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- All Subjects: Condensed Matter Physics
- All Subjects: Surface chemistry
- Creators: Menéndez, Jose
Description
The thesis studies new methods to fabricate optoelectronic Ge1-ySny/Si(100) alloys and investigate their photoluminescence (PL) properties for possible applications in Si-based photonics including IR lasers. The work initially investigated the origin of the difference between the PL spectrum of bulk Ge, dominated by indirect gap emission, and the PL spectrum of Ge-on-Si films, dominated by direct gap emission. It was found that the difference is due to the supression of self-absorption effects in Ge films, combined with a deviation from quasi-equilibrium conditions in the conduction band of undoped films. The latter is confirmed by a model suggesting that the deviation is caused by the shorter recombination lifetime in the films relative to bulk Ge. The knowledge acquired from this work was then utilized to study the PL properties of n-type Ge1-ySny/Si (y=0.004-0.04) samples grown via chemical vapor deposition of Ge2H6/SnD4/P(GeH3)3. It was found that the emission intensity (I) of these samples is at least 10x stronger than observed in un-doped counterparts and that the Idir/Iind ratio of direct over indirect gap emission increases for high-Sn contents due to the reduced gamma-L valley separation, as expected. Next the PL investigation was expanded to samples with y=0.05-0.09 grown via a new method using the more reactive Ge3H8 in place of Ge2H6. Optical quality, 1-um thick Ge1-ySny/Si(100) layers were produced using Ge3H10/SnD4 and found to exhibit strong, tunable PL near the threshold of the direct-indirect bandgap crossover. A byproduct of this study was the development of an enhanced process to produce Ge3H8, Ge4H10, and Ge5H12 analogs for application in ultra-low temperature deposition of Group-IV semiconductors. The thesis also studies synthesis routes of an entirely new class of semiconductor compounds and alloys described by Si5-2y(III-V)y (III=Al, V= As, P) comprising of specifically designed diamond-like structures based on a Si parent lattice incorporating isolated III-V units. The common theme of the two thesis topics is the development of new mono-crystalline materials on ubiquitous silicon platforms with the objective of enhancing the optoelectronic performance of Si and Ge semiconductors, potentially leading to the design of next generation optical devices including lasers, detectors and solar cells.
ContributorsGrzybowski, Gordon (Author) / Kouvetakis, John (Thesis advisor) / Chizmeshya, Andrew (Committee member) / Menéndez, Jose (Committee member) / Arizona State University (Publisher)
Created2013
Description
The work contained in this dissertation is focused on the optical properties of direct band gap semiconductors which crystallize in a wurtzite structure: more specifically, the III-nitrides and ZnO. By using cathodoluminescence spectroscopy, many of their properties have been investigated, including band gaps, defect energy levels, carrier lifetimes, strain states, exciton binding energies, and effects of electron irradiation on luminescence. Part of this work is focused on p-type Mg-doped GaN and InGaN. These materials are extremely important for the fabrication of visible light emitting diodes and diode lasers and their complex nature is currently not entirely understood. The luminescence of Mg-doped GaN films has been correlated with electrical and structural measurements in order to understand the behavior of hydrogen in the material. Deeply-bound excitons emitting near 3.37 and 3.42 eV are observed in films with a significant hydrogen concentration during cathodoluminescence at liquid helium temperatures. These radiative transitions are unstable during electron irradiation. Our observations suggest a hydrogen-related nature, as opposed to a previous assignment of stacking fault luminescence. The intensity of the 3.37 eV transition can be correlated with the electrical activation of the Mg acceptors. Next, the acceptor energy level of Mg in InGaN is shown to decrease significantly with an increase in the indium composition. This also corresponds to a decrease in the resistivity of these films. In addition, the hole concentration in multiple quantum well light emitting diode structures is much more uniform in the active region when Mg-doped InGaN (instead of Mg-doped GaN) is used. These results will help improve the efficiency of light emitting diodes, especially in the green/yellow color range. Also, the improved hole transport may prove to be important for the development of photovoltaic devices. Cathodoluminescence studies have also been performed on nanoindented ZnO crystals. Bulk, single crystal ZnO was indented using a sub-micron spherical diamond tip on various surface orientations. The resistance to deformation (the "hardness") of each surface orientation was measured, with the c-plane being the most resistive. This is due to the orientation of the easy glide planes, the c-planes, being positioned perpendicularly to the applied load. The a-plane oriented crystal is the least resistive to deformation. Cathodoluminescence imaging allows for the correlation of the luminescence with the regions located near the indentation. Sub-nanometer shifts in the band edge emission have been assigned to residual strain the crystals. The a- and m-plane oriented crystals show two-fold symmetry with regions of compressive and tensile strain located parallel and perpendicular to the ±c-directions, respectively. The c-plane oriented crystal shows six-fold symmetry with regions of tensile strain extending along the six equivalent a-directions.
