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1.
Chem Sci ; 15(27): 10625-10637, 2024 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-38994408

RESUMO

Solar CO2 reduction to renewable hydrocarbon fuels offers a promising pathway to carbon neutrality, but it is retarded by tough CO2 activation, complicated mechanisms, sluggish charge transport kinetics, and a scarcity of strategies for precise tuning of charge transport pathways. Herein, we first conceptually design a novel insulating polymer-mediated electron-tunneling artificial photosystem via progressive interface configuration regulation, wherein tailor-made Ag@citrate nanocrystals (NCs) are controllably self-assembled on transition metal chalcogenides (TMCs) assisted by an ultrathin insulating polymer interim layer, i.e., poly(allylamine hydrochloride) (PAH). In this multilayered nano-architecture, a solid ultra-thin insulating PAH interim layer serves as an unexpected charge tunneling mediator to stimulate smooth electron transfer from the TMC substrate to the terminal electron reservoirs of Ag@citrate NCs, engendering the tandem charge transfer route and significantly boosting the visible-light-driven photocatalytic CO2-to-syngas conversion performances. Furthermore, we have ascertained that such TMC-insulating polymer-metal NC tunneling photosystems are universal. This study would spark new inspiration for unleashing the long-term neglected charge tunneling capability of insulating polymers and diversifying non-conjugated polymer-based artificial photosystems for solar-to-fuel energy conversion.

2.
Nano Lett ; 24(22): 6722-6729, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38717299

RESUMO

Double-layer quantum systems are promising platforms for realizing novel quantum phases. Here, we report a study of quantum oscillations (QOs) in a weakly coupled double-layer system composed of a large-angle twisted-double-bilayer graphene (TDBG). We quantify the interlayer coupling strength by measuring the interlayer capacitance from the QOs pattern at low temperatures, revealing electron-hole asymmetry. At high temperatures when SdHOs are thermally smeared, we observe resistance peaks when Landau levels (LLs) from two moiré minivalleys are aligned, regardless of carrier density; eventually, it results in a 2-fold increase of oscillating frequency in D, serving as compelling evidence of the magneto-intersub-band oscillations (MISOs) in double-layer systems. The temperature dependence of MISOs suggests that electron-electron interactions play a crucial role and the scattering times obtained from MISO thermal damping are correlated with the interlayer coupling strength. Our study reveals intriguing interplays among Landau quantization, moiré band structure, and scatterings.

3.
Nat Commun ; 15(1): 1888, 2024 Feb 29.
Artigo em Inglês | MEDLINE | ID: mdl-38424092

RESUMO

Stacking order plays a crucial role in determining the crystal symmetry and has significant impacts on electronic, optical, magnetic, and topological properties. Electron-phonon coupling, which is central to a wide range of intriguing quantum phenomena, is expected to be intricately connected with stacking order. Understanding the stacking order-dependent electron-phonon coupling is essential for understanding peculiar physical phenomena associated with electron-phonon coupling, such as superconductivity and charge density waves. In this study, we investigate the effect of stacking order on electron-infrared phonon coupling in graphene trilayers. By using gate-tunable Raman spectroscopy and excitation frequency-dependent near-field infrared nanoscopy, we show that rhombohedral ABC-stacked trilayer graphene has a significant electron-infrared phonon coupling strength. Our findings provide novel insights into the superconductivity and other fundamental physical properties of rhombohedral ABC-stacked trilayer graphene, and can enable nondestructive and high-throughput imaging of trilayer graphene stacking order using Raman scattering.

4.
Sci Bull (Beijing) ; 68(11): 1127-1133, 2023 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-37210331

RESUMO

We report an observation of quantum oscillations (QOs) in the correlated insulators with valley anisotropy of twisted double bilayer graphene (TDBG). The anomalous QOs are best captured in the magneto resistivity oscillations of the insulators at v = -2, with a period of 1/B and an oscillation amplitude as high as 150 kΩ. The QOs can survive up to ∼10 K, and above 12 K, the insulating behaviors are dominant. The QOs of the insulator are strongly D dependent: the carrier density extracted from the 1/B periodicity decreases almost linearly with D from -0.7 to -1.1 V/nm, suggesting a reduced Fermi surface; the effective mass from Lifshitz-Kosevich analysis depends nonlinearly on D, reaching a minimal value of 0.1 me at D = ∼ -1.0 V/nm. Similar observations of QOs are also found at v = 2, as well as in other devices without graphite gate. We interpret the D sensitive QOs of the correlated insulators in the picture of band inversion. By reconstructing an inverted band model with the measured effective mass and Fermi surface, the density of state at the gap, calculated from thermal broadened Landau levels, agrees qualitatively with the observed QOs in the insulators. While more theoretical understandings are needed in the future to fully account for the anomalous QOs in this moiré system, our study suggests that TDBG is an excellent platform to discover exotic phases where correlation and topology are at play.


