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1.
Nat Commun ; 14(1): 5548, 2023 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-37684279

RESUMO

We report the emergence of dark-excitons in transition-metal-dichalcogenide (TMD) heterostructures that strongly rely on the stacking sequence, i.e., momentum-dark K-Q exciton located exclusively at the top layer of the heterostructure. The feature stems from band renormalization and is distinct from those of typical neutral excitons or trions, regardless of materials, substrates, and even homogeneous bilayers, which is further confirmed by scanning tunneling spectroscopy. To understand the unusual stacking sequence, we introduce the excitonic Elliot formula by imposing strain exclusively on the top layer that could be a consequence of the stacking process. We further find that the intensity ratio of Q- to K-excitons in the same layer is inversely proportional to laser power, unlike for conventional K-K excitons. This can be a metric for engineering the intensity of dark K-Q excitons in TMD heterostructures, which could be useful for optical power switches in solar panels.

2.
Inorg Chem ; 62(32): 12674-12682, 2023 Aug 14.
Artigo em Inglês | MEDLINE | ID: mdl-37531606

RESUMO

Although magnetic order is suppressed by a strong frustration, it appears in complex forms such as a cycloid or spin density wave in weakly frustrated systems. Herein, we report a weakly magnetically frustrated two-dimensional (2D) van der Waals material CrPSe3. Polycrystalline CrPSe3 was synthesized at an optimized temperature of 700 °C to avoid the formation of any secondary phases (e.g., Cr2Se3). The antiferromagnetic transition appeared at TN ≈ 127 K with a large Curie-Weiss temperature θCW ≈ -301 K via magnetic susceptibility measurements, indicating weak frustration in CrPSe3 with a frustration factor of f (|θCW|/TN) ≈ 2.4. Evidently, the formation of a long-range incommensurate antiferromagnetic order was revealed by neutron diffraction measurements at low temperatures (below 120 K). The monoclinic crystal structure of the C2/m symmetry is preserved over the studied temperature range down to 20 K, as confirmed by Raman spectroscopy measurements. Our findings on the incommensurate antiferromagnetic order in 2D magnetic materials, not previously observed in the MPX3 family, are expected to enrich the physics of magnetism at the 2D limit, thereby opening opportunities for their practical applications in spintronics and quantum devices.

3.
Small ; 18(20): e2106368, 2022 May.
Artigo em Inglês | MEDLINE | ID: mdl-35451163

RESUMO

Advances in large-area and high-quality 2D transition metal dichalcogenides (TMDCs) growth are essential for semiconductor applications. Here, the gas-phase alkali metal-assisted metal-organic chemical vapor deposition (GAA-MOCVD) of 2D TMDCs is reported. It is determined that sodium propionate (SP) is an ideal gas-phase alkali-metal additive for nucleation control in the MOCVD of 2D TMDCs. The grain size of MoS2 in the GAA-MOCVD process is larger than that in the conventional MOCVD process. This method can be applied to the growth of various TMDCs (MoS2 , MoSe2 , WSe2 , and WSe2 ) and the generation of large-scale continuous films. Furthermore, the growth behaviors of MoS2 under different SP and oxygen injection time conditions are systematically investigated to determine the effects of SP and oxygen on nucleation control in the GAA-MOCVD process. It is found that the combination of SP and oxygen increases the grain size and nucleation suppression of MoS2 . Thus, the GAA-MOCVD with a precise and controllable supply of a gas-phase alkali metal and oxygen allows achievement of optimum growth conditions that maximizes the grain size of MoS2 . It is expected that GAA-MOCVD can provide a way for batch fabrication of large-scale atomically thin electronic devices based on 2D semiconductors.

4.
ACS Nano ; 15(12): 20267-20277, 2021 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-34807575

RESUMO

While valley polarization with strong Zeeman splitting is the most prominent characteristic of two-dimensional (2D) transition metal dichalcogenide (TMD) semiconductors under magnetic fields, enhancement of the Zeeman splitting has been demonstrated by incorporating magnetic dopants into the host materials. Unlike Fe, Mn, and Co, V is a distinctive dopant for ferromagnetic semiconducting properties at room temperature with large Zeeman shifting of band edges. Nevertheless, little known is the excitons interacting with spin-polarized carriers in V-doped TMDs. Here, we report anomalous circularly polarized photoluminescence (CPL) in a V-doped WSe2 monolayer at room temperature. Excitons couple to V-induced spin-polarized holes to generate spin-selective positive trions, leading to differences in the populations of neutral excitons and trions between left and right CPL. Using transient absorption spectroscopy, we elucidate the origin of excitons and trions that are inherently distinct for defect-mediated and impurity-mediated trions. Ferromagnetic characteristics are further confirmed by the significant Zeeman splitting of nanodiamonds deposited on the V-doped WSe2 monolayer.

