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1.
J Phys Chem Lett ; 14(41): 9200-9206, 2023 Oct 19.
Artículo en Inglés | MEDLINE | ID: mdl-37801730

RESUMEN

Two-dimensional (2D) transition metal dichalcogenides (TMDCs) are ideal platforms for exploring excitonic physics because of the tightly bound excitons. In this work, we observed the onset of band-edge exciton formation in monolayer MoS2 (WS2) and bilayer MoS2-WS2 by measuring the transient optical response upon excitation with ultrashort laser pulses. In addition to wavelength dependence on excitation under nonresonant excitation, we found that the onset of band-edge exciton formation in monolayer MoS2 (WS2) pumped in the exciton state is significantly faster than that with pumping in the nonexciton state, which could be attributed to the effective transition between exciton states induced by the excitonic effect. Besides, the onset of band-edge exciton formation in van der Waals heterostructures is similar to that for monolayer TMDCs regardless of charge transfer at the interface. Our work contributes to a better understanding of exciton dynamics in 2D TMDCs, providing a solid basis of the rational design of the 2D optoelectronic applications based on TMDCs.

2.
Adv Sci (Weinh) ; 10(26): e2302554, 2023 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-37395386

RESUMEN

2D lead halide perovskites (LHPs) show strong excitonic and spin-orbit coupling effects, generating a facile spin injection. Besides, they possess a polaron character due to the soft crystal lattice, which can prolong the spin lifetime, making them favorable materials for spintronic applications. Here, the spin dynamics of 2D PEA2 PbI4 (MAPbI3 )n -l thin films with different layers by temperature- and pump fluence-dependent circularly polarization-resolved transient absorption (TA) measurements is studied. These results indicate that the spin depolarization mechanism is gradually converted from the Maialle-Silva-Sham (MSS) mechanism to the polaronic states protection mechanism with the layer number increasing from = 1 to 3, which is determined by the interplay between the strength of Coulomb exchange interaction and the strength of polaronic effect. While for ≥ 4, the Elliot-Yafet (EY) impurities mechanism is proposed, in which the formed polaronic states with free charge carriers no longer play the protective role.

3.
Hepatobiliary Pancreat Dis Int ; 22(1): 54-63, 2023 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-36041973

RESUMEN

BACKGROUND: Hepatocellular carcinoma (HCC) is the fourth leading cause of cancer-related death worldwide. Due to the high prevalence of hepatitis B virus (HBV) infection in China, the incidence of HCC in China is high, and liver cirrhosis caused by chronic hepatitis also brings great challenges to treatment. This paper reviewed the latest research progress on minimally invasive treatments for HCC, including percutaneous thermal ablation and new nonthermal ablation techniques, and introduced the principles, advantages, and clinical applications of various therapeutic methods in detail. DATA SOURCES: The data of treatments for HCC were systematically collected from the PubMed, ScienceDirect, American Chemical Society and Web of Science databases published in English, using "minimally invasive" and "hepatocellular carcinoma" or "liver cancer" as the keywords. RESULTS: Percutaneous thermal ablation is still a first-line strategy for the minimally invasive treatment of HCC. The effect of microwave ablation (MWA) on downgrading treatment before liver transplantation is better than that of radiofrequency ablation (RFA), while RFA is more widely used in the clinical practice. High-intensity focused ultrasound (HIFU) is mainly used for the palliative treatment of advanced liver cancer. Electrochemotherapy (ECT) delivers chemotherapeutic drugs to the target cells while reducing the blood supply around HCC. Irreversible electroporation (IRE) uses a microsecond-pulsed electric field that induces apoptosis and necrosis and triggers a systemic immune response. The nanosecond pulsed electric field (nsPEF) has achieved a good response in the ablation of mice with HCC, but it has not been reported in China for the treatment of human HCC. CONCLUSIONS: A variety of minimally invasive treatments provide a sufficient survival advantage for HCC patients. Nonthermal ablation will lead to a new wave with its unique advantage of antitumor recurrence and metastasis.


