Magnetic Doping Of Semiconductor Molecular Models And Colloidal Nanocrystals PDF Download
Are you looking for read ebook online? Search for your book and save it on your Kindle device, PC, phones or tablets. Download Magnetic Doping Of Semiconductor Molecular Models And Colloidal Nanocrystals PDF full book. Access full book title Magnetic Doping Of Semiconductor Molecular Models And Colloidal Nanocrystals by Swamy Pittala. Download full books in PDF and EPUB format.
Author: Swamy Pittala
Publisher:
ISBN:
Category :
Languages : en
Pages :
Get Book Here
Book Description
Spin-based electronics use the spins of electrons in addition to their charges and have potential applications to create a next generation of quantum computers, capable of storing vast amounts of data in an energy-efficient way. Diluted magnetic semiconductor quantum dots (DMS-QDs) have shown great promise as ideal materials for application in spin-based electronics. However, doping impurities into quantum confined colloidal nanocrystals (NCs) has been a great challenge due to the lack of control over the dopant reactivity during the specific stages of nucleation and growth. The mechanism of dopant incorporation into nanocrystals is complex and well-defined and atomically precise molecular clusters can provide detailed knowledge and novel insights into the doping process. This work focuses on the synthesis of Co2+ substituted CdS and ZnS based molecular clusters and understanding doping mechanism at the molecular level and use these clusters as precursors to make doped nanocrystals. The cation exchange rates and thermodynamic stability of dopants in the smallest tetrameric clusters is found to depend mainly on the identity of the host cation in the cluster. The surface ligand dynamics of clusters directly control the rate of dopant ion exchange into molecular clusters. As the size of molecular clusters increases the ligand dynamics decreases and dopant exchange into these larger clusters becomes less feasible. We developed a method to synthesize doped NCs using these pre-doped magnetic molecular chalcogenide clusters, as single-source precursors. We obtained very high concentration of cobalt impurities into CdS nanocrystals without undergoing spinodal decomposition. This high doping level is attributed to the growth mechanism that involves formation of dopant substituted metastable magic-sized nuclei (CdS)34 before the critical nuclei during the synthesis. Furthermore, the particular growth mechanism of doped nanocrystals can be controlled by the size of diluted magnetic molecular precursors. The synthetic strategy demonstrated here utilizes magnetic inorganic clusters as true single-source precursors and provides an effective and tunable route to synthesize doped nanocrystals with high dopant concentrations.
Author: Swamy Pittala
Publisher:
ISBN:
Category :
Languages : en
Pages :
Get Book Here
Book Description
Spin-based electronics use the spins of electrons in addition to their charges and have potential applications to create a next generation of quantum computers, capable of storing vast amounts of data in an energy-efficient way. Diluted magnetic semiconductor quantum dots (DMS-QDs) have shown great promise as ideal materials for application in spin-based electronics. However, doping impurities into quantum confined colloidal nanocrystals (NCs) has been a great challenge due to the lack of control over the dopant reactivity during the specific stages of nucleation and growth. The mechanism of dopant incorporation into nanocrystals is complex and well-defined and atomically precise molecular clusters can provide detailed knowledge and novel insights into the doping process. This work focuses on the synthesis of Co2+ substituted CdS and ZnS based molecular clusters and understanding doping mechanism at the molecular level and use these clusters as precursors to make doped nanocrystals. The cation exchange rates and thermodynamic stability of dopants in the smallest tetrameric clusters is found to depend mainly on the identity of the host cation in the cluster. The surface ligand dynamics of clusters directly control the rate of dopant ion exchange into molecular clusters. As the size of molecular clusters increases the ligand dynamics decreases and dopant exchange into these larger clusters becomes less feasible. We developed a method to synthesize doped NCs using these pre-doped magnetic molecular chalcogenide clusters, as single-source precursors. We obtained very high concentration of cobalt impurities into CdS nanocrystals without undergoing spinodal decomposition. This high doping level is attributed to the growth mechanism that involves formation of dopant substituted metastable magic-sized nuclei (CdS)34 before the critical nuclei during the synthesis. Furthermore, the particular growth mechanism of doped nanocrystals can be controlled by the size of diluted magnetic molecular precursors. The synthetic strategy demonstrated here utilizes magnetic inorganic clusters as true single-source precursors and provides an effective and tunable route to synthesize doped nanocrystals with high dopant concentrations.
