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InGaN quantum dot formation mechanism on hexagonal GaN/InGaN/GaN pyramids
Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, The Institute of Technology.ORCID iD: 0000-0003-3203-7935
Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
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2012 (English)In: Nanotechnology, ISSN 0957-4484, E-ISSN 1361-6528, Vol. 23, no 30, 305708- p.Article in journal (Refereed) Published
Abstract [en]

Growing InGaN quantum dots (QDs) at the apex of hexagonal GaN pyramids is an elegant approach to achieve a deterministic positioning of QDs. Despite similar synthesis procedures by metal–organic chemical vapor deposition, the optical properties of the QDs reported in the literature vary drastically. The QDs tend to exhibit either narrow or broad emission lines in the micro-photoluminescence spectra. By coupled microstructural and optical investigations, the QDs giving rise to narrow emission lines were concluded to nucleate in association with a (0001) facet at the apex of the GaN pyramid.

Place, publisher, year, edition, pages
Institute of Physics (IOP), 2012. Vol. 23, no 30, 305708- p.
National Category
Atom and Molecular Physics and Optics
Identifiers
URN: urn:nbn:se:liu:diva-79321DOI: 10.1088/0957-4484/23/30/305708ISI: 000306333500030OAI: oai:DiVA.org:liu-79321DiVA: diva2:540387
Available from: 2012-07-10 Created: 2012-07-10 Last updated: 2017-12-07Bibliographically approved
In thesis
1. Controlled growth of hexagonal GaN pyramids and InGaN QDs
Open this publication in new window or tab >>Controlled growth of hexagonal GaN pyramids and InGaN QDs
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Gallium-nitride (GaN) and its related alloys are direct band gap semiconductors, with a wide variety of applications. The white light emitting diode (LED) is of particular importance as it is expected to replace energy inefficient light bulb and hazardous incandescent lamps used today. However, today’s planar hetero epitaxial grown LEDs  structures contain an unavoidable number of dislocations, which serves as non-radiative recombination centers. The dislocations harm the luminous efficiency of the LEDs and generate additional heat. Pseudomorphically grown quantum dots (QDs) are expected to be dislocation free thus the injected carriers captured by the QDs essentially recombine radiatively since the dislocations remain outside the QD. Furthermore the continuous character of the density of states in bulk materials is redistributed when the size of the dot is reduced within the Bohr radius of the material. Fully discret energy levels are eventually reached, which offers additional control of the optical properties. The Coulomb interaction between the confined carriers also has influence on the emission energy of the recombining carriers, which opens up the possibility of manufacturing novel light sources such as the single photon emitter. Single photon emitters are essential building blocks for quantum cryptography and teleportation applications.

The main contribution of the present work is the investigation of growth and characterization of sitecontrolled indium-gallium-nitride QDs embedded in GaN matrixes. The goal has been to demonstrate the ability to grow site-controlled InGaN QDs at the apex of hexagonal GaN pyramids in a controlled way using hot-wall metal organic chemical vapor deposition (MOCVD). Strong emphasis was set on the controlled growth of InGaN QDs. For example the growth of a single InGaN QD located at the apex of hexagonal GaN pyramids with tunable emission energy, the QD emission energy impact on the mask design, and a novel approach for the growth of InGaN QDs with polarization deterministic photon vectors were reported. The thesis is mainly based on experimental investigations by secondary electron microscope (SEM), micro photo-luminescence (μPL), and scanning transition electron microscopy ((S)TEM) characterization techniques.

In Paper 1 and 2, we present the growth of symmetric GaN hexagonal pyramids which served as template for the InGaN QDs grown. In paper 1, it was concluded that the selective area growth (SAG) of hexagonal GaN pyramids by MOCVD through symmetric openings in a SIN mask roughly can be divided in two regimes where either the pyramid expands laterally or not. When the pyramid expanded laterally the resulting pyramid apex became (0001) truncated even after prolonged growth times. Lateral expansion also had major impact on the pyramid-to-pyramid uniformity. In paper 2, the MOCVD process parameter impact on the pyramid morphology was investigated. By tuning the growth temperature, the ammonia, and TMGa-flows a self limited pyramid structure with only {1101} facets visible was achieved. The presence of the {1101}, {1102}, and {1100} facets were discussed from surface stabilities under various growth conditions.

Paper 3 and 4 concern the growth of InGaN QDs located at the apex of hexagonal GaN pyramids. In paper 3, we showed that it is possible to grow single QDs at the apex of hexagonal pyramids with emission line widths in the Ångström range. The QD emission energy was demonstrated to be tunable by the growth temperature. Basic spectroscopy data is also presented on a single QD in paper 3. In paper 4, the growth mechanisms of the QDs presented in paper 3 are presented. We concluded that (0001) truncated GaN pyramid base initiated the growth of InGaN QDs which gave rise to narrow luminescence peaks in the μPL spectra.