5.
ACS Nano ; 15(8): 13770-13780, 2021 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-34296605

RESUMO

ReS2 exhibits strong anisotropic optical and electrical responses originating from the asymmetric lattice. Here, we show that the anisotropy of monolayer (1L) ReS2 in optical scattering and electrical transport can be practically erased by lattice engineering via lithium (Li) treatment. Scanning transmission electron microscopy revealed that significant strain is induced in the lattice of Li-treated 1L-ReS2, due to high-density electron doping and the resultant formation of continuous tiling of nanodomains with randomly rotating orientations of 60°, which produced a nearly isotropic response of polarized Raman scattering and absorption of Li-treated 1L-ReS2. With Li treatment, the in-plane conductance of 1L-ReS2 increased by an order of magnitude, and its angle dependence became negligible. Our result that the asymmetric phase was converted into the isotropic phase by electron injection could significantly expand the optoelectronic applications of polymorphic two-dimensional transition metal dichalcogenides.

6.
ACS Nano ; 13(12): 14437-14446, 2019 Dec 24.
Artigo em Inglês | MEDLINE | ID: mdl-31756072

RESUMO

Structural phase transitions in layered two-dimensional (2D) materials are of significant interest owing to their ability to exist in multiple metastable states with distinctive properties. However, phase transition in bulk MoS2 by nondestructive electron infusion has not yet been realized. In this study, we report the 2H to 1T' phase transition and in-between intermediates in bulk MoS2 using MoS2/[Ca2N]+·e- heterostructures, in which kinetic free electrons were directly injected into MoS2. We observed various phases in MoS2 ranging from heavily doped 2H to a distorted lattice state and then on to a complete 1T' state. Snapshots of the multiphase transition were captured by extraordinary Raman shift and bandgap reduction and were further elucidated by theoretical calculations. We also observed a weakening in interlayer coupling in the vicinity of the metallic regime, which led to an unusually strong photoluminescence emission, suggesting light-efficient bulk MoS2. Our results thus suggest the optoelectronic applications that can fully utilize the multiphase transition of bulk 2D materials.

7.
Light Sci Appl ; 7: 98, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30510694

RESUMO

Here, we investigate the ultrafast carrier dynamics and electronic states of exfoliated ReS2 films using time-resolved second harmonic generation (TSHG) microscopy and density functional theory (DFT) calculations. The second harmonic generation (SHG) of layers with various thicknesses is probed using a 1.19-eV beam. Up to ~13 nm, a gradual increment is observed, followed by a decrease caused by bulk interferometric light absorption. The addition of a pump pulse tuned to the exciton band gap (1.57 eV) creates a decay-to-rise TSHG profile as a function of the probe delay. The power and thickness dependencies indicate that the electron-hole recombination is mediated by defects and surfaces. The two photon absorptions of 2.38 eV in the excited state that are induced by pumping from 1.57 to 1.72 eV are restricted because these transitions highly correlate with the forbidden d-d intrasubshell orbital transitions. However, the combined usage of a frequency-doubled pump (2.38 eV) with wavelength-variant SHG probes (2.60-2.82 eV) allows us to vividly monitor the variations in TSHG profiles from decay-to-rise to rise-to-decay, which imply the existence of an additional electron absorption state (s-orbital) at an approximate distance of 5.05 eV from the highest occupied molecular orbital states. This observation was critically examined by considering the allowance of each electronic transition and a small upper band gap (~0.5 eV) using modified DFT calculations.

