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1.
Nature ; 622(7981): 63-68, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37315640

ABSTRACT

The interplay between spontaneous symmetry breaking and topology can result in exotic quantum states of matter. A celebrated example is the quantum anomalous Hall (QAH) state, which exhibits an integer quantum Hall effect at zero magnetic field owing to intrinsic ferromagnetism1-3. In the presence of strong electron-electron interactions, fractional QAH (FQAH) states at zero magnetic field can emerge4-8. These states could host fractional excitations, including non-Abelian anyons-crucial building blocks for topological quantum computation9. Here we report experimental signatures of FQAH states in a twisted molybdenum ditelluride (MoTe2) bilayer. Magnetic circular dichroism measurements reveal robust ferromagnetic states at fractionally hole-filled moiré minibands. Using trion photoluminescence as a sensor10, we obtain a Landau fan diagram showing linear shifts in carrier densities corresponding to filling factor v = -2/3 and v = -3/5 ferromagnetic states with applied magnetic field. These shifts match the Streda formula dispersion of FQAH states with fractionally quantized Hall conductance of [Formula: see text] and [Formula: see text], respectively. Moreover, the v = -1 state exhibits a dispersion corresponding to Chern number -1, consistent with the predicted QAH state11-14. In comparison, several non-ferromagnetic states on the electron-doping side do not disperse, that is, they are trivial correlated insulators. The observed topological states can be electrically driven into topologically trivial states. Our findings provide evidence of the long-sought FQAH states, demonstrating MoTe2 moiré superlattices as a platform for exploring fractional excitations.

2.
Nature ; 622(7981): 74-79, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37591304

ABSTRACT

The integer quantum anomalous Hall (QAH) effect is a lattice analogue of the quantum Hall effect at zero magnetic field1-3. This phenomenon occurs in systems with topologically non-trivial bands and spontaneous time-reversal symmetry breaking. Discovery of its fractional counterpart in the presence of strong electron correlations, that is, the fractional QAH effect4-7, would open a new chapter in condensed matter physics. Here we report the direct observation of both integer and fractional QAH effects in electrical measurements on twisted bilayer MoTe2. At zero magnetic field, near filling factor ν = -1 (one hole per moiré unit cell), we see an integer QAH plateau in the Hall resistance Rxy quantized to h/e2 ± 0.1%, whereas the longitudinal resistance Rxx vanishes. Remarkably, at ν = -2/3 and -3/5, we see plateau features in Rxy at [Formula: see text] and [Formula: see text], respectively, whereas Rxx remains small. All features shift linearly versus applied magnetic field with slopes matching the corresponding Chern numbers -1, -2/3 and -3/5, precisely as expected for integer and fractional QAH states. Additionally, at zero magnetic field, Rxy is approximately 2h/e2 near half-filling (ν = -1/2) and varies linearly as ν is tuned. This behaviour resembles that of the composite Fermi liquid in the half-filled lowest Landau level of a two-dimensional electron gas at high magnetic field8-14. Direct observation of the fractional QAH and associated effects enables research in charge fractionalization and anyonic statistics at zero magnetic field.

3.
Nature ; 604(7906): 468-473, 2022 04.
Article in English | MEDLINE | ID: mdl-35444320

ABSTRACT

Many-body interactions between carriers lie at the heart of correlated physics. The ability to tune such interactions would allow the possibility to access and control complex electronic phase diagrams. Recently, two-dimensional moiré superlattices have emerged as a promising platform for quantum engineering such phenomena1-3. The power of the moiré system lies in the high tunability of its physical parameters by adjusting the layer twist angle1-3, electrical field4-6, moiré carrier filling7-11 and interlayer coupling12. Here we report that optical excitation can highly tune the spin-spin interactions between moiré-trapped carriers, resulting in ferromagnetic order in WS2 /WSe2 moiré superlattices. Near the filling factor of -1/3 (that is, one hole per three moiré unit cells), as the excitation power at the exciton resonance increases, a well-developed hysteresis loop emerges in the reflective magnetic circular dichroism signal as a function of magnetic field, a hallmark of ferromagnetism. The hysteresis loop persists down to charge neutrality, and its shape evolves as the moiré superlattice is gradually filled, indicating changes of magnetic ground state properties. The observed phenomenon points to a mechanism in which itinerant photoexcited excitons mediate exchange coupling between moiré-trapped holes. This exciton-mediated interaction can be of longer range than direct coupling between moiré-trapped holes9, and thus magnetic order arises even in the dilute hole regime. This discovery adds a dynamic tuning knob to the rich many-body Hamiltonian of moiré quantum matter13-19.

