Towards higher electron mobility in modulation doped GaAs/AlGaAs core shell nanowires.

Nanoscale 9 (2017) 7839-7846

JL Boland, G Tütüncüoglu, JQ Gong, S Conesa-Boj, CL Davies, LM Herz, A Fontcuberta I Morral, MB Johnston

Precise control over the electrical conductivity of semiconductor nanowires is a crucial prerequisite for implementation of these nanostructures into novel electronic and optoelectronic devices. Advances in our understanding of doping mechanisms in nanowires and their influence on electron mobility and radiative efficiency are urgently required. Here, we investigate the electronic properties of n-type modulation doped GaAs/AlGaAs nanowires via optical pump terahertz (THz) probe spectroscopy and photoluminescence spectroscopy over the temperature range 5 K-300 K. We directly determine an ionization energy of 6.7 ± 0.5 meV (T = 52 K) for the Si donors within the AlGaAs shell that create the modulation doping structure. We further elucidate the temperature dependence of the electron mobility, photoconductivity lifetime and radiative efficiency, and determine the charge-carrier scattering mechanisms that limit electron mobility. We show that below the donor ionization temperature, charge scattering is limited by interactions with interfaces, leading to an excellent electron mobility of 4360 ± 380 cm2 V-1 s-1 at 5 K. Above the ionization temperature, polar scattering via longitudinal optical (LO) phonons dominates, leading to a room temperature mobility of 2220 ± 130 cm2 V-1 s-1. In addition, we show that the Si donors effectively passivate interfacial trap states in the nanowires, leading to prolonged photoconductivity lifetimes with increasing temperature, accompanied by an enhanced radiative efficiency that exceeds 10% at room temperature.

Impact of microstructure on the electron-hole interaction in lead halide perovskites


AM Soufiani, Z Yang, T Young, A Miyata, A Surrente, A Pascoe, K Galkowski, M Abdi-Jalebi, R Brenes, J Urban, N Zhang, V Bulovic, O Portugall, Y-B Cheng, RJ Nicholas, A Ho-Baillie, MA Green, P Plochocka, SD Stranks

Ultrahigh magnetic field spectroscopy reveals the band structure of the three-dimensional topological insulator Bi2Se3

PHYSICAL REVIEW B 96 (2017) ARTN 121111

A Miyata, Z Yang, A Surrente, O Drachenko, DK Maude, O Portugall, LB Duffy, T Hesjedal, P Plochocka, RJ Nicholas

High-temperature performance of non-polar (11-20) InGaN quantum dots grown by a quasi-two-temperature method


T Wang, TJ Puchtler, T Zhu, JC Jarman, RA Oliver, RA Taylor

Spectroscopic Insights into Carbon Dot Systems.

The journal of physical chemistry letters 8 (2017) 2236-2242

M Righetto, A Privitera, I Fortunati, D Mosconi, M Zerbetto, ML Curri, M Corricelli, A Moretto, S Agnoli, L Franco, R Bozio, C Ferrante

The controversial nature of the fluorescent properties of carbon dots (CDs), ascribed either to surface states or to small molecules adsorbed onto the carbon nanostructures, is an unresolved issue. To date, an accurate picture of CDs and an exhaustive structure-property correlation are still lacking. Using two unconventional spectroscopic techniques, fluorescence correlation spectroscopy (FCS) and time-resolved electron paramagnetic resonance (TREPR), we contribute to fill this gap. Although electron micrographs indicate the presence of carbon cores, FCS reveals that the emission properties of CDs are based neither on those cores nor on molecular species linked to them, but rather on free molecules. TREPR provides deeper insights into the structure of carbon cores, where C sp2 domains are embedded within C sp3 scaffolds. FCS and TREPR prove to be powerful techniques, characterizing CDs as inherently heterogeneous systems, providing insights into the nature of such systems and paving the way to standardization of these nanomaterials.

Crystallization Kinetics and Morphology Control of Formamidinium-Cesium Mixed-Cation Lead Mixed-Halide Perovskite via Tunability of the Colloidal Precursor Solution.

Advanced materials (Deerfield Beach, Fla.) 29 (2017)

DP McMeekin, Z Wang, W Rehman, F Pulvirenti, JB Patel, NK Noel, MB Johnston, SR Marder, LM Herz, HJ Snaith

The meteoric rise of the field of perovskite solar cells has been fueled by the ease with which a wide range of high-quality materials can be fabricated via simple solution processing methods. However, to date, little effort has been devoted to understanding the precursor solutions, and the role of additives such as hydrohalic acids upon film crystallization and final optoelectronic quality. Here, a direct link between the colloids concentration present in the [HC(NH2 )2 ]0.83 Cs0.17 Pb(Br0.2 I0.8 )3 precursor solution and the nucleation and growth stages of the thin film formation is established. Using dynamic light scattering analysis, the dissolution of colloids over a time span triggered by the addition of hydrohalic acids is monitored. These colloids appear to provide nucleation sites for the perovskite crystallization, which critically impacts morphology, crystal quality, and optoelectronic properties. Via 2D X-ray diffraction, highly ordered and textured crystals for films prepared from solutions with lower colloidal concentrations are observed. This increase in material quality allows for a reduction in microstrain along with a twofold increase in charge-carrier mobilities leading to values exceeding 20 cm2 V-1 s-1 . Using a solution with an optimized colloidal concentration, devices that reach current-voltage measured power conversion efficiency of 18.8% and stabilized efficiency of 17.9% are fabricated.

