Academic literature on the topic 'Trion Charged biexciton'

The emission lines of strongly confined (211)B InAs/GaAs quantum dots (QDs), embedded in short-period GaAs/AlAs superlattices, are thoroughly characterized by a range of single-dot spectroscopy techniques, including cross correlation photon-counting measurements. Contrary to what is expected for a piezoelectric QD system, the single-dot biexciton line is found redshifted with respect to the exciton one by as many as 6 meV. This comes in striking contrast to previous reports on the same QD system, without additional confinement, where the biexciton lines always showed up at higher energies than the exciton, by 4–13 meV. In addition, two charged exciton lines are identified for the first time in a piezoelectric InAs-based QD. A positively charged (Χ+) and a negatively charged (Χ−) trion line are observed 1.5 and 7.5 meV below the neutral exciton line, respectively. Our results pave the way to an enhanced understanding of the excitonic transitions in (211)B QDs and highlight the possible role of strong confinement and accompanying correlation effects as a means to tailor the transition energies of multi-particle states in semiconductor QDs.

Monolayers of transition metal dichalcogenides (TMDs) with their unique physical properties are very promising for future applications in novel electronic devices. In TMDs monolayers, strong and opposite spin splittings of the energy gaps at the K points allow for exciting carriers with various combinations of valley and spin indices using circularly polarized light, which can further be used in spintronics and valleytronics. The physical properties of van der Waals heterostructures composed of TMDs monolayers and hexagonal boron nitride (hBN) layers significantly depend on different kinds of interactions. Here, we report on observing both a strong increase in the emission intensity as well as a preservation of the helicity of the excitation light in the emission from hBN/WSe2/hBN heterostructures related to interlayer electron-phonon coupling. In combined low-temperature (T = 7 K) reflectivity contrast and photoluminescence excitation experiments, we find that the increase in the emission intensity is attributed to a double resonance, where the laser excitation and the combined Raman mode A′1 (WSe2) + ZO (hBN) are in resonance with the excited (2s) and ground (1s) states of the A exciton in a WSe2 monolayer. In reference to the 2s state, our interpretation is in contrast with previous reports, in which this state has been attributed to the hybrid exciton state existing only in the hBN-encapsulated WSe2 monolayer. Moreover, we observe that the electron-phonon coupling also enhances the helicity preservation of the exciting light in the emission of all observed excitonic complexes. The highest helicity preservation of more than 60% is obtained in the emission of the neutral biexciton and negatively charged exciton (trion) in its triplet state. Additionally, to the best of our knowledge, the strongly intensified emission of the neutral biexciton XX0 at double resonance condition is observed for the first time.

Colloidal semiconductor quantum dots (QDs) are excellent materials for studying the photophysics of exciton complexes such as biexcitons, triexcitons, and charged excitons (trions). Dynamics of exciton complexes usually determines the performance of optoelectronic devices [1]. For example, trions reduce the optical gain threshold in QD lasers and multiexcitons increase photon-to-current conversion efficiencies via carrier multiplication processes in QD solar cells. In addition, unconventional properties of multiexcitons emerge in coherent processes in QD systems. We recently discovered the high-frequency coherent oscillations with integer multiples of the exciton resonance frequency, which is called multiexciton harmonic quantum coherence [2,3]. The multiexciton coherent properties have been investigated using optical methods. However, to clarify their roles in optoelectronic devices, it is necessary to conduct the electrical detection of multiexciton coherence. Here, we performed photocurrent detection of exciton quantum interference signals in QD thin films. The samples used in this study were closely packed PbS QD thin films. The QD films were sandwiched between the electron and hole transport layers to extract photogenerated carriers. Multiexcitons were generated by phase-locked femtosecond laser pulses, and then their photocurrent quantum interference signals were measured by using a quantum interference technique [4]. The photocurrent interference signal in the weak excitation shows a single sinusoidal oscillation originating from single excitons, while the interference signal changes to the profile involving multiple sinusoidal oscillations with increasing excitation intensity. This means that the multiexciton quantum coherence exhibiting harmonic oscillations is successfully detected in a photocurrent technique [5]. Furthermore, the amplitudes of harmonic quantum coherent signals in coupled QDs are significantly larger than those in isolated QDs. We clarified that the enhancement of the amplitudes is caused by cooperative processes in coupled QDs, where excitons in adjacent QDs interact with each other through their inter-QD coherent coupling. This cooperative effect can provide a new way to use inter-QD coherent coupling in advanced optoelectronic applications, e.g., amplifiers of coherent signals. Part of this work was supported by JSPS KAKENHI (JP19H05465 and JP22H01990) and JST CREST (JPMJCR21B4). References [1] Kanemitsu, Y. Trion dynamics in lead halide perovskite nanocrystals. J. Chem. Phys. 151, 170902 (2019). [2] Tahara, H.; Sakamoto, M.; Teranishi, T.; Kanemitsu, Y. Harmonic Quantum Coherence of Multiple Excitons in PbS/CdS Core-Shell Nanocrystals. Phys. Rev. Lett. 119, 247401 (2017). [3] Tahara, H.; Sakamoto, M.; Teranishi, T.; Kanemitsu, Y. Quantum coherence of multiple excitons governs absorption cross-sections of PbS/CdS core/shell nanocrystals. Nat. Commun. 9, 3179 (2018). [4] Tahara, H.; Kanemitsu, Y. Quantum Interference Measurements and Their Application to Analysis of Ultrafast Photocarrier Dynamics in Semiconductor Solar Cell Materials. Adv. Quantum Technol. 3, 1900098 (2020). [5] Tahara, H.; Sakamoto, M.; Teranishi, T.; Kanemitsu, Y. Collective enhancement of quantum coherence in coupled quantum dot films. Phys. Rev. B 104, L241405 (2021).

