Two-dimensional (2D) compounds provide unique building blocks for novel layered devices and hybrid photonic structures. However, large surface-to-volume ratio in thin films enhances the significance of surface interactions and charging effects requir
ing new understanding. Here we use micro-photoluminescence (PL) and ultrasonic force microscopy to explore the influence of the dielectric environment on optical properties of a few monolayer MoS2 films. PL spectra for MoS2 films deposited on SiO2 substrates are found to vary widely. This film-to-film variation is suppressed by additional capping of MoS2 with SiO2 and SiN, improving mechanical coupling of MoS2 with surrounding dielectrics. We show that the observed PL non-uniformities are related to strong variation in the local electron charging of MoS2 films. In completely encapsulated films, negative charging is enhanced leading to uniform optical properties. Observed great sensitivity of optical characteristics of 2D films to surface interactions has important implications for optoelectronics applications of layered materials.
We use photoluminescence spectroscopy of bright and dark exciton states in single InP/GaInP quantum dots to measure hyperfine interaction of the valence band hole with nuclear spins polarized along the sample growth axis. The ratio of the hyperfine c
onstants for the hole (C) and electron (A) is found to be C/A~-0.11. In InP dots the contribution of spin 1/2 phosphorus nuclei to the hole-nuclear interaction is weak, which enables us to determine experimentally the value of C for spin 9/2 indium nuclei as C_In~-5 micro-eV. This high value of C is in good agreement with recent theoretical predictions and suggests that the hole-nuclear spin interaction has to be taken into account when considering spin qubits based on holes.
We report optically detected nuclear magnetic resonance (ODNMR) measurements on small ensembles of nuclear spins in single GaAs quantum dots. Using ODNMR we make direct measurements of the inhomogeneous Knight field from a photo-excited electron whic
h acts on the nuclei in the dot. The resulting shifts of the NMR peak can be optically controlled by varying the electron occupancy and its spin orientation, and lead to strongly asymmetric lineshapes at high optical excitation. The all-optical control of the NMR lineshape will enable position-selective control of small groups of nuclear spins in a dot. Our calculations also show that the asymmetric NMR peak lineshapes can provide information on the volume of the electron wave-function, and may be used for measurements of non-uniform distributions of atoms in nano-structures.
We demonstrate that efficient optical pumping of nuclear spins in semiconductor quantum dots (QDs) can be achieved by resonant pumping of optically forbidden transitions. This process corresponds to one-to-one conversion of a photon absorbed by the d
ot into a polarized nuclear spin, which also has potential for initialization of hole spin in QDs. Pumping via the forbidden transition is a manifestation of the optical solid effect, an optical analogue of the effect previously observed in electron spin resonance experiments in the solid state. We find that by employing this effect, nuclear polarization of 65% can be achieved, the highest reported so far in optical orientation studies in QDs. The efficiency of the spin pumping exceeds that employing the allowed transition, which saturates due to the low probability of electron-nuclear spin flip-flop.
The nature of the nano-scale environment presents a major challenge for solid-state implementation of spin-based qubits. In this work, a single electron spin in an optically pumped nanometer-sized III-V semiconductor quantum dot is used to control a
macroscopic nuclear spin of several thousand nuclei, freezing its decay and leading to spin life-times exceeding 100 seconds at low temperatures. Few-millisecond-fast optical initialization of the nuclear spin is followed by a slow decay exhibiting random telegraph signals at long delay times, arising from low probability electron jumps out of the dot. The remarkably long spin life-time in a dot surrounded by a densely-packed nuclear spin environment arises from the Knight field created by the resident electron, which leads to suppression of nuclear spin depolarization.
Sharp threshold-like transitions between two stable nuclear spin polarizations are observed in optically pumped individual InGaAs self-assembled quantum dots embedded in a Schottky diode when the bias applied to the diode is tuned. The abrupt transit
ions lead to the switching of the Overhauser field in the dot by up to 3 Tesla. The bias-dependent photoluminescence measurements reveal the importance of the electron-tunneling-assisted nuclear spin pumping. We also find evidence for the resonant LO-phonon-mediated electron co-tunneling, the effect controlled by the applied bias and leading to the reduction of the nuclear spin pumping rate.
Sizable nuclear spin polarization is pumped in individual InP/GaInP dots in a wide range of external magnetic fields B_ext=0-5T by circularly polarized optical excitation. We observe nuclear polarization of up to ~40% at Bext=1.5T and corresponding t
o an Overhauser field of ~1.2T. We find a strong feedback of the nuclear spin on the spin pumping efficiency. This feedback, produced by the Overhauser field, leads to nuclear spin bi-stability at low magnetic fields of Bext=0.5-1.5T. We find that the exciton Zeeman energy increases markedly, when the Overhauser field cancels the external field. This counter-intuitive result is shown to arise from the opposite contribution of the electron and hole Zeeman splittings to the total exciton Zeeman energy.
Nuclear polarization dynamics are measured in the nuclear spin bi-stability regime in a single optically pumped InGaAs/GaAs quantum dot. The controlling role of nuclear spin diffusion from the dot into the surrounding material is revealed in pump-pro
be measurements of the non-linear nuclear spin dynamics. We measure nuclear spin decay times in the range 0.2-5 sec, strongly dependent on the optical pumping time. The long nuclear spin decay arises from polarization of the material surrounding the dot by spin diffusion for long (>5sec) pumping times. The time-resolved methods allow the detection of the unstable nuclear polarization state in the bi-stability regime otherwise undetectable in cw experiments.
