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Dynamic characteristics of the exciton and the biexciton in a single InGaN quantum dot
Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, The Institute of Technology.
Linköping University, Department of Physics, Chemistry and Biology. Linköping University, The Institute of Technology.
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: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 101, no 6Article in journal (Refereed) Published
Abstract [en]

The dynamics of the exciton and the biexciton related emission from a single InGaN quantum dot (QD) have been measured by time-resolved microphotoluminescence spectroscopy. An exciton-biexciton pair of the same QD was identified by the combination of power dependence and polarization-resolved spectroscopy. Moreover, the spectral temperature evolution was utilized in order to distinguish the biexciton from a trion. Both the exciton and the biexciton related emission reveal mono-exponential decays corresponding to time constants of similar to 900 and similar to 500 ps, respectively. The obtained lifetime ratio of similar to 1.8 indicates that the QD is small, with a size comparable to the exciton Bohr radius.

Place, publisher, year, edition, pages
American Institute of Physics (AIP) , 2012. Vol. 101, no 6
National Category
Engineering and Technology
Identifiers
URN: urn:nbn:se:liu:diva-84908DOI: 10.1063/1.4742343ISI: 000307862400022OAI: oai:DiVA.org:liu-84908DiVA: diva2:562903
Note

Funding Agencies|Thaksin University in Thailand||Swedish Research Council (VR)||Swedish Foundation for Strategic Research (SSF)||Knut and Alice Wallenberg Foundation||

Available from: 2012-10-26 Created: 2012-10-26 Last updated: 2017-12-07
In thesis
1. Polarization-resolved photoluminescence spectroscopy of III-nitride quantum dots
Open this publication in new window or tab >>Polarization-resolved photoluminescence spectroscopy of III-nitride quantum dots
2013 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In this thesis, results from studies on (In)GaN quantum dots (QDs) are presented, including investigations of the structural, optical and electronic properties. The experimental studies were performed on GaN and InGaN QDs grown by molecular beam epitaxy, taking advantage of the Stranki-Krastanov growth mode for the GaN QD samples and the composition segregation for the InGaN QD samples.

Optical spectroscopy of the (In)GaN QDs was performed with a combination of different experimental techniques, e.g. stationary microphotoluminescence (μPL) and timeresolved μPL. The μPL spectroscopy is suitable for studies of single QDs due to the wellfocused excitation laser spot, and it typically does not require any special sample preparation. The powerful combination of power and polarization dependences was used to distinguish the exciton and the biexciton emissions from other emission lines in the recorded spectra.

The QDs could be observed with random in-plane anisotropy, as determined by the strong linear polarization for single QDs but with different angular orientation from dot to dot. Additionally, these experimental results are in good agreement with the computational results revealing a similar degree of polarization for the exciton and the biexciton emissions. Further, the theory predicts that the discrepancy of the polarization degree is larger between the positive and negative trions in comparison with the exciton and the biexciton. Based on this result, polarization resolved spectroscopy is proposed as a simple tool for the identification of trions and their charge states.

The fine-structure splitting (FSS) and the biexciton binding energy (Ebxx) are essential QD parameters of relevance for the possible generation of quantum entangled photon pairs in a cascade recombination of the biexciton. In general, the Coulomb interaction between the negatively charged electron and the positively charged hole lifts the fourfold degeneracy of the electron and hole pair ground state, forming a set of zero-dimensional exciton states of unequal energies. This Coulomb-induced splitting, referred to as the FSS, results in an electronic fine structure, which is strongly dependent on the symmetry of the exciton wave function. The FSS was in this work resolved and investigated for excitons in InGaN QDs, using polarization-sensitive μPL spectroscopy employed on the cleaved-edge of the samples. As expected, the FSS is found to exhibit identical magnitudes, but with reversed sign for the exciton and the biexciton. For quantum information applications, a vanishing FSS is required, since otherwise the emissions of the polarization-entangled photon pairs in the cascade biexciton recombination will be prohibited.

The biexcitons are found to exhibit both positive and negative binding energies for the investigated QDs. Since a negative binding energy indicates a repulsive Coulomb interaction, such biexcitons (or exciton complexes) cannot exist in structures of higher dimensionality. On the other hand, a biexciton with a negative binding energy can be found in QDs, since the exciton complexes still remain bound due to their three dimensional confinement. Moreover, the biexciton binding energy depends on the dot size, which implies that a careful size control of dots could enable manipulation of the biexciton binding energy. A large Ebxx value enables better and cheaper spectral filtering, in order to purify the single photon emission, while a proposed time reordering scheme relies on zero Ebxx for the generation of entangled photons.

The dynamics of the exciton and the biexciton emissions from InGaN QD were measured by means of time-resolved μPL. The lifetimes of the exciton related emissions are demonstrated to depend on the dot size. Both the exciton and the biexciton emissions reveal mono-exponential decays, with a biexciton lifetime, which is about two times shorter than the exciton lifetime. This implies that the QD is small, with a size comparable to the exciton Bohr radius. The photon generation rates can be manipulated by controlling the QDs size, which in turn can be utilized for generation of single- and entangled-photons on demand, with a potential for applications in e.g. quantum information.

The polarization of the emitted single photons can be manipulated by using a polarizer, but to the prize of photon loss and reduced emission intensity. Alternative methods to control the polarization of the emission light are a manipulation of the dot symmetry statically by its shape or dynamically by an externally applied electric field. Predictions based on performed calculations show that in materials with a small spin-orbit split-off energy (ΔSO), like the III-nitride materials, the polarization degree of the emission is more sensitive to dot asymmetry than in materials with a large value for ΔSO, e.g. the III-arsenide materials. Moreover, for an electric field applied in the 1͞10 and the 11͞2 directions of the zinc-blende lens-shaped QDs grown on the (111) plane, the polarization degree of InN QDs is found to be significantly more, by a factor of ~50 times, sensitive to the electric field than for GaN QDs. This work demonstrates that especially the InN based QD, are suitable for manipulation of the polarization by the direct control of the dot symmetry or by externally applied electric fields.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2013. 68 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1494
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-87748 (URN)978-91-7519-715-9 (ISBN)
Public defence
2013-02-07, Plank, Fysikhuset, Campus Valla, Linköpings universitet, Linköping, 10:15 (English)
Opponent
Supervisors
Available from: 2013-01-22 Created: 2013-01-22 Last updated: 2015-01-23Bibliographically approved
2. 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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