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Polariton condensation in photonic crystals with high molecular orientation
摘要： We study Frenkel exciton-polariton Bose–Einstein condensation in a two-dimensional defect-free triangular photonic crystal with an organic semiconductor active medium containing bound excitons with dipole moments oriented perpendicular to the layers. We ?nd photonic Bloch modes of the structure and consider their strong coupling regime with the excitonic component. Using the Gross– Pitaevskii equation for exciton polaritons and the Boltzmann equation for the external exciton reservoir, we demonstrate the formation of condensate at the points in reciprocal space where photon group velocity equals zero. Further, we demonstrate condensation at non-zero momentum states for transverse magnetic-polarized photons in the case of a system with incoherent pumping, and show that the condensation threshold varies for different points in the reciprocal space, controlled by detuning.
关键词： organic semiconductors,photonic crystalls,photonics,exciton polaritons,Bose–Einstein condensate
更新于2025-09-23 15:21:01
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Li 1<i>s</i> core exciton in LiH studied by X-ray Raman scattering spectroscopy
摘要： The Li 1s core excitation spectra in LiH was studied by means of X-ray Raman scattering (XRS) spectroscopy in a wide range of momentum transfers q. The analysis of the near-edge region of the measured spectra in combination with q-dependent ab initio calculations of XRS spectra based on the Bethe-Salpeter equation (BSE) reveals that the prominent peak at the excitation onset arises from two main contributions, namely a pre-edge peak associated to a p-type core exciton and strong transitions to empty states near the bottom of the conduction band, which is in contrast to previous experimental studies that attributed that feature to a single excitonic peak. The p-like angular symmetry of the core exciton is supported by BSE calculations of the relative contributions to the XRS spectra from monopole and dipole transitions and by the observed decrease of its normalised intensity for increasing momentum transfers. Higher energy spectral features in the measured XRS spectra are well reproduced by BSE, as well as by real-space multiple-scattering calculations.
关键词： lithium hydride,core-exciton,X-ray Raman scattering
更新于2025-09-23 15:21:01
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Ultrafast Exciton Dissociation at the 2D-WS <sub/>2</sub> Monolayer/Perovskite Interface
摘要： In order for an excitonic photovoltaic (PV) device to perform efficiently, photogenerated excitons in the charge donor need to be dissociated through charge transfer (CT) to the acceptor rapidly after their photogeneration, and remain separated for a longer time to allow the collection of charges. To improve the efficiency of these steps, several combination of materials have been examined. Due to their excellent optical properties, two-dimensional transition metal dichalcogenides (2D-TMDs) have recently been explored. Another promising class of materials to platform efficient PVs is organic-inorganic perovskites. Here, we report on the ultrafast exciton dissociation through electron transfer from a 2D tungsten disulfide (WS2) monolayer to a thin layer of methylammonium lead iodide (CH3NH3PbI3) perovskites. Photoluminescence (PL) measurements showed that when the 2D-WS2 monolayer was covered with perovskites, its emission completely quenched, suggesting that the CT process is highly efficient. Despite that pump-probe spectroscopy measurements were carried out with a ~ 45 fs temporal resolution, the CT dynamics were not captured. A comparison of the ultrafast dynamics of the two band-edge excitons of the charge donor (2D-WS2) suggested that electron transfer is the dominant pathway of CT. Furthermore, these pump-probe measurements indicated that a small fraction of transferred electrons remained in the perovskites up to almost 2 ns. These findings may open a new horizon for understanding the dissociation of photogenerated excitons in 2D-TMD through hybridization with other class of nanomaterials.
