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Author: Grafiati
Published: 24 June 2023

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1

Golovatenko, Aleksandr A., Ina V. Kalitukha, Grigorii S. Dimitriev, Victor F. Sapega, Maxim V. Rakhlin, Aidar I. Galimov, Tatiana V. Shubina, et al. "A Comparative Study of the Band-Edge Exciton Fine Structure in Zinc Blende and Wurtzite CdSe Nanocrystals." Nanomaterials 12, no. 23 (December 1, 2022): 4269. http://dx.doi.org/10.3390/nano12234269.

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In this paper, we studied the role of the crystal structure in spheroidal CdSe nanocrystals on the band-edge exciton fine structure. Ensembles of zinc blende and wurtzite CdSe nanocrystals are investigated experimentally by two optical techniques: fluorescence line narrowing (FLN) and time-resolved photoluminescence. We argue that the zero-phonon line evaluated by the FLN technique gives the ensemble-averaged energy splitting between the lowest bright and dark exciton states, while the activation energy from the temperature-dependent photoluminescence decay is smaller and corresponds to the energy of an acoustic phonon. The energy splittings between the bright and dark exciton states determined using the FLN technique are found to be the same for zinc blende and wurtzite CdSe nanocrystals. Within the effective mass approximation, we develop a theoretical model considering the following factors: (i) influence of the nanocrystal shape on the bright–dark exciton splitting and the oscillator strength of the bright exciton, and (ii) shape dispersion in the ensemble of the nanocrystals. We show that these two factors result in similar calculated zero-phonon lines in zinc blende and wurtzite CdSe nanocrystals. The account of the nanocrystals shape dispersion allows us to evaluate the linewidth of the zero-phonon line.
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2

Hou, Lei, Philippe Tamarat, and Brahim Lounis. "Revealing the Exciton Fine Structure in Lead Halide Perovskite Nanocrystals." Nanomaterials 11, no. 4 (April 20, 2021): 1058. http://dx.doi.org/10.3390/nano11041058.

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Lead-halide perovskite nanocrystals (NCs) are attractive nano-building blocks for photovoltaics and optoelectronic devices as well as quantum light sources. Such developments require a better knowledge of the fundamental electronic and optical properties of the band-edge exciton, whose fine structure has long been debated. In this review, we give an overview of recent magneto-optical spectroscopic studies revealing the entire excitonic fine structure and relaxation mechanisms in these materials, using a single-NC approach to get rid of their inhomogeneities in morphology and crystal structure. We highlight the prominent role of the electron-hole exchange interaction in the order and splitting of the bright triplet and dark singlet exciton sublevels and discuss the effects of size, shape anisotropy and dielectric screening on the fine structure. The spectral and temporal manifestations of thermal mixing between bright and dark excitons allows extracting the specific nature and strength of the exciton–phonon coupling, which provides an explanation for their remarkably bright photoluminescence at low temperature although the ground exciton state is optically inactive. We also decipher the spectroscopic characteristics of other charge complexes whose recombination contributes to photoluminescence. With the rich knowledge gained from these experiments, we provide some perspectives on perovskite NCs as quantum light sources.
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3

Baranowski, Michał, Mateusz Dyksik, and Paulina Płochocka. "2D Metal Halide Perovskites: A New Fascinating Playground for Exciton Fine Structure Investigations." Scientiae Radices 01, no. 01 (November 18, 2022): 3–25. http://dx.doi.org/10.58332/v22i1a01.

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Two-dimensional (2D) metal halide perovskites are natural quantum wells which consist of low bandgap metal-halide slabs, surrounded by organic spacers barriers. The quantum and dielectric confinements provided by the organic part lead to the extreme exciton binding energy which results in a huge enhancement of exciton fine structure in this material system. This makes 2D perovskites a fascinating playground for fundamental excitonic physics studies. In this review, we summarize the current understanding and quantification of the exciton fine structure in 2D perovskites. We discuss what is the role of exciton fine structure in the optical response of 2D perovskites and how it challenges our understanding of this fundamental excitation. Finally, we highlight some controversy related to particularly large bright-dark exciton states splitting and high efficiency of light emission from these materials. This can result from the unique synergy of excitonic and mechanical properties of 2D perovskites crystals.
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4

SHAVER, J., A. SRIVASTAVA, J. KONO, S. A. CROOKER, H. HTOON, V. I. KLIMOV, J. A. FAGAN, et al. "HIGH FIELD MAGNETO-OPTICAL SPECTROSCOPY OF HIGHLY ALIGNED INDIVIDUAL AND ENSEMBLE SINGLE-WALLED CARBON NANOTUBES." International Journal of Modern Physics B 23, no. 12n13 (May 20, 2009): 2667–75. http://dx.doi.org/10.1142/s0217979209062153.