Asunto(s)
Técnicas de Ablación , Carcinoma Hepatocelular , Ablación por Catéter , Neoplasias Hepáticas , Ablación por Radiofrecuencia , Humanos , Animales , Ratones , Carcinoma Hepatocelular/patología , Neoplasias Hepáticas/patología , Técnicas de Ablación/efectos adversos , Técnicas de Ablación/métodos , Ablación por Catéter/efectos adversos , Ablación por Catéter/métodos , Resultado del Tratamiento
4.
Phys Chem Chem Phys ; 24(27): 16538-16544, 2022 Jul 13.
Artículo en Inglés | MEDLINE | ID: mdl-35788232

RESUMEN

Excitonic devices based on two-dimensional (2D) transition metal dichalcogenides (TMDCs) can combine spintronics with valleytronics due to its special energy band structure. In this work, we studied the generation and relaxation processes of spin/valley polarized excitons dynamics in monolayer WSe2 and its van der Waals (vdW) heterojunction with graphene using a circularly polarized femtosecond pump-probe system. The spin/valley depolarization dynamics of the A exciton in monolayer WSe2 is found to exhibit a biexponential decay. The fast relaxation process is due to the ultrafast intervalley electron-hole spin-flip exchange coupling and electron-phonon scattering. And the slow relaxation process originates from the recombination and relaxation of the trion states. Graphene has an electron extraction effect on WSe2, which prevents the formation of trions. Therefore, the spin/valley depolarization process of the A exciton in the heterojunction exhibits only a fast relaxation process. In both monolayer WSe2 and its heterojunction with graphene, B/A' excitons exhibit a negative spin/valley polarization which is mainly due to two-photon absorption and excited Bose scattering. Our work systematically studied the spin/valley depolarization dynamics of excitons and revealed possible mechanisms of their differences in isolated 2D WSe2 and vdW heterojunctions.

5.
J Phys Chem Lett ; 13(24): 5501-5507, 2022 Jun 23.
Artículo en Inglés | MEDLINE | ID: mdl-35695739

RESUMEN

The appearance of van der Waals heterostructures offers a new solution to valleytronics. Here, we observe the spin-valley depolarization process of electrons and holes in type-II MoS2-WSe2 heterostructures simultaneously for the first time by valley-resolved broad-band femtosecond pump-probe experiments. The different depolarization paths between electrons and holes make them have different spin-valley polarization lifetimes. The spin-valley depolarization pathway of holes is mainly dominated by a phonon-assisted intervalley scattering process, while intra- and intervalley coupling can trigger additional depolarization pathways for electrons. The hole polarization lifetime can be further prolonged to more than three times in trilayer heterostructure 2MoS2-WSe2. For MoS2-WS2 that has strong orbital hybridization of Mo and W atoms, both electrons and holes lose the spin-valley polarization extremely soon after charge separation, behaving similarly to intraexcitons in a monolayer. Our work advances the basic understanding of spin-valley depolarization of van der Waals heterostructures and facilitates the effort toward longer lifetime valleytronic devices for information transfer and storage applications.

6.
Mil Med Res ; 9(1): 32, 2022 06 17.
Artículo en Inglés | MEDLINE | ID: mdl-35715833

RESUMEN

BACKGROUND: Due to the outbreak and rapid spread of coronavirus disease 2019 (COVID-19), more than 160 million patients have become convalescents worldwide to date. Significant alterations have occurred in the gut and oral microbiome and metabonomics of patients with COVID-19. However, it is unknown whether their characteristics return to normal after the 1-year recovery. METHODS: We recruited 35 confirmed patients to provide specimens at discharge and one year later, as well as 160 healthy controls. A total of 497 samples were prospectively collected, including 219 tongue-coating, 129 stool and 149 plasma samples. Tongue-coating and stool samples were subjected to 16S rRNA sequencing, and plasma samples were subjected to untargeted metabolomics testing. RESULTS: The oral and gut microbiome and metabolomics characteristics of the 1-year convalescents were restored to a large extent but did not completely return to normal. In the recovery process, the microbial diversity gradually increased. Butyric acid-producing microbes and Bifidobacterium gradually increased, whereas lipopolysaccharide-producing microbes gradually decreased. In addition, sphingosine-1-phosphate, which is closely related to the inflammatory factor storm of COVID-19, increased significantly during the recovery process. Moreover, the predictive models established based on the microbiome and metabolites of patients at the time of discharge reached high efficacy in predicting their neutralizing antibody levels one year later. CONCLUSIONS: This study is the first to characterize the oral and gut microbiome and metabonomics in 1-year convalescents of COVID-19. The key microbiome and metabolites in the process of recovery were identified, and provided new treatment ideas for accelerating recovery. And the predictive models based on the microbiome and metabolomics afford new insights for predicting the recovery situation which benefited affected individuals and healthcare.