ContributorsJuday, Reid (Author) / Ponce, Fernando A. (Thesis advisor) / Drucker, Jeff (Committee member) / Mccartney, Martha R (Committee member) / Menéndez, Jose (Committee member) / Shumway, John (Committee member) / Arizona State University (Publisher)
Created2013
Description
Nitride semiconductors have wide applications in electronics and optoelectronics technologies. Understanding the nature of the optical recombination process and its effects on luminescence efficiency is important for the development of novel devices. This dissertation deals with the optical properties of nitride semiconductors, including GaN epitaxial layers and more complex heterostructures. The emission characteristics are examined by cathodoluminescence spectroscopy and imaging, and are correlated with the structural and electrical properties studied by transmission electron microscopy and electron holography. Four major areas are covered in this dissertation, which are described next. The effect of strain on the emission characteristics in wurtzite GaN has been studied. The values of the residual strain in GaN epilayers with different dislocation densities are determined by x-ray diffraction, and the relationship between exciton emission energy and the in-plane residual strain is demonstrated. It shows that the emission energy increases withthe magnitude of the in-plane compressive strain. The temperature dependence of the emission characteristics in cubic GaN has been studied. It is observed that the exciton emission and donor-acceptor pair recombination behave differently with temperature. The donor-bound exciton binding energy has been measured to be 13 meV from the temperature dependence of the emission spectrum. It is also found that the ionization energies for both acceptors and donors are smaller in cubic compared with hexagonal structures, which should contribute to higher doping efficiencies. A comprehensive study on the structural and optical properties is presented for InGaN/GaN quantum wells emitting in the blue, green, and yellow regions of the electromagnetic spectrum. Transmission electron microscopy images indicate the presence of indium inhomogeneties which should be responsible for carrier localization. The temperature dependence of emission luminescence shows that the carrier localization effects become more significant with increasing emission wavelength. On the other hand, the effect of non-radiative recombination on luminescence efficiency also varies with the emission wavelength. The fast increase of the non-radiative recombination rate with temperature in the green emitting QWs contributes to the lower efficiency compared with the blue emitting QWs. The possible saturation of non-radiative recombination above 100 K may explain the unexpected high emission efficiency for the yellow emitting QWs Finally, the effects of InGaN underlayers on the electronic and optical properties of InGaN/GaN quantum wells emitting in visible spectral regions have been studied. A significant improvement of the emission efficiency is observed, which is associated with a blue shift in the emission energy, a reduced recombination lifetime, an increased spatial homogeneity in the luminescence, and a weaker internal field across the quantum wells. These are explained by a partial strain relaxation introduced by the InGaN underlayer, which is measured by reciprocal space mapping of the x-ray diffraction intensity.
ContributorsLi, Di (Author) / Ponce, Fernando (Thesis advisor) / Culbertson, Robert (Committee member) / Yu, Hongbin (Committee member) / Shumway, John (Committee member) / Menéndez, Jose (Committee member) / Arizona State University (Publisher)
Created2012
Description
The theory of geometric quantum mechanics describes a quantum system as a Hamiltonian dynamical system, with a projective Hilbert space regarded as the phase space. This thesis extends the theory by including some aspects of the symplectic topology of the quantum phase space. It is shown that the quantum mechanical uncertainty principle is a special case of an inequality from J-holomorphic map theory, that is, J-holomorphic curves minimize the difference between the quantum covariance matrix determinant and a symplectic area. An immediate consequence is that a minimal determinant is a topological invariant, within a fixed homology class of the curve. Various choices of quantum operators are studied with reference to the implications of the J-holomorphic condition. The mean curvature vector field and Maslov class are calculated for a lagrangian torus of an integrable quantum system. The mean curvature one-form is simply related to the canonical connection which determines the geometric phases and polarization linear response. Adiabatic deformations of a quantum system are analyzed in terms of vector bundle classifying maps and related to the mean curvature flow of quantum states. The dielectric response function for a periodic solid is calculated to be the curvature of a connection on a vector bundle.
