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Register a new userSpatially, Temporally and Polarization-Resolved Photoluminescence Exploration of Excitons in Crystalline Phthalocyanine Thin Films
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The lack of long range order in organic semiconductor thin films prevents the unveiling of the complete nature of excitons in optical experiments, because the diffraction limited beam diameters in the bandgap region far exceed typical crystalline grain sizes. Here we present spatially-, temporally- and polarization-resolved dual photoluminescence/linear dichroism microscopy experiments that investigate exciton states within a single crystalline grain in solution-processed phthalocyanine thin films. These experiments reveal the existence of a delocalized singlet exciton, polarized along the high mobility axis in this quasi-1D electronic system. The strong delocalized {pi} orbitals overlap controlled by the molecular stacking along the high mobility axis is responsible for breaking the radiative recombination selection rules. Using our linear dichroism scanning microscopy setup we further established a rotation of molecules (i.e. a structural phase transition) that occurs above 100 K prevents the observation of this exciton at room temperature.
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The origins of indirect spin exchange in crystalline thin films of Copper Octabutoxy Phthalocyanine (Cu-OBPc) are investigated using Magnetic Circular Dichroism (MCD) spectroscopy. These studies are made possible by a solution deposition technique which produces highly ordered films with macroscopic grain sizes suitable for optical studies. For temperatures lower than 2 K, the contribution of a specific state in the valence band manifold originating from the hybridized lone pair in nitrogen orbitals of the Phthalocyanine ring, bears the Brillouin-like signature of an exchange interaction with the localized $textit{d}$-shell Cu spins. A comprehensive MCD spectral analysis coupled with a molecular field model of a $sigmapi-d$ exchange analogous to $textit{sp-d}$ interactions in Diluted Magnetic Semiconductors (DMS) renders an enhanced Zeeman splitting and a modified $textit{g}$-factor of -4 for the electrons that mediate the interaction. These studies define an experimental tool for identifying electronic states involved in spin-dependent exchange interactions in organic materials.
Ultrafast pump-probe technique is a powerful tool to understand and manipulate properties of materials for designing novel quantum devices. An intense, single cycle terahertz pulse can change the intrinsic properties of semiconductor quantum dots to have different luminescence. In a hybrid system of plasmon and exciton, the coherence and coupling between these two degrees of freedom play an important role on their optical properties. Therefore, we consider a terahertz pump optical probe experiment in the hybrid systems where the terahertz pump pulse couples to the exciton degrees of freedom on the quantum dot. The time resolved photoluminescence of the hybrid system shows that the response of the characteristic frequency shifts according to the overlap between the pump and probe pulses. Furthermore, the resonance between the exciton and plasmons can be induced by the terahertz pump pulse in some parameter regimes. Our results show the terahertz driven hybrid system can be a versatile tool for manipulating the material properties and open a new route to design modern optical devices.
In magnetic topological phases of matter, the quantum anomalous Hall (QAH) effect is an emergent phenomenon driven by ferromagnetic doping, magnetic proximity effects and strain engineering. The realization of QAH states with multiple dissipationless edge and surface conduction channels defined by a Chern number $mathcal{C}geq1$ was foreseen for the ferromagnetically ordered SnTe class of topological crystalline insulators (TCIs). From magnetotransport measurements on Sn$_{1-x}$Mn$_{x}$Te ($0.00leq{x}leq{0.08}$)(111) epitaxial thin films grown by molecular beam epitaxy on BaF$_{2}$ substrates, hole mediated ferromagnetism is observed in samples with $xgeq0.06$ and the highest $T_mathrm{c}sim7.5,mathrm{K}$ is inferred from an anomalous Hall behavior in Sn$_{0.92}$Mn$_{0.08}$Te. The sizable anomalous Hall angle $sim$0.3 obtained for Sn$_{0.92}$Mn$_{0.08}$Te is one of the greatest reported for magnetic topological materials. The ferromagnetic ordering with perpendicular magnetic anisotropy, complemented by the inception of anomalous Hall effect in the Sn$_{1-x}$Mn$_{x}$Te layers for a thickness commensurate with the decay length of the top and bottom surface states, points at Sn$_{1-x}$Mn$_{x}$Te as a preferential platform for the realization of QAH states in ferromagnetic TCIs.
Raman scattering and photoluminescence spectroscopy are used to investigate the optical properties of single layer black phosphorus obtained by mechanical exfoliation of bulk crystals under an argon atmosphere. The Raman spectroscopy, performed in situ on the same flake as the photoluminescence measurements, demonstrates the single layer character of the investigated samples. The emission spectra, dominated by excitonic effects, display the expected in plane anisotropy. The emission energy depends on the type of substrate on which the flake is placed due to the different dielectric screening. Finally, the blue shift of the emission with increasing temperature is well described using a two oscillator model for the temperature dependence of the band gap.
The photoluminescence (PL) spectrum of transition metal dichalcogenides (TMDs) shows a multitude of emission peaks below the bright exciton line and not all of them have been explained yet. Here, we study the emission traces of phonon-assisted recombinations of momentum-dark excitons. To this end, we develop a microscopic theory describing simultaneous exciton, phonon and photon interaction and including consistent many-particle dephasing. We explain the drastically different PL below the bright exciton in tungsten- and molybdenum-based materials as result of different configurations of bright and dark states. In good agreement with experiments, we show that WSe$_2$ exhibits clearly visible low-temperature PL signals stemming from the phonon-assisted recombination of momentum-dark excitons.
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