particularly interesting, because nanocrystals may be formulated with tunable surface properties into stable inks, and printed to form devices in an additive manner. We report our investigation of an In2O3 nanocrystal synthesis for high-performance solution-deposited semiconductor layers for thin-film transistors (TFTs). We studied the effects of various synthesis parameters on the nanocrystals themselves, and how those changes ultimately impacted the performance of TFTs. Using a sintered film of solution-deposited In2O3 nanocrystals as the TFT channel material, we fabricated devices that exhibit field effect mobility of 10 cm(2)/(V s) and an on/off current ratio greater than 1 × 10(6). These results outperform previous air-stable nanocrystal TFTs, and demonstrate the suitability of colloidal nanocrystal inks for high-performance printed electronics. PMID:25915094

  3. Early stage of nanocrystal growth

    SciTech Connect

    2012-01-01

    Berkeley Lab researchers at the Molecular Foundry have elucidated important mechanisms behind oriented attachment, the phenomenon that drives biomineralization and the growth of nanocrystals. This electron microscopy movie shows the early stage of nanocrystal growth. Nanoparticles make transient contact at many points and orientations until their lattices are perfectly matched. The particles then make a sudden jump-to-contact to form attached aggregates. (Movie courtesy of Jim DeYoreo)

  4. The dependence of lead-salt nanocrystal properties on morphology and dielectric environment

    NASA Astrophysics Data System (ADS)

    Bartnik, Adam Christopher

    The IV-VI semiconductors, and specifically the lead-salts (PbS, PbSe, and PbTe), are a natural choice for nanocrystal science. In nanocrystals, because of their narrow band gap, small effective masses, and large dielectric constants, they offer a unique combination of both strong confinement and strong dielectric contrast with their environment. Studying how these two effects modify optical and electrical properties of nanocrystals will be the topic of this dissertation. We begin with a summary of the synthesis of high-quality PbS and PbSe nanocrystals. Special care is taken to explain the chemical procedures in detail to an audience not expected to have significant prior chemistry knowledge. The synthesized nanocrystals have bright and tunable emission that spans the edge of the visible to the near-IR spectrum (700--1800 nm), and they are capped with organic ligands making them easily adaptable to different substrates or hosts. This combination of high optical quality and flexible device engineering make them extremely desirable for application. Moving beyond single-material nanocrystals, we next explore nanocrystal heterostructures, specifically materials with a spherical core of one semiconductor and a shell of another. Core-shell structures are commonly used in nanocrystals as a method to separate the core material, where the electrons and holes are expected to stay, from interfering effects at the surface. This typically results in improvements in stability and fluorescence quantum efficiency. To that end, we develop a model to explain how confinement plays out across abrupt changes in material, focusing on the optical and electrical properties of recently synthesized PbSe/PbS core-shell quantum dots. We show that for typical sizes of these nanocrystals, a novel type of nanocrystal heterostructure is created, where electrons and holes extend uniformly across the abrupt material boundary, and the shell does not act as a protecting layer. For very large sizes

  5. Synthesis and photocatalytic properties of multi-morphological AuCu3-ZnO hybrid nanocrystals

    NASA Astrophysics Data System (ADS)

    Zeng, Deqian; Chen, Yuanzhi; Peng, Jian; Xie, Qingshui; Peng, Dong-Liang

    2015-10-01

    Noble metal-semiconductor hybrid nanocrystals represent an important class of materials for many potential applications, especially for photocatalysis. The utilization of transition metals to form alloys with noble metals can not only reduce the preparation costs, but may also offer tunable optical and catalytic properties for a broader range of applications. In this study, we report on the solution synthesis of AuCu3-ZnO hybrid nanocrystals with three interesting morphologies, including urchin-like, flower-like and multipod-like nanocrystals. In the synthetic strategy, Au-Cu bimetallic alloy seeds formed in situ are used to induce the heteroepitaxial growth of ZnO nanocrystals on the surface of bimetallic alloy cores; thus different types of morphologies can be achieved by controlling the reaction conditions. Through high-resolution transmission electron microscopy observations, well-defined interfaces between ZnO and AuCu3 are observed, which indicate that ZnO has a (0001) orientation and prefers to grow on AuCu3 {111} facets. The as-prepared hybrid nanocrystals demonstrate morphology- and composition-dependent surface plasmon resonance (SPR) absorption bands. In addition, much higher photocatalytic efficiency than pure ZnO nanocrystals is observed for the hybrid nanocrystals in the degradation of methylene blue. In particular, the multipod-like AuCu3-ZnO hybrid nanocrystals show the highest catalytic performance, as well as more than three times higher photocurrent density than the pure ZnO sample. The reported synthetic strategy provides a facile route to the effective combination of a plasmonic alloy with semiconductor components at the nanoscale in a controlled manner.

  6. Symmetry-defying iron pyrite (FeS₂) nanocrystals through oriented attachment.

    PubMed

    Gong, Maogang; Kirkeminde, Alec; Ren, Shenqiang

    2013-01-01

    Iron pyrite (fool's gold, FeS₂) is a promising earth abundant and environmentally benign semiconductor material that shows promise as a strong and broad absorber for photovoltaics and high energy density cathode material for batteries. However, controlling FeS₂ nanocrystal formation (composition, size, shape, stoichiometry, etc.) and defect mitigation still remains a challenge. These problems represent significant limitations in the ability to control electrical, optical and electrochemical properties to exploit pyrite's full potential for sustainable energy applications. Here, we report a symmetry-defying oriented attachment FeS₂ nanocrystal growth by examining the nanostructure evolution and recrystallization to uncover how the shape, size and defects of FeS₂ nanocrystals changes during growth. It is demonstrated that a well-controlled reaction temperature and annealing time results in polycrystal-to-monocrystal formation and defect annihilation, which correlates with the performance of photoresponse devices. This knowledge opens up a new tactic to address pyrite's known defect problems.

  7. Formation of Ru nanocrystals by plasma enhanced atomic layer deposition for nonvolatile memory applications

    SciTech Connect

    Yim, Sung-Soo; Lee, Moon-Sang; Kim, Ki-Su; Kim, Ki-Bum

    2006-08-28

    The formation of Ru nanocrystals is demonstrated on a SiO{sub 2} substrate by plasma enhanced atomic layer deposition using diethylcyclopentadienyl ruthenium and NH{sub 3} plasma. The island growth of Ru was observed at the initial stages of the film formation up to a nominal thickness of 11.1 nm. A maximum Ru nanocrystal spatial density of 9.7x10{sup 11} /cm{sup 2} was achieved with an average size of 3.5 nm and standard deviation of the size of 20%. Electron charging/discharging effect in the Ru nanocrystals is demonstrated by measuring the flatband voltage shift in the capacitance-voltage measurement of metal-oxide-semiconductor memory capacitor structure.

  8. Physical preparation and optical properties of CuSbS2 nanocrystals by mechanical alloying process

    NASA Astrophysics Data System (ADS)

    Zhang, Huihui; Xu, Qishu; Tan, Guolong

    2016-09-01

    CuSbS2 nanocrystals have been synthesized through mechanical alloying Cu, Sb and S elemental powders for 40 hs. The optical spectrum of as-milled CuSbS2 nano-powders demonstrates a direct gap of 1.35 eV and an indirect gap of 0.36 eV, which are similar to that of silicon and reveals the evidence for the indirect semiconductor characterization of CuSbS2. Afterwards, CuSbS2 nanocrystals were capped with trioctylphosphine oxide/trioctylphosphine/pyridine (TOPO/TOP). There appear four sharp absorption peaks within the region of 315 to 355 nm for the dispersion solution containing the capped nanocrystals. The multiple peaks are proposed to be originating from the energy level splitting of 1S electronic state into four discrete sub-levels, where electrons were excited into the conduction band and thus four exciton absorption peaks were produced.

  9. Electronic Band Structures and Native Point Defects of Ultrafine ZnO Nanocrystals.

    PubMed

    Zeng, Yu-Jia; Schouteden, Koen; Amini, Mozhgan N; Ruan, Shuang-Chen; Lu, Yang-Fan; Ye, Zhi-Zhen; Partoens, Bart; Lamoen, Dirk; Van Haesendonck, Chris

    2015-05-20

    Ultrafine ZnO nanocrystals with a thickness down to 0.25 nm are grown by a metalorganic chemical vapor deposition method. Electronic band structures and native point defects of ZnO nanocrystals are studied by a combination of scanning tunneling microscopy/spectroscopy and first-principles density functional theory calculations. Below a critical thickness of ∼1 nm ZnO adopts a graphitic-like structure and exhibits a wide band gap similar to its wurtzite counterpart. The hexagonal wurtzite structure, with a well-developed band gap evident from scanning tunneling spectroscopy, is established for a thickness starting from ∼1.4 nm. With further increase of the thickness to 2 nm, VO-VZn defect pairs are easily produced in ZnO nanocrystals due to the self-compensation effect in highly doped semiconductors. PMID:25923131

  10. Effect of hydrogen passivation on the electronic structure of ionic semiconductor nanostructures

    NASA Astrophysics Data System (ADS)

    Deng, Hui-Xiong; Li, Shu-Shen; Li, Jingbo; Wei, Su-Huai

    2012-05-01

    In theoretical studies of thin film and nanostructured semiconductors, pseudohydrogen (PH) is widely used to passivate the surface dangling bonds. Based on these calculations, it is often believed that nanostructured semiconductors, due to quantum confinement, have a larger band gap than their bulk counterparts. Using first-principles band structure theory calculation and comparing systematically the differences between PH-passivated and real-hydrogen-passivated (RH-passivated) semiconductor surfaces and nanocrystals, we show that, unlike PH passivation that always increases the band gap with respect to the bulk value, RH passivation of the nanostructured semiconductors can either increase or decrease the band gap, depending on the ionicity of the nanocompounds. The differences between PH and RH passivations decreases when the covalency of the semiconductor increases and can be explained using a band coupling model. This observation greatly increases the tunability of nanostructured semiconductor properties, especially for wide-gap ionic semiconductors.

  11. Assemblies of Cellulose Nanocrystals

    NASA Astrophysics Data System (ADS)

    Kumacheva, Eugenia

    The entropically driven coassembly of nanorods (cellulose nanocrystals, CNCs) and different types of nanoparticles (NPs), including dye-labeled latex NPs, carbon dots and plasmonic NPs was experimentally studied in aqueous suspensions and in solid films. In mixed CNC-NP suspensions, phase separation into an isotropic NP-rich and a chiral nematic CNC-rich phase took place; the latter contained a significant amount of NPs. Drying the mixed suspension resulted in CNC-NP films with planar disordered layers of NPs, which alternated with chiral nematic CNC-rich regions. In addition, NPs were embedded in the chiral nematic domains. The stratified morphology of the films, together with a random distribution of NPs in the anisotropic phase, led to the films having close-to-uniform fluorescence, birefringence, and circular dichroism properties.

  12. Luminescent nanocrystal stress gauge

    PubMed Central

    Choi, Charina L.; Koski, Kristie J.; Olson, Andrew C. K.; Alivisatos, A. Paul

    2010-01-01

    Microscale mechanical forces can determine important outcomes ranging from the site of material fracture to stem cell fate. However, local stresses in a vast majority of systems cannot be measured due to the limitations of current techniques. In this work, we present the design and implementation of the CdSe-CdS core-shell tetrapod nanocrystal, a local stress sensor with bright luminescence readout. We calibrate the tetrapod luminescence response to stress and use the luminescence signal to report the spatial distribution of local stresses in single polyester fibers under uniaxial strain. The bright stress-dependent emission of the tetrapod, its nanoscale size, and its colloidal nature provide a unique tool that may be incorporated into a variety of micromechanical systems including materials and biological samples to quantify local stresses with high spatial resolution. PMID:21098301

  13. Diffraction by nanocrystals II.

    PubMed

    Chen, Joe P J; Millane, Rick P

    2014-08-01

    Nanocrystals with more than one molecule in the unit cell will generally crystallize with incomplete unit cells on the crystal surface. Previous results show that the ensemble-averaged diffraction by such crystals consists of a usual Bragg component and two other Bragg-like components due to the incomplete unit cells. Using an intrinsic flexibility in the definition of the incomplete-unit-cell part of a crystal, the problem is formulated such that the magnitude of the Bragg-like components is minimized, which leads to a simpler and more useful interpretation of the diffraction. Simulations show the nature of the relative magnitudes of the diffraction components in different regions of reciprocal space and the effect of crystal faceting. PMID:25121528

  14. Tunable and responsive plasmonic properties of metal oxide nanocrystals

    NASA Astrophysics Data System (ADS)

    Milliron, Delia

    2015-03-01

    Degenerately doped metal oxide semiconductors, like ITO, exhibit plasmonic resonance at near and mid-infrared wavelengths tunable by varying their composition. Nanocrystals of many such materials have now been synthesized and applications are emerging that leverage the responsiveness of their localized surface plasmon resonance (LSPR) to electronic charging and discharging. For example, electrochromic glass that can dynamically control heat loads in buildings is under development. In biological systems, plasmonic oxide nanocrystals can act as remote sensors, where changes in their optical absorption indicates biochemical redox has occurred. Nonetheless, significant fundamental questions remain open regarding the nature of the infrared optical response in these doped oxides. Dopant impurities influence the optoelectronic properties beyond simply donating free carriers. For example, the distribution of Sn in ITO was found to dramatically influence the line shape of the LSPR and the effective electron mobility. In addition, by post-synthetically modifying carrier concentrations (through photodoping or electrochemical doping), we have observed that aliovalent doping and electronic doping each modify LSPR spectra, providing access to a broad range of tunable optical properties. Heterogeneous broadening, uncovered by single nanocrystal spectroscopy, also contributes to ensemble line shapes, complicating direct interpretation of LSPR spectra. Finally, the possibility of electric field enhancement by metal oxide LSPRs is critically examined to suggest what future applications might be on the horizon.

  15. Acoustic vibrations of semiconductor nanocrystals in doped glasses

    NASA Astrophysics Data System (ADS)

    Verma, Prabhat; Cordts, W.; Irmer, G.; Monecke, J.

    1999-08-01

    Polarization-dependent low-frequency off-resonant Raman scattering has been studied from various commercially available filter glass samples, which contain CdSxSe1-x nanoparticles embedded in a glass matrix. In order to distinguish the confined acoustic phonons from the glass background, the spectra have been compared with those obtained from the base material, which does not contain nanoparticles. Polarized and depolarized scattering from confined acoustic phonons was distinctly resolved near the laser line and overtones of the polarized modes were observed. A theoretical treatment, which establishes a relation between the particle size, the frequencies, and the widths of various phonons, taking into account the matrix influence on the vibrational spectrum and on its damping, is presented. The material-dependent generalized form of this model enables one to use it for any given combination of particle and matrix materials. A good agreement between the experimental and the theoretical results is found. The nanoparticle sizes obtained from Raman scattering agree well with those obtained from transmission electron microscope and anomalous small angle x-ray scattering experiments.

  16. Methods for synthesis of semiconductor nanocrystals and thermoelectric compositions

    NASA Technical Reports Server (NTRS)

    Ren, Zhifeng (Inventor); Chen, Gang (Inventor); Poudel, Bed (Inventor); Kumar, Shankar (Inventor); Wang, Wenzhong (Inventor); Dresselhaus, Mildred (Inventor)

    2007-01-01

    The present invention provides methods for synthesis of IV VI nanostructures, and thermoelectric compositions formed of such structures. In one aspect, the method includes forming a solution of a Group IV reagent, a Group VI reagent and a surfactant. A reducing agent can be added to the solution, and the resultant solution can be maintained at an elevated temperature, e.g., in a range of about 20.degree. C. to about 360.degree. C., for a duration sufficient for generating nanoparticles as binary alloys of the IV VI elements.

  17. Methods for synthesis of semiconductor nanocrystals and thermoelectric compositions

    DOEpatents

    Ren, Zhifeng; Chen, Gang; Poudel, Bed; Kumar, Shankar; Wang, Wenzhong; Dresselhaus, Mildred

    2007-08-14

    The present invention provides methods for synthesis of IV VI nanostructures, and thermoelectric compositions formed of such structures. In one aspect, the method includes forming a solution of a Group IV reagent, a Group VI reagent and a surfactant. A reducing agent can be added to the solution, and the resultant solution can be maintained at an elevated temperature, e.g., in a range of about 20.degree. C. to about 360.degree. C., for a duration sufficient for generating nanoparticles as binary alloys of the IV VI elements.

  18. Cu nanocrystal growth on peptide nanotubes by biomineralization: Size control of Cu nanocrystals by tuning peptide conformation

    NASA Astrophysics Data System (ADS)

    Banerjee, Ipsita A.; Yu, Lingtao; Matsui, Hiroshi

    2003-12-01

    With recent interest in seeking new biologically inspired device-fabrication methods in nanotechnology, a new biological approach was examined to fabricate Cu nanotubes by using sequenced histidine-rich peptide nanotubes as templates. The sequenced histidine-rich peptide molecules were assembled as nanotubes, and the biological recognition of the specific sequence toward Cu lead to efficient Cu coating on the nanotubes. Cu nanocrystals were uniformly coated on the histidine-incorporated nanotubes with high packing density. In addition, the diameter of Cu nanocrystal was controlled between 10 and 30 nm on the nanotube by controlling the conformation of histidine-rich peptide by means of pH changes. Those nanotubes showed significant change in electronic structure by varying the nanocrystal diameter; therefore, this system may be developed to a conductivity-tunable building block for microelectronics and biological sensors. This simple biomineralization method can be applied to fabricate various metallic and semiconductor nanotubes with peptides whose sequences are known to mineralize specific ions.

  19. Silicon nanocrystal-noble metal hybrid nanoparticles

    NASA Astrophysics Data System (ADS)

    Sugimoto, H.; Fujii, M.; Imakita, K.

    2016-05-01

    We report a novel and facile self-limiting synthesis route of silicon nanocrystal (Si NC)-based colloidally stable semiconductor-metal (gold, silver and platinum) hybrid nanoparticles (NPs). For the formation of hybrid NPs, we employ ligand-free colloidal Si NCs with heavily boron (B) and phosphorus (P) doped shells. By simply mixing B and P codoped colloidal Si NCs with metal salts, hybrid NPs consisting of metal cores and Si NC shells are spontaneously formed. We demonstrate the synthesis of highly uniform and size controllable hybrid NPs. It is shown that codoped Si NCs act as a reducing agent for metal salts and also as a protecting layer to stop metal NP growth. The process is thus self-limiting. The development of a variety of Si NC-based hybrid NPs is a promising first step for the design of biocompatible multifunctional NPs with broad material choices for biosensing, bioimaging and solar energy conversion.We report a novel and facile self-limiting synthesis route of silicon nanocrystal (Si NC)-based colloidally stable semiconductor-metal (gold, silver and platinum) hybrid nanoparticles (NPs). For the formation of hybrid NPs, we employ ligand-free colloidal Si NCs with heavily boron (B) and phosphorus (P) doped shells. By simply mixing B and P codoped colloidal Si NCs with metal salts, hybrid NPs consisting of metal cores and Si NC shells are spontaneously formed. We demonstrate the synthesis of highly uniform and size controllable hybrid NPs. It is shown that codoped Si NCs act as a reducing agent for metal salts and also as a protecting layer to stop metal NP growth. The process is thus self-limiting. The development of a variety of Si NC-based hybrid NPs is a promising first step for the design of biocompatible multifunctional NPs with broad material choices for biosensing, bioimaging and solar energy conversion. Electronic supplementary information (ESI) available: Additional TEM images and extinction spectra of Si-metal hybrid NPs are shown in Fig. S1

  20. Controlled Crystallinity and Fundamental Coupling Interactions in Nanocrystals

    NASA Astrophysics Data System (ADS)

    Ouyang, Min

    2009-03-01

    Metal and semiconductor nanocrystals show many unusual properties and functionalities, and can serve as model system to explore fundamental quantum and classical coupling interactions as well as building blocks of many practical applications. However, because of their small size, these nanoparticles typically exhibit different crystalline properties as compared with their bulk counterpart, and controlling crystallinity (and structural defects) within nanoparticles has posed significant technical challenges. In this talk, I will firstly apply silver metal nanoparticles as an example and present a novel chemical synthetic technique to achieve unprecedented crystallinity control at the nanoscale. This engineering of nanocrystallinity enables manipulation of intrinsic chemical functionalities, physical properties as well as nano-device performance [1]. For example, I will highlight that electron- phonon coupling constant can be significantly reduced by about four times and elastic modulus is increased ˜40% in perfect single crystalline silver nanoparticles as compared with those in disordered twinned nanoparticles. One important application of metal nanoparticles is nanoscale sensors. I will thus demonstrate that performance of nanoparticles based molecular sensing devices can be optimized with three times improvement of figure-of-merit if perfect single crystalline nanoparticles are applied. Lastly, I will present our related studies on semiconductor nanocrystals as well as their hybrid heterostructures. These discussions should offer important implications for our understanding of the fundamental properties at nanoscale and potential applications of metal nanoparticles. [4pt] [1] Yun Tang and Min Ouyang, Nature Materials, 6, 754, 2007.

  1. High efficiency solution processed sintered CdTe nanocrystal solar cells: the role of interfaces.

    PubMed

    Panthani, Matthew G; Kurley, J Matthew; Crisp, Ryan W; Dietz, Travis C; Ezzyat, Taha; Luther, Joseph M; Talapin, Dmitri V

    2014-02-12

    Solution processing of photovoltaic semiconducting layers offers the potential for drastic cost reduction through improved materials utilization and high device throughput. One compelling solution-based processing strategy utilizes semiconductor layers produced by sintering nanocrystals into large-grain semiconductors at relatively low temperatures. Using n-ZnO/p-CdTe as a model system, we fabricate sintered CdTe nanocrystal solar cells processed at 350 °C with power conversion efficiencies (PCE) as high as 12.3%. JSC of over 25 mA cm(-2) are achieved, which are comparable or higher than those achieved using traditional, close-space sublimated CdTe. We find that the VOC can be substantially increased by applying forward bias for short periods of time. Capacitance measurements as well as intensity- and temperature-dependent analysis indicate that the increased VOC is likely due to relaxation of an energetic barrier at the ITO/CdTe interface.

  2. Off-Resonance Photosensitization of a Photorefractive Polymer Composite Using PbS Nanocrystals

    SciTech Connect

    Moon, Jong-Sik; Liang, Yichen; Stevens, Tyler E.; Monson, Todd C.; Huber, Dale L.; Mahala, Benjamin D.; Winiarz, Jeffrey G.

    2015-05-26

    The photosensitization of photorefractive polymeric composites for operation at 633 nm is accomplished through the inclusion of narrow band gap semiconductor nanocrystals composed of PbS. Unlike previous studies involving photosensitization of photorefractive polymer composites with inorganic nanocrystals, we employ an off-resonance approach where the first excitonic transition associated with the PbS nanocrystals lies at ~1220 nm and not the wavelength of operation. Using this methodology, internal diffraction efficiencies exceeding 82%, two-beam-coupling gain coefficients of 211 cm–1, and response times of 34 ms have been observed, representing some of the best figures of merit reported for this class of materials. Furthermore, these data demonstrate the ability of semiconductor nanocrystals to compete effectively with traditional organic photosensitizers. In addition to superior performance, this approach also offers an inexpensive and easy means by which to photosensitize composite materials. Additionally, the photoconductive characteristics of the composites used for this study will also be considered.

  3. Off-Resonance Photosensitization of a Photorefractive Polymer Composite Using PbS Nanocrystals

    DOE PAGESBeta

    Moon, Jong-Sik; Liang, Yichen; Stevens, Tyler E.; Monson, Todd C.; Huber, Dale L.; Mahala, Benjamin D.; Winiarz, Jeffrey G.

    2015-05-26

    The photosensitization of photorefractive polymeric composites for operation at 633 nm is accomplished through the inclusion of narrow band gap semiconductor nanocrystals composed of PbS. Unlike previous studies involving photosensitization of photorefractive polymer composites with inorganic nanocrystals, we employ an off-resonance approach where the first excitonic transition associated with the PbS nanocrystals lies at ~1220 nm and not the wavelength of operation. Using this methodology, internal diffraction efficiencies exceeding 82%, two-beam-coupling gain coefficients of 211 cm–1, and response times of 34 ms have been observed, representing some of the best figures of merit reported for this class of materials. Furthermore,more » these data demonstrate the ability of semiconductor nanocrystals to compete effectively with traditional organic photosensitizers. In addition to superior performance, this approach also offers an inexpensive and easy means by which to photosensitize composite materials. Additionally, the photoconductive characteristics of the composites used for this study will also be considered.« less

  4. Laser-induced growth of nanocrystals embedded in porous materials

    PubMed Central

    2013-01-01

    Space localization of the linear and nonlinear optical properties in a transparent medium at the submicron scale is still a challenge to yield the future generation of photonic devices. Laser irradiation techniques have always been thought to structure the matter at the nanometer scale, but combining them with doping methods made it possible to generate local growth of several types of nanocrystals in different kinds of silicate matrices. This paper summarizes the most recent works developed in our group, where the investigated nanoparticles are either made of metal (gold) or chalcogenide semiconductors (CdS, PbS), grown in precursor-impregnated porous xerogels under different laser irradiations. This review is associated to new results on silver nanocrystals in the same kind of matrices. It is shown that, depending on the employed laser, the particles can be formed near the sample surface or deep inside the silica matrix. Photothermal and/or photochemical mechanisms may be invoked to explain the nanoparticle growth, depending on the laser, precursor, and matrix. One striking result is that metal salt reduction, necessary to the production of the corresponding nanoparticles, can efficiently occur due to the thermal wrenching of electrons from the matrix itself or due to multiphoton absorption of the laser light by a reducer additive in femtosecond regime. Very localized semiconductor quantum dots could also be generated using ultrashort pulses, but while PbS nanoparticles grow faster than CdS particles due to one-photon absorption, this better efficiency is counterbalanced by a sensitivity to oxidation. In most cases where the reaction efficiency is high, particles larger than the pores have been obtained, showing that a fast diffusion of the species through the interconnected porosity can modify the matrix itself. Based on our experience in these techniques, we compare several examples of laser-induced nanocrystal growth in porous silica xerogels, which allows

  5. Laser-induced growth of nanocrystals embedded in porous materials

    NASA Astrophysics Data System (ADS)

    Capoen, Bruno; Chahadih, Abdallah; El Hamzaoui, Hicham; Cristini, Odile; Bouazaoui, Mohamed

    2013-06-01

    Space localization of the linear and nonlinear optical properties in a transparent medium at the submicron scale is still a challenge to yield the future generation of photonic devices. Laser irradiation techniques have always been thought to structure the matter at the nanometer scale, but combining them with doping methods made it possible to generate local growth of several types of nanocrystals in different kinds of silicate matrices. This paper summarizes the most recent works developed in our group, where the investigated nanoparticles are either made of metal (gold) or chalcogenide semiconductors (CdS, PbS), grown in precursor-impregnated porous xerogels under different laser irradiations. This review is associated to new results on silver nanocrystals in the same kind of matrices. It is shown that, depending on the employed laser, the particles can be formed near the sample surface or deep inside the silica matrix. Photothermal and/or photochemical mechanisms may be invoked to explain the nanoparticle growth, depending on the laser, precursor, and matrix. One striking result is that metal salt reduction, necessary to the production of the corresponding nanoparticles, can efficiently occur due to the thermal wrenching of electrons from the matrix itself or due to multiphoton absorption of the laser light by a reducer additive in femtosecond regime. Very localized semiconductor quantum dots could also be generated using ultrashort pulses, but while PbS nanoparticles grow faster than CdS particles due to one-photon absorption, this better efficiency is counterbalanced by a sensitivity to oxidation. In most cases where the reaction efficiency is high, particles larger than the pores have been obtained, showing that a fast diffusion of the species through the interconnected porosity can modify the matrix itself. Based on our experience in these techniques, we compare several examples of laser-induced nanocrystal growth in porous silica xerogels, which allows

  6. Optical properties and ensemble characteristics of size purified Silicon nanocrystals

    NASA Astrophysics Data System (ADS)

    Miller, Joseph Bradley

    Nanotechnology is at the forefront of current scientific research and nanocrystals are being hailed as the 'artificial' atoms of the 21st century. Semiconducting silicon nanocrystals (SiNCs) are prime candidates for potential commercial applications because of silicon's already ubiquitous presence in the semiconductor industry, nontoxicity and abundance in nature. For realization of these potential applications, the properties and behavior of SiNCs need to be understood and enhanced. In this report, some of the main SiNC synthesis schemes are discussed, including those we are currently experimenting with to create our own SiNCs and the one utilized to create the SiNCs used in this study. The underlying physics that governs the unique behavior of SiNCs is then presented. The properties of the as-produced SiNCs are determined to depend strongly on surface passivation and environment. Size purification, an important aspect of nanomaterial utilization, was successfully performed on our SiNCs though density gradient ultracentrifugation. We demonstrate that the size-purified fractions exhibit an enhanced ability for colloidal self-assembly, with better aligned nanocrystal energy levels which promotes greater photostability in close-packed films and produces a slight increase in photoluminescence (PL) quantum yield. The qualities displayed by the fractions are exploited to form SiNC clusters that exhibit photostable PL. An analysis of SiNC cluster (from individual nanocrystals to collections of more than one thousand) blinking and PL shows an improvement in their PL emitting 'on' times. Pure SiNC films and SiNC-polymer nanocomposites are created and the dependence of their PL on temperature is measured. For such nanocomposites, the coupling between the 'coffee-ring' effect and liquid-liquid phase separation is also examined for ternary mixtures of solvent, polymer and semiconducting nanocrystal. We discover that with the right SiNC-polymer concentration and polymer

  7. A dual-colored bio-marker made of doped ZnO nanocrystals

    NASA Astrophysics Data System (ADS)

    Wu, Y. L.; Fu, S.; Tok, A. I. Y.; Zeng, X. T.; Lim, C. S.; Kwek, L. C.; Boey, F. C. Y.

    2008-08-01

    Bio-compatible ZnO nanocrystals doped with Co, Cu and Ni cations, surface capped with two types of aminosilanes and titania are synthesized by a soft chemical process. Due to the small particle size (2-5 nm), surface functional groups and the high photoluminescence emissions at the UV and blue-violet wavelength ranges, bio-imaging on human osteosarcoma (Mg-63) cells and histiocytic lymphoma U-937 monocyte cells showed blue emission at the nucleus and bright turquoise emission at the cytoplasm simultaneously. This is the first report on dual-color bio-images labeled by one semiconductor nanocrystal colloidal solution. Bright green emission was detected on mung bean seedlings labeled by all the synthesized ZnO nanocrystals. Cytotoxicity tests showed that the aminosilanes capped nanoparticles are non-toxic. Quantum yields of the nanocrystals varied from 79% to 95%. The results showed the potential of the pure ZnO and Co-doped ZnO nanocrystals for live imaging of both human cells and plant systems.

  8. Influence of dopant distribution on the plasmonic properties of indium tin oxide nanocrystals.

    PubMed

    Lounis, Sebastien D; Runnerstrom, Evan L; Bergerud, Amy; Nordlund, Dennis; Milliron, Delia J

    2014-05-14

    Doped metal oxide nanocrystals represent an exciting frontier for colloidal synthesis of plasmonic materials, displaying unique optoelectronic properties and showing promise for a variety of applications. However, fundamental questions about the nature of doping in these materials remain. In this article, the strong influence of radial dopant distribution on the optoelectronic properties of colloidal indium tin oxide nanocrystals is reported. Comparing elemental depth-profiling by X-ray photoelectron spectroscopy (XPS) with detailed modeling and simulation of the optical extinction of these nanocrystals using the Drude model for free electrons, a correlation between surface segregation of tin ions and the average activation of dopants is observed. A strong influence of surface segregation of tin on the line shape of the localized surface plasmon resonance (LSPR) is also reported. Samples with tin segregated near the surface show a symmetric line shape that suggests weak or no damping of the plasmon by ionized impurities. It is suggested that segregation of tin near the surface facilitates compensation of the dopant ions by electronic defects and oxygen interstitials, thus reducing activation. A core-shell model is proposed to explain the observed differences in line shape. These results demonstrate the nuanced role of dopant distribution in determining the optoelectronic properties of semiconductor nanocrystals and suggest that more detailed study of the distribution and structure of defects in plasmonic colloidal nanocrystals is warranted.

  9. A dual-colored bio-marker made of doped ZnO nanocrystals.

    PubMed

    Wu, Y L; Fu, S; Tok, A I Y; Zeng, X T; Lim, C S; Kwek, L C; Boey, F C Y

    2008-08-27

    Bio-compatible ZnO nanocrystals doped with Co, Cu and Ni cations, surface capped with two types of aminosilanes and titania are synthesized by a soft chemical process. Due to the small particle size (2-5 nm), surface functional groups and the high photoluminescence emissions at the UV and blue-violet wavelength ranges, bio-imaging on human osteosarcoma (Mg-63) cells and histiocytic lymphoma U-937 monocyte cells showed blue emission at the nucleus and bright turquoise emission at the cytoplasm simultaneously. This is the first report on dual-color bio-images labeled by one semiconductor nanocrystal colloidal solution. Bright green emission was detected on mung bean seedlings labeled by all the synthesized ZnO nanocrystals. Cytotoxicity tests showed that the aminosilanes capped nanoparticles are non-toxic. Quantum yields of the nanocrystals varied from 79% to 95%. The results showed the potential of the pure ZnO and Co-doped ZnO nanocrystals for live imaging of both human cells and plant systems.

  10. Influence of Dopant Distribution on the Plasmonic Properties of Indium Tin Oxide Nanocrystals

    SciTech Connect

    Lounis, SD; Runnerstrom, EL; Bergerud, A; Nordlund, D; Milliron, DJ

    2014-05-14

    Doped metal oxide nanocrystals represent an exciting frontier for colloidal synthesis of plasmonic materials, displaying unique optoelectronic properties and showing promise for a variety of applications. However, fundamental questions about the nature of doping in these materials remain. In this article, the strong influence of radial dopant distribution on the optoelectronic properties of colloidal indium tin oxide nanocrystals is reported. Comparing elemental depth-profiling by X-ray photoelectron spectroscopy (XPS) with detailed modeling and simulation of the optical extinction of these nanocrystals using the Drude model for free electrons, a correlation between surface segregation of tin ions and the average activation of dopants is observed. A strong influence of surface segregation of tin on the line shape of the localized surface plasmon resonance (LSPR) is also reported. Samples with tin segregated near the surface show a symmetric line shape that suggests weak or no damping of the plasmon by ionized impurities. It is suggested that segregation of tin near the surface facilitates compensation of the dopant ions by electronic defects and oxygen interstitials, thus reducing activation. A core shell model is proposed to explain the observed differences in line shape. These results demonstrate the nuanced role of dopant distribution in determining the optoelectronic properties of semiconductor nanocrystals and suggest that more detailed study of the distribution and structure of defects in plasmonic colloidal nanocrystals is warranted.

