Site-selective measurement of coupled spin pairs in an organic semiconductor.

From organic electronics to biological systems, understanding the role of intermolecular interactions between spin pairs is a key challenge. Here we show how such pairs can be selectively addressed with combined spin and optical sensitivity. We demonstrate this for bound pairs of spin-triplet excitations formed by singlet fission, with direct applicability across a wide range of synthetic and biological systems. We show that the site sensitivity of exchange coupling allows distinct triplet pairs to be resonantly addressed at different magnetic fields, tuning them between optically bright singlet ([Formula: see text]) and dark triplet quintet ([Formula: see text]) configurations: This induces narrow holes in a broad optical emission spectrum, uncovering exchange-specific luminescence. Using fields up to 60 T, we identify three distinct triplet-pair sites, with exchange couplings varying over an order of magnitude (0.3-5 meV), each with its own luminescence spectrum, coexisting in a single material. Our results reveal how site selectivity can be achieved for organic spin pairs in a broad range of systems.This work was supported by HFMLRU/ FOM and LNCMI-CNRS, members of the European Magnetic Field Laboratory (EMFL) and by EPSRC (UK) via its membership to the EMFL (grant no. EP/N01085X/1 and NS/A000060/1) and through grant no. EP/M005143/1. L.R.W. acknowledges support of the Gates-Cambridge and Winton Scholarships. We acknowledge support from Labex ANR-10-LABX-0039-PALM, ANR SPINEX, and DFG SPP-1601 (Bi-464/10-2)

Shape characterization of polymersome morphologies via light scattering techniques

\u3cp\u3ePolymersomes, vesicles self-assembled from amphiphilic block copolymers, are well known for their robustness and for their broad applicability. Generating polymersomes of different shape is a topic of recent attention, specifically in the field of biomedical applications. To obtain information about their exact shape, tomography based on cryo-electron microscopy is usually the most preferred technique. Unfortunately, this technique is rather time consuming and expensive. Here we demonstrate an alternative analytical approach for the characterization of differently shaped polymersomes such as spheres, prolates and discs via the combination of multi-angle light scattering (MALS) and quasi-elastic light scattering (QELS). The use of these coupled techniques allowed for accurate determination of both the radius of gyration (R\u3csub\u3eg\u3c/sub\u3e) and the hydrodynamic radius (R\u3csub\u3eh\u3c/sub\u3e). This afforded us to determine the shape ratio ρ (R\u3csub\u3eg\u3c/sub\u3e/R\u3csub\u3eh\u3c/sub\u3e) with which we were able to distinguish between polymersome spheres, discs and rods.\u3c/p\u3

Separate electron-hole confinement in composite InAsyP 1-y/Ga xIn1-xAs quantum wells

Composite double qunatum wells made from materials with a type-II band line-up have been grown to realize separate confinement in real space for electrons and holes. We have observed a substantial blue shift of the lowest energy transition in such composite double quantum wells. The photocurrent measurements demonstrate a linear Stark shift due to the separate confinement in real space for electrons and holes. The charge separation is up to 45 Å in the strain balanced InAs0.42P0.58/Ga0.67In0.33As samples. The experimental results agree very well with calculations in the framework of Bir-Pikus strain Hamiltonian

Shaping polymersomes into predictable morphologies via out-of-equilibrium self-assembly

Polymersomes are bilayer vesicles, self-assembled from amphiphilic block copolymers. They are versatile nanocapsules with adjustable properties, such as flexibility, permeability, size and functionality. However, so far no methodological approach to control their shape exists. Here we demonstrate a mechanistically fully understood procedure to precisely control polymersome shape via an out-of-equilibrium process. Carefully selecting osmotic pressure and permeability initiates controlled deflation, resulting in transient capsule shapes, followed by reinflation of the polymersomes. The shape transformation towards stomatocytes, bowl-shaped vesicles, was probed with magnetic birefringence, permitting us to stop the process at any intermediate shape in the phase diagram. Quantitative electron microscopy analysis of the different morphologies reveals that this shape transformation proceeds via a long-predicted hysteretic deflation–inflation trajectory, which can be understood in terms of bending energy. Because of the high degree of controllability and predictability, this study provides the design rules for accessing polymersomes with all possible different shapes

Dark excitons and the elusive valley polarization in transition metal dichalcogenides

A rate equation model for the dark and bright excitons kinetics is proposed which explains the wide variation in the observed degree of circular polarization of the PL emission in different TMDs monolayers. Our work suggests that the dark exciton states play an important, and previously unsuspected role in determining the degree of polarization of the PL emission. A dark exciton ground state provides a robust reservoir for valley polarization, which tries to maintain a Boltzmann distribution of the bright exciton states in the same valley via the intra valley bright dark exciton scattering mechanism. The dependence of the degree of circular polarization on the detuning energy of the excitation in MoSe2 suggests that the electron-hole exchange interaction dominates over two LA phonon emission mechanism for inter valley scattering in TMDs

Tuneable paramagnetic susceptibility and exciton g-factor in Mn-doped PbS colloidal nanocrystals

We report on PbS colloidal nanocrystals that combine within one structure solubility in physiological solvents with near-infrared photoluminescence, and magnetic and optical properties tuneable by the controlled incorporation of magnetic impurities (Mn). We use high magnetic fields (B up to 30 T) to measure the magnetization of the nanocrystals in liquid and the strength of the sp-d exchange interaction between the exciton and the Mn-ions. With increasing Mn-content from 0.1% to 7%, the mass magnetic susceptibility increases at a rate of ∼10 m kg per Mn percentage; correspondingly, the exciton g-factor decreases from 0.47 to 0.10. The controlled modification of the paramagnetism, fluorescence and exciton g-factor of the nanocrystals is relevant to the implementation of these paramagnetic semiconductor nanocrystals in quantum technologies ranging from quantum information to magnetic resonance imaging. This journal is © the Partner Organisations 2014

Intervalley Scattering of Interlayer Excitons in a MoS2/MoSe2/MoS2 Heterostructure in High Magnetic Field

Degenerate extrema in the energy dispersion of charge carriers in solids, also referred to as valleys, can be regarded as a binary quantum degree of freedom, which can potentially be used to implement valleytronic concepts in van der Waals heterostructures based on transition metal dichalcogenides. Using magneto-photoluminescence spectroscopy, we achieve a deeper insight into the valley polarization and depolarization mechanisms of interlayer excitons formed across a MoS2/MoSe2 /MoS2 heterostructure. We account for the nontrivial behavior of the valley polarization as a function of the magnetic field by considering the interplay between exchange interaction and phonon-mediated intervalley scattering in a system consisting of Zeeman-split energy levels. Our results represent a crucial step toward the understanding of the properties of interlayer excitons with strong implications for the implementation of atomically thin valleytronic devices

Erratum : Excited states of ring-shaped (InGa)As quantum dots in a GaAs/(AlGa)As quantum well

No abstract: erratu