Investigations on the physical origin of lateral photovoltage in PbS-colloidal quantum dot/Si heterojunctions

Restricted area heterojunctions, an array of lead sulfide colloidal quantum dots (PbS-CQDs) and crystalline silicon, are studied with a non-destructive remote contact light beam induced current (RC-LBIC) technique. As well as getting good quality active area images we observed an anomalous unipolar signal response for the PbS-CQD/n-Si devices and a conventionally expected bipolar signal profile for the PbS-CQD/p-Si devices. Interestingly, our simulation results consistently yielded a unipolar and bipolar nature in the signals related to the PbSCQD/n-Si and PbS-CQD/p-Si heterostructures, respectively. In order to explain the physical mechanism involved in the unipolar signal response of the PbS-CQD/n-Si devices, we propose a model based on the band alignment in the heterojunctions, in addition to the distribution of photo-induced excess majority carriers across the junction. Given that the RC-LBIC technique is well suited to this context, the presence of these two distinct mechanisms (the bipolar and unipolar nature of the signals) needs to be considered in order to have a better interpretation of the data in the characterization of an array of homo/heterojunctions.

Growth and characterization of novel, III-V semiconductor heterostructures

The material presented in this thesis concerns the growth and characterization of III-V semiconductor heterostructures. Studies of the interactions between bound states in coupled quantum wells and between well and barrier bound states in AlAs/GaAs heterostructures are presented. We also demonstrate the broad array of novel tunnel structures realizable in the InAs/GaSb/AlSb material system. Because of the unique broken-gap band alignment of InAs/GaSb these structures involve transport between the conduction- and valence-bands of adjacent layers. These devices possess a wide range of electrical properties and are fundamentally different from conventional AlAs/GaAs tunnel devices. We report on the fabrication of a novel tunnel transistor with the largest reported room temperature current gains. We also present time-resolved studies of the growth fronts of InAs/GainSb strained layer superlattices and investigations of surface anion exchange reactions.

Chapter 2 covers tunneling studies of conventional AlAs/GaAs RTD's. The results of two studies are presented: (i) A test of coherent vs. sequential tunneling in triple barrier heterostructures, (ii) An optical measurement of the effect of barrier X-point states on Γ-point well states. In the first it was found if two quantum wells are separated by a sufficiently thin barrier, then the eigenstates of the system extend coherently across both wells and the central barriers. For thicker barriers between the wells, the electrons become localized in the individual wells and transport is best described by the electrons hopping between the wells. In the second, it was found that Γ-point well states and X-point barrier states interact strongly. The barrier X-point states modify the energies of the well states and increase the escape rate for carriers in the quantum well.

The results of several experimental studies of a novel class of tunnel devices realized in the InAs/GaSb/AlSb material system are presented in Chapter 3. These interband tunnel structures involve transport between conduction- and valence-band states in adjacent material layers. These devices are compared and contrasted with the conventional AlAs/GaAs structures discussed in Chapter 2 and experimental results are presented for both resonant and nonresonant devices. These results are compared with theoretical simulations and necessary extensions to the theoretical models are discussed.

In chapter 4 experimental results from a novel tunnel transistor are reported. The measured current gains in this transistor exceed 100 at room temperature. This is the highest reported gain at room temperature for any tunnel transistor. The device is analyzed and the current conduction and gain mechanisms are discussed.

Chapters 5 and 6 are studies of the growth of structures involving layers with different anions. Chapter 5 covers the growth of InAs/GainSb superlattices for far infrared detectors and time resolved, in-situ studies of their growth fronts. It was found that the bandgap of superlattices with identical layer thicknesses and compositions varied by as much as 40 meV depending on how their internal interfaces are formed. The absorption lengths in superlattices with identical bandgaps but whose interfaces were formed in different ways varied by as much as a factor of two. First the superlattice is discussed including an explanation of the device and the complications involved in its growth. The experimental technique of reflection high energy electron diffraction (RHEED) is reviewed, and the results of RHEED studies of the growth of these complicated structures are presented. The development of a time resolved, in-situ characterization of the internal interfaces of these superlattices is described. Chapter 6 describes the result of a detailed study of some of the phenomena described in chapter 5. X-ray photoelectron spectroscopy (XPS) studies of anion exchange reactions on the growth fronts of these superlattices are reported. Concurrent RHEED studies of the same physical systems studied with XPS are presented. Using the RHEED and XPS results, a real-time, indirect measurement of surface exchange reactions was developed.