  11. Molybdenum and Tungsten Sulfide Ligands for Versatile Functionalization of All-Inorganic Nanocrystals.

    PubMed

    Ban, Hyeong Woo; Park, Sangmin; Jeong, Hyewon; Gu, Da Hwi; Jo, Seungki; Park, Sung Hoon; Park, Jongnam; Son, Jae Sung

    2016-09-15

    We report a strategy toward the synthesis of colloidal nanocrystals capped with inorganic molybdenum and tungsten sulfide ligands. MoS4(2-) and WS4(2-) thiometalates were utilized to replace organic ligands capping a wide range of nanocrystals such as metals, semiconductors, and well-conserved primary properties of nanocrystals in polar media. Especially, MoS4(2-)- and WS4(2-)-capped CdSe nanocryatals showed the dramatic enhancement of photoluminescence properties by the photo-oxidation treatment, which originated from the preferential formation of MoSxOy layers on the CdSe surface. The highest quantum yield reached up to 51%. Furthermore, we studied the charge-transport properties of MoS4(2-)-capped PbS nanocryatals by the fabrication of a field-effect transistor and photodetectors. Finally, MoS4(2-)- and WS4(2-)-capped nanocrystals were used for the production of two-dimensional MoS2 and WS2 thin layers on nanostructures by heat treatment. Such versatility of these thiometalate ligands offers an additional degree of control over the functionality of nanocrystals for optoelectronic and catalytic applications. PMID:27571033

  12. Colloidal CIGS and CZTS nanocrystals: A precursor route to printed photovoltaics

    SciTech Connect

    Akhavan, Vahid A.; Goodfellow, Brian W.; Panthani, Matthew G.; Steinhagen, Chet; Harvey, Taylor B.; Stolle, C. Jackson; Korgel, Brian A.

    2012-05-15

    This review article summarizes our research focused on Cu(In{sub 1-x}Ga{sub x})Se{sub 2} (CIGS) nanocrystals, including their synthesis and implementation as the active light absorbing material in photovoltaic devices (PVs). CIGS PV layers are typically made using a high temperature (>450 Degree-Sign C) process in which Cu, In and Ga are sequentially or co-evaporated and selenized. We have sought to use CIGS nanocrystals synthesized with the desired stoichiometry to deposit PV device layers without high temperature processing. This approach, using spray deposition of the CIGS light absorber layers, without high temperature selenization, has enabled up to 3.1% power conversion efficiency under AM 1.5 solar illumination. Although the device efficiency is too low for commercialization, these devices provide a proof-of-concept that solution-deposited CIGS nanocrystal films can function in PV devices, enabling unconventional device architectures and materials combinations, including the use of flexible, inexpensive and light-weight plastic substrates. - Graphical abstract: The semiconductor light-absorbing layers in photovoltaic devices can be deposited under ambient conditions using nanocrystal inks. Devices can be fabricated on glass or on mechanically flexible plastic substrates. Highlights: Black-Right-Pointing-Pointer CIGS and CZTS nanocrystals are synthesized and formulated into inks. Black-Right-Pointing-Pointer Nanocrystal films are spray deposited and used as light absorbing layers in photovoltaic devices. Black-Right-Pointing-Pointer Photovoltaic devices were constructed from nanowire mats. Black-Right-Pointing-Pointer Photovoltaic device efficiency is limited by electrical transport in the nanocrystal layers.

  13. Linearly arranged polytypic CZTSSe nanocrystals

    PubMed Central

    Fan, Feng-Jia; Wu, Liang; Gong, Ming; Chen, Shi You; Liu, Guang Yao; Yao, Hong-Bin; Liang, Hai-Wei; Wang, Yi-Xiu; Yu, Shu-Hong

    2012-01-01

    Even colloidal polytypic nanostructures show promising future in band-gap tuning and alignment, researches on them have been much less reported than the standard nano-heterostructures because of the difficulties involved in synthesis. Up to now, controlled synthesis of colloidal polytypic nanocrsytals has been only realized in II-VI tetrapod and octopod nanocrystals with branched configurations. Herein, we report a colloidal approach for synthesizing non-branched but linearly arranged polytypic I2-II-IV-VI4 nanocrystals, with a focus on polytypic non-stoichiometric Cu2ZnSnSxSe4−x nanocrystals. Each synthesized polytypic non-stoichiometric Cu2ZnSnSxSe4−x nanocrystal is consisted of two zinc blende-derived ends and one wurtzite-derived center part. The formation mechanism has been studied and the phase composition can be tuned through adjusting the reaction temperature, which brings a new band-gap tuning approach to Cu2ZnSnSxSe4-x nanocrystals. PMID:23233871

  14. The flow reactor system for in-line synthesis of semiconductor nanoparticle

    NASA Astrophysics Data System (ADS)

    Ryzhov, O. A.; Matyushkin, L. B.

    2015-11-01

    A flow reactor nanoparticle synthesis technique is proposed as replacement for «hot injection» synthesis of semiconductor nanocrystals in a glass flask. The main advantages are possibility of continuous nanoparticles production, technology flexibility and lower cost of the final products in comparison with currently applied methods.

  15. Nanocrystal powered nanomotor

    DOEpatents

    Regan, Brian C.; Zettl, Alexander K.; Aloni, Shaul

    2011-01-04

    A nanoscale nanocrystal which may be used as a reciprocating motor is provided, comprising a substrate having an energy differential across it, e.g. an electrical connection to a voltage source at a proximal end; an atom reservoir on the substrate distal to the electrical connection; a nanoparticle ram on the substrate distal to the atom reservoir; a nanolever contacting the nanoparticle ram and having an electrical connection to a voltage source, whereby a voltage applied between the electrical connections on the substrate and the nanolever causes movement of atoms between the reservoir and the ram. Movement of the ram causes movement of the nanolever relative to the substrate. The substrate and nanolever preferably comprise multiwalled carbon nanotubes (MWNTs) and the atom reservoir and nanoparticle ram are preferably metal (e.g. indium) deposited as small particles on the MWNTs. The substrate may comprise a silicon chip that has been fabricated to provide the necessary electrodes and other electromechanical structures, and further supports an atomic track, which may comprise an MWNT.

  16. Nanocrystal assembly for tandem catalysis

    DOEpatents

    Yang, Peidong; Somorjai, Gabor; Yamada, Yusuke; Tsung, Chia-Kuang; Huang, Wenyu

    2014-10-14

    The present invention provides a nanocrystal tandem catalyst comprising at least two metal-metal oxide interfaces for the catalysis of sequential reactions. One embodiment utilizes a nanocrystal bilayer structure formed by assembling sub-10 nm platinum and cerium oxide nanocube monolayers on a silica substrate. The two distinct metal-metal oxide interfaces, CeO.sub.2--Pt and Pt--SiO.sub.2, can be used to catalyze two distinct sequential reactions. The CeO.sub.2--Pt interface catalyzed methanol decomposition to produce CO and H.sub.2, which were then subsequently used for ethylene hydroformylation catalyzed by the nearby Pt--SiO.sub.2 interface. Consequently, propanal was selectively produced on this nanocrystal bilayer tandem catalyst.

  17. Optimizing Photovoltaic Response by Tuning Light-Harvesting Nanocrystal Shape Synthesized Using a Quick Liquid-Gas Phase Reaction.

    PubMed

    Mazumdar, Sayantan; Tamilselvan, Muthusamy; Bhattacharyya, Aninda J

    2015-12-30

    The electron recombination lifetime in a sensitized semiconductor assembly is greatly influenced by the crystal structure and geometric form of the light-harvesting semiconductor nanocrystal. When such light harvesters with varying structural characteristics are configured in a photoanode, its interface with the electrolyte becomes equally important and directly influences the photovoltaic efficiency. We have systematically probed here the influence of nanocrystal crystallographic structure and shape on the electron recombination lifetime and its eventual influence on the light to electricity conversion efficiency of a liquid junction semiconductor sensitized solar cell. The light-harvesting cadmium sulfide (CdS) nanocrystals of distinctly different and controlled shapes are obtained using a novel and simple liquid-gas phase synthesis method performed at different temperatures involving very short reaction times. High-resolution synchrotron X-ray diffraction and spectroscopic studies respectively exhibit different crystallographic phase content and optical properties. When assembled on a mesoscopic TiO2 film by a linker molecule, they exhibit remarkable variation in electron recombination lifetime by 1 order of magnitude, as determined by ac-impedance spectroscopy. This also drastically affects the photovoltaic efficiency of the differently shaped nanocrystal sensitized solar cells.

  18. Doping silicon nanocrystals and quantum dots.

    PubMed

    Oliva-Chatelain, Brittany L; Ticich, Thomas M; Barron, Andrew R

    2016-01-28

    The ability to incorporate a dopant element into silicon nanocrystals (NC) and quantum dots (QD) is one of the key technical challenges for the use of these materials in a number of optoelectronic applications. Unlike doping of traditional bulk semiconductor materials, the location of the doping element can be either within the crystal lattice (c-doping), on the surface (s-doping) or within the surrounding matrix (m-doping). A review of the various synthetic strategies for doping silicon NCs and QDs is presented, concentrating on the efficacy of the synthetic routes, both in situ and post synthesis, with regard to the structural location of the dopant and the doping level. Methods that have been applied to the characterization of doped NCs and QDs are summarized with regard to the information that is obtained, in particular to provide researchers with a guide to the suitable techniques for determining dopant concentration and location, as well as electronic and photonic effectiveness of the dopant.

  19. Doping silicon nanocrystals and quantum dots

    NASA Astrophysics Data System (ADS)

    Oliva-Chatelain, Brittany L.; Ticich, Thomas M.; Barron, Andrew R.

    2016-01-01

    The ability to incorporate a dopant element into silicon nanocrystals (NC) and quantum dots (QD) is one of the key technical challenges for the use of these materials in a number of optoelectronic applications. Unlike doping of traditional bulk semiconductor materials, the location of the doping element can be either within the crystal lattice (c-doping), on the surface (s-doping) or within the surrounding matrix (m-doping). A review of the various synthetic strategies for doping silicon NCs and QDs is presented, concentrating on the efficacy of the synthetic routes, both in situ and post synthesis, with regard to the structural location of the dopant and the doping level. Methods that have been applied to the characterization of doped NCs and QDs are summarized with regard to the information that is obtained, in particular to provide researchers with a guide to the suitable techniques for determining dopant concentration and location, as well as electronic and photonic effectiveness of the dopant.

  20. Injected nanocrystals for targeted drug delivery

    PubMed Central

    Lu, Yi; Li, Ye; Wu, Wei

    2016-01-01

    Nanocrystals are pure drug crystals with sizes in the nanometer range. Due to the advantages of high drug loading, platform stability, and ease of scaling-up, nanocrystals have been widely used to deliver poorly water-soluble drugs. Nanocrystals in the blood stream can be recognized and sequestered as exogenous materials by mononuclear phagocytic system (MPS) cells, leading to passive accumulation in MPS-rich organs, such as liver, spleen and lung. Particle size, morphology and surface modification affect the biodistribution of nanocrystals. Ligand conjugation and stimuli-responsive polymers can also be used to target nanocrystals to specific pathogenic sites. In this review, the progress on injected nanocrystals for targeted drug delivery is discussed following a brief introduction to nanocrystal preparation methods, i.e., top-down and bottom-up technologies. PMID:27006893

  1. Generalized syntheses of nanocrystal-graphene hybrids in high-boiling-point organic solvents

    NASA Astrophysics Data System (ADS)

    Pang, Danny Wei-Ping; Yuan, Fang-Wei; Chang, Yan-Cheng; Li, Guo-An; Tuan, Hsing-Yu

    2012-07-01

    Nanocrystal-graphene have been proposed as a new kind of promising hybrid for a wide range of application areas including catalysts, electronics, sensors, biomedicine, and energy storage, etc. Although a variety of methods have been developed for the preparation of hybrids, a facile and general synthetic approach is still highly required. In this study, nanocrystal-graphene hybrids were successfully synthesized in high-boiling-point organic solvents. Graphene oxide (GO) nanosheets were modified by oleylamine (OLA) to form a OLA-GO complex in order to be readily incorporated into hydrophobic synthesis. A rich library of highly crystalline nanocrystals, with types including noble metal, metal oxide, magnetic material and semiconductor were successfully grown on chemically converted graphene (CCG), which is simultaneously reduced from GO during the synthesis. High boiling-point solvents afford sufficient thermal energy to assure the high-quality crystalline nature of NCs, therefore the post-annealing process is obviated. Controlled experiments revealed that OLA-GO triggers heterogeneous nucleation and serves as excellent nuclei anchorage media. The protocol developed here brings one step closer to achieve ``unity in diversity'' on the preparation of nanocrystal-graphene hybrids.Nanocrystal-graphene have been proposed as a new kind of promising hybrid for a wide range of application areas including catalysts, electronics, sensors, biomedicine, and energy storage, etc. Although a variety of methods have been developed for the preparation of hybrids, a facile and general synthetic approach is still highly required. In this study, nanocrystal-graphene hybrids were successfully synthesized in high-boiling-point organic solvents. Graphene oxide (GO) nanosheets were modified by oleylamine (OLA) to form a OLA-GO complex in order to be readily incorporated into hydrophobic synthesis. A rich library of highly crystalline nanocrystals, with types including noble metal, metal

  2. Mid-IR band gap engineering of CdxPb1-xS nanocrystals by mechanochemical reaction

    NASA Astrophysics Data System (ADS)

    Tan, Guo-Long; Liu, Limin; Wu, Weibing

    2014-06-01

    Composition-tunable ternary CdxPb1-xS nanocrystals (NCs) are very important materials for remote sensing and detecting in the infrared (IR) wavelength region. They are, however, almost exclusively prepared by wet chemical routes which lead to surface-capped nanoparticles. The surface capping molecules could move their absorption peaks from mid-IR to near IR wavelength region. However, surface clean CdxPb1-xS nanocrystals (NCs) would demonstrate intrinsic optical spectrum in the mid-IR region. Herein, we present a physical mechanical alloying (MA) process being applied to prepare tens of grams of surface clean CdxPb1-xS nanocrystals within the composition range of x = 0.0 to 0.4. The average particle size is smaller than 9 nm. The as-milled nanocrystals are chemically homogenous. The CdxPb1-xS nanocrystals show a continuous lattice contraction with Cd content. There is an exponential indirect band gap-composition relationship. This MA method shows the ability to continuously and precisely tune the band gap energies of ternary CdxPb1-xS semiconductor nanocrystals from mid-IR region (2638 nm) to NIR wavelength region (1240 nm) through chemical composition.

  3. Non-native Co-, Mn-, and Ti-oxyhydroxide nanocrystals in ferritin for high efficiency solar energy conversion.

    PubMed

    Erickson, S D; Smith, T J; Moses, L M; Watt, R K; Colton, J S

    2015-01-01

    Quantum dot solar cells seek to surpass the solar energy conversion efficiencies achieved by bulk semiconductors. This new field requires a broad selection of materials to achieve its full potential. The 12 nm spherical protein ferritin can be used as a template for uniform and controlled nanocrystal growth, and to then house the nanocrystals for use in solar energy conversion. In this study, precise band gaps of titanium, cobalt, and manganese oxyhydroxide nanocrystals within ferritin were measured, and a change in band gap due to quantum confinement effects was observed. The range of band gaps obtainable from these three types of nanocrystals is 2.19-2.29 eV, 1.93-2.15 eV, and 1.60-1.65 eV respectively. From these measured band gaps, theoretical efficiency limits for a multi-junction solar cell using these ferritin-enclosed nanocrystals are calculated and found to be 38.0% for unconcentrated sunlight and 44.9% for maximally concentrated sunlight. If a ferritin-based nanocrystal with a band gap similar to silicon can be found (i.e. 1.12 eV), the theoretical efficiency limits are raised to 51.3% and 63.1%, respectively. For a current matched cell, these latter efficiencies become 41.6% (with an operating voltage of 5.49 V), and 50.0% (with an operating voltage of 6.59 V), for unconcentrated and maximally concentrated sunlight respectively.

  4. Solvent-like ligand-coated ultrasmall cadmium selenide nanocrystals: strong electronic coupling in a self-organized assembly.

    PubMed

    Lawrence, Katie N; Johnson, Merrell A; Dolai, Sukanta; Kumbhar, Amar; Sardar, Rajesh

    2015-07-21

    Strong inter-nanocrystal electronic coupling is a prerequisite for delocalization of exciton wave functions and high conductivity. We report 170 meV electronic coupling energy of short chain poly(ethylene glycol) thiolate-coated ultrasmall (<2.5 nm in diameter) CdSe semiconductor nanocrystals (SNCs) in solution. Cryo-transmission electron microscopy analysis showed the formation of a pearl-necklace assembly of nanocrystals in solution with regular inter-nanocrystal spacing. The electronic coupling was studied as a function of CdSe nanocrystal size where the smallest nanocrystals exhibited the largest coupling energy. The electronic coupling in spin-cast thin-film (<200 nm in thickness) of poly(ethylene glycol) thiolate-coated CdSe SNCs was studied as a function of annealing temperature, where an unprecedentedly large, ∼400 meV coupling energy was observed for 1.6 nm diameter SNCs, which were coated with a thin layer of poly(ethylene glycol) thiolates. Small-angle X-ray scattering measurements showed that CdSe SNCs maintained an order array inside the films. The strong electronic coupling of SNCs in a self-organized film could facilitate the large-scale production of highly efficient electronic materials for advanced optoelectronic device application. PMID:26098759

  5. Spatial Separation of Charge Carriers in In2O3-x(OH)y Nanocrystal Superstructures for Enhanced Gas-Phase Photocatalytic Activity.

    PubMed

    He, Le; Wood, Thomas E; Wu, Bo; Dong, Yuchan; Hoch, Laura B; Reyes, Laura M; Wang, Di; Kübel, Christian; Qian, Chenxi; Jia, Jia; Liao, Kristine; O'Brien, Paul G; Sandhel, Amit; Loh, Joel Y Y; Szymanski, Paul; Kherani, Nazir P; Sum, Tze Chien; Mims, Charles A; Ozin, Geoffrey A

    2016-05-24

    The development of strategies for increasing the lifetime of photoexcited charge carriers in nanostructured metal oxide semiconductors is important for enhancing their photocatalytic activity. Intensive efforts have been made in tailoring the properties of the nanostructured photocatalysts through different ways, mainly including band-structure engineering, doping, catalyst-support interaction, and loading cocatalysts. In liquid-phase photocatalytic dye degradation and water splitting, it was recently found that nanocrystal superstructure based semiconductors exhibited improved spatial separation of photoexcited charge carriers and enhanced photocatalytic performance. Nevertheless, it remains unknown whether this strategy is applicable in gas-phase photocatalysis. Using porous indium oxide nanorods in catalyzing the reverse water-gas shift reaction as a model system, we demonstrate here that assembling semiconductor nanocrystals into superstructures can also promote gas-phase photocatalytic processes. Transient absorption studies prove that the improved activity is a result of prolonged photoexcited charge carrier lifetimes due to the charge transfer within the nanocrystal network comprising the nanorods. Our study reveals that the spatial charge separation within the nanocrystal networks could also benefit gas-phase photocatalysis and sheds light on the design principles of efficient nanocrystal superstructure based photocatalysts. PMID:27159793

  6. "Nanocrystal bilayer for tandem catalysis"

    SciTech Connect

    Yamada, Yusuke; Tsung, Chia Kuang; Huang, Wenyu; Huo, Ziyang; E.Habas, Susan E; Soejima, Tetsuro; Aliaga, Cesar E; Samorjai, Gabor A; Yang, Peidong

    2011-01-24

    Supported catalysts are widely used in industry and can be optimized by tuning the composition and interface of the metal nanoparticles and oxide supports. Rational design of metal-metal oxide interfaces in nanostructured catalysts is critical to achieve better reaction activities and selectivities. We introduce here a new class of nanocrystal tandem catalysts that have multiple metal-metal oxide interfaces for the catalysis of sequential reactions. We utilized a nanocrystal bilayer structure formed by assembling platinum and cerium oxide nanocube monolayers of less than 10 nm on a silica substrate. The two distinct metal-metal oxide interfaces, CeO2-Pt and Pt-SiO2, can be used to catalyse two distinct sequential reactions. The CeO2-Pt interface catalysed methanol decomposition to produce CO and H2, which were subsequently used for ethylene hydroformylation catalysed by the nearby Pt-SiO2 interface. Consequently, propanal was produced selectively from methanol and ethylene on the nanocrystal bilayer tandem catalyst. This new concept of nanocrystal tandem catalysis represents a powerful approach towards designing high-performance, multifunctional nanostructured catalysts

  7. Tailoring lanthanide nanocrystals for nanomedicine

    NASA Astrophysics Data System (ADS)

    Zhang, Yan; Tan, Timothy T. Y.

    2013-02-01

    Lanthanide nanocrystals have demonstrated strong potentials in nanomedicine due to its up-conversion and strong magnetic properties, and low toxicity. This talk will focus on strategies in lanthanide nanostructure tailoring to achieve up-conversion color emission tuning, MRI T1 and T2 contrast tuning, and the use of up-conversion fluorescence in drug delivery and cancer cells ablation.

  8. Nanocrystals Research for Energy Efficient and Clean Energy Technologies:

    SciTech Connect

    Rosenthal, Sandra J

    2013-12-17

    Efforts centered on: nanocrystal photovoltaic fabrication, ultrafast dynamics and aberration-corrected STEM characterization of II-VI core, core/shell and alloyed nanocrystals, and fundamental investigation and applications of ultrasmall white light-emitting CdSe nanocrystal.

  9. A new family of wurtzite-phase Cu2ZnAS4-x and CuZn2AS4 (A = Al, Ga, In) nanocrystals for solar energy conversion applications.

    PubMed

    Ghosh, Anima; Palchoudhury, Soubantika; Thangavel, Rajalingam; Zhou, Ziyou; Naghibolashrafi, Nariman; Ramasamy, Karthik; Gupta, Arunava

    2016-01-01

    A new family of quaternary semiconductors Cu2ZnAS4-x and CuZn2AS4 (A = Al, Ga, In) has been synthesized in the form of wurtzite phase nanocrystals for the first time. The nanocrystals can be converted to the stannite phase via thermal annealing under a N2 atmosphere. A direct band gap in the visible wavelength region combined with a high absorption cross-section makes these materials promising for solar energy conversion applications. PMID:26466863

  10. Metal-free inorganic ligands for colloidal nanocrystals: S2-, HS-, Se2-, HSe-, Te2-, HTe-, TeS3(2-), OH-, and NH2- as surface ligands.

    PubMed

    Nag, Angshuman; Kovalenko, Maksym V; Lee, Jong-Soo; Liu, Wenyong; Spokoyny, Boris; Talapin, Dmitri V

    2011-07-13

    All-inorganic colloidal nanocrystals were synthesized by replacing organic capping ligands on chemically synthesized nanocrystals with metal-free inorganic ions such as S(2-), HS(-), Se(2-), HSe(-), Te(2-), HTe(-), TeS(3)(2-), OH(-) and NH(2)(-). These simple ligands adhered to the NC surface and provided colloidal stability in polar solvents. The versatility of such ligand exchange has been demonstrated for various semiconductor and metal nanocrystals of different size and shape. We showed that the key aspects of Pearson's hard and soft acids and bases (HSAB) principle, originally developed for metal coordination compounds, can be applied to the bonding of molecular species to the nanocrystal surface. The use of small inorganic ligands instead of traditional ligands with long hydrocarbon tails facilitated the charge transport between individual nanocrystals and opened up interesting opportunities for device integration of colloidal nanostructures.

  11. Penternary chalcogenides nanocrystals as catalytic materials for efficient counter electrodes in dye-synthesized solar cells

    NASA Astrophysics Data System (ADS)

    Özel, Faruk; Sarılmaz, Adem; Istanbullu, Bilal; Aljabour, Abdalaziz; Kuş, Mahmut; Sönmezoğlu, Savaş

    2016-07-01

    The penternary chalcogenides Cu2CoSn(SeS)4 and Cu2ZnSn(SeS)4 were successfully synthesized by hot-injection method, and employed as a catalytic materials for efficient counter electrodes in dye-synthesized solar cells (DSSCs). The structural, compositional, morphological and optical properties of these pentenary semiconductors were characterized by X-ray diffraction (XRD), Raman spectroscopy, transmission electron microscopy (TEM), energy-dispersive spectrometer (EDS) and ultraviolet-visible (UV–Vis) spectroscopy. The Cu2CoSn(SeS)4 and Cu2ZnSn(SeS)4 nanocrystals had a single crystalline, kesterite phase, adequate stoichiometric ratio, 18–25 nm particle sizes which are forming nanospheres, and band gap energy of 1.18 and 1.45 eV, respectively. Furthermore, the electrochemical impedance spectroscopy and cyclic voltammograms indicated that Cu2CoSn(SeS)4 nanocrystals as counter electrodes exhibited better electrocatalytic activity for the reduction of iodine/iodide electrolyte than that of Cu2ZnSn(SeS)4 nanocrystals and conventional platinum (Pt). The photovoltaic results demonstrated that DSSC with a Cu2CoSn(SeS)4 nanocrystals-based counter electrode achieved the best efficiency of 6.47%, which is higher than the same photoanode employing a Cu2ZnSn(SeS)4 nanocrystals (3.18%) and Pt (5.41%) counter electrodes. These promising results highlight the potential application of penternary chalcogen Cu2CoSn(SeS)4 nanocrystals in low-cost, high-efficiency, Pt-free DSSCs.

  12. Penternary chalcogenides nanocrystals as catalytic materials for efficient counter electrodes in dye-synthesized solar cells.

    PubMed

    Özel, Faruk; Sarılmaz, Adem; İstanbullu, Bilal; Aljabour, Abdalaziz; Kuş, Mahmut; Sönmezoğlu, Savaş

    2016-01-01

    The penternary chalcogenides Cu2CoSn(SeS)4 and Cu2ZnSn(SeS)4 were successfully synthesized by hot-injection method, and employed as a catalytic materials for efficient counter electrodes in dye-synthesized solar cells (DSSCs). The structural, compositional, morphological and optical properties of these pentenary semiconductors were characterized by X-ray diffraction (XRD), Raman spectroscopy, transmission electron microscopy (TEM), energy-dispersive spectrometer (EDS) and ultraviolet-visible (UV-Vis) spectroscopy. The Cu2CoSn(SeS)4 and Cu2ZnSn(SeS)4 nanocrystals had a single crystalline, kesterite phase, adequate stoichiometric ratio, 18-25 nm particle sizes which are forming nanospheres, and band gap energy of 1.18 and 1.45 eV, respectively. Furthermore, the electrochemical impedance spectroscopy and cyclic voltammograms indicated that Cu2CoSn(SeS)4 nanocrystals as counter electrodes exhibited better electrocatalytic activity for the reduction of iodine/iodide electrolyte than that of Cu2ZnSn(SeS)4 nanocrystals and conventional platinum (Pt). The photovoltaic results demonstrated that DSSC with a Cu2CoSn(SeS)4 nanocrystals-based counter electrode achieved the best efficiency of 6.47%, which is higher than the same photoanode employing a Cu2ZnSn(SeS)4 nanocrystals (3.18%) and Pt (5.41%) counter electrodes. These promising results highlight the potential application of penternary chalcogen Cu2CoSn(SeS)4 nanocrystals in low-cost, high-efficiency, Pt-free DSSCs. PMID:27380957

  13. Penternary chalcogenides nanocrystals as catalytic materials for efficient counter electrodes in dye-synthesized solar cells

    PubMed Central

    Özel, Faruk; Sarılmaz, Adem; İstanbullu, Bilal; Aljabour, Abdalaziz; Kuş, Mahmut; Sönmezoğlu, Savaş

    2016-01-01

    The penternary chalcogenides Cu2CoSn(SeS)4 and Cu2ZnSn(SeS)4 were successfully synthesized by hot-injection method, and employed as a catalytic materials for efficient counter electrodes in dye-synthesized solar cells (DSSCs). The structural, compositional, morphological and optical properties of these pentenary semiconductors were characterized by X-ray diffraction (XRD), Raman spectroscopy, transmission electron microscopy (TEM), energy-dispersive spectrometer (EDS) and ultraviolet-visible (UV–Vis) spectroscopy. The Cu2CoSn(SeS)4 and Cu2ZnSn(SeS)4 nanocrystals had a single crystalline, kesterite phase, adequate stoichiometric ratio, 18–25 nm particle sizes which are forming nanospheres, and band gap energy of 1.18 and 1.45 eV, respectively. Furthermore, the electrochemical impedance spectroscopy and cyclic voltammograms indicated that Cu2CoSn(SeS)4 nanocrystals as counter electrodes exhibited better electrocatalytic activity for the reduction of iodine/iodide electrolyte than that of Cu2ZnSn(SeS)4 nanocrystals and conventional platinum (Pt). The photovoltaic results demonstrated that DSSC with a Cu2CoSn(SeS)4 nanocrystals-based counter electrode achieved the best efficiency of 6.47%, which is higher than the same photoanode employing a Cu2ZnSn(SeS)4 nanocrystals (3.18%) and Pt (5.41%) counter electrodes. These promising results highlight the potential application of penternary chalcogen Cu2CoSn(SeS)4 nanocrystals in low-cost, high-efficiency, Pt-free DSSCs. PMID:27380957

  14. Cellulose nanocrystals: synthesis, functional properties, and applications.

    PubMed

    George, Johnsy; Sabapathi, S N

    2015-01-01

    Cellulose nanocrystals are unique nanomaterials derived from the most abundant and almost inexhaustible natural polymer, cellulose. These nanomaterials have received significant interest due to their mechanical, optical, chemical, and rheological properties. Cellulose nanocrystals primarily obtained from naturally occurring cellulose fibers are biodegradable and renewable in nature and hence they serve as a sustainable and environmentally friendly material for most applications. These nanocrystals are basically hydrophilic in nature; however, they can be surface functionalized to meet various challenging requirements, such as the development of high-performance nanocomposites, using hydrophobic polymer matrices. Considering the ever-increasing interdisciplinary research being carried out on cellulose nanocrystals, this review aims to collate the knowledge available about the sources, chemical structure, and physical and chemical isolation procedures, as well as describes the mechanical, optical, and rheological properties, of cellulose nanocrystals. Innovative applications in diverse fields such as biomedical engineering, material sciences, electronics, catalysis, etc, wherein these cellulose nanocrystals can be used, are highlighted. PMID:26604715

  15. Cellulose nanocrystals: synthesis, functional properties, and applications

    PubMed Central

    George, Johnsy; Sabapathi, SN

    2015-01-01

    Cellulose nanocrystals are unique nanomaterials derived from the most abundant and almost inexhaustible natural polymer, cellulose. These nanomaterials have received significant interest due to their mechanical, optical, chemical, and rheological properties. Cellulose nanocrystals primarily obtained from naturally occurring cellulose fibers are biodegradable and renewable in nature and hence they serve as a sustainable and environmentally friendly material for most applications. These nanocrystals are basically hydrophilic in nature; however, they can be surface functionalized to meet various challenging requirements, such as the development of high-performance nanocomposites, using hydrophobic polymer matrices. Considering the ever-increasing interdisciplinary research being carried out on cellulose nanocrystals, this review aims to collate the knowledge available about the sources, chemical structure, and physical and chemical isolation procedures, as well as describes the mechanical, optical, and rheological properties, of cellulose nanocrystals. Innovative applications in diverse fields such as biomedical engineering, material sciences, electronics, catalysis, etc, wherein these cellulose nanocrystals can be used, are highlighted. PMID:26604715

  16. (Plasmonic Metal Core)/(Semiconductor Shell) Nanostructures

    NASA Astrophysics Data System (ADS)

    Fang, Caihong

    Over the past several years, integration of metal nanocrystals that can support localized surface plasmon has been demonstrated as one of the most promising methods to the improvement of the light-harvesting efficiency of semiconductors. Ag and Au nanocrystals have been extensively hybridized with semiconductors by either deposition or anchoring. However, metal nanocrystals tend to aggregate, reshape, detach, or grow into large nanocrystals, leading to a loss of the unique properties seen in the original nanocrystals. Fortunately, core/shell nanostructures, circumventing the aforementioned problems, have been demonstrated to exhibit superior photoactivities. To further improve the light-harvesting applications of (plasmonic metal core)/(semiconductor shell) nanostructures, it is vital to understand the plasmonic and structural evolutions during the preparation processes, design novel hybrid nanostructures, and improve their light-harvesting performances. In this thesis, I therefore studied the plasmonic and structural evolutions during the formation of (Ag core)/(Ag2S shell) nanostructures. Moreover, I also prepared (noble metal core)/(TiO2 shell) nanostructures and investigated their plasmonic properties and photon-harvesting applications. Clear understanding of the sulfidation process can enable fine control of the plasmonic properties as well as the structural composition of Ag/Ag 2S nanomaterials. Therefore, I investigated the plasmonic and structural variations during the sulfidation process of Ag nanocubes both experimentally and numerically. The sulfidation reactions were carried out at both the ensemble and single-particle levels. Electrodynamic simulations were also employed to study the variations of the plasmonic properties and plasmon modes. Both experiment and simulation results revealed that sulfidation initiates at the vertices of Ag nanocubes. Ag nanocubes are then gradually truncated and each nanocube becomes a nanosphere eventually. The cubic

  17. Spectroscopic and Computational Studies of Light and Heat Generation in Semiconductor Nanomaterials

    NASA Astrophysics Data System (ADS)

    Hannah, Daniel C.

    In crystalline semiconductors, the reduction of material dimensions to the nanometer length scale often has a profound impact on the optical, structural, and thermal properties exhibited by the material. While the optical properties of semiconductor nanocrystals have been studied for over two decades, many fundamental questions persist regarding thermal processes in this material class. For example, on what time scale do excited charge carriers dissipate energy and into which degrees of freedom? How is heat generated during carrier thermalization transported out of the nanocrystal? Can these processes be manipulated by structural modification? In the first part of this thesis, we utilize a combination of ultrafast spectroscopic methods and computational modeling to answer these questions. Overall, our results indicate that heat generation begins with hole thermalization, and that the subsequent transport of heat is heavily influenced by the semiconductor surface structure and surface chemistry. These findings lead us to propose and demonstrate several methods of independently tuning nanocrystal optical and thermal properties. In the second part of this thesis, we investigate a long standing issue in nanoscience: the efficient emission of light by group-IV nanocrystals. Again, utilizing a combination of optical spectroscopy and theoretical modeling, we are able to attribute long-lived, band-edge photoluminescence from Si nanocrystals to emission from the crystalline core, which remains indirect-gap in character despite substantial quantum confinement. We also attribute rapid, high-energy photoluminescence to a persistent amorphous surface layer. Finally, we explore some of the interesting structural behavior exhibited by group-IV nanocrystals at high pressure.