Assuntos
Excipientes , Grafite , Humanos , Anisotropia , Inversão Cromossômica , Meio Ambiente
5.
Phys Rev Lett ; 131(25): 256201, 2023 Dec 22.
Artigo em Inglês | MEDLINE | ID: mdl-38181343

RESUMO

Moiré superlattices have emerged as an exciting condensed-matter quantum simulator for exploring the exotic physics of strong electronic correlations. Notable progress has been witnessed, but such correlated states are achievable usually at low temperatures. Here, we report evidence of possible room-temperature correlated electronic states and layer-hybridized SU(4) model simulator in AB-stacked MoS_{2} homobilayer moiré superlattices. Correlated insulating states at moiré band filling factors v=1, 2, 3 are unambiguously established in twisted bilayer MoS_{2}. Remarkably, the correlated electronic state at v=1 shows a giant correlated gap of ∼126 meV and may persist up to a record-high critical temperature over 285 K. The realization of a possible room-temperature correlated state with a large correlated gap in twisted bilayer MoS_{2} can be understood as the cooperation effects of the stacking-specific atomic reconstruction and the resonantly enhanced interlayer hybridization, which largely amplify the moiré superlattice effects on electronic correlations. Furthermore, extreme large nonlinear Hall responses up to room temperature are uncovered near correlated electronic states, demonstrating the quantum geometry of moiré flat conduction band.

6.
Nat Commun ; 13(1): 3292, 2022 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-35672329

RESUMO

New phase of matter usually emerges when a given symmetry breaks spontaneously, which can involve charge, spin, and valley degree of freedoms. Here, we report an observation of new correlated insulators evolved from spin-polarized states to valley-polarized states in twisted double bilayer graphene (TDBG) driven by the displacement field (D). At a high field |D | > 0.7 V/nm, we observe valley polarized correlated insulators with a big Zeeman g factor of ~10, both at v = 2 in the moiré conduction band and more surprisingly at v = -2 in the moiré valence band. Moreover, we observe a valley polarized Chern insulator with C = 2 emanating at v = 2 in the electron side and a valley polarized Fermi surface around v = -2 in the hole side. Our results demonstrate a feasible way to realize isospin control and to obtain new phases of matter in TDBG by the displacement field, and might benefit other twisted or non-twisted multilayer systems.

7.
J Safety Res ; 76: 154-165, 2021 02.
Artigo em Inglês | MEDLINE | ID: mdl-33653546

RESUMO

INTRODUCTION: Fatal crashes that include at least one fatality of an occupant within 30 days of the crash cause large numbers of injured persons and property losses, especially when a truck is involved. METHOD: To better understand the underlying effects of truck-driver-related characteristics in fatal crashes, a five-year (from 2012 to 2016) dataset from the Fatality Analysis Reporting System (FARS) was used for analysis. Based on demographic attributes, driving violation behavior, crash histories, and conviction records of truck drivers, a latent class clustering analysis was applied to classify truck drivers into three groups, namely, ''middle-aged and elderly drivers with low risk of driving violations and high historical crash records," ''drivers with high risk of driving violations and high historical crash records," and ''middle-aged drivers with no driving violations and conviction records." Next, equivalent fatalities were used to scale fatal crash severities into three levels. Subsequently, a partial proportional odds (PPO) model for each driver group was developed to identify the risk factors associated with the crash severity. Results' Conclusions: The model estimation results showed that the risk factors, as well as their impacts on different driver groups, were different. Adverse weather conditions, rural areas, curved alignments, tractor-trailer units, heavier weights and various collision manners were significantly associated with the crash severities in all driver groups, whereas driving violation behaviors such as driving under the influence of alcohol or drugs, fatigue, or carelessness were significantly associated with the high-risk group only, and fewer risk factors and minor marginal effects were identified for the low-risk groups. Practical Applications: Corresponding countermeasures for specific truck driver groups are proposed. And drivers with high risk of driving violations and high historical crash records should be more concerned.


Assuntos
Acidentes de Trânsito/estatística & dados numéricos , Condução de Veículo/estatística & dados numéricos , Veículos Automotores/classificação , Adulto , Idoso , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Porto Rico , Fatores de Risco , Estados Unidos , Adulto Jovem
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