J Phys Chem C Nanomater Interfaces
March 2024
Solution-processable semiconductors with antiferromagnetic (AFM) order are attractive for future spintronics and information storage technology. Halide perovskites containing magnetic ions have emerged as multifunctional materials, demonstrating a cross-link between structural, optical, electrical, and magnetic properties. However, stable optoelectronic halide perovskites that are antiferromagnetic remain sparse, and the critical design rules to optimize magnetic coupling still must be developed.
View Article and Find Full Text PDFUsing the diamagnetic anisotropy of polymers for the characterization of polymers and polymer aggregates is a relatively new approach in the field of soft-matter and polymer research. So far, a good and thorough quantitative description of these diamagnetic properties has been lacking. Using a simple equation that links the magnetic properties of an average polymer repeating unit to those of the polymer vesicle of any shape, we measured, using magnetic birefringence, the average diamagnetic anisotropy of a polystyrene (PS) repeating unit, Δ, inside a poly(ethylene glycol)-polystyrene (PEG-PS) polymersome membrane as a function of the PS-length and as a function of the preparation method.
View Article and Find Full Text PDFThe interplay of the nonequivalent corners in the Brillouin zone of transition metal dichalcogenides (TMDCs) has been investigated extensively. While experimental and theoretical works contributed to a detailed understanding of the relaxation of selective optical excitations and the related relaxation rates, only limited microscopic descriptions of stationary experiments are available so far. Here we present microscopic calculations for the nonequilibrium steady state properties of excitons during continuous wave pumping exemplary for monolayer MoSe_{2}.
View Article and Find Full Text PDFNanocontainers that can sense and respond to environmental stimuli like cells are desirable for next-generation delivery systems. However, it is still a grand challenge for synthetic nanocontainers to mimic or even surpass the shape adaption of cells, which may produce novel compartments for cargo loading. Here, this work reports the engineering of compartment network with a single polymer vesicle by unraveling osmotic stress-dependent deformation.
View Article and Find Full Text PDFThe excellent optoelectronic performance of lead halide perovskites has generated great interest in their fundamental properties. The polar nature of the perovskite lattice means that electron-lattice coupling is governed by the Fröhlich interaction. Still, considerable ambiguity exists regarding the phonon modes that participate in this crucial mechanism.
View Article and Find Full Text PDFAdvanced van der Waals (vdW) heterostructure devices rely on the incorporation of high quality dielectric materials which need to possess a low defect density as well as being atomically smooth and uniform. In this work we explore the use of talc dielectrics as a potentially clean alternative substrate to hexagonal boron nitride (hBN) for few-layer transition metal dichalcogenide (TMDC) transistors and excitonic TMDC monolayers. We find that talc dielectric transistors show small hysteresis which does not depend strongly on sweep rate and show negligible leakage current for our studied dielectric thicknesses.
View Article and Find Full Text PDFWe report the direct observation of strong coupling between magnons and phonons in a two-dimensional antiferromagnetic semiconductor FePS_{3}, via magneto-Raman spectroscopy at magnetic fields up to 30 Tesla. A Raman-active magnon at 121 cm^{-1} is identified through Zeeman splitting in an applied magnetic field. At a field-driven resonance with a nearby phonon mode, a hybridized magnon-phonon quasiparticle is formed due to strong coupling between the two modes.
View Article and Find Full Text PDFFor decades, it has been reported that some organic crystals suddenly crack, break, or jump when they are heated from room temperature. Recently, such crystals have been intensively studied both in fundamental science and for high-speed mechanical device applications. According to these studies, the sudden crystal motions have been attributed to structural phase transitions induced by heating.
View Article and Find Full Text PDFThe recombination dynamics and spin polarization of excitons in CdSe nanocrystals synthesized in a glass matrix are investigated using polarized photoluminescence in high magnetic fields up to 30 Tesla. The dynamics are accelerated by increasing temperature and magnetic field, confirming the dark exciton nature of low-temperature photoluminescence (PL). The circularly polarized PL in magnetic fields reveals several unusual appearances: (i) a spectral dependence of the polarization degree, (ii) its low saturation value, and (iii) a stronger intensity of the Zeeman component which is higher in energy.
View Article and Find Full Text PDFThe formation of wurtzite (WZ) phase in III-V nanowires (NWs) such as GaAs and InP is a complication hindering the growth of pure-phase NWs, but it can also be exploited to form NW homostructures consisting of alternate zincblende (ZB) and WZ segments. This leads to different forms of nanostructures, such as crystal-phase superlattices and quantum dots. Here, we investigate the electronic properties of the simplest, yet challenging, of such homostructures: InP NWs with a single homojunction between pure ZB and WZ segments.