  18. Synthesis and size-dependent properties of zinc-blende semiconductor quantum rods.

    PubMed

    Kan, Shihai; Mokari, Taleb; Rothenberg, Eli; Banin, Uri

    2003-03-01

    Dimensionality and size are two factors that govern the properties of semiconductor nanostructures. In nanocrystals, dimensionality is manifested by the control of shape, which presents a key challenge for synthesis. So far, the growth of rod-shaped nanocrystals using a surfactant-controlled growth mode, has been limited to semiconductors with wurtzite crystal structures, such as CdSe (ref. 3). Here, we report on a general method for the growth of soluble nanorods applied to semiconductors with the zinc-blende cubic lattice structure. InAs quantum rods with controlled lengths and diameters were synthesized using the solution-liquid-solid mechanism with gold nanocrystals as catalysts. This provides an unexpected link between two successful strategies for growing high-quality nanomaterials, the vapour-liquid-solid approach for growing nanowires, and the colloidal approach for synthesizing soluble nanocrystals. The rods exhibit both length- and shape-dependent optical properties, manifested in a red-shift of the bandgap with increased length, and in the observation of polarized emission covering the near-infrared spectral range relevant for telecommunications devices. PMID:12612671

  19. Synthesis and size-dependent properties of zinc-blende semiconductor quantum rods

    NASA Astrophysics Data System (ADS)

    Kan, Shihai; Mokari, Taleb; Rothenberg, Eli; Banin, Uri

    2003-03-01

    Dimensionality and size are two factors that govern the properties of semiconductor nanostructures. In nanocrystals, dimensionality is manifested by the control of shape, which presents a key challenge for synthesis. So far, the growth of rod-shaped nanocrystals using a surfactant-controlled growth mode, has been limited to semiconductors with wurtzite crystal structures, such as CdSe (ref. 3). Here, we report on a general method for the growth of soluble nanorods applied to semiconductors with the zinc-blende cubic lattice structure. InAs quantum rods with controlled lengths and diameters were synthesized using the solution-liquid-solid mechanism with gold nanocrystals as catalysts. This provides an unexpected link between two successful strategies for growing high-quality nanomaterials, the vapour-liquid-solid approach for growing nanowires, and the colloidal approach for synthesizing soluble nanocrystals. The rods exhibit both length- and shape-dependent optical properties, manifested in a red-shift of the bandgap with increased length, and in the observation of polarized emission covering the near-infrared spectral range relevant for telecommunications devices.

  20. Internal structure of InP/ZnS nanocrystals unraveled by high-resolution soft X-ray photoelectron spectroscopy.

    PubMed

    Huang, Kai; Demadrille, Renaud; Silly, Mathieu G; Sirotti, Fausto; Reiss, Peter; Renault, Olivier

    2010-08-24

    High-energy resolution photoelectron spectroscopy (DeltaE < 200 meV) is used to investigate the internal structure of semiconductor quantum dots containing low Z-contrast elements. In InP/ZnS core/shell nanocrystals synthesized using a single-step procedure (core and shell precursors added at the same time), a homogeneously alloyed InPZnS core structure is evidenced by quantitative analysis of their In3d(5/2) spectra recorded at variable excitation energy. When using a two-step method (core InP nanocrystal synthesis followed by subsequent ZnS shell growth), XPS analysis reveals a graded core/shell interface. We demonstrate the existence of In-S and S(x)-In-P(1-x) bonding states in both types of InP/ZnS nanocrystals, which allows a refined view on the underlying reaction mechanisms. PMID:20666468

  1. Modeling and simulation of floating gate nanocrystal FET devices and circuits

    NASA Astrophysics Data System (ADS)

    Hasaneen, El-Sayed A. M.

    The nonvolatile memory market has been growing very fast during the last decade, especially for mobile communication systems. The Semiconductor Industry Association International Technology Roadmap for Semiconductors states that the difficult challenge for nonvolatile semiconductor memories is to achieve reliable, low power, low voltage performance and high-speed write/erase. This can be achieved by aggressive scaling of the nonvolatile memory cells. Unfortunately, scaling down of conventional nonvolatile memory will further degrade the retention time due to the charge loss between the floating gate and drain/source contacts and substrate which makes conventional nonvolatile memory unattractive. Using nanocrystals as charge storage sites reduces dramatically the charge leakage through oxide defects and drain/source contacts. Floating gate nanocrystal nonvolatile memory, FG-NCNVM, is a candidate for future memory because it is advantageous in terms of high-speed write/erase, small size, good scalability, low-voltage, low-power applications, and the capability to store multiple bits per cell. Many studies regarding FG-NCNVMs have been published. Most of them have dealt with fabrication improvements of the devices and device characterizations. Due to the promising FG-NCNVM applications in integrated circuits, there is a need for circuit a simulation model to simulate the electrical characteristics of the floating gate devices. In this thesis, a FG-NCNVM circuit simulation model has been proposed. It is based on the SPICE BSIM simulation model. This model simulates the cell behavior during normal operation. Model validation results have been presented. The SPICE model shows good agreement with experimental results. Current-voltage characteristics, transconductance and unity gain frequency (fT) have been studied showing the effect of the threshold voltage shift (DeltaVth) due to nanocrystal charge on the device characteristics. The threshold voltage shift due to

  2. Electronic Structure of Germanium Nanocrystal Films Probed with Synchrotron Radiation

    SciTech Connect

    Bostedt, C

    2002-05-01

    The fundamental structure--property relationship of semiconductor quantum dots has been investigated. For deposited germanium nanocrystals strong quantum confinement effects have been determined with synchrotron radiation based x-ray absorption and photoemission techniques. The nanocrystals are condensed out of the gas phase with a narrow size distribution and subsequently deposited in situ onto various substrates. The particles are crystalline in the cubic phase with a structurally disordered surface shell and the resulting film morphology depends strongly on the substrate material and condition. The disordered surface region has an impact on the overall electronic structure of the particles. In a size-dependent study, the conduction and valence band edge of germanium nanocrystals have been measured for the first time and compared to the bulk crystal. The band edges move to higher energies as the particle size is decreased, consistent with quantum confinement theory. To obtain a more accurate analysis of confinement effects in the empty states, a novel analysis method utilizing an effective particle size for the x-ray absorption experiment, which allows a deconvolution of absorption edge broadening effects, has been introduced. Comparison of the present study to earlier studies on silicon reveals that germanium exhibits stronger quantum confinement effects than silicon. Below a critical particle size of 2.3 {+-} 0.7 nm, the band gap of germanium becomes larger than that of silicon--even if it is the opposite for bulk materials. This result agrees phenomenologically with effective mass and tight binding theories but contradicts the findings of recent pseudopotential calculations. The discrepancy between theory and experiments is attributed to the differences in the theoretical models and experimental systems. The experimentally observed structural disorder of the particle surface has to be included in the theoretical models.

  3. New materials for tunable plasmonic colloidal nanocrystals.

    PubMed

    Comin, Alberto; Manna, Liberato

    2014-06-01

    We present a review on the emerging materials for novel plasmonic colloidal nanocrystals. We start by explaining the basic processes involved in surface plasmon resonances in nanoparticles and then discuss the classes of nanocrystals that to date are particularly promising for tunable plasmonics: non-stoichiometric copper chalcogenides, extrinsically doped metal oxides, oxygen-deficient metal oxides and conductive metal oxides. We additionally introduce other emerging types of plasmonic nanocrystals and finally we give an outlook on nanocrystals of materials that could potentially display interesting plasmonic properties.

  4. Anisotropic Gold Nanocrystals:. Synthesis and Characterization

    NASA Astrophysics Data System (ADS)

    Stiufiuc, R.; Toderas, F.; Iosin, M.; Stiufiuc, G.

    In this letter we report on successful preparation and characterization of anisotropic gold nanocrystals bio-synthesized by reduction of aqueous chloroaurate ions in pelargonium plant extract. The nanocrystals have been characterized by means of Transmission Electron Microscopy (TEM), UV-VIS absorption spectroscopy and tapping mode atomic force microscopy (TM-AFM). Using these investigation techniques, the successful formation of anisotropic single nanocrystals with the preferential growth direction along the gold (111) plane has been confirmed. The high detail phase images could give us an explanation concerning the growth mechanism of the nanocrystals.

  5. Size distributions of chemically synthesized Ag nanocrystals

    NASA Astrophysics Data System (ADS)

    Thøgersen, Annett; Bonsak, Jack; Fosli, Carl Huseby; Muntingh, Georg

    2011-08-01

    Silver nanocrystals made by a chemical reduction of silver salts (AgNO3) by sodium borohydride (NaBH4) were studied using transmission electron microscopy and light scattering simulations. For various AgNO3/NaBH4 molar ratios, the size distributions of the nanocrystals were found to be approximately log-normal. In addition, a linear relation was found between the mean nanocrystal size and the molar ratio. In order to relate the size distribution of Ag nanocrystals of the various molar ratios to the scattering properties of Ag nanocrystals in solar cell devices, light scattering simulations of Ag nanocrystals in Si, SiO2, SiN, and Al2O3 matrices were carried out using MiePlot. These light scattering spectra for the individual nanocrystal sizes were combined into light scattering spectra for the fitted size distributions. The evolution of these scattering spectra with respect to an increasing mean nanocrystal size was then studied. From these findings, it is possible to find the molar ratio for which the corresponding nanocrystal size distribution has maximum scattering at a particular wavelength in the desired matrix.

  6. High-performance thermoelectric nanocomposites from nanocrystal building blocks

    NASA Astrophysics Data System (ADS)

    Ibáñez, Maria; Luo, Zhishan; Genç, Aziz; Piveteau, Laura; Ortega, Silvia; Cadavid, Doris; Dobrozhan, Oleksandr; Liu, Yu; Nachtegaal, Maarten; Zebarjadi, Mona; Arbiol, Jordi; Kovalenko, Maksym V.; Cabot, Andreu

    2016-03-01

    The efficient conversion between thermal and electrical energy by means of durable, silent and scalable solid-state thermoelectric devices has been a long standing goal. While nanocrystalline materials have already led to substantially higher thermoelectric efficiencies, further improvements are expected to arise from precise chemical engineering of nanoscale building blocks and interfaces. Here we present a simple and versatile bottom-up strategy based on the assembly of colloidal nanocrystals to produce consolidated yet nanostructured thermoelectric materials. In the case study on the PbS-Ag system, Ag nanodomains not only contribute to block phonon propagation, but also provide electrons to the PbS host semiconductor and reduce the PbS intergrain energy barriers for charge transport. Thus, PbS-Ag nanocomposites exhibit reduced thermal conductivities and higher charge carrier concentrations and mobilities than PbS nanomaterial. Such improvements of the material transport properties provide thermoelectric figures of merit up to 1.7 at 850 K.

  7. High-performance thermoelectric nanocomposites from nanocrystal building blocks.

    PubMed

    Ibáñez, Maria; Luo, Zhishan; Genç, Aziz; Piveteau, Laura; Ortega, Silvia; Cadavid, Doris; Dobrozhan, Oleksandr; Liu, Yu; Nachtegaal, Maarten; Zebarjadi, Mona; Arbiol, Jordi; Kovalenko, Maksym V; Cabot, Andreu

    2016-03-07

    The efficient conversion between thermal and electrical energy by means of durable, silent and scalable solid-state thermoelectric devices has been a long standing goal. While nanocrystalline materials have already led to substantially higher thermoelectric efficiencies, further improvements are expected to arise from precise chemical engineering of nanoscale building blocks and interfaces. Here we present a simple and versatile bottom-up strategy based on the assembly of colloidal nanocrystals to produce consolidated yet nanostructured thermoelectric materials. In the case study on the PbS-Ag system, Ag nanodomains not only contribute to block phonon propagation, but also provide electrons to the PbS host semiconductor and reduce the PbS intergrain energy barriers for charge transport. Thus, PbS-Ag nanocomposites exhibit reduced thermal conductivities and higher charge carrier concentrations and mobilities than PbS nanomaterial. Such improvements of the material transport properties provide thermoelectric figures of merit up to 1.7 at 850 K.

  8. Dual-color electroluminescence from dot-in-bulk nanocrystals.

    PubMed

    Brovelli, Sergio; Bae, Wan Ki; Galland, Christophe; Giovanella, Umberto; Meinardi, Francesco; Klimov, Victor I

    2014-02-12

    The emission color from colloidal semiconductor nanocrystals (NCs) is usually tuned through control of particle size, while multicolor emission is obtained by mixing NCs of different sizes within an emissive layer. Here, we demonstrate that recently introduced "dot-in-bulk" (DiB) nanocrystals can emit two-color light under both optical excitation and electrical injection. We show that the effective emission color can be controlled by adjusting the relative amplitudes of the core and shell emission bands via the intensity of optical excitation or applied bias in the cases of photoluminescence (PL) and electroluminescence (EL), respectively. To investigate the role of nonradiative carrier losses due to trapping at intragap states, we incorporate DiB NCs into functional light-emitting diodes and study their PL as a function of applied bias below the EL excitation threshold. We show that voltage-dependent changes in core and shell emissions are not due to the applied electric field but rather arise from the transfer of charges between the anode and the NC intragap trap sites. The changes in the occupancy of trap states can be described in terms of the raising (lowering) of the Fermi level for reverse (direct) bias. We find that the applied voltage affects the overall PL intensity primarily via the electron-trapping channel while bias-induced changes in hole-trapping play a less significant role, limited to a weak effect on core emission. PMID:24328946

  9. Plasmon dynamics in colloidal Cu₂-xSe nanocrystals.

    PubMed

    Scotognella, Francesco; Della Valle, Giuseppe; Srimath Kandada, Ajay Ram; Dorfs, Dirk; Zavelani-Rossi, Margherita; Conforti, Matteo; Miszta, Karol; Comin, Alberto; Korobchevskaya, Kseniya; Lanzani, Guglielmo; Manna, Liberato; Tassone, Francesco

    2011-11-01

    The optical response of metallic nanostructures after intense excitation with femtosecond-laser pulses has recently attracted increasing attention: such response is dominated by ultrafast electron-phonon coupling and offers the possibility to achieve optical modulation with unprecedented terahertz bandwidth. In addition to noble metal nanoparticles, efforts have been made in recent years to synthesize heavily doped semiconductor nanocrystals so as to achieve a plasmonic behavior with spectrally tunable features. In this work, we studied the dynamics of the localized plasmon resonance exhibited by colloidal Cu(2-x)Se nanocrystals of 13 nm in diameter and with x around 0.15, upon excitation by ultrafast laser pulses via pump-probe experiments in the near-infrared, with ∼200 fs resolution time. The experimental results were interpreted according to the two-temperature model and revealed the existence of strong nonlinearities in the plasmonic absorption due to the much lower carrier density of Cu(2-x)Se compared to noble metals, which led to ultrafast control of the probe signal with modulation depth exceeding 40% in transmission. PMID:21939261

  10. Plasmon dynamics in colloidal Cu₂-xSe nanocrystals.

    PubMed

    Scotognella, Francesco; Della Valle, Giuseppe; Srimath Kandada, Ajay Ram; Dorfs, Dirk; Zavelani-Rossi, Margherita; Conforti, Matteo; Miszta, Karol; Comin, Alberto; Korobchevskaya, Kseniya; Lanzani, Guglielmo; Manna, Liberato; Tassone, Francesco

    2011-11-01

    The optical response of metallic nanostructures after intense excitation with femtosecond-laser pulses has recently attracted increasing attention: such response is dominated by ultrafast electron-phonon coupling and offers the possibility to achieve optical modulation with unprecedented terahertz bandwidth. In addition to noble metal nanoparticles, efforts have been made in recent years to synthesize heavily doped semiconductor nanocrystals so as to achieve a plasmonic behavior with spectrally tunable features. In this work, we studied the dynamics of the localized plasmon resonance exhibited by colloidal Cu(2-x)Se nanocrystals of 13 nm in diameter and with x around 0.15, upon excitation by ultrafast laser pulses via pump-probe experiments in the near-infrared, with ∼200 fs resolution time. The experimental results were interpreted according to the two-temperature model and revealed the existence of strong nonlinearities in the plasmonic absorption due to the much lower carrier density of Cu(2-x)Se compared to noble metals, which led to ultrafast control of the probe signal with modulation depth exceeding 40% in transmission.

  11. Dual-color electroluminescence from dot-in-bulk nanocrystals.

    PubMed

    Brovelli, Sergio; Bae, Wan Ki; Galland, Christophe; Giovanella, Umberto; Meinardi, Francesco; Klimov, Victor I

    2014-02-12

    The emission color from colloidal semiconductor nanocrystals (NCs) is usually tuned through control of particle size, while multicolor emission is obtained by mixing NCs of different sizes within an emissive layer. Here, we demonstrate that recently introduced "dot-in-bulk" (DiB) nanocrystals can emit two-color light under both optical excitation and electrical injection. We show that the effective emission color can be controlled by adjusting the relative amplitudes of the core and shell emission bands via the intensity of optical excitation or applied bias in the cases of photoluminescence (PL) and electroluminescence (EL), respectively. To investigate the role of nonradiative carrier losses due to trapping at intragap states, we incorporate DiB NCs into functional light-emitting diodes and study their PL as a function of applied bias below the EL excitation threshold. We show that voltage-dependent changes in core and shell emissions are not due to the applied electric field but rather arise from the transfer of charges between the anode and the NC intragap trap sites. The changes in the occupancy of trap states can be described in terms of the raising (lowering) of the Fermi level for reverse (direct) bias. We find that the applied voltage affects the overall PL intensity primarily via the electron-trapping channel while bias-induced changes in hole-trapping play a less significant role, limited to a weak effect on core emission.

  12. Atomistic understanding of cation exchange in PbS nanocrystals using simulations with pseudoligands

    PubMed Central

    Fan, Zhaochuan; Lin, Li-Chiang; Buijs, Wim; Vlugt, Thijs J. H.; van Huis, Marijn A.

    2016-01-01

    Cation exchange is a powerful tool for the synthesis of nanostructures such as core–shell nanocrystals, however, the underlying mechanism is poorly understood. Interactions of cations with ligands and solvent molecules are systematically ignored in simulations. Here, we introduce the concept of pseudoligands to incorporate cation-ligand-solvent interactions in molecular dynamics. This leads to excellent agreement with experimental data on cation exchange of PbS nanocrystals, whereby Pb ions are partially replaced by Cd ions from solution. The temperature and the ligand-type control the exchange rate and equilibrium composition of cations in the nanocrystal. Our simulations reveal that Pb ions are kicked out by exchanged Cd interstitials and migrate through interstitial sites, aided by local relaxations at core–shell interfaces and point defects. We also predict that high-pressure conditions facilitate strongly enhanced cation exchange reactions at elevated temperatures. Our approach is easily extendable to other semiconductor compounds and to other families of nanocrystals. PMID:27160371

  13. Generalized syntheses of nanocrystal-graphene hybrids in high-boiling-point organic solvents.

    PubMed

    Pang, Danny Wei-Ping; Yuan, Fang-Wei; Chang, Yan-Cheng; Li, Guo-An; Tuan, Hsing-Yu

    2012-08-01

    Nanocrystal-graphene have been proposed as a new kind of promising hybrid for a wide range of application areas including catalysts, electronics, sensors, biomedicine, and energy storage, etc. Although a variety of methods have been developed for the preparation of hybrids, a facile and general synthetic approach is still highly required. In this study, nanocrystal-graphene hybrids were successfully synthesized in high-boiling-point organic solvents. Graphene oxide (GO) nanosheets were modified by oleylamine (OLA) to form a OLA-GO complex in order to be readily incorporated into hydrophobic synthesis. A rich library of highly crystalline nanocrystals, with types including noble metal, metal oxide, magnetic material and semiconductor were successfully grown on chemically converted graphene (CCG), which is simultaneously reduced from GO during the synthesis. High boiling-point solvents afford sufficient thermal energy to assure the high-quality crystalline nature of NCs, therefore the post-annealing process is obviated. Controlled experiments revealed that OLA-GO triggers heterogeneous nucleation and serves as excellent nuclei anchorage media. The protocol developed here brings one step closer to achieve "unity in diversity" on the preparation of nanocrystal-graphene hybrids.

  14. Enhancing the performance of polymer solar cells using CuPc nanocrystals as additives.

    PubMed

    Zhang, Yajie; Wei, Zhixiang

    2015-05-22

    There is an increasing interest in the use of different nanoparticles as additives in polymer solar cells for enhancing the light absorption of active layers as well as their power conversion efficiency (PCE). In this paper, we report a PCE enhancement by simply adding copper phthalocyanine (CuPc) nanocrystals into photovoltaic devices based on a poly(3-hexylthiophene) (P3HT): fullerene system. Two kinds of device structure were studied: the first one is a CuPc nanocrystal suspension spin coated on the poly(3,4-ethylenedioxythiophene) polystyrene sulfonate-coated substrate; the second one is the CuPc nanocrystal suspension added into the active layer solutions. It is proved that incorporating organic semiconductor nanocrystals into the active layer can help trap light and enhance the crystallinity of the active layers, thus improving the device performance. This strategy might be generally compatible with a broad range of organic photovoltaic materials and offers an effective approach to enhance the device performance. PMID:25912794

  15. Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites

    PubMed Central

    Yakunin, Sergii; Protesescu, Loredana; Krieg, Franziska; Bodnarchuk, Maryna I.; Nedelcu, Georgian; Humer, Markus; De Luca, Gabriele; Fiebig, Manfred; Heiss, Wolfgang; Kovalenko, Maksym V.

    2015-01-01

    Metal halide semiconductors with perovskite crystal structures have recently emerged as highly promising optoelectronic materials. Despite the recent surge of reports on microcrystalline, thin-film and bulk single-crystalline metal halides, very little is known about the photophysics of metal halides in the form of uniform, size-tunable nanocrystals. Here we report low-threshold amplified spontaneous emission and lasing from ∼10 nm monodisperse colloidal nanocrystals of caesium lead halide perovskites CsPbX3 (X=Cl, Br or I, or mixed Cl/Br and Br/I systems). We find that room-temperature optical amplification can be obtained in the entire visible spectral range (440–700 nm) with low pump thresholds down to 5±1 μJ cm−2 and high values of modal net gain of at least 450±30 cm−1. Two kinds of lasing modes are successfully observed: whispering-gallery-mode lasing using silica microspheres as high-finesse resonators, conformally coated with CsPbX3 nanocrystals and random lasing in films of CsPbX3 nanocrystals. PMID:26290056

  16. Enhancing the performance of polymer solar cells using CuPc nanocrystals as additives

    NASA Astrophysics Data System (ADS)

    Zhang, Yajie; Wei, Zhixiang

    2015-05-01

    There is an increasing interest in the use of different nanoparticles as additives in polymer solar cells for enhancing the light absorption of active layers as well as their power conversion efficiency (PCE). In this paper, we report a PCE enhancement by simply adding copper phthalocyanine (CuPc) nanocrystals into photovoltaic devices based on a poly(3-hexylthiophene) (P3HT): fullerene system. Two kinds of device structure were studied: the first one is a CuPc nanocrystal suspension spin coated on the poly(3,4-ethylenedioxythiophene) polystyrene sulfonate-coated substrate; the second one is the CuPc nanocrystal suspension added into the active layer solutions. It is proved that incorporating organic semiconductor nanocrystals into the active layer can help trap light and enhance the crystallinity of the active layers, thus improving the device performance. This strategy might be generally compatible with a broad range of organic photovoltaic materials and offers an effective approach to enhance the device performance.

  17. Efficiency of the coherent biexciton admixture mechanism for multiple exciton generation in InAs nanocrystals

    NASA Astrophysics Data System (ADS)

    Kowalski, Piotr; Machnikowski, Paweł

    2015-12-01

    We study the coherent mixing between two-particle (single exciton) and four-particle (biexciton) states of a semiconductor nanocrystal resulting from the Coulomb coupling between states with different numbers of electron-hole pairs. Using a simple model of the nanocrystal wave functions and an envelope function approach, we estimate the efficiency of the multiple exciton generation (MEG) process resulting from such coherent admixture mechanism, including all the relevant states in a very broad energy interval. We show that in a typical ensemble of nanocrystals with an average radius of 3nm, the onset of the MEG process appears about 1 eV above the lower edge of the biexciton density of states. This is due to the angular momentum conservation that imposes selection rules and limits the available MEG pathways, thus taking over the role of momentum conservation that hinders this process in bulk. The efficiency of the MEG process reaches 50% for photon energies around 5 eV. The MEG onset shifts to lower energies and therefore the efficiency increases in a certain energy range as the radius grows. The energy dependence of the MEG efficiency differs considerably between ensembles with small and large inhomogeneity of nanocrystal sizes.

  18. Colloidal nanocrystals for quality lighting and displays: milestones and recent developments

    NASA Astrophysics Data System (ADS)

    Erdem, Talha; Demir, Hilmi Volkan

    2016-06-01

    Recent advances in colloidal synthesis of nanocrystals have enabled high-quality high-efficiency light-emitting diodes, displays with significantly broader color gamut, and optically-pumped lasers spanning the whole visible regime. Here we review these colloidal platforms covering the milestone studies together with recent developments. In the review, we focus on the devices made of colloidal quantum dots (nanocrystals), colloidal quantum rods (nanorods), and colloidal quantum wells (nanoplatelets) as well as those of solution processed perovskites and phosphor nanocrystals. The review starts with an introduction to colloidal nanocrystal photonics emphasizing the importance of colloidal materials for light-emitting devices. Subsequently,we continue with the summary of important reports on light-emitting diodes, in which colloids are used as the color converters and then as the emissive layers in electroluminescent devices. Also,we review the developments in color enrichment and electroluminescent displays. Next, we present a summary of important reports on the lasing of colloidal semiconductors. Finally, we summarize and conclude the review presenting a future outlook.

  19. Quantitative tunneling spectroscopy of nanocrystals

    SciTech Connect

    First, Phillip N; Whetten, Robert L; Schaaff, T Gregory

    2007-05-25

    The proposed goals of this collaborative work were to systematically characterize the electronic structure and dynamics of 3-dimensional metal and semiconducting nanocrystals using scanning tunneling microscopy/spectroscopy (STM/STS) and ballistic electron emission spectroscopy (BEES). This report describes progress in the spectroscopic work and in the development of methods for creating and characterizing gold nanocrystals. During the grant period, substantial effort also was devoted to the development of epitaxial graphene (EG), a very promising materials system with outstanding potential for nanometer-scale ballistic and coherent devices ("graphene" refers to one atomic layer of graphitic, sp2 -bonded carbon atoms [or more loosely, few layers]). Funding from this DOE grant was critical for the initial development of epitaxial graphene for nanoelectronics

  20. Formation of Copper Zinc Tin Sulfide Thin Films from Colloidal Nanocrystal Dispersions via Aerosol-Jet Printing and Compaction.

    PubMed

    Williams, Bryce A; Mahajan, Ankit; Smeaton, Michelle A; Holgate, Collin S; Aydil, Eray S; Francis, Lorraine F

    2015-06-01

    A three-step method to create dense polycrystalline semiconductor thin films from nanocrystal liquid dispersions is described. First, suitable substrates are coated with nanocrystals using aerosol-jet printing. Second, the porous nanocrystal coatings are compacted using a weighted roller or a hydraulic press to increase the coating density. Finally, the resulting coating is annealed for grain growth. The approach is demonstrated for making polycrystalline films of copper zinc tin sulfide (CZTS), a new solar absorber composed of earth-abundant elements. The range of coating morphologies accessible through aerosol-jet printing is examined and their formation mechanisms are revealed. Crack-free albeit porous films are obtained if most of the solvent in the aerosolized dispersion droplets containing the nanocrystals evaporates before they impinge on the substrate. In this case, nanocrystals agglomerate in flight and arrive at the substrate as solid spherical agglomerates. These porous coatings are mechanically compacted, and the density of the coating increases with compaction pressure. Dense coatings annealed in sulfur produce large-grain (>1 μm) polycrystalline CZTS films with microstructure suitable for thin-film solar cells. PMID:25989610

  1. Aligned magnetic domains in p- and n-type ferromagnetic nanocrystals and in pn-junction nanodiodes.

    PubMed

    Bera, Abhijit; Pal, Amlan J

    2013-11-27

    We form pn- and np-junctions between monolayers of p- and n-type nanocrystals that exhibit current rectification in the nanodiodes when characterized with a scanning tunneling microscope (STM) tip. With the use of ferromagnetic nanocrystals, we study the effect of mutual alignment of magnetization vectors on current rectification in the junction between the two nanocrystals. We show that when the magnetization vectors of the p- and of the n-type nanocrystals are parallel to each other (and both facing toward the apex of the STM tip) tunneling current in both bias modes increases with correspondingly a higher rectification ratio. This is in contrast to the parameters of the nanodiodes in which magnetization vectors of the components are unaligned or randomized. To analyze the results, we record scanning tunneling spectroscopy of the monolayer of the components having magnetization vectors aligned or unaligned to locate their valence and conduction band edges and to determine the effect of the alignment on the band edges. Upon alignment of the magnetization vectors of the nanocrystals in a monolayer, the conduction band edge of the p-type and valence band edge of the n-type semiconductor shift towards the Fermi energy leading to a change in energy levels of the pn-junctions and accounting for the improved parameters of the nanodiodes.

  2. Time Dependent Study of Multiple Exciton Generation in Nanocrystal Quantum Dots

    NASA Astrophysics Data System (ADS)

    Damtie, Fikeraddis A.; Wacker, Andreas

    2016-03-01

    We study the exciton dynamics in an optically excited nanocrystal quantum dot. Multiple exciton formation is more efficient in nanocrystal quantum dots compared to bulk semiconductors due to enhanced Coulomb interactions and the absence of conservation of momentum. The formation of multiple excitons is dependent on different excitation parameters and the dissipation. We study this process within a Lindblad quantum rate equation using the full many-particle states. We optically excite the system by creating a single high energy exciton ESX in resonance to a double exciton EDX. With Coulomb electron-electron interaction, the population can be transferred from the single exciton to the double exciton state by impact ionisation (inverse Auger process). The ratio between the recombination processes and the absorbed photons provide the yield of the structure. We observe a quantum yield of comparable value to experiment assuming typical experimental conditions for a 4 nm PbS quantum dot.

  3. Hollow nanocrystals and method of making

    DOEpatents

    Alivisatos, A. Paul; Yin, Yadong; Erdonmez, Can Kerem

    2011-07-05

    Described herein are hollow nanocrystals having various shapes that can be produced by a simple chemical process. The hollow nanocrystals described herein may have a shell as thin as 0.5 nm and outside diameters that can be controlled by the process of making.

  4. Structure Map for Embedded Binary Alloy Nanocrystals

    SciTech Connect

    Yuan, C.W.; Shin, S.J.; Liao, C.Y.; Guzman, J.; Stone, P.R.; Watanabe, M.; Ager III, J.W.; Haller, E.E.; Chrzan, D.C.

    2008-09-20

    The equilibrium structure of embedded nanocrystals formed from strongly segregating binary-alloys is considered within a simple thermodynamic model. The model identifies two dimensionlessinterface energies that dictate the structure, and allows prediction of the stable structure for anychoice of these parameters. The resulting structure map includes three distinct nanocrystal mor-phologies: core/shell, lobe/lobe, and completely separated spheres.

  5. Functional assemblies of nanocrystal quantum dots on microtubule scaffolds

    NASA Astrophysics Data System (ADS)

    Jeong, Sohee

    2005-11-01

    We assembled semiconductor nanocrystal quantum dots (NQDs) using microtubule (MT) fibers as nanoscale scaffolds and characterized structure and function of the assemblies. MTs were chosen as the biotemplate as these biomolecules, in conjunction with kinesin motor proteins, offer the potential for dynamic transport of nanoscale cargo. Ultimately, the ability to control and direct the reconfigurable assembly of nanomaterials from the nano- to the macro-scales will likely depend on the degree to which the specific interactions between artificial inorganic/organic nano-components and natural, biological components are understood. Thus, the work here addressed two fundamental issues key to this understanding: (1) The extent to which NQD stability and photophysical properties are affected by being rendered "biocompatible" and (2) The impact on "biofunction" when biomolecules are coupled with artificial nanomaterials. These issues were addressed by first investigating several strategies for transforming hydrophobic nanocrystals into water-soluble, biocompatible materials. The resulting particles were compared in terms of their optical properties (e.g., retention of high emission quantum yields) and chemical stability (using a novel fluorescence resonance energy transfer, FRET, method to study particle aggregation). Second, a previously described strategy for rendering nanocrystals water soluble by exchanging as-prepared surface ligands with bifunctional thiol ligands was studied by investigating the effect of thiols on the optical properties of NQDs as a function of time, concentration, pH and moiety. Thiolate anions were found to both passivate existing electron traps (enhancing emission) and introduce new hole traps (decreasing emission). Third, NQDs were assembled onto MT supports by way of streptavidin-biotin and electrostatic interactions. Interdot "communication" through interparticle energy transfer was then used to determine the nanoscale structure of the

  6. Copper selenide nanocrystals for photothermal therapy.

    PubMed

    Hessel, Colin M; Pattani, Varun P; Rasch, Michael; Panthani, Matthew G; Koo, Bonil; Tunnell, James W; Korgel, Brian A

    2011-06-01

    Ligand-stabilized copper selenide (Cu(2-x)Se) nanocrystals, approximately 16 nm in diameter, were synthesized by a colloidal hot injection method and coated with amphiphilic polymer. The nanocrystals readily disperse in water and exhibit strong near-infrared (NIR) optical absorption with a high molar extinction coefficient of 7.7 × 10(7) cm(-1) M(-1) at 980 nm. When excited with 800 nm light, the Cu(2-x)Se nanocrystals produce significant photothermal heating with a photothermal transduction efficiency of 22%, comparable to nanorods and nanoshells of gold (Au). In vitro photothermal heating of Cu(2-x)Se nanocrystals in the presence of human colorectal cancer cell (HCT-116) led to cell destruction after 5 min of laser irradiation at 33 W/cm(2), demonstrating the viabilitiy of Cu(2-x)Se nanocrystals for photothermal therapy applications. PMID:21553924

  7. Copper Selenide Nanocrystals for Photothermal Therapy

    PubMed Central

    Hessel, Colin M.; Pattani, Varun; Rasch, Michael; Panthani, Matthew G.; Koo, Bonil; Tunnell, James W.; Korgel, Brian A.