4.
Nature ; 599(7885): 383-392, 2021 11.
Article in English | MEDLINE | ID: mdl-34789905

ABSTRACT

The design and control of material interfaces is a foundational approach to realize technologically useful effects and engineer material properties. This is especially true for two-dimensional (2D) materials, where van der Waals stacking allows disparate materials to be freely stacked together to form highly customizable interfaces. This has underpinned a recent wave of discoveries based on excitons in stacked double layers of transition metal dichalcogenides (TMDs), the archetypal family of 2D semiconductors. In such double-layer structures, the elegant interplay of charge, spin and moiré superlattice structure with many-body effects gives rise to diverse excitonic phenomena and correlated physics. Here we review some of the recent discoveries that highlight the versatility of TMD double layers to explore quantum optics and many-body effects. We identify outstanding challenges in the field and present a roadmap for unlocking the full potential of excitonic physics in TMD double layers and beyond, such as incorporating newly discovered ferroelectric and magnetic materials to engineer symmetries and add a new level of control to these remarkable engineered materials.

5.
Plant Cell ; 2023 Oct 05.
Article in English | MEDLINE | ID: mdl-37795677

ABSTRACT

Plant inflorescence architecture is determined by inflorescence meristem (IM) activity and controlled by genetic mechanisms associated with environmental factors. In Arabidopsis (Arabidopsis thaliana), TERMINAL FLOWER1 (TFL1) is expressed in the IM and is required to maintain indeterminate growth, whereas LEAFY (LFY) is expressed in the floral meristems (FMs) formed at the periphery of the IM and is required to activate determinate floral development. Here, we address how Arabidopsis indeterminate inflorescence growth is determined. We show that the 26S proteasome subunit REGULATORY PARTICLE AAA-ATPASE 2a (RPT2a) is required to maintain the indeterminate inflorescence architecture in Arabidopsis. rpt2a mutants display reduced TFL1 expression levels and ectopic LFY expression in the IM and develop a determinate zigzag-shaped inflorescence. We further found that RPT2a promotes DNA METHYLTRANSFERASE1 degradation, leading to DNA hypomethylation upstream of TFL1 and high TFL1 expression levels in the wild-type IM. Overall, our work reveals that proteolytic input into the epigenetic regulation of TFL1 expression directs inflorescence architecture in Arabidopsis, adding an additional layer to stem cell regulation.

6.
Proc Natl Acad Sci U S A ; 120(32): e2306584120, 2023 Aug 08.
Article in English | MEDLINE | ID: mdl-37527343

ABSTRACT

Placed in cavity resonators with three-dimensionally confined electromagnetic wave, the interaction between quasiparticles in solids can be induced by exchanging virtual cavity photons, which can have a nonlocal characteristic. Here, we investigate the possibility of utilizing this nonlocality to realize the remote control of the topological transition in mesoscopic moiré superlattices at full filling (one electron/hole per supercell) embedded in a split-ring terahertz electromagnetic resonator. We show that gate tuning one moiré superlattice can remotely drive a topological band inversion in another moiré superlattice not in contact but embedded in the same cavity. Our study of remote on/off switching of a topological transition provides a paradigm for the control of material properties via cavity vacuum fields.

