Publications by Michael Johnston


Raman Spectrum of the Organic-Inorganic Halide Perovskite CH3NH3PbI3 from First Principles and High-Resolution Low-Temperature Raman Measurements

JOURNAL OF PHYSICAL CHEMISTRY C 122 (2018) 21703-21717

MA Perez-Osorio, Q Lin, RT Phillips, RL Milot, LM Herz, MB Johnston, F Giustino


High electron mobility and insights into temperature-dependent scattering mechanisms in InAsSb nanowires

Nano Letters American Chemical Society 18 (2018) 3703–3710-

JL Boland, F Amaduzzi, S Sterzl, H Potts, LM Herz, AFI Fontcuberta i Morral, M Johnston

InAsSb nanowires are promising elements for thermoelectric devices, infrared photodetectors, high-speed transistors, as well as thermophotovoltaic cells. By changing the Sb alloy fraction the mid-infrared bandgap energy and thermal conductivity may be tuned for specific device applications. Using both terahertz and Raman noncontact probes, we show that Sb alloying increases the electron mobility in the nanowires by over a factor of 3 from InAs to InAs0.65Sb0.35. We also extract the temperature-dependent electron mobility via both terahertz and Raman spectroscopy, and we report the highest electron mobilities for InAs0.65Sb0.35 nanowires to date, exceeding 16,000 cm2 V–1 s–1 at 10 K.


Temperature-dependent refractive index of quartz at terahertz frequencies

Journal of Infrared, Millimeter and Terahertz Waves Springer Verlag 39 (2018) 1236-1248

CL Davies, JB Patel, CQ Xia, LM Herz, M Johnston

Characterisation of materials often requires the use of a substrate to support the sample being investigated. For optical characterisation at terahertz frequencies, quartz is commonly used owing to its high transmission and low absorption at these frequencies. Knowledge of the complex refractive index of quartz is required for analysis of time-domain terahertz spectroscopy and optical pump terahertz probe spectroscopy for samples on a quartz substrate. Here, we present the refractive index and extinction coefficient for α-quartz between 0.5 THz and 5.5 THz (17–183 cm^−1) taken at 10, 40, 80, 120, 160, 200 and 300 K. Quartz shows excellent transmission and is thus an ideal optical substrate over the THz band, apart from the region 3.9 ± 0.1 THz owing to a spectral feature originating from the lowest energy optical phonon modes. We also present the experimentally measured polariton dispersion of α-quartz over this frequency range.


Modification of the fluorinated tin oxide/electron-transporting material interface by a strong reductant and its effect on perovskite solar cell efficiency

Molecular Systems Design and Engineering Royal Society of Chemistry 3 (2018) 741-747

F Pulvirenti, B Wegner, NK Noel, G Mazzotta, R Hill, JB Patel, LM Herz, MB Johnston, MK Riede, HJ Snaith, N Koch, S Barlow

To date, the most efficient hybrid metal halide peroskite solar cells employ TiO2 as electron-transporting material (ETM), making these devices unstable under UV light exposure. Replacing TiO2 with fullerene derivatives has been shown to result in improved electronic contact and increased device lifetime, making it of interest to assess whether similar improvements can be achieved by using other organic semiconductors as ETMs. In this work, we investigate perylene-3,4:9,10-tetracarboxylic bis(benzimidazole) as a vacuum-processable ETM, and we minimize electron-collection losses at the electron-selective contact by depositing pentamethylcyclopentadienyl cyclopentadienyl rhodium dimer, (RhCp*Cp)2, on fluorinated tin oxide. With (RhCp*Cp)2 as an interlayer, ohmic contacts can be formed, there is interfacial doping of the ETM, and stabilized power conversion efficiencies of up to 14.2% are obtained.


