Site-controlled telecom-wavelength single-photon emitters in atomically-thin MoTe2

Quantum emitters (QEs) in two-dimensional transition metal dichalcogenides (2D TMDCs) have advanced to the forefront of quantum communication and transduction research. To date, QEs capable of operating in O-C telecommunication bands have not been demonstrated in TMDCs. Here we report site-controlled creation of telecom QEs emitting over the 1080 to 1550 nm telecommunication wavelength range via coupling of 2D molybdenum ditelluride (MoTe2) to strain inducing nano-pillar arrays. Hanbury Brown and Twiss experiments conducted at 10 K reveal clear photon antibunching with 90% single-photon purity. The photon antibunching can be observed up to liquid nitrogen temperature (77 K). Polarization analysis further reveals that while some QEs display cross-linearly polarized doublets with ~1 meV splitting resulting from the strain induced anisotropic exchange interaction, valley degeneracy is preserved in other QEs. Valley Zeeman splitting as well as restoring of valley symmetry in cross-polarized doublets are observed under 8 T magnetic field.

Slow Magnetic Relaxation in {[CoCxAPy)] 2.15 H2O}n MOF Built from Ladder-Structured 2D Layers with Dimeric SMM Rungs

We present the magnetic properties of the metal-organic framework {[CoCxAPy]·2.15 H2O}n (Cx = bis(carboxypropyl)tetramethyldisiloxane; APy = 4,4`-azopyridine) (1) that builds up from the stacking of 2D coordination polymers. The 2D-coordination polymer in the bc plane is formed by the adjacent bonding of [CoCxAPy] 1D two-leg ladders with Co dimer rungs, running parallel to the c-axis. The crystal packing of 2D layers shows the presence of infinite channels running along the c crystallographic axis, which accommodate the disordered solvate molecules. The Co(II) is six-coordinated in a distorted octahedral geometry, where the equatorial plane is occupied by four carboxylate oxygen atoms. Two nitrogen atoms from APy ligands are coordinated in apical positions. The single-ion magnetic anisotropy has been determined by low temperature EPR and magnetization measurements on an isostructural compound {[Zn0.8Co0.2CxAPy]·1.5 CH3OH}n (2). The results show that the Co(II) ion has orthorhombic anisotropy with the hard-axis direction in the C2V main axis, lying the easy axis in the distorted octahedron equatorial plane, as predicted by the ab initio calculations of the g-tensor. Magnetic and heat capacity properties at very low temperatures are rationalized within a S* = 1/2 magnetic dimer model with anisotropic antiferromagnetic interaction. The magnetic dimer exhibits slow relaxation of the magnetization (SMM) below 6 K in applied field, with a tlf ≈ 2 s direct process at low frequencies, and an Orbach process at higher frequencies with U/kB = 6.7 ± 0.5 K. This compound represents a singular SMM MOF built-up of Co-dimers with an anisotropic exchange interaction.

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.

Site-Controlled Telecom Single-Photon Emitters in Atomically-thin MoTe2

Quantum emitters (QEs) in two-dimensional transition metal dichalcogenides (2D TMDCs) have advanced to the forefront of quantum communication and transduction research1. To date, QEs capable of operating in O-C telecommunication bands have not been demonstrated in TMDCs.2-5 Here we report a deterministic creation of such telecom QEs emitting over the 1080 to 1550 nm wavelength range via coupling of 2D molybdenum ditelluride (MoTe2) to strain inducing nano-pillar arrays.6, 7 Our Hanbury Brown and Twiss experiment conducted at 10 K reveals clear photon antibunching with 90% single photon purity. The photon antibuching can be observed up to liquid nitrogen temperature (77 K). Polarization analysis further reveals that while some QEs display cross-linearly polarized doublets with ~1 meV splitting resulting from the strain induced anisotropic exchange interaction, valley degeneracy is preserved in other QEs. Valley Zeeman splitting as well as restoring of valley symmetry in cross-polarized doublets are observed under 8T magnetic field.

Site-Controlled Telecom Single-Photon Emitters in Atomically-thin MoTe2

Quantum emitters (QEs) in two-dimensional transition metal dichalcogenides (2D TMDCs) have advanced to the forefront of quantum communication and transduction research1 due to their unique potentials in accessing valley pseudo-spin degree of freedom (DOF)2 and facile integration into quantum-photonic, electronic and sensing platforms via the layer-by-layer-assembly approach.3 To date, QEs capable of operating in O-C telecommunication bands have not been demonstrated in TMDCs.4-7 Here we report a deterministic creation of such telecom QEs emitting over the 1080 to 1550 nm wavelength range via coupling of 2D molybdenum ditelluride (MoTe2) to strain inducing nano-pillar arrays.8,9 Our Hanbury Brown and Twiss experiment conducted at 10 K reveals clear photon antibunching with 90% single photon purity. Ultra-long lifetimes, 4-6 orders of magnitude longer than that of the 2D exciton, are also observed. Polarization analysis further reveals that while some QEs display cross-linearly polarized doublets with ~1 meV splitting resulting from the strain induced anisotropic exchange interaction, valley degeneracy is preserved in other QEs. Valley Zeeman splitting as well as restoring of valley symmetry in cross-polarized doublets are observed under 8T magnetic field. In contrast to other telecom QEs,10-12 our QEs which offer the potential to access valley DOF through single photons, could lead to unprecedented advantages in optical fiber-based quantum networks.

Anisotropic exchange interaction and field-induced SMM behaviour in a mixed valence {CoII4CoIII2} complex

We report a combined computational and experimental study of SMM behaviour in a mixed valent {CoIII2CoII4} complex with anisotropic exchange interactions.