    2011-01-01

    Ligand-stabilized copper selenide (Cu2−xSe) nanocrystals, approximately 16 nm in diameter, were synthesized by a colloidal hot injection method and coated with amphiphilic polymer. The nanocrystals readily disperse in water and exhibit strong near infrared (NIR) optical absorption with a high molar extinction coefficient of 7.7 × 107 cm−1 M−1 at 980 nm. When excited with 800 nm light, the Cu2−xSe nanocrystals produce significant photothermal heating with a photothermal transduction efficiency of 22%, comparable to nanorods and nanoshells of gold (Au). In vitro photothermal heating of Cu2−xSe nanocrystals in the presence of human colorectal cancer cell (HCT-116) led to cell destruction after 5 minutes of laser irradiation at 33 W/cm2, demonstrating the viabilitiy of Cu2−xSe nanocrystals for photothermal therapy applications. PMID:21553924

  8. Nanocrystal technology, drug delivery and clinical applications

    PubMed Central

    Junghanns, Jens-Uwe A H; Müller, Rainer H

    2008-01-01

    Nanotechnology will affect our lives tremendously over the next decade in very different fields, including medicine and pharmacy. Transfer of materials into the nanodimension changes their physical properties which were used in pharmaceutics to develop a new innovative formulation principle for poorly soluble drugs: the drug nanocrystals. The drug nanocrystals do not belong to the future; the first products are already on the market. The industrially relevant production technologies, pearl milling and high pressure homogenization, are reviewed. The physics behind the drug nanocrystals and changes of their physical properties are discussed. The marketed products are presented and the special physical effects of nanocrystals explained which are utilized in each market product. Examples of products in the development pipelines (clinical phases) are presented and the benefits for in vivo administration of drug nanocrystals are summarized in an overview. PMID:18990939

  9. Unitary lens semiconductor device

    DOEpatents

    Lear, K.L.

    1997-05-27

    A unitary lens semiconductor device and method are disclosed. The unitary lens semiconductor device is provided with at least one semiconductor layer having a composition varying in the growth direction for unitarily forming one or more lenses in the semiconductor layer. Unitary lens semiconductor devices may be formed as light-processing devices such as microlenses, and as light-active devices such as light-emitting diodes, photodetectors, resonant-cavity light-emitting diodes, vertical-cavity surface-emitting lasers, and resonant cavity photodetectors. 9 figs.

  10. Unitary lens semiconductor device

    DOEpatents

    Lear, Kevin L.

    1997-01-01

    A unitary lens semiconductor device and method. The unitary lens semiconductor device is provided with at least one semiconductor layer having a composition varying in the growth direction for unitarily forming one or more lenses in the semiconductor layer. Unitary lens semiconductor devices may be formed as light-processing devices such as microlenses, and as light-active devices such as light-emitting diodes, photodetectors, resonant-cavity light-emitting diodes, vertical-cavity surface-emitting lasers, and resonant cavity photodetectors.

  11. Exploiting the colloidal nanocrystal library to construct electronic devices

    NASA Astrophysics Data System (ADS)

    Choi, Ji-Hyuk; Wang, Han; Oh, Soong Ju; Paik, Taejong; Sung, Pil; Sung, Jinwoo; Ye, Xingchen; Zhao, Tianshuo; Diroll, Benjamin T.; Murray, Christopher B.; Kagan, Cherie R.

    2016-04-01

    Synthetic methods produce libraries of colloidal nanocrystals with tunable physical properties by tailoring the nanocrystal size, shape, and composition. Here, we exploit colloidal nanocrystal diversity and design the materials, interfaces, and processes to construct all-nanocrystal electronic devices using solution-based processes. Metallic silver and semiconducting cadmium selenide nanocrystals are deposited to form high-conductivity and high-mobility thin-film electrodes and channel layers of field-effect transistors. Insulating aluminum oxide nanocrystals are assembled layer by layer with polyelectrolytes to form high–dielectric constant gate insulator layers for low-voltage device operation. Metallic indium nanocrystals are codispersed with silver nanocrystals to integrate an indium supply in the deposited electrodes that serves to passivate and dope the cadmium selenide nanocrystal channel layer. We fabricate all-nanocrystal field-effect transistors on flexible plastics with electron mobilities of 21.7 square centimeters per volt-second.

  12. Exploiting the colloidal nanocrystal library to construct electronic devices

    NASA Astrophysics Data System (ADS)

    Choi, Ji-Hyuk; Wang, Han; Oh, Soong Ju; Paik, Taejong; Sung, Pil; Sung, Jinwoo; Ye, Xingchen; Zhao, Tianshuo; Diroll, Benjamin T.; Murray, Christopher B.; Kagan, Cherie R.

    2016-04-01

    Synthetic methods produce libraries of colloidal nanocrystals with tunable physical properties by tailoring the nanocrystal size, shape, and composition. Here, we exploit colloidal nanocrystal diversity and design the materials, interfaces, and processes to construct all-nanocrystal electronic devices using solution-based processes. Metallic silver and semiconducting cadmium selenide nanocrystals are deposited to form high-conductivity and high-mobility thin-film electrodes and channel layers of field-effect transistors. Insulating aluminum oxide nanocrystals are assembled layer by layer with polyelectrolytes to form high-dielectric constant gate insulator layers for low-voltage device operation. Metallic indium nanocrystals are codispersed with silver nanocrystals to integrate an indium supply in the deposited electrodes that serves to passivate and dope the cadmium selenide nanocrystal channel layer. We fabricate all-nanocrystal field-effect transistors on flexible plastics with electron mobilities of 21.7 square centimeters per volt-second.

  13. Exploiting the colloidal nanocrystal library to construct electronic devices.

    PubMed

    Choi, Ji-Hyuk; Wang, Han; Oh, Soong Ju; Paik, Taejong; Sung, Pil; Sung, Jinwoo; Ye, Xingchen; Zhao, Tianshuo; Diroll, Benjamin T; Murray, Christopher B; Kagan, Cherie R

    2016-04-01

    Synthetic methods produce libraries of colloidal nanocrystals with tunable physical properties by tailoring the nanocrystal size, shape, and composition. Here, we exploit colloidal nanocrystal diversity and design the materials, interfaces, and processes to construct all-nanocrystal electronic devices using solution-based processes. Metallic silver and semiconducting cadmium selenide nanocrystals are deposited to form high-conductivity and high-mobility thin-film electrodes and channel layers of field-effect transistors. Insulating aluminum oxide nanocrystals are assembled layer by layer with polyelectrolytes to form high-dielectric constant gate insulator layers for low-voltage device operation. Metallic indium nanocrystals are codispersed with silver nanocrystals to integrate an indium supply in the deposited electrodes that serves to passivate and dope the cadmium selenide nanocrystal channel layer. We fabricate all-nanocrystal field-effect transistors on flexible plastics with electron mobilities of 21.7 square centimeters per volt-second. PMID:27124455

  14. Nanocrystal-based Optoelectronic Devices

    NASA Astrophysics Data System (ADS)

    Evans, Kenneth; Herzog, Joseph; Ward, Daniel; Natelson, Douglas

    2012-02-01

    Optoelectronic devices capable of detecting and emitting light on a scale well below its wavelength could have a profound impact on basic and applied experimental research in light-based electronics, on-demand photon generation, and for studying poorly understood quantum phenomena such as blinking and spectral wandering. We present a fabrication procedure for ultrasmall, nanocrystal optoelectronic devices based on self-assembled layers of quantum dots in plasmonically-active gold nanogaps. We provide preliminary experimental results which examine the possibility for surfaced-enhanced fluorescence, subwavelength detection and emission of light as well as plasmon-based optical trapping in these systems.

  15. Colloidal synthesis of Cu-ZnO and Cu@CuNi-ZnO hybrid nanocrystals with controlled morphologies and multifunctional properties

    NASA Astrophysics Data System (ADS)

    Zeng, Deqian; Gong, Pingyun; Chen, Yuanzhi; Zhang, Qinfu; Xie, Qingshui; Peng, Dong-Liang

    2016-06-01

    Metal-semiconductor hybrid nanocrystals have received extensive attention owing to their multiple functionalities which can find wide technological applications. The utilization of low-cost non-noble metals to construct novel metal-semiconductor hybrid nanocrystals is important and meaningful for their large-scale applications. In this study, a facile solution approach is developed for the synthesis of Cu-ZnO hybrid nanocrystals with well-controlled morphologies, including nanomultipods, core-shell nanoparticles, nanopyramids and core-shell nanowires. In the synthetic strategy, Cu nanocrystals formed in situ serve as seeds for the heterogeneous nucleation and growth of ZnO, and it eventually forms various Cu-ZnO hetero-nanostructures under different reaction conditions. These hybrid nanocrystals possess well-defined and stable heterostructure junctions. The ultraviolet-visible-near infrared spectra reveal morphology-dependent surface plasmon resonance absorption of Cu and the band gap absorption of ZnO. Furthermore, we construct a novel Cu@CuNi-ZnO ternary hetero-nanostructure by incorporating the magnetic metal Ni into the pre-synthesized colloidal Cu nanocrystals. Such hybrid nanocrystals possess a magnetic Cu-Ni intermediate layer between the ZnO shell and the Cu core, and exhibit ferromagnetic/superparamagnetic properties which expand their functionalities. Finally, enhanced photocatalytic activities are observed in the as-prepared non-noble metal-ZnO hybrid nanocrystals. This study not only provides an economical way to prepare high-quality morphology-controlled Cu-ZnO hybrid nanocrystals for potential applications in the fields of photocatalysis and photovoltaic devices, but also opens up new opportunities in designing ternary non-noble metal-semiconductor hybrid nanocrystals with multifunctionalities.Metal-semiconductor hybrid nanocrystals have received extensive attention owing to their multiple functionalities which can find wide technological applications

  16. Colloidal synthesis of Cu-ZnO and Cu@CuNi-ZnO hybrid nanocrystals with controlled morphologies and multifunctional properties

    NASA Astrophysics Data System (ADS)

    Zeng, Deqian; Gong, Pingyun; Chen, Yuanzhi; Zhang, Qinfu; Xie, Qingshui; Peng, Dong-Liang

    2016-06-01

    Metal-semiconductor hybrid nanocrystals have received extensive attention owing to their multiple functionalities which can find wide technological applications. The utilization of low-cost non-noble metals to construct novel metal-semiconductor hybrid nanocrystals is important and meaningful for their large-scale applications. In this study, a facile solution approach is developed for the synthesis of Cu-ZnO hybrid nanocrystals with well-controlled morphologies, including nanomultipods, core-shell nanoparticles, nanopyramids and core-shell nanowires. In the synthetic strategy, Cu nanocrystals formed in situ serve as seeds for the heterogeneous nucleation and growth of ZnO, and it eventually forms various Cu-ZnO hetero-nanostructures under different reaction conditions. These hybrid nanocrystals possess well-defined and stable heterostructure junctions. The ultraviolet-visible-near infrared spectra reveal morphology-dependent surface plasmon resonance absorption of Cu and the band gap absorption of ZnO. Furthermore, we construct a novel Cu@CuNi-ZnO ternary hetero-nanostructure by incorporating the magnetic metal Ni into the pre-synthesized colloidal Cu nanocrystals. Such hybrid nanocrystals possess a magnetic Cu-Ni intermediate layer between the ZnO shell and the Cu core, and exhibit ferromagnetic/superparamagnetic properties which expand their functionalities. Finally, enhanced photocatalytic activities are observed in the as-prepared non-noble metal-ZnO hybrid nanocrystals. This study not only provides an economical way to prepare high-quality morphology-controlled Cu-ZnO hybrid nanocrystals for potential applications in the fields of photocatalysis and photovoltaic devices, but also opens up new opportunities in designing ternary non-noble metal-semiconductor hybrid nanocrystals with multifunctionalities.Metal-semiconductor hybrid nanocrystals have received extensive attention owing to their multiple functionalities which can find wide technological applications

  17. Spinel ferrite nanocrystals embedded inside ZnO: magnetic, electronic andmagneto-transport properties

    SciTech Connect

    Zhou, Shengqiang; Potzger, K.; Xu, Qingyu; Kuepper, K.; Talut, G.; Marko, D.; Mucklich, A.; Helm, M.; Fassbender, J.; Arenholz, E.; Schmidt, H.

    2009-08-21

    In this paper we show that spinel ferrite nanocrystals (NiFe{sub 2}O{sub 4}, and CoFe{sub 2}O{sub 4}) can be texturally embedded inside a ZnO matrix by ion implantation and post-annealing. The two kinds of ferrites show different magnetic properties, e.g. coercivity and magnetization. Anomalous Hall effect and positive magnetoresistance have been observed. Our study suggests a ferrimagnet/semiconductor hybrid system for potential applications in magneto-electronics. This hybrid system can be tuned by selecting different transition metal ions (from Mn to Zn) to obtain various magnetic and electronic properties.

  18. Using x-ray diffraction to identify precipitates in transition metal doped semiconductors

    NASA Astrophysics Data System (ADS)

    Zhou, Shengqiang; Potzger, K.; Talut, G.; von Borany, J.; Skorupa, W.; Helm, M.; Fassbender, J.

    2008-04-01

    In the past decade, room temperature ferromagnetism was often observed in transition metal doped semiconductors, which were claimed as diluted magnetic semiconductors (DMS). Nowadays intensive activities are devoted to clarify wether the observed ferromagnetism stems from carrier mediated magnetic impurities, ferromagnetic precipitates, or spinodal decomposition. In this paper, we have correlated the structural and magnetic properties of transition metal doped ZnO, TiO2, and Si, prepared by ion implantation. Crystalline precipitates, i.e., transition metal (Co, Ni) and Mn-silicide nanocrystals, are responsible for the magnetism. Additionally due to their orientation nature with respect to the host, these nanocrystals in some cases are not detectable by conventional x-ray diffraction (XRD). This nature results in the pitfall of using XRD to exclude magnetic precipitates in DMS materials.

  19. Structural Investigations of Surfaces and Orientation-SpecificPhenomena in Nanocrystals and Their Assemblies

    SciTech Connect

    Aruguete, Deborah Michiko

    2006-01-01

    Studies of colloidal nanocrystals and their assemblies are presented. Two of these studies concern the atomic-level structural characterization of the surfaces, interfaces, and interiors present in II-VI semiconductor nanorods. The third study investigates the crystallographic arrangement of cobalt nanocrystals in self-assembled aggregates. Crystallographically-aligned assemblies of colloidal CdSe nanorods are examined with linearly-polarized Se-EXAFS spectroscopy, which probes bonding along different directions in the nanorod. This orientation-specific probe is used, because it is expected that the presence of specific surfaces in a nanorod might cause bond relaxations specific to different crystallographic directions. Se-Se distances are found to be contracted along the long axis of the nanorod, while Cd-Se distances display no angular dependence, which is different from the bulk. Ab-initio density functional theory calculations upon CdSe nanowires indicate that relaxations on the rod surfaces cause these changes. ZnS/CdS-CdSe core-shell nanorods are studied with Se, Zn, Cd, and S X-ray absorption spectroscopy (XAS). It is hypothesized that there are two major factors influencing the core and shell structures of the nanorods: the large surface area-to-volume ratio, and epitaxial strain. The presence of the surface may induce bond rearrangements or relaxations to minimize surface energy; epitaxial strain might cause the core and shell lattices to contract or expand to minimize strain energy. A marked contraction of Zn-S bonds is observed in the core-shell nanorods, indicating that surface relaxations may dominate the structure of the nanorod (strain might otherwise drive the Zn-S lattice to accommodate the larger CdS or CdSe lattices via bond expansion). EXAFS and X-ray diffraction (XRD) indicate that Cd-Se bond relaxations might be anisotropic, an expected phenomenon for a rod-shaped nanocrystal. Ordered self-assembled aggregates of cobalt nanocrystals are

  20. Controlling upconversion nanocrystals for emerging applications

    NASA Astrophysics Data System (ADS)

    Zhou, Bo; Shi, Bingyang; Jin, Dayong; Liu, Xiaogang

    2015-11-01

    Lanthanide-doped upconversion nanocrystals enable anti-Stokes emission with pump intensities several orders of magnitude lower than required by conventional nonlinear optical techniques. Their exceptional properties, namely large anti-Stokes shifts, sharp emission spectra and long excited-state lifetimes, have led to a diversity of applications. Here, we review upconversion nanocrystals from the perspective of fundamental concepts and examine the technical challenges in relation to emission colour tuning and luminescence enhancement. In particular, we highlight the advances in functionalization strategies that enable the broad utility of upconversion nanocrystals for multimodal imaging, cancer therapy, volumetric displays and photonics.

  1. Progress in the study of drug nanocrystals.

    PubMed

    Shi, Jing; Guo, Fei; Zheng, Aiping; Zhang, Xiaoyan; Sun, Jianxu

    2015-12-01

    The poor water solubility of many candidate drugs remains a major obstacle to their development and clinical use, especially for oral drug delivery. Nanocrystal technology can improve the solubility and dissolution rates of many poorly water-soluble drugs very effectively, significantly improving their oral bioavailability and decreasing the food effect. For this reason, this technology is becoming a key area of drug delivery research. This review presents much of the recent progress in nanocrystal drug pharmaceuticals, including the characteristics, composition, preparation technology, and clinical applications of these drugs. Finally, the effect of nanocrystal technology on insoluble drugs is quantified and described. PMID:26817271

  2. Semiconductor ohmic contact

    NASA Technical Reports Server (NTRS)

    Hawrylo, Frank Zygmunt (Inventor); Kressel, Henry (Inventor)

    1977-01-01

    A semiconductor device has one surface of P type conductivity material having a wide energy bandgap and a large crystal lattice parameter. Applied to the P type surface of the semiconductor device is a degenerate region of semiconductor material, preferably a group III-V semiconductor material, having a narrower energy bandgap. The degenerate region is doped with tin to increase the crystal lattice of the region to more closely approximate the crystal lattice of the one surface of the semiconductor device. The degenerate region is compensatingly doped with a P type conductivity modifier. An electrical contact is applied to one surface of the degenerate region forming an ohmic contact with the semiconductor device.

  3. Shape-dependent plasmonic response and directed self-assembly in a new semiconductor building block, indium-doped cadmium oxide (ICO).

    PubMed

    Gordon, Thomas R; Paik, Taejong; Klein, Dahlia R; Naik, Gururaj V; Caglayan, Humeyra; Boltasseva, Alexandra; Murray, Christopher B

    2013-06-12

    The influence of particle shape on plasmonic response and local electric field strength is well-documented in metallic nanoparticles. Morphologies such as rods, plates, and octahedra are readily synthesized and exhibit drastically different extinction spectra than spherical particles. Despite this fact, the influence of composition and shape on the optical properties of plasmonic semiconductor nanocrystals, in which free electrons result from heavy doping, has not been well-studied. Here, we report the first observation of plasmonic resonance in indium-doped cadmium oxide (ICO) nanocrystals, which exhibit the highest quality factors reported for semiconductor nanocrystals. Furthermore, we are able to independently control the shape and free electron concentration in ICO nanocrystals, allowing for the influence of shape on the optical response of a plasmonic semiconductor to be conclusively demonstrated. The highly uniform particles may be self-assembled into ordered single component and binary nanocrystal superlattices, and in thin films, exhibit negative permittivity in the near infrared (NIR) region, validating their use as a new class of tunable low-loss plasmonic building blocks for 3-D optical metamaterials.

  4. Semiconductor bridge (SCB) detonator

    DOEpatents

    Bickes, Jr., Robert W.; Grubelich, Mark C.

    1999-01-01

    The present invention is a low-energy detonator for high-density secondary-explosive materials initiated by a semiconductor bridge igniter that comprises a pair of electrically conductive lands connected by a semiconductor bridge. The semiconductor bridge is in operational or direct contact with the explosive material, whereby current flowing through the semiconductor bridge causes initiation of the explosive material. Header wires connected to the electrically-conductive lands and electrical feed-throughs of the header posts of explosive devices, are substantially coaxial to the direction of current flow through the SCB, i.e., substantially coaxial to the SCB length.

  5. Semiconductor bridge (SCB) detonator

    DOEpatents

    Bickes, R.W. Jr.; Grubelich, M.C.

    1999-01-19

    The present invention is a low-energy detonator for high-density secondary-explosive materials initiated by a semiconductor bridge (SCB) igniter that comprises a pair of electrically conductive lands connected by a semiconductor bridge. The semiconductor bridge is in operational or direct contact with the explosive material, whereby current flowing through the semiconductor bridge causes initiation of the explosive material. Header wires connected to the electrically-conductive lands and electrical feed-throughs of the header posts of explosive devices, are substantially coaxial to the direction of current flow through the SCB, i.e., substantially coaxial to the SCB length. 3 figs.

  6. Interconnected semiconductor devices

    DOEpatents

    Grimmer, Derrick P.; Paulson, Kenneth R.; Gilbert, James R.

    1990-10-23

    Semiconductor layer and conductive layer formed on a flexible substrate, divided into individual devices and interconnected with one another in series by interconnection layers and penetrating terminals.

  7. Solvent-like ligand-coated ultrasmall cadmium selenide nanocrystals: strong electronic coupling in a self-organized assembly

    NASA Astrophysics Data System (ADS)

    Lawrence, Katie N.; Johnson, Merrell A.; Dolai, Sukanta; Kumbhar, Amar; Sardar, Rajesh

    2015-07-01

    Strong inter-nanocrystal electronic coupling is a prerequisite for delocalization of exciton wave functions and high conductivity. We report 170 meV electronic coupling energy of short chain poly(ethylene glycol) thiolate-coated ultrasmall (<2.5 nm in diameter) CdSe semiconductor nanocrystals (SNCs) in solution. Cryo-transmission electron microscopy analysis showed the formation of a pearl-necklace assembly of nanocrystals in solution with regular inter-nanocrystal spacing. The electronic coupling was studied as a function of CdSe nanocrystal size where the smallest nanocrystals exhibited the largest coupling energy. The electronic coupling in spin-cast thin-film (<200 nm in thickness) of poly(ethylene glycol) thiolate-coated CdSe SNCs was studied as a function of annealing temperature, where an unprecedentedly large, ~400 meV coupling energy was observed for 1.6 nm diameter SNCs, which were coated with a thin layer of poly(ethylene glycol) thiolates. Small-angle X-ray scattering measurements showed that CdSe SNCs maintained an order array inside the films. The strong electronic coupling of SNCs in a self-organized film could facilitate the large-scale production of highly efficient electronic materials for advanced optoelectronic device application.Strong inter-nanocrystal electronic coupling is a prerequisite for delocalization of exciton wave functions and high conductivity. We report 170 meV electronic coupling energy of short chain poly(ethylene glycol) thiolate-coated ultrasmall (<2.5 nm in diameter) CdSe semiconductor nanocrystals (SNCs) in solution. Cryo-transmission electron microscopy analysis showed the formation of a pearl-necklace assembly of nanocrystals in solution with regular inter-nanocrystal spacing. The electronic coupling was studied as a function of CdSe nanocrystal size where the smallest nanocrystals exhibited the largest coupling energy. The electronic coupling in spin-cast thin-film (<200 nm in thickness) of poly(ethylene glycol) thiolate

  8. Semiconductor Quantum Rods as Single Molecule FluorescentBiological Labels

    SciTech Connect

    Fu, Aihua; Gu, Weiwei; Boussert, Benjamine; Koski, Kristie; Gerion, Daniele; Manna, Liberato; Le Gros, Mark; Larabell, Carolyn; Alivisatos, A. Paul

    2006-05-29

    In recent years, semiconductor quantum dots have beenapplied with great advantage in a wide range of biological imagingapplications. The continuing developments in the synthesis of nanoscalematerials and specifically in the area of colloidal semiconductornanocrystals have created an opportunity to generate a next generation ofbiological labels with complementary or in some cases enhanced propertiescompared to colloidal quantum dots. In this paper, we report thedevelopment of rod shaped semiconductor nanocrystals (quantum rods) asnew fluorescent biological labels. We have engineered biocompatiblequantum rods by surface silanization and have applied them fornon-specific cell tracking as well as specific cellular targeting. Theproperties of quantum rods as demonstrated here are enhanced sensitivityand greater resistance for degradation as compared to quantum dots.Quantum rods have many potential applications as biological labels insituations where their properties offer advantages over quantumdots.

  9. Materials chemistry. Composition-matched molecular "solders" for semiconductors.

    PubMed

    Dolzhnikov, Dmitriy S; Zhang, Hao; Jang, Jaeyoung; Son, Jae Sung; Panthani, Matthew G; Shibata, Tomohiro; Chattopadhyay, Soma; Talapin, Dmitri V

    2015-01-23

    We propose a general strategy to synthesize largely unexplored soluble chalcogenidometallates of cadmium, lead, and bismuth. These compounds can be used as "solders" for semiconductors widely used in photovoltaics and thermoelectrics. The addition of solder helped to bond crystal surfaces and link nano- or mesoscale particles together. For example, CdSe nanocrystals with Na2Cd2Se3 solder was used as a soluble precursor for CdSe films with electron mobilities exceeding 300 square centimeters per volt-second. CdTe, PbTe, and Bi2Te3 powders were molded into various shapes in the presence of a small additive of composition-matched chalcogenidometallate or chalcogel, thus opening new design spaces for semiconductor technologies. PMID:25569110

  10. Materials chemistry. Composition-matched molecular "solders" for semiconductors.

    PubMed

    Dolzhnikov, Dmitriy S; Zhang, Hao; Jang, Jaeyoung; Son, Jae Sung; Panthani, Matthew G; Shibata, Tomohiro; Chattopadhyay, Soma; Talapin, Dmitri V

    2015-01-23

    We propose a general strategy to synthesize largely unexplored soluble chalcogenidometallates of cadmium, lead, and bismuth. These compounds can be used as "solders" for semiconductors widely used in photovoltaics and thermoelectrics. The addition of solder helped to bond crystal surfaces and link nano- or mesoscale particles together. For example, CdSe nanocrystals with Na2Cd2Se3 solder was used as a soluble precursor for CdSe films with electron mobilities exceeding 300 square centimeters per volt-second. CdTe, PbTe, and Bi2Te3 powders were molded into various shapes in the presence of a small additive of composition-matched chalcogenidometallate or chalcogel, thus opening new design spaces for semiconductor technologies.

  11. Bonding pathways of gold nanocrystals in solution.

    PubMed

    Aabdin, Zainul; Lu, Jingyu; Zhu, Xi; Anand, Utkarsh; Loh, N Duane; Su, Haibin; Mirsaidov, Utkur

    2014-11-12

    Nanocrystal bonding is an important phenomenon in crystal growth and nanoscale welding. Here, we show that for gold nanocrystals bonding in solution can follow two distinct pathways: (1) coherent, defect-free bonding occurs when two nanocrystals attach with their lattices aligned to within a critical angle; and (2) beyond this critical angle, defects form at the interfaces where the nanocrystals merge. The critical misalignment angle for ∼10 nm crystals is ∼15° in both in situ experiments and full-atom molecular dynamics simulations. Understanding the origin of this critical angle during bonding may help us predict and manage strain profiles in nanoscale assemblies and inspire techniques toward reproducible and extensible architectures using only basic crystalline blocks.

  12. Resonant tunneling of carriers in silicon nanocrystals

    NASA Astrophysics Data System (ADS)

    Derbenyova, N. V.; Konakov, A. A.; Burdov, V. A.

    2016-10-01

    The rates of resonant and nearly resonant tunnel transitions have been calculated within the envelope function approximation for electrons and holes in silicon nanocrystals embedded in a silicon dioxide matrix. It is shown that, if the nanocrystals are close enough, the rates of resonant tunneling reach the values of the order of 1012-1014 s-1, which considerably exceed the rates of radiative recombination and other basic non-radiative processes, such as the Auger recombination and capture on surface defects. The transition rate is found to be very sensitive to inter-crystallite distance, crystallite size, and effective mass of the carriers in the oxide matrix. Electron tunneling turns out to be faster than the hole one, especially, at greater distances between the nanocrystals. Thus, the tunnel migration in a dense ensemble of nanocrystals is mainly electronic.

  13. Colloidal nanocrystals and method of making

    SciTech Connect

    Kahen, Keith

    2015-10-06

    A tight confinement nanocrystal comprises a homogeneous center region having a first composition and a smoothly varying region having a second composition wherein a confining potential barrier monotonically increases and then monotonically decreases as the smoothly varying region extends from the surface of the homogeneous center region to an outer surface of the nanocrystal. A method of producing the nanocrystal comprises forming a first solution by combining a solvent and at most two nanocrystal precursors; heating the first solution to a nucleation temperature; adding to the first solution, a second solution having a solvent, at least one additional and different precursor to form the homogeneous center region and at most an initial portion of the smoothly varying region; and lowering the solution temperature to a growth temperature to complete growth of the smoothly varying region.

  14. Zirconia nanocrystals as submicron level biological label

    NASA Astrophysics Data System (ADS)

    Smits, K.; Liepins, J.; Gavare, M.; Patmalnieks, A.; Gruduls, A.; Jankovica, D.

    2012-08-01

    Inorganic nanocrystals are of increasing interest for their usage in biology and pharmacology research. Our interest was to justify ZrO2 nanocrystal usage as submicron level biological label in baker's yeast Saccharomyces cerevisia culture. For the first time (to our knowledge) images with sub micro up-conversion luminescent particles in biologic media were made. A set of undoped as well as Er and Yb doped ZrO2 samples at different concentrations were prepared by sol-gel method. The up-conversion luminescence for free standing and for nanocrystals with baker's yeast cells was studied and the differences in up-conversion luminescence spectra were analyzed. In vivo toxic effects of ZrO2 nanocrystals were tested by co-cultivation with baker's yeast.

  15. Tunable plasmonic lattices of silver nanocrystals

    NASA Astrophysics Data System (ADS)

    Tao, Andrea; Sinsermsuksakul, Prasert; Yang, Peidong

    2007-07-01

    Silver nanocrystals are ideal building blocks for plasmonic materials that exhibit a wide range of unique and potentially useful optical phenomena. Individual nanocrystals display distinct optical scattering spectra and can be assembled into hierarchical structures that couple strongly to external electromagnetic fields. This coupling, which is mediated by surface plasmons, depends on the shape and arrangement of the nanocrystals. Here we demonstrate the bottom-up assembly of polyhedral silver nanocrystals into macroscopic two-dimensional superlattices using the Langmuir-Blodgett technique. Our ability to control interparticle spacing, density and packing symmetry allows for tunability of the optical response over the entire visible range. This assembly strategy offers a new, practical approach to making novel plasmonic materials for application in spectroscopic sensors, subwavelength optics and integrated devices that utilize field-enhancement effects.

  16. Tunable plasmonic lattices of silver nanocrystals.

    PubMed

    Tao, Andrea; Sinsermsuksakul, Prasert; Yang, Peidong

    2007-07-01

    Silver nanocrystals are ideal building blocks for plasmonic materials that exhibit a wide range of unique and potentially useful optical phenomena. Individual nanocrystals display distinct optical scattering spectra and can be assembled into hierarchical structures that couple strongly to external electromagnetic fields. This coupling, which is mediated by surface plasmons, depends on the shape and arrangement of the nanocrystals. Here we demonstrate the bottom-up assembly of polyhedral silver nanocrystals into macroscopic two-dimensional superlattices using the Langmuir-Blodgett technique. Our ability to control interparticle spacing, density and packing symmetry allows for tunability of the optical response over the entire visible range. This assembly strategy offers a new, practical approach to making novel plasmonic materials for application in spectroscopic sensors, subwavelength optics and integrated devices that utilize field-enhancement effects.

  17. Tunable mid IR plasmon in GZO nanocrystals.

    PubMed

    Hamza, M K; Bluet, J-M; Masenelli-Varlot, K; Canut, B; Boisron, O; Melinon, P; Masenelli, B

    2015-07-28

    Degenerate metal oxide nanoparticles are promising systems to expand the significant achievements of plasmonics into the infrared (IR) range. Among the possible candidates, Ga-doped ZnO nanocrystals are particularly suited for mid IR, considering their wide range of possible doping levels and thus of plasmon tuning. In the present work, we report on the tunable mid IR plasmon induced in degenerate Ga-doped ZnO nanocrystals. The nanocrystals are produced by a plasma expansion and exhibit unprotected surfaces. Tuning the Ga concentration allows tuning the localized surface plasmon resonance. Moreover, the plasmon resonance is characterized by a large damping. By comparing the plasmon of nanocrystal assemblies to that of nanoparticles dispersed in an alumina matrix, we investigate the possible origins of such damping. We demonstrate that it partially results from the self-organization of the naked particles and also from intrinsic inhomogeneity of dopants.

  18. Lifetime blinking in nonblinking nanocrystal quantum dots

    NASA Astrophysics Data System (ADS)

    Galland, Christophe; Ghosh, Yagnaseni; Steinbrück, Andrea; Hollingsworth, Jennifer A.; Htoon, Han; Klimov, Victor I.

    2012-06-01

    Nanocrystal quantum dots are attractive materials for applications as nanoscale light sources. One impediment to these applications is fluctuations of single-dot emission intensity, known as blinking. Recent progress in colloidal synthesis has produced nonblinking nanocrystals; however, the physics underlying blinking suppression remains unclear. Here we find that ultra-thick-shell CdSe/CdS nanocrystals can exhibit pronounced fluctuations in the emission lifetimes (lifetime blinking), despite stable nonblinking emission intensity. We demonstrate that lifetime variations are due to switching between the neutral and negatively charged state of the nanocrystal. Negative charging results in faster radiative decay but does not appreciably change the overall emission intensity because of suppressed nonradiative Auger recombination for negative trions. The Auger process involving excitation of a hole (positive trion pathway) remains efficient and is responsible for charging with excess electrons, which occurs via Auger-assisted ionization of biexcitons accompanied by ejection of holes.