Trends in Perovskite Solar Cells and Optoelectronics: Status of Research and Applications from the PSCO Conference

ACS ENERGY LETTERS 2 (2017) 857-861

F De Angelis, D Meggiolaro, E Mosconi, A Petrozza, MK Nazeeruddin, HJ Snaith

Two-Dimensional Excitonic Photoluminescence in Graphene on a Cu Surface.

ACS nano 11 (2017) 3207-3212

Y Park, Y Kim, CW Myung, RA Taylor, CCS Chan, BPL Reid, TJ Puchtler, RJ Nicholas, LT Singh, G Lee, C-C Hwang, C-Y Park, KS Kim

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.

Band-Tail Recombination in Hybrid Lead Iodide Perovskite


AD Wright, RL Milot, GE Eperon, HJ Snaith, MB Johnston, LM Herz

Impact of the Halide Cage on the Electronic Properties of Fully Inorganic Cesium Lead Halide Perovskites

ACS ENERGY LETTERS 2 (2017) 1621-1627

Z Yang, A Surrente, K Galkowski, A Miyata, O Portugall, RJ Sutton, AA Haghighirad, HJ Snaith, DK Maude, P Plochocka, RJ Nicholas

Single n+-i-n+ InP nanowires for highly sensitive terahertz detection.

Nanotechnology 28 (2017) 125202-

K Peng, P Parkinson, Q Gao, JL Boland, Z Li, F Wang, S Mokkapati, L Fu, MB Johnston, HH Tan, C Jagadish

Developing single-nanowire terahertz (THz) electronics and employing them as sub-wavelength components for highly-integrated THz time-domain spectroscopy (THz-TDS) applications is a promising approach to achieve future low-cost, highly integrable and high-resolution THz tools, which are desirable in many areas spanning from security, industry, environmental monitoring and medical diagnostics to fundamental science. In this work, we present the design and growth of n+-i-n+ InP nanowires. The axial doping profile of the n+-i-n+ InP nanowires has been calibrated and characterized using combined optical and electrical approaches to achieve nanowire devices with low contact resistances, on which the highly-sensitive InP single-nanowire photoconductive THz detectors have been demonstrated. While the n+-i-n+ InP nanowire detector has a only pA-level response current, it has a 2.5 times improved signal-to-noise ratio compared with the undoped InP nanowire detector and is comparable to traditional bulk THz detectors. This performance indicates a promising path to nanowire-based THz electronics for future commercial applications.

Solution-Processed Cesium Hexabromopalladate(IV), Cs2PdBr6, for Optoelectronic Applications.

Journal of the American Chemical Society 139 (2017) 6030-6033

N Sakai, AA Haghighirad, MR Filip, PK Nayak, S Nayak, A Ramadan, Z Wang, F Giustino, HJ Snaith

Lead halide perovskites are materials with excellent optoelectronic and photovoltaic properties. However, some hurdles remain prior to commercialization of these materials, such as chemical stability, phase stability, sensitivity to moisture, and potential issues due to the toxicity of lead. Here, we report a new type of lead-free perovskite related compound, Cs2PdBr6. This compound is solution processable, exhibits long-lived photoluminescence, and an optical band gap of 1.6 eV. Density functional theory calculations indicate that this compound has dispersive electronic bands, with electron and hole effective masses of 0.53 and 0.85 me, respectively. In addition, Cs2PdBr6 is resistant to water, in contrast to lead-halide perovskites, indicating excellent prospects for long-term stability. These combined properties demonstrate that Cs2PdBr6 is a promising novel compound for optoelectronic applications.

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

NANOPHOTONICS 6 (2017) 1175-1183

T Wang, TJ Puchtler, SK Patra, T Zhu, M Ali, TJ Badcock, T Ding, RA Oliver, S Schulz, RA Taylor

Efficient and Air-Stable Mixed-Cation Lead Mixed-Halide Perovskite Solar Cells with n-Doped Organic Electron Extraction Layers.

Advanced materials (Deerfield Beach, Fla.) 29 (2017)

Z Wang, DP McMeekin, N Sakai, S van Reenen, K Wojciechowski, JB Patel, MB Johnston, HJ Snaith

Air-stable doping of the n-type fullerene layer in an n-i-p planar heterojunction perovskite device is capable of enhancing device efficiency and improving device stability. Employing a (HC(NH2 )2 )0.83 Cs0.17 Pb(I0.6 Br0.4 )3 perovskite as the photoactive layer, glass-glass laminated devices are reported, which sustain 80% of their "post burn-in" efficiency over 3400 h under full sun illumination in ambient conditions.

How to Avoid Artifacts in Surface Photovoltage Measurements: A Case Study with Halide Perovskites.