Asunto(s)
COVID-19 , Microbioma Gastrointestinal , Estudios de Seguimiento , Humanos , Metabolómica , ARN Ribosómico 16S/genética
7.
J Phys Chem Lett ; 13(18): 4073-4081, 2022 May 12.
Artículo en Inglés | MEDLINE | ID: mdl-35499477

RESUMEN

The interaction between organic cations and inorganic metal halide octahedral units strongly affects the properties of organic-inorganic hybrid metal halides. The "soft" property of the lattice provides the possibility of its strong exciton-phonon interaction. Here we report one-dimensional (1D) lead-free chiral organic-inorganic hybrid metal halide single crystals of (R/S)-methylbenzylamine bismuth iodide (R/S-MBA)2Bi2I8, which exhibits a high level of octahedral bond distortion. The introduction of chiral amines leads to a strong chiroptical response in the range of 200-600 nm. The strong exciton-phonon coupling can be observed through the coherent oscillation spectrum of transient absorption dynamics at room temperature. The coherent phonon oscillation frequencies are ∼97 and ∼130 cm-1, corresponding to the symmetrical stretching or bending of the Bi-I octahedron. Our work provides new insights for the study of exciton-phonon coupling in 1D chiral hybrid metal halides.

8.
Hepatol Int ; 16(3): 649-657, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35412215

RESUMEN

AIMS: To evaluate the efficiency of ultrasonic spleen thickness (UST), routine variables and (expanded) Baveno VI criteria for high-risk gastroesophageal varices (HRGOV) detection in cirrhotic patients. METHODS: In total, 305 cirrhotic patients were retrospectively enrolled in the deriving cohort and 328 cirrhotic patients with hepatitis B sustained viral response were prospectively enrolled in the validation cohort. HRGOV was defined as medium and severe gastroesophageal varices (GOV), mild GOV with red signs or Child-Pugh C. The cut-offs for HRGOV were determined by likelihood ratio indicating strong evidences. Algorithms of Spleen thickness-Age-Liver stiffness measurement (LSM, by Fibroscan®)-Albumin (SALA) and Spleen thickness-Platelet-Albumin (SPA) were derived by multivariate analyses. RESULTS: The area under receiver operating characteristics curve of SALA, SPA, UST, platelet, and LSM were 0.849, 0.835, 0.808, 0.746, and 0.655 in the deriving cohort, and improved to 0.901, 0.904, 0.858, 0.876, and 0.811 in the validation cohort, respectively. While SALA, SPA, UST, platelet, Baveno VI criteria (BVI), and expanded BVI spared 46.6%, 38.0%, 29.2%, 21.0%, 12.1%, and 23.6% esophagogastroduodenoscopy in the deriving cohort, these numbers were improved to 68.1%, 66.8%, 27.1%, 37.8%, 36.0%, and 61.0% in the validating cohort, respectively; however, the negative likelihood ratio of expanded BVI was up to 0.16. SPA spared less esophagogastroduodenoscopy than SALA, which can be supplemented by stepwise applying UST and SPA. Sequentially combining UST and SALA, BVI and SALA exempted additional 10-5% endoscopies. CONCLUSIONS: SPA, without LSM, improves HRGOV detection comparing with BVI. UST based algorithms combination can achieve the best efficiency especially in sustained virus response hepatitis B.