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The tubular nature of single-walled carbon nanotube (SWCNT) crystals allows them to exhibit non-intuitive quantum phenomena when threaded by a magnetic flux, which breaks the time reversal symmetry and adds an Aharonov-Bohm phase to the circumferential boundary conditions on the electronic wave function. We demonstrate that such a symmetry-breaking magnetic field can dramatically "brighten" an optically-inactive, or dark, exciton state at low temperature. This phenomenon, magnetic brightening, can be understood as a consequence of interplay between the strong intervalley Coulomb mixing and field-induced lifting of valley degeneracy. Most recently, we made the direct observation of the dark excitonic state in individual SWCNTs using low-temperature micro-photoluminescence (PL) and and verified the importance of a parallel, tube-threading magentic field with ensemble spectroscopy. For micro-PL, a magnetic field up to 5 T, applied along the nanotube axis, brightened the dark state, leading to the emergence of a new emission peak. The peak rapidly grew in intensity with increasing field at the expense of the originally-dominant bright exciton peak and finally became dominant at fields > 3 T. The directly measured dark-bright splitting values were 1-4 meV for tube diameters 1.0-1.3 nm. For ensemble PL, we used fields up to 55 T in two collection geometries to demonstrate the importance of the tube-threading component. These experiments have provided one of the most critical tests for recently-proposed theories of 1-D excitons taking into account the strong 1-D Coulomb interactions and unique band structure on an equal footing.
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5

Ghribi, Amal, Rim Ben Aich, Kaïs Boujdaria, Thierry Barisien, Laurent Legrand, Maria Chamarro, and Christophe Testelin. "Dielectric Confinement and Exciton Fine Structure in Lead Halide Perovskite Nanoplatelets." Nanomaterials 11, no. 11 (November 13, 2021): 3054. http://dx.doi.org/10.3390/nano11113054.

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Owing to their flexible chemical synthesis and the ability to shape nanostructures, lead halide perovskites have emerged as high potential materials for optoelectronic devices. Here, we investigate the excitonic band edge states and their energies levels in colloidal inorganic lead halide nanoplatelets, particularly the influence of dielectric effects, in a thin quasi-2D system. We use a model including band offset and dielectric confinements in the presence of Coulomb interaction. Short- and long-range contributions, modified by dielectric effects, are also derived, leading to a full modelization of the exciton fine structure, in cubic, tetragonal and orthorhombic phases. The fine splitting structure, including dark and bright excitonic states, is discussed and compared to recent experimental results, showing the importance of both confinement and dielectric contributions.
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6

Heyn, Christian, Andreas Gräfenstein, Geoffrey Pirard, Leonardo Ranasinghe, Kristian Deneke, Ahmed Alshaikh, Gabriel Bester, and Wolfgang Hansen. "Dot-Size Dependent Excitons in Droplet-Etched Cone-Shell GaAs Quantum Dots." Nanomaterials 12, no. 17 (August 28, 2022): 2981. http://dx.doi.org/10.3390/nano12172981.

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Strain-free GaAs quantum dots (QDs) are fabricated by filling droplet-etched nanoholes in AlGaAs. Using a template of nominally identical nanoholes, the QD size is precisely controlled by the thickness of the GaAs filling layer. Atomic force microscopy indicates that the QDs have a cone-shell shape. From single-dot photoluminescence measurements, values of the exciton emission energy (1.58...1.82 eV), the exciton–biexciton splitting (1.8...2.5 meV), the exciton radiative lifetime of bright (0.37...0.58 ns) and dark (3.2...6.7 ns) states, the quantum efficiency (0.89...0.92), and the oscillator strength (11.2...17.1) are determined as a function of the dot size. The experimental data are interpreted by comparison with an atomistic model.
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7

Oshima, Tsuyoshi, Kazunori Matsuno, and Hidekatsu Suzuura. "Energy splitting between bright and dark excitons in carbon nanotubes." Physica E: Low-dimensional Systems and Nanostructures 42, no. 4 (February 2010): 779–82. http://dx.doi.org/10.1016/j.physe.2009.11.131.