View Article and Find Full Text PDFIn traditional tissue engineering, synthetic or natural scaffolds are usually used as removable temporal support, which involves some biotechnology limitations. The concept of "scaffield" approach utilizing the physical fields instead of biomaterial scaffold has been proposed recently. In particular, a combination of intense magnetic and acoustic fields can enable rapid levitational bioassembly of complex-shaped 3D tissue constructs from tissue spheroids at low concentration of paramagnetic agent (gadolinium salt) in the medium.
View Article and Find Full Text PDFThe fast-growing field of atomically thin semiconductors urges a new understanding of two-dimensional excitons, which entirely determine their optical responses. Here, taking layered lead halide perovskites as an example of unconventional two-dimensional semiconductors, by means of versatile optical spectroscopy measurements, we resolve fine-structure splitting of bright excitons of up to ∼2 meV, which is among the largest values in two-dimensional semiconducting systems. The large fine-structure splitting is attributed to the strong electron-hole exchange interaction in layered perovskites, which is proven by the optical emission in high magnetic fields of up to 30 T.
View Article and Find Full Text PDFThe feasibility of magnetic levitational bioassembly of tissue-engineered constructs from living tissue spheroids in the presence of paramagnetic ions (i.e. Gd) was recently demonstrated.
View Article and Find Full Text PDFHeterostructured two-dimensional colloidal nanoplatelets are a class of material that has attracted great interest for optoelectronic applications due to their high photoluminescence yield, atomically tunable thickness, and ultralow lasing thresholds. Of particular interest are laterally heterostructured core-crown nanoplatelets with a type-II band alignment, where the in-plane spatial separation of carriers leads to indirect (or charge transfer) excitons with long lifetimes and bright, highly Stokes shifted emission. Despite this, little is known about the nature of the lowest energy exciton states responsible for emission in these materials.
View Article and Find Full Text PDFColloidal InP core nanocrystals are taking over CdSe-based nanocrystals, notably in optoelectronic applications. Despite their use in commercial devices, such as display screens, the optical properties of InP nanocrystals and especially their relation to the exciton fine structures remain poorly understood. In this work, we show that the ensemble magneto-optical properties of InP-based core/shell nanocrystals investigated in strong magnetic fields up to 30 T are strikingly different from other colloidal nanostructures.
View Article and Find Full Text PDFThe fine structure of exciton states in colloidal quantum dots (QDs) results from the compound effect of anisotropy and electron-hole exchange. By means of single-dot photoluminescence spectroscopy, we show that the emission of photoexcited InP/ZnSe QDs originates from radiative recombination of such fine structure exciton states. Depending on the excitation power, we identify a bright exciton doublet, a trion singlet, and a biexciton doublet line that all show pronounced polarization.
View Article and Find Full Text PDFNanocrystalline InP quantum dots (QDs) hold promise for heavy-metal-free optoelectronic applications due to their bright and size-tunable emission in the visible range. Photochemical stability and high photoluminescence (PL) quantum yield are obtained by a diversity of epitaxial shells around the InP core. To understand and optimize the emission line shapes, the exciton fine structure of InP core/shell QD systems needs be investigated.
View Article and Find Full Text PDFAtomically thin semiconductors provide an ideal testbed to investigate the physics of Coulomb-bound many-body states. We shed light on the intricate structure of such complexes by studying the magnetic-field-induced splitting of biexcitons in monolayer WS_{2} using polarization-resolved photoluminescence spectroscopy in out-of-plane magnetic fields up to 30 T. The observed g factor of the biexciton amounts to about -3.
View Article and Find Full Text PDFDegenerate 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 MoS/MoSe/MoS 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.
View Article and Find Full Text PDFWe study the band-edge exciton fine structure and in particular its bright-dark splitting in colloidal semiconductor nanocrystals by four different optical methods based on fluorescence line narrowing and time-resolved measurements at various temperatures down to 2 K. We demonstrate that all these methods provide consistent splitting values and discuss their advances and limitations. Colloidal CdSe nanoplatelets with thicknesses of 3, 4 and 5 monolayers are chosen for experimental demonstrations.
View Article and Find Full Text PDFWe address spin properties and spin dynamics of carriers and charged excitons in CdSe/CdS colloidal nanoplatelets with thick shells. Magneto-optical studies are performed by time-resolved and polarization-resolved photoluminescence, spin-flip Raman scattering and picosecond pump-probe Faraday rotation in magnetic fields up to 30 T. We show that at low temperatures the nanoplatelets are negatively charged so that their photoluminescence is dominated by radiative recombination of negatively charged excitons (trions).
View Article and Find Full Text PDFMonolayers of semiconducting transition metal dichalcogenides exhibit intriguing fundamental physics of strongly coupled spin and valley degrees of freedom for charge carriers. While the possibility of exploiting these properties for information processing stimulated concerted research activities towards the concept of valleytronics, maintaining control over spin-valley polarization proved challenging in individual monolayers. A promising alternative route explores type II band alignment in artificial van der Waals heterostructures.
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