Author: Lijun Zu
Publisher:
ISBN:
Category :
Languages : en
Pages : 352
Get Book Here
Book Description
Author: Volkmar Dierolf
Publisher: Woodhead Publishing
ISBN: 008100060X
Category : Science
Languages : en
Pages : 472
Get Book Here
Book Description
Rare Earth and Transition Metal Doping of Semiconductor Material explores traditional semiconductor devices that are based on control of the electron’s electric charge. This book looks at the semiconductor materials used for spintronics applications, in particular focusing on wide band-gap semiconductors doped with transition metals and rare earths. These materials are of particular commercial interest because their spin can be controlled at room temperature, a clear opposition to the most previous research on Gallium Arsenide, which allowed for control of spins at supercold temperatures. Part One of the book explains the theory of magnetism in semiconductors, while Part Two covers the growth of semiconductors for spintronics. Finally, Part Three looks at the characterization and properties of semiconductors for spintronics, with Part Four exploring the devices and the future direction of spintronics. Examines materials which are of commercial interest for producing smaller, faster, and more power-efficient computers and other devices Analyzes the theory behind magnetism in semiconductors and the growth of semiconductors for spintronics Details the properties of semiconductors for spintronics
Author: Tejinder Singh
Publisher:
ISBN:
Category : Doped semiconductors
Languages : en
Pages : 225
Get Book Here
Book Description
Doping in bulk semiconductors (e.g., n- or p- type doping in silicon) allows for precise control of their properties and forms the basis for the development of electronic and photovoltaic devices. Recently, there have been reports on the successful synthesis of doped semiconductor nanocrystals (or quantum dots) for potential applications in solar cells and spintronics. For example, nanocrystals of ZnSe (with zinc-blende lattice structure) and CdSe and ZnO (with wurtzite lattice structure) have been doped successfully with transition-metal (TM) elements (Mn, Co, or Ni). Despite the recent progress, however, the underlying mechanisms of doping in colloidal nanocrystals are not well understood. This thesis reports a comprehensive theoretical analysis toward a fundamental kinetic and thermodynamic understanding of doping in ZnO, CdSe, and ZnSe quantum dots based on first-principles density-functional theory (DFT) calculations. The theoretical predictions of this thesis are consistent with experimental measurements and provide fundamental interpretations for the experimental observations. The mechanisms of doping of colloidal ZnO nanocrystals with the TM elements Mn, Co, and Ni is investigated. The dopant atoms are found to have high binding energies for adsorption onto the Zn-vacancy site of the (0001) basal surface and the O-vacancy site of the (0001) basal surface of ZnO nanocrystals; therefore, these surface vacancies provide viable sites for substitutional doping, which is consistent with experimental measurements. However, the doping efficiencies are affected by the strong tendencies of the TM dopants to segregate at the nanocrystal surface facets, as indicated by the corresponding computed dopant surface segregation energy profiles. Furthermore, using the Mn doping of CdSe as a case study, the effect of nanocrystal size on doping efficiency is explored. It is shown that Mn adsorption onto small clusters of CdSe is characterized by high binding energies, which, in conjunction with the Mn surface segregation characteristics on CdSe nanocrystals, explains experimental reports of high doping efficiency for small-size CdSe clusters. In addition, this thesis presents a systematic analysis of TM doping in ZnSe nanocrystals. The analysis focuses on the adsorption and surface segregation of Mn dopants on ZnSe nanocrystal surface facets, as well as dopant-induced nanocrystal morphological transitions, and leads to a fundamental understanding of the underlying mechanisms of dopant incorporation into growing nanocrystals. Both surface kinetics (dopant adsorption onto the nanocrystal surface facets) and thermodynamics (dopant surface segregation) are found to have a significant effect on the doping efficiencies in ZnSe nanocrystals. The analysis also elucidates the important role in determining the doping efficiency of ZnSe nanocrystals played by the chemical potentials of the growth precursor species, which determine the surface structure and morphology of the nanocrystals.
Author: Kipp van Schooten
Publisher: Springer Science & Business Media
ISBN: 3319005901
Category : Technology & Engineering
Languages : en
Pages : 102
Get Book Here
Book Description
Colloidal nanocrystals show much promise as an optoelectronics architecture due to facile control over electronic properties afforded by chemical control of size, shape, and heterostructure. Unfortunately, realizing practical devices has been forestalled by the ubiquitous presence of charge "trap" states which compete with band-edge excitons and result in limited device efficiencies. Little is known about the defining characteristics of these traps, making engineered strategies for their removal difficult. This thesis outlines pulsed optically detected magnetic resonance as a powerful spectroscopy of the chemical and electronic nature of these deleterious states. Counterintuitive for such heavy atom materials, some trap species possess very long spin coherence lifetimes (up to 1.6 μs). This quality allows use of the trapped charge's magnetic moment as a local probe of the trap state itself and its local environment. Beyond state characterization, this spectroscopy can demonstrate novel effects in heterostructured nanocrystals, such as spatially-remote readout of spin information and the coherent control of light harvesting yield.