  19. Lifetime blinking in nonblinking nanocrystal quantum dots.

    PubMed

    Galland, Christophe; Ghosh, Yagnaseni; Steinbrück, Andrea; Hollingsworth, Jennifer A; Htoon, Han; Klimov, Victor I

    2012-06-19

    Nanocrystal quantum dots are attractive materials for applications as nanoscale light sources. One impediment to these applications is fluctuations of single-dot emission intensity, known as blinking. Recent progress in colloidal synthesis has produced nonblinking nanocrystals; however, the physics underlying blinking suppression remains unclear. Here we find that ultra-thick-shell CdSe/CdS nanocrystals can exhibit pronounced fluctuations in the emission lifetimes (lifetime blinking), despite stable nonblinking emission intensity. We demonstrate that lifetime variations are due to switching between the neutral and negatively charged state of the nanocrystal. Negative charging results in faster radiative decay but does not appreciably change the overall emission intensity because of suppressed nonradiative Auger recombination for negative trions. The Auger process involving excitation of a hole (positive trion pathway) remains efficient and is responsible for charging with excess electrons, which occurs via Auger-assisted ionization of biexcitons accompanied by ejection of holes.

  20. Gas phase grown silicon germanium nanocrystals

    NASA Astrophysics Data System (ADS)

    Mohan, A.; Tichelaar, F. D.; Kaiser, M.; Verheijen, M. A.; Schropp, R. E. I.; Rath, J. K.

    2016-09-01

    We report on the gas phase synthesis of highly crystalline and homogeneously alloyed Si1-xGex nanocrystals in continuous and pulsed plasmas. Agglomerated nanocrystals have been produced with remarkable control over their composition by altering the precursor GeH4 gas flow in a continuous plasma. We specially highlight that in the pulsed plasma mode, we obtain quantum-sized free standing alloy nanocrystals with a mean size of 7.3 nm. The presence of Si1-xGex alloy particles is confirmed with multiple techniques, i.e. Raman spectroscopy, XRD (Xray diffraction) and HRTEM (high resolution transmission electron microscopy) studies, with each of these methods consistently yielding the same composition. The nanocrystals synthesized here have potential applications in band-gap engineering for multijunction solar cells.

  1. Structure and performance of dielectric films based on self-assembled nanocrystals with a high dielectric constant

    SciTech Connect

    Huang, LM; Liu, SY; Van Tassell, BJ; Liu, XH; Byro, A; Zhang, HN; Leland, ES; Akins, DL; Steingart, DA; Li, J; O'Brien, S

    2013-09-24

    Self-assembled films built from nanoparticles with a high dielectric constant are attractive as a foundation for new dielectric media with increased efficiency and range of operation, due to the ability to exploit nanofabrication techniques and emergent electrical properties originating from the nanoscale. However, because the building block is a discrete one-dimensional unit, it becomes a challenge to capture potential enhancements in dielectric performance in two or three dimensions, frequently due to surface effects or the presence of discontinuities. This is a recurring theme in nanoparticle film technology when applied to the realm of thin film semiconductor and device electronics. We present the use of chemically synthesized. (Ba; Sr)TiO3 nanocrystals, and a novel deposition-polymerization technique, as a means to fabricate the dielectric layer. The effective dielectric constant of the film is tunable according to nanoparticle size, and effective film dielectric constants of up to 34 are enabled. Wide area and multilayer dielectrics of up to 8 cm(2) and 190 nF are reported, for which the building block is an 8 nm nanocrystal. We describe models for assessing dielectric performance, and distinct methods for improving the dielectric constant of a nanocrystal thin film. The approach relies on evaporatively driven assembly of perovskite nanocrystals with uniform size distributions in a tunable 7-30 nm size range, coupled with the use of low molecular weight monomer/polymer precursor chemistry that can infiltrate the porous nanocrystal thin film network post assembly. The intercrystal void space (low k dielectric volume fraction) is minimized, while simultaneously promoting intercrystal connectivity and maximizing volume fraction of the high k dielectric component. Furfuryl alcohol, which has good affinity to the surface of. (Ba; Sr ) TiO3 nanocrystals and miscibility with a range of solvents, is demonstrated

  2. Tailorable, Visible Light Emission From Silicon Nanocrystals

    SciTech Connect

    Samara, G.A.; Wilcoxon, J.P.

    1999-07-20

    J. P. Wilcoxon and G. A. Samara Crystalline, size-selected Si nanocrystals in the size range 1.8-10 nm grown in inverse micellar cages exhibit highly structured optical absorption and photoluminescence (PL) across the visible range of the spectrum. The most intense PL for the smallest nanocrystals produced This report was prepared as an account of work sponsored by an agency of the United States Government. Neither the United States Government nor any agency thereof, nor any of their employees, make any warranty, express or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof. to induce a useful level of visible photoluminescence (PL) from silicon (Si). The approaches understood. Visible PL has been observed from Si nanocrystals, or quantum dots, produced by a variety of techniques including aerosols,2 colloids,3 and ion implantation.4 However, all of The optical absorption spectra of our nanocrystals are much richer in spectral features spectrum of bulk Si where the spectral features reflect the details of the band structure shown in nanocrystals estimated to have a Si core diameter of 1-2 nm. These measured quantum those in the spectrum of bulk Si in Fig. 1 are striking indicating that nanocrystals of this size 8-Room temperature PL results on an HPLC size-selected, purified 2 nm nanocrystals but blue shifted by -0.4 eV due to quantum confinement. Excitation at 245 nm yields

  3. 3D Assembly of All-Inorganic Colloidal Nanocrystals into Gels and Aerogels.

    PubMed

    Sayevich, Vladimir; Cai, Bin; Benad, Albrecht; Haubold, Danny; Sonntag, Luisa; Gaponik, Nikolai; Lesnyak, Vladimir; Eychmüller, Alexander

    2016-05-17

    We report an efficient approach to assemble a variety of electrostatically stabilized all-inorganic semiconductor nanocrystals (NCs) by their linking with appropriate ions into multibranched gel networks. These all-inorganic non-ordered 3D assemblies benefit from strong interparticle coupling, which facilitates charge transport between the NCs with diverse morphologies, compositions, sizes, and functional capping ligands. Moreover, the resulting dry gels (aerogels) are highly porous monolithic structures, which preserve the quantum confinement of their building blocks. The inorganic semiconductor aerogel made of 4.5 nm CdSe colloidal NCs capped with I(-) ions and bridged with Cd(2+) ions had a large surface area of 146 m(2)  g(-1) . PMID:27100131

  4. Optical refrigeration of Yb3+:YAG nanocrystals

    NASA Astrophysics Data System (ADS)

    Nemova, Galina; Kashyap, Raman

    2015-03-01

    We have theoretically investigated the laser cooling process in Yb3+:YAG nanocrystals. We have developed an approach, which permits not only estimate the cooling process in Yb3+:YAG nanocrystals but compare this process with the laser cooling of the Yb3+:YAG bulk samples. The temperature dependences of all parameters of the system are taken into account. The cooperative effects such as re-absorption, the energy migration and cooperative luminescence have been considered.

  5. Nanocrystal coated beads for optical coding and whispering gallery modes

    NASA Astrophysics Data System (ADS)

    Allen, Claudine Nì; Lequeux, Nicolas; Chassenieux, Christophe; Cyr, Guillaume; Tessier, Gilles; Dubertret, Benoit

    2007-06-01

    Semiconductor quantum dot nanocrystals (QDs) have unique optical properties such as size tunable photoluminescence (PL) wavelength and a chemically functionalized sufrace. Our CdSe/ZnS quantum dot nanocrystals have been made water-soluble by encapsulation in a micelle of positively charged amphiphilic copolymers. Layer-by-layer deposition of these QDs was done on sub-micrometer silica beads as well as magnetic and polymeric micro-sized beads. The negative surface charge of these various beads allowed successive stacking of cationic polyethylnimine, anionic polyacrylic acid sodium salt and the cationic encapsulated QDs. Multiple QD layers can be added by repeating the stacking process. The PL spectral of green QDs is moduoated by whispering galley mode resonances when the QDs arecoating a singe 3 μm bead. Depending on the quality factor of this microsphere, it can also be possible to detect perturbations caused by sufficient adsorption of biomolecules or even living microorganisms on a bead's surface by observing spectral shifts of the resonances. If different colorsof QDs are used to coat smaller beads where the modes are not spectrally resolved, an optical coating system can be devised base on the relative emission intensity for each color. The uniformity of a bead ensemble coded with 2 QD colors has been invesetigated, revealing a ~20% relataive standard deviation for various intensity levels. Better control of photobleaching through QD passivation reduced this number to ~8%, which would allow us to differentiate up to 2.6x10 10 optical codes on our setup. Labelling large amount of molecules in solution, e.g. DNA sequences, then becomes possible with an appropriate biofunctionalization of bead surfaces.

  6. 25th anniversary article: Ion exchange in colloidal nanocrystals.

    PubMed

    Gupta, Shuchi; Kershaw, Stephen V; Rogach, Andrey L

    2013-12-23

    We review the progress in ion exchange in a variety of nanocrystal structures from the earliest accounts dating back over two decades ago to the present day. In recent years the number of groups using this method to form otherwise difficult or inaccessible nanoparticle shapes and morphologies has increased considerably and the field has experienced a resurgence of interest. Whilst most of the early work on cation exchange centered on II-VI materials, the methodology has been expanded to cover a far broader range of semiconductor nanocrystals including low toxicity I-III-VI materials and the much less facile III-V materials. The extent of exchange can be controlled leading to lightly doped nanoparticles, alloys, core-shells, segmented rods and dots-in-rods. Progress has been driven by a better understanding of the underlying principles of the exchange process - from thermodynamic factors (differences in cation solubilities); the interactions between ions and transfer agents (solvents, ligands, anions, co-dopants); ionic in-diffusion mechanisms and kinetics. More recent availability of very detailed electron microscopy coupled with image reconstruction techniques has been a valuable tool to investigate the resulting heterostructures and internal interfaces. We start by surveying the range of synthetic approaches most often used to carry out ion exchange, mainly focusing on cation replacement strategies, and then describe the rich variety of nanostructures these techniques can bring forth. We also describe some of the principles that are used to establish the relative ease of exchange and to systematically improve the process where the basic energetics are less favorable. To help further the understanding of the underlying fundamentals we have gathered together useful data from the literature on solubilities, cation and anion hardness, ligand and solvent Lewis acid or base strengths for a wide range of chemical species generally used. We offer a perspective on the

  7. Synthesis of semiconductor nanoparticles.

    PubMed

    Chen, Xianfeng; Dobson, Peter J

    2012-01-01

    Here, we describe typical methods and provide detailed experimental protocols for synthesizing and processing various semiconductor nanoparticles which have potential application in biology and medicine. These include synthesis of binary semiconductor nanoparticles; core@shell nanoparticles and alloyed nanoparticles; size-selective precipitation to obtain monodisperse nanoparticles; and strategies for phase transfer of nanoparticles from organic solution to aqueous media. PMID:22791427

  8. A luminescent nanocrystal stress gauge

    SciTech Connect

    Choi, Charina; Koski, Kristie; Olson, Andrew; Alivisatos, Paul

    2010-10-25

    Microscale mechanical forces can determine important outcomes ranging from the site of material fracture to stem cell fate. However, local stresses in a vast majority of systems cannot be measured due to the limitations of current techniques. In this work, we present the design and implementation of the CdSe/CdS core/shell tetrapod nanocrystal, a local stress sensor with bright luminescence readout. We calibrate the tetrapod luminescence response to stress, and use the luminescence signal to report the spatial distribution of local stresses in single polyester fibers under uniaxial strain. The bright stress-dependent emission of the tetrapod, its nanoscale size, and its colloidal nature provide a unique tool that may be incorporated into a variety of micromechanical systems including materials and biological samples to quantify local stresses with high spatial resolution.

  9. Polyimide Cellulose Nanocrystal Composite Aerogels

    NASA Technical Reports Server (NTRS)

    Nguyen, Baochau N.; Meador, Mary Ann; Rowan, Stuart; Cudjoe, Elvis; Sandberg, Anna

    2014-01-01

    Polyimide (PI) aerogels are highly porous solids having low density, high porosity and low thermal conductivity with good mechanical properties. They are ideal for various applications including use in antenna and insulation such as inflatable decelerators used in entry, decent and landing operations. Recently, attention has been focused on stimuli responsive materials such as cellulose nano crystals (CNCs). CNCs are environmentally friendly, bio-renewable, commonly found in plants and the dermis of sea tunicates, and potentially low cost. This study is to examine the effects of CNC on the polyimide aerogels. The CNC used in this project are extracted from mantle of a sea creature called tunicates. A series of polyimide cellulose nanocrystal composite aerogels has been fabricated having 0-13 wt of CNC. Results will be discussed.

  10. Solution synthesis of germanium nanocrystals

    DOEpatents

    Gerung, Henry; Boyle, Timothy J.; Bunge, Scott D.

    2009-09-22

    A method for providing a route for the synthesis of a Ge(0) nanometer-sized material from. A Ge(II) precursor is dissolved in a ligand heated to a temperature, generally between approximately 100.degree. C. and 400.degree. C., sufficient to thermally reduce the Ge(II) to Ge(0), where the ligand is a compound that can bond to the surface of the germanium nanomaterials to subsequently prevent agglomeration of the nanomaterials. The ligand encapsulates the surface of the Ge(0) material to prevent agglomeration. The resulting solution is cooled for handling, with the cooling characteristics useful in controlling the size and size distribution of the Ge(0) materials. The characteristics of the Ge(II) precursor determine whether the Ge(0) materials that result will be nanocrystals or nanowires.

  11. Symmetry-Defying Iron Pyrite (FeS2) Nanocrystals through Oriented Attachment

    PubMed Central

    Gong, Maogang; Kirkeminde, Alec; Ren, Shenqiang

    2013-01-01

    Iron pyrite (fool's gold, FeS2) is a promising earth abundant and environmentally benign semiconductor material that shows promise as a strong and broad absorber for photovoltaics and high energy density cathode material for batteries. However, controlling FeS2 nanocrystal formation (composition, size, shape, stoichiometry, etc.) and defect mitigation still remains a challenge. These problems represent significant limitations in the ability to control electrical, optical and electrochemical properties to exploit pyrite's full potential for sustainable energy applications. Here, we report a symmetry-defying oriented attachment FeS2 nanocrystal growth by examining the nanostructure evolution and recrystallization to uncover how the shape, size and defects of FeS2 nanocrystals changes during growth. It is demonstrated that a well-controlled reaction temperature and annealing time results in polycrystal-to-monocrystal formation and defect annihilation, which correlates with the performance of photoresponse devices. This knowledge opens up a new tactic to address pyrite's known defect problems. PMID:23807691

  12. Photonic effects on the radiative decay rate and luminescence quantum yield of doped nanocrystals.

    PubMed

    Senden, Tim; Rabouw, Freddy T; Meijerink, Andries

    2015-02-24

    Nanocrystals (NCs) doped with luminescent ions form an emerging class of materials. In contrast to excitonic transitions in semiconductor NCs, the optical transitions are localized and not affected by quantum confinement. The radiative decay rates of the dopant emission in NCs are nevertheless different from their bulk analogues due to photonic effects, and also the luminescence quantum yield (QY, important for applications) is affected. In the past, different theoretical models have been proposed to describe the photonic effects for dopant emission in NCs, with little experimental validation. In this work we investigate the photonic effects on the radiative decay rate of luminescent doped NCs using 4 nm LaPO4 NCs doped with Ce(3+) or Tb(3+) ions in different refractive index solvents and bulk crystals. We demonstrate that the measured influence of the refractive index on the radiative decay rate of the Ce(3+) emission, having near unity QY, is in excellent agreement with the theoretical nanocrystal-cavity model. Furthermore, we show how the nanocrystal-cavity model can be used to quantify the nonunity QY of Tb(3+)-doped LaPO4 NCs and demonstrate that, as a general rule, the QY is higher in media with higher refractive index.

  13. Spin-dependent exciton quenching and spin coherence in CdSe/CdS nanocrystals.

    PubMed

    van Schooten, Kipp J; Huang, Jing; Baker, William J; Talapin, Dmitri V; Boehme, Christoph; Lupton, John M

    2013-01-01

    Large surface-to-volume ratios of semiconductor nanocrystals cause susceptibility to charge trapping, which can modify luminescence yields and induce single-particle blinking. Optical spectroscopies cannot differentiate between bulk and surface traps in contrast to spin-resonance techniques, which in principle avail chemical information on such trap sites. Magnetic resonance detection via spin-controlled photoluminescence enables the direct observation of interactions between emissive excitons and trapped charges. This approach allows the discrimination of three radical species located in two functionally different trap states in CdSe/CdS nanocrystals, underlying the fluorescence quenching and thus blinking mechanisms: a spin-dependent Auger process in charged particles; and a charge-separated state pair process, which leaves the particle neutral. The paramagnetic trap centers offer control of the energy transfer yield from the wide-gap CdS to the narrow-gap CdSe, that is, light harvesting within the heterostructure. Coherent spin motion within the trap states of the CdS arms of nanocrystal tetrapods is reflected by spatially remote luminescence from CdSe cores with surprisingly long coherence times of >300 ns at 3.5 K, illustrating coherent control of light harvesting. PMID:23189974

  14. Transport mechanisms and charge trapping in thin dielectric/Si nano-crystals structures

    NASA Astrophysics Data System (ADS)

    De Salvo, B.; Ghibaudo, G.; Luthereau, P.; Baron, T.; Guillaumot, B.; Reimbold, G.

    2001-08-01

    In this work the transport mechanisms and charge trapping of novel dielectric systems based on semiconductor nano-crystals embedded in a dielectric matrix are studied. In particular, stacked films composed of a thin bottom dielectric (2-4 nm thick SiO2 or Si3N4), with an embedded two-dimensional (2-D) array of Si nano-crystals (obtained by low pressure chemical vapor deposition or by annealing of silicon rich oxide) and a thick top dielectric (8 nm-thick SiO2) are investigated. Gate leakage currents, at medium/high electric fields, are examined at temperatures varying between 77 and 473 K. Charge trapping phenomena, occurring at low electric fields, are studied as a function of the stressing gate voltage and the stressing time. Experimental results are explained by means of an elastic tunneling model, which takes into account the main structural characteristics of the Si-dots (size dispersion, density, spatial distribution) as well as the effect of trapped charges in the silicon nano-crystals.

  15. Physical preparation and optical properties of CuSbS2 nanocrystals by mechanical alloying process

    NASA Astrophysics Data System (ADS)

    Zhang, Huihui; Xu, Qishu; Tan, Guolong

    2016-08-01

    CuSbS2 nanocrystals have been synthesized through mechanical alloying Cu, Sb and S elemental powders for 40 hs. The optical spectrum of as-milled CuSbS2 nano-powders demonstrates a direct gap of 1.35 eV and an indirect gap of 0.36 eV, which are similar to that of silicon and reveals the evidence for the indirect semiconductor characterization of CuSbS2. Afterwards, CuSbS2 nanocrystals were capped with trioctylphosphine oxide/trioctylphosphine/pyridine (TOPO/TOP). There appear four sharp absorption peaks within the region of 315 to 355 nm for the dispersion solution containing the capped nanocrystals. The multiple peaks are proposed to be originating from the energy level splitting of 1S electronic state into four discrete sub-levels, where electrons were excited into the conduction band and thus four exciton absorption peaks were produced. [Figure not available: see fulltext.

  16. Photoluminescence of CuInS2 nanocrystals: effect of surface modification

    NASA Astrophysics Data System (ADS)

    Kim, Young-Kuk; Cho, Young-Sang; Chung, Kookchae; Choi, Chul-Jin

    2011-09-01

    We have synthesized highly luminescent Cu-In-S(CIS) nanocrystals (NCs) by heating the mixture of metal carboxylates and alkylthiol under inert atmosphere. We modified the surface of CIS NCs with zinc carboxylate and subsequent injection of alkylthiol. As a result of the surface modification, highly luminescent CIS@ZnS core/shell nanocrystals were synthesized. The luminescence quantum yield (QY) of best CIS@ZnS NCs was above 50%, which is 10 times higher than the initial QY of CIS NCs before surface modification (QY=3%). Detailed study on the luminescence mechanism implies that etching of the surface of NCs by dissociated carboxylate group (CH3COO-) and formation of epitaxial shell by Zn with sulfur from alkylthiol efficiently removed the surface defects which are known to be major non-radiative recombination sites in semiconductor nanocrystals. In this study, we developed a novel surface modification route for monodispersed highly luminescent Cu-In-S NCs with less toxic and highly stable precursors. Investigation with the timeand the temperature-dependent photoluminescence showed that the trap related emission was minimized by surface modification and the donor-acceptor pair recombination was enhanced by controlling copper stoichiometry.xb

  17. Enhanced Charge Separation in Ternary P3HT/PCBM/CuInS2 Nanocrystals Hybrid Solar Cells

    PubMed Central

    Lefrançois, Aurélie; Luszczynska, Beata; Pepin-Donat, Brigitte; Lombard, Christian; Bouthinon, Benjamin; Verilhac, Jean-Marie; Gromova, Marina; Faure-Vincent, Jérôme; Pouget, Stéphanie; Chandezon, Frédéric; Sadki, Saïd; Reiss, Peter

    2015-01-01

    Geminate recombination of bound polaron pairs at the donor/acceptor interface is one of the major loss mechanisms in organic bulk heterojunction solar cells. One way to overcome Coulomb attraction between opposite charge carriers and to achieve their full dissociation is the introduction of high dielectric permittivity materials such as nanoparticles of narrow band gap semiconductors. We selected CuInS2 nanocrystals of 7.4 nm size, which present intermediate energy levels with respect to poly(3-hexylthiophene) (P3HT) and Phenyl-C61-butyric acid methyl ester (PCBM). Efficient charge transfer from P3HT to nanocrystals takes place as evidenced by light-induced electron spin resonance. Charge transfer between nanocrystals and PCBM only occurs after replacing bulky dodecanethiol (DDT) surface ligands with shorter 1,2-ethylhexanethiol (EHT) ligands. Solar cells containing in the active layer a ternary blend of P3HT:PCBM:CuInS2-EHT nanocrystals in 1:1:0.5 mass ratio show strongly improved short circuit current density and a higher fill factor with respect to the P3HT:PCBM reference device. Complementary measurements of the absorption properties, external quantum efficiency and charge carrier mobility indicate that enhanced charge separation in the ternary blend is at the origin of the observed behavior. The same trend is observed for blends using the glassy polymer poly(triarylamine) (PTAA). PMID:25588811

  18. A facile strategy to decorate Cu9S5 nanocrystals on polyaniline nanowires and their synergetic catalytic properties

    PubMed Central

    Lu, Xiao-feng; Bian, Xiu-jie; Li, Zhi-cheng; Chao, Dan-ming; Wang, Ce

    2013-01-01

    Here, we demonstrated a novel method to decorate Cu9S5 nanocrystals on polyaniline (PANI) nanowires using the dopant of mercaptoacetic acid (MAA) in the PANI matrix as the sulfur source under a hydrothermal reaction. TEM images showed that Cu9S5 nanocrystals with a size in the range of 5–20 nm were uniformly formed on the surface of PANI nanowires. Significantly, the as-prepared PANI/Cu9S5 composite nanowires have been proven to be novel peroxidase mimics toward the oxidation of the peroxidase substrate 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2. Due to the synergetic effects between polyaniline nanowires and Cu9S5 nanocrystals, the obtained PANI/Cu9S5 composite nanowires exhibit superior catalytic activity over the independent components. This work not only presents a simple and versatile method to decorate semiconductor nanocrystals on the surface of conducting polymer nanostructures, but also provides fundamental guidelines for further investigations into the synergetic effect between conducting polymers and other materials. PMID:24129741

  19. Enhanced Charge Separation in Ternary P3HT/PCBM/CuInS2 Nanocrystals Hybrid Solar Cells

    NASA Astrophysics Data System (ADS)

    Lefrançois, Aurélie; Luszczynska, Beata; Pepin-Donat, Brigitte; Lombard, Christian; Bouthinon, Benjamin; Verilhac, Jean-Marie; Gromova, Marina; Faure-Vincent, Jérôme; Pouget, Stéphanie; Chandezon, Frédéric; Sadki, Saïd; Reiss, Peter

    2015-01-01

    Geminate recombination of bound polaron pairs at the donor/acceptor interface is one of the major loss mechanisms in organic bulk heterojunction solar cells. One way to overcome Coulomb attraction between opposite charge carriers and to achieve their full dissociation is the introduction of high dielectric permittivity materials such as nanoparticles of narrow band gap semiconductors. We selected CuInS2 nanocrystals of 7.4 nm size, which present intermediate energy levels with respect to poly(3-hexylthiophene) (P3HT) and Phenyl-C61-butyric acid methyl ester (PCBM). Efficient charge transfer from P3HT to nanocrystals takes place as evidenced by light-induced electron spin resonance. Charge transfer between nanocrystals and PCBM only occurs after replacing bulky dodecanethiol (DDT) surface ligands with shorter 1,2-ethylhexanethiol (EHT) ligands. Solar cells containing in the active layer a ternary blend of P3HT:PCBM:CuInS2-EHT nanocrystals in 1:1:0.5 mass ratio show strongly improved short circuit current density and a higher fill factor with respect to the P3HT:PCBM reference device. Complementary measurements of the absorption properties, external quantum efficiency and charge carrier mobility indicate that enhanced charge separation in the ternary blend is at the origin of the observed behavior. The same trend is observed for blends using the glassy polymer poly(triarylamine) (PTAA).

  20. A facile strategy to decorate Cu9S5 nanocrystals on polyaniline nanowires and their synergetic catalytic properties

    NASA Astrophysics Data System (ADS)

    Lu, Xiao-Feng; Bian, Xiu-Jie; Li, Zhi-Cheng; Chao, Dan-Ming; Wang, Ce

    2013-10-01

    Here, we demonstrated a novel method to decorate Cu9S5 nanocrystals on polyaniline (PANI) nanowires using the dopant of mercaptoacetic acid (MAA) in the PANI matrix as the sulfur source under a hydrothermal reaction. TEM images showed that Cu9S5 nanocrystals with a size in the range of 5-20 nm were uniformly formed on the surface of PANI nanowires. Significantly, the as-prepared PANI/Cu9S5 composite nanowires have been proven to be novel peroxidase mimics toward the oxidation of the peroxidase substrate 3,3',5,5'-tetramethylbenzidine (TMB) in the presence of H2O2. Due to the synergetic effects between polyaniline nanowires and Cu9S5 nanocrystals, the obtained PANI/Cu9S5 composite nanowires exhibit superior catalytic activity over the independent components. This work not only presents a simple and versatile method to decorate semiconductor nanocrystals on the surface of conducting polymer nanostructures, but also provides fundamental guidelines for further investigations into the synergetic effect between conducting polymers and other materials.

  1. Germanium nanocrystals: Synthesis, characterization, and applications

    NASA Astrophysics Data System (ADS)

    Gerung, Henry

    The aim of this work was to demonstrate a simple synthesis route of Ge nanostructures (nanoparticles and nanowires), to characterize the physical and optical properties of Ge nanocrystal, and to demonstrate their biological and optoelectronics applications. The appropriate organometallic Ge 2+ precursors for the synthesis of Ge nanocrystals were identified. These precursors were used to develop a simple route that produced high quality Ge nanocrystals in high yield under mild conditions without using potentially contaminating catalysts and forming byproducts. The particle size was varied from 1 to 10 nm, depending on the reaction parameters. The relatively low-temperature, low-pressure nanocrystal synthesis condition allowed the use of organic solvents and surfactants. We also demonstrated morphological control over Ge nanocrystals via Ge2+ precursor reactivity modification. During synthesis, the surfactants passivate the nanocrystal surface and minimize surface oxidation. This synthesis method allowed optical characterization of Ge nanocrystals decoupled from contamination and oxidation. When excited with photons, Ge nanoparticles exhibit quantum confinement effect in both infrared and ultraviolet regions, as well as optical nonlinearity by the presence of two-photon absorption. These free-standing Ge nanocrystals could be further become integral elements in various optoelectronic devices. Herein, the production of water-soluble Ge nanoparticles was demonstrated as a proof of the effectiveness of our synthesis method. Addition of secondary layer surfactants such as cationic cetyltrimethylammonium bromide (CTAB) or functionalized polyethylene glycol (PEG), transforms the Ge nanoparticles to become water-soluble. The biocompatible, functionalized, water-soluble Ge nanoparticles were bound to extracellular receptors and also incorporated into the cells as a proof-of-concept demonstration for potential biomarker applications. In expectation of forming a 3-D

  2. 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.

  3. Tunable surface plasmon resonance and enhanced electrical conductivity of In doped ZnO colloidal nanocrystals

    NASA Astrophysics Data System (ADS)

    Ghosh, Sirshendu; Saha, Manas; de, S. K.

    2014-05-01

    We report a new synthesis process of colloidal indium (In) doped zinc oxide (ZIO) nanocrystals by a hot injection technique. By fine tuning the synthesis we reached the same nucleation temperature for indium oxide and zinc oxide which helped us to study a dopant precursor dependent In incorporation into the ZnO matrix by using different In sources. The dopant induced shape evolution changes the hexagonal pyramid structured ZnO to a platelet like structure upon 8% In doping. The introduction of trivalent In3+ into the ZnO lattice and consequent substitution of divalent Zn2+ generates free electrons in the conduction band which produces a plasmonic resonance in the infrared region. The electron concentration controls plasmon frequency as well as the band gap of host ZnO. The variation of the band gap and the modification of the conduction band have been explained by the Burstein-Moss effect and Mie's theory respectively. The In dopant changes the defect chemistry of pure ZnO nanocrystals which has been studied by photoluminescence and other spectroscopic measurements. The nanocrystals are highly stable in the organic medium and can be deposited as a crack free thin film on different substrates. Careful ligand exchange and thermal annealing of the spin cast film lead to a good conductive film (720 Ω per square to 120 Ω per square) with stable inherent plasmonic absorption in the infrared and 90% transmittance in the visible region. A temperature induced metal-semiconductor transition was found for doped ZnO nanocrystals. The transition temperature shifts to a lower temperature with increase of the doping concentration.We report a new synthesis process of colloidal indium (In) doped zinc oxide (ZIO) nanocrystals by a hot injection technique. By fine tuning the synthesis we reached the same nucleation temperature for indium oxide and zinc oxide which helped us to study a dopant precursor dependent In incorporation into the ZnO matrix by using different In sources. The

  4. Tuning the surface oxygen concentration of {111} surrounded ceria nanocrystals for enhanced photocatalytic activities

    NASA Astrophysics Data System (ADS)

    Younis, Adnan; Chu, Dewei; Kaneti, Yusuf Valentino; Li, Sean

    2015-12-01

    For oxide semiconductors, the morphology, particle size and oxygen vacancies are usually considered as key influential parameters for photocatalytic degradation of organic pollutants/dyes. It is widely accepted that cation doping not only modifies their phase and microstructures but also introduces variations in oxygen vacancy concentration. Herein, we report the fabrication of sub-10 nm sized pure and indium doped CeO2 nanocrystals (NCs) via a facile, green hydrothermal method for the investigation of photocatalytic activities. X-ray diffraction and transmission electron microscopy were employed to examine the crystal phase and morphology of the as-prepared nanocrystals. Raman and X-ray photoelectron spectroscopy techniques were implemented to investigate the presence and variations in oxygen vacancy concentration in un-doped and indium doped CeO2 nanocrystals. The photocatalytic activity results revealed that 10 at% doping is the optimal indium doping level to demonstrate superior dye removal efficiency (~40%) over un-doped and doped CeO2 NCs. Moreover, the 10% In-doped CeO2 nanocrystals expressed excellent cycling stability and superior photocatalytic performance toward other dye pollutants. Finally, on the basis of our findings, a possible photocatalytic mechanism in which indium doping can generate more surface oxygen vacancies in the ceria lattice which delay the electron-hole recombination rates, thus increasing the lifetime of electron-hole separation for enhanced photocatalytic performances was proposed.For oxide semiconductors, the morphology, particle size and oxygen vacancies are usually considered as key influential parameters for photocatalytic degradation of organic pollutants/dyes. It is widely accepted that cation doping not only modifies their phase and microstructures but also introduces variations in oxygen vacancy concentration. Herein, we report the fabrication of sub-10 nm sized pure and indium doped CeO2 nanocrystals (NCs) via a facile

  5. Enhanced ferroelectric-nanocrystal-based hybrid photocatalysis by ultrasonic-wave-generated piezophototronic effect.

    PubMed

    Li, Haidong; Sang, Yuanhua; Chang, Sujie; Huang, Xin; Zhang, Yan; Yang, Rusen; Jiang, Huaidong; Liu, Hong; Wang, Zhong Lin

    2015-04-01

    An electric field built inside a crystal was proposed to enhance photoinduced carrier separation for improving photocatalytic property of semiconductor photocatalysts. However, a static built-in electric field can easily be saturated by the free carriers due to electrostatic screening, and the enhancement of photocatalysis, thus, is halted. To overcome this problem, here, we propose sonophotocatalysis based on a new hybrid photocatalyst, which combines ferroelectric nanocrystals (BaTiO3) and semiconductor nanoparticles (Ag2O) to form an Ag2O-BaTiO3 hybrid photocatalyst. Under periodic ultrasonic excitation, a spontaneous polarization potential of BaTiO3 nanocrystals in responding to ultrasonic wave can act as alternating built-in electric field to separate photoinduced carriers incessantly, which can significantly enhance the photocatalytic activity and cyclic performance of the Ag2O-BaTiO3 hybrid structure. The piezoelectric effect combined with photoelectric conversion realizes an ultrasonic-wave-driven piezophototronic process in the hybrid photocatalyst, which is the fundamental of sonophotocatalysis.

  6. Controlled synthesis of hyper-branched inorganic nanocrystals withrich three-dimensional structures

    SciTech Connect

    Kanaras, Antonios G.; Sonnichsen, Carsten; Liu, Haitao; Alivisatos, A. Paul

    2005-07-27

    Studies of crystal growth kinetics are tightly integrated with advances in the creation of new nanoscale inorganic building blocks and their functional assemblies 1-11. Recent examples include the development of semiconductor nanorods which have potential uses in solar cells 12-17, and the discovery of a light driven process to create noble metal particles with sharp corners that can be used in plasmonics 18,19. In the course of studying basic crystal growth kinetics we developed a process for preparing branched semiconductor nanocrystals such as tetrapods and inorganic dendrimers of precisely controlled generation 20,21. Here we report the discovery of a crystal growth kinetics regime in which a new class of hyper-branched nanocrystals are formed. The shapes range from 'thorny balls', to tree-like ramified structures, to delicate 'spider net'-like particles. These intricate shapes depend crucially on a delicate balance of branching and extension. The multitudes of resulting shapes recall the diverse shapes of snowflakes 22.The three dimensional nature of the branch points here, however, lead to even more complex arrangements than the two dimensionally branched structures observed in ice. These hyper-branched particles not only extend the available three-dimensional shapes in nanoparticle synthesis ,but also provide a tool to study growth kinetics by carefully observing and modeling particle morphology.

