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1.
Adv Mater ; 36(24): e2312004, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38402422

RESUMEN

Quantum anomalous Hall (QAH) insulators transport charge without resistance along topologically protected chiral 1D edge states. Yet, in magnetic topological insulators to date, topological protection is far from robust, with zero-magnetic field QAH effect only realized at temperatures an order of magnitude below the Néel temperature TN, though small magnetic fields can stabilize QAH effect. Understanding why topological protection breaks down is therefore essential to realizing QAH effect at higher temperatures. Here a scanning tunneling microscope is used to directly map the size of exchange gap (Eg,ex) and its spatial fluctuation in the QAH insulator 5-layer MnBi2Te4. Long-range fluctuations of Eg,ex are observed, with values ranging between 0 (gapless) and 70 meV, appearing to be uncorrelated to individual surface point defects. The breakdown of topological protection is directly imaged, showing that the gapless edge state, the hallmark signature of a QAH insulator, hybridizes with extended gapless regions in the bulk. Finally, it is unambiguously demonstrated that the gapless regions originate from magnetic disorder, by demonstrating that a small magnetic field restores Eg,ex in these regions, explaining the recovery of topological protection in magnetic fields. The results indicate that overcoming magnetic disorder is the key to exploiting the unique properties of QAH insulators.

2.
ACS Nano ; 17(15): 14545-14554, 2023 Aug 08.
Artículo en Inglés | MEDLINE | ID: mdl-37494826

RESUMEN

Coherent optical manipulation of electronic bandstructures via Floquet Engineering is a promising means to control quantum systems on an ultrafast time scale. However, the ultrafast switching on/off of the driving field comes with questions regarding the limits of the Floquet formalism (which is defined for an infinite periodic drive) through the switching process and to what extent the transient changes can be driven adiabatically. Experimentally addressing these questions has been difficult, in large part due to the absence of an established technique to measure coherent dynamics through the duration of the pulse. Here, using multidimensional coherent spectroscopy we explicitly excite, control, and probe a coherent superposition of excitons in the K and K' valleys in monolayer WS2. With a circularly polarized, red-detuned pump pulse, the degeneracy of the K and K' excitons can be lifted, and the phase of the coherence rotated. We directly measure phase rotations greater than π during the 100 fs driving pulse and show that this can be described by a combination of the AC-Stark shift of excitons in one valley and the Bloch-Siegert shift of excitons in the opposite valley. Despite showing a smooth evolution of the phase that directly follows the intensity envelope of the nonresonant pump pulse, the process is not perfectly adiabatic. By measuring the magnitude of the macroscopic coherence as it evolves before, during, and after the nonresonant pump pulse we show that there is additional decoherence caused by power broadening in the presence of the nonresonant pump. This nonadiabaticity arises as a result of interactions with the otherwise adiabatic Floquet states and may be a problem for many applications, such as manipulating qubits in quantum information processing; however, these measurements also suggest ways such effects can be minimized or eliminated.

3.
J Phys Chem Lett ; 11(1): 136-143, 2020 Jan 02.
Artículo en Inglés | MEDLINE | ID: mdl-31829600

RESUMEN

The dynamics of photogenerated carriers and mobile ions in operational cesium lead halide (CsPbI3) perovskite solar cells (PSCs) under working conditions are studied using nanoscale-resolved fluorescence lifetime imaging microscopy (FLIM). The temporally and spatially resolved photoluminescence (PL) changes in the perovskite film during and after bias light soaking are dynamically monitored. Through the analysis of the dynamic variations of PL intensity and PL lifetime of an open-circuit PSC, the impacts of light soaking are revealed by a dynamic model of photogenerated charge carrier and mobile ions. We confirmed the different behaviors between morphological domain interiors and domain boundaries during light soaking, which shed light on the engineering of the domain interiors in addition to the commonly considered domain boundary strategies. This work provides a full picture of the photogenerated process in an operational PSC and therefore guides the design and operation of perovskite-based optoelectronic devices.

4.
Nat Commun ; 9(1): 3143, 2018 08 07.
Artículo en Inglés | MEDLINE | ID: mdl-30087328

RESUMEN

Interest in bringing p- and n-type monolayer semiconducting transition metal dichalcogenides (TMD) into contact to form rectifying pn diode has thrived since it is crucial to control the electrical properties in two-dimensional (2D) electronic and optoelectronic devices. Usually this involves vertically stacking different TMDs with pn heterojunction or, laterally manipulating carrier density by gate biasing. Here, by utilizing a locally reversed ferroelectric polarization, we laterally manipulate the carrier density and created a WSe2 pn homojunction on the supporting ferroelectric BiFeO3 substrate. This non-volatile WSe2 pn homojunction is demonstrated with optical and scanning probe methods and scanning photoelectron micro-spectroscopy. A homo-interface is a direct manifestation of our WSe2 pn diode, which can be quantitatively understood as a clear rectifying behavior. The non-volatile confinement of carriers and associated gate-free pn homojunction can be an addition to the 2D electron-photon toolbox and pave the way to develop laterally 2D electronics and photonics.

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