Author: Fumitoshi Kato
Publisher:
ISBN:
Category :
Languages : en
Pages :
Get Book Here
Book Description
Diluted magnetic semiconductor quantum dots (DMS-QDs) is a class of material prepared by introducing a small percentage of magnetic impurities to impart new magneto-optical properties to the host nanocrystal (NC). Such materials are regarded as promising candidates for their potential application in spintronic devices. The overall functionality of the DMS-QD is highly dependent on the dopant position within the host structure. A thorough understanding of the doping mechanism is, therefore, critical to gain better control over the dopant speciation in nanocrystal lattice and material properties. In this work, we utilized II-VI molecular clusters that are analogous to bulk semiconductors as model systems to obtain mechanistic insight into the doping process. More specifically, we developed new protocols for dopant speciation and to achieve precision doping in these clusters. These molecular clusters are often studied to gain a detailed understanding of the size-property relationship in quantum-confined semiconductor nanocrystals. However, studies of the doping of these structurally well-defined materials and the effect on the host properties are rare. The work presented here focuses on elucidating the solution dynamic of clusters in order to develop controlled doping strategies. The work is primarily centered on Mn2+ and Co2+ as the dopants and CdS molecular cluster as the host. Monitoring the relative peak intensity of both doped and undoped fragments of Mn2+ or Co2+ substituted CdS cluster by electrospray ionization mass spectrometry (ESI-MS) is demonstrated to be an effective method determining for dopant speciation. The cluster-cluster equilibria unraveled from our investigations led us to establish a process that allows for precision doping of clusters. Synthetic methods were formulated based on our understanding of equilibria to yield a larger sized cluster. Furthermore, the presence of impurity ions was found to have a significant impact on the equilibria as well, demonstrating that dopants participate in both cation exchange reactions and the cluster evolution. In addition, the solution dynamic of the isolated clusters was observed and shown to have higher sensitivity towards its surrounding environment. New equilibria were rapidly established once small traces of metal ions were introduced to a solution of pure clusters. The solvent and core chalcogenide ions were found to have a profound effect on the equilibrium as well as the disintegration and growth processes. The studies of solution dynamics presented in this work provide insights relevant to the development of synthetic routes for precise impurity ion doping at the molecular level and to the cluster growth mechanism.
Author: Alina Marie Schimpf
Publisher:
ISBN:
Category :
Languages : en
Pages : 229
Get Book Here
Book Description
This thesis presents investigations of semiconductor nanocrystals doped with impurity ions, excess charge carriers, or both. The introduction of excess charge carriers into colloidal semiconductor nanocrystals constitutes a longstanding challenge in the development of nanocrystal building blocks for various technologies including solar cells, photovoltaic devices and electroluminescent devices. Chapter 1 discusses methods for electronic doping in semiconductor nanocrystals, focusing on photodoping and aliovent doping strategies. Of the various successful strategies for electronic doping, photodoping is particularly useful as a post-synthetic method for reversible and quantifiable tuning of carrier density. Alternatively, aliovalently doped nanocrystals are attractive due to the great stability of charge carriers. Chapter 2 presents a comparative study of conduction-band electrons in colloidal ZnO nanocrystals added via photodoping or aliovalent doping. The studies show that, although they have very similar spectroscopic properties, the reactivites of the electrons are vastly different, owing to the relative mobilities of their charge-compensating cations. Chapters 3, 4 and 5 present investigations of the ability to add excess electrons to a variety of systems via photodoping. The study in Chapter 3 shows that the maximum number of elecrons that may be added photochemically is dependent on the nanocrystal volume, such that all nanocrystals may be photodoped to the same electron density. Furthermore, the identities of the sacrifical reductant and the charge-compensating cation determine the maximum photodoping density. For the first time, alkyl borohydrides were used as sacrificial reductants to photodope ZnO, leading to much larger carrier densities than previously observed. These findings informed the first demonstration of photodoping in CdE (E= S, Se, Te) nanocrystals, presented in Chapter 4. Chapter 5 presents a combination of photodoping and aliovalent doping in In2O3 nanocrystals to investigate the redox chemistries in In2O3 and ITO nanocrystals. The study shows that all nanocrystals have the same Fermi level, and Sn4[superscript +] stabilizes that conduction band to allow accumulation of excess delocalized electrons. Moreover, regardless of Sn4[superscript +] doping and therefore of initial carrier density, all nanocrystals have the same number of electrons that may be added photochemically. These results, in conjunction with those presented in Chapters 3 and 4, suggest maximum photodoping density is thermodynamically limited, and is not an intrinsic property of the nanocrystal, nor a result of competition between productive hole-quenching and non-productive Auger recombination in the photoexcited nanocrystals. The ability to reversibly tune the carrier densities in colloidal semiconductor nanocrystals via photodoping allows new photophsyical investigations of electronically doped systems. Chapters 5 and 6 use photodoping to investigate the properties of plasmon resonances in ZnO and In2O3 nanocrystals. Chapter 5 shows that the plasmon energy is affected by both carrier density and Sn4[superscript +] doping. Chapter 6 shows that plasmons in ZnO nanocrystals are subject to quantum confinement and therefore may not be understood with a classical Drude picture. The large magnetic exchange interaction between charge carriers and magnetic dopants make diluted magnetic semiconductors (DMSs) particularly attractive for spin-based information processing. Chapter 7 uses pulsed electron paramagnetic resonance (pEPR) spectroscopy to investigate the affect of excess electrons on the Mn2[superscript +] spin dynamics in doped ZnO nancorystals, showing that Mn2[superscript +] spin relaxation is greatly accelerated by the presence of even one conduction-band electron. Chapter 8 uses pEPR to investigate the intrinsic spin dynamics of Mn2[superscript] in a variety of II-VI colloidal semiconductor nanocrystals. Finally, Chapter 9 shows the ability to tune the effective g value in DMSs at low fields using temperature.
