A comprehensive study of the optical properties of PbS nanocrystals (NCs) is reported that includes the temperature dependent absorption, photoluminescence (PL) and PL lifetime in the range of 3-300 K. The absorption and PL are found to display different temperature dependent behaviour though both redshift as temperature is reduced. This results in a temperature dependent Stokes shift which increases from ∼75 meV at 300 K with reducing temperature until saturating at ∼130 meV below ∼150 K prior to a small reduction to 125 meV upon cooling from 25 to 3 K. The PL lifetime is found to be single exponential at 3 K with a lifetime of τ(1) = 6.5 μs. Above 3 K biexponential behaviour is observed with the lifetime for each process displaying a different temperature dependence. The Stokes shift is modelled using a three-level rate equation model incorporating temperature dependent parameter values obtained via fitting phenomenological relationships to the observed absorption and PL behaviour. This results in a predicted energy difference between the two emitting states of ∼6 meV which is close to the excitonic exchange energy splitting predicted theoretically for these systems.

Over the last two decades, prototype devices for future classical and quantum computing technologies have been fabricated, by using scanning tunneling microscopy and hydrogen resist lithography to position phosphorus atoms in silicon with atomic-scale precision. Despite these successes, phosphine remains the only donor precursor molecule to have been demonstrated as compatible with the hydrogen resist lithography technique. The potential benefits of atomic-scale placement of alternative dopant species have, until now, remained unexplored. In this work, we demonstrate the successful fabrication of atomic-scale structures of arsenic-in-silicon. Using a scanning tunneling microscope tip, we pattern a monolayer hydrogen mask to selectively place arsenic atoms on the Si(001) surface using arsine as the precursor molecule. We fully elucidate the surface chemistry and reaction pathways of arsine on Si(001), revealing significant differences to phosphine. We explain how these differences result in enhanced surface immobilization and inplane confinement of arsenic compared to phosphorus, and a dose-rate independent arsenic saturation density of 0.24±0.04 monolayers. We demonstrate the successful encapsulation of arsenic delta-layers using silicon molecular beam epitaxy, and find electrical characteristics that are competitive with equivalent structures fabricated with phosphorus. Arsenic delta-layers are also found to offer improvement in out-of-plane confinement compared to similarly prepared phosphorus layers, while still retaining >80% carrier activation and sheet resistances of <2 kΩ/□. These excellent characteristics of arsenic represent opportunities to enhance existing capabilities of atomic-scale fabrication of dopant structures in silicon, and are particularly important for threedimensional devices, where vertical control of the position of device components is critical. TOC GRAPHICS

Laboratory spectroscopy of atomic hydrogen in a magnetic flux density of 10 5 T (1 gigagauss), the maximum observed on high-field magnetic white dwarfs, is impossible because practically available fields are about a thousand times less. In this regime, the cyclotron and binding energies become equal. Here we demonstrate Lyman series spectra for phosphorus impurities in silicon up to the equivalent field, which is scaled to 32.8 T by the effective mass and dielectric constant. The spectra reproduce the high-field theory for free hydrogen, with quadratic Zeeman splitting and strong mixing of spherical harmonics. They show the way for experiments on He and H 2 analogues, and for investigation of He 2 , a bound molecule predicted under extreme field conditions.

We measure transverse magnetically focused photocurrent signals in an InSb/InAlSb quantum well device. Using optical spin orientation by modulated circularly polarized light an electron spin dependent signal is observed due to the spin-orbit interaction. Simulations of the focusing signal are performed using a classical billiard ball model which includes both spin precession and a spin dependent electron energy. The simulated data suggests that a signal dependent on the helicity of the incident light is expected for a Rashba parameter α > 0.1 eVÅ and that a splitting of the focusing signal is not expected to be observed in linear polarised photocurrent and purely electrical measurements.

The ability to control dynamics of quantum states by optical interference, and subsequent electrical read-out, is crucial for solid state quantum technologies. Ramsey interference has been successfully observed for spins in silicon and nitrogen vacancy centres in diamond, and for orbital motion in InAs quantum dots. Here we demonstrate terahertz optical excitation, manipulation and destruction via Ramsey interference of orbital wavepackets in Si:P with electrical read-out. We show milliradian control over the wavefunction phase for the two-level system formed by the 1s and 2p states. The results have been verified by all-optical echo detection methods, sensitive only to coherent excitations in the sample. The experiments open a route to exploitation of donors in silicon for atom trap physics, with concomitant potential for quantum computing schemes, which rely on orbital superpositions to, for example, gate the magnetic exchange interactions between impurities.