In paper 5, the QD emission energy impact of the mask design was investigated. To our big surprise the QD emission energy increased with increasing pyramid pitch while the emission energy of the InGaN quantum wells located on the {1101} facets of the pyramids energetically shifted towards lower energies. The energy shift at the apex was found to be associated with the (0001) truncation diameter of the underlying GaN pyramid since no energy shift was observed for (0001) truncated pyramids with truncation diameters larger than 100 nm.

In paper 6, the symmetry of the GaN pyramids were intentionally broken through the introduction of elongated openings in the SiN mask (symmetric openings was used in the previous five papers). The emission polarization vectors of the subsequently grown InGaN QDs were deterministically linked to the in-plane orientation of the pyramid it was nucleated upon, implying that the QDs inhibit an inplane anisotropy directly inherited from the pyramid template.

Finally, paper 7 describes a hot-wall MOCVD reactor improvement by inserting insulating pyrolytic boron-nitride (PBN) stripes in the growth chamber. By doing this, we have completely eliminated the arcing problem between different susceptor parts. As a consequence, the reactor gained run-to-run reproducibility. Growth of state of the art advanced aluminum-gallium-nitride high electron mobility transistor structures on a 100 mm wafer with electron mobility above 2000 Vs/cm2 was demonstrated by the improved process.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2012. 53 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1464
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-79326 (URN)978-91-7519-842-2 (ISBN)
Public defence
2012-09-20, Planck, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2012-07-10 Created: 2012-07-10 Last updated: 2012-12-04Bibliographically approved
2. InGaN Quantum Dots Grown on GaN Pyramid Arrays
Open this publication in new window or tab >>InGaN Quantum Dots Grown on GaN Pyramid Arrays
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Selective-area growth (SAG) of InGaN on GaN pyramids, which allows the formation of additional hybrid quantum structures, including quantum wires and quantum dots (QDs) in a site-controlled fashion, is attractive for both fundamental research and device application. The site-controlled growth of QDs showing sharp emission lines is seen as the first step toward the frontier quantum information application (QIA). Note that, in such case, one QD represents one device unless the challenge of fabricating identical QDs is overcome.

The concept of SAG GaN pyramids hosting InGaN QDs has been reported since 2000. However, the observation of sharp emission lines, which can be ascribed to three-dimensional carrier confinement in QDs, seems to be occasional.

The main outcome of this work is the investigation of the InGaN QDs grown on GaN hexagonal pyramids. This work covers the formation mechanism of InGaN QDs to the emission properties of individual InGaN QDs. A modified SAG approach to obtain InGaN QDs emitting photons with heralded polarization directions is also demonstrated. The inherent high polarization degree of photons emitted by InGaN QDs together with heralded polarization direction reveals a promising potential for the direct generation of linearly-polarized photons by site-controlled InGaN QDs.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2013. 59 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1534
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-97412 (URN)978-91-7519-550-6 (ISBN)
Public defence
2013-09-05, Planck, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2013-09-12 Created: 2013-09-12 Last updated: 2013-09-16Bibliographically approved
3. Photoluminescence Characteristics of III-Nitride Quantum Dots and Films
Open this publication in new window or tab >>Photoluminescence Characteristics of III-Nitride Quantum Dots and Films
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

III-Nitride semiconductors are very promising in both electronics and optical devices. The ability of the III-Nitride semiconductors as light emitters to span the electromagnetic spectrum from deep ultraviolet light, through the entire visible region, and into the infrared part of the spectrum, is a very important feature, making this material very important in the field of light emitting devices. In fact, the blue emission from Indium Gallium Nitride (InGaN), which was awarded the 2014 Nobel Prize in Physics, is the basis of the common and important white light emitting diode (LED).

Quantum dots (QDs) have properties that make them very interesting for light emitting devices for a range of different applications, such as the possibility of increasing device efficiency. The spectrally well-defined emission from QDs also allows accurate color reproduction and high-performance communication devices. The small size of QDs, combined with selective area growth allows for an improved display resolution. By control of the polarization direction of QDs, they can be used in more efficient displays as well as in traditional communication devices. The possibility of sending out entangled photon pairs is another QD property of importance for quantum key distribution used for secure communication.

QDs can hold different exciton complexes, such as the neutral single exciton, consisting of one electron and one hole, and the biexciton, consisting of two excitons. The integrated PL intensity of the biexciton exhibits a quadratic dependence with respect to the excitation power, as compared to the linear power dependence of the neutral single exciton. The lifetime of the neutral exciton is 880 ps, whereas the biexciton, consisting of twice the number of charge carriers and lacks a dark state, has a considerably shorter lifetime of only 500 ps. The ratio of the lifetimes is an indication that the size of the QD is in the order of the exciton Bohr radius of the InGaN crystal making up these QDs in the InGaN QW.

A large part of the studies of this thesis has been focused on InGaN QDs on top of hexagonal Gallium Nitride (GaN) pyramids, selectively grown by Metal Organic Chemical Vapor Deposition (MOCVD). On top of the GaN pyramids, an InGaN layer and a GaN capping layer were grown. From structural and optical investigations, InGaN QDs have been characterized as growing on (0001) facets on truncated GaN pyramids. These QDs exhibit both narrow photoluminescence linewidths and are linearly polarized in directions following the symmetry of the pyramids.

