Ben F. Spencer

Electronic and surface properties of PbS nanoparticles exhibiting efficient multiple exciton generation

Ultrafast transient absorption measurements have been used to study multiple exciton generation in solutions of PbS nanoparticles vigorously stirred to avoid the effects of photocharging. The threshold and slope efficiency of multiple exciton generation are found to be 2.5 ± 0.2 ×E(g) and 0.34 ± 0.08, respectively. Photoemission measurements as a function of nanoparticle size and ageing show that the position of the valence band maximum is pinned by surface effects, and that a thick layer of surface oxide is rapidly formed at the nanoparticle surfaces on exposure to air.

Charge dynamics at heterojunctions for PbS/ZnO colloidal quantum dot solar cells probed with time-resolved surface photovoltage spectroscopy

Time-resolved laser-pump X-ray-photoemission-probe spectroscopy of a ZnO ( 101¯0) substrate with and without PbS quantum dots (QDs) chemically linked to the surface is performed, using laser photon energies resonant with and below the band gap energy of the substrate (λ = 372 and 640 nm, hν = 3.33 and 1.94 eV). Charge injection from the photoexcited QDs to ZnO is demonstrated through the change in the surface photovoltage of the ZnO substrate observed when the heterojunction is illuminated with 1.94 eV radiation. The measured carrier dynamics are limited by the persistent photoconductivity of ZnO, giving dark carrier lifetimes of the order of 200 μs in a depletion layer at the interface. The chemical specificity of soft X-rays is used to separately measure the charge dynamics in the quantum dots and the substrate, yielding evidence that the depletion region at the interface extends into the PbS QD layer.

Terahertz cyclotron resonance spectroscopy of an AlGaN/GaN heterostructure using a high-field pulsed magnet and an asynchronous optical sampling technique

The effective mass, sheet carrier concentration, and mobility of electrons within a two-dimensional electron gas in an AlGaN/GaN heterostructure were determined using a laboratory-based terahertz cyclotron resonance spectrometer. The ability to perform terahertz cyclotron resonance spectroscopy with magnetic fields of up to 31 T was enabled by combining a high-field pulsed magnet with a modified asynchronous optical sampling terahertz detection scheme. This scheme allowed around 100 transmitted terahertz waveforms to be recorded over the 14 ms magnetic field pulse duration. The sheet density and mobility were measured to be 8.0 × 1012 cm−2 and 9000 cm2 V−1 s−1 at 77 K. The in-plane electron effective mass at the band edge was determined to be 0.228 ± 0.002m0.

Ambient-air-stable inorganic Cs2SnI6 double perovskite thin films via aerosol-assisted chemical vapour deposition

Air-stable caesium tin iodide double perovskite (Cs2SnI6) thin films have been fabricated via aerosol-assisted chemical vapour deposition (AACVD). We compare the properties of the double perovskite films made using AACVD with those made by the widely used spin-coating method. Films with purer crystalline phase (less CsI impurity) and far better stability in ambient air can be obtained by AACVD compared with spin coating. The AACVD-grown Cs2SnI6 films retain high phase purity for at least ∼100 days aging in air with negligible CsI impurities detected over this time, as determined by X-ray diffraction. The films exhibit an optical band gap energy (Eg) of ca. 1.3 eV and a homogeneous morphology with the expected nominal stoichiometry within error, as probed by energy-dispersive X-ray spectroscopy. Overall, the characteristics of the Cs2SnI6 films are highly process-dependent, e.g. they are influenced by the presence of hydroiodic acid (HI) in the precursor solution. Without HI addition, an iodine-deficient film with more CsI is produced, which also exhibits a larger Eg of ca. 1.6 eV. In addition to bulk properties, we utilise X-ray photoelectron spectroscopy (XPS) to scrutinise the surface characteristics in detail. We find excess Sn and I located at the surfaces. This can be attributed to the presence of SnI4 from the deposition precursor vapour. Furthermore, following aging in air, an increase in CsI impurity for the AACVD (+HI)-grown film is observed, along with a reduction in SnI4 at the surfaces. Near-ambient pressure XPS (NAP-XPS) is used to examine the surface stability of AACVD (+HI)-grown films on exposure to O2 and H2O. No enhancement in the amount of CsI impurity is observed after both H2O vapour (9 mbar) and O2 (5 mbar) exposure. Nevertheless, the concentrations of tin and iodine change after exposure, suggesting that SnI4 protects Cs2SnI6 from degradation. This passivation effect of SnI4 on Cs2SnI6 surfaces is proposed to explain the additional stability of Cs2SnI6 fabricated via AACVD.

Terahertz Magnetospectroscopy Studies of an AlGaN/GaN Heterostructure

A laboratory based terahertz cyclotron resonance spectrometer is used to determine 2D electron gas parameters in an AlGaN/GaN heterostructure. The modified ASOPS system acquires ~100 terahertz-traces under a 14 ms long multi-Tesla magnetic field pulse.

Developing InP-based solar cells: Time-resolved terahertz measurements of photoconductivity and carrier multiplication efficiencies

Time-resolved terahertz spectroscopic studies were carried out on bulk InP to measure photoconductivity on the picosecond timescale. Comparison of the carrier multiplication quantum yields obtained with those of colloidal InP nanoparticles clearly demonstrate the potential benefit of InP nanoparticle-based next-generation solar cells.