Asunto(s)
Diagnóstico por Imagen de Elasticidad , Várices Esofágicas y Gástricas , Hepatitis B , Várices , Albúminas , Várices Esofágicas y Gástricas/diagnóstico por imagen , Várices Esofágicas y Gástricas/patología , Hepatitis B/complicaciones , Hepatitis B/diagnóstico por imagen , Virus de la Hepatitis B , Humanos , Cirrosis Hepática/complicaciones , Cirrosis Hepática/diagnóstico por imagen , Recuento de Plaquetas , Estudios Retrospectivos , Bazo/diagnóstico por imagen , Bazo/patología , Ultrasonido , Várices/patología
9.
Nucleic Acids Res ; 50(4): 2005-2018, 2022 02 28.
Artículo en Inglés | MEDLINE | ID: mdl-35137179

RESUMEN

The second cell fate decision in the early stage of mammalian embryonic development is pivotal; however, the underlying molecular mechanism is largely unexplored. Here, we report that Prmt1 acts as an important regulator in primitive endoderm (PrE) formation. First, Prmt1 depletion promotes PrE gene expression in mouse embryonic stem cells (ESCs). Single-cell RNA sequencing and flow cytometry assays demonstrated that Prmt1 depletion in mESCs contributes to an emerging cluster, where PrE genes are upregulated significantly. Furthermore, the efficiency of extraembryonic endoderm stem cell induction increased in Prmt1-depleted ESCs. Second, the pluripotency factor Klf4 methylated at Arg396 by Prmt1 is required for recruitment of the repressive mSin3a/HDAC complex to silence PrE genes. Most importantly, an embryonic chimeric assay showed that Prmt1 inhibition and mutated Klf4 at Arg 396 induce the integration of mouse ESCs into the PrE lineage. Therefore, we reveal a regulatory mechanism for cell fate decisions centered on Prmt1-mediated Klf4 methylation.


Asunto(s)
Embrión de Mamíferos/metabolismo , Endodermo , Proteína-Arginina N-Metiltransferasas/metabolismo , Animales , Diferenciación Celular , Desarrollo Embrionario , Endodermo/metabolismo , Femenino , Factor 4 Similar a Kruppel/metabolismo , Ratones , Células Madre Embrionarias de Ratones , Embarazo
10.
Front Radiol ; 2: 1036026, 2022.
Artículo en Inglés | MEDLINE | ID: mdl-37492681

RESUMEN

Purpose: To analyze the safety and feasibility of computed tomography (CT)-guided thermal ablation of multiple pulmonary nodules combined with intraoperative biopsy. Methods: The data of 431 patients with 540 lung nodules undergoing CT-guided biopsy or ablation were retrospectively analyzed. Biopsy-only group (A): 107 patients (107 lesions) received CT-guided percutaneous lung biopsy only; Ablation-only group (B): 117 cases (117 lesions) only received CT-guided thermal ablation; Single focal ablation combined with biopsy group (C): 103 patients (103 lesions) received CT-guided thermal ablation combined with intraoperative immediate biopsy; Multifocal ablation combined with biopsy group (D): 104 patients (213 lesions) received CT-guided thermal ablation combined with intraoperative biopsy. The success rate of this technique was calculated, the complications were recorded, and the positive rate of pathological diagnosis of the specimens was evaluated (the tissue specimens could be confirmed as positive by pathological diagnosis). Results: All 431 patients with pulmonary nodules successfully completed the operation, and the technical success rate was 100% (431/431). In group A, hemoptysis occurred in seven cases after operation, while no hemoptysis was observed in the other groups. Pneumothorax occurred in 8 cases in group A, 14 cases in group B, 11 cases in group C, and 13 cases in group D. Hydrothorax occurred in 4 cases in group A, 7 cases in group B, 5 cases in group C and 9 cases in group D, and there were no significant differences between the groups. The positive rate of pathological diagnosis was 84.1% (90/107) in group A, 81.5% (84/103) in group C, and 82.6% (176/213) in group D, and there was no significant difference among the groups (P > 0.05). A total of 15 cases in group C and 23 cases in group D underwent gene testing and analysis, and the biopsy tissue samples all met quality control standards. Conclusion: CT-guided thermal ablation of multiple pulmonary nodules combined with intraoperative biopsy does not prolong the length of hospital stay or increase the risk of postoperative complications. It can meet the requirements of clinical, pathological and genetic testing, and is safe and reliable.

