Distinctive g-Factor of Moiré-Confined Excitons in van der Waals Heterostructures.

We investigated the valley Zeeman splitting of excitonic peaks in the microphotoluminescence (µPL) spectra of high-quality hBN/WS2/MoSe2/hBN heterostructures under perpendicular magnetic fields up to 20 T. We identify two neutral exciton peaks in the µPL spectra; the lower-energy peak exhibits a reduced g-factor relative to that of the higher energy peak and much lower than the recently reported values for interlayer excitons in other van der Waals (vdW) heterostructures. We provide evidence that such a discernible g-factor stems from the spatial confinement of the exciton in the potential landscape created by the moiré pattern due to lattice mismatch or interlayer twist in heterobilayers. This renders magneto-µPL an important tool to reach a deeper understanding of the effect of moiré patterns on excitonic confinement in vdW heterostructures.

Revealing the impact of strain in the optical properties of bubbles in monolayer MoSe2.

Strain plays an important role for the optical properties of monolayer transition metal dichalcogenides (TMDCs). Here, we investigate strain effects in a monolayer MoSe2 sample with a large bubble region using µ-Raman, second harmonic generation (SHG), µ-photoluminescence and magneto µ-photoluminescence at low temperature. Remarkably, our results reveal the presence of a non-uniform strain field and the observation of emission peaks at lower energies which are the signatures of exciton and trion quasiparticles red-shifted by strain effects in the bubble region, in agreement with our theoretical predictions. Furthermore, we have observed that the emission in the strained region decreases the trion binding energy and enhances the valley g-factors as compared to non-strained regions. Considering uniform biaxial strain effects within the unit cell of the TMDC monolayer (ML), our first principles calculations predict the observed enhancement of the exciton valley Zeeman effect. In addition, our results suggest that the exciton-trion fine structure plays an important role for the optical properties of strained TMDC ML. In summary, our study provides fundamental insights on the behaviour of excitons and trions in strained monolayer MoSe2 which are particularly relevant to properly characterize and understand the fine structure of excitonic complexes in strained TMDC systems/devices.

Terahertz Optomagnetism: Nonlinear THz Excitation of GHz Spin Waves in Antiferromagnetic FeBO_{3}.

A nearly single cycle intense terahertz (THz) pulse with peak electric and magnetic fields of 0.5 MV/cm and 0.16 T, respectively, excites both modes of spin resonances in the weak antiferromagnet FeBO_{3}. The high frequency quasiantiferromagnetic mode is excited resonantly and its amplitude scales linearly with the strength of the THz magnetic field, whereas the low frequency quasiferromagnetic mode is excited via a nonlinear mechanism that scales quadratically with the strength of the THz electric field and can be regarded as a THz inverse Cotton-Mouton effect. THz optomagnetism is shown to be more energy efficient than similar effects reported previously for the near-infrared spectral range.

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.

Magnetoquantum Oscillations at THz Frequencies in InSb.

The ac magnetoconductance of bulk InSb at THz frequencies in high magnetic fields, as measured by the transmission of THz radiation, shows a field-induced transmission, which at high temperatures (≈100 K) is well explained with classical magnetoplasma effects (helicon waves). However, at low temperatures (4 K), the transmitted radiation intensity shows magnetoquantum oscillations that represent the Shubnikov-de Haas effect at THz frequencies. At frequencies above 0.9 THz, when the radiation period is shorter than the Drude scattering time, an anomalously high transmission is observed in the magnetic quantum limit that can be interpreted as carrier localization at high frequencies.

A low-temperature scanning tunneling microscope capable of microscopy and spectroscopy in a Bitter magnet at up to 34 T.

We present the design and performance of a cryogenic scanning tunneling microscope (STM) which operates inside a water-cooled Bitter magnet, which can attain a magnetic field of up to 38 T. Due to the high vibration environment generated by the magnet cooling water, a uniquely designed STM and a vibration damping system are required. The STM scan head is designed to be as compact and rigid as possible, to minimize the effect of vibrational noise as well as fit the size constraints of the Bitter magnet. The STM uses a differential screw mechanism for coarse tip-sample approach, and operates in helium exchange gas at cryogenic temperatures. The reliability and performance of the STM are demonstrated through topographic imaging and scanning tunneling spectroscopy on highly oriented pyrolytic graphite at T = 4.2 K and in magnetic fields up to 34 T.

Ultrafast Magnetism of a Ferrimagnet across the Spin-Flop Transition in High Magnetic Fields.