Bimolecular recombination in methylammonium lead triiodide perovskite is an inverse absorption process

Nature Communications Springer Nature 9 (2018) 293

CL Davies, MR Filip, JB Patel, TW Crothers, C Verdi, AD Wright, RL Milot, F Giustino, MB Johnston, L Herz

Photovoltaic devices based on metal halide perovskites are rapidly improving in efficiency. Once the Shockley–Queisser limit is reached, charge-carrier extraction will be limited only by radiative bimolecular recombination of electrons with holes. Yet, this fundamental process, and its link with material stoichiometry, is still poorly understood. Here we show that bimolecular charge-carrier recombination in methylammonium lead triiodide perovskite can be fully explained as the inverse process of absorption. By correctly accounting for contributions to the absorption from excitons and electron-hole continuum states, we are able to utilise the van Roosbroeck–Shockley relation to determine bimolecular recombination rate constants from absorption spectra. We show that the sharpening of photon, electron and hole distribution functions significantly enhances bimolecular charge recombination as the temperature is lowered, mirroring trends in transient spectroscopy. Our findings provide vital understanding of band-to-band recombination processes in this hybrid perovskite, which comprise direct, fully radiative transitions between thermalized electrons and holes.


Hybrid perovskites: prospects for concentrator solar cells

Advanced Science Wiley 5 (2018) 1700792

Q Lin, Z Wang, HJ Snaith, M Johnston, L Herz

Perovskite solar cells have shown a meteoric rise of power conversion efficiency and a steady pace of improvements in their stability of operation. Such rapid progress has triggered research into approaches that can boost efficiencies beyond the Shockley-Queisser limit stipulated for a single-junction cell under normal solar illumination conditions. The tandem solar cell architecture is one concept here that has recently been successfully implemented. However, the approach of solar concentration has not been sufficiently explored so far for perovskite photovoltaics, despite its frequent use in the area of inorganic semiconductor solar cells. Here, the prospects of hybrid perovskites are assessed for use in concentrator solar cells. Solar cell performance parameters are theoretically predicted as a function of solar concentration levels, based on representative assumptions of charge-carrier recombination and extraction rates in the device. It is demonstrated that perovskite solar cells can fundamentally exhibit appreciably higher energy-conversion efficiencies under solar concentration, where they are able to exceed the Shockley-Queisser limit and exhibit strongly elevated open-circuit voltages. It is therefore concluded that sufficient material and device stability under increased illumination levels will be the only significant challenge to perovskite concentrator solar cell applications.


Publisher Correction: High irradiance performance of metal halide perovskites for concentrator photovoltaics

Nature Energy Springer Nature America, Inc (2018)

Z Wang, Q Lin, B Wenger, M Christoforo, Y-H Lin, MT Klug, MICHAEL Johnston, LAURA Herz, HJ Snaith

© 2018, Springer Nature Limited. When this Article was originally published, an old version of the associated Supplementary Information file was uploaded. This has now been replaced.


Preface to special topic: frontiers on THz photonic devices

APL Photonics AIP Publishing 3 (2018) 051501-1

S Atakaramians, M Johnston, W Padilla, R Mendis

Terahertz (THz) photonic devices are now exploiting emerging materials systems, while novel device designs utilise plasmonic effects, nanophotinics, and metamaterials. The scope of this special topic highlights and reviews the recent cutting-edge THz photonic devices which have been revolutionised from the advances in the above research areas.


Impact of the organic cation on the optoelectronic properties of formamidinium lead triiodide

Journal of Physical Chemistry Letters American Chemical Society 9 (2018) 4502-4511

CL Davies, J Borchert, CQ Xia, RL Milot, H Kraus, MB Johnston, L Herz

Metal halide perovskites have proven to be excellent light-harvesting materials in photovoltaic devices whose efficiencies are rapidly improving. Here, we examine the temperature-dependent photon absorption, exciton binding energy, and band gap of FAPbI3 (thin film) and find remarkably different behavior across the β–γ phase transition compared with MAPbI3. While MAPbI3 has shown abrupt changes in the band gap and exciton binding energy, values for FAPbI3 vary smoothly over a range of 100–160 K in accordance with a more gradual transition. In addition, we find that the charge-carrier mobility in FAPbI3 exhibits a clear T–0.5 trend with temperature, in excellent agreement with theoretical predictions that assume electron–phonon interactions to be governed by the Fröhlich mechanism but in contrast to the T–1.5 dependence previously observed for MAPbI3. Finally, we directly observe intraexcitonic transitions in FAPbI3 at low temperature, from which we determine a low exciton binding energy of only 5.3 meV at 10 K.