12.
Nanoscale ; 13(40): 17093-17100, 2021 Oct 21.
Artículo en Inglés | MEDLINE | ID: mdl-34623366

RESUMEN

Monolayer transition metal dichalcogenide quantum dots (TMDC QDs) could exhibit unique photophysical properties, because of both lateral quantum confinement effect and edge effect. However, there is little fundamental study on the quantum-confined exciton dynamics in monolayer TMDC QDs, to date. Here, by selective excitations of monolayer WS2 QDs in broadband transient absorption (TA) spectroscopy experiments, the excitation-wavelength-dependent ground state bleaching signals corresponding to the quantum-confined exciton states are directly observed. Compared to the time-resolved photophysical properties of WS2 nanosheets, the selected monolayer WS2 QDs only show one ground state bleaching peak with larger initial values for the linear polarization anisotropy of band-edge excitons, probably due to the expired spin-orbit coupling. This suggests a complete change of the band structure for monolayer WS2 QDs. In the femtosecond time-resolved circular polarization anisotropy experiments, a valley depolarization time of ∼100 fs is observed for WS2 nanosheets at room temperature, which is not observed for monolayer WS2 QDs. Our findings suggest a strong state-mixing of band-edge valley excitons responsible for the large linear polarization in monolayer WS2 QDs, which could be helpful for understanding the exciton relaxation mechanisms in colloidal monolayer TMDC QDs.

13.
Phys Chem Chem Phys ; 23(39): 22430-22436, 2021 Oct 13.
Artículo en Inglés | MEDLINE | ID: mdl-34585679

RESUMEN

Since excitonic quasiparticles, including excitons, trions and charges, have a great influence on the photoelectric characteristics of two-dimensional (2D) transition metal dichalcogenides (TMDs), systematic explorations of the trion dynamics and charge photogeneration in 2D TMDs are important for their future optoelectronic applications. Here, broadband femtosecond transient absorption spectroscopic experiments are performed first to investigate the peak shifting and broadening kinetics in MoS2 nanosheets in solution prepared by liquid phase exfoliation (LPE-MoS2, ∼9 layers, 9L), which reveal that the binding energies for the A-, B-, and C-exciton states are ∼77 meV, ∼76 meV, and -70 meV (the energy difference between free charges and excitons; the negative sign for C-excitons means a spontaneous dissociation nature in band-nesting regions), respectively. Then, the trion dynamics and charge photogeneration in LPE-MoS2 nanosheets have been studied in detail, demonstrating that they are comparable to those in chemical vapor deposition grown MoS2 films (1L-, 3L- and 7L-MoS2). These experimental results suggest that LPE-TMD nanosheets also have the potential for use in charge-related optoelectronic devices based on 2D TMDs.

14.
Nanoscale ; 13(33): 14081-14088, 2021 Sep 07.
Artículo en Inglés | MEDLINE | ID: mdl-34477689

RESUMEN

Strain is one of the effective ways to modulate the band structure of monolayer transition metal dichalcogenides (TMDCs), which has been reported in theoretical and steady-state spectroscopic studies. However, the strain effects on the charge transfer processes in TMDC heterostructures have not been experimentally addressed thus far. Here, we systematically investigate the strain-mediated transient spectral evolutions corresponding to excitons at band-edge and higher energy states for monolayer MoS2 and monolayer WSe2. It is demonstrated that Γ and K valleys in monolayer WSe2 and monolayer MoS2 present different strain responses, according to the broadband femtosecond pump-probe experimental results. It is further observed that the resulting band offset changes tuned by applied tensile strains in MoS2-WSe2 heterostructures would not affect the band-edge electron transfer profiles, where only monolayer WSe2 is excited. From a flexible optoelectronic applications perspective, the robust charge transfer under strain engineering in TMDC heterostructures is very advantageous.