  7. Enhanced ferroelectric-nanocrystal-based hybrid photocatalysis by ultrasonic-wave-generated piezophototronic effect.

    PubMed

    Li, Haidong; Sang, Yuanhua; Chang, Sujie; Huang, Xin; Zhang, Yan; Yang, Rusen; Jiang, Huaidong; Liu, Hong; Wang, Zhong Lin

    2015-04-01

    An electric field built inside a crystal was proposed to enhance photoinduced carrier separation for improving photocatalytic property of semiconductor photocatalysts. However, a static built-in electric field can easily be saturated by the free carriers due to electrostatic screening, and the enhancement of photocatalysis, thus, is halted. To overcome this problem, here, we propose sonophotocatalysis based on a new hybrid photocatalyst, which combines ferroelectric nanocrystals (BaTiO3) and semiconductor nanoparticles (Ag2O) to form an Ag2O-BaTiO3 hybrid photocatalyst. Under periodic ultrasonic excitation, a spontaneous polarization potential of BaTiO3 nanocrystals in responding to ultrasonic wave can act as alternating built-in electric field to separate photoinduced carriers incessantly, which can significantly enhance the photocatalytic activity and cyclic performance of the Ag2O-BaTiO3 hybrid structure. The piezoelectric effect combined with photoelectric conversion realizes an ultrasonic-wave-driven piezophototronic process in the hybrid photocatalyst, which is the fundamental of sonophotocatalysis. PMID:25803813

  8. Photodeposition of Pt on Colloidal CdS and CdSe/CdS Semiconductor Nanostructures

    SciTech Connect

    Dukovic, Gordana; Merkle, Maxwell G.; Nelson, James H.; Hughes, Steven M.; Alivisatos, A. Paul

    2008-08-06

    Semiconductor photocatalysis has been identified as a promising avenue for the conversion of solar energy into environmentally friendly fuels, most notably by the production of hydrogen from water.[1-5] Nanometer-scale materials in particular have attracted considerable scientific attention as the building blocks for light-harvesting applications.[6,7] Their desirable attributes include tunability of the optical properties with size, amenability to relatively inexpensive low-temperature processing, and a high degree of synthetic sophistication leading to increasingly complex and multi-functional architectures. For photocatalysis in particular, the high surface-to-volume ratios in nanoscale materials should lead to an increased availability of carriers for redox reactions on the nanoparticle surface. Recombination of photoexcited carriers directly competes with photocatalytic activity.[3] Charge separation is often achieved with multi-component heterostructures. An early example is the case of TiO2 powders functionalized with Pt and RuO2 particles, where photoexcited electrons are transferred to Pt (the reduction site) and holes to RuO2 (the oxidation site).[8] More recently, many colloidally synthesized nanometer-scale metal-semiconductor heterostructures have been reported.[7,9,10] A majority of these structures are made by thermal methods.[7,10] We have chosen to study photochemical formation of metal-semiconductor heterostructures. The detailed understanding of the mechanisms involved in photodeposition of metals on nanometer-scale semiconductors is necessary to enable a high degree of synthetic control. At the same time, because the results of metal deposition can be directly observed by electron microscopy, it can be used to understand how factors such as nanocrystal composition, shape, carrier dynamics, and surface chemistry influence the photochemical properties of semiconductor nanocrystals. In this communication, we report on the photodeposition of Pt on

  9. Nanocrystal Bioassembly: Asymmetry, Proximity, and Enzymatic Manipulation

    SciTech Connect

    Claridge, Shelley A.

    2008-05-01

    Research at the interface between biomolecules and inorganic nanocrystals has resulted in a great number of new discoveries. In part this arises from the synergistic duality of the system: biomolecules may act as self-assembly agents for organizing inorganic nanocrystals into functional materials; alternatively, nanocrystals may act as microscopic or spectroscopic labels for elucidating the behavior of complex biomolecular systems. However, success in either of these functions relies heavily uponthe ability to control the conjugation and assembly processes.In the work presented here, we first design a branched DNA scaffold which allows hybridization of DNA-nanocrystal monoconjugates to form discrete assemblies. Importantly, the asymmetry of the branched scaffold allows the formation of asymmetric2assemblies of nanocrystals. In the context of a self-assembled device, this can be considered a step toward the ability to engineer functionally distinct inputs and outputs.Next we develop an anion-exchange high performance liquid chromatography purification method which allows large gold nanocrystals attached to single strands of very short DNA to be purified. When two such complementary conjugates are hybridized, the large nanocrystals are brought into close proximity, allowing their plasmon resonances to couple. Such plasmon-coupled constructs are of interest both as optical interconnects for nanoscale devices and as `plasmon ruler? biomolecular probes.We then present an enzymatic ligation strategy for creating multi-nanoparticle building blocks for self-assembly. In constructing a nanoscale device, such a strategy would allow pre-assembly and purification of components; these constructs can also act as multi-label probes of single-stranded DNA conformational dynamics. Finally we demonstrate a simple proof-of-concept of a nanoparticle analog of the polymerase chain reaction.

  10. Semiconductor active plasmonics

    NASA Astrophysics Data System (ADS)

    Mendach, Stefan; Nötzel, Richard

    2013-12-01

    Plasmonics is a research area in nanophotonics attracting increasing interest due to the potential applications in sensing and detecting, sub-wavelength confinement of light, integrated circuits, and many others. In particular, when plasmonic structures such as metal nanostructures or highly doped semiconductor particles are combined with active semiconductor materials and nanostructures, novel exciting physics and applications arise. This special section on semiconductor active plasmonics covers several of the most important and complementary directions in the field. First is the modification of the optical properties of a semiconductor nanostructure due to the close proximity of a metallic film or nanostructure. These arise from the formation hybrid plasmon/exciton states and may lead to enhanced spontaneous emission rates, directional far field emission patterns, strong coupling phenomena, and many more. Second is the realization of sub-wavelength scale nanolasers by coupling a semiconductor gain medium with a plasmonic metallic cavity. Particular emphasis is given on the major technical challenges in the fabrication of these nanolasers, such as device patterning, surface passivation, and metal deposition. While the above topics address mainly active structures and devices operating in the visible or near-infrared wavelength region, in the third, the enhanced THz extinction by periodic arrays of semiconductor particles is discussed. This is based on the build-up of surface plasmon resonances in the doped semiconductor particles which can be resonantly coupled and widely tuned by the carrier density in the semiconductor. We believe these highly diverse aspects give insight into the wide variety of new physics and applications that semiconductor active plasmonics is offering. Finally, we would like to thank the IOP editorial staff, in particular Alice Malhador, for their support, and we would also like to thank the contributors for their efforts and participation

  11. Tunable surface plasmon resonance and enhanced electrical conductivity of In doped ZnO colloidal nanocrystals.

    PubMed

    Ghosh, Sirshendu; Saha, Manas; De, S K

    2014-06-21

    We report a new synthesis process of colloidal indium (In) doped zinc oxide (ZIO) nanocrystals by a hot injection technique. By fine tuning the synthesis we reached the same nucleation temperature for indium oxide and zinc oxide which helped us to study a dopant precursor dependent In incorporation into the ZnO matrix by using different In sources. The dopant induced shape evolution changes the hexagonal pyramid structured ZnO to a platelet like structure upon 8% In doping. The introduction of trivalent In(3+) into the ZnO lattice and consequent substitution of divalent Zn(2+) generates free electrons in the conduction band which produces a plasmonic resonance in the infrared region. The electron concentration controls plasmon frequency as well as the band gap of host ZnO. The variation of the band gap and the modification of the conduction band have been explained by the Burstein-Moss effect and Mie's theory respectively. The In dopant changes the defect chemistry of pure ZnO nanocrystals which has been studied by photoluminescence and other spectroscopic measurements. The nanocrystals are highly stable in the organic medium and can be deposited as a crack free thin film on different substrates. Careful ligand exchange and thermal annealing of the spin cast film lead to a good conductive film (720 Ω per square to 120 Ω per square) with stable inherent plasmonic absorption in the infrared and 90% transmittance in the visible region. A temperature induced metal-semiconductor transition was found for doped ZnO nanocrystals. The transition temperature shifts to a lower temperature with increase of the doping concentration. PMID:24842309

  12. Biomolecularly capped uniformly sized nanocrystalline materials: glutathione-capped ZnS nanocrystals

    NASA Astrophysics Data System (ADS)

    Torres-Martínez, Claudia L.; Nguyen, Liem; Kho, Richard; Bae, Weon; Bozhilov, Krassimir; Klimov, Victor; Mehra, Rajesh K.

    1999-09-01

    Micro-organisms such as bacteria and yeasts form CdS to detoxify toxic cadmium ions. Frequently, CdS particles formed in yeasts and bacteria were found to be associated with specific biomolecules. It was later determined that these biomolecules were present at the surface of CdS. This coating caused a restriction in the growth of CdS particles and resulted in the formation of nanometre-sized semiconductors (NCs) that exhibited typical quantum confinement properties. Glutathione and related phytochelatin peptides were shown to be the biomolecules that capped CdS nanocrystallites synthesized by yeasts Candida glabrata and Schizosaccharomyces pombe. Although early studies showed the existence of specific biochemical pathways for the synthesis of biomolecularly capped CdS NCs, these NCs could be formed in vitro under appropriate conditions. We have recently shown that cysteine and cysteine-containing peptides such as glutathione and phytochelatins can be used in vitro to dictate the formation of discrete sizes of CdS and ZnS nanocrystals. We have evolved protocols for the synthesis of ZnS or CdS nanocrystals within a narrow size distribution range. These procedures involve three steps: (1) formation of metallo-complexes of cysteine or cysteine-containing peptides, (2) introduction of stoichiometric amounts of inorganic sulfide into the metallo-complexes to initiate the formation of nanocrystallites and finally (3) size-selective precipitation of NCs with ethanol in the presence of Na+. The resulting NCs were characterized by optical spectroscopy, high-resolution transmission electron microscopy (HRTEM), x-ray diffraction and electron diffraction. HRTEM showed that the diameter of the ZnS-glutathione nanocrystals was 3.45+/-0.5 nm. X-ray diffraction and electron diffraction analyses indicated ZnS-glutathione to be hexagonal. Photocatalytic studies suggest that glutathione-capped ZnS nanocrystals prepared by our procedure are highly efficient in degrading a test model

  13. Introduction to Semiconductor Devices

    NASA Astrophysics Data System (ADS)

    Brennan, Kevin F.

    2005-03-01

    This volume offers a solid foundation for understanding the most important devices used in the hottest areas of electronic engineering today, from semiconductor fundamentals to state-of-the-art semiconductor devices in the telecommunications and computing industries. Kevin Brennan describes future approaches to computing hardware and RF power amplifiers, and explains how emerging trends and system demands of computing and telecommunications systems influence the choice, design and operation of semiconductor devices. In addition, he covers MODFETs and MOSFETs, short channel effects, and the challenges faced by continuing miniaturization. His book is both an excellent senior/graduate text and a valuable reference for practicing engineers and researchers.

  14. Metal halide solid-state surface treatment for nanocrystal materials

    DOEpatents

    Luther, Joseph M.; Crisp, Ryan; Beard, Matthew C.

    2016-04-26

    Methods of treating nanocrystal and/or quantum dot devices are described. The methods include contacting the nanocrystals and/or quantum dots with a solution including metal ions and halogen ions, such that the solution displaces native ligands present on the surface of the nanocrystals and/or quantum dots via ligand exchange.

  15. Diversity of sub-bandgap states in lead-sulfide nanocrystals: real-space spectroscopy and mapping at the atomic-scale.

    PubMed

    Gervasi, Christian F; Kislitsyn, Dmitry A; Allen, Thomas L; Hackley, Jason D; Maruyama, Ryuichiro; Nazin, George V

    2015-12-14

    Colloidal semiconductor nanocrystals have emerged as a promising class of technological materials with optoelectronic properties controllable through quantum-confinement effects. Despite recent successes in this field, an important factor that remains difficult to control is the impact of the nanocrystal surface structure on the photophysics and electron transport in nanocrystal-based materials. In particular, the presence of surface defects and irregularities can result in the formation of localized sub-bandgap states that can dramatically affect the dynamics of charge carriers and electronic excitations. Here we use Scanning Tunneling Spectroscopy (STS) to investigate, in real space, sub-bandgap states in individual ligand-free PbS nanocrystals. In the majority of studied PbS nanocrystals, spatial mapping of electronic density of states with STS shows atomic-scale variations attributable to the presence of surface reconstructions. STS spectra show that the presence of surface reconstructions results in formation of surface-bound sub-bandgap electronic states. The nature of the surface reconstruction varies depending on the surface stoichiometry, with lead-rich surfaces producing unoccupied sub-bandgap states, and sulfur-rich areas producing occupied sub-bandgap states. Highly off-stoichiometric areas produce both occupied and unoccupied states showing dramatically reduced bandgaps. Different reconstruction patterns associated with specific crystallographic directions are also found for different nanocrystals. This study provides insight into the mechanisms of sub-bandgap state formation that, in a modified form, are likely to be applicable to ligand-passivated nanocrystal surfaces, where steric hindrance between ligands can result in under-coordination of surface atoms.

  16. Multiple exciton generation in nano-crystals revisited: consistent calculation of the yield based on pump-probe spectroscopy.

    PubMed

    Karki, Khadga J; Ma, Fei; Zheng, Kaibo; Zidek, Karel; Mousa, Abdelrazek; Abdellah, Mohamed A; Messing, Maria E; Wallenberg, L Reine; Yartsev, Arkadi; Pullerits, Tõnu

    2013-01-01

    Multiple exciton generation (MEG) is a process in which more than one exciton is generated upon the absorption of a high energy photon, typically higher than two times the band gap, in semiconductor nanocrystals. It can be observed experimentally using time resolved spectroscopy such as the transient absorption measurements. Quantification of the MEG yield is usually done by assuming that the bi-exciton signal is twice the signal from a single exciton. Herein we show that this assumption is not always justified and may lead to significant errors in the estimated MEG yields. We develop a methodology to determine proper scaling factors to the signals from the transient absorption experiments. Using the methodology we find modest MEG yields in lead chalcogenide nanocrystals including the nanorods.

  17. Synthesis and surface modification of PbSe/PbS core shell nanocrystals for potential device applications

    NASA Astrophysics Data System (ADS)

    Xu, Jian; Cui, Dehu; Zhu, Ting; Paradee, Gary; Liang, Ziqi; Wang, Qing; Xu, Shengyong; Wang, Andrew Y.

    2006-11-01

    We report in this paper the growth of PbS shells over colloidal PbSe nanocrystal quantum dots (NQDs) with monolayer-precision. The technique of successive ion layer adsorption and reaction (SILAR) has been adapted to the growth of high-quality core-shell nanocrystals. The core-shell infrared NQDs were ligand-exchanged with short-chain octylamine, and the photoluminescence efficiency of the surface-engineered core-shell nanoparticles was substantially higher than that of the plain core structures undergoing the same surface processing, which reveals less ligand dependence and enhanced chemical robustness in the core-shell NQDs. The reported results open up the possibility of incorporating semiconductor infrared NQDs in the silicon matrix to develop all-inorganic light-emitting heterojunctions on silicon substrates.

  18. Optical properties of colloidal germanium nanocrystals

    SciTech Connect

    WILCOXON,JESS P.; PROVENCIO,PAULA P.; SAMARA,GEORGE A.

    2000-05-01

    Highly crystalline germanium (Ge) nanocrystals in the size range 2--10 nm were grown in inverse micelles and purified and size-separated by high pressure liquid chromatography with on-line optical and electrical diagnostics. The nanocrystals retain the diamond structure of bulk Ge down to at least 2.0 nm (containing about 150 Ge atoms). The background- and impurity-free extinction and photoluminescence (PL) spectra of these nanocrystals revealed rich structure which was interpreted in terms of the bandstructure of Ge shifted to higher energies by quantum confinement. The shifts ranged from {minus}0.1 eV to over 1 eV for the various transitions. PL in the range 350--700 nm was observed from nanocrystals 2--5 nm in size. The 2.0 nm nanocrystals yielded the most intense PL (at 420 nm) which is believed to be intrinsic and attributed to direct recombination at {Gamma}. Excitation at high energy (250 nm) populates most of the conduction bands resulting in competing recombination channels and the observed broad PL spectra.

  19. Isotopically controlled semiconductors

    SciTech Connect

    Haller, E.E.

    2004-11-15

    A review of recent research involving isotopically controlled semiconductors is presented. Studies with isotopically enriched semiconductor structures experienced a dramatic expansion at the end of the Cold War when significant quantities of enriched isotopes of elements forming semiconductors became available for worldwide collaborations. Isotopes of an element differ in nuclear mass, may have different nuclear spins and undergo different nuclear reactions. Among the latter, the capture of thermal neutrons which can lead to neutron transmutation doping, can be considered the most important one for semiconductors. Experimental and theoretical research exploiting the differences in all the properties has been conducted and will be illustrated with selected examples. Manuel Cardona, the longtime editor-in-chief of Solid State Communications has been and continues to be one of the major contributors to this field of solid state physics and it is a great pleasure to dedicate this review to him.

  20. SLM based semiconductor maskwriter

    NASA Astrophysics Data System (ADS)

    Diez, Steffen; Jehle, Achim

    2015-09-01

    The high-end semiconductor mask fabrication is dominated by e-beam technology. But still more than 50% of all semiconductor masks are produced by laser writers. The current laser writers are based on the same technology that was used 25 years ago. They are reliable and fast but not very economical. Heidelberg Instruments has developed a new economical and fast laser writer based on the latest technologies.

  1. Strained-bond semiconductors

    NASA Astrophysics Data System (ADS)

    Dow, John D.

    1994-05-01

    Theories of strained-bond semiconductors and superconductors have been developed that promise to have significant impact on future electronic devices of interest to the Air Force. These include: (1) development of a theory of high-temperature superconductivity based on the idea of strained-layer superlattices, (2) elucidation of the physics of doping in Type-2 semiconductor superlattices, which is now central to the development of high-speed field-effect transistors, (3) a theory of dimerization and reconstruction on (001) semiconductor surfaces, (4) theory of Mobius transforms as applied to physics and remote sensing, (5) new understanding of how defects affect the vibrational properties of semiconductors, (6) new methods of efficiently computing the trajectories of atoms in semiconductors by a priori molecular dynamics, (7) elucidation of the criteria affecting quantum-well luminescence from Si, (8) models of the effects of vacancies in large-gap Al(x)Ga(1-x)N alloys, (9) physics of rare-earth-doped silicon, (10) models of Co adsorption to silicon surfaces, (11) theories of how defects affect the properties of large band-gap superlattices, and (12) models of the effects of electronic structure on the properties of semiconductors.

  2. Gold nanocrystals with DNA-directed morphologies

    PubMed Central

    Ma, Xingyi; Huh, June; Park, Wounjhang; Lee, Luke P.; Kwon, Young Jik; Sim, Sang Jun

    2016-01-01

    Precise control over the structure of metal nanomaterials is important for developing advanced nanobiotechnology. Assembly methods of nanoparticles into structured blocks have been widely demonstrated recently. However, synthesis of nanocrystals with controlled, three-dimensional structures remains challenging. Here we show a directed crystallization of gold by a single DNA molecular regulator in a sequence-independent manner and its applications in three-dimensional topological controls of crystalline nanostructures. We anchor DNA onto gold nanoseed with various alignments to form gold nanocrystals with defined topologies. Some topologies are asymmetric including pushpin-, star- and biconcave disk-like structures, as well as more complex jellyfish- and flower-like structures. The approach of employing DNA enables the solution-based synthesis of nanocrystals with controlled, three-dimensional structures in a desired direction, and expands the current tools available for designing and synthesizing feature-rich nanomaterials for future translational biotechnology. PMID:27633935

  3. Self-Organized Ultrathin Oxide Nanocrystals

    SciTech Connect

    Huo, Ziyang; Tsung, Chia-kuang; Huang, Wenyu; Fardy, Melissa; Yan, Ruoxue; Li, Yadong; Yang, Piedong; Zhang, Xiaofeng

    2009-01-08

    Sub-2-nm (down to one-unit cell) uniform oxide nanocrystals and highly ordered superstructures were obtained in one step using oleylamine and oleic acid as capping and structure directing agents. The cooperative nature of the nanocrystal growth and assembly resulted in mesoscopic one-dimensional ribbon-like superstructures made of these ultrathin nanocrystals. The process reported here is general and can be readily extended to the production of many other transition metal (TiO2, ZnO, Nb2O5) and rare earth oxide (Eu2O3, Sm2O3, Er2O3, Y2O3, Tb2O3, and Yb2O3) systems.

  4. Gold nanocrystals with DNA-directed morphologies.

    PubMed

    Ma, Xingyi; Huh, June; Park, Wounjhang; Lee, Luke P; Kwon, Young Jik; Sim, Sang Jun

    2016-01-01

    Precise control over the structure of metal nanomaterials is important for developing advanced nanobiotechnology. Assembly methods of nanoparticles into structured blocks have been widely demonstrated recently. However, synthesis of nanocrystals with controlled, three-dimensional structures remains challenging. Here we show a directed crystallization of gold by a single DNA molecular regulator in a sequence-independent manner and its applications in three-dimensional topological controls of crystalline nanostructures. We anchor DNA onto gold nanoseed with various alignments to form gold nanocrystals with defined topologies. Some topologies are asymmetric including pushpin-, star- and biconcave disk-like structures, as well as more complex jellyfish- and flower-like structures. The approach of employing DNA enables the solution-based synthesis of nanocrystals with controlled, three-dimensional structures in a desired direction, and expands the current tools available for designing and synthesizing feature-rich nanomaterials for future translational biotechnology.

  5. Gold nanocrystals with DNA-directed morphologies

    NASA Astrophysics Data System (ADS)

    Ma, Xingyi; Huh, June; Park, Wounjhang; Lee, Luke P.; Kwon, Young Jik; Sim, Sang Jun

    2016-09-01

    Precise control over the structure of metal nanomaterials is important for developing advanced nanobiotechnology. Assembly methods of nanoparticles into structured blocks have been widely demonstrated recently. However, synthesis of nanocrystals with controlled, three-dimensional structures remains challenging. Here we show a directed crystallization of gold by a single DNA molecular regulator in a sequence-independent manner and its applications in three-dimensional topological controls of crystalline nanostructures. We anchor DNA onto gold nanoseed with various alignments to form gold nanocrystals with defined topologies. Some topologies are asymmetric including pushpin-, star- and biconcave disk-like structures, as well as more complex jellyfish- and flower-like structures. The approach of employing DNA enables the solution-based synthesis of nanocrystals with controlled, three-dimensional structures in a desired direction, and expands the current tools available for designing and synthesizing feature-rich nanomaterials for future translational biotechnology.

  6. Gold nanocrystals with DNA-directed morphologies.

    PubMed

    Ma, Xingyi; Huh, June; Park, Wounjhang; Lee, Luke P; Kwon, Young Jik; Sim, Sang Jun

    2016-01-01

    Precise control over the structure of metal nanomaterials is important for developing advanced nanobiotechnology. Assembly methods of nanoparticles into structured blocks have been widely demonstrated recently. However, synthesis of nanocrystals with controlled, three-dimensional structures remains challenging. Here we show a directed crystallization of gold by a single DNA molecular regulator in a sequence-independent manner and its applications in three-dimensional topological controls of crystalline nanostructures. We anchor DNA onto gold nanoseed with various alignments to form gold nanocrystals with defined topologies. Some topologies are asymmetric including pushpin-, star- and biconcave disk-like structures, as well as more complex jellyfish- and flower-like structures. The approach of employing DNA enables the solution-based synthesis of nanocrystals with controlled, three-dimensional structures in a desired direction, and expands the current tools available for designing and synthesizing feature-rich nanomaterials for future translational biotechnology. PMID:27633935

  7. Shaping metal nanocrystals through epitaxial seeded growth

    SciTech Connect

    Habas, Susan E.; Lee, Hyunjoo; Radmilovic, Velimir; Somorjai,Gabor A.; Yang, Peidong

    2008-02-17

    Morphological control of nanocrystals has becomeincreasingly important, as many of their physical and chemical propertiesare highly shape-dependent. Nanocrystal shape control for both single andmultiple material systems, however, remains fairly empirical andchallenging. New methods need to be explored for the rational syntheticdesign of heterostructures with controlled morphology. Overgrowth of adifferent material on well-faceted seeds, for example, allows for the useof the defined seed morphology to control nucleation and growth of thesecondary structure. Here, we have used highly faceted cubic Pt seeds todirect the epitaxial overgrowth of a secondary metal. We demonstrate thisconcept with lattice matched Pd to produce conformal shape-controlledcore-shell particles, and then extend it to lattice mismatched Au to giveanisotropic growth. Seeding with faceted nanocrystals may havesignificant potential towards the development of shape-controlledheterostructures with defined interfaces.

  8. Controllable synthesis of metal selenide heterostructures mediated by Ag2Se nanocrystals acting as catalysts

    NASA Astrophysics Data System (ADS)

    Zhou, Jiangcong; Huang, Feng; Xu, Ju; Wang, Yuansheng

    2013-09-01

    Ag2Se nanocrystals were demonstrated to be novel semiconductor mediators, or in other word catalysts, for the growth of semiconductor heterostructures in solution. This is a result of the unique feature of Ag2Se as a fast ion conductor, allowing foreign cations to dissolve and then to heterogrow the second phase. Using Ag2Se nanocrystals as catalysts, dimeric metal selenide heterostructures such as Ag2Se-CdSe and Ag2Se-ZnSe, and even multi-segment heterostructures such as Ag2Se-CdSe-ZnSe and Ag2Se-ZnSe-CdSe, were successfully synthesized. Several interesting features were found in the Ag2Se based heterogrowth. At the initial stage of heterogrowth, a layer of the second phase forms on the surface of an Ag2Se nanosphere, with a curved junction interface between the two phases. With further growth of the second phase, the Ag2Se nanosphere tends to flatten the junction surface by modifying its shape from sphere to hemisphere in order to minimize the conjunct area and thus the interfacial energy. Notably, the crystallographic relationship of the two phases in the heterostructure varies with the lattice parameters of the second phase, in order to reduce the lattice mismatch at the interface. Furthermore, a small lattice mismatch at the interface results in a straight rod-like second phase, while a large lattice mismatch would induce a tortuous product. The reported results may provide a new route for developing novel selenide semiconductor heterostructures which are potentially applicable in optoelectronic, biomedical, photovoltaic and catalytic fields.Ag2Se nanocrystals were demonstrated to be novel semiconductor mediators, or in other word catalysts, for the growth of semiconductor heterostructures in solution. This is a result of the unique feature of Ag2Se as a fast ion conductor, allowing foreign cations to dissolve and then to heterogrow the second phase. Using Ag2Se nanocrystals as catalysts, dimeric metal selenide heterostructures such as Ag2Se-CdSe and Ag2Se

  9. Defect Engineering in Plasmonic Metal Oxide Nanocrystals.

    PubMed

    Runnerstrom, Evan L; Bergerud, Amy; Agrawal, Ankit; Johns, Robert W; Dahlman, Clayton J; Singh, Ajay; Selbach, Sverre M; Milliron, Delia J

    2016-05-11

    Defects may tend to make crystals interesting but they do not always improve performance. In doped metal oxide nanocrystals with localized surface plasmon resonance (LSPR), aliovalent dopants and oxygen vacancies act as centers for ionized impurity scattering of electrons. Such electronic damping leads to lossy, broadband LSPR with low quality factors, limiting applications that require near-field concentration of light. However, the appropriate dopant can mitigate ionized impurity scattering. Herein, we report the synthesis and characterization of a novel doped metal oxide nanocrystal material, cerium-doped indium oxide (Ce:In2O3). Ce:In2O3 nanocrystals display tunable mid-infrared LSPR with exceptionally narrow line widths and the highest quality factors observed for nanocrystals in this spectral region. Drude model fits to the spectra indicate that a drastic reduction in ionized impurity scattering is responsible for the enhanced quality factors, and high electronic mobilities reaching 33 cm(2)V(-1) s(-1) are measured optically, well above the optical mobility for tin-doped indium oxide (ITO) nanocrystals. We investigate the microscopic mechanisms underlying this enhanced mobility with density functional theory calculations, which suggest that scattering is reduced because cerium orbitals do not hybridize with the In orbitals that dominate the bottom of the conduction band. Ce doping may also reduce the equilibrium oxygen vacancy concentration, further enhancing mobility. From the absorption spectra of single Ce:In2O3 nanocrystals, we determine the dielectric function and by simulation predict strong near-field enhancement of mid-IR light, especially around the vertices of our synthesized nanocubes.

  10. Defect Engineering in Plasmonic Metal Oxide Nanocrystals.

    PubMed

    Runnerstrom, Evan L; Bergerud, Amy; Agrawal, Ankit; Johns, Robert W; Dahlman, Clayton J; Singh, Ajay; Selbach, Sverre M; Milliron, Delia J

    2016-05-11

    Defects may tend to make crystals interesting but they do not always improve performance. In doped metal oxide nanocrystals with localized surface plasmon resonance (LSPR), aliovalent dopants and oxygen vacancies act as centers for ionized impurity scattering of electrons. Such electronic damping leads to lossy, broadband LSPR with low quality factors, limiting applications that require near-field concentration of light. However, the appropriate dopant can mitigate ionized impurity scattering. Herein, we report the synthesis and characterization of a novel doped metal oxide nanocrystal material, cerium-doped indium oxide (Ce:In2O3). Ce:In2O3 nanocrystals display tunable mid-infrared LSPR with exceptionally narrow line widths and the highest quality factors observed for nanocrystals in this spectral region. Drude model fits to the spectra indicate that a drastic reduction in ionized impurity scattering is responsible for the enhanced quality factors, and high electronic mobilities reaching 33 cm(2)V(-1) s(-1) are measured optically, well above the optical mobility for tin-doped indium oxide (ITO) nanocrystals. We investigate the microscopic mechanisms underlying this enhanced mobility with density functional theory calculations, which suggest that scattering is reduced because cerium orbitals do not hybridize with the In orbitals that dominate the bottom of the conduction band. Ce doping may also reduce the equilibrium oxygen vacancy concentration, further enhancing mobility. From the absorption spectra of single Ce:In2O3 nanocrystals, we determine the dielectric function and by simulation predict strong near-field enhancement of mid-IR light, especially around the vertices of our synthesized nanocubes. PMID:27111427

  11. Robust, functional nanocrystal solids by infilling with atomic layer deposition

    SciTech Connect

    Liu, Yao; Gibbs, Markelle; Perkins, Craig L.; Tolentino, Jason; Zarghami, Mohammad H.; Bustamante, Jr., Jorge; Law, Matt

    2011-12-14

    Thin films of colloidal semiconductor nanocrystals (NCs) are inherently metatstable materials prone to oxidative and photothermal degradation driven by their large surface-to-volume ratios and high surface energies. The fabrication of practical electronic devices based on NC solids hinges on preventing oxidation, surface diffusion, ripening, sintering, and other unwanted physicochemical changes that can plague these materials. Here we use low-temperature atomic layer deposition (ALD) to infill conductive PbSe NC solids with metal oxides to produce inorganic nanocomposites in which the NCs are locked in place and protected against oxidative and photothermal damage. Infilling NC field-effect transistors and solar cells with amorphous alumina yields devices that operate with enhanced and stable performance for at least months in air. Furthermore, ALD infilling with ZnO lowers the height of the inter-NC tunnel barrier for electron transport, yielding PbSe NC films with electron mobilities of 1 cm² V-1 s-1. Our ALD technique is a versatile means to fabricate robust NC solids for optoelectronic devices.

  12. CdSe nanocrystal based chem-/bio- sensors.

    PubMed

    Somers, Rebecca C; Bawendi, Moungi G; Nocera, Daniel G

    2007-04-01

    Semiconductor nanocrystals (NCs) have found application in biology mostly as optical imaging agents where the photophysical properties of the NCs are insensitive to species in their environment. This tutorial review examines the application of CdSe NCs as optical sensing agents where the NC's photophysical properties are sensitive to species in their environment. For this case, the NC is modified at the surface with a conjugate, which interacts with an external agent by physical (i.e. recognition) or chemical means. Signal transduction in these chem-bio (CB) sensitive NCs is derived primarily from energy transfer between the NC and the external agent, which functions as the energy transfer acceptor or donor. Signaling may be obtained by directly detecting luminescence from the NC and/or the conjugate. New developments for the use of NCs as gain materials in micro-lasing cavities (distributed feedback gratings and spherical resonators) opens the way to designing CB-sensitive NCs for high-gain sensing applications. PMID:17387407

  13. High-performance thermoelectric nanocomposites from nanocrystal building blocks

    PubMed Central

    Ibáñez, Maria; Luo, Zhishan; Genç, Aziz; Piveteau, Laura; Ortega, Silvia; Cadavid, Doris; Dobrozhan, Oleksandr; Liu, Yu; Nachtegaal, Maarten; Zebarjadi, Mona; Arbiol, Jordi; Kovalenko, Maksym V.; Cabot, Andreu

    2016-01-01

    The efficient conversion between thermal and electrical energy by means of durable, silent and scalable solid-state thermoelectric devices has been a long standing goal. While nanocrystalline materials have already led to substantially higher thermoelectric efficiencies, further improvements are expected to arise from precise chemical engineering of nanoscale building blocks and interfaces. Here we present a simple and versatile bottom–up strategy based on the assembly of colloidal nanocrystals to produce consolidated yet nanostructured thermoelectric materials. In the case study on the PbS–Ag system, Ag nanodomains not only contribute to block phonon propagation, but also provide electrons to the PbS host semiconductor and reduce the PbS intergrain energy barriers for charge transport. Thus, PbS–Ag nanocomposites exhibit reduced thermal conductivities and higher charge carrier concentrations and mobilities than PbS nanomaterial. Such improvements of the material transport properties provide thermoelectric figures of merit up to 1.7 at 850 K. PMID:26948987

  14. Plasmonic Properties of Silicon Nanocrystals Doped with Boron and Phosphorus.

    PubMed

    Kramer, Nicolaas J; Schramke, Katelyn S; Kortshagen, Uwe R

    2015-08-12

    Degenerately doped silicon nanocrystals are appealing plasmonic materials due to silicon's low cost and low toxicity. While surface plasmonic resonances of boron-doped and phosphorus-doped silicon nanocrystals were recently observed, there currently is poor understanding of the effect of surface conditions on their plasmonic behavior. Here, we demonstrate that phosphorus-doped silicon nanocrystals exhibit a plasmon resonance immediately after their synthesis but may lose their plasmonic response with oxidation. In contrast, boron-doped nanocrystals initially do not exhibit plasmonic response but become plasmonically active through postsynthesis oxidation or annealing. We interpret these results in terms of substitutional doping being the dominant doping mechanism for phosphorus-doped silicon nanocrystals, with oxidation-induced defects trapping free electrons. The behavior of boron-doped silicon nanocrystals is more consistent with a strong contribution of surface doping. Importantly, boron-doped silicon nanocrystals exhibit air-stable plasmonic behavior over periods of more than a year.

