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Theory of relaxation oscillations in exciton-polariton condensates
摘要： We provide an analytical and numerical description of relaxation oscillations in the nonresonantly pumped polariton condensate. Presented considerations are based on coupled rate equations that are derived from the open dissipative Gross-Pitaevskii model. The evolution of the condensate density can be explained qualitatively by studying the topology of the trajectory in phase space. We use a ?xed points analysis for the classi?cation of the different regimes of condensate dynamics, including fast stabilization, slow oscillations, and ultrashort pulse emission. We obtain an analytical condition for the occurrence of relaxation oscillations. Continuous and pulsed condensate excitations are considered and we demonstrate that, in the latter case, the existence of the second reservoir is necessary for the emergence of oscillations. We show that relaxation oscillations should be expected to occur in systems with relatively short polariton lifetimes.
关键词： phase space,nonresonantly pumped,relaxation oscillations,fixed points analysis,exciton-polariton condensates,Gross-Pitaevskii model
更新于2025-09-09 09:28:46
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Mg-pair isoelectronic bound exciton identified by its isotopic fingerprint in
摘要： We use the greatly improved optical linewidths provided by highly enriched 28Si to study a photoluminescence line near 1017 meV previously observed in the luminescence spectrum of natural Si diffused with Mg and suggested to result from the recombination of an isoelectronic bound exciton localized at a Mg-pair center. In 28Si, this no-phonon line is found to consist of ?ve components whose relative intensities closely match the relative abundances of Mg pairs formed by random combinations of the three stable isotopes of Mg, thus con?rming the Mg-pair hypothesis. We further present the results of temperature-dependence studies of this center that reveal unusual and as-yet unexplained behavior.
关键词： isotopic fingerprint,28Si,isoelectronic bound exciton,Mg-pair,photoluminescence
更新于2025-09-09 09:28:46
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Excitonic complexes in anisotropic atomically thin two-dimensional materials: Black phosphorus and
摘要： The effect of anisotropy in the energy spectrum on the binding energy and structural properties of excitons, trions, and biexcitons is investigated. To this end we employ the stochastic variational method with a correlated Gaussian basis. We present results for the binding energy of different excitonic complexes in black phosphorus (bP) and TiS3 and compare them with recent results in the literature when available, for which we find good agreement. The binding energies of excitonic complexes in bP are larger than those in TiS3. We calculate the different average interparticle distances in bP and TiS3 and show that excitonic complexes in bP are strongly anisotropic whereas in TiS3 they are almost isotropic, even though the constituent particles have an anisotropic energy spectrum. This is also confirmed by the correlation functions.
关键词： biexciton,TiS3,binding energy,black phosphorus,trion,anisotropy,stochastic variational method,exciton
更新于2025-09-09 09:28:46
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Prospects and applications of plasmon-exciton interactions in the near-field regime
摘要： Plasmonics is a rapidly developing field at the boundary of fundamental sciences and device engineering, which exploits the ability of metal nanostructures to concentrate electromagnetic radiation. The principal challenge lies in achieving an efficient conversion of the plasmon-concentrated field into some form of useful energy. To date, a substantial progress has been made within the scientific community in identifying the major pathways of the plasmon energy conversion. Strategies based on the hot electron injection and the near-field energy transfer have already shown promise in a number of proof-of-principle plasmonic architectures. Nevertheless, there are several fundamental questions that need to be addressed in the future to facilitate the transition of plasmonics to a variety of applications in both light amplification and optical detection. Of particular interest is a plasmon-induced resonance energy transfer (PIRET) process that couples the plasmon evanescent field to a semiconductor absorber via dipole-dipole interaction. This relatively unexplored mechanism has emerged as a promising light conversion strategy in the areas of photovoltaics and photocatalysis and represents the main focus of the present minireview. Along these lines, we highlight the key advances in this area and review some of the challenges associated with applications of the PIRET mechanism in nanostructured systems.
关键词： plasmon-exciton,PIRET,plasmonics,plasmon
更新于2025-09-09 09:28:46
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Tailoring the confined states for exciton-polaritons in a one-dimensional ZnO microrod
摘要： The application of confinement potential is an efficient way to improve the optical properties of exciton polaritons. In this work, we report experimental studies on the effects of potential landscapes on confined polariton states. The spatial confinement of polaritons was realized by imposing two optically-controlled barriers on a one-dimensional ZnO microrod. Two types of quantized polariton states were observed, where energies of the levels depend either linearly or quadratically on their quantum number. The formation of optical traps with parabolic or square-well profiles was confirmed to be responsible for the observed different states. These results demonstrate the importance of the potential landscapes in tailoring the optical properties of exciton polaritons, which would be helpful in the design of polariton-based optoelectronic devices.
关键词： optoelectronic devices,exciton-polaritons,optical traps,ZnO microrod,confinement potential
更新于2025-09-09 09:28:46
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ECCD characterization of monotopically binding guests in host-guest complexes with a bis-(zinc porphyrin) tweezer
摘要： We have investigated the possibility to use a stiff-stilbene linked bisporphyrin tweezer with inherent helicity for Exciton-Coupled Circular Dichroism (ECCD) characterization of a series of monotopically binding amine guest molecules. CD signals were observed for a variety of monoamines at relatively low tweezer:amine (host:guest) ratios between 1:10 to 1:70. For the amines producing the most intense CD signals a binding stoichiometry of 1:2 was found. A likely explanation is the presence of guest-guest interactions in the complexes. This is supported by observing a correlation between CD signal intensity and magnitude of possible non-covalent binding between the guests, which we can divide into three groups showing no, moderate or strong response, respectively. Further support for this rationalization comes from molecular modelling.
