Longitudinal and transversal spin dynamics of donor-bound electrons in fluorine-doped ZnSe: spin inertia versus Hanle effect

The spin dynamics of the strongly localized, donor-bound electrons in fluorine-doped ZnSe epilayers is studied by pump-probe Kerr rotation techniques. A method exploiting the spin inertia is developed and used to measure the longitudinal spin relaxation time, $T_1$, in a wide range of magnetic fields, temperatures, and pump densities. The $T_1$ time of the donor-bound electron spin of about 1.6 $\mu$s remains nearly constant for external magnetic fields varied from zero up to 2.5 T (Faraday geometry) and in a temperature range $1.8-45$ K. The inhomogeneous spin dephasing time, $T_2^*=8-33$ ns, is measured using the resonant spin amplification and Hanle effects under pulsed and steady-state pumping, respectively. These findings impose severe restrictions on possible spin relaxation mechanisms.Comment: 10 pages, 7 figure

Inhomogeneous nuclear spin polarization induced by helicity-modulated optical excitation of fluorine-bound electron spins in ZnSe

Optically-induced nuclear spin polarization in a fluorine-doped ZnSe epilayer is studied by time-resolved Kerr rotation using resonant excitation of donor-bound excitons. Excitation with helicity-modulated laser pulses results in a transverse nuclear spin polarization, which is detected as a change of the Larmor precession frequency of the donor-bound electron spins. The frequency shift in dependence on the transverse magnetic field exhibits a pronounced dispersion-like shape with resonances at the fields of nuclear magnetic resonance of the constituent zinc and selenium isotopes. It is studied as a function of external parameters, particularly of constant and radio frequency external magnetic fields. The width of the resonance and its shape indicate a strong spatial inhomogeneity of the nuclear spin polarization in the vicinity of a fluorine donor. A mechanism of optically-induced nuclear spin polarization is suggested based on the concept of resonant nuclear spin cooling driven by the inhomogeneous Knight field of the donor-bound electron.Comment: 12 pages, 11 figure

Multi-level Meta-workflows: New Concept for Regularly Occurring Tasks in Quantum Chemistry

Background: In Quantum Chemistry, many tasks are reoccurring frequently, e.g. geometry optimizations, benchmarking series etc. Here, workflows can help to reduce the time of manual job definition and output extraction. These workflows are executed on computing infrastructures and may require large computing and data resources. Scientific workflows hide these infrastructures and the resources needed to run them. It requires significant efforts and specific expertise to design, implement and test these workflows. Significance: Many of these workflows are complex and monolithic entities that can be used for particular scientific experiments. Hence, their modification is not straightforward and it makes almost impossible to share them. To address these issues we propose developing atomic workflows and embedding them in meta-workflows. Atomic workflows deliver a well-defined research domain specific function. Publishing workflows in repositories enables workflow sharing inside and/or among scientific communities. We formally specify atomic and meta-workflows in order to define data structures to be used in repositories for uploading and sharing them. Additionally, we present a formal description focused at orchestration of atomic workflows into meta-workflows. Conclusions: We investigated the operations that represent basic functionalities in Quantum Chemistry and developed that relevant atomic workflows and combined them into meta-workflows. Having these workflows we defined the structure of the Quantum Chemistry workflow library and uploaded these workflows in the SHIWA Workflow Repository

Lasing of donor-bound excitons in ZnSe microdisks

Excitons bound to flourine atoms in ZnSe have the potential for several quantum optical applications. Examples include optically accessible quantum memories for quantum information processing and lasing without inversion. These applications require the bound-exciton transitions to be coupled to cavities with high cooperativity factors, which results in the experimental observation of low-threshold lasing. We report such lasing from fluorine-doped ZnSe quantum wells in 3 and 6 micron microdisk cavities. Photoluminescence and selective photoluminescence spectroscopy confirm that the lasing is due to bound-exciton transitions.Comment: 4 pages, 3 figures; introduction rewritte

Extended spin coherence of the zinc-vacancy centers in ZnSe with fast optical access

Qubits based on crystal defect centers have been shown to exhibit long spin coherence times, up to seconds at room temperature. However, they are typically characterized by a comparatively slow initialization timescale. Here, fluorine implantation into ZnSe epilayers is used to induce defect states that are identified as zinc vacancies. We study the carrier spin relaxation in these samples using various pump-probe measurement methods, assessing phenomena such as resonant spin amplification, polarization recovery, and spin inertia in transverse or longitudinal magnetic field. The spin dynamics in isotopically natural ZnSe show a significant influence of the nuclear spin bath. Removing this source of relaxation by using isotopic purification, we isolate the anisotropic exchange interaction as the main spin dephasing mechanism and find spin coherence times of 100 ns at room temperature, with the possibility of fast optical access on the picosecond time scales through excitonic transitions of ZnSe