15.
Dalton Trans ; 50(29): 10237-10242, 2021 Jul 27.
Artículo en Inglés | MEDLINE | ID: mdl-34241613

RESUMEN

In this work, a novel multichromic cationic coordination polymer, named [Zn4(BTC)3(bcbpy)2]·5H2O (1), based on a new flexible viologen ligand 1,1'-bis(3-cyanobenzyl)-[4,4'-bipyridine]-1,1'-diium (H2bcbpy·2Cl), Zn(NO3)2·6H2O and pyromellitic acid (H4BTC) was synthesized. Compound 1 has good photosensitive activity and can respond to sunlight at room temperature. The colour of compound 1 changes rapidly in response to UV light and blue ray irradiation within 5 s. We rarely obtained the crystal structures after irradiation under UV light and blue ray. At the same time, compound 1 shows the hydrochromism phenomenon when heated at 120 °C, and it also shows the ability of detecting aniline and NO2- under low-concentration conditions (10-4 M).

16.
Prenat Diagn ; 41(6): 766-771, 2021 May.
Artículo en Inglés | MEDLINE | ID: mdl-33782977

RESUMEN

OBJECTIVE: To review the prenatal and postnatal clinical characteristics and pathological subtypes, as well as the surgical outcome for congenital mesoblastic nephroma (CMN) cases. METHOD: A retrospective review was performed in 11 cases with CMN prenatally diagnosed at a single center between 2015 and 2019. The clinical characteristics, surgical outcome, histopathology, and follow-up were retrospectively obtained and reviewed. RESULTS: The median gestational age at which the sonographic diagnosis was made was 35 weeks. Polyhydramnios was found in four (36.4%) cases, and all resulted in a preterm birth. Nine infants had hypertension. Ten cases underwent radical nephrectomy, and one underwent radical nephrectomy and partial adrenalectomy. The pathological results showed that six tumors were classical variants, four mixed variants, and one was a cellular variant. Three cases presented as a stage I, eight as stage II, and no stage III or IV cases were diagnosed. All patients are alive so far. At a median follow-up of 14 months, no local recurrence, or remote metastases were found. CONCLUSION: The prognosis of prenatal CMN cases is excellent after early surgery.


Asunto(s)
Nefroma Mesoblástico/diagnóstico , Nefroma Mesoblástico/terapia , Adulto , China/epidemiología , Femenino , Humanos , Recién Nacido , Riñón/patología , Riñón/fisiopatología , Imagen por Resonancia Magnética/métodos , Nefroma Mesoblástico/epidemiología , Embarazo , Diagnóstico Prenatal/métodos , Diagnóstico Prenatal/estadística & datos numéricos , Pronóstico , Estudios Retrospectivos
17.
Intervirology ; 64(2): 69-80, 2021.
Artículo en Inglés | MEDLINE | ID: mdl-33709967

RESUMEN

OBJECTIVE: To investigate the relationship between hematologic tumors and Epstein-Barr virus (EBV)-encoded small noncoding RNA (EBER) variations as well as latent membrane protein 1 (LMP1) variations. METHODS: Patients with leukemia and myelodysplastic syndrome (MDS) were selected as subjects. Genotypes 1/2 and genotypes F/f were analyzed using the nested PCR technology, while EBER and LMP1 subtypes were analyzed by the nested PCR and DNA sequencing. RESULTS: Type 1 was more dominant than type 2, found in 59 out of 82 (72%) leukemia and in 31 out of 35 (88.6%) MDS, while type F was more prevalent than type f in leukemia (83/85, 97.6%) and MDS (29/31, 93.5%) samples. The distribution of EBV genotypes 1/2 was not significantly different among leukemia, MDS, and healthy donor groups, neither was that of EBV genotypes F/f. EB-6m prototype was the dominant subtype of EBER in leukemia and MDS (73.2% [30/41] and 83.3% [10/12], respectively). The frequency of EB-6m was lower than that of healthy people (96.7%, 89/92), and the difference was significant (p < 0.05). China 1 subtype was the dominant subtype of LMP1 in leukemia and MDS (70% [28/40] and 90% [9/10], respectively), and there was no significant difference in the distribution of LMP1 subtypes among the 3 groups (p > 0.05). CONCLUSION: The distribution of EBV 1/2, F/f, EBER, and LMP1 subtypes in leukemia and MDS was similar to that in the background population in Northern China, which means that these subtypes may be rather region-restricted but not associated with leukemia and MDS pathogenesis.