AbstractControlling the interaction between light and matter at micro- and nano-scale can provide new opportunities for modern optics and optoelectronics. An archetypical example is polariton, a half-light-half-matter quasi particle inheriting simultaneously the robust coherence of light and the strong interaction of matter, which plays an important role in many exotic phenomena. Here, we open up a new kind of cooperative coupling between plasmon and different excitonic complexes in WS2-silver nanocavities, namely plasmon-exciton-trion-charged biexciton four coupling states. Thanks to the large Bohr radius of up to 5 nm, the charged biexciton polariton exhibits strong saturation nonlinearity, ~30 times higher than the neutral exciton polariton. Transient absorption dynamics further reveal the ultrafast many-body interaction nature, with a timescale of <100 fs. The demonstration of biexciton polariton here combines high nonlinearity, simple processing and strong scalability, permitting access for future energy-efficient optical switching and information processing.

AbstractTransition metal dichalcogenides monolayers host strongly bounded Coulomb complexes such as exciton and trion due to charge confinement and screening reduction in two dimensions. Biexciton, a bound state of two electrons and two holes, has also been observed in these materials with a binding energy which is one order of magnitude larger than its counterpart in conventional semiconductors. Here, using first principles methods, we address the biexciton in WSe2 monolayer and unravel the important role of the electron-hole exchange interaction in dictating the valley character of biexciton states and their fine structure. In particular, the fundamental biexciton transition which is located between the exciton and trion peaks is shown to have a fine structure of 2.8 meV mainly due to the splitting of the dark exciton state under the intervalley electron-hole exchange interaction. Non equilibrium effects are also addressed and optical fingerprints of non-thermalized biexciton population are discussed.

AbstractLead halide perovskites open great prospects for optoelectronics and a wealth of potential applications in quantum optical and spin-based technologies. Precise knowledge of the fundamental optical and spin properties of charge-carrier complexes at the origin of their luminescence is crucial in view of the development of these applications. On nearly bulk Cesium-Lead-Bromide single perovskite nanocrystals, which are the test bench materials for next-generation devices as well as theoretical modeling, we perform low temperature magneto-optical spectroscopy to reveal their entire band-edge exciton fine structure and charge-complex binding energies. We demonstrate that the ground exciton state is dark and lays several millielectronvolts below the lowest bright exciton sublevels, which settles the debate on the bright-dark exciton level ordering in these materials. More importantly, combining these results with spectroscopic measurements on various perovskite nanocrystal compounds, we show evidence for universal scaling laws relating the exciton fine structure splitting, the trion and biexciton binding energies to the band-edge exciton energy in lead-halide perovskite nanostructures, regardless of their chemical composition. These scaling laws solely based on quantum confinement effects and dimensionless energies offer a general predictive picture for the interaction energies within charge-carrier complexes photo-generated in these emerging semiconductor nanostructures.

Ce travail analyse la formation d'états liés par interaction coulombienne d'excitons dans un ensemble de nanotubes de carbone de chiralité (6,5) en solution. Sous l'action d'une impulsion laser de forte intensité, une grande densité d'excitons est formée dans le nanotube et conduit à la formation d'état de trion et de biexciton. Les mécanismes physiques responsables de la photogénération de ces états ont été analysés dans le cadre de cette thèse. Ces travaux sont effectués à l'aide d'une expérience pompe-sonde dans laquelle le faisceau sonde est un continuum de lumière blanche permettant ainsi l'observation simultanée des états d'exciton, de trion et de biexciton. Cela conduit à l'obtention des énergies de liaison des différentes contributions excitoniques. En outre la dynamique de ces états excitoniques a aussi pu être obtenue avec une résolution temporelle de l'ordre de la centaine de femtosecondes.