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8

Li, Wei-Hua, Jhen-Dong Lin, Ping-Yuan Lo, Guan-Hao Peng, Ching-Yu Hei, Shao-Yu Chen, and Shun-Jen Cheng. "The Key Role of Non-Local Screening in the Environment-Insensitive Exciton Fine Structures of Transition-Metal Dichalcogenide Monolayers." Nanomaterials 13, no. 11 (May 26, 2023): 1739. http://dx.doi.org/10.3390/nano13111739.

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In this work, we present a comprehensive theoretical and computational investigation of exciton fine structures of WSe2-monolayers, one of the best-known two-dimensional (2D) transition-metal dichalcogenides (TMDs), in various dielectric-layered environments by solving the first-principles-based Bethe–Salpeter equation. While the physical and electronic properties of atomically thin nanomaterials are normally sensitive to the variation of the surrounding environment, our studies reveal that the influence of the dielectric environment on the exciton fine structures of TMD-MLs is surprisingly limited. We point out that the non-locality of Coulomb screening plays a key role in suppressing the dielectric environment factor and drastically shrinking the fine structure splittings between bright exciton (BX) states and various dark-exciton (DX) states of TMD-MLs. The intriguing non-locality of screening in 2D materials can be manifested by the measurable non-linear correlation between the BX-DX splittings and exciton-binding energies by varying the surrounding dielectric environments. The revealed environment-insensitive exciton fine structures of TMD-ML suggest the robustness of prospective dark-exciton-based optoelectronics against the inevitable variation of the inhomogeneous dielectric environment.
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9

Cheng, Haowei, Kun Liang, Xuyan Deng, Lei Jin, Jingcheng Shangguan, Jiasen Zhang, Jiaqi Guo, and Li Yu. "Optical Chirality of Gold Chiral Helicoid Nanoparticles in the Strong Coupling Region." Photonics 10, no. 3 (February 27, 2023): 251. http://dx.doi.org/10.3390/photonics10030251.

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The far- and near-field chirality properties are usually characterized by circular dichroism (CD) and optical chirality (OC), respectively. As a light–matter interaction for the hybrid states consisting of plasmons and excitons, the strong coupling interactions can affect the original chiral electromagnetic modes. However, there are few works on this influence process, which prevents an in-depth understanding of chirality. Here, we theoretically investigate both the far-field and near-field characteristics of the chiral plasmonic gold helicoid nanoparticle (GHNP) to explore the chirality mechanism further. We found that the electromagnetic field distribution of GHNP consists of one dark mode and two bright modes. The dark mode is observed more clearly in CD than in extinction spectra. Two bright modes can strongly couple with excitons respectively, which is confirmed by the anticrossing behavior and mode splitting exhibited in the extinction and CD spectra. We also analyzed the near-field OC distribution of the GHNP hybrid system and obtained the chiral responses as well as the spectral correspondence between OC and CD. Furthermore, although the strong coupling interaction changes the energy levels, resulting in mode splitting, the chiral hotspot distributions of both the upper polariton branch and lower polariton branch are consistent with the original bright mode in OC maps. Our findings provide guidance for the design of structures with strong chiral responses and enhance the comprehension of chiral strong coupling systems.
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10

Sukkabot, Worasak. "Atomistic Tight-Binding Theory of Electron-Hole Exchange Interaction in Morphological Evolution of CdSe/ZnS Core/Shell Nanodisk to CdSe/ZnS Core/Shell Nanorod." Journal of Nanomaterials 2016 (2016): 1–6. http://dx.doi.org/10.1155/2016/1572641.

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Based on the atomistic tight-binding theory (TB) and a configuration interaction (CI) description, the electron-hole exchange interaction in the morphological transformation of CdSe/ZnS core/shell nanodisk to CdSe/ZnS core/shell nanorod is described with the aim of understanding the impact of the structural shapes on the change of the electron-hole exchange interaction. Normally, the ground hole states confined in typical CdSe/ZnS core/shell nanocrystals are of heavy hole-like character. However, the atomistic tight-binding theory shows that a transition of the ground hole states from heavy hole-like to light hole-like contribution with the increasing aspect ratios of the CdSe/ZnS core/shell nanostructures is recognized. According to the change in the ground-state hole characters, the electron-hole exchange interaction is also significantly altered. To do so, optical band gaps, ground-state electron character, ground-state hole character, oscillation strengths, ground-state coulomb energies, ground-state exchange energies, and dark-bright (DB) excitonic splitting (stoke shift) are numerically demonstrated. These atomistic computations obviously show the sensitivity with the aspect ratios. Finally, the alteration in the hole character has a prominent effect on dark-bright (DB) excitonic splitting.
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11

Nicholas, R. J., I. B. Mortimer, L. J. Li, A. Nish, O. Portugall, and G. L. J. A. Rikken. "Temperature and Magnetic Field Dependent Photoluminescence from Carbon Nanotubes." International Journal of Modern Physics B 21, no. 08n09 (April 10, 2007): 1180–88. http://dx.doi.org/10.1142/s0217979207042616.