  15. Cloning nanocrystal morphology with soft templates

    NASA Astrophysics Data System (ADS)

    Thapa, Dev Kumar; Pandey, Anshu

    2016-08-01

    In most template directed preparative methods, while the template decides the nanostructure morphology, the structure of the template itself is a non-general outcome of its peculiar chemistry. Here we demonstrate a template mediated synthesis that overcomes this deficiency. This synthesis involves overgrowth of silica template onto a sacrificial nanocrystal. Such templates are used to copy the morphologies of gold nanorods. After template overgrowth, gold is removed and silver is regrown in the template cavity to produce a single crystal silver nanorod. This technique allows for duplicating existing nanocrystals, while also providing a quantifiable breakdown of the structure - shape interdependence.

  16. Silicon and germanium nanocrystals: properties and characterization

    PubMed Central

    Carvalho, Alexandra; Coutinho, José

    2014-01-01

    Summary Group-IV nanocrystals have emerged as a promising group of materials that extends the realm of application of bulk diamond, silicon, germanium and related materials beyond their traditional boundaries. Over the last two decades of research, their potential for application in areas such as optoelectronic applications and memory devices has been progressively unraveled. Nevertheless, new challenges with no parallel in the respective bulk material counterparts have arisen. In this review, we consider what has been achieved and what are the current limitations with regard to growth, characterization and modeling of silicon and germanium nanocrystals and related materials. PMID:25383290

  17. Antioxidant properties of cerium oxide nanocrystals as a function of nanocrystal diameter and surface coating.

    PubMed

    Lee, Seung Soo; Song, Wensi; Cho, Minjung; Puppala, Hema L; Nguyen, Phuc; Zhu, Huiguang; Segatori, Laura; Colvin, Vicki L

    2013-11-26

    This work examines the effect of nanocrystal diameter and surface coating on the reactivity of cerium oxide nanocrystals with H2O2 both in chemical solutions and in cells. Monodisperse nanocrystals were formed in organic solvents from the decomposition of cerium precursors, and subsequently phase transferred into water using amphiphiles as nanoparticle coatings. Quantitative analysis of the antioxidant capacity of CeO2-x using gas chromatography and a luminol test revealed that 2 mol of H2O2 reacted with every mole of cerium(III), suggesting that the reaction proceeds via a Fenton-type mechanism. Smaller diameter nanocrystals containing more cerium(III) were found to be more reactive toward H2O2. Additionally, the presence of a surface coating did not preclude the reaction between the nanocrystal surface cerium(III) and hydrogen peroxide. Taken together, the most reactive nanoparticles were the smallest (e.g., 3.8 nm diameter) with the thinnest surface coating (e.g., oleic acid). Moreover, a benchmark test of their antioxidant capacity revealed these materials were 9 times more reactive than commercial antioxidants such as Trolox. A unique feature of these antioxidant nanocrystals is that they can be applied multiple times: over weeks, cerium(IV) rich particles slowly return to their starting cerium(III) content. In nearly all cases, the particles remain colloidally stable (e.g., nonaggregated) and could be applied multiple times as antioxidants. These chemical properties were also observed in cell culture, where the materials were able to reduce oxidative stress in human dermal fibroblasts exposed to H2O2 with efficiency comparable to their solution phase reactivity. These data suggest that organic coatings on cerium oxide nanocrystals do not limit the antioxidant behavior of the nanocrystals, and that their redox cycling behavior can be preserved even when stabilized. PMID:24079896

  18. Connecting the Particles in the Box - Controlled Fusion of Hexamer Nanocrystal Clusters within an AB6 Binary Nanocrystal Superlattice

    PubMed Central

    Treml, Benjamin E.; Lukose, Binit; Clancy, Paulette; Smilgies, Detlef-M; Hanrath, Tobias

    2014-01-01

    Binary nanocrystal superlattices present unique opportunities to create novel interconnected nanostructures by partial fusion of specific components of the superlattice. Here, we demonstrate the binary AB6 superlattice of PbSe and Fe2O3 nanocrystals as a model system to transform the central hexamer of PbSe nanocrystals into a single fused particle. We present detailed structural analysis of the superlattices by combining high-resolution X-ray scattering and electron microscopy. Molecular dynamics simulations show optimum separation of nanocrystals in agreement with the experiment and provide insights into the molecular configuration of surface ligands. We describe the concept of nanocrystal superlattices as a versatile ‘nanoreactor' to create and study novel materials based on precisely defined size, composition and structure of nanocrystals into a mesostructured cluster. We demonstrate ‘controlled fusion' of nanocrystals in the clusters in reactions initiated by thermal treatment and pulsed laser annealing. PMID:25339169

  19. Equilibrium Compositional Distribution in Freestanding Ternary Semiconductor Quantum Dots: The Case of In(x)Ga(1-x)As

    SciTech Connect

    Pandey, Sumeet C.; Maroudas, Dimitrios

    2011-01-01

    We report the findings of a systematic computational study that addresses the effects of surface segregation on the atomic distribution at equilibrium of constituent group-III atoms in freestanding ternary semiconductor InxGa1-xAs nanocrystals. Our analysis is based on density functional theory calculations in conjunction with Monte Carlo simulations of the freestanding nanocrystals using a DFT-re-parameterized valence force field description of interatomic interactions. We have determined the equilibrium concentration profiles as a function of nanocrystal size (d), composition (x), and temperature (T). The ranges of d, x, and T are explored and demonstrate surface segregation and phase separation that leads to different extents of alloying in the nanocrystal core and in the near-surface regions. We find that formation of core/shell-like quantum dots characterized by an In-deficient core and an In-rich shell with a diffuse interface is favored at equilibrium. The analysis elucidates the relationship between the constituent species distribution in the nanocrystal and the parameters that can be tuned experimentally to design synthesis routes for tailoring the properties of ternary quantum dots.

  20. A flexible method for depositing dense nanocrystal thin films: impaction of germanium nanocrystals

    SciTech Connect

    Holman, Zachary C.; Kortshagen, Uwe R.

    2010-07-27

    Nanomaterials are exciting candidates for use in new optical and electronic devices ranging from solar cells to gas sensors. However, to reach their full potential, nanomaterials must be deposited as dense thin films on flexible substrates using inexpensive processing technologies such as roll-to-roll printing. We report a new, flexible technique for depositing aerosolized nanocrystals that lends itself to roll-to-roll processes. Germanium nanocrystals produced in a plasma are accelerated through a slit orifice by a supersonic gas jet and are impacted onto a translated substrate. A uniform nanocrystal film is quickly deposited over large areas, and features as small as 2 µm can then be patterned using conventional lift-off photolithography. The density of a deposited film depends on the pressures upstream and downstream of the orifice, their ratio, and the distance between the orifice and the substrate. Nanocrystal film densities exceeding 50% of the density of bulk germanium are routinely achieved with several sizes of nanocrystals, approaching the theoretical limit for randomly packed spheres. A simple model is presented that shows that the calculated nanocrystal velocity upon impaction is strongly correlated with the resulting film density.

  1. Method of doping a semiconductor

    DOEpatents

    Yang, Chiang Y.; Rapp, Robert A.

    1983-01-01

    A method for doping semiconductor material. An interface is established between a solid electrolyte and a semiconductor to be doped. The electrolyte is chosen to be an ionic conductor of the selected impurity and the semiconductor material and electrolyte are jointly chosen so that any compound formed from the impurity and the semiconductor will have a free energy no lower than the electrolyte. A potential is then established across the interface so as to allow the impurity ions to diffuse into the semiconductor. In one embodiment the semiconductor and electrolyte may be heated so as to increase the diffusion coefficient.

  2. Synthesis and the enhanced visible-light-driven photocatalytic activity of BiVO4 nanocrystals coupled with Ag nanoparticles

    NASA Astrophysics Data System (ADS)

    Wang, W. Z.; Meng, Shan; Tan, Miao; Jia, L. J.; Zhou, Y. X.; Wu, Shuang; Huang, X. W.; Liang, Y. J.; Shi, H. L.

    2015-03-01

    BiVO4 nanocrystals coupled with Ag nanoparticles (Ag-BiVO4 heterogeneous nanostructures) have been prepared by a new strategy via combining a hydrothermal route with a polyol process, in which BiVO4 nanocrystals were first synthesized by a hydrothermal route, and then, Ag nanoparticles were grown on the surfaces of the presynthesized BiVO4 nanocrystals through a polyol process. The photocatalytic evaluations demonstrate that BiVO4 nanocrystals coupled with Ag nanoparticles exhibit the enhanced visible-light-driven photocatalytic activity for the degradation of methylene blue (MB) and rhodamine B (RhB). The energy alignment and diffuse reflectance property of Ag-BiVO4 heterogeneous nanostructures demonstrate that Ag nanoparticles attached on the surfaces of BiVO4 nanocrystals play double roles for the enhanced visible-light-driven photocatalytic activity. First, the Ag nanoparticles grown on the surfaces of BiVO4 nanocrystals may act as electron sinks to retard the recombination of the photogenerated electrons and holes in BiVO4 so as to improve the charge separation on its surfaces. Second, the Ag nanoparticles increase the visible light absorption of the Ag-BiVO4 photocatalyst due to surface plasmon resonance (SPR) of Ag nanoparticles. These double roles of Ag nanoparticles make Ag-BiVO4 heterogeneous nanostructures to exhibit the enhanced photocatalytic activity to decompose MB and RhB under visible light irradiation, compared to the pure BiVO4 nanocrystals. The enhanced photocatalytic activity is attributed to the charge transfer from BiVO4 to the attached Ag nanoparticles as well as SPR absorption of Ag nanoparticles. The present work not only provides an efficient route to enhance visible-light-driven photocatalytic activity of BiVO4, but also offers a new strategy for fabricating metal-semiconductor heterogeneous nanostructure photocatalysts, which are expected to show considerable potential applications in solar-driven wastewater treatment and water

  3. Photoinduced superconductivity in semiconductors

    NASA Astrophysics Data System (ADS)

    Goldstein, Garry; Aron, Camille; Chamon, Claudio

    2015-02-01

    We show that optically pumped semiconductors can exhibit superconductivity. We illustrate this phenomenon in the case of a two-band semiconductor tunnel-coupled to broad-band reservoirs and driven by a continuous wave laser. More realistically, we also show that superconductivity can be induced in a two-band semiconductor interacting with a broad-spectrum light source. We furthermore discuss the case of a three-band model in which the middle band replaces the broad-band reservoirs as the source of dissipation. In all three cases, we derive the simple conditions on the band structure, electron-electron interaction, and hybridization to the reservoirs that enable superconductivity. We compute the finite superconducting pairing and argue that the mechanism can be induced through both attractive and repulsive interactions and is robust to high temperatures.

  4. Giant Raman gain in silicon nanocrystals

    PubMed Central

    Sirleto, Luigi; Antonietta Ferrara, Maria; Nikitin, Timur; Novikov, Sergei; Khriachtchev, Leonid

    2012-01-01

    Nanostructured silicon has generated a lot of interest in the past decades as a key material for silicon-based photonics. The low absorption coefficient makes silicon nanocrystals attractive as an active medium in waveguide structures, and their third-order nonlinear optical properties are crucial for the development of next generation nonlinear photonic devices. Here we report the first observation of stimulated Raman scattering in silicon nanocrystals embedded in a silica matrix under non-resonant excitation at infrared wavelengths (~1.5 μm). Raman gain is directly measured as a function of the silicon content. A giant Raman gain from the silicon nanocrystals is obtained that is up to four orders of magnitude greater than in crystalline silicon. These results demonstrate the first Raman amplifier based on silicon nanocrystals in a silica matrix, thus opening new perspectives for the realization of more efficient Raman lasers with ultra-small sizes, which would increase the synergy between electronic and photonic devices. PMID:23187620

  5. Heterostructures Prepared by Surface Modification of Nanocrystals

    ERIC Educational Resources Information Center

    Lee, Bo Hyun

    2009-01-01

    Inorganic nanocrystals (NCs) have drawn the attention from many researchers due to their promising potentials for next generation technologies, from photovoltaics to biological applications. Various types of NCs have become available by synthetic protocols developed in the last two decades. In addition, multicomponent hybrid NCs which can be…

  6. Thick-shell nanocrystal quantum dots

    DOEpatents

    Hollingsworth, Jennifer A.; Chen, Yongfen; Klimov, Victor I.; Htoon, Han; Vela, Javier

    2011-05-03

    Colloidal nanocrystal quantum dots comprising an inner core having an average diameter of at least 1.5 nm and an outer shell, where said outer shell comprises multiple monolayers, wherein at least 30% of the quantum dots have an on-time fraction of 0.80 or greater under continuous excitation conditions for a period of time of at least 10 minutes.

  7. Coherent interfaces between crystals in nanocrystal composites.

    PubMed

    Liu, Hongwei; Zheng, Zhanfeng; Yang, Dongjiang; Ke, Xuebin; Jaatinen, Esa; Zhao, Jin-Cai; Zhu, Huai Yong

    2010-10-26

    Numerous materials are polycrystalline or consist with crystals of different phases. However, materials consisting of crystals on the nanometer scale (nanocrystals) are not simply aggregates of randomly oriented crystals as is generally regarded. We found, that in four different materials that consist of nanocrystals of two different phases and were obtained by different approaches, the nanocrystals of different phases are combined coherently forming interfaces with a close crystallographic registry between adjacent crystals (coherent interfaces). The four materials were fabricated by (i) depositing Ag(2)O nanoparticles on titanate nanofibers, (ii) phase transition from TiO(2)(B) nanofibers to the nanofibers of mixed TiO(2)(B) and anatase phases, (iii) dehydration of the single crystal fibril titanate core coated with anatase nanocrystals, and (iv) attaching zeolite Y nanocrystals on the surface of titanate nanofibers. The finding suggests that preferred orientations and coherent interfaces generally exist in nanocrystal systems, and according to our results, they are largely unaffected by the fabrication process that was used. This is because the preferred orientations require that the engaged crystal planes from two connected crystals have the same basal spacing and that the crystals can interlock tightly at the atomic level to form thermodynamically stable interfaces. Hence it is rational that the preferred orientations and coherent interfaces dominant the nanostructures formed between the different nanocrystals and play a key role in assembling the composite nanostructures. The orientation and interfaces between crystals of different phases in mixed-phase materials are extremely difficult to determine. Nonetheless, the thermodynamic stability of the coherent interfaces allows us to apply phase-transformation invariant line strain theory to predict the preferred orientation (and thus the structure of the coherent interfaces). The theoretical predications agree

  8. The photophysics of ionic semiconductors at low temperatures: Silver bromide, silver iodide, and cuprous oxide

    NASA Astrophysics Data System (ADS)

    Rodney, Paul James

    Three ionic semiconductors that differ in the character of their lowest energy transitions were examined. Silver bromide (AgBr) has an indirect gap, silver iodide (AgI) a direct gap, and cuprous oxide (Cu2O) a direct but parity forbidden lowest energy transition. Donor-acceptor (D-A) pair recombination was identified in the three materials using time-resolved spectroscopy and the decay dynamics were compared to a previously developed theoretical model. Nanocrystals of each material were synthesized and the effects of quantum confinement on the low temperature recombination dynamics were studied. The dynamics of the emission from aqueous prepared nanocrystals of AgBr was compared to that of larger crystals. The observed lifetime of the free exciton increased from ~20 μs to ~600 μs as the size of the crystallite decreased from 41 to 8 nm. The D- A pair recombination kinetics were bulk-like in 41 nm AgBr while in the 8 nm samples the decay lasted longer. Factorial experiments led to methods of synthesis of nanocrystals in aqueous solvents allowing the dying of the nanocrystals. Preliminary spectroscopic evidence indicated J-aggregates of pseudoisocyanine (PIC) dye were adsorbed to the nanocrystal surface. Tabular AgI nanocrystals exhibiting one dimensional confinement were synthesized. The D-A nature of the broad luminescence observed in emission from AgI has been confirmed. The D-A emission decay rates for 0.5 μm and 52 nm crystals were indistinguishable. Quantum confinement effects are manifest in a blue shift of the emission and a loss of the longer lived decay components in ~5 nm thick tabular AgI nanocrystals. Measurements of the rise time and decay time of exciton luminescence using photoluminescence upconversion were attempted. Microcrystals and nanocrystals of Cu2O were synthesized via aqueous methods with the intention of completing previous quantum confinement studies where severely heat treated purchased Cu2O was compared to aqueous prepared poly

  9. Superconductivity in doped semiconductors

    NASA Astrophysics Data System (ADS)

    Bustarret, E.

    2015-07-01

    A historical survey of the main normal and superconducting state properties of several semiconductors doped into superconductivity is proposed. This class of materials includes selenides, tellurides, oxides and column-IV semiconductors. Most of the experimental data point to a weak coupling pairing mechanism, probably phonon-mediated in the case of diamond, but probably not in the case of strontium titanate, these being the most intensively studied materials over the last decade. Despite promising theoretical predictions based on a conventional mechanism, the occurrence of critical temperatures significantly higher than 10 K has not been yet verified. However, the class provides an enticing playground for testing theories and devices alike.

  10. GUARD RING SEMICONDUCTOR JUNCTION

    DOEpatents

    Goulding, F.S.; Hansen, W.L.

    1963-12-01

    A semiconductor diode having a very low noise characteristic when used under reverse bias is described. Surface leakage currents, which in conventional diodes greatly contribute to noise, are prevented from mixing with the desired signal currents. A p-n junction is formed with a thin layer of heavily doped semiconductor material disposed on a lightly doped, physically thick base material. An annular groove cuts through the thin layer and into the base for a short distance, dividing the thin layer into a peripheral guard ring that encircles the central region. Noise signal currents are shunted through the guard ring, leaving the central region free from such currents. (AEC)

  11. Semiconductor laser diode

    SciTech Connect

    Amann, M.C.

    1982-09-28

    A semiconductor laser diode is disclosed with a connection electrode consisting of a chromium/gold alloy on a highly-doped gallium arsenide layer. The gallium arsenide layer is strip shaped and overlies a further lesser doped layer of gallium aluminum arsenide. The chromium/gold contact has a low-resistance junction only in the region of the more highly doped layer so that a strip shaped restriction of the current path occurs in the semiconductor body. Accordingly, a laser-active zone which is only strip-shaped is achieved.

  12. Semiconductor surface protection material

    NASA Technical Reports Server (NTRS)

    Packard, R. D. (Inventor)

    1973-01-01

    A method and a product for protecting semiconductor surfaces is disclosed. The protective coating material is prepared by heating a suitable protective resin with an organic solvent which is solid at room temperature and converting the resulting solution into sheets by a conventional casting operation. Pieces of such sheets of suitable shape and thickness are placed on the semiconductor areas to be coated and heat and vacuum are then applied to melt the sheet and to drive off the solvent and cure the resin. A uniform adherent coating, free of bubbles and other defects, is thus obtained exactly where it is desired.

  13. Three-Dimensional Percolation and Performance of Nanocrystal Field-Effect Transistors

    NASA Astrophysics Data System (ADS)

    Aigner, Willi; Wiesinger, Markus; Wiggers, Hartmut; Stutzmann, Martin; Pereira, Rui N.

    2016-05-01

    The understanding of charge transport through films of semiconductor nanocrystals (NCs) is fundamental for most applications envisaged for these materials, e.g., light-emitting diodes, solar cells, and thin-film field-effect transistors (FETs). In this work, we show that three-dimensional film-thickness-dependent percolation effects taking place above the percolation threshold strongly affect the charge transport in NC films and greatly determine the performance of NC devices such as NC FETs. We use thin films of Si NCs with a wide range of thicknesses controllable by spray coating of NC inks to thoroughly investigate the electronic properties and charge transport in thin NC films. We find a steep (superlinear) increase of the electrical conductivity with increasing film thickness, which is not observed in bulk semiconductor thin films with bandlike charge transport. We explain this increase by an exponentially increasing number of charge percolation paths in a system dominated by hopping charge transport. Thin-film NC FETs reveal thickness-independent field-effect mobilities and threshold voltages, whereas on:off current ratios decrease quickly with increasing film thickness. We show that the steep enhancement of electrical conductivity with increasing film thickness provided by three-dimensional percolation effects is, in fact, responsible for the dramatic degradation of NC FET performance observed with increasing film thickness. Our work demonstrates that the performance of NC FETs is much more critically sensitive to film thickness than in conventional FET-based bulk semiconductor materials.

  14. Stabilization of Novel Narrow Gap Semiconductor Phases Through Size Reduction to the Nanoscale

    NASA Astrophysics Data System (ADS)

    Soriano, Ronald B.

    The work on this dissertation is aimed at (1) preparations of multinary narrow gap semiconductor nanoparticles using hot-injection technique, (2) stabilization of novel narrow gap semiconductor nanocrystal phases, (3) elucidate the resulting structure and investigate their properties, and (4) understand the thermodynamic stability of the prepared nanomaterials. The first colloidal synthetic route for the synthesis of amorphous GeTe NPs using an amido-germanium precursor was reported. Interestingly, the amorphous particles prepared at low temperature conditions exhibit a well-defined local structure related to that of high-pressure orthorhombic GeTe. Furthermore, the amorphous GeTe NPs display nearly spherical morphology, narrow size dispersity and undergo amorphous-to-crystalline phase transition at slightly elevated temperatures compared to the bulk material. Nearly all activity in nanoparticle science to date has focused on preparing nanocrystals of almost any known bulk phase to investigate size-dependent properties. An unexplored frontier in this field is stabilizing materials with compositions and structures in the nanoscale that do not exist in the bulk, representing an unprecedented approach with the potential to introduce entirely new nanomaterials. The synthesis of single phase semiconductor Pb 2-xSnxS2 nanocrystals with cubic rock salt structure (Fm m) in a composition range that exists in the bulk as an orthorhombic structure (0.6 < x < 1) was demonstrated. New ternary nanocrystals of Pb-Sb-Te with cubic rock-salt type structure, which are mixtures of PbTe and Sb2Te3 in the bulk was successfully prepared. Pbm Sb2n Tem+3n nanocrystals are single phases and tend to phase separate at moderately high temperature. The new Pbm Sb2n Tem+3n nanocrystals define a new class of nanomaterials that only exist on the nanoscale but are unstable in the bulk. This approach of stabilizing novel phases is extended to both Pb-Sb-Se and Pb-Sb-S systems. Novel Pbm Sb2n Sem+3n

  15. Kansas Advanced Semiconductor Project

    SciTech Connect

    Baringer, P.; Bean, A.; Bolton, T.; Horton-Smith, G.; Maravin, Y.; Ratra, B.; Stanton, N.; von Toerne, E.; Wilson, G.

    2007-09-21

    KASP (Kansas Advanced Semiconductor Project) completed the new Layer 0 upgrade for D0, assumed key electronics projects for the US CMS project, finished important new physics measurements with the D0 experiment at Fermilab, made substantial contributions to detector studies for the proposed e+e- international linear collider (ILC), and advanced key initiatives in non-accelerator-based neutrino physics.

  16. Chemically Derivatized Semiconductor Photoelectrodes.

    ERIC Educational Resources Information Center

    Wrighton, Mark S.

    1983-01-01

    Deliberate modification of semiconductor photoelectrodes to improve durability and enhance rate of desirable interfacial redox processes is discussed for a variety of systems. Modification with molecular-based systems or with metals/metal oxides yields results indicating an important role for surface modification in devices for fundamental study…

  17. Amorphous semiconductor solar cell

    DOEpatents

    Dalal, Vikram L.

    1981-01-01

    A solar cell comprising a back electrical contact, amorphous silicon semiconductor base and junction layers and a top electrical contact includes in its manufacture the step of heat treating the physical junction between the base layer and junction layer to diffuse the dopant species at the physical junction into the base layer.

  18. Physics of Organic Semiconductors

    NASA Astrophysics Data System (ADS)

    Brütting, Wolfgang

    2004-05-01

    Organic semiconductors are of steadily growing interest as active components in electronics and optoelectronics. Due to their flexibility, low cost and ease-of-production they represent a valid alternative to conventional inorganic semiconductor technology in a number of applications, such as flat panel displays and illumination, plastic integrated circuits or solar energy conversion. Although first commercial applications of this technology are being realized nowadays, there is still the need for a deeper scientific understanding in order to achieve optimum device performance.This special issue of physica status solidi (a) tries to give an overview of our present-day knowledge of the physics behind organic semiconductor devices. Contributions from 17 international research groups cover various aspects of this field ranging from the growth of organic layers and crystals, their electronic properties at interfaces, their photophysics and electrical transport properties to the application of these materials in different devices like organic field-effect transistors, photovoltaic cells and organic light-emitting diodes.Putting together such a special issue one soon realizes that it is simply impossible to fully cover the whole area of organic semiconductors. Nevertheless, we hope that the reader will find the collection of topics in this issue useful for getting an up-to-date review of a field which is still developing very dynamically.

  19. All-Inorganic Germanium Nanocrystal Films by Cationic Ligand Exchange.

    PubMed

    Wheeler, Lance M; Nichols, Asa W; Chernomordik, Boris D; Anderson, Nicholas C; Beard, Matthew C; Neale, Nathan R

    2016-03-01

    We introduce a new paradigm for group IV nanocrystal surface chemistry based on room temperature surface activation that enables ionic ligand exchange. Germanium nanocrystals synthesized in a gas-phase plasma reactor are functionalized with labile, cationic alkylammonium ligands rather than with traditional covalently bound groups. We employ Fourier transform infrared and (1)H nuclear magnetic resonance spectroscopies to demonstrate the alkylammonium ligands are freely exchanged on the germanium nanocrystal surface with a variety of cationic ligands, including short inorganic ligands such as ammonium and alkali metal cations. This ionic ligand exchange chemistry is used to demonstrate enhanced transport in germanium nanocrystal films following ligand exchange as well as the first photovoltaic device based on an all-inorganic germanium nanocrystal absorber layer cast from solution. This new ligand chemistry should accelerate progress in utilizing germanium and other group IV nanocrystals for optoelectronic applications.

  20. All-inorganic Germanium nanocrystal films by cationic ligand exchange

    DOE PAGESBeta

    Wheeler, Lance M.; Nichols, Asa W.; Chernomordik, Boris D.; Anderson, Nicholas C.; Beard, Matthew C.; Neale, Nathan R.

    2016-01-21

    In this study, we introduce a new paradigm for group IV nanocrystal surface chemistry based on room temperature surface activation that enables ionic ligand exchange. Germanium nanocrystals synthesized in a gas-phase plasma reactor are functionalized with labile, cationic alkylammonium ligands rather than with traditional covalently bound groups. We employ Fourier transform infrared and 1H nuclear magnetic resonance spectroscopies to demonstrate the alkylammonium ligands are freely exchanged on the germanium nanocrystal surface with a variety of cationic ligands, including short inorganic ligands such as ammonium and alkali metal cations. This ionic ligand exchange chemistry is used to demonstrate enhanced transport inmore » germanium nanocrystal films following ligand exchange as well as the first photovoltaic device based on an all-inorganic germanium nanocrystal absorber layer cast from solution. This new ligand chemistry should accelerate progress in utilizing germanium and other group IV nanocrystals for optoelectronic applications.« less

  1. Structure and transformation of tactoids in cellulose nanocrystal suspensions

    NASA Astrophysics Data System (ADS)

    Wang, Pei-Xi; Hamad, Wadood Y.; MacLachlan, Mark J.

    2016-05-01

    Cellulose nanocrystals obtained from natural sources are of great interest for many applications. In water, cellulose nanocrystals form a liquid crystalline phase whose hierarchical structure is retained in solid films after drying. Although tactoids, one of the most primitive components of liquid crystals, are thought to have a significant role in the evolution of this phase, they have evaded structural study of their internal organization. Here we report the capture of cellulose nanocrystal tactoids in a polymer matrix. This method allows us to visualize, for the first time, the arrangement of cellulose nanocrystals within individual tactoids by electron microscopy. Furthermore, we can follow the structural evolution of the liquid crystalline phase from tactoids to iridescent-layered films. Our insights into the early nucleation events of cellulose nanocrystals give important information about the growth of cholesteric liquid crystalline phases, especially for cellulose nanocrystals, and are crucial for preparing photonics-quality films.

  2. Nonthermal Plasma Synthesis of Nanocrystals: Fundamental Principles, Materials, and Applications.

    PubMed

    Kortshagen, Uwe R; Sankaran, R Mohan; Pereira, Rui N; Girshick, Steven L; Wu, Jeslin J; Aydil, Eray S

    2016-09-28

    Nonthermal plasmas have emerged as a viable synthesis technique for nanocrystal materials. Inherently solvent and ligand-free, nonthermal plasmas offer the ability to synthesize high purity nanocrystals of materials that require high synthesis temperatures. The nonequilibrium environment in nonthermal plasmas has a number of attractive attributes: energetic surface reactions selectively heat the nanoparticles to temperatures that can strongly exceed the gas temperature; charging of nanoparticles through plasma electrons reduces or eliminates nanoparticle agglomeration; and the large difference between the chemical potentials of the gaseous growth species and the species bound to the nanoparticle surfaces facilitates nanocrystal doping. This paper reviews the state of the art in nonthermal plasma synthesis of nanocrystals. It discusses the fundamentals of nanocrystal formation in plasmas, reviews practical implementations of plasma reactors, surveys the materials that have been produced with nonthermal plasmas and surface chemistries that have been developed, and provides an overview of applications of plasma-synthesized nanocrystals.

  3. Study of nanocrystals in the dynamic slip zone

    NASA Astrophysics Data System (ADS)

    Sobolev, G. A.; Kireenkova, S. M.; Morozov, Yu. A.; Smul'skaya, A. I.; Vettegren, V. I.; Kulik, V. B.; Mamalimov, R. I.

    2012-09-01

    Mineral composition is studied and a search to detect nanocrystals is conducted in the surface layers of slickensides formed due to dynamic slip in arkose sandstone. The infrared and Raman spectroscopy show that the slickensided layer is composed of nanocrystals of montmorillonite and anatase measuring ≈15 nm and 3 nm, respectively. The crystalline lattice of the nanocrystals of montmorillonite is stretched by ≈2.5% while the lattice of the nanocrystals of anatase is compressed by ≈0.12%. Deeper than 3 mm below the slickenside surface, the sandstone contains nanocrystals of montmorillonite, beidellite and nontronite, quartz, plagioclase, and anatase. The nanocrystals of anatase have a linear size of ≈8 nm. Their crystalline lattice is compressed by ≈0.03%. It is supposed that montmorillonite in the slickensides was formed due to hydrolytic decomposition of silicates under friction of the fault planes sliding past each other.

  4. Observation of Single Colloidal Platinum Nanocrystal Growth Trajectories

    SciTech Connect

    Zheng, Haimei; Smith, Rachel; Jun, Young-wook; Kisielowski, Christian; Dahmen, Ulrich; Alivisatos, A. Paul

    2009-02-09

    It is conventionally assumed that the growth of monodisperse colloidal nanocrystals requires a temporally discrete nucleation followed by monomer attachment onto the existing nuclei. However, recent studies have reported violations of this classical growth model, and have suggested that inter-particle interactions are also involved during the growth. Mechanisms of nanocrystal growth still remain controversial. Using in situ transmission electron microscopy, we show that platinum nanocrystals can grow either by monomer attachment from solution onto the existing particles or by coalescence between the particles. Surprisingly, an initially broad size distribution of the nanocrystals can spontaneously narrow. We suggest that nanocrystals take different pathways of growth based on their size- and morphology-dependent internal energies. These observations are expected to be highly relevant for other nanocrystal systems.

  5. Structure and transformation of tactoids in cellulose nanocrystal suspensions

    PubMed Central

    Wang, Pei-Xi; Hamad, Wadood Y.; MacLachlan, Mark J.

    2016-01-01

    Cellulose nanocrystals obtained from natural sources are of great interest for many applications. In water, cellulose nanocrystals form a liquid crystalline phase whose hierarchical structure is retained in solid films after drying. Although tactoids, one of the most primitive components of liquid crystals, are thought to have a significant role in the evolution of this phase, they have evaded structural study of their internal organization. Here we report the capture of cellulose nanocrystal tactoids in a polymer matrix. This method allows us to visualize, for the first time, the arrangement of cellulose nanocrystals within individual tactoids by electron microscopy. Furthermore, we can follow the structural evolution of the liquid crystalline phase from tactoids to iridescent-layered films. Our insights into the early nucleation events of cellulose nanocrystals give important information about the growth of cholesteric liquid crystalline phases, especially for cellulose nanocrystals, and are crucial for preparing photonics-quality films. PMID:27143197

  6. Nonthermal Plasma Synthesis of Nanocrystals: Fundamental Principles, Materials, and Applications.

    PubMed

    Kortshagen, Uwe R; Sankaran, R Mohan; Pereira, Rui N; Girshick, Steven L; Wu, Jeslin J; Aydil, Eray S

    2016-09-28

    Nonthermal plasmas have emerged as a viable synthesis technique for nanocrystal materials. Inherently solvent and ligand-free, nonthermal plasmas offer the ability to synthesize high purity nanocrystals of materials that require high synthesis temperatures. The nonequilibrium environment in nonthermal plasmas has a number of attractive attributes: energetic surface reactions selectively heat the nanoparticles to temperatures that can strongly exceed the gas temperature; charging of nanoparticles through plasma electrons reduces or eliminates nanoparticle agglomeration; and the large difference between the chemical potentials of the gaseous growth species and the species bound to the nanoparticle surfaces facilitates nanocrystal doping. This paper reviews the state of the art in nonthermal plasma synthesis of nanocrystals. It discusses the fundamentals of nanocrystal formation in plasmas, reviews practical implementations of plasma reactors, surveys the materials that have been produced with nonthermal plasmas and surface chemistries that have been developed, and provides an overview of applications of plasma-synthesized nanocrystals. PMID:27550744

  7. Shaped nanocrystal particles and methods for making the same

    DOEpatents

    Alivisatos, A. Paul; Scher, Erik C; Manna, Liberato

    2013-12-17

    Shaped nanocrystal particles and methods for making shaped nanocrystal particles are disclosed. One embodiment includes a method for forming a branched, nanocrystal particle. It includes (a) forming a core having a first crystal structure in a solution, (b) forming a first arm extending from the core having a second crystal structure in the solution, and (c) forming a second arm extending from the core having the second crystal structure in the solution.

