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1.
Nat Commun ; 13(1): 413, 2022 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-35058434

RESUMO

Compelling evidence suggests distinct correlated electron behavior may exist only in clean 2D materials such as 1T-TaS2. Unfortunately, experiment and theory suggest that extrinsic disorder in free standing 2D layers disrupts correlation-driven quantum behavior. Here we demonstrate a route to realizing fragile 2D quantum states through endotaxial polytype engineering of van der Waals materials. The true isolation of 2D charge density waves (CDWs) between metallic layers stabilizes commensurate long-range order and lifts the coupling between neighboring CDW layers to restore mirror symmetries via interlayer CDW twinning. The twinned-commensurate charge density wave (tC-CDW) reported herein has a single metal-insulator phase transition at ~350 K as measured structurally and electronically. Fast in-situ transmission electron microscopy and scanned nanobeam diffraction map the formation of tC-CDWs. This work introduces endotaxial polytype engineering of van der Waals materials to access latent 2D ground states distinct from conventional 2D fabrication.

2.
Phys Rev Lett ; 127(12): 126401, 2021 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-34597104

RESUMO

We show the ferro-rotational nature of the commensurate charge density wave (CCDW) in 1T-TaS_{2} and track its dynamic modulations by temperature-dependent and time-resolved electric quadrupole rotation anisotropy-second harmonic generation (EQ RA-SHG), respectively. The ultrafast modulations manifest as the breathing and the rotation of the EQ RA-SHG patterns at three frequencies around the reported single CCDW amplitude mode frequency. A sudden shift of the triplet frequencies and a dramatic increase in the breathing and rotation magnitude further reveal a photoinduced transient CDW phase across a critical pump fluence of ∼0.5 mJ/cm^{2}.

3.
Adv Sci (Weinh) ; 8(18): e2003046, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34250750

RESUMO

Perovskite photovoltaic ABX3 systems are being studied due to their high energy-conversion efficiencies with current emphasis placed on pure inorganic systems. In this work, synchrotron single-crystal diffraction measurements combined with second harmonic generation measurements reveal the absence of inversion symmetry below room temperature in CsPbBr3 . Local structural analysis by pair distribution function and X-ray absorption fine structure methods are performed to ascertain the local ordering, atomic pair correlations, and phase evolution in a broad range of temperatures. The currently accepted space group assignments for CsPbBr3 are found to be incorrect in a manner that profoundly impacts physical properties. New assignments are obtained for the bulk structure: I m 3 ¯ (above ≈410 K), P21 /m (between ≈300 K and ≈410 K), and the polar group Pm (below ≈300 K), respectively. The newly observed structural distortions exist in the bulk structure consistent with the expectation of previous photoluminescence and Raman measurements. High-pressure measurements reveal multiple low-pressure phases, one of which exists as a metastable phase at ambient pressure. This work should help guide research in the perovskite photovoltaic community to better control the structure under operational conditions and further improve transport and optical properties.

4.
Nat Commun ; 11(1): 4780, 2020 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-32963250

RESUMO

Exciton dynamics can be strongly affected by lattice vibrations through electron-phonon coupling. This is rarely explored in two-dimensional magnetic semiconductors. Focusing on bilayer CrI3, we first show the presence of strong electron-phonon coupling through temperature-dependent photoluminescence and absorption spectroscopy. We then report the observation of periodic broad modes up to the 8th order in Raman spectra, attributed to the polaronic character of excitons. We establish that this polaronic character is dominated by the coupling between the charge-transfer exciton at 1.96 eV and a longitudinal optical phonon at 120.6 cm-1. We further show that the emergence of long-range magnetic order enhances the electron-phonon coupling strength by ~50% and that the transition from layered antiferromagnetic to ferromagnetic order tunes the spectral intensity of the periodic broad modes, suggesting a strong coupling among the lattice, charge and spin in two-dimensional CrI3. Our study opens opportunities for tailoring light-matter interactions in two-dimensional magnetic semiconductors.

5.
Proc Natl Acad Sci U S A ; 117(40): 24664-24669, 2020 Oct 06.
Artigo em Inglês | MEDLINE | ID: mdl-32968024

RESUMO

We used a combination of polarized Raman spectroscopy experiment and model magnetism-phonon coupling calculations to study the rich magneto-Raman effect in the two-dimensional (2D) magnet CrI3 We reveal a layered-magnetism-assisted phonon scattering mechanism below the magnetic onset temperature, whose Raman excitation breaks time-reversal symmetry, has an antisymmetric Raman tensor, and follows the magnetic phase transitions across critical magnetic fields, on top of the presence of the conventional phonon scattering with symmetric Raman tensors in N-layer CrI3 We resolve in data and by calculations that the first-order A g phonon of the monolayer splits into an N-fold multiplet in N-layer CrI3 due to the interlayer coupling [Formula: see text] and that the phonons within the multiplet show distinct magnetic field dependence because of their different layered-magnetism-phonon coupling. We further find that such a layered-magnetism-phonon coupled Raman scattering mechanism extends beyond first-order to higher-order multiphonon scattering processes. Our results on the magneto-Raman effect of the first-order phonons in the multiplet and the higher-order multiphonons in N-layer CrI3 demonstrate the rich and strong behavior of emergent magneto-optical effects in 2D magnets and underline the unique opportunities of spin-phonon physics in van der Waals layered magnets.

6.
Materials (Basel) ; 13(1)2019 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-31861800

RESUMO

In this paper, a multi-layer and multi-track finite element model of 24CrNiMo alloy steel by selective laser melting (SLM) is established by using the ABAQUS software. The distribution and evolution of temperature field and stress field and the influence of process parameters on them are systematically studied. The results show that the peak temperature increases from 2153 °C to 3105 °C and the residual stress increases from 335 MPa to 364 MPa with increasing laser power from 200 W to 300 W; the peak temperature decreases from 2905 °C to 2405 °C and the residual stress increases from 327 MPa to 363 MPa with increasing scanning speed from 150 mm/s to 250 mm/s; the peak temperature increases from 2621 °C to 2914 °C and the residual stress decreases from 354 MPa to 300 MPa with increasing preheating temperature from 25 °C to 400 °C. Far away from scanning area, far away from starting point, and the adjacent areas with vertical scanning direction, resulting in a uniform temperature distribution, help to reduce the residual stress. Due to the remelting effect, the interlayer scanning angle changing helps to release the residual stress of the former layer causing a smaller residual stress after redistribution.

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