Padhraic Mulligan

Bio: Padhraic Mulligan is an academic researcher from Oak Ridge National Laboratory. The author has contributed to research in topics: Gallium nitride & Particle detector. The author has an hindex of 9, co-authored 16 publications receiving 4424 citations. Previous affiliations of Padhraic Mulligan include Ohio State University.

Electron-hole diffusion lengths > 175 μm in solution-grown CH3NH3PbI3 single crystals

Abstract: Long, balanced electron and hole diffusion lengths greater than 100 nanometers in the polycrystalline organolead trihalide compound CH3NH3PbI3 are critical for highly efficient perovskite solar cells. We found that the diffusion lengths in CH3NH3PbI3 single crystals grown by a solution-growth method can exceed 175 micrometers under 1 sun (100 mW cm(-2)) illumination and exceed 3 millimeters under weak light for both electrons and holes. The internal quantum efficiencies approach 100% in 3-millimeter-thick single-crystal perovskite solar cells under weak light. These long diffusion lengths result from greater carrier mobility, longer lifetime, and much smaller trap densities in the single crystals than in polycrystalline thin films. The long carrier diffusion lengths enabled the use of CH3NH3PbI3 in radiation sensing and energy harvesting through the gammavoltaic effect, with an efficiency of 3.9% measured with an intense cesium-137 source.

Sensitive X-ray detectors made of methylammonium lead tribromide perovskite single crystals

Abstract: Single-crystal perovskite devices 2–3 mm thick exhibit 16.4% X-ray detection efficiency with sensitivity four times higher than α-Se X-ray detectors.

Review of using gallium nitride for ionizing radiation detection

Abstract: With the largest band gap energy of all commercial semiconductors, GaN has found wide application in the making of optoelectronic devices. It has also been used for photodetection such as solar blind imaging as well as ultraviolet and even X-ray detection. Unsurprisingly, the appreciable advantages of GaN over Si, amorphous silicon (a-Si:H), SiC, amorphous SiC (a-SiC), and GaAs, particularly for its radiation hardness, have drawn prompt attention from the physics, astronomy, and nuclear science and engineering communities alike, where semiconductors have traditionally been used for nuclear particle detection. Several investigations have established the usefulness of GaN for alpha detection, suggesting that when properly doped or coated with neutron sensitive materials, GaN could be turned into a neutron detection device. Work in this area is still early in its development, but GaN-based devices have already been shown to detect alpha particles, ultraviolet light, X-rays, electrons, and neutrons. Furthermo...

Measurement of internal conversion electrons from Gd neutron capture

Abstract: Gadolinium (Gd) is a suitable material for neutron conversion because of its superior neutron absorption cross-section. However, the principal secondary particles that generate electron-hole pairs in a semiconductor detector after Gd neutron capture are low-energy internal conversion (IC) electrons. We measured the IC electron spectrum due to Gd neutron capture by using a thermal neutron beam and a digitizer-based multidetector spectroscopy. We also discussed the effective use of the IC electrons in the context of a twin-detector design and the associated gamma-ray rejection issues. Extensive simulations of the spectra of IC electrons and gamma rays agreed well with the experimental results; both types of results support the feasibility of the proposed n – γ separation method.

Evaluation of freestanding GaN as an alpha and neutron detector

Abstract: The wide bandgap (3.39) eV and large dislocation energy of the III–V semiconductor gallium nitride (GaN) make this a desirable material for charged particle spectroscopy in high temperature, high radiation environments. While other research groups have established that charged particle detectors can be fabricated from high quality, thin films of molecular beam epitaxy (MBE) and metal organic chemical vapor deposition (MOCVD) grown GaN, this work demonstrates the feasibility of ionizing radiation detectors created from significantly thicker freestanding n-type GaN, grown via hydride vapor phase epitaxy (HVPE). Detectors were fabricated by depositing Ni/Au pads on n-type GaN, forming a Schottky barrier diode. Capacitance–voltage measurements on the detectors showed an intrinsic carrier concentration in the range of 10 −16 cm −3 –10 –15 cm −3 , and indicated an inhomogeneous distribution between diodes on the same wafer. The radiation sensitivity of the fabricated detectors was analyzed using alpha particles from an 241 Am source. Charge collection efficiency (CCE) calculations from these experiments indicate an efficiency of 100 percent. The detectors were also successfully used to detect neutron induced charged particles using a Li 2 O foil in a neutron beam.