关键词： Ultrafast Exciton Dissociation,Perovskite Interface,Hybrid Materials,Magnetic,Plasmonics,2D-WS2 Monolayer,Optical
更新于2025-09-23 15:21:01
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Self-hybridized exciton-polaritons in multilayers of transition metal dichalcogenides for efficient light absorption
摘要： Transition metal dichalcogenides (TMDCs) have attracted significant attention recently in the context of strong light-matter interaction. To observe strong coupling using these materials, excitons are typically hybridized with resonant photonic modes of stand-alone optical cavities, such as Fabry-Pérot microcavities or plasmonic nanoantennas. Here, we show that thick flakes of layered van der Waals TMDCs can themselves serve as low quality resonators due to their high background permittivity. Optical modes of such “cavities” can in turn hybridize with excitons in the same material. We perform an experimental and theoretical study of such self-hybridization in thick flakes of four common TMDC materials: WS2, WSe2, MoS2, and MoSe2. We observe splitting in reflection and transmission spectra in all four cases and provide angle-resolved dispersion measurements of exciton-polaritons as well as thickness-dependent data. Moreover, we observe significant enhancement and broadening of absorption in thick TMDC multilayers, which can be interpreted in terms of strong light-matter coupling. Remarkably, absorption reaches >50% efficiency across the entire visible spectrum, while simultaneously being weakly dependent on polarization and angle-of-incidence. Our results thus suggest formation of self-hybridized exciton-polaritons in thick TMDC flakes, which in turn may pave the way towards polaritonic and optoelectronic devices in these simple systems.
关键词： transition metal dichalcogenides,exciton-polaritons,strong coupling,nanocavities
更新于2025-09-23 15:21:01
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Long coherent dynamics of localized excitons in (In,Ga)N/GaN quantum wells
摘要： We study the coherent dynamics of localized excitons in 100 periods of 2.5-nm-thick (In,Ga)N/GaN quantum wells with 7.5% indium concentration, measured with spectroscopic resolution through two-pulse and three-pulse photon echoes at the temperature of 1.5 K. A long-lived coherent exciton dynamics is observed in the (In,Ga)N quantum wells: When the laser photon energy is tuned across the 43-meV-wide inhomogeneously broadened resonance line, the coherence time T2 varies between 45 and 255 ps, increasing with stronger exciton localization. The corresponding narrow homogeneous linewidths ranging from 5.2 to 29 μeV as well as the relatively weak exciton-phonon interaction (0.7 μeV/K) confirm a strong, quantum-dot-like exciton localization in a static disordered potential inside the (In,Ga)N quantum well layers.
关键词： localized excitons,photon echoes,exciton-phonon interaction,coherent dynamics,(In,Ga)N/GaN quantum wells
更新于2025-09-23 15:21:01
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Null Exciton Splitting in Chromophoric Greek Cross?(+) Aggregate
摘要： Exciton interactions in molecular aggregates play a crucial role in tailoring the optical behaviour of p-conjugated materials. Though vital for optoelectronic applications, ideal Greek cross-dipole (a = 908) stacking of chromophores remains elusive. We report a novel Greek cross (+) assembly of 1,7-dibromoperylene-3,4,9,10-tetracarboxylic tetrabutylester (PTE-Br2) which exhibits null exciton coupling mediated monomer-like optical characteristics in the crystalline state. In contrast, nonzero exciton coupling in X-type (a = 70.28, PTE-Br0) and J-type (a = 08, q = 48.48, PTE-Br4) assemblies have perturbed optical properties. Additionally, the semi-classical Marcus theory of charge-transfer rates predicts a selective hole transport phenomenon in the orthogonally stacked PTE-Br2. Precise rotation angle dependent optoelectronic properties in crystalline PTE-Br2 can have consequences in the rational design of novel p-conjugated materials for photonic and molecular electronic applications.
关键词： crystal engineering,chromophore aggregate,fluorescence,charge mobility,exciton splitting
更新于2025-09-23 15:21:01
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Significant Enhancement in Quantum Dot Light-Emitting Device Stability via a Cascading Hole Transport Layer
摘要： This work investigates the effect of the hole transport layer (HTL) on the stability of electroluminescent quantum dot light-emitting devices (QDLEDs). The electroluminescence half-life (LT50) of QDLEDs can be improved by 25x through the utilization of a cascading HTL (CHTL) structure with consecutive steps in highest occupied molecular orbital energy level. Using this approach, a LT50 of 864,000 hours (for an initial luminance of 100 cd m-2) is obtained for red QDLEDs using a conventional core/shell QD emitter. The CHTL primarily improves QDLED stability by shifting excessive hole accumulation away from the QD/HTL interface and toward the inter-layer HTL/HTL interfaces. The wider electron-hole recombination zone in the CHTL for electrons that have leaked from the QD layer results in less HTL degradation at the QD/HTL interface. This work highlights the significant influence of the HTL on QDLED stability and represents the longest LT50 for a QDLED based on the conventional core/shell QD structure.