Zn-VI/Cu2O Heterojunctions for Earth-Abundant Photovoltaics

The need for sustainable energy production motivates the study of photovoltaic materials, which convert energy from sunlight directly into electricity. This work has focused on the development of Cu₂O as an earth-abundant solar absorber due to the abundance of its constituent elements in the earth's crust, its suitable band gap, and its potential for low cost processing. Crystalline wafers of Cu₂O with minority carrier diffusion lengths on the order of microns can be manufactured in a uniquely simple fashion — directly from copper foils by thermal oxidation. Furthermore, Cu₂O has an optical band gap of 1.9 eV, which gives it a detailed balance energy conversion efficiency of 24.7% and the possibility for an independently connected Si/Cu₂O dual junction with a detailed balance efficiency of 44.3%.

However, the highest energy conversion efficiency achieved in a photovoltaic device with a Cu₂O absorber layer is currently only 5.38% despite the favorable optical and electronic properties listed above. There are several challenges to making a Cu₂O photovoltaic device, including an inability to dope the material, its relatively low chemical stability compared to other oxides, and a lack of suitable heterojunction partners due to an unusually small electron affinity. We have addressed the low chemical stability, namely the fact that Cu₂O is an especially reactive oxide due to its low enthalpy of formation (ΔH_f⁰ = -168.7 kJ/mol), by developing a novel surface preparation technique. We have addressed the lack of suitable heterojunction partners by investigating the heterojunction band alignment of several Zn-VI materials with Cu₂O. Finally, We have addressed the typically high series resistance of Cu₂O wafers by developing methods to make very thin, bulk Cu₂O, including devices on Cu₂O wafers as thin as 20 microns. Using these methods we have been able to achieve photovoltages over 1 V, and have demonstrated the potential of a new heterojunction material, Zn(O,S).

Role of interface dipole in metal gate/high-k effective work function modulation by aluminum incorporation

The interface dipole and its role in the effective work function (EWF) modulation by Al incorporation are investigated. Our study shows that the interface dipole located at the high-k/SiO2 interface causes an electrostatic potential difference across the metal/high-k interface, which significantly shifts the band alignment between the metal and high-k, consequently modulating the EWF. The electrochemical potential equalization and electrostatic potential methods are used to evaluate the interface dipole and its contribution. The calculated EWF modulation agrees with experimental data and can provide insight to the control of EWF in future pMOS technology.

p-type doping of GaInNAs quaternary alloys

Using the first-principles band-structure method, we investigate the p-type doping properties and band structural parameters of the random Ga1-xInxN1-yAsy quaternary alloys. We show that the Mg-Ga substitution is a better choice than ZnGa to realize the p-type doping because of the lower transition energy level and lower formation energy. The natural valence band alignment of GaAs and GaInNAs alloys is also calculated, and we find that the valence band maximum becomes higher with the increasing in composition. Therefore, we can tailor the band offset as desired which is helpful to confine the electrons effectively in optoelectronic devices. (C) 2008 Published by Elsevier B.V.

Molecular beam epitaxy growth and photoluminescence of type-II (GaAs1-xSbx/InyGa1-yAs)/GaAs bilayer quantum well

We report a systematical study on the molecular beam epitaxy growth and optical property of (GaAs1-xSbx/In-y Ga1-yAs)/GaAs bilayer quantum well (BQW) structures. It is shown that the growth temperature of the wells and the sequence of layer growth have significant influence on the interface quality and the subsequent photoluminescence (PL) spectra. Under optimized growth conditions, three high-quality (GaAsSb0.29/In0.4GaAs)/GaAs BQWs are successfully fabricated and a room temperature PL at 1314 nm is observed. The transition mechanism in the BQW is also discussed by photoluminescence and photoreflectance measurements. The results confirm experimentally a type-II band alignment of the interface between the GaAsSb and InGaAs layers.