Cesium-containing triple cation perovskite solar cells: improved stability, reproducibility and high efficiency

Abstract: Today's best perovskite solar cells use a mixture of formamidinium and methylammonium as the monovalent cations. With the addition of inorganic cesium, the resulting triple cation perovskite compositions are thermally more stable, contain less phase impurities and are less sensitive to processing conditions. This enables more reproducible device performances to reach a stabilized power output of 21.1% and ∼18% after 250 hours under operational conditions. These properties are key for the industrialization of perovskite photovoltaics.

Surface passivation of perovskite film for efficient solar cells

Abstract: In recent years, the power conversion efficiency of perovskite solar cells has increased to reach over 20%. Finding an effective means of defect passivation is thought to be a promising route for bringing further increases in the power conversion efficiency and the open-circuit voltage (VOC) of perovskite solar cells. Here, we report the use of an organic halide salt phenethylammonium iodide (PEAI) on HC(NH2)2–CH3NH3 mixed perovskite films for surface defect passivation. We find that PEAI can form on the perovskite surface and results in higher-efficiency cells by reducing the defects and suppressing non-radiative recombination. As a result, planar perovskite solar cells with a certificated efficiency of 23.32% (quasi-steady state) are obtained. In addition, a VOC as high as 1.18 V is achieved at the absorption threshold of 1.53 eV, which is 94.4% of the Shockley–Queisser limit VOC (1.25 V). Planar perovskite solar cells that have been passivated using the organic halide salt phenethylammonium iodide are shown to have suppressed non-radiative recombination and operate with a certified power conversion efficiency of 23.3%.

Metal-halide perovskites for photovoltaic and light-emitting devices

Abstract: Metal-halide perovskites are crystalline materials originally developed out of scientific curiosity. Unexpectedly, solar cells incorporating these perovskites are rapidly emerging as serious contenders to rival the leading photovoltaic technologies. Power conversion efficiencies have jumped from 3% to over 20% in just four years of academic research. Here, we review the rapid progress in perovskite solar cells, as well as their promising use in light-emitting devices. In particular, we describe the broad tunability and fabrication methods of these materials, the current understanding of the operation of state-of-the-art solar cells and we highlight the properties that have delivered light-emitting diodes and lasers. We discuss key thermal and operational stability challenges facing perovskites, and give an outlook of future research avenues that might bring perovskite technology to commercialization.

Efficient and stable large-area perovskite solar cells with inorganic charge extraction layers

Abstract: The recent dramatic rise in power conversion efficiencies (PCEs) of perovskite solar cells (PSCs) has triggered intense research worldwide. However, high PCE values have often been reached with poor stability at an illuminated area of typically less than 0.1 square centimeter. We used heavily doped inorganic charge extraction layers in planar PSCs to achieve very rapid carrier extraction, even with 10- to 20-nanometer-thick layers, avoiding pinholes and eliminating local structural defects over large areas. The robust inorganic nature of the layers allowed for the fabrication of PSCs with an aperture area >1 square centimeter that have a PCE >15%, as certified by an accredited photovoltaic calibration laboratory. Hysteresis in the current-voltage characteristics was eliminated; the PSCs were stable, with >90% of the initial PCE remaining after 1000 hours of light soaking.

Impact of microstructure on local carrier lifetime in perovskite solar cells

Abstract: The remarkable performance of hybrid perovskite photovoltaics is attributed to their long carrier lifetimes and high photoluminescence (PL) efficiencies. High-quality films are associated with slower PL decays, and it has been claimed that grain boundaries have a negligible impact on performance. We used confocal fluorescence microscopy correlated with scanning electron microscopy to spatially resolve the PL decay dynamics from films of nonstoichiometric organic-inorganic perovskites, CH3NH3PbI3(Cl). The PL intensities and lifetimes varied between different grains in the same film, even for films that exhibited long bulk lifetimes. The grain boundaries were dimmer and exhibited faster nonradiative decay. Energy-dispersive x-ray spectroscopy showed a positive correlation between chlorine concentration and regions of brighter PL, whereas PL imaging revealed that chemical treatment with pyridine could activate previously dark grains.