ContributorsSanborn, Barbara (Author) / Suslov, Sergei K (Thesis advisor) / Suslov, Sergei (Committee member) / Spielberg, John (Committee member) / Quigg, John (Committee member) / Menéndez, Jose (Committee member) / Jones, Donald (Committee member) / Arizona State University (Publisher)
Created2011
Description
Optoelectronic and microelectronic applications of germanium-based materials have received considerable research interest in recent years. A novel method for Ge on Si heteroepitaxy required for such applications was developed via molecular epitaxy of Ge5H12. Next, As(GeH3)3, As(SiH3)3, SbD3, S(GeH3)2 and S(SiH3)2 molecular sources were utilized in degenerate n-type doping of Ge. The epitaxial Ge films produced in this work incorporate donor atoms at concentrations above the thermodynamic equilibrium limits. The donors are nearly fully activated, and led to films with lowest resistivity values thus far reported.
Band engineering of Ge was achieved by alloying with Sn. Epitaxy of the alloy layers was conducted on virtual Ge substrates, and made use of the germanium hydrides Ge2H6 and Ge3H8, and the Sn source SnD4. These films exhibit stronger emission than equivalent material deposited directly on Si, and the contributions from the direct and indirect edges can be separated. The indirect-direct crossover composition for Ge1-ySny alloys was determined by photoluminescence (PL). By n-type doping of the Ge1-ySny alloys via P(GeH3)3, P(SiH3)3 and As(SiH3)3, it was possible to enhance photoexcited emission by more than an order-of-magnitude.
The above techniques for deposition of direct gap Ge1-ySny alloys and doping of Ge were combined with p-type doping methods for Ge1-ySny using B2H6 to fabricate pin heterostructure diodes with active layer compositions up to y=0.137. These represent the first direct gap light emitting diodes made from group IV materials. The effect of the single defected n-i¬ interface in a n-Ge/i-Ge1-ySny/p-Ge1-zSnz architecture on electroluminescence (EL) was studied. This led to lattice engineering of the n-type contact layer to produce diodes of n-Ge1-xSnx/i-Ge1-ySny/p-Ge1-zSnz architecture which are devoid of interface defects and therefore exhibit more efficient EL than the previous design. Finally, n-Ge1-ySny/p-Ge1-zSnz pn junction devices were synthesized with varying composition and doping parameters to investigate the effect of these properties on EL.
Band engineering of Ge was achieved by alloying with Sn. Epitaxy of the alloy layers was conducted on virtual Ge substrates, and made use of the germanium hydrides Ge2H6 and Ge3H8, and the Sn source SnD4. These films exhibit stronger emission than equivalent material deposited directly on Si, and the contributions from the direct and indirect edges can be separated. The indirect-direct crossover composition for Ge1-ySny alloys was determined by photoluminescence (PL). By n-type doping of the Ge1-ySny alloys via P(GeH3)3, P(SiH3)3 and As(SiH3)3, it was possible to enhance photoexcited emission by more than an order-of-magnitude.
The above techniques for deposition of direct gap Ge1-ySny alloys and doping of Ge were combined with p-type doping methods for Ge1-ySny using B2H6 to fabricate pin heterostructure diodes with active layer compositions up to y=0.137. These represent the first direct gap light emitting diodes made from group IV materials. The effect of the single defected n-i¬ interface in a n-Ge/i-Ge1-ySny/p-Ge1-zSnz architecture on electroluminescence (EL) was studied. This led to lattice engineering of the n-type contact layer to produce diodes of n-Ge1-xSnx/i-Ge1-ySny/p-Ge1-zSnz architecture which are devoid of interface defects and therefore exhibit more efficient EL than the previous design. Finally, n-Ge1-ySny/p-Ge1-zSnz pn junction devices were synthesized with varying composition and doping parameters to investigate the effect of these properties on EL.