7.
Nat Mater ; 23(2): 224-229, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38177379

ABSTRACT

Moiré excitons are emergent optical excitations in two-dimensional semiconductors with moiré superlattice potentials. Although these excitations have been observed on several platforms, a system with dynamically tunable moiré potential to tailor their properties is yet to be realized. Here we present a continuously tunable moiré potential in monolayer WSe2, enabled by its proximity to twisted bilayer graphene (TBG) near the magic angle. By tuning local charge density via gating, TBG provides a spatially varying and dynamically tunable dielectric superlattice for modulation of monolayer WSe2 exciton wave functions. We observed emergent moiré exciton Rydberg branches with increased energy splitting following doping of TBG due to exciton wave function hybridization between bright and dark Rydberg states. In addition, emergent Rydberg states can probe strongly correlated states in TBG at the magic angle. Our study provides a new platform for engineering moiré excitons and optical accessibility to electronic states with small correlation gaps in TBG.

8.
Nat Mater ; 23(1): 65-70, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37563291

ABSTRACT

Moiré superlattices host a rich variety of correlated electronic phases. However, the moiré potential is fixed by interlayer coupling, and it is dependent on the nature of carriers and valleys. In contrast, it has been predicted that twisted hexagonal boron nitride (hBN) layers can impose a periodic electrostatic potential capable of engineering the properties of adjacent functional layers. Here, we show that this potential is described by a theory of electric polarization originating from the interfacial charge redistribution, validated by its dependence on supercell sizes and distance from the twisted interfaces. This enables controllability of the potential depth and profile by controlling the twist angles between the two interfaces. Employing this approach, we further demonstrate how the electrostatic potential from a twisted hBN substrate impedes exciton diffusion in semiconductor monolayers, suggesting opportunities for engineering the properties of adjacent functional layers using the surface potential of a twisted hBN substrate.

9.
Nature ; 567(7746): 66-70, 2019 03.
Article in English | MEDLINE | ID: mdl-30804526

ABSTRACT

The formation of moiré patterns in crystalline solids can be used to manipulate their electronic properties, which are fundamentally influenced by periodic potential landscapes. In two-dimensional materials, a moiré pattern with a superlattice potential can be formed by vertically stacking two layered materials with a twist and/or a difference in lattice constant. This approach has led to electronic phenomena including the fractal quantum Hall effect1-3, tunable Mott insulators4,5 and unconventional superconductivity6. In addition, theory predicts that notable effects on optical excitations could result from a moiré potential in two-dimensional valley semiconductors7-9, but these signatures have not been detected experimentally. Here we report experimental evidence of interlayer valley excitons trapped in a moiré potential in molybdenum diselenide (MoSe2)/tungsten diselenide (WSe2) heterobilayers. At low temperatures, we observe photoluminescence close to the free interlayer exciton energy but with linewidths over one hundred times narrower (around 100 microelectronvolts). The emitter g-factors are homogeneous across the same sample and take only two values, -15.9 and 6.7, in samples with approximate twist angles of 60 degrees and 0 degrees, respectively. The g-factors match those of the free interlayer exciton, which is determined by one of two possible valley-pairing configurations. At twist angles of approximately 20 degrees the emitters become two orders of magnitude dimmer; however, they possess the same g-factor as the heterobilayer at a twist angle of approximately 60 degrees. This is consistent with the umklapp recombination of interlayer excitons near the commensurate 21.8-degree twist angle7. The emitters exhibit strong circular polarization of the same helicity for a given twist angle, which suggests that the trapping potential retains three-fold rotational symmetry. Together with a characteristic dependence on power and excitation energy, these results suggest that the origin of the observed effects is interlayer excitons trapped in a smooth moiré potential with inherited valley-contrasting physics. This work presents opportunities to control two-dimensional moiré optics through variation of the twist angle.

10.
Nature ; 572(7770): 497-501, 2019 08.
Article in English | MEDLINE | ID: mdl-31367036

ABSTRACT

Layered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. The van der Waals magnet chromium triiodide (CrI3) has been shown to be a layered antiferromagnetic insulator in its few-layer form1, opening up opportunities for various functionalities2-7 in electronic and optical devices. Here we report an emergent nonreciprocal second-order nonlinear optical effect in bilayer CrI3. The observed second-harmonic generation (SHG; a nonlinear optical process that converts two photons of the same frequency into one photon of twice the fundamental frequency) is several orders of magnitude larger than known magnetization-induced SHG8-11 and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far12,13 (for example, molybdenum disulfide). We show that although the parent lattice of bilayer CrI3 is centrosymmetric, and thus does not contribute to the SHG signal, the observed giant nonreciprocal SHG originates only from the layered antiferromagnetic order, which breaks both the spatial-inversion symmetry and the time-reversal symmetry. Furthermore, polarization-resolved measurements reveal underlying C2h crystallographic symmetry-and thus monoclinic stacking order-in bilayer CrI3, providing key structural information for the microscopic origin of layered antiferromagnetism14-18. Our results indicate that SHG is a highly sensitive probe of subtle magnetic orders and open up possibilities for the use of two-dimensional magnets in nonlinear and nonreciprocal optical devices.