We show that applying magnetic fields up to 30 T has a dramatic effect on the ultrafast spin dynamics in ferrimagnetic GdFeCo. Upon increasing the field beyond a critical value, the dynamics induced by a femtosecond laser excitation strongly increases in amplitude and slows down significantly. Such a change in spin response is explained by different dynamics of the Gd and FeCo magnetic sublattices following a spin-flop phase transition from a collinear to a noncollinear spin state.

Value and Anisotropy of the Electron and Hole Mass in Pure Wurtzite InP Nanowires.

The effective mass of electrons and holes in semiconductors is pivotal in determining the dynamics of carriers and their confinement energy in nanostructured materials. Surprisingly, this quantity is still unknown in wurtzite (WZ) nanowires (NWs) made of III-V compounds (e.g., GaAs, InAs, GaP, InP), where the WZ phase has no bulk counterpart. Here, we investigate the magneto-optical properties of InP WZ NWs grown by selective-area epitaxy that provides perfectly ordered NWs featuring high-crystalline quality. The combined analysis of the energy of free exciton states and impurity levels under magnetic field (B up to 29 T) allows us to disentangle the dynamics of oppositely charged carriers from the Coulomb interaction and thus to determine the values of the electron and hole effective mass. By application of B⃗ along different crystallographic directions, we also assess the dependence of the transport properties with respect to the NW growth axis (namely, the WZ c axis). The effective mass of electrons along c is me∥ = (0.078 ± 0.002) m0 (m0 is the electron mass in vacuum) and perpendicular to c is me⊥ = (0.093 ± 0.001) m0, resulting in a 20% mass anisotropy. Holes exhibit a much larger (∼320%) and opposite mass anisotropy with their effective mass along and perpendicular to c equal to mh∥ = (0.81 ± 0.18) m0 and mh⊥ = (0.250 ± 0.016) m0, respectively. While no full consensus is found with current theoretical results on WZ InP, our findings show trends remarkably similar to the experimental data available in WZ bulk materials, such as InN, GaN, and ZnO.

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.

Optical Investigation of Monolayer and Bulk Tungsten Diselenide (WSe2) in High Magnetic Fields.

Optical spectroscopy in high magnetic fields B ≤ 65 T is used to reveal the very different nature of carriers in monolayer and bulk transition metal dichalcogenides. In monolayer WSe2, the exciton emission shifts linearly with the magnetic field and exhibits a splitting that originates from the magnetic field induced valley splitting. The monolayer data can be described using a single particle picture with a Dirac-like Hamiltonian for massive Dirac Fermions, with an additional term to phenomenologically include the valley splitting. In contrast, in bulk WSe2 where the inversion symmetry is restored, transmission measurements show a distinctly excitonic behavior with absorption to the 1s and 2s states. Magnetic field induces a spin splitting together with a small diamagnetic shift and cyclotron like behavior at high fields, which is best described within the hydrogen model.

Polymersome magneto-valves for reversible capture and release of nanoparticles.

Stomatocytes are polymersomes with an infolded bowl-shaped architecture. This internal cavity is connected to the outside environment via a small 'mouth' region. Stomatocytes are assembled from diamagnetic amphiphilic block-copolymers with a highly anisotropic magnetic susceptibility, which permits to magnetically align and deform the polymeric self-assemblies. Here we show the reversible opening and closing of the mouth region of stomatocytes in homogeneous magnetic fields. The control over the size of the opening yields magneto-responsive supramolecular valves that are able to reversibly capture and release cargo. Furthermore, the increase in the size of the opening is gradual and starts at fields below 10 T, which opens the possibility of using these structures for delivery and nanoreactor applications.

Magneto-optical properties of wurtzite-phase InP nanowires.

The possibility to grow in zincblende (ZB) and/or wurtzite (WZ) crystal phase widens the potential applications of semiconductor nanowires (NWs). This is particularly true in technologically relevant III-V compounds, such as GaAs, InAs, and InP, for which WZ is not available in bulk form. The WZ band structure of many III-V NWs has been widely studied. Yet, transport (that is, carrier effective mass) and spin (that is, carrier g-factor) properties are almost experimentally unknown. We address these issues in a well-characterized material: WZ indium phosphide. The value and anisotropy of the reduced mass (µ exc) and g-factor (g exc) of the band gap exciton are determined by photoluminescence measurements under intense magnetic fields (B, up to 28 T) applied along different crystallographic directions. µ exc is 14% greater in WZ NWs than in a ZB bulk reference and it is 6% greater in a plane containing the WZ c axis than in a plane orthogonal to c. The Zeeman splitting is markedly anisotropic with g exc = |ge| = 1.4 for B⊥c (where ge is the electron g-factor) and g exc = |ge - gh,//| = 3.5 for B//c (where gh,// is the hole g-factor). A noticeable B-induced circular dichroism of the emitted photons is found only for B//c, as expected in WZ-phase materials.