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Photoluminescence as a function of temperature and magnetic field from single walled carbon nanotube solutions is described. This is modelled assuming that it is dominated by the small energy splitting between the dark and bright states of the singlet excitons which are found to be in the region of 1-5 meV for nanotubes of 0.8-1.2nm. The emission energies show a large red-shift due to the introduction of an Aharanov-Bohm phase by magnetic field along the tube axis and the luminescence intensity is strongly enhanced at low temperatures due to the mixing of the different valley states of the excitons.
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12

Lu, Zhengguang, Daniel Rhodes, Zhipeng Li, Dinh Van Tuan, Yuxuan Jiang, Jonathan Ludwig, Zhigang Jiang, et al. "Magnetic field mixing and splitting of bright and dark excitons in monolayer MoSe 2." 2D Materials 7, no. 1 (November 21, 2019): 015017. http://dx.doi.org/10.1088/2053-1583/ab5614.

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13

Ding, Huaiyi, Mei Liu, Nan Pan, Yiyun Dong, Yue Lin, Taishen Li, Jiangtao Zhao, Zhenlin Luo, Yi Luo, and Xiaoping Wang. "Lattice Disorder-Engineered Energy Splitting between Bright and Dark Excitons in CsPbBr3 Quantum Wires." Journal of Physical Chemistry Letters 10, no. 6 (March 7, 2019): 1355–60. http://dx.doi.org/10.1021/acs.jpclett.9b00551.

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14

Chen, Lan, Bin Li, Chunfeng Zhang, Xinyu Huang, Xiaoyong Wang, and Min Xiao. "Composition-Dependent Energy Splitting between Bright and Dark Excitons in Lead Halide Perovskite Nanocrystals." Nano Letters 18, no. 3 (February 21, 2018): 2074–80. http://dx.doi.org/10.1021/acs.nanolett.8b00184.

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15

Biadala, Louis, Benjamin Siebers, Raquel Gomes, Zeger Hens, Dmitri R. Yakovlev, and Manfred Bayer. "Tuning Energy Splitting and Recombination Dynamics of Dark and Bright Excitons in CdSe/CdS Dot-in-Rod Colloidal Nanostructures." Journal of Physical Chemistry C 118, no. 38 (September 12, 2014): 22309–16. http://dx.doi.org/10.1021/jp505887u.

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16

Hwang, Hyeong-Yong, Sehyuk Lee, Yong-Hoon Kim, Farman Ullah, Chinh Tam Le, Yong Soo Kim, Ki-Ju Yee, Christopher J. Stanton, and Young-Dahl Jho. "Shear-strain-mediated photoluminescence manipulation in two-dimensional transition metal dichalcogenides." 2D Materials 9, no. 1 (November 15, 2021): 015011. http://dx.doi.org/10.1088/2053-1583/ac351d.

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Abstract In two-dimensional transition metal dichalcogenides, normal strain can modulate electronic band structures, yet leaving the optical selection rules intact. In contrast, a shear strain can perturb the spin-valley locked band structures and possibly induce mixing of the spin subbands which in turn can transfer oscillator strength between spin-allowed bright and spin-forbidden dark excitons. Here, we report a novel scheme to manipulate photoluminescence (PL) in a monolayer WSe2-MoSe2 lateral heterostructures, controlled by an external bending method in which strong out-of-plane shear strain (OSS) of up to 5.6% accompanies weak in-plane normal strain up to 0.72%. The spectra revealed a striking dependence on the bending direction that is stagnant in the negative (compressive) strain region and then rapidly changes with increasing positive (tensile) strain. The dependency of the PL signal under tensile bending was represented not only by the large energy shift ( > 40 meV) of the lowest excited states of both the WSe2 and MoSe2 monolayers, but also by the tendency to violate the optical selection rules that brightens (darkens) the excitons of the WSe2 (MoSe2) side. The analyses on the observed energy shifts and PL intensity changes confirm the different origins in compressive bending compared with tensile bending. The well-established band-anticrossing is identified to be affecting only the compressive deformation region. The spectral changes in the tensile region, on the other hand, originates mainly from the generation of an off-diagonal perturbation to a spin-specific Hamiltonian induced by OSS. The degree of spin-state mixing, which correlates precisely with the spin-flip coefficient of the theoretical model, is further represented by the OSS matrix elements, the spin splitting energy, and the shear deformation potential.
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17

Combescot, Monique, Francois Dubin, and Shiue Yuan Shiau. "Signature of electromagnetic quantum fluctuations in exciton physics." Europhysics Letters, February 21, 2022. http://dx.doi.org/10.1209/0295-5075/ac5700.