Suppression of exciton recombination in symmetric GaAs0.7Sb0.3/GaAs/GaAs0.7P0.3 coupled quantum wells induced by an in-plane magnetic field

Suppression of the exciton recombination in GaAs0.7Sb0.3/GaAs/GaAs0.7P0.3 coupled quantum well (CQW) induced by an external magnetic field is investigated theoretically. Unlike the usual electro-Stark effect, the exciton energy dispersion of an exciton is modified by an external in-plane magnetic field, the ground state of the magnetoexciton shifts from a zero in-plane center of mass (CM) momentum to a finite CM momentum, and the Lorentz force induces the spatial separation of electron and hole. Consequently, this effect renders the ground state of magnetoexciton stable against radiative recombination due to momentum conservation. This effect depends sensitively on the thickness and height of GaAs0.7Sb0.3 layer, therefore it could provide us useful infometion about the band alignment of CQW. (C) 2004 American Institute of Physics.

Photoluminescence study of (GaAs1-xSbx/InyGa1-yAs)/GaAs bilayer quantum well grown by molecular beam epitaxy

Photoluminescence study of (GaAs1-xSbx/InyGa1-yAs)/GaAs bilayer quantum wells (BQWs) grown by molecular beam epitaxy (MBE) were carried out. Temperature and excitation power dependent photoluminescence (PL) study indicated that the band alignment of the BQWs is type - II. The origin of the double-peak luminescence was discussed. Under optimized growth conditions, the PL emission wavelength from the BQWs has been extend up to 1.31 mu m with a single peak at room temperature.

Molecular beam epitaxy growth and photoluminescence study of room temperature 1.31 mu m (InyGa1-yAs/GaAs1-x Sb-x)/ GaAs bilayer quantum wells

Molecular beam epitaxy (MBE) growth of (InyGa1-yAs/GaAs1-xSbx)/GaAs bilayer quantum well (BQW) structures has been investigated. It is evidenced by photo luminescence (PL) that a strong blue shift of the PL peak energy of 47 meV with increasing PL excitation power from 0.63 to 20 mW was observed, indicating type II band alignment of the BQW. The emission wavelength at room temperature from (InyGa1-yAs/GaAs1-xSbx)/GaAs BQW is longer (above 1.2 μ m) than that from InGaAs/GaAs and GaAsSb/GaAs SQW structures (1.1 μ m range), while the emission efficiency from the BQW structures is comparable to that of the SQW. Through optimizing growth conditions, we have obtained room temperature 1.31 μ m wavelength emission from the (InyGa1-yAs/GaAs1-xSbx)/GaAs BQW. Our results have proved experimentally that the GaAs-based bilayer (InyGa1-yAs/GaAs1-xSbx)/GaAs quantum well is a useful structure for the fabrication of near-infrared wavelength optoelectronic devices. © 2005 Elsevier B.V. All rights reserved.

Structural and optical properties of strain-compensated GaAsSb/GaAs quantum wells with high Sb composition

The structural and optical properties of GaAsSb/GaAs quantum wells (QWs) and strain-compensated GaAsP/GaAs/GaAsSb/GaAs/GaAsP QWs grown on a GaAs substrate by molecular beam epitaxy are investigated using high-resolution x-ray diffraction and photoluminescence (PL) measurements. We demonstrated that the insertion of tensile GaAsP layers into the active region of GaAsSb/GaAs QWs effectively improves the structural and optical quality. Even the Sb composition is as high as 0.39. The PL spectra at 11 K and room temperature indicate that the PL peak of strain-compensated QWs has a narrower linewidth and higher intensity in comparison to the sample without strain compensation. The results of PL peak blueshift with increasing excitation show the strain-compensated GaAsSb/GaAs interface characteristic of type-I band alignment. (C) 2003 American Institute of Physics.