8.
Nanoscale ; 10(46): 21978-21984, 2018 Nov 29.
Artigo em Inglês | MEDLINE | ID: mdl-30451270

RESUMO

Molybdenum ditellurides (MoTe2) have recently attracted attention owing to their excellent structurally tunable nature between 1T'(metallic)- and 2H(semiconducting)-phases; thus, the controllable fabrication and critical identification of MoTe2 are highly desired. Here, we semi-controllably synthesized 1T'- and 2H-MoTe2 crystals using the atmospheric pressure chemical vapor deposition (APCVD) technique and studied their grain-orientation dependency using polarization-sensitive optical microscopy, Raman scattering, and second-harmonic generation (SHG) microspectroscopy. The polycrystalline 1T'-MoTe2 phase with quasi-1D "Mo-Mo" zigzag chains showed anisotropic optical absorption, leading to a clear visualization of the lattice domains. On the other hand, 2H-MoTe2 lattice grains did not exhibit any discernible difference under polarized light illumination. The combined aforementioned microscopy techniques could be used as an easy-to-access and non-destructive tool for a quick and solid identification of intended lattice orientation development in industry-scale MoTe2 crystal manufacturing.

9.
Adv Mater ; 30(14): e1705190, 2018 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-29436068

RESUMO

Understanding the collaborative behaviors of the excitons and phonons that result from light-matter interactions is important for interpreting and optimizing the underlying fundamental physics at work in devices made from atomically thin materials. In this study, the generation of exciton-coupled phonon vibration from molybdenum disulfide (MoS2 ) nanosheets in a pre-excitonic resonance condition is reported. A strong rise-to-decay profile for the transient second-harmonic generation (TSHG) of the probe pulse is achieved by applying substantial (20%) beam polarization normal to the nanosheet plane, and tuning the wavelength of the pump beam to the absorption of the A-exciton. The time-dependent TSHG signals clearly exhibit acoustic phonon generation at vibration modes below 10 cm-1 (close to the Γ point) after the photoinduced energy is transferred from exciton to phonon in a nonradiative fashion. Interestingly, by observing the TSHG signal oscillation period from MoS2 samples of varying thicknesses, the speed of the supersonic waves generated in the out-of-plane direction (Mach 8.6) is generated. Additionally, TSHG microscopy reveals critical information about the phase and amplitude of the acoustic phonons from different edge chiralities (armchair and zigzag) of the MoS2 monolayers. This suggests that the technique could be used more broadly to study ultrafast physics and chemistry in low-dimensional materials and their hybrids with ultrahigh fidelity.

10.
Nano Lett ; 17(12): 7744-7750, 2017 12 13.
Artigo em Inglês | MEDLINE | ID: mdl-29136472

RESUMO

We report on the thickness-dependent Raman spectroscopy of ultrathin silicon (Si) nanomembranes (NMs), whose thicknesses range from 2 to 18 nm, using several excitation energies. We observe that the Raman intensity depends on the thickness and the excitation energy due to the combined effects of interference and resonance from the band-structure modulation. Furthermore, confined acoustic phonon modes in the ultrathin Si NMs were observed in ultralow-frequency Raman spectra, and strong thickness dependence was observed near the quantum limit, which was explained by calculations based on a photoelastic model. Our results provide a reliable method with which to accurately determine the thickness of Si NMs with thicknesses of less than a few nanometers.

11.
J Environ Manage ; 203(Pt 1): 171-181, 2017 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-28783013

RESUMO

Green infrastructure (GI) revitalizes vegetation and soil, restores hydro-ecological processes destroyed by traditional urbanization, and naturally manages stormwater on-site, offering numerous sustainability benefits. However, despite being sustainable and despite being the object of unrelenting expert advocacy for more than two decades, GI implementation remains slow. On the other hand, the practice of traditional gray infrastructure, which is known to have significant adverse impacts on the environment, is still ubiquitous in urban areas throughout the world. This relationship between knowledge and practice seems unaccountable, which has not yet received adequate attention from academia, policy makers, or research communities. We deal with this problem in this paper. The specific objective of the paper is to explore the barriers to GI, and suggest policies that can both overcome these barriers and expedite implementation. By surveying the status of implementation in 10 US cities and assessing the relevant city, state and federal policies, we identified 29 barriers and grouped them into 5 categories. The findings show that most of the barriers stem from cognitive limitations and socio-institutional arrangements. Accordingly, we suggest 33 policies, also grouped into 5 categories, which span from conducting public education and awareness programs to changing policies and governance structures.