The journal of physical chemistry letters 8 (2017) 2941-2943

I Levine, G Hodes, HJ Snaith, PK Nayak

The influence of surfaces on the transient terahertz conductivity and electron mobility of GaAs nanowires


HJ Joyce, SA Baig, P Parkinson, CL Davies, JL Boland, HH Tan, C Jagadish, LM Herz, MB Johnston

Tuning Biocompatible Block Copolymer Micelles by Varying Solvent Composition: Core/Corona Structure and Solvent Uptake

Macromolecules 50 (2017) 4322-4334

TJ Cooksey, A Singh, KM Le, S Wang, EG Kelley, L He, S Vajjala Kesava, ED Gomez, BE Kidd, LA Madsen, ML Robertson

© 2017 American Chemical Society. Block copolymer micelles enable the formation of widely tunable self-assembled structures in liquid phases, with applications ranging from drug delivery to personal care products to nanoreactors. In order to understand fundamental aspects of micelle assembly and dynamics, the structural properties and solvent uptake of biocompatible poly(ethylene oxide-b-ϵ-caprolactone) (PEO-PCL) diblock copolymers in deuterated water (D 2 O)/tetrahydrofuran (THF-d 8 ) mixtures were investigated with a combination of small-angle neutron scattering, nuclear magnetic resonance, and transmission electron microscopy. PEO-PCL block copolymers, of varying molecular weight yet constant block ratio, formed spherical micelles through a wide range of solvent compositions. Varying the solvent composition from 10 to 60 vol % THF-d 8 in D 2 O/THF-d 8 mixtures was a convenient means of varying the core-corona interfacial tension in the micelle system. An increase in THF-d 8 content in the bulk solvent increased the solvent uptake within the micelle core, which was comparable for the two series, irrespective of the polymer molecular weight. Whereas the smaller molecular weight micelle series exhibited a decrease in aggregation number with increasing THF-d 8 content in the bulk solvent, as anticipated due to changes in the core-corona interfacial tension, the aggregation number of the larger molecular weight series was surprisingly invariant with bulk solvent composition. Differences in the dependencies of the micelle size parameters (core radius and overall micelle radius) on the solvent composition originated from the differing trends in aggregation number for the two micelle series. Incorporation of the known unimer content determined from NMR (described in the companion paper), and directly accounting for impacts of solvent swelling of the micelle core on the neutron scattering length density of the core, allowed refinement of and increased confidence in extracted micelle parameters. In summary, the two micelle series showed similar solvent uptake that was independent of the polymer molecular weight yet significantly different dependencies of their aggregation number and size parameters on the solvent composition.

The 2017 terahertz science and technology roadmap


SS Dhillon, MS Vitiello, EH Linfield, AG Davies, MC Hoffmann, J Booske, C Paoloni, M Gensch, P Weightman, GP Williams, E Castro-Camus, DRS Cumming, F Simoens, I Escorcia-Carranza, J Grant, S Lucyszyn, M Kuwata-Gonokami, K Konishi, M Koch, CA Schmuttenmaer, TL Cocker, R Huber, AG Markelz, ZD Taylor, VP Wallace, JA Zeitler, J Sibik, TM Korter, B Ellison, S Rea, P Goldsmith, KB Cooper, R Appleby, D Pardo, PG Huggard, V Krozer, H Shams, M Fice, C Renaud, A Seeds, A Stoehr, M Naftaly, N Ridler, R Clarke, JE Cunningham, MB Johnston

Highly polarized electrically driven single-photon emission from a non-polar InGaN quantum dot


CC Kocher, TJ Puchtler, JC Jarman, T Zhu, T Wang, L Nuttall, RA Oliver, RA Taylor

Electron injection and scaffold effects in perovskite solar cells.

Journal of materials chemistry. C 5 (2017) 634-644

M Anaya, W Zhang, BC Hames, Y Li, F Fabregat-Santiago, ME Calvo, HJ Snaith, H Míguez, I Mora-Seró

In spite of the impressive efficiencies reported for perovskite solar cells (PSCs), key aspects of their working principles, such as electron injection at the contacts or the suitability of the utilization of a specific scaffold layer, are not yet fully understood. Increasingly complex scaffolds attained by the sequential deposition of TiO2 and SiO2 mesoporous layers onto transparent conducting substrates are used to perform a systematic characterization of both the injection process at the electron selective contact and the scaffold effect in PSCs. By forcing multiple electron injection processes at a controlled sequence of perovskite-TiO2 interfaces before extraction, interfacial injection effects are magnified and hence characterized in detail. An anomalous injection behavior is observed, the fingerprint of which is the presence of significant inductive loops in the impedance spectra with a magnitude that correlates with the number of interfaces in the scaffold. Analysis of the resistive and capacitive behavior of the impedance spectra indicates that the scaffolds could hinder ion migration, with positive consequences such as lowering the recombination rate and implications for the current-potential curve hysteresis. Our results suggest that an appropriate balance between these advantageous effects and the unavoidable charge transport resistive losses introduced by the scaffolds will help in the optimization of PSC performance.