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Abstract Quantum fluctuations of the electromagnetic field are known to produce the atomic Lamb shift. We here reveal their iconic signature in semiconductor physics, through the blue-shift they produce to optically bright excitons, thus lifting the energy of these excitons above their dark counterparts. The electromagnetic field here acts in its full complexity: in addition to the longitudinal part via interband virtual Coulomb processes, the transverse part---which has been missed up to now---also acts via resonant and nonresonant virtual photons. These two parts beautifully combine to produce a bright exciton blue-shift independent of the exciton wave-vector direction. Our work readily leads to a striking prediction: long-lived excitons must have a small bright-dark splitting. Although the analogy between exciton and hydrogen atom could lead us to see the bright exciton shift as a Lamb shift, this is not fully so: the atom shift entirely comes from virtual photons, whereas the Coulomb interaction also contributes to the exciton shift through the so-called ``electron-hole exchange''.
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18

Kapuściński, Piotr, Alex Delhomme, Diana Vaclavkova, Artur O. Slobodeniuk, Magdalena Grzeszczyk, Miroslav Bartos, Kenji Watanabe, Takashi Taniguchi, Clément Faugeras, and Marek Potemski. "Rydberg series of dark excitons and the conduction band spin-orbit splitting in monolayer WSe2." Communications Physics 4, no. 1 (August 19, 2021). http://dx.doi.org/10.1038/s42005-021-00692-3.

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AbstractStrong Coulomb correlations together with multi-valley electronic bands in the presence of spin-orbit interaction are at the heart of studies of the rich physics of excitons in monolayers of transition metal dichalcogenides (TMD). Those archetypes of two-dimensional systems promise a design of new optoelectronic devices. In intrinsic TMD monolayers the basic, intravalley excitons, are formed by a hole from the top of the valence band and an electron either from the lower or upper spin-orbit-split conduction band subbands: one of these excitons is optically active, the second one is dark, although possibly observed under special conditions. Here we demonstrate the s-series of Rydberg dark exciton states in tungsten diselenide monolayer, which appears in addition to a conventional bright exciton series in photoluminescence spectra measured in high in-plane magnetic fields. The comparison of energy ladders of bright and dark Rydberg excitons is shown to be a method to experimentally evaluate one of the missing band parameters in TMD monolayers: the amplitude of the spin-orbit splitting of the conduction band.
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19

Luo, J. W., A. Franceschetti, and A. Zunger. "Nonmonotonic size dependence of the dark/bright exciton splitting in GaAs nanocrystals." Physical Review B 79, no. 20 (May 8, 2009). http://dx.doi.org/10.1103/physrevb.79.201301.

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20

Tamarat, Philippe, Elise Prin, Yullia Berezovska, Anastasiia Moskalenko, Thi Phuc Tan Nguyen, Chenghui Xia, Lei Hou, et al. "Universal scaling laws for charge-carrier interactions with quantum confinement in lead-halide perovskites." Nature Communications 14, no. 1 (January 16, 2023). http://dx.doi.org/10.1038/s41467-023-35842-4.

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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.
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21

Wang, Shuli, Mateusz Dyksik, Carola Lampe, Moritz Gramlich, Duncan K. Maude, Michał Baranowski, Alexander S. Urban, Paulina Plochocka, and Alessandro Surrente. "Thickness-Dependent Dark-Bright Exciton Splitting and Phonon Bottleneck in CsPbBr3-Based Nanoplatelets Revealed via Magneto-Optical Spectroscopy." Nano Letters, August 29, 2022. http://dx.doi.org/10.1021/acs.nanolett.2c01826.

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22

Echeverry, J. P., B. Urbaszek, T. Amand, X. Marie, and I. C. Gerber. "Splitting between bright and dark excitons in transition metal dichalcogenide monolayers." Physical Review B 93, no. 12 (March 16, 2016). http://dx.doi.org/10.1103/physrevb.93.121107.

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