Asunto(s)
Infecciones por Virus de Epstein-Barr , Neoplasias Hematológicas , ARN Pequeño no Traducido , China/epidemiología , Infecciones por Virus de Epstein-Barr/epidemiología , Herpesvirus Humano 4/genética , Humanos , Proteínas de la Membrana , ARN Viral , Proteínas de la Matriz Viral
18.
Nanotechnology ; 32(13)2021 Jan 08.
Artículo en Inglés | MEDLINE | ID: mdl-33427201

RESUMEN

Band renormalization effects play a significant role for two-dimensional (2D) materials in designing a device structure and customizing their optoelectronic performance. However, the intrinsic physical mechanism about the influence of these effects cannot be revealed by general steady-state studies. Here, band renormalization effects in organic superacid treated monolayer MoS2, untreated monolayer MoS2and few-layer MoS2are quantitatively analyzed by using broadband femtosecond transient absorption spectroscopy. In comparison with the untreated monolayer, organic superacid treated monolayer MoS2maintains a direct bandgap structure with two thirds of carriers populated at K valley, even when the initial exciton density is as high as 2.05 × 1014cm-2(under 400 nm excitations). While for untreated monolayer and few-layer MoS2, many-particle induced band renormalizations lead to a stronger imbalance for the carrier population between K and Q valleys inkspace, and the former experiences a direct-to-indirect bandgap transition when the initial exciton density exceeds 5.0 × 1013cm-2(under 400 nm excitations). Those many-particle induced band renormalization processes further suggest a band-structure-controlling method in practical 2D devices.

19.
J Phys Chem Lett ; 11(22): 9649-9655, 2020 Nov 19.
Artículo en Inglés | MEDLINE | ID: mdl-33125851

RESUMEN

Understanding and controlling the charge transfer processes of two-dimensional (2D) materials are fundamental for the optimized device performance based on 2D semiconductors and heterostructures. The charge transfer rate is very robust in transition metal disulfide (TMD) heterostructures with type II band alignments, which can be manipulated by intercalating a dielectric layer like hBN to isolate the donor and acceptor monolayers. This study shows that there is an alternative way to change the electron transfer and recombination rates in the case of nLMoS2/mLWSe2 multilayer heterostructures, where the donor-acceptor distance is maintained, but the rate of electron transfer is strongly layer dependent and shows asymmetry for the layer number of donor and acceptor monolayers. Especially, the 1LMoS2/2LWSe2 heterostructure slows electron transfer and charge recombination rates ∼2.3 and ∼12 times that of the 1LMoS2/1LWSe2 heterostructure, respectively, which have been competitive with that in the 1LMoS2/hBN/1LWSe2 heterostructure. From an application perspective, the noninterfacial electron transfer in which photogenerated electrons should across more than one atomically thin layer is not favorable due to the built-in electric field established by the initial interfacial electron transfer.

20.
J Phys Chem Lett ; 11(4): 1483-1489, 2020 Feb 20.
Artículo en Inglés | MEDLINE | ID: mdl-32017570

RESUMEN

It is well-established that the electronic states of graphene oxide (GO) consist of sp2 clusters with different sizes and the surrounding sp3 matrix according to recent reports. However, addressing the excitation energy migration/redistribution among those electronic states in GO-based complex systems from spectroscopic experiments is still a challenge. Here, we combine the time-resolved absorption and fluorescence depolarization experiments to reveal the excitation energy migration processes in electronic states in GO. We demonstrate that, in sp3 domains of GO, there are charge-transfer states between sp3-hybridized carbon atoms and the oxygen-containing functional groups, and the energy redistribution and charge migration in sp3 matrix occur on the time scale from subpicoseconds to tens of picoseconds. In contrast, the electronic states of sp2 clusters in GO are rather localized and dominantly contribute to the excitation-wavelength-dependent red fluorescence of GO.

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