11.
Nano Lett ; 24(26): 8017-8023, 2024 Jul 03.
Article in English | MEDLINE | ID: mdl-38899935

ABSTRACT

We show that interlayer charge transfer in 2D materials can be driven by an in-plane electric field, giving rise to electrical multipole generation in linear and second order in-plane field. The linear and nonlinear effects have quantum geometric origins in the Berry curvature and quantum metric, respectively, defined in extended parameter spaces characteristic of layered materials. We elucidate their symmetry characters and demonstrate sizable dipole and quadrupole polarizations, respectively, in twisted bilayers and trilayers of transition metal dichalcogenides. Furthermore, we show that this effect is strongly enhanced during the topological phase transition tuned by interlayer translation. The effects point to a new electric control on the layer quantum degree of freedom.

12.
Nano Lett ; 24(28): 8741-8751, 2024 Jul 17.
Article in English | MEDLINE | ID: mdl-38953486

ABSTRACT

The degradation of oncoproteins mediated by proteolysis-targeting chimera (PROTAC) has emerged as a potent strategy in cancer therapy. However, the clinical application of PROTACs is hampered by challenges such as poor water solubility and off-target adverse effects. Herein, we present an ultrasound (US)-activatable PROTAC prodrug termed NPCe6+PRO for actuating efficient sono-immunotherapy in a spatiotemporally controllable manner. Specifically, US irradiation, which exhibits deep-tissue penetration capability, results in Ce6-mediated generation of ROS, facilitating sonodynamic therapy (SDT) and inducing immunogenic cell death (ICD). Simultaneously, the generated ROS cleaves the thioketal (TK) linker through a ROS-responsive mechanism, realizing the on-demand activation of the PROTAC prodrug in deep tissues. This prodrug activation results in the degradation of the target protein BRD4, while simultaneously reversing the upregulation of PD-L1 expression associated with the SDT process. In the orthotopic mouse model of pancreatic tumors, NPCe6+PRO effectively suppressed tumor growth in conjunction with US stimulation.


Subject(s)
Immunotherapy , Pancreatic Neoplasms , Prodrugs , Animals , Prodrugs/pharmacology , Prodrugs/therapeutic use , Prodrugs/chemistry , Pancreatic Neoplasms/therapy , Pancreatic Neoplasms/drug therapy , Pancreatic Neoplasms/pathology , Pancreatic Neoplasms/immunology , Mice , Humans , Cell Line, Tumor , Proteolysis/drug effects , Ultrasonic Therapy/methods , B7-H1 Antigen , Transcription Factors , Cell Cycle Proteins , Reactive Oxygen Species/metabolism , Bromodomain Containing Proteins
13.
J Cell Physiol ; 239(6): e31272, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38646844

ABSTRACT

The inhibition of cell surface crystal adhesion and an appropriate increase in crystal endocytosis contribute to the inhibition of kidney stone formation. In this study, we investigated the effects of different degrees of carboxymethylation on these processes. An injury model was established by treating human renal proximal tubular epithelial (HK-2) cells with 98.3 ± 8.1 nm calcium oxalate dihydrate (nanoCOD) crystals. The HK-2 cells were protected with carboxy (-COOH) Desmodium styracifolium polysaccharides at 1.17% (DSP0), 7.45% (CDSP1), 12.2% (CDSP2), and 17.7% (CDSP3). Changes in biochemical indexes and effects on nanoCOD adhesion and endocytosis were detected. The protection of HK-2 cells from nanoCOD-induced oxidative damage by carboxymethylated Desmodium styracifolium polysaccharides (CDSPs) is closely related to the protection of subcellular organelles, such as mitochondria. CDSPs can reduce crystal adhesion on the cell surface and maintain appropriate crystal endocytosis, thereby reducing the risk of kidney stone formation. CDSP2 with moderate -COOH content showed the strongest protective activity among the CDSPs.