Assuntos
Cidades , Política Ambiental , Urbanização , Meio Ambiente , Pesquisa
12.
Nanotechnology ; 28(18): 185702, 2017 May 05.
Artigo em Inglês | MEDLINE | ID: mdl-28319028

RESUMO

Organic/inorganic hybrid structures have been widely studied because of their enhanced physical and chemical properties. Monolayers of transition metal dichalcogenides (1L-TMDs) and organic nanoparticles can provide a hybridization configuration between zero- and two-dimensional systems with the advantages of convenient preparation and strong interface interaction. Here, we present such a hybrid system made by dispersing π-conjugated organic (tris (8-hydroxyquinoline) aluminum(III)) (Alq3) nanoparticles (NPs) on 1L-MoS2. Hybrids of Alq3 NP/1L-MoS2 exhibited a two-fold increase in the photoluminescence of Alq3 NPs on 1L-MoS2 and the n-doping effect of 1L-MoS2, and these spectral and electronic modifications were attributed to the charge transfer between Alq3 NPs and 1L-MoS2. Our results suggested that a hybrid of organic NPs/1L-TMD can offer a convenient platform to study the interface interactions between organic and inorganic nano objects and to engineer optoelectronic devices with enhanced performance.

13.
Adv Mater ; 28(43): 9519-9525, 2016 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-27619888

RESUMO

An ambipolar dual-channel field-effect transistor (FET) with a WSe2 /MoS2 heterostructure formed by separately controlled individual channel layers is demonstrated. The FET shows a switchable ambipolar behavior with independent carrier transport of electrons and holes in the individual layers of MoS2 and WSe2 , respectively. Moreover, the photoresponse is studied at the heterointerface of the WSe2 /MoS2 dual-channel FET.

14.
J Trop Med ; 2016: 4230235, 2016.
Artigo em Inglês | MEDLINE | ID: mdl-27047548

RESUMO

Background. Leprosy is one of the most stigmatized diseases known today. The stigma surrounding leprosy can be a major burden and affects many dimensions of a person's life, including intimate relationships. We aimed to investigate the experiences of women affected by leprosy regarding marital life and sexuality, comparing these to the experiences of women with other physical disabilities and to those of able-bodied women in South-East Nepal. Methods. This study used a qualitative approach and a cross-sectional, nonrandom survey design. Thirty women underwent in-depth interviews about their marital and sexual relationship by means of a semi-structured interview guide. These thirty women included ten women affected by leprosy, ten women with other physical disabilities, and ten able-bodied women living in South-East Nepal. Results. We found that many women faced violence and abuse in their marriages. However, women affected by leprosy appeared to face more problems with regard to their marital and sexual relationships than women with physical disabilities and able-bodied women. Some of these related to the fear of leprosy. Conclusions. Further research is recommended to investigate the extent of this problem and ways to ameliorate the situation of the affected women. Education and counselling at diagnosis may help prevent many of the problems reported.

15.
Environ Manage ; 57(5): 1112-24, 2016 May.
Artigo em Inglês | MEDLINE | ID: mdl-26837617

RESUMO

Traditional urban stormwater management involves rapid removal of stormwater through centralized conveyance systems of curb-gutter-pipe networks. This results in many adverse impacts on the environment including hydrological disruption, groundwater depletion, downstream flooding, receiving water quality degradation, channel erosion, and stream ecosystem damage. In order to mitigate these adverse impacts, urban stormwater managers are increasingly using green infrastructure that promote on-site infiltration, restore hydrological functions of the landscape, and reduce surface runoff. Existing stormwater governance, however, is centralized and structured to support the conventional systems. This governance approach is not suited to the emerging distributed management approach, which involves multiple stakeholders including parcel owners, government agencies, and non-governmental organizations. This incongruence between technology and governance calls for a paradigm shift in the governance from centralized and technocratic to distributed and participatory governance. This paper evaluates how five US cities have been adjusting their governance to address the discord. Finally, the paper proposes an alternative governance model, which provides a mechanism to involve stakeholders and implement distributed green infrastructure under an integrative framework.