关键词： absolute stereochemistry,molecular modelling,bis-porphyrin tweezers,monotopic binding,exciton-coupled circular dichroism
更新于2025-09-09 09:28:46
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Fluorescent Metal-Semiconductor Hybrid Structures by Ultrasound-Assisted In-Situ Growth of Gold Nanoparticles on Silica-Coated CdSe-Dot/CdS-Rod Nanocrystals
摘要： Gold nanocrystals (AuNCs) were grown on the surface of silica coated CdSe-dot/CdS-rod core/shell nanocrystals by reduction of Au3+ ions in polyethylene glycol under ultrasonic irradiation. The polyethylene glycol not only prevents the penetration of gold ions or precursor molecules into the silica shell, but it also acts as the reducing agent for Au3+ ions. The silica shell’s surface promotes the heterogeneous nucleation of gold nanocrystals, while the ultrasonic irradiation accelerates and enhances the gold nucleation on the silica surface, and ensures the formation of AuNCs with a relatively narrow size distribution. The plasmon-exciton interaction in these metal-semiconductor hybrid systems leads to decreased fluorescence lifetimes and strongly reduced fluorescence blinking of individual hybrid structures.
关键词： ultrasonic irradiation,Gold nanocrystals,CdSe-dot/CdS-rod nanocrystals,plasmon-exciton interaction,polyethylene glycol
更新于2025-09-09 09:28:46
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Probing Exciton Delocalization in Organic Semiconductors: Insight from Time-Resolved Electron Paramagnetic Resonance and Magnetophotoselection Experiments
摘要： Delocalization of excited states of organic semiconductors is directly related to their e?ciency in devices. Time-resolved electron paramagnetic resonance spectroscopy provides unique capabilities in this respect because of its high spectral resolution and capability to probe the geometry and extent of excitons. Using magnetophotoselection experiments, the mode of exciton delocalization, along the backbone or parallel to the π?π stacking direction of the conjugated polymers, can be revealed. We demonstrate the robustness of this approach by applying it to building blocks of a prototypical conjugated polymer showing a symmetry of their excited states being far from ideal for this experiment. This renders magnetophotoselection superior to other approaches because it is applicable to a wealth of other organic semiconductors. The insight gained into exciton delocalization is crucial to the structure?function relationship of organic semiconductors and directly relevant for developing highly e?cient materials.
关键词： time-resolved electron paramagnetic resonance,conjugated polymers,exciton delocalization,organic semiconductors,magnetophotoselection
更新于2025-09-09 09:28:46
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Torsionally induced exciton localization and decoherence in <i>π</i> -conjugated polymers
摘要： We develop a model of excitons coupled to the rotational motion of monomers to study the torsionally induced relaxation and decoherence of excitons in π-conjugated polymers. The model assumes that the monomer units are described by elastically uncoupled harmonic oscillators and that there is a linear exciton-roton coupling. Although the rotational degrees of freedom are much slower than the exciton, so that the adiabatic approximation is generally expected to be valid, we also investigate possible quantized roton corrections via coupled time evolving block decimation-Ehrenfest equations of motion. For the relaxation of the lowest-excited exciton, we find that (1) for a polymer chain with a ground state spiral torsional conformation, the equilibrium angular displacement of each monomer is proportional to the difference of the exciton bond-orders on the neighboring bridging bonds. Consequently, this displacement vanishes in the long chain limit and a classical (Landau) exciton-polaron is not formed. (2) For a polymer chain with a ground state staggered torsional conformation, the equilibrium angular displacement of each monomer is proportional to the sum of the exciton bond-orders on the neighboring bridging bonds. Consequently, there is significant angular displacement and local planarization causing exciton density localization. A classical (Landau) exciton-polaron is formed where the staggered angular displacement is proportional to the exciton density. (3) Generally, in the adiabatic limit, the decay of off-diagonal long-range order (i.e., exciton decoherence) mirrors the localization of the exciton density. However, quantum corrections to the rotational motion alter this adiabatic prediction because of correlated exciton-roton dynamics within the first rotational half-period. In particular, exciton-polaron quasiparticle formation causes more rapid and oscillatory exciton decoherence and slower exciton density localization.
关键词： π-conjugated polymers,exciton,decoherence,torsional relaxation,Landau exciton-polaron
更新于2025-09-04 15:30:14
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Simulating Fluorescence Detected Two-Dimensional Electronic Spectroscopy of Multi-Chromophoric Systems
摘要： We present a theory for modeling fluorescence detected two-dimensional electronic spectroscopy of multichromophoric systems. The theory is tested by comparison of the predicted spectra of the light-harvesting complex LH2 with experimental data. A qualitative explanation of the strong cross-peaks as compared to conventional two-dimensional electronic spectra is given. The strong cross-peaks are attributed to the clean ground state signal that is revealed when the annihilation of exciton pairs created on the same LH2 complex cancels oppositely-signed signals from the doubly-excited state. This annihilation process occurs much faster than the non-radiative relaxation. Furthermore, the lineshape difference is attributed to slow dynamics, exciton delocalization within the bands and intraband exciton-exciton annihilation. This is in line with existing theories presented for model systems. We further propose the use of time-resolved fluorescence detected two-dimensional spectroscopy to study state resolved exciton-exciton annihilation.
关键词： fluorescence detected two-dimensional electronic spectroscopy,multichromophoric systems,light-harvesting complex LH2,exciton-exciton annihilation,time-resolved fluorescence detected two-dimensional spectroscopy
更新于2025-09-04 15:30:14