ContributorsSenaratne, Charutha Lasitha (Author) / Kouvetakis, John (Thesis advisor) / Chizmeshya, Andrew (Committee member) / Menéndez, Jose (Committee member) / Arizona State University (Publisher)
Created2016
Description
As the world energy demand increases, semiconductor devices with high energy conversion efficiency become more and more desirable. The energy conversion consists of two distinct processes, namely energy generation and usage. In this dissertation, novel multi-junction solar cells and light emitting diodes (LEDs) are proposed and studied for high energy conversion efficiency in both processes, respectively. The first half of this dissertation discusses the practically achievable energy conversion efficiency limit of solar cells. Since the demonstration of the Si solar cell in 1954, the performance of solar cells has been improved tremendously and recently reached 41.6% energy conversion efficiency. However, it seems rather challenging to further increase the solar cell efficiency. The state-of-the-art triple junction solar cells are analyzed to help understand the limiting factors. To address these issues, the monolithically integrated II-VI and III-V material system is proposed for solar cell applications. This material system covers the entire solar spectrum with a continuous selection of energy bandgaps and can be grown lattice matched on a GaSb substrate. Moreover, six four-junction solar cells are designed for AM0 and AM1.5D solar spectra based on this material system, and new design rules are proposed. The achievable conversion efficiencies for these designs are calculated using the commercial software package Silvaco with real material parameters. The second half of this dissertation studies the semiconductor luminescence refrigeration, which corresponds to over 100% energy usage efficiency. Although cooling has been realized in rare-earth doped glass by laser pumping, semiconductor based cooling is yet to be realized. In this work, a device structure that monolithically integrates a GaAs hemisphere with an InGaAs/GaAs quantum-well thin slab LED is proposed to realize cooling in semiconductor. The device electrical and optical performance is calculated. The proposed device then is fabricated using nine times photolithography and eight masks. The critical process steps, such as photoresist reflow and dry etch, are simulated to insure successful processing. Optical testing is done with the devices at various laser injection levels and the internal quantum efficiency, external quantum efficiency and extraction efficiency are measured.
ContributorsWu, Songnan (Author) / Zhang, Yong-Hang (Thesis advisor) / Menéndez, Jose (Committee member) / Ponce, Fernando (Committee member) / Belitsky, Andrei (Committee member) / Schroder, Dieter (Committee member) / Arizona State University (Publisher)
Created2010
Description
A highly uniform and repeatable method for synthesizing the single-layer transition metal dichalcogenides (TMDs) molybdenum disulfide, MoS2, and tungsten disulfide, WS2, was developed. This method employed chemical vapor deposition (CVD) of precursors in a custom built cold-wall reaction chamber designed to allow independent control over the growth parameters. Iterations of this reaction chamber were employed to overcome limitations to the growth method. First, molybdenum trioxide, MoO3, and S were co-evaporated from alumina coated W baskets to grow MoS2 on SiO2/Si substrates. Using this method, films were found to have repeatable coverage, but unrepeatable morphology. Second, the reaction chamber was modified to include a pair of custom bubbler delivery systems to transport diethyl sulfide (DES) and molybdenum hexacarbonyl (MHC) to the substrate as a S and Mo precursors. Third, tungsten hexacarbonyl (WHC) replaced MHC as a transition metal precursor for the synthesis of WS2 on Al2O3, substrates. This method proved repeatable in both coverage and morphology allowing the investigation of the effect of varying the flow of Ar, varying the substrate temperature and varying the flux of DES to the sample. Increasing each of these parameters was found to decrease the nucleation density on the sample and, with the exception of the Ar flow, induce multi-layer feature growth. This combination of precursors was also used to investigate the reported improvement in feature morphology when NaCl is placed upstream of the substrate. This was found to have no effect on experiments in the configurations used. A final effort was made to adequately increase the feature size by switching from DES to hydrogen sulfide, H2S, as a source of S. Using H2S and WHC to grow WS2 films on Al2O3, it was found that increasing the substrate temperature and increasing the H2S flow both decrease nucleation density. Increasing the H2S flow induced bi-layer growth. Ripening of synthesized WS2 crystals was demonstrated to occur when the sample was annealed, post-growth, in an Ar, H2, and H2S flow. Finally, it was verified that the final H2S and WHC growth method yielded repeatability and uniformity matching, or improving upon, the other methods and precursors investigated.
ContributorsLunceford, Chad (Author) / Drucker, Jeff (Thesis advisor) / Menéndez, Jose (Committee member) / Smith, David J. (Committee member) / Rez, Peter (Committee member) / Arizona State University (Publisher)
Created2019