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1.
Nat Nanotechnol ; 17(2): 182-189, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-34857931

RESUMEN

Two-dimensional (2D) crystals have renewed opportunities in design and assembly of artificial lattices without the constraints of epitaxy. However, the lack of thickness control in exfoliated van der Waals (vdW) layers prevents realization of repeat units with high fidelity. Recent availability of uniform, wafer-scale samples permits engineering of both electronic and optical dispersions in stacks of disparate 2D layers with multiple repeating units. Here we present optical dispersion engineering in a superlattice structure comprising alternating layers of 2D excitonic chalcogenides and dielectric insulators. By carefully designing the unit cell parameters, we demonstrate greater than 90% narrow band absorption in less than 4 nm of active layer excitonic absorber medium at room temperature, concurrently with enhanced photoluminescence in square-centimetre samples. These superlattices show evidence of strong light-matter coupling and exciton-polariton formation with geometry-tuneable coupling constants. Our results demonstrate proof of concept structures with engineered optical properties and pave the way for a broad class of scalable, designer optical metamaterials from atomically thin layers.

2.
Nano Lett ; 21(14): 6245-6252, 2021 Jul 28.
Artículo en Inglés | MEDLINE | ID: mdl-34260259

RESUMEN

Light-matter coupling in excitonic materials has been the subject of intense recent investigations due to emergence of new materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room temperature with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-matter coupling in Ruddlesden-Popper phase 2D HOIP crystals without the necessity of an external cavity. We report the concurrent occurrence of multiple orders of hybrid light-matter states via both reflectance and luminescence spectroscopy in thick (>100 nm) crystals and near-unity absorption in thin (<20 nm) crystals. We observe resonances with quality factors of >250 in hybridized exciton-polaritons and identify a linear correlation between exciton-polariton mode splitting and extinction coefficient of the various 2D HOIPs. Our work opens the door to studying polariton dynamics in self-hybridized and open cavity systems with broad applications in optoelectronics and photochemistry.

3.
Nano Lett ; 20(4): 2907-2915, 2020 Apr 08.
Artículo en Inglés | MEDLINE | ID: mdl-32196351

RESUMEN

van der Waals (vdW) semiconductors are attractive for highly scaled devices and heterogeneous integration as they can be isolated into self-passivated, two-dimensional (2D) layers that enable superior electrostatic control. These attributes have led to numerous demonstrations of field-effect devices ranging from transistors to triodes. By exploiting the controlled, substitutional doping schemes in covalently bonded, three-dimensional (3D) semiconductors and the passivated surfaces of 2D semiconductors, one can construct devices that can exceed performance metrics of "all-2D" vdW heterojunctions. Here, we demonstrate 2D/3D semiconductor heterojunctions using MoS2 as the prototypical 2D semiconductor laid upon Si and GaN as the 3D semiconductor layers. By tuning the Fermi levels in MoS2, we demonstrate devices that concurrently exhibit over 7 orders of magnitude modulation in rectification ratios and conductance. Our results further suggest that the interface quality does not necessarily affect Fermi level tuning at the junction, opening up possibilities for novel 2D/3D heterojunction device architectures.

4.
Nanoscale ; 11(47): 22762-22771, 2019 Dec 21.
Artículo en Inglés | MEDLINE | ID: mdl-31482913

RESUMEN

Two-dimensional (2D) materials usually exhibit interesting layer-dependent dielectric and optical properties, which play important roles in structure optimization and performance improvement of related devices. Recently, 2D WSe2 has attracted considerable attention in atomically thin electronics and optoelectronics, due to its exotic photoelectric properties. In this paper, high-quality, continuous, and centimeter-scale 2D WSe2 with different layers on a sapphire substrate are prepared by an ultrafast ambient-pressure chemical vapor deposition method. We comprehensively investigate the evolution of the layer-dependent dielectric and optical properties of 2D WSe2 from a single layer to five layers by spectroscopic ellipsometry over an ultra-broad energy range (0.73-6.42 eV). We identify the critical points (CPs) in the dielectric function spectra of 2D WSe2 with different layers, and reveal physical origins of the corresponding optical transitions at these CPs by the CP analysis method and first-principles calculations. Results demonstrate that the center energies of these CPs exhibit intriguing layer-dependencies, which can be interpreted as the alternative domination of the decreasing exciton binding energy and the striking band renormalization. For the first time, we found that the imaginary part of the dielectric function of WSe2 at these CPs exhibits a valley-like shape versus the layer number, and the bottom appears at 3-layers. This non-monotonic evolution is explained as a competition between the layer-dependent decrease of the exciton effect and the layer-dependent increase of the joint density of states.

5.
J Phys Chem Lett ; 10(20): 6246-6252, 2019 Oct 17.
Artículo en Inglés | MEDLINE | ID: mdl-31490075

RESUMEN

The complex optical conductivities of two-dimensaionl (2D) materials are fundamental for extended applications of related optoelectronic devices. Here, we systematically investigate the layer-dependent evolutions in the complex optical conductivities of 1-6 layer 2D MoS2 over an ultrawide spectral range (0.73-6.42 eV) by spectroscopic ellipsometry. We identify five feature peaks (A-E) in the optical conductivity spectra, which present interesting layer dependencies due to the scaling effect. Results suggest that the center energies of peaks A and B are nearly layer-independent, while those of peaks C and D exhibit redshifts as the layer increases. We interpret these layer-dependent evolutions as the competition between the decreasing exciton effect and the prominent band shrinkage with the increasing layer number. Additionally, the applicability of the classical slab model and the surface current model in evaluating the optical conductivities of 2D MoS2 with different layers is discussed from an experimental perspective.

6.
ACS Appl Mater Interfaces ; 11(18): 16272-16279, 2019 May 08.
Artículo en Inglés | MEDLINE | ID: mdl-31020828

RESUMEN

Graphene and its clean transfer methods have gathered growing interest and concern in recent decades. Here, we develop a novel large-scale intact transferring technology of paraffin wax onto arbitrary substrates. The wax will then be removed by thermal evaporation, avoiding uncontrollable reactions and leaving no residues. For characterizations, we adopt Raman, FT-IR, XPS, and DRS to measure the optical reflection difference on various surfaces and the thickness of graphene accurately. All the results demonstrate transferred surfaces' cleanliness and our method's validity. This technique allows for an effective transfer of graphene and enables a wider range of applications in many fields.

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