Subject(s)
Calcium Oxalate , Endocytosis , Kidney Calculi , Polysaccharides , Humans , Calcium Oxalate/metabolism , Cell Adhesion/drug effects , Cell Line , Crystallization , Endocytosis/drug effects , Epithelial Cells/drug effects , Epithelial Cells/metabolism , Epithelial Cells/pathology , Kidney Calculi/prevention & control , Kidney Calculi/drug therapy , Kidney Tubules, Proximal/drug effects , Kidney Tubules, Proximal/pathology , Kidney Tubules, Proximal/metabolism , Oxidative Stress/drug effects , Polysaccharides/pharmacology , Polysaccharides/chemistry , Cell Survival/drug effects , Cell Cycle/drug effects , Calcium/metabolism , Intracellular Space/metabolism , Reactive Oxygen Species/metabolism , Membrane Potential, Mitochondrial/drug effects
14.
Rep Prog Phys ; 87(10)2024 Sep 18.
Article in English | MEDLINE | ID: mdl-39241785

ABSTRACT

Supersymmetry (SUSY) of a Hamiltonian dictates double degeneracy between a pair of superpartners (SPs) transformed by supercharge, except at zero energy where modes remain unpaired in many cases. Here we explore a SUSY of complete isospectrum between SPs-with paired zero modes-realized by 2D electrons in zero-flux periodic gauge fields, which can describe twisted or periodically strained 2D materials. We find their low-energy sector containing zero (or threshold) modes must be topologically non-trivial, by proving that Chern numbers of the two SPs have a finite difference dictated by the number of zero modes and energy dispersion in their vicinity. In 30° twisted bilayer (double bilayer) transition metal dichalcogenides subject to periodic strain, we find one SP is topologically trivial in its lowest miniband, while the twin SP of identical dispersion has a Chern number of 1 (2), in stark contrast to time-reversal partners that have to be simultaneously trivial or nontrivial. For systems whose physical Hamiltonian corresponds to the square root of a SUSY Hamiltonian, such as twisted or strained bilayer graphene, we reveal that topological properties of the two SUSY SPs are transferred respectively to the conduction and valence bands, including the contrasted topology in the low-energy sector and identical topology in the high-energy sector. This offers a unified perspective for understanding topological properties in many flat-band systems described by such square-root models. Both types of SUSY systems provide unique opportunities for exploring correlated and topological phases of matter.

15.
Br J Cancer ; 131(5): 832-842, 2024 Sep.
Article in English | MEDLINE | ID: mdl-38971951

ABSTRACT

IMPORTANCE: Intra-arterial therapies(IATs) are promising options for unresectable hepatocellular carcinoma(HCC). Stratifying the prognostic risk before administering IAT is important for clinical decision-making and for designing future clinical trials. OBJECTIVE: To develop and validate a machine learning(ML)-based decision support model(MLDSM) for recommending IAT modalities for unresectable HCC. DESIGN, SETTING, AND PARTICIPANTS: Between October 2014 and October 2022, a total of 2,959 patients with HCC who underwent initial IATs were enroled retrospectively from 13 tertiary hospitals. These patients were divided into the training cohort (n = 1700), validation cohort (n = 428), and test cohort (n = 200). MAIN OUTCOMES AND MEASURES: Thirty-two clinical variables were input, and five supervised ML algorithms, including eXtreme Gradient Boosting (XGBoost), Categorical Gradient Boosting (CatBoost), Gradient Boosting Decision Tree (GBDT), Light Gradient Boosting Machine (LGBM) and Random Forest (RF), were compared using the areas under the receiver operating characteristic curve (AUC) with the DeLong test. RESULTS: A total of 1856 patients were assigned to the IAT alone Group(I-A), and 1103 patients were assigned to the IAT combination Group(I-C). The 12-month death rates were 31.9% (352/1103) in the I-A group and 50.4% (936/1856) in the I-C group. For the test cohort, in the I-C group, the CatBoost model achieved the best discrimination when 30 variables were input, with an AUC of 0.776 (95% confidence intervals [CI], 0.833-0.868). In the I-A group, the LGBM model achieved the best discrimination when 24 variables were input, with an AUC of 0.776 (95% CI, 0.833-0.868). According to the decision trees, BCLC grade, local therapy, and diameter as top three variables were used to guide clinical decisions between IAT modalities. CONCLUSIONS AND RELEVANCE: The MLDSM can accurately stratify prognostic risk for HCC patients who received IATs, thus helping physicians to make decisions about IAT and providing guidance for surveillance strategies in clinical practice.