Author: Vladimir Lesnyak
Publisher: Frontiers Media SA
ISBN: 2889632695
Category :
Languages : en
Pages : 110
Get Book Here
Book Description
Author:
Publisher:
ISBN:
Category :
Languages : en
Pages : 6
Get Book Here
Book Description
Strong quantum confinement in semiconductors can compress the wavefunctions of band electrons and holes to nanometre-scale volumes, significantly enhancing interactions between themselves and individual dopants. In magnetically doped semiconductors, where paramagnetic dopants (such as Mn2+, Co2+ and so on) couple to band carriers via strong sp-d spin exchange, giant magneto-optical effects can therefore be realized in confined geometries using few or even single impurity spins. Importantly, however, thermodynamic spin fluctuations become increasingly relevant in this few-spin limit. In nanoscale volumes, the statistical √N fluctuations of N spins are expected to generate giant effective magnetic fields Beff, which should dramatically impact carrier spin dynamics, even in the absence of any applied field. In this paper, we directly and unambiguously reveal the large Beff that exist in Mn2+-doped CdSe colloidal nanocrystals using ultrafast optical spectroscopy. At zero applied magnetic field, extremely rapid (300-600 GHz) spin precession of photoinjected electrons is observed, indicating Beff ~ 15-30 T for electrons. Precession frequencies exceed 2 THz in applied magnetic fields. Finally, these signals arise from electron precession about the random fields due to statistically incomplete cancellation of the embedded Mn2+ moments, thereby revealing the initial coherent dynamics of magnetic polaron formation, and highlighting the importance of magnetization fluctuations on carrier spin dynamics in nanomaterials.
Author: Tahereh Sabergharesou
Publisher:
ISBN:
Category :
Languages : en
Pages :
Get Book Here
Book Description
Diluted magnetic semiconductor oxides (DMSOs) have received great attention recently due to their outstanding applications in optoelectronic and spintronic devices. Ever since the initial observation of ferromagnetism at room temperature in cobalt-doped titania, extensive effort is concentrated on preparation of transition metal doped wide band gap semiconductors, especially Mn- doped ZnO. Compared to Mn-doped ZnO, magnetic interactions in SnO! and In!O! semiconductors have been underexplored. SnO! and In!O! semiconductors have many applications, owing to their high charge carrier density and mobility as well as high optical transparency. Investigation on electronic structure changes induced by dopants during the synthesis procedure can effectively influence magnetic interactions between charge carriers. In this work, a combination of structural and spectroscopic methods was used to probe as-synthesized SnO! and In!O! nanocrystals doped with Mn!! and Mn!! as precursors. X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectroscopy are powerful techniques to explore formal oxidation state of manganese dopant, electronic environment, number of nearest neighbors around the absorbent, and bond lengths to the neighboring atoms. Analysis reveals the presence of multiple oxidation states in the doped nanocrystals, and establishes a relation between!"!! ratio and expansion or contraction of lattice parameters.!"!! Although doping semiconductors are crucial for manipulating the functional properties, the influence of dopants on nanocrystals structure is not well understood. Nanocrystalline films prepared from colloidal Mn-doped SnO! and In!O! nanocrystals through spin coating process exhibit ferromagnetic behavior in temperatures ranging from 5 K to 300 K. Magnetic transformation from paramagnetic in free-standing Mn-doped nanocrystals to strong ferromagnetic ordering in nanocrystalline films is attributed to the formation of extended structural defects, e.g., oxygen vacancies at the nanocrystals interface. Magnetic circular dichroism (MCD) studies clearly show that Mn!! occupies different symmetry sites in indium oxide, when bixbyite and rhombohedral In!O! nanocrystals (NCs) are compared.
