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1.
Microb Pathog ; 179: 106109, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37040845

RESUMO

Human Cytomegalovirus (HCMV) infection is associated with bad obstetric history (BOH) and adverse pregnancy outcomes (APO). Here, we characterized antiviral humoral profiles, systemic and virus specific cellular immune responses concurrently in pregnant women (n = 67) with complications including BOH and associated these signatures with pregnancy outcomes. Infection status was determined using nested blood PCR, seropositivity and IgG avidity by ELISA. Systemic and HCMV specific (pp65) cellular immune responses were evaluated by flow cytometry. Seropositivity was determined for other TORCH pathogens (n = 33) on samples with recorded pregnancy outcomes. This approach was more sensitive in detecting HCMV infection. Blood PCR positive participants, irrespective of their IgG avidity status, had higher cytotoxic potential in circulating CD8+ T cells (p < 0.05) suggesting that infection associated cellular dysfunction was uncoupled with avidity maturation of antiviral humoral responses. Also, impaired anamnestic degranulation of HCMV-pp65-specific T cells compared to HCMV blood PCR negative participants (p < 0.05) was observed. APO correlated with HCMV blood PCR positivity but not serostatus (p = 0.0039). Most HCMV IgM positive participants (5/6) were HCMV blood PCR positive with APO. None were found to be IgM positive for other TORCH pathogens. Multiple TORCH seropositivity however was significantly enriched in the APO group (p = 0.024). Generation of HCMV specific high avidity IgG antibodies had no bearing on APO (p = 0.9999). Our study highlights the utility of an integrated screening approach for antenatal HCMV infection in the context of BOH, where infection is associated with systemic and virus specific cellular immune dysfunction as well as APO.


Assuntos
Infecções por Citomegalovirus , Complicações Infecciosas na Gravidez , Gravidez , Humanos , Feminino , Resultado da Gravidez , Gestantes , Infecções por Citomegalovirus/diagnóstico , Linfócitos T CD8-Positivos , Monitorização Imunológica , Citomegalovirus , Anticorpos Antivirais , Imunoglobulina G , Imunoglobulina M
2.
J Phys Chem Lett ; 13(45): 10543-10549, 2022 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-36342415

RESUMO

Nanosized molecular clusters (MCs) composed of PbBr2 and neutral ligand butylamine (BTYA) with unique optical properties in solution and solid states have been synthesized using ligand-assisted reprecipitation and spin-coating, separately. The studies of their optical properties using ultraviolet-visible (UV-vis) absorption and photoluminescence (PL) show the first electronic absorption and PL band of the MCs at 401 and 411 nm, respectively, for the solution and solid state samples that exhibit good stability under ambient conditions. Low-temperature PL spectra below 30 K show vibronic peaks indicative of a single size or a very narrow size distribution of the MCs. On the basis of Raman, X-ray diffraction, and transmission electron microscopy measurements, a layered structural model is proposed for the MCs with a BTYA ligand capping on the surface of the corner-shared tilted [PbBr6]4- octahedral framework. The stable and retained structure of MCs in the solid state is promising for photonics applications.


Assuntos
Ligantes , Difração de Raios X , Microscopia Eletrônica de Transmissão
3.
iScience ; 25(2): 103737, 2022 Feb 18.
Artigo em Inglês | MEDLINE | ID: mdl-35118357

RESUMO

Utilizing hot electrons generated from localized surface plasmon resonance is of widespread interest in the photocatalysis of metallic nanoparticles. However, hot holes, especially generated from interband transitions, have not been fully explored for photocatalysis yet. In this study, a photocatalyzed Suzuki-Miyaura reaction using mesoporous Pd nanoparticle photocatalyst served as a model to study the role of hot holes. Quantum yields of the photocatalysts increase under shorter wavelength excitations and correlate to "deeper" energy of the holes from the Fermi level. This work suggests that deeper holes in the d-band catalyze the oxidative addition of aryl halide R-X onto Pd0 at the nanoparticles' surface to form R-PdII-X complex, thus accelerating the rate-determining step of the catalytic cycle. The hot electrons do not play a decisive role. In the future, catalytic mechanisms induced by deep holes should deserve as much attention as the well-known hot electron transfer mechanism.

4.
Sci Rep ; 12(1): 844, 2022 Jan 17.
Artigo em Inglês | MEDLINE | ID: mdl-35039592

RESUMO

We investigate the effect of bis(imino)pyridine (BIP) ligands in guiding self-assembly of semiconducting CdSe/ZnS quantum dots (QDs) into three-dimensional multi-layered shells with diameters spanning the entire mesoscopic range, from 200 nm to 2 µm. The assembly process is directed by guest-host interactions between the BIP ligands and a thermotropic liquid crystal (LC), with the latter's phase transition driving the process. Characterization of the shell structures, through scanning electron microscopy and dynamic light scattering, demonstrates that the average shell diameter depends on the BIP structure, and that changing one functional group in the chemical scaffold allows systematic tuning of shell sizes across the entire range. Differential scanning calorimetry confirms a relationship between shell sizes and the thermodynamic perturbation of the BIP molecules to the LC phase transition temperature, allowing analytical modeling of shell assembly energetics. This novel mechanism to controllably tune shell sizes over the entire mesoscale via one standard protocol is a significant development for research on in situ cargo/drug delivery platforms using nano-assembled structures.