关键词： quantum dot,EL stability,exciton-polaron interactions,QDLED,organic hole transport layer,exciton-induced degradation
更新于2025-09-23 15:19:57
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Quantum Dots - Theory and Applications || Theory of Excitons and Excitonic Quasimolecules Formed from Spatially Separated Electrons and Holes in Quasi-Zero- Dimensional Nanostructures
摘要： The theory of an exciton formed from a spatially separated electron and a hole is developed within the framework of the modified effective mass method. The effect of significantly increasing the exciton binding energy in quantum dots of zinc selenide, synthesized in a borosilicate glass matrix and relative to that in a zinc selenide single crystal is revealed. It is shown that the short-wavelength shift of the peak of the low-temperature luminescence spectrum of samples containing zinc selenide quantum dots, observed under experimental conditions, is caused by quantum confinement of the ground-state energy of the exciton with a spatially separated electron and hole. A review devoted to the theory of excitonic quasimolecules (biexcitons) (made up of spatially separated electrons and holes) in a nanosystem that consists of ZnSe quantum dots synthesized in a borosilicate glass matrix is developed within the context of the modified effective mass approximation. It is shown that biexciton (exciton quasimolecule) formation has a threshold character and is possible in a nanosystem, where the spacing between quantum dots' surfaces is larger than a certain critical arrangement. An analogy of the spectroscopy of the electronic states of superatoms (or artificial atoms) and individual alkali metal atoms theoretically predicted a new artificial atom that was similar to the new alkali metal atom.
关键词： excitonic quasimolecules,Excitons,superatoms,spatially separated electrons and holes,exciton binding energy,quantum dots
更新于2025-09-23 15:19:57
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Many-particle excitations in non-covalently doped single-walled carbon nanotubes
摘要： Doping of single-walled carbon nanotubes leads to the formation of new energy levels which are able to participate in optical processes. Here, we investigate (6,5)-single walled carbon nanotubes doped in a solution of hydrochloric acid using optical absorption, photoluminescence, and pump-probe transient absorption techniques. We find that, beyond a certain level of doping, the optical spectra of such nanotubes exhibit the spectral features related to two doping-induced levels, which we assign to a localized exciton X and a trion T, appearing in addition to an ordinary exciton E1. We evaluate the formation and relaxation kinetics of respective states and demonstrate that the kinetics difference between E1 and X energy levels perfectly matches the kinetics of the state T. This original finding evidences the formation of trions through nonradiative relaxation via the X level, rather than via a direct optical excitation from the ground energy state of nanotubes.
关键词： exciton,doping,optical absorption,pump-probe transient absorption,photoluminescence,trion,single-walled carbon nanotubes
更新于2025-09-23 15:19:57
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Measurement and Theoretical Interpretation of Exciton Diffusion as a Function of Intermolecular Separation for Squaraines Targeted for Bulk Heterojunction Solar Cells
摘要： The efficiency of bulk heterojunction (BHJ) organic photovoltaic (OPV) devices depends significantly upon absorption of photons and the migration of the photogenerated excited state to the heterojunction interface between the electron donor and electron acceptor. Within anilino-squaraine, molecules known for their successful use in the active layer of OPV devices, electronic aggregation strongly influences the absorption spectrum, energy transfer (EnT), and exciton migration to this heterojunction interface. Therefore, the long-range transition dipole coupling and the relative populations of the associated excited states dictate the general effectiveness of these materials in optoelectronic devices. This work presents subpicosecond transient absorption (TA) data that probe the excited-state photophysics of samples with a continuum of intermolecular separation, from monomers in solution to high-concentration solid solution thin films analogous to OPV active layers. EnT times are calculated for each squaraine concentration, and pump-power dependence provides evidence for significant EnT despite a high preponderance of H-aggregation. Theoretical modeling of essential states supports the interpretation from TA spectra that excited states relax into more tightly packed H-aggregates. This work prompts further questions regarding a far-reaching mechanistic EnT bottleneck for molecular and polymeric BHJ devices.
关键词： H-aggregation,squaraine,organic photovoltaic,bulk heterojunction,exciton diffusion,energy transfer
更新于2025-09-23 15:19:57