Darren M. Graham

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.

Controlled Synthesis of Tuned Bandgap Nanodimensional Alloys of PbSxSe1−x

Truly alloyed PbS(x)Se(1-x) (x = 0-1) nanocrystals (∼5 nm in size) have been prepared, and their resulting optical properties are red-shifted systematically as the sulfur content of the materials increases. Their optical properties are discussed using a modified Vegards approach and the bowing parameter for these nanoalloys is reported for the first time. The alloyed structure of the nanocrystals is supported by the energy-filtered transmission electron microscope images of the samples, which show a homogeneous distribution of sulfur and selenium within the nanocrystals. X-ray photoelectron spectroscopy studies on ligand-exchanged nanocrystals confirmed the expected stoichiometry and various oxidized species.

Resonant excitation photoluminescence studies of InGaN∕GaN single quantum well structures

The optical properties of InGaN∕GaN quantum well structures, with indium fractions of 0.15 and 0.25, have been studied under resonant excitation conditions. The low-temperature (T=6K) photoluminescence spectra revealed a broad recombination peak that the authors have attributed to the acoustic-phonon assisted emission from a distribution of localized states, excited via an acoustic-phonon assisted absorption process. Comparing these results with theoretical calculations, where the authors consider the deformation potential coupling of the separately localized electron/hole pairs to an effectively continuous distribution of acoustic phonons, gives a value of approximately 2.5A for the in-plane localization length scale.

High photoluminescence quantum efficiency InGaN multiple quantum well structures emitting at 380 nm

In this paper we report the design of high room temperature photoluminescence internal efficiency InGaN-based quantum well structures emitting in the near ultraviolet at 380nm. To counter the effects of nonradiative recombination the quantum wells were designed to have a large indium fraction, high barriers, and a small quantum well thickness. To minimize the interwell and interbarrier thickness fluctuations we used Al0.2In0.005Ga0.795N barriers, where the inclusion of the small fraction of indium was found to lead to fewer structural defects and a reduction in the layer thickness fluctuations. This approach has led us to achieve, for an In0.08Ga0.92N∕Al0.2In0.005Ga0.795N multiple quantum well structure with a well width of 1.5nm, a photoluminescence internal efficiency of 67% for peak emission at 382nm at room temperature.

GaN-InGaN Quantum Well and LED Structures Grown in a Close Coupled Showerhead (CCS) MOCVD Reactor

A Close Coupled Showerhead MOCVD reactor has been used to grow GaN-InGaN quantum well (QW) structures and LEDs using two different growth regimes, one in which the wells are grown at a lower temperature than the barriers and the other in which both are grown at the same temperature. In general the optical quality of single temperature multi-quantum wells (MQWs) are superior to that of structures grown at two temperatures but the latter have been proved easier to optimise for operation at longer wavelengths. Improved emission wavelength uniformity has been noted for the single temperature structures and XRD and low temperature PL measurements of the latter have indicated that high quality structures have been achieved. Time resolved PL has shown that the radiative carrier lifetime increases with the indium content of the quantum wells making longer wavelength structures more susceptible to competition from non-radiative recombination.

Electronic Structure of a Mixed-Metal Fluoride-Centered Triangle Complex: A Potential Qubit Component

A novel fluoride-centered triangular-bridged carboxylate complex, [Ni2Cr(μ3-F)(O2C(t)Bu)6(HO2C(t)Bu)3] (1), is reported. Simple postsynthetic substitution of the terminal pivalic acids in 1 with pyridine and 4-methylpyridine led to the isolation of [Ni2Cr(μ3-F)(O2C(t)Bu)6(C5H5N)3] (2) and [Ni2Cr(μ3-F)(O2C(t)Bu)6((4-CH3)C5H4N)3] (3). Structural and magnetic characterizations carried out on the series reveal a dominating antiferromagnetic interaction between the nickel and chromium centers leading to an S = (1)/2 ground state with a very unusual value of geff = 2.48.

Role of misalignment-induced angular chirp in the electro-optic detection of THz waves.

A general description of electro-optic detection including non-collinear phase matching and finite transverse beam profiles is presented. It is shown theoretically and experimentally that non-collinear phase matching in ZnTe (and similar materials) produces an angular chirp in the χ(2)-generated optical signal. Due to this, in non-collinear THz and probe arrangements such as single-shot THz measurements or through accidental misalignment, measurement of an undistorted THz signal is critically dependent on having sufficient angular acceptance in the optical probe path. The associated spatial walk-off can also preclude the phase retardation approximation used in THz-TDS. The rate of misalignment-induced chirping in commonly used ZnTe and GaP schemes is tabulated, allowing ready analysis of a detection system.

Demonstration of sub-luminal propagation of single-cycle terahertz pulses for particle acceleration

The sub-luminal phase velocity of electromagnetic waves in free space is generally unobtainable, being closely linked to forbidden faster than light group velocities. The requirement of sub-luminal phase-velocity in laser-driven particle acceleration schemes imposes a limit on the total acceleration achievable in free space, and necessitates the use of dispersive structures or waveguides for extending the field-particle interaction. We demonstrate a travelling source approach that overcomes the sub-luminal propagation limits. The approach exploits ultrafast optical sources with slow group velocity propagation, and a group-to-phase front conversion through nonlinear optical interaction. The concept is demonstrated with two terahertz generation processes, nonlinear optical rectification and current-surge rectification. We report measurements of longitudinally polarised single-cycle electric fields with phase and group velocity between 0.77c and 1.75c. The ability to scale to multi-megavolt-per-metre field strengths is demonstrated. Our approach paves the way towards the realisation of cheap and compact particle accelerators with femtosecond scale control of particles.Controlled generation of terahertz radiation with subluminal phase velocities is a key issue in laser-driven particle acceleration. Here, the authors demonstrate a travelling-source approach utilizing the group-to-phase front conversion to overcome the sub-luminal propagation limit.

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.

Generation of longitudinally polarized terahertz pulses with field amplitudes exceeding 2 kV/cm

We demonstrate the generation of near-single cycle longitudinally polarized terahertz radiation using a large-area radially biased photoconductive antenna with a longitudinal field amplitude in excess of 2 kV/cm. The 76 mm diameter antenna was photo-excited by a 0.5 mJ amplified near-infrared femtosecond laser system and biased with a voltage of up to 100 kV applied over concentric electrodes. Amplitudes for both the transverse and longitudinal field components of the source were measured using a calibrated electro-optic detection scheme. By tightly focusing the radiation emitted from the photoconductive antenna, we obtained a maximum longitudinal field amplitude of 2.22 kV/cm with an applied bias field of 38.5 kV/cm.