5.
Adv Sci (Weinh) ; 8(23): e2102077, 2021 12.
Artigo em Inglês | MEDLINE | ID: mdl-34687166

RESUMO

The authors reveal a thermal actuating bilayer that undergoes reversible deformation in response to low-energy thermal stimuli, for example, a few degrees of temperature increase. It is made of an aligned carbon nanotube (CNT) sheet covalently connected to a polymer layer in which dibenzocycloocta-1,5-diene (DBCOD) actuating units are oriented parallel to CNTs. Upon exposure to low-energy thermal stimulation, coordinated submolecular-level conformational changes of DBCODs result in macroscopic thermal contraction. This unique thermal contraction offers distinct advantages. It's inherently fast, repeatable, low-energy driven, and medium independent. The covalent interface and reversible nature of the conformational change bestow this bilayer with excellent repeatability, up to at least 70 000 cycles. Unlike conventional CNT bilayer systems, this system can achieve high precision actuation readily and can be scaled down to nanoscale. A new platform made of poly(vinylidene fluoride) (PVDF) in tandem with the bilayer can harvest low-grade thermal energy and convert it into electricity. The platform produces 86 times greater energy than PVDF alone upon exposure to 6 °C thermal fluctuations above room temperature. This platform provides a pathway to low-grade thermal energy harvesting. It also enables low-energy driven thermal artificial robotics, ultrasensitive thermal sensors, and remote controlled near infrared (NIR) driven actuators.

6.
J Conserv Dent ; 24(4): 348-353, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-35282580

RESUMO

Background: Short-term complications after root canal therapy (RCT) include mild pain or flare-up. Patients regard these complications as a benchmark for the assessment of clinician's abilities. In this context, the evidence for recommending either one- or two-visit RCT is not consistent. Aims: This study aims to compare the prevalence of postoperative pain and tenderness to percussion after single-visit (SV) versus two-visit RCT on the mandibular first molar. Materials and Methods: The study was registered with www.ctri.nic.in (CTRI/2019/05/019067). Seventy individuals requiring RCT on a mandibular first molar were selected and randomly ascribed to either single- (Group 1, n = 35) or two-visit RCT (Group 2, n = 35). Postoperative pain levels were assessed using heft parker visual analog scale. The treated teeth were appraised for tenderness to percussion after 1 week of obturation. Statistical Analysis: Thirty-four patients were evaluated in each group: One patient, each, dropped out from both the groups. The data analysis was done using Student's t-test and Chi-square test. Results and Conclusion: Pain score in multiple-visit (MV) was significantly higher than SV after 12- (P = 0.039) and 48 h (P = 0.043). Short-term postoperative pain was higher in MV than SV RCT of mandibular first molar teeth.

7.
J Phys Chem Lett ; 11(24): 10368-10374, 2020 Dec 17.
Artigo em Inglês | MEDLINE | ID: mdl-33236909

RESUMO

We investigate the mechanisms of energy transfer in Mn2+-doped ethylammonium lead bromide (EA2PbBr4:Mn2+), a two-dimensional layered perovskite (2DLP), using cryogenic optical spectroscopy. At temperature T > 120 K, photoluminescence (PL) is dominated by emission from Mn2+, with complete suppression of band edge (BE) emission and self-trapped exciton (STE) emission. However, for T < 120 K, in addition to Mn2+ emission, PL is observed from BE and STEs. Data further reveal that for 20 K < T < 120 K, STEs form the most dominant routes in assisting energy transfer (ET) from 2DLP to Mn2+ dopants. However, at higher Mn2+ concentration, higher activation energies indicate defect states come into play, successfully competing with STEs for ET both from BE to STE states and from STE to Mn2+. Finally, using polarization-resolved spectroscopy, we demonstrate optical spin orientation of the Mn2+ ions via ET from 2DLP excitons at zero magnetic field. Our results reveal fundamental insights on the interactions between quantum confined charge carriers and dopants in organometal halide perovskites.

8.
J Phys Chem Lett ; 11(18): 7886-7892, 2020 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-32870009

RESUMO

We investigate the effect of functionalization by acid/amine combinations of four aromatic capping ligands on the optoelectronic properties of CH3NH3PbBr3 perovskite quantum dots (PQDs). These include benzoic acid (BA), phenylacetic acid (PAA), benzylamine, and isopropyl benzylamine. We observe that charge transfer efficiency in PQD films comprising BA-ligated samples varies between 