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1.
Nature ; 613(7942): 53-59, 2023 01.
Article in English | MEDLINE | ID: mdl-36600061

ABSTRACT

Interlayer electronic coupling in two-dimensional materials enables tunable and emergent properties by stacking engineering. However, it also results in significant evolution of electronic structures and attenuation of excitonic effects in two-dimensional semiconductors as exemplified by quickly degrading excitonic photoluminescence and optical nonlinearities in transition metal dichalcogenides when monolayers are stacked into van der Waals structures. Here we report a van der Waals crystal, niobium oxide dichloride (NbOCl2), featuring vanishing interlayer electronic coupling and monolayer-like excitonic behaviour in the bulk form, along with a scalable second-harmonic generation intensity of up to three orders higher than that in monolayer WS2. Notably, the strong second-order nonlinearity enables correlated parametric photon pair generation, through a spontaneous parametric down-conversion (SPDC) process, in flakes as thin as about 46 nm. To our knowledge, this is the first SPDC source unambiguously demonstrated in two-dimensional layered materials, and the thinnest SPDC source ever reported. Our work opens an avenue towards developing van der Waals material-based ultracompact on-chip SPDC sources as well as high-performance photon modulators in both classical and quantum optical technologies1-4.

2.
Nano Lett ; 22(6): 2244-2250, 2022 Mar 23.
Article in English | MEDLINE | ID: mdl-35274532

ABSTRACT

Single photon emitters (SPEs) are critical components of photon-based quantum technology. Recently, the interaction between surface plasmons and emitters has attracted increasing attention because of its potential to improve the quality of single-photon sources through stronger light-matter interactions. In this work, we use a hybrid plasmonic probe composed of a fiber taper and silver nanowire to controllably modulate the radiation properties of SPEs with differently oriented polarization. For out-of-plane oriented SPEs such as single CdSe quantum dots, the radiation lifetime could be reduced by a factor as large as seven; for in-plane oriented SPEs such as hBN defect SPEs, the average modulation amplitude varied from 0.69 to 1.23, depending on the position of the probe. The experimental results were highly consistent with the simulations and theory. This work provides an efficient approach for optimizing the properties of SPEs for quantum photonic integration.

3.
Phys Rev Lett ; 128(6): 060501, 2022 Feb 11.
Article in English | MEDLINE | ID: mdl-35213196

ABSTRACT

As an important degree of freedom (d.o.f.) in photonic integrated circuits, the orthogonal transverse mode provides a promising and flexible way to increase communication capability, for both classical and quantum information processing. To construct large-scale on-chip multimode multi-d.o.f.s quantum systems, a transverse mode-encoded controlled-NOT (CNOT) gate is necessary. Here, with the help of our new transverse mode-dependent directional coupler and attenuator, we demonstrate the first multimode implementation of a 2-qubit quantum gate. The ability of the gate is demonstrated by entangling two separated transverse mode qubits with an average fidelity of 0.89±0.02 and the achievement of 10 standard deviations of violations in the quantum nonlocality verification. In addition, a fidelity of 0.82±0.01 is obtained from quantum process tomography used to completely characterize the CNOT gate. Our work paves the way for universal transverse mode-encoded quantum operations and large-scale multimode multi-d.o.f.s quantum systems.

4.
J Am Chem Soc ; 141(27): 10729-10735, 2019 Jul 10.
Article in English | MEDLINE | ID: mdl-31246444

ABSTRACT

Designing high-efficiency catalyst is at the heart of a transition to future renewable energy systems. Great achievements have been made to optimize thermodynamics to reduce energetic barriers of the catalytic reactions. However, little attention has been paid to design catalysts to improve kinetics to enrich the local concentration of reactant molecules surrounding electrocatalysts. Here, we find that well-designed nanocatalysts with periodic structures can optimize kinetics to accelerate mass-transport from bulk electrolyte to the catalyst surface, leading to the enhanced catalytic performance. This achievement stems from regulation of the surface reactant flux due to the gradient of the microelectric field directing uniformly to the nearest catalyst on ordered pattern, so that all of the reactant molecules are utilized sufficiently for reactions, enabling the boost of the electrocatalytic performance. This novel concept is further confirmed in various catalytic systems and nanoassemblies, such as nanoparticles, nanorods, and nanoflakes.

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