Distinguishing cap and core contributions to the photoconductive terahertz response of single GaAs based core–shell–cap nanowire detectors

Lithuanian Journal of Physics Lithuanian Academy of Sciences 58 (2018) 15-23

K Peng, P Parkinson, L Fu, Q Gao, JL Boland, Y-N Guo, N Jian, HH Tan, MB Johnston, C Jagadish

GaAs nanowires are promising candidates for advanced optoelectronic devices, despite their high surface recombination velocity and large surface-area-to-volume ratio, which renders them problematic for applications that require efficient charge collection and long charge-carrier lifetimes. Overcoating a bare GaAs nanowire core with an optimized larger-bandgap AlGaAs shell, followed by a capping layer of GaAs to prevent oxidation, has proven an effective way to passivate the nanowire surface and thereby improve electrical properties for enhanced device performance. However, it is difficult to quantify and distinguish the contributions between the nanowire core and cap layer when measuring the optoelectronic properties of a nanowire device. Here, we investigated the photoconductive terahertz (THz) response characteristics of single GaAs/AlGaAs/GaAs core–shell–cap nanowire detectors designed for THz time-domain spectroscopy. We present a detailed study of the contributions of the GaAs cap layer and GaAs core on the ultrafast optoelectronic performance of the detector. We show that both the GaAs cap and core contribute to the photoconductive signal in proportion to their relative volume in the nanowire. By increasing the cap volume ratio to above 90% of the total GaAs volume, a quasi-direct-sampling type photoconductive nanowire detector can be achieved that is highly desirable for low-noise and fast data acquisition detection.


Interplay of structural and optoelectronic properties in formamidinium mixed tin-lead triiodide perovskites

Advanced Functional Materials Wiley 28 (2018)

ES Parrott, T Green, RL Milot, MB Johnston, HJ Snaith, LM Herz

Mixed lead-tin triiodide perovskites are promising absorber materials for low band-gap bottom cells in all-perovskite tandem photovoltaic devices. Key structural and electronic properties of the FAPb1-xSnxI3 perovskite are presented here as a function of lead:tin content across the alloy series. Temperature-dependent photoluminescence and optical absorption measurements are used to identify changes in the band-gap and phase transition temperature. The large band-gap bowing parameter, a crucial element for the attainment of low band-gaps in this system, is shown to depend on the structural phase, reaching a value of 0.84 eV in the low-temperature phase and 0.73 eV at room temperature. The parabolic nature of the bowing at all temperatures is compatible with a mechanism arising from bond bending to accommodate the random placement of unevenly sized lead and tin ions. Charge-carrier recombination dynamics are shown to fall into two regimes. Tin-rich compositions exhibit fast, mono-exponential recombination that is almost temperature independent, in accordance with high levels of electrical doping. Lead-rich compositions show slower, stretched-exponential charge-carrier recombination that is strongly temperature-dependent, in accordance with a multi-phonon assisted process. These results highlight the importance of structure and composition for control of band-gap bowing and charge-carrier recombination mechanisms in low band-gap absorbers for all-perovskite tandem solar cells.


Engineering III-V nanowires for optoelectronics: from epitaxy to terahertz photonics

Proceedings of SPIE Society of Photo-optical Instrumentation Engineers 10543 (2018)

HJ Joyce, C Uswachoke, SO Adeyemo, JL Boland, DA Damry, CL Davies, J Wong-Leung, HH Tan, C Jagadish, L Herz, M Johnston

Downloading of the abstract is permitted for personal use only. Nanowires show unique promise as nanoscale building blocks for a multitude of optoelectronic devices, ranging from solar cells to terahertz photonic devices. We will discuss the epitaxial growth of these nanowires in novel geometries and crystallographic phases, and the use of terahertz conductivity spectroscopy to guide the development of nanowire-based devices. As an example, we will focus on the development of nanowire-based polarization modulators for terahertz communications systems.