Subject(s)
Carcinoma, Hepatocellular , Liver Neoplasms , Machine Learning , Humans , Carcinoma, Hepatocellular/therapy , Carcinoma, Hepatocellular/pathology , Liver Neoplasms/therapy , Liver Neoplasms/pathology , Male , Female , Middle Aged , Aged , Retrospective Studies , Decision Support Techniques , Clinical Decision-Making , Prognosis , Chemoembolization, Therapeutic/methods
16.
Small ; 20(22): e2307961, 2024 May.
Article in English | MEDLINE | ID: mdl-38126911

ABSTRACT

Activating the stimulator of the interferon gene (STING) is a promising immunotherapeutic strategy for converting "cold" tumor microenvironment into "hot" one to achieve better immunotherapy for malignant tumors. Herein, a manganese-based nanotransformer is presented, consisting of manganese carbonyl and cyanine dye, for MRI/NIR-II dual-modality imaging-guided multifunctional carbon monoxide (CO) gas treatment and photothermal therapy, along with triggering cGAS-STING immune pathway against triple-negative breast cancer. This nanosystem is able to transfer its amorphous morphology into a crystallographic-like formation in response to the tumor microenvironment, achieved by breaking metal-carbon bonds and forming coordination bonds, which enhances the sensitivity of magnetic resonance imaging. Moreover, the generated CO and photothermal effect under irradiation of this nanotransformer induce immunogenic death of tumor cells and release damage-associated molecular patterns. Simultaneously, the Mn acts as an immunoactivator, potentially stimulating the cGAS-STING pathway to augment adaptive immunity, resulting in promoting the secretion of type I interferon, the proliferation of cytotoxic T lymphocytes and M2-macrophages repolarization. This nanosystem-based gas-photothermal treatment and immunoactivating therapy synergistic effect exhibit excellent antitumor efficacy both in vitro and in vivo, reducing the risk of triple-negative breast cancer recurrence and metastasis; thus, this strategy presents great potential as multifunctional immunotherapeutic agents for cancer treatment.


Subject(s)
Immunotherapy , Manganese , Photothermal Therapy , Triple Negative Breast Neoplasms , Triple Negative Breast Neoplasms/therapy , Immunotherapy/methods , Manganese/chemistry , Humans , Animals , Photothermal Therapy/methods , Cell Line, Tumor , Female , Magnetic Resonance Imaging/methods , Mice , Tumor Microenvironment , Nanoparticles/chemistry , Phototherapy/methods
17.
Nat Mater ; 22(5): 599-604, 2023 May.
Article in English | MEDLINE | ID: mdl-36894775

ABSTRACT

Excitons, Coulomb-bound electron-hole pairs, play a crucial role in both optical excitation and correlated phenomena in solids. When excitons interact with other quasiparticles, few- and many-body excited states can appear. Here we report an interaction between exciton and charges enabled by unusual quantum confinement in two-dimensional moiré superlattices, which results in many-body ground states composed of moiré excitons and correlated electron lattices. In an H-stacked (60o-twisted) WS2/WSe2 heterobilayer, we found an interlayer moiré exciton whose hole is surrounded by its partner electron's wavefunction distributed among three adjacent moiré traps. This three-dimensional excitonic structure enables large in-plane electrical quadrupole moments in addition to the vertical dipole. Upon doping, the quadrupole facilitates the binding of interlayer moiré excitons to the charges in neighbouring moiré cells, forming intercell charged exciton complexes. Our work provides a framework for understanding and engineering emergent exciton many-body states in correlated moiré charge orders.