  8. Shaped nanocrystal particles and methods for working the same

    DOEpatents

    Alivisatos, A. Paul; Sher, Eric C.; Manna, Liberato

    2007-12-25

    Shaped nanocrystal particles and methods for making shaped nanocrystal particles are disclosed. One embodiment includes a method for forming a branched, nanocrystal particle. It includes (a) forming a core having a first crystal structure in a solution, (b) forming a first arm extending from the core having a second crystal structure in the solution, and (c) forming a second arm extending from the core having the second crystal structure in the solution.

  9. Shaped nanocrystal particles and methods for making the same

    DOEpatents

    Alivisatos, A. Paul; Scher, Erik C.; Manna, Liberato

    2011-11-22

    Shaped nanocrystal particles and methods for making shaped nanocrystal particles are disclosed. One embodiment includes a method for forming a branched, nanocrystal particle. It includes (a) forming a core having a first crystal structure in a solution, (b) forming a first arm extending from the core having a second crystal structure in the solution, and (c) forming a second arm extending from the core having the second crystal structure in the solution.

  10. Nanocomposites based on highly luminescent nanocrystals and semiconducting conjugated polymer for inkjet printing.

    PubMed

    Binetti, E; Ingrosso, C; Striccoli, M; Cosma, P; Agostiano, A; Pataky, K; Brugger, J; Curri, M L

    2012-02-24

    In this work nanocomposites based on organic-capped semiconductor nanocrystals formed of a core of CdSe coated with a shell of ZnS (CdSe@ZnS), with different sizes, and a semiconducting conjugated polymer, namely poly[(9,9-dihexylfluoren-2,7-diyl)-alt- (2,5-dimethyl-1,4-phenylene)] (PF-DMB) have been investigated. The nanocomposites are prepared by mixing the pre-synthesized components in organic solvents, thereby assisting the dispersion of the organic-coated nano-objects in the polymer host. UV-vis steady state and time-resolved spectroscopy along with (photo)electrochemical techniques have been performed to characterize the obtained materials. The study shows that the embedded nanocrystals increase the PF-DMB stability against oxidation and, at the same time, extend the light harvesting capability to the visible spectral region, thus resulting in detectable photocurrent signals. The nanocomposites have been dispensed by means of a piezo-actuated inkjet system. Such inks present viscosity and surface tension properties well suited for stable and reliable drop-on-demand printing using an inkjet printer. The fabrication of arrays of single-color pixels made of the nanocomposites and micrometers in size has been performed. Confocal and atomic force microscopy have confirmed that inkjet-printed microstructures present the intrinsic emission properties of both the embedded nanocrystals and PF-DMB, resulting in a combined luminescence. Finally, the morphology of the printed pixels is influenced by the embedded nanofillers. PMID:22261314

  11. Bright White Light Emission from Ultrasmall Cadmium Selenide Nanocrystals

    SciTech Connect

    Rosson, Teresa; Claiborne, Sarah; McBride, James; Stratton, Benjamin S; Rosenthal, Sandra

    2012-01-01

    A simple treatment method using formic acid has been found to increase the fluorescence quantum yield of ultrasmall white light-emitting CdSe nanocrystals from 8% to 45%. Brighter white-light emission occurs with other carboxylic acids as well, and the magnitude of the quantum yield enhancement is shown to be dependent on the alkyl chain length. Additionally, the nanocrystal luminescence remains enhanced relative to the untreated nanocrystals over several days. This brightened emission opens the possibility for even further quantum yield improvement and potential for use of these white-light nanocrystals in solid-state lighting applications.

  12. Ultrasonication of Bismuth Telluride Nanocrystals Fabricated by Solvothermal Method

    NASA Technical Reports Server (NTRS)

    Chu, Sang-Hyon; Choi, Sang H.; Kim, Jae-Woo; King, Glen C.; Elliott, James R.

    2006-01-01

    The objective of this study is to evaluate the effect of ultrasonication on bismuth telluride nanocrystals prepared by solvothermal method. In this study, a low dimensional nanocrystal of bismuth telluride (Bi2Te3) was synthesized by a solvothermal process in an autoclave at 180 C and 200 psi. During the solvothermal reaction, organic surfactants effectively prevented unwanted aggregation of nanocrystals in a selected solvent while controlling the shape of the nanocrystal. The atomic ratio of bismuth and tellurium was determined by energy dispersive spectroscopy (EDS). The cavitational energy created by the ultrasonic probe was varied by the ultrasonication process time, while power amplitude remained constant. The nanocrystal size and its size distribution were measured by field emission scanning electron microscopy (FESEM) and a dynamic light scattering system. When the ultrasonication time increased, the average size of bismuth telluride nanocrystal gradually increased due to the direct collision of nanocrystals. The polydispersity of the nanocrystals showed a minimum when the ultrasonication was applied for 5 min. Keywords: bismuth telluride, nanocrystal, low-dimensional, ultrasonication, solvothermal

  13. Controlling PbS nanocrystal aggregation in conducting polymers.

    PubMed

    Warner, Jamie H; Watt, Andrew A R; Tilley, Richard D

    2005-10-01

    PbS nanocrystals were synthesized directly in the conducting polymer, poly(3-hexylthiophene-2,5-diyl). Transmission electron microscopy shows that the PbS nanocrystals are faceted and relatively uniform in size with a mean size of 10 nm. FFT analysis of the atomic lattice planes observed in TEM and selected area electron diffraction confirm that the nanocrystals have the PbS rock salt structure. The synthesis conditions are explored to show control over the aggregation of PbS nanocrystals in the thiophene conducting polymer. PMID:20818021

  14. Light-Harvesting Antennae Based on Silicon Nanocrystals.

    PubMed

    Romano, Francesco; Yu, Yixuan; Korgel, Brian A; Bergamini, Giacomo; Ceroni, Paola

    2016-08-01

    Silicon (Si) nanocrystals are relatively strong light emitters, but are weak light absorbers as a result of their indirect band gap. One way to enhance light absorption is to functionalize the nanocrystals with chromophores that are strong light absorbers. By designing systems that enable efficient energy transfer from the chromophore to the Si nanocrystal, the brightness of the nanocrystals can be significantly increased. There have now been a few experimental systems in which covalent attachment of chromophores, efficient energy transfer and significantly increased brightness have been demonstrated. This review discusses progress on these systems and the remaining challenges. PMID:27573405

  15. Curvature-induced and thermal strain in polyhedral gold nanocrystals

    SciTech Connect

    Kim, J. W.; Dietze, S. H.; Ulvestad, A.; Fohtung, E.; Shpyrko, O. G.; Manna, S.; Fullerton, E. E.; Harder, R.

    2014-10-27

    We use coherent x-ray diffractive imaging to map the local distribution of strain in gold (Au) polyhedral nanocrystals grown on a silicon (Si) substrate by a single-step thermal chemical vapor deposition process. The lattice strain at the surface of the octahedral nanocrystal agrees well with the predictions of the Young-Laplace equation quantitatively, but exhibits a discrepancy near the nanocrystal-substrate interface. We attribute this discrepancy to the dissimilar interfacial energies between Au/Air and Au/Si and to the difference in thermal expansion between the nanocrystal and the substrate during the cooling process.

  16. Silicon nanocrystals dispersed in water: Photosensitizers for molecular oxygen

    NASA Astrophysics Data System (ADS)

    Goller, B.; Polisski, S.; Wiggers, H.; Kovalev, D.

    2010-05-01

    We report on the synthesis of freestanding silicon spheres having sizes in the range of 3-10 nm. As-prepared luminescent silicon nanocrystals have H-passivated surface. Therefore, energy transfer from excitons confined in Si nanocrystals to oxygen molecules is found to be efficient. It is demonstrated that a termination of silicon nanocrystal H-passivated hydrophobic surface by lipids provides their water solubility. We found that this procedure preserves photosensitizing ability of silicon nanocrystals. Therefore, this material system can potentially be employed for a variety of biomedical applications.

  17. Strain-dependent photoluminescence behavior in three geometries of CdSe/CdS nanocrystals

    SciTech Connect

    Choi, Charina L; Koski, Kristie J; Sivasankar, Sanjeevi; Alivisatos, A Paul

    2009-05-26

    In recent years, a new generation of quantum confined colloidal semiconductor structures has emerged, with more complex shapes than simple quantum dots1, 2. These include nanorods3 and tetrapods4. Beyond shape, it is also now possible to spatially vary the electron and hole potentials within these nanoparticles by varying the composition. Examples of these new structures include seeded dots, rods, and tetrapods, which contain a CdSe core embedded within a CdS shell5, 6. These structures may have many uses beyond those envisioned for simple quantum dots, which are frequently employed in luminescent applications7. This paper is concerned with changes in the optoelectronic properties of tetrapods when the arms are bent. We demonstrate that seeded tetrapods can serve as an optical strain gauge, capable of measuring forces on the order of nanonewtons. We anticipate that a nanocrystal strain gauge with optical readout will be useful for applications ranging from sensitive optomechanical devices to biological force investigations.

  18. Real-time optical imaging using quantum dot and related nanocrystals

    PubMed Central

    Kosaka, Nobuyuki; McCann, Thomas E; Mitsunaga, Makoto; Choyke, Peter L; Kobayashi, Hisataka

    2012-01-01

    Biomedical optical imaging is rapidly evolving because of its desirable features of rapid frame rates, high sensitivity, low cost, portability and lack of radiation. Quantum dots are attractive as imaging agents owing to their high brightness, and photo- and bio-stability. Here, the current status of in vitro and in vivo real-time optical imaging with quantum dots is reviewed. In addition, we consider related nanocrystals based on solid-state semiconductors, including upconverting nanoparticles and bioluminescence resonance energy transfer quantum dots. These particles can improve the signal-to-background ratio for real-time imaging largely by suppressing background signal. Although toxicity and biodistribution of quantum dots and their close relatives remain prime concerns for translation to human imaging, these agents have many desirable features that should be explored for medical purposes. PMID:20662647

  19. Structural and optical properties of Sb{sub 2}S{sub 3} nanocrystals in glass

    SciTech Connect

    Mishra, Rakesh K. Kashyap, Raman Vedeshwar, A. G. Tandon, R. P.

    2014-04-24

    In this work conventional solid state precipitation method is adopted to fabricate Sb{sub 2}S{sub 3} nanocrystals in glass. The glass composition is optimized for proper host glass matrix to grow antimony trisulphide semiconductor quantum dots. The dot size is modified by heat treatment of glass samples in the temperature range from 550°C to 700°C for various time durations. Structural studies are carried out by X-ray diffraction and transmission electron microscopy and nanoparticles with size ranges from 8 nm to 70 nm are obtained. Quantum dots so grown were further characterized by optical absorption spectroscopy and a blue shift is observed for absorption edge energy that conform the quantum confinement effect.

  20. High efficiency carrier multiplication in PbSe nanocrystals: implications for solar energy conversion.

    PubMed

    Schaller, R D; Klimov, V I

    2004-05-01

    We demonstrate for the first time that impact ionization (II) (the inverse of Auger recombination) occurs with very high efficiency in semiconductor nanocrystals (NCs). Interband optical excitation of PbSe NCs at low pump intensities, for which less than one exciton is initially generated per NC on average, results in the formation of two or more excitons (carrier multiplication) when pump photon energies are more than 3 times the NC band gap energy. The generation of multiexcitons from a single photon absorption event is observed to take place on an ultrafast (picosecond) time scale and occurs with up to 100% efficiency depending upon the excess energy of the absorbed photon. Efficient II in NCs can be used to considerably increase the power conversion efficiency of NC-based solar cells.

  1. Perspective on the prospects of a carrier multiplication nanocrystal solar cell

    SciTech Connect

    Nair, G.; Chang, L. -Y; Geyer, S. M.; Bawendi, Moungi G.

    2011-05-11

    This article presents a perspective on the experimental and theoretical work to date on the efficiency of carrier multiplication (CM) in colloidal semiconductor nanocrystals (NCs). Early reports on CM in NCs suggested large CM efficiency enhancements. However, recent experiments have shown that CM in nanocrystalline samples is not significantly stronger, and often is weaker, than in the parent bulk when compared on an absolute photon energy basis. This finding is supported by theoretical consideration of the CM process and the competing intraband relaxation. We discuss the experimental artifacts that may have led to the apparently strong CM estimated in early reports. The finding of bulklike CM in NCs suggests that the main promise of quantum confinement is to boost the photovoltage at which carriers can be extracted. With this in mind, we discuss research directions that may result in effective use of CM in a solar cell.

  2. Role of the inversion layer on the charge injection in silicon nanocrystal multilayered light emitting devices

    NASA Astrophysics Data System (ADS)

    Tondini, S.; Pucker, G.; Pavesi, L.

    2016-09-01

    The role of the inversion layer on injection and recombination phenomena in light emitting diodes (LEDs) is here studied on a multilayer (ML) structure of silicon nanocrystals (Si-NCs) embedded in SiO2. Two Si-NC LEDs, which are similar for the active material but different in the fabrication process, elucidate the role of the non-radiative recombination rates at the ML/substrate interface. By studying current- and capacitance-voltage characteristics as well as electroluminescence spectra and time-resolved electroluminescence under pulsed and alternating bias pumping scheme in both the devices, we are able to ascribe the different experimental results to an efficient or inefficient minority carrier (electron) supply by the p-type substrate in the metal oxide semiconductor LEDs.

  3. Tuning the Optical Properties of Cesium Lead Halide Perovskite Nanocrystals by Anion Exchange Reactions

    PubMed Central

    2015-01-01

    We demonstrate that, via controlled anion exchange reactions using a range of different halide precursors, we can finely tune the chemical composition and the optical properties of presynthesized colloidal cesium lead halide perovskite nanocrystals (NCs), from green emitting CsPbBr3 to bright emitters in any other region of the visible spectrum, and back, by displacement of Cl– or I– ions and reinsertion of Br– ions. This approach gives access to perovskite semiconductor NCs with both structural and optical qualities comparable to those of directly synthesized NCs. We also show that anion exchange is a dynamic process that takes place in solution between NCs. Therefore, by mixing solutions containing perovskite NCs emitting in different spectral ranges (due to different halide compositions) their mutual fast exchange dynamics leads to homogenization in their composition, resulting in NCs emitting in a narrow spectral region that is intermediate between those of the parent nanoparticles. PMID:26214734

  4. CsPbBr3 nanocrystal saturable absorber for mode-locking ytterbium fiber laser

    NASA Astrophysics Data System (ADS)

    Zhou, Yan; Hu, Zhiping; Li, Yue; Xu, Jianqiu; Tang, Xiaosheng; Tang, Yulong

    2016-06-01

    Cesium lead halide perovskite nanocrystals (CsPbX3, X = Cl, Br, I) have been reported as efficient light-harvesting and light-emitting semiconductor materials, but their nonlinear optical properties have been seldom touched upon. In this paper, we prepare layered CsPbBr3 nanocrystal films and characterize their physical properties. Broadband linear absorption from ˜0.8 to over 2.2 μm and nonlinear optical absorption at the 1-μm wavelength region are measured. The CsPbBr3 saturable absorber (SA), manufactured by drop-casting of colloidal CsPbBr3 liquid solution on a gold mirror, shows modulation depth and saturation intensity of 13.1% and 10.7 MW/cm2, respectively. With this SA, mode-locking operation of a polarization-maintained ytterbium fiber laser produces single pulses with duration of ˜216 ps, maximum average output power of 10.5 mW, and the laser spectrum is centered at ˜1076 nm. This work shows that CsPbBr3 films can be efficient SA candidates for fiber lasers and also have great potential to become broadband linear and nonlinear optical materials for photonics and optoelectronics.

  5. Magnetic properties of Cd(1 - x)Mn(x)Te/C nanocrystals.

    PubMed

    Bhattacharyya, Sayan; Zitoun, D; Gedanken, A

    2011-02-18

    Mn doped CdTe nanocrystals coated by carbon (Cd(1 - x)Mn(x)Te/C) were synthesized by a one-step, kinetically controlled solid state reaction under autogenic pressure at elevated temperatures. Electron microscopic analysis confirmed that the 40-52 nm Cd(1 - x)Mn(x)Te core was encapsulated by a 6-9 nm carbon shell. The efficient doping by Mn(2+) in the zinc blende Cd(1 - x)Mn(x)Te lattice, up to an atomic ratio of Mn/Cd of 0.031, was confirmed from electron paramagnetic resonance (EPR) experiments. In the case of higher doping, it is likely that manganese is partially expelled to the nanocrystal surface. All the doped samples exhibit ferromagnetism at room temperature. The lowest doped sample has the highest magnetic moment (1.91 ± 0.02 µ(B)/Mn). The more concentrated samples exhibit weaker ferromagnetic interactions, probably due to an incomplete coupling between carriers in the host CdTe semiconductor and dopant spins.

  6. Small silicon, big opportunities: the development and future of colloidally-stable monodisperse silicon nanocrystals.

    PubMed

    Mastronardi, Melanie L; Henderson, Eric J; Puzzo, Daniel P; Ozin, Geoffrey A

    2012-11-14

    Nanomaterials are becoming increasingly widespread in consumer technologies, but there is global concern about the toxicity of nanomaterials to humans and the environment as they move rapidly from the research laboratory to the market place. With this in mind, it makes sense to intensify the nanochemistry community's global research effort on the synthesis and study of nanoparticles that are purportedly "green". One potentially green nanoparticle that seems to be a most promising candidate in this context is silicon, whose appealing optical, optoelectronic, photonic, and biomedical attributes are recently gaining much attention. In this paper, we outline some of our recent contributions to the development of the growing field of silicon nanocrystals (ncSi) in order to stress the importance of continued study of ncSi as a green alternative to the archetypal semiconductor nanocrystals like CdSe, InAs, and PbS. While a variety of developments in synthetic methods, characterization techniques, and applications have been reported in recent years, the ability to prepare colloidally-stable monodisperse ncSi samples may prove to have the largest impact on the field, as it opens the door to study and access the tunable size-dependent properties of ncSi. Here, we summarize our recent contributions in size-separation methods to achieve monodisperse samples, the characterization of size-dependant property trends, the development of ncSi applications, and their potential impact on the promising future of ncSi.

  7. High Resolution Fluorescence Imaging of Cancers Using Lanthanide Ion-Doped Upconverting Nanocrystals

    PubMed Central

    Naccache, Rafik; Rodríguez, Emma Martín; Bogdan, Nicoleta; Sanz-Rodríguez, Francisco; de la Cruz, Maria del Carmen Iglesias; de la Fuente, Ángeles Juarranz; Vetrone, Fiorenzo; Jaque, Daniel; Solé, José García; Capobianco, John A.

    2012-01-01

    During the last decade inorganic luminescent nanoparticles that emit visible light under near infrared (NIR) excitation (in the biological window) have played a relevant role for high resolution imaging of cancer. Indeed, semiconductor quantum dots (QDs) and metal nanoparticles, mostly gold nanorods (GNRs), are already commercially available for this purpose. In this work we review the role which is being played by a relatively new class of nanoparticles, based on lanthanide ion doped nanocrystals, to target and image cancer cells using upconversion fluorescence microscopy. These nanoparticles are insulating nanocrystals that are usually doped with small percentages of two different rare earth (lanthanide) ions: The excited donor ions (usually Yb3+ ion) that absorb the NIR excitation and the acceptor ions (usually Er3+, Ho3+ or Tm3+), that are responsible for the emitted visible (or also near infrared) radiation. The higher conversion efficiency of these nanoparticles in respect to those based on QDs and GNRs, as well as the almost independent excitation/emission properties from the particle size, make them particularly promising for fluorescence imaging. The different approaches of these novel nanoparticles devoted to “in vitro” and “in vivo” cancer imaging, selective targeting and treatment are examined in this review. PMID:24213500

  8. Direct Probe of Spectral Inhomogeneity Reveals Synthetic Tunability of Single-Nanocrystal Spectral Linewidths

    PubMed Central

    Cui, Jian; Beyler, Andrew P.; Marshall, Lisa F.; Chen, Ou; Harris, Daniel K.; Wanger, Darcy D.; Brokmann, Xavier; Bawendi, Moungi G.

    2013-01-01

    The spectral linewidth of an ensemble of fluorescent emitters is dictated by a combination of the single emitter linewidths and sample inhomogeneities. For semiconductor nanocrystals, efforts to tune ensemble linewidths for optical applications have focused primarily on eliminating sample inhomogeneities because conventional single-molecule methods cannot reliably build accurate ensemble-level statistics for single-particle linewidths. Photon-correlation Fourier spectroscopy in solution (S-PCFS) offers a unique approach to investigating single-nanocrystal spectra with large sample statistics, without user selection bias, with high signal-to-noise ratios, and at fast timescales. With S-PCFS, we directly and quantitatively deconstruct the ensemble linewidth into contributions from the average single-particle linewidth and from sample inhomogeneity. We demonstrate that single-particle linewidths vary significantly from batch to batch and can be synthetically controlled. These findings crystallize our understanding of the synthetic challenges facing underdeveloped nanomaterials such as InP and InAs core/shell particles and introduce new avenues for the synthetic optimization of fluorescent nanoparticles. PMID:23787751

  9. Energy harvesting of non-emissive triplet excitons in tetracene by emissive PbS nanocrystals

    NASA Astrophysics Data System (ADS)

    Thompson, Nicholas J.; Wilson, Mark W. B.; Congreve, Daniel N.; Brown, Patrick R.; Scherer, Jennifer M.; Bischof, Thomas S.; Wu, Mengfei; Geva, Nadav; Welborn, Matthew; Voorhis, Troy Van; Bulović, Vladimir; Bawendi, Moungi G.; Baldo, Marc A.

    2014-11-01

    Triplet excitons are ubiquitous in organic optoelectronics, but they are often an undesirable energy sink because they are spin-forbidden from emitting light and their high binding energy hinders the generation of free electron-hole pairs. Harvesting their energy is consequently an important technological challenge. Here, we demonstrate direct excitonic energy transfer from ‘dark’ triplets in the organic semiconductor tetracene to colloidal PbS nanocrystals, thereby successfully harnessing molecular triplet excitons in the near infrared. Steady-state excitation spectra, supported by transient photoluminescence studies, demonstrate that the transfer efficiency is at least (90 ± 13)%. The mechanism is a Dexter hopping process consisting of the simultaneous exchange of two electrons. Triplet exciton transfer to nanocrystals is expected to be broadly applicable in solar and near-infrared light-emitting applications, where effective molecular phosphors are lacking at present. In particular, this route to ‘brighten’ low-energy molecular triplet excitons may permit singlet exciton fission sensitization of conventional silicon solar cells.

  10. A facile route to violet- to orange-emitting CdxZn1-xSe alloy nanocrystals via cation exchange reaction

    NASA Astrophysics Data System (ADS)

    Zhong, Xinhua; Feng, Yaoyu; Zhang, Yuliang; Gu, Zhenyu; Zou, Lei

    2007-09-01

    The most advanced CdSe-based binary semiconductor system does not work well for emission in the short wavelength spectral region from 420 to 500 nm, which is of special interest for the preparation of nanocrystal-based blue LEDs and white light generation. CdxZn1-xSe alloy nanocrystals are proven to be an attractive alternative as their emission color can be tuned from the UV spectral region (ZnSe) to the red region (CdSe) by changing the composition of the Zn/Cd ratio in the alloy. Herein we report a facile and 'green' alloying approach for the preparation of highly luminescent CdxZn1-xSe nanocrystals via cation exchange reaction of the pre-prepared ZnSe nanocrystals with Cd2+ at intermediate temperatures. Through this new synthetic strategy, high-quality alloy QDs with different desired emission wavelengths or colors (ranging from 370 to 600 nm) can be made reproducibly and precisely by varying the predetermined amounts of the reaction precursors.

  11. Photogenerated excitons in plain core CdSe nanocrystals with unity radiative decay in single channel: the effects of surface and ligands.

    PubMed

    Gao, Yuan; Peng, Xiaogang

    2015-04-01

    A systematic and reproducible method was developed to study the decay dynamics of an exciton, a photogenerated electron-hole pair, in semiconductor nanocrystals in solution. Results revealed that the excitons in plain core CdSe nanocrystals in either zinc-blende or wurtzite or mixed lattice structures could be reproducibly prepared to decay radiatively in unity quantum yield and in single channel. The single-channel lifetime was found to increase monotonically by increasing size of the CdSe nanocrystals, with zinc-blende ones increasing in a relatively slow pace. Surface inorganic stoichiometry was found to be a sensitive parameter to affect the exciton decay dynamics for all crystal structures with different sizes. Excess Se (Cd) sites on the surface were found to induce short (long) lifetime channels for the excitons. Both types of traps reduced the quantum yield of the radiative decay of the excitons, and the hole traps associated with Se sites were nearly not emissive. With optimal surface inorganic stoichiometry, primary amines were identified as "ideal" organic ligands for CdSe core nanocrystals to achieve unity radiative decay of excitons in single channel in comparison to other types of neutral ligands commonly applied in the field.

  12. Fast Anion-Exchange in Highly Luminescent Nanocrystals of Cesium Lead Halide Perovskites (CsPbX3, X = Cl, Br, I)

    PubMed Central

    2015-01-01

    Postsynthetic chemical transformations of colloidal nanocrystals, such as ion-exchange reactions, provide an avenue to compositional fine-tuning or to otherwise inaccessible materials and morphologies. While cation-exchange is facile and commonplace, anion-exchange reactions have not received substantial deployment. Here we report fast, low-temperature, deliberately partial, or complete anion-exchange in highly luminescent semiconductor nanocrystals of cesium lead halide perovskites (CsPbX3, X = Cl, Br, I). By adjusting the halide ratios in the colloidal nanocrystal solution, the bright photoluminescence can be tuned over the entire visible spectral region (410–700 nm) while maintaining high quantum yields of 20–80% and narrow emission line widths of 10–40 nm (from blue to red). Furthermore, fast internanocrystal anion-exchange is demonstrated, leading to uniform CsPb(Cl/Br)3 or CsPb(Br/I)3 compositions simply by mixing CsPbCl3, CsPbBr3, and CsPbI3 nanocrystals in appropriate ratios. PMID:26207728

  13. Fast Anion-Exchange in Highly Luminescent Nanocrystals of Cesium Lead Halide Perovskites (CsPbX3, X = Cl, Br, I).

    PubMed

    Nedelcu, Georgian; Protesescu, Loredana; Yakunin, Sergii; Bodnarchuk, Maryna I; Grotevent, Matthias J; Kovalenko, Maksym V

    2015-08-12

    Postsynthetic chemical transformations of colloidal nanocrystals, such as ion-exchange reactions, provide an avenue to compositional fine-tuning or to otherwise inaccessible materials and morphologies. While cation-exchange is facile and commonplace, anion-exchange reactions have not received substantial deployment. Here we report fast, low-temperature, deliberately partial, or complete anion-exchange in highly luminescent semiconductor nanocrystals of cesium lead halide perovskites (CsPbX3, X = Cl, Br, I). By adjusting the halide ratios in the colloidal nanocrystal solution, the bright photoluminescence can be tuned over the entire visible spectral region (410-700 nm) while maintaining high quantum yields of 20-80% and narrow emission line widths of 10-40 nm (from blue to red). Furthermore, fast internanocrystal anion-exchange is demonstrated, leading to uniform CsPb(Cl/Br)3 or CsPb(Br/I)3 compositions simply by mixing CsPbCl3, CsPbBr3, and CsPbI3 nanocrystals in appropriate ratios. PMID:26207728

  14. Spectroscopy of carrier multiplication in nanocrystals.

    PubMed

    Bruhn, Benjamin; Limpens, Rens; Chung, Nguyen Xuan; Schall, Peter; Gregorkiewicz, Tom

    2016-01-01

    Carrier multiplication in nanostructures promises great improvements in a number of widely used technologies, among others photodetectors and solar cells. The decade since its discovery was ridden with fierce discussions about its true existence, magnitude, and mechanism. Here, we introduce a novel, purely spectroscopic approach for investigation of carrier multiplication in nanocrystals. Applying this method to silicon nanocrystals in an oxide matrix, we obtain an unambiguous spectral signature of the carrier multiplication process and reveal details of its size-dependent characteristics-energy threshold and efficiency. The proposed method is generally applicable and suitable for both solid state and colloidal samples, as well as for a great variety of different materials. PMID:26852922

  15. Tunable plasmonic lattices of silver nanocrystals

    SciTech Connect

    Tao, Andrea; Sinsermsuksakul, Prasert; Yang, Peidong

    2008-02-18

    Silver nanocrystals are ideal building blocks for plasmonicmaterials that exhibit a wide range of unique and potentially usefuloptical phenomena. Individual nanocrystals display distinct opticalscattering spectra and can be assembled into hierarchical structures thatcouple strongly to external electromagnetic fields. This coupling, whichis mediated by surface plasmons, depends on their shape and arrangement.Here we demonstrate the bottom-up assembly of polyhedral silvernanocrystals into macroscopic two-dimensional superlattices using theLangmuir-Blodgett technique. Our ability to control interparticlespacing, density, and packing symmetry allows for tunability of theoptical response over the entire visible range. This assembly strategyoffers a new, practical approach to making novel plasmonic materials forapplication in spectroscopic sensors, sub-wavelength optics, andintegrated devices that utilize field enhancement effects.

  16. Atomic Diffusion within Individual Gold Nanocrystal

    PubMed Central

    Xiong, Gang; Clark, Jesse N.; Nicklin, Chris; Rawle, Jonathan; Robinson, Ian K.

    2014-01-01

    Due to their excess surface free energy and structural instabilities, nanoparticles exhibit interesting physical and chemical properties. There has been an ever-growing interest in investigating these properties, driven by the desire to further miniaturize electronic devices, develop new functional materials and catalysts. Here, the intriguing question of how diffusion evolves in a single nanoparticle is investigated by measuring the spatial and temporal variations of the diffracted coherent X-ray intensity during copper diffusion into a gold nanocrystal. Dislocation loops formed from the insertion of single layer of extra atoms between neighbouring gold host lattice planes are detected. Au-Cu alloy channels are found to penetrate the nanocrystal due to the differential diffusion rate along different directions. With the advent of higher brilliance sources and free-electron-lasers, Bragg Coherent X-ray Diffraction Imaging can play an important role in unveiling atomic behaviours in three dimensions for nanomaterials during various fundamental processes. PMID:25341377

  17. Colloidal Synthesis of Hollow Cobalt Sulfide Nanocrystals

    SciTech Connect

    Yin, Yadong; Erdonmez, Can K.; Cabot, Andreu; Hughes, Steven; Alivisatos, A. Paul

    2006-03-16

    Formation of cobalt sulfide hollow nanocrystals through amechanism similar to the Kirkendall Effect has been investigated indetail. It was found that performing the reaction at>120oC leads tofast formation of a single void ins ide each shell, whereas at roomtemperature multiple voids are formed within each shell, which can beattributed to strongly temperature-dependent diffusivities for vacancies.The void formation process is dominated by outward diffusion of cobaltcations; still, significant inward transport of sulfur anions can beinferred to occur as the final voids are smaller in diameter than theoriginal cobalt nanocrystals. Comparison of volume distributions forinitial and final nanostructures indicates excess apparent volume inshells implying significant porosity and/or a defective structure.Indirect evidence for shells to fracture during growth at lowertemperatures was observed in shell size statisticsand TEM of as-grownshells. An idealized model of the diffusional process imposes two minimalrequirements on material parameters for shell growth to be obtainablewithin a specific synthetic system.

  18. Tunable lifetime multiplexing using luminescent nanocrystals

    NASA Astrophysics Data System (ADS)

    Lu, Yiqing; Zhao, Jiangbo; Zhang, Run; Liu, Yujia; Liu, Deming; Goldys, Ewa M.; Yang, Xusan; Xi, Peng; Sunna, Anwar; Lu, Jie; Shi, Yu; Leif, Robert C.; Huo, Yujing; Shen, Jian; Piper, James A.; Robinson, J. Paul; Jin, Dayong

    2014-01-01

    Optical multiplexing plays an important role in applications such as optical data storage, document security, molecular probes and bead assays for personalized medicine. Conventional fluorescent colour coding is limited by spectral overlap and background interference, restricting the number of distinguishable identities. Here, we show that tunable luminescent lifetimes τ in the microsecond region can be exploited to code individual upconversion nanocrystals. In a single colour band, one can generate more than ten nanocrystal populations with distinct lifetimes ranging from 25.6 µs to 662.4 µs and decode their well-separated lifetime identities, which are independent of both colour and intensity. Such `τ-dots' potentially suit multichannel bioimaging, high-throughput cytometry quantification, high-density data storage, as well as security codes to combat counterfeiting. This demonstration extends the optical multiplexing capability by adding the temporal dimension of luminescent signals, opening new opportunities in the life sciences, medicine and data security.

  19. Atomic Diffusion within Individual Gold Nanocrystal

    NASA Astrophysics Data System (ADS)

    Xiong, Gang; Clark, Jesse N.; Nicklin, Chris; Rawle, Jonathan; Robinson, Ian K.

    2014-10-01

    Due to their excess surface free energy and structural instabilities, nanoparticles exhibit interesting physical and chemical properties. There has been an ever-growing interest in investigating these properties, driven by the desire to further miniaturize electronic devices, develop new functional materials and catalysts. Here, the intriguing question of how diffusion evolves in a single nanoparticle is investigated by measuring the spatial and temporal variations of the diffracted coherent X-ray intensity during copper diffusion into a gold nanocrystal. Dislocation loops formed from the insertion of single layer of extra atoms between neighbouring gold host lattice planes are detected. Au-Cu alloy channels are found to penetrate the nanocrystal due to the differential diffusion rate along different directions. With the advent of higher brilliance sources and free-electron-lasers, Bragg Coherent X-ray Diffraction Imaging can play an important role in unveiling atomic behaviours in three dimensions for nanomaterials during various fundamental processes.

  20. Process for making surfactant capped nanocrystals

    DOEpatents

    Alivisatos, A Paul; Rockenberger, Joerg

    2002-01-01

    Disclosed is a process for making surfactant capped nanocrystals of transition metal oxides. The process comprises reacting a metal cupferron complex of the formula M Cup, wherein M is a transition metal, and Cup is a cupferron, with a coordinating surfactant, the reaction being conducted at a temperature ranging from about 250 to about 300 C., for a period of time sufficient to complete the reaction.