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(-7) m(3) kg(-1) 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.

Giant magnetic susceptibility of gold nanorods detected by magnetic alignment.

We have determined the magnetic properties of single-crystalline Au nanorods in solution using an optically detected magnetic alignment technique. The rods exhibit a large anisotropy in the magnetic volume susceptibility (Δχ(V)). Δχ(V) increases with decreasing rod size and increasing aspect ratio and corresponds to an average volume susceptibility (χ(V)), which is drastically enhanced relative to bulk Au. This high value of χ(V) is confirmed by SQUID magnetometry and is temperature independent (between 5 and 300 K). Given this peculiar size, shape, and temperature dependence, we speculate that the enhanced χ(V) is the result of orbital magnetism due to mesoscopic electron trajectories within the nanorods.

Doubly periodic instability pattern in a smectic-A liquid crystal.

We report the observation of a doubly periodic surface defect pattern in the liquid crystal 8CB, formed during the nematic-smectic-A phase transition. The pattern results from the antagonistic alignment of the 8CB molecules, which is homeotropic at the surface and planar in the bulk of the sample cell. Within the continuum Landau-de Gennes theory of smectic liquid crystals, we find that the long period (≈10 µm) of the pattern is given by the balance between the surface anchoring and the elastic energy of curvature wall defects. The short period (≈1 µm) we attribute to a saddle-splay distortion, leading to a nonzero Gaussian curvature and causing the curvature walls to break up.

High magnetic field reveals the nature of excitons in a single GaAs/AlAs core/shell nanowire.

Magneto-photoluminescence measurements of individual zinc-blende GaAs/AlAs core/shell nanowires are reported. At low temperature, a strong emission line at 1.507 eV is observed under low power (nW) excitation. Measurements performed in high magnetic field allowed us to detect in this emission several lines associated with excitons bound to defect pairs. Such lines were observed before in epitaxial GaAs of very high quality, as reported by Kunzel and Ploog. This demonstrates that the optical quality of our GaAs/AlAs core/shell nanowires is comparable to the best GaAs layers grown by molecular beam epitaxy. Moreover, strong free exciton emission is observed even at room temperature. The bright optical emission of our nanowires in room temperature should open the way for numerous optoelectronic device applications.

Selection of supramolecular chirality by application of rotational and magnetic forces.

Many essential biological molecules exist only in one of two possible mirror-image structures, either because they possess a chiral unit or through their structure (helices, for example, are intrinsically chiral), but so far the origin of this homochirality has not been unraveled. Here we demonstrate that the handedness of helical supramolecular aggregates formed by achiral molecules can be directed by applying rotational, gravitational and orienting forces during the self-assembly process. In this system, supramolecular chirality is determined by the relative directions of rotation and magnetically tuned effective gravity, but the magnetic orientation of the aggregates is also essential. Applying these external forces only during the nucleation step of the aggregation is sufficient to achieve chiral selection. This result shows that an almost instantaneous chiral perturbation can be transferred and amplified in growing supramolecular self-assemblies, and provides evidence that a falsely chiral influence is able to induce absolute enantioselection.

Topological instabilities of spherical vesicles.

Within the framework of the Helfrich elastic theory of membranes and of differential geometry, we study the relative stability of spherical vesicles and double bubbles. We find that not only temperature but also magnetic fields can induce topological transformations between spherical vesicles and double bubbles and provide a phase diagram for the equilibrium shapes.

Tailoring the physical properties of thiol-capped PbS quantum dots by thermal annealing.

We show that the thermal annealing of thiol-capped PbS colloidal quantum dots provides a means of narrowing the nanoparticle size distribution, increasing the size of the quantum dots and facilitating their coalescence preferentially along the 100 crystallographic axes. We exploit these phenomena to tune the photoluminescence emission of an ensemble of dots and to narrow the optical linewidth to values that compare with those reported at room temperature for single PbS quantum dots. We probe the influence of annealing on the electronic properties of the quantum dots by temperature dependent studies of the photoluminescence and magneto-photoluminescence.

Oscillatory persistent currents in self-assembled quantum rings.

We report the direct measurement of the persistent current carried by a single electron by means of magnetization experiments on self-assembled InAs/GaAs quantum rings. We measured the first Aharonov-Bohm oscillation at a field of 14 T, in perfect agreement with our model based on the structural properties determined by cross-sectional scanning tunneling microscopy measurements. The observed oscillation magnitude of the magnetic moment per electron is remarkably large for the topology of our nanostructures, which are singly connected and exhibit a pronounced shape asymmetry.