18.
Phys Rev Lett ; 133(8): 086501, 2024 Aug 23.
Article in English | MEDLINE | ID: mdl-39241712

ABSTRACT

Moiré superlattices of layered transition metal dichalcogenides are proven to host periodic electron crystals due to strong correlation effects. These electron crystals can also be intertwined with intricate magnetic phenomena. In this Letter, we present our findings on the moiré exchange effect, resulting from the modulation of local magnetic moments by electron crystals within well-aligned WSe_{2}/WS_{2} heterobilayers. Employing polarization-resolved magneto-optical spectroscopy, we unveil a high-energy excitonic resonance near one hole per moiré unit cell (v=-1), which possesses a giant g factor several times greater than the already very large g factor of the WSe_{2} A exciton in this heterostructure. Supported by continuum model calculations, these high-energy states are found to be dark excitons brightened through Umklapp scattering from the moiré mini-Brillouin zone. When the carriers form a Mott insulating state near v=-1, the Coulomb exchange between doped carriers and excitons forms an effective magnetic field with moiré periodicity. This moiré exchange effect gives rise to the observed giant g factor for the excitonic Umklapp state.

19.
Environ Res ; : 120061, 2024 Sep 24.
Article in English | MEDLINE | ID: mdl-39326652

ABSTRACT

Although the production and usage of polybrominated biphenyls (PBBs) as brominated flame retardants have already been prohibited, they still pose a threat to the environment and human health. However, the evolutionary behaviors and decomposition mechanisms of PBBs during thermal treatment of waste remain unclear. In the present work, the mechanism and kinetics of thermal decomposition of decabromobiphenyl (deca-BB), one of the most frequently-used PBB congeners, are studied in detail using quantum chemical calculations. Results indicate that the high bond dissociation energies and large energy gap of deca-BB make its self-decomposition reaction difficult to occur, while its reactions with several reactive radicals (including hydrogen, bromine, and hydroxyl radicals) in the combustion environment are universally carried out at low energy barriers. Hydrogen, bromine, and hydroxyl radicals all exhibit a high selectivity for the para-C/Br atoms of deca-BB, resulting in the generation of several debromination products or intermediates. This study also investigates the formation mechanism of polybrominated dibenzofurans (PBDFs) from deca-BB and the effect of polymeric materials on this process. We found that the oxidation of ortho-phenyl-type radical, followed by evolution into PBDFs, is a very exothermic and relatively low-barrier process. Thus, the emergence of ortho-phenyl-type radicals from the loss of ortho-Br atoms is a critical step in the formation of PBDFs. Influence of polymeric materials on the formation of PBDFs is reflected in that various alkyl radicals and diradicals produced by their decomposition can readily abstract ortho-Br atoms to generate ortho-phenyl-type radicals, thus facilitating the formation of PBDFs. The mechanistic pathways and kinetic parameters presented in this study can offer theoretical guidance for controlling contaminant emissions in the thermal treatment of deca-BB-containing waste.

20.
J Chem Phys ; 160(14)2024 Apr 14.
Article in English | MEDLINE | ID: mdl-38606736

ABSTRACT

Two-dimensional (2D) transition metal dichalcogenides have emerged as promising quantum functional blocks benefitting from their unique combination of spin, valley, and layer degrees of freedom, particularly for the tremendous flexibility of moiré superlattices formed by van der Waals stacking. These degrees of freedom coupled with the enhanced Coulomb interaction in 2D structures allow excitons to serve as on-chip information carriers. However, excitons are spatially circumscribed due to their low mobility and limited lifetime. One way to overcome these limitations is through the coupling of excitons with surface plasmon polaritons (SPPs), which facilitates an interaction between remote quantum states. Here, we showcase the successful coupling of SPPs with interlayer excitons in molybdenum diselenide/tungsten diselenide heterobilayers. Our results indicate that the valley polarization can be efficiently transferred to SPPs, enabling preservation of polarization information even after propagating tens of micrometers.

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