Tim J. Puchtler

Morphological, structural, and emission characterization of trench defects in InGaN/GaN quantum well structures

In a wide variety of InGaN/GaN quantum well (QW) structures, defects are observed which consist of a trench partially or fully enclosing a region of the QW having altered emission properties. For various different defect morphologies, cathodoluminescence studies suggest that the emission is redshifted in the enclosed region. Based on transmission electron microscopy and atomic force microscopy data, we suggest that the sub-surface structure of the trench defect consists of a basal plane stacking fault bounded by a stacking mismatch boundary, which terminates at the apex of a V-shaped trench.

Distinctive signature of indium gallium nitride quantum dot lasing in microdisk cavities.

Significance The III-nitride family of materials has already demonstrated tremendous optical efficiency and versatility for devices across a broad range of wavelengths. Quantum dots formed in these materials, with advantages such as improved carrier confinement, should offer even greater device efficiency. They are also important constituents for fundamental studies of light−matter interaction. However, that promise has been far from realized, and this is a complex problem to address. This work, through a comparative study of quantum dot, quantum well, and fragmented quantum well gain media in compact microdisk cavities, allows better understanding of the limitations to lasing for the quantum dot samples. These results allow both improved device efficiency and fundamental insights into quantum dot−cavity interactions in these materials. Low-threshold lasers realized within compact, high-quality optical cavities enable a variety of nanophotonics applications. Gallium nitride materials containing indium gallium nitride (InGaN) quantum dots and quantum wells offer an outstanding platform to study light−matter interactions and realize practical devices such as efficient light-emitting diodes and nanolasers. Despite progress in the growth and characterization of InGaN quantum dots, their advantages as the gain medium in low-threshold lasers have not been clearly demonstrated. This work seeks to better understand the reasons for these limitations by focusing on the simpler, limited-mode microdisk cavities, and by carrying out comparisons of lasing dynamics in those cavities using varying gain media including InGaN quantum wells, fragmented quantum wells, and a combination of fragmented quantum wells with quantum dots. For each gain medium, we use the distinctive, high-quality (Q∼5,500) modes of the cavities, and the change in the highest-intensity mode as a function of pump power to better understand the dominant radiative processes. The variations of threshold power and lasing wavelength as a function of gain medium help us identify the possible limitations to lower-threshold lasing with quantum dot active medium. In addition, we have identified a distinctive lasing signature for quantum dot materials, which consistently lase at wavelengths shorter than the peak of the room temperature gain emission. These findings not only provide better understanding of lasing in nitride-based quantum dot cavity systems but also shed insight into the more fundamental issues of light−matter coupling in such systems.

Ultrafast, Polarized, Single-Photon Emission from m-Plane InGaN Quantum Dots on GaN Nanowires

We demonstrate single-photon emission from self-assembled m-plane InGaN quantum dots (QDs) embedded on the side-walls of GaN nanowires. A combination of electron microscopy, cathodoluminescence, time-resolved microphotoluminescence (μPL), and photon autocorrelation experiments give a thorough evaluation of the QD structural and optical properties. The QD exhibits antibunched emission up to 100 K, with a measured autocorrelation function of g(2)(0) = 0.28(0.03) at 5 K. Studies on a statistically significant number of QDs show that these m-plane QDs exhibit very fast radiative lifetimes (260 ± 55 ps) suggesting smaller internal fields than any of the previously reported c-plane and a-plane QDs. Moreover, the observed single photons are almost completely linearly polarized aligned perpendicular to the crystallographic c-axis with a degree of linear polarization of 0.84 ± 0.12. Such InGaN QDs incorporated in a nanowire system meet many of the requirements for implementation into quantum information systems and could potentially open the door to wholly new device concepts.

Effect of Threading Dislocations on the Quality Factor of InGaN/GaN Microdisk Cavities

In spite of the theoretical advantages associated with nitride microcavities, the quality factors of devices with embedded indium gallium nitride (InGaN) or gallium nitride (GaN) optical emitters still remain low. In this work we identify threading dislocations (TDs) as a major limitation to the fabrication of high quality factor devices in the nitrides. We report on the use of cathodoluminescence (CL) to identify individual TD positions within microdisk lasers containing either InGaN quantum wells or quantum dots. Using CL to accurately count the number, and map the position, of dislocations within several individual cavities, we have found a clear correlation between the density of defects in the high-field region of a microdisk and its corresponding quality factor (Q). We discuss possible mechanisms associated with defects, photon scattering, and absorption, which could be responsible for degraded device performance.