Assuntos
Cidades , Conservação dos Recursos Naturais/métodos , Política Ambiental , Chuva , Qualidade da Água , Ecossistema , Monitoramento Ambiental , Inundações , Illinois , Modelos Teóricos , New York , Oregon , Pennsylvania , Washington
16.
Nanoscale ; 6(21): 13028-35, 2014 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-25247614

RESUMO

We performed a nanoscale confocal absorption spectral imaging to obtain the full absorption spectra (over the range 1.5-3.2 eV) within regions having different numbers of layers and studied the variation of optical transition depending on the atomic thickness of the MoS2 film. Three distinct absorption bands corresponding to A and B excitons and a high-energy background (BG) peak at 2.84 eV displayed a gradual redshift as the MoS2 film thickness increased from the monolayer, to the bilayer, to the bulk MoS2 and this shift was attributed to the reduction of the gap energy in the Brillouin zone at the K-point as the atomic thickness increased. We also performed n-type chemical doping of MoS2 films using reduced benzyl viologen (BV) and the confocal absorption spectra modified by the doping showed a strong dependence on the atomic thickness: A and B exciton peaks were greatly quenched in the monolayer MoS2 while much less effect was shown in larger thickness and the BG peak either showed very small quenching for 1 L MoS2 or remained constant for larger thicknesses. Our results indicate that confocal absorption spectral imaging can provide comprehensive information on optical transitions of microscopic size intrinsic and doped two-dimensional layered materials.

17.
J Biomed Opt ; 19(5): 051210, 2014 May.
Artigo em Inglês | MEDLINE | ID: mdl-24407597

RESUMO

We demonstrate a simple method of stretching DNA to its full length, suitable for optical imaging and atomic force microscopy (AFM). Two competing forces on the DNA molecules, which are the electrostatic attraction between positively charged dye molecules (YOYO-1) intercalated into DNA and the negatively charged surface of glass substrate, and the centrifugal force of the rotating substrate, are mainly responsible for the effective stretching and the dispersion of single strands of DNA. The density of stretched DNA molecules could be controlled by the concentration of the dye-stained DNA solution. Stretching of single DNA molecules was confirmed by AFM imaging and the photoluminescence spectra of single DNA molecule stained with YOYO-1 were obtained, suggesting that our method is useful for spectroscopic analysis of DNA at the single molecule level.


Assuntos
DNA/química , Microscopia de Fluorescência/métodos , Espectrometria de Fluorescência/métodos , Benzoxazóis/química , Feminino , Corantes Fluorescentes/química , Vidro , Humanos , Microscopia de Força Atômica , Microscopia de Fluorescência/instrumentação , Imagem Molecular/instrumentação , Imagem Molecular/métodos , Placenta/química , Gravidez , Compostos de Quinolínio/química , Espectrometria de Fluorescência/instrumentação
18.
Lepr Rev ; 78(1): 70-9, 2007 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-17518099

RESUMO

OBJECTIVE: To evaluate the use of the ML Flow test as an additional, serological, tool for the classification of new leprosy patients. DESIGN: In Brazil, Nepal and Nigeria, 2632 leprosy patients were classified by three METHODS: : (1) as multibacillary (MB) or paucibacillary (PB) according to the number of skin lesions (WHO classification), (2) by slit skin smear examination, and (3) by serology using the ML Flow test detecting IgM antibodies to Mycobacterium leprae-specific phenolic glycolipid-I. RESULTS: The proportion of MB leprosy patients was 39.5, 35.6 and 19.4% in Brazil, Nepal and Nigeria, respectively. The highest seropositivity in patients was observed in Nigeria (62.9%), followed by Brazil (50.8%) and Nepal (35.6%). ML Flow test results and smears were negative in 69.1 and 82.7% of PB patients, while smears were positive in 58.6% of MB patients in Brazil and 28.3% in Nepal. In MB patients, both smears and ML Flow tests were negative in 15.6% in Brazil and 38.3%, in Nepal. Testing all PB patients with the ML Flow test to prevent under-treatment would increase the MB group by 18, 11 and 46.2% for Brazil, Nepal and Nigeria, respectively. Using the ML Flow test as the sole criterion for classification would result in an increase of 11.3 and 43.5% of patients requiring treatment for MB leprosy in Brazil and Nigeria, respectively, and a decrease of 3.7% for Nepal. CONCLUSIONS: The ML Flow test could be used to strengthen classification, reduce the risk of under-treatment and minimize the need for slit skin smears.


Assuntos
Anticorpos Antibacterianos/sangue , Hanseníase/diagnóstico , Técnicas de Diagnóstico Molecular , Sistemas Automatizados de Assistência Junto ao Leito , Antígenos de Bactérias/imunologia , Brasil , Glicolipídeos/imunologia , Humanos , Imunoglobulina M/sangue , Mycobacterium leprae/imunologia , Nepal , Nigéria , Sensibilidade e Especificidade
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