The effects of doping density and temperature on the optoelectronic properties of formamidinium tin triiodide thin films

Advanced Materials Wiley 30 (2018) 1804506-

RL Milot, MT Klug, C Davies, Z Wang, HAP Kraus, HJ Snaith, MB Johnston, LM Herz

Intrinsic and extrinsic optoelectronic properties are unraveled for formamidinium tin triiodide (FASnI3) thin films, whose background hole doping density was varied through SnF2 addition during film fabrication. Monomolecular charge-carrier recombination exhibits both a dopant-mediated part that grows linearly with hole doping density and remnant contributions that remain under tin-enriched processing conditions. At hole densities near 1020 cm-3, a strong Burstein-Moss effect increases absorption onset energies by ~300meV beyond the band gap energy of undoped FASnI3 (shown to be 1.2 eV at 5 K and 1.35 eV at room temperature). At very high doping densities (1020 cm-3), temperature-dependent measurements indicate that the effective charge-carrier mobility is suppressed through scattering with ionized dopants. Once the background hole concentration is nearer 1019 cm-3 and below, the charge-carrier mobility increases with decreasing temperature according to ~T-1.2, suggesting it is limited mostly by intrinsic interactions with lattice vibrations. For the lowest doping concentration of 7.2´1018 cm^-3, charge-carrier mobilities reach a value of 67 cm2V-1s-1at room temperature and 470 cm2V-1s-1 at 50 K. Intra-excitonic transitions observed in the THz-frequency photoconductivity spectra at 5K reveal an exciton binding energy of only 3.1 meV for FASnI3, in agreement with the low bandgap energy exhibited by this perovskite.


Photocurrent spectroscopy of perovskite solar cells over a wide temperature range from 15 to 350 K

Journal of Physical Chemistry Letters American Chemical Society 2018 (2017) 263-268

J Patel, Q Lin, O Zadvorna, C Davies, L Herz, M Johnston

Solar cells based on metal halide perovskite thin films show great promise for energy generation in a range of environments from terrestrial installations to space applications. Here we assess the device characteristics of the prototypical perovskite solar cells based on methylammonium lead triiodide (CH3NH3PbI3) over a broad temperature range from 15 to 350 K (−258 to 77 °C). For these devices, we observe a peak in the short-circuit current density and open-circuit voltage at 200 K (−73 °C) with decent operation maintained up to 350 K. We identify the clear signature of crystalline PbI2 contributing directly to the low-temperature photocurrent spectra, showing that PbI2 plays an active role (beyond passivation) in CH3NH3PbI3 solar cells. Finally we observe a blue-shift in the photocurrent spectrum with respect to the absorption spectrum at low temperature (15 K), allowing us to extract a lower limit on the exciton binding energy of 9.1 meV for CH3NH3PbI3.


High irradiance performance of metal halide perovskites for concentrator photovoltaics

Nature Energy Nature Publishing Group 3 (2018) 855-861

Z Wang, Q Lin, B Wenger, MG Christoforo, Y-H Lin, MT Klug, MB Johnston, LM Herz, HJ Snaith

Traditionally, III–V multi-junction cells have been used in concentrator photovoltaic (CPV) applications, which deliver extremely high efficiencies but have failed to compete with ‘flat-plate’ silicon technologies owing to cost. Here, we assess the feasibility of using metal halide perovskites for CPVs, and we evaluate their device performance and stability under concentrated light. Under simulated sunlight, we achieve a peak efficiency of 23.6% under 14 Suns (that is, 14 times the standard solar irradiance), as compared to 21.1% under 1 Sun, and measure 1.26 V open-circuit voltage under 53 Suns, for a material with a bandgap of 1.63 eV. Importantly, our encapsulated devices maintain over 90% of their original efficiency after 150 h aging under 10 Suns at maximum power point. Our work reveals the potential of perovskite CPVs, and may lead to new PV deployment strategies combining perovskites with low-concentration factor and lower-accuracy solar tracking systems.