Origins of Spectral Diffusion in the Micro-Photoluminescence of Single InGaN Quantum Dots

We report on optical characterization of self-assembled InGaN quantum dots (QDs) grown on three GaN pseudo-substrates with differing threading dislocation densities. QD density is estimated via microphotoluminscence on a masked sample patterned with circular apertures, and appears to increase with dislocation density. A non-linear excitation technique is used to observe the sharp spectral lines characteristic of QD emission. Temporal variations of the wavelength of emission from single QDs are observed and attributed to spectral diffusion. The magnitude of these temporal variations is seen to increase with dislocation density, suggesting locally fluctuating electric fields due to charges captured by dislocations are responsible for the spectral diffusion in this system.

Direct generation of linearly polarized single photons with a deterministic axis in quantum dots

Abstract We report the direct generation of linearly polarized single photons with a deterministic polarization axis in self-assembled quantum dots (QDs), achieved by the use of non-polar InGaN without complex device geometry engineering. Here, we present a comprehensive investigation of the polarization properties of these QDs and their origin with statistically significant experimental data and rigorous k·p modeling. The experimental study of 180 individual QDs allows us to compute an average polarization degree of 0.90, with a standard deviation of only 0.08. When coupled with theoretical insights, we show that these QDs are highly insensitive to size differences, shape anisotropies, and material content variations. Furthermore, 91% of the studied QDs exhibit a polarization axis along the crystal [1–100] axis, with the other 9% polarized orthogonal to this direction. These features give non-polar InGaN QDs unique advantages in polarization control over other materials, such as conventional polar nitride, InAs, or CdSe QDs. Hence, the ability to generate single photons with polarization control makes non-polar InGaN QDs highly attractive for quantum cryptography protocols.

Structure-activity correlations for Brønsted acid, Lewis Acid, and photocatalyzed reactions of exfoliated crystalline niobium oxides

Exfoliated crystalline niobium oxides that contain exposed but interconnected NbO6 octahedra with different degrees of structural distortion and defects are known to catalyze Brønsted acid (BA), Lewis acid (LA), and photocatalytic (PC) reactions efficiently but their structure–activity relationships are far from clear. Here, three exfoliated niobium oxides, namely, HSr2Nb3O10, HCa2Nb3O10, and HNb3O8, are synthesized, characterized extensively, and tested for selected BA, LA, and PC reactions. The structural origin for BA is associated mainly with acidic hydroxyl groups of edge‐shared NbO6 octahedra as proton donors; that of LA is associated with the vacant band position of Nb5+ to receive electron pairs from substrate; and that of PC is associated with the terminal Nb=O of NbO6 octahedra for photon capture and charge transfer to long‐lived surface adsorbed substrate complex through associated oxygen vacancies in close proximity. It is believed that an understanding of the structure–activity relationships could lead to the tailored design of NbOx catalysts for industrially important reactions.

Temperature-dependent fine structure splitting in InGaN quantum dots

This research was supported by the Engineering and Physical Sciences Research Council (EPSRC) U.K. (Grant No. EP/M012379/1 and EP/M011682/1) T.W. is grateful for the award of a National Science Scholarship (NSS) as PhD funding by the Singapore Agency for Science, Technology and Research (A*STAR). C.C.K. is grateful for the support provided by a Clarendon Scholarship and a Mary Frances and Philip Wagley Graduate Scholarship. R.A.O. is grateful to the Royal Academy of Engineering and the Leverhulme Trust for a Senior Research Fellowship.

Two-Dimensional Excitonic Photoluminescence in Graphene on a Cu Surface

Despite having outstanding electrical properties, graphene is unsuitable for optical devices because of its zero band gap. Here, we report two-dimensional excitonic photoluminescence (PL) from graphene grown on a Cu(111) surface, which shows an unexpected and remarkably sharp strong emission near 3.16 eV (full width at half-maximum ≤3 meV) and multiple emissions around 3.18 eV. As temperature increases, these emissions blue shift, displaying the characteristic negative thermal coefficient of graphene. The observed PL originates from the significantly suppressed dispersion of excited electrons in graphene caused by hybridization of graphene π and Cu d orbitals of the first and second Cu layers at a shifted saddle point 0.525(M+K) of the Brillouin zone. This finding provides a pathway to engineering optoelectronic graphene devices, while maintaining the outstanding electrical properties of graphene.

Defects in III-Nitride Microdisk Cavities

The original research shown in this article has been funded by the European Research Council under the European Community’s Seventh Framework Programme (FP7/2007-2013)/ ERC grant agreement no. 279361 (MACONS). RAO acknowledges the Royal Academy of Engineering Leverhulme Trust Senior Research Fellowship scheme.