Study of optical properties in GaAs1-xSbx/GaAs single quantum wells

GaAsSb/GaAs single quantum wells (SQWs) grown by molecular beam epitaxy are studied by selectively-excited photoluminescence (SEPL) measurement. For the first time, we have simultaneously observed the PL, from both type I and type II transitions in GaAsSb/GaAs heterostructure in the SEPL. The two transitions exhibit different PL, behaviours under different excitation energy. As expected, the peak energy of type I emission remains constant in the whole excitation energy range we used, while type U transition shows a significant blue shift with increasing excitation energy. The observed blue shift is well explained in terms of electron-hole charge separation model at the interface. Time-resolved(TR) PL exhibits more type 11 characteristic of GaAsSb/GaAs QW. Moreover, the results of the excitation-power-dependent PL and TRPL provide more direct information on the type-II nature of the band alignment in GaAsSb/GaAs quantum-well structures. By combining the experimental results with some simple calculations, we have obtained the strained and unstrained valence band offsets of Q(v) = 1.145 and Q(v)(0) = 0. 76 in our samples, respectively.

Temperature dependence of photoluminescence of flat and undulated SiGe/Si multiple quantum wells

Photoluminescence (PL) of strained SiGe/Si multiple quantum wells (MQW) with flat and undulated SiGe well layers was studied at different temperature. With elevated temperature from 10K, the no-phonon (NP) peak of the SiGe layers in the flat sample has firstly a blue shift due to the dominant transition converting from bound excitons (BE) to free excitons (FE), and then has a red shift when the temperature is higher than 30K because of the narrowing of the band gap. In the undulated sample, however, monotonous blue shift was observed as the temperature was elevated from 10 K to 287 K. The thermally activated electrons, confined in Si due to type-II band alignment, leak into the SiGe crest regions, and the leakage is enhanced with the elevated temperature. It results in a blue shift of the SiGe luminescence spectra.

Selectively excited photoluminescence of GaAs1-xSbx/GaAs single quantum wells

GaAsSb/GaAs single quantum wells grown by molecular-beam epitaxy are studied by selectively excited photoluminescence measurements. We have simultaneously observed the photoluminescence (PL) from both type-I and type-II transitions in the samples. The two transitions exhibit different PL behavior under different excitation energies. As expected, the peak energy of the type-I emission remains constant in the entire excitation energy range we used, while the type-II transition shows a significant blueshift with increasing excitation energy. The observed blueshift can be well explained by an electron-hole charge separation model at interface. This result, along with the excitation-power-dependent PL and the measured longer carrier decay time, provides more direct information on the type-II nature of the band alignment in GaAsSb/GaAs quantum well structures. (C) 2002 American Institute of Physics.

Electronic structure of diluted magnetic semiconductor superlattices: In-plane magnetic field effect

The electronic structure of diluted magnetic semiconductor (DMS) superlattices under an in-plane magnetic field is studied within the framework of the effective-mass theory; the strain effect is also included in the calculation. The numerical results show that an increase of the in-plane magnetic field renders the DMS superlattice from the direct band-gap system to the indirect band-gap system, and spatially separates the electron and the hole by changing the type-I band alignment to a type-II band alignment. The optical transition probability changes from type I to type II and back to type I like at large magnetic field. This phenomenon arises from the interplay among the superlattice potential profile, the external magnetic field, and the sp-d exchange interaction between the carriers and the magnetic ions. The shear strain induces a strong coupling of the light- and heavy-hole states and a transition of the hole ground states from "light"-hole to "heavy"-hole-like states.

Different transfer paths for thermally activated electrons and holes in self-organized Ge/Si(001) islands in a multilayer structure

We investigated the temperature dependence (10-250 K) of the photoluminescence (PL) emission spectrum of self-organized Ge/Si(001) islands in a multilayer structure. With elevated temperature, we find that the thermally activated holes and electrons are gathered by the Ge islands in different ways. The holes drift from the wetting layer into the islands, while the electrons, confined in Si due to type-II band alignment, leak into the Ge islands by the electrostatic interaction with the holes accumulated there. It results in an increase of the integrated intensity of island-related PL at a certain temperature range and a reduction of the phonon energy in the phonon-assisted PL of the islands by involving a type-I transition into a type-II transition. (C) 2001 American Institute of Physics.