In this work, the neutral single exciton, and the more rare negatively charged exciton, have been investigated. At low excitation power, the integrated intensity of the PL peak of the neutral exciton increases linearly with the excitation power. The negatively charged exciton, on the other hand, exhibits a quadratic power dependence, just like that of the biexciton. Upon increasing the temperature, the power dependence of the negatively charged exciton changes to linear, just like the neutral exciton. This change in power dependence is explained in terms of electrons in potential traps close to the QD escaping by thermal excitation, leading to a surplus of electrons in the vicinity of the QD. Consequently, only a single exciton needs to be created by photoexcitation in order to form a negatively charged exciton, while the extra electron is supplied to the QD by thermal excitation.

Upon a close inspection of the PL of the neutral exciton, a splitting of the peak of just below 0.4 meV is revealed. There is an observed competition in the integrated intensity between these two peaks, similar to that between an exciton and a biexciton. The high energy peak of this split exciton emission is explained in terms of a remotely charged exciton. This exciton state consists of a neutral single exciton in the QD with an extra electron or hole in close vicinity of the QD, which screens the built-in field in the QD.

The InGaN QDs are very small; estimated to be on the order of the exciton Bohr radius of the InGaN crystal, or even smaller. The lifetimes of the neutral exciton and the negatively charged exciton are approximately 320 ps and 130 ps, respectively. The ratio of the lifetimes supports the claim of the QD size being on the order of the exciton Bohr radius or smaller, as is further supported by power dependence results. Under the assumption of a spherical QD, theoretical calculations predict an emission energy shift of 0.7 meV, for a peak at 3.09 eV, due to the built-in field for a QD with a diameter of 1.3 nm, in agreement with the experimental observations.

Studying the InGaN QD PL from neutral and charged excitons at elevated temperatures (4 K to 166 K) has revealed that the QDs are surrounded by potential fluctuations that trap charge carriers with an energy of around 20 meV, to be compared with the exciton trapping energy in the QDs of approximately 50 meV. The confinement of electrons close to the QD is predicted to be smaller than for holes, which accounts for the negative charge of the charged exciton, and for the higher probability of capturing free electrons. We have estimated the lifetimes of free electrons and holes in the GaN barrier to be 45 ps and 60 ps, in consistence with excitons forming quickly in the barrier upon photoexcitation and that free electrons and holes get trapped quickly in local potential traps close to the QDs. This analysis also indicates that there is a probability of 35 % to have an electron in the QD between the photoexcitation pulses, in agreement with a lower than quadratic power dependence of the negatively charged exciton.

InN is an attractive material due to its infrared emission, for applications such as light emitters for communication purposes, but it is more difficult to grow with high quality and low doping concentration as compared to GaN. QDs with a higher In-composition or even pure InN is an interesting prospect as being a route towards increased quantum confinement and room temperature device operation. For all optical devices, p-type doping is needed. Even nominally undoped InN samples tend to be heavily n-type doped, causing problems to make pn-junctions as needed for LEDs. In our work, we present Mg-doped p-type InN films, which when further increasing the Mg-concentration revert to n-type conductivity. We have focused on the effect of the Mg-doping on the light emission properties of these films. The low Mg doped InN film is inhomogeneous and is observed to contain areas with n-type conductivity, so called n-type pockets in the otherwise p-type InN film. A higher concentration of Mg results in a higher crystalline quality and the disappearance of the n-type pockets. The high crystalline quality has enabled us to determine the binding energy of the Mg dopants to 64 meV. Upon further increase of the Mg concentration, the film reverts to ntype conductivity. The highly Mg doped sample also exhibits a red-shifted emission with features that are interpreted as originating from Zinc-Blende inclusions in the Wurtzite InN crystal, acting as quantum wells. The Mg doping is an important factor in controlling the conductivity of InN, as well as its light emission properties, and ultimately construct InN-based devices.

In summary, in this thesis, both pyramidal InGaN QDs and InGaN QDs in a QW have been investigated. Novel discoveries of exciton complexes in these QD systems have been reported. Knowledge has also been gained about the challenging material InN, including a study of the effect of the Mg-doping concentration on the semiconductor crystalline quality and its light emission properties. The outcome of this thesis enriches the knowledge of the III-Nitride semiconductor community, with the long-term objective to improve the device performance of III-Nitride based light emitting devices.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2017. 45 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1867
National Category
Condensed Matter Physics Atom and Molecular Physics and Optics Other Physics Topics Theoretical Chemistry Materials Chemistry
Identifiers
urn:nbn:se:liu:diva-139766 (URN)10.3384/diss.diva-139766 (DOI)978-91-7685-487-7 (ISBN)
Public defence
2017-09-04, Planck, Fysikhuset, Campus Valla, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2017-08-15 Created: 2017-08-15 Last updated: 2017-08-17Bibliographically approved

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