Highly crystalline methylammonium lead tribromide perovskite films for efficient photovoltaic devices

ACS Energy Letters American Chemical Society 3 (2018) 1233−1240-

N Noel, B Wenger, S Habisreutinger, J Patel, T Crothers, Z Wang, R Nicholas, M Johnston, L Herz, H Snaith

The rise of metal-halide perovskite solar cells has captivated the research community, promising to disrupt the current energy landscape. While a sizable percentage of the research done on this class of materials has been focused on the neat and iodide-rich perovskites, bromide-based perovskites can deliver substantially higher voltages because of their relatively wide band gaps of over 2 eV. The potential for efficient, high-voltage devices makes materials such as these incredibly attractive for multijunction photovoltaic applications. Here, we use the acetonitrile/methylamine solvent system to deposit smooth, highly crystalline films of CH3NH3PbBr3. By using choline chloride as a passivating agent for these films, we achieve photoluminescence quantum efficiencies of up to 5.5% and demonstrate charge-carrier mobilities of 17.8 cm2/(V s). Incorporating these films into photovoltaic devices, we achieve scanned power conversion efficiencies of up to 8.9%, with stabilized efficiencies of 7.6%, providing a simple route to realizing efficient, high-voltage CH3NH3PbBr3 planar-heterojunction devices.


Large-area, highly uniform evaporated formamidinium lead triiodide thin-films for solar cells

ACS Energy Letters American Chemical Society 2 (2017) 2799-2804

J Borchert, R Milot, JB Patel, CL Davies, A Wright, LM Maestro, HJ Snaith, LM Hertz, M Johnston

Perovskite thin-film solar cells are one of the most promising emerging renewable energy technologies because of their potential for low-cost, large-area fabrication combined with high energy conversion efficiencies. Recently, formamidinium lead triiodide (FAPbI3) and other formamidinium (CH(NH2)2) based perovskites have been explored as interesting alternatives to methylammonium lead triiodide (MAPbI3) because they exhibit better thermal stability. However, at present a major challenge is the scale-up of perovskite solar cells from small test-cells to full solar modules. We show that coevaporation is a scalable method for the deposition of homogeneous FAPbI3 thin films over large areas. The method allows precise control over film thickness and results in highly uniform, pinhole-free layers. Our films exhibited a high charge-carrier mobility of 26 cm2 V–1s–1, excellent optical properties, and a bimolecular recombination constant of 7 × 10–11 cm3 s–1. Solar cells fabricated using these vapor-deposited layers within a regular device architecture produced stabilized power conversion efficiencies of up to 14.2%. Thus, we demonstrate that efficient FAPbI3 solar cells can be vapor-deposited, which opens up a pathway toward large-area stable perovskite photovoltaics.


THz modulators and detectors based on semiconductor nanowires

2017 42nd International Conference on Infrared, Millimeter, and Terahertz Waves (IRMMW-THz) IEEE (2017)

M Johnston

Semiconductors nanowires have to potential to be building blocks for future nano-optoelectronic devices. We have recently demonstrated high performance THz photonic devices based on GaAs and InP nanowires. These include ultrafast optically switched modulators of THz radiation and single nanowire photoconductive detectors of THz pulses.


Modulation of terahertz polarization on picosecond timescales using polymer-encapsulated semiconductor nanowires

Conference on Lasers and Electro-Optics (CLEO 2017) Optical Society of America 2017-January (2017) 1-2

J Boland, D Damry, HH Tan, C Jagadish, HJ Joyce, M Johnston

We exploit the photoconductivity of semiconductor nanowires to achieve ultrafast broad-bandwidth modulation of THz pulses. A modulation depth of -8 dB was exhibited by a polarizer consisting of 14 layers of nanowires encapsulated in polymer.


Modulation of terahertz polarization on picosecond timescales using polymer-encapsulated semiconductor nanowires

2017 Conference on Lasers and Electro-Optics, CLEO 2017 - Proceedings 2017-January (2017) 1-2

SA Baig, JL Boland, DA Damry, H Hoe Tan, C Jagadish, HJ Joyce, MB Johnston

© OSA 2017. We exploit the photoconductivity of semiconductor nanowires to achieve ultrafast broad-bandwidth modulation of THz pulses. A modulation depth of -8 dB was exhibited by a polarizer consisting of 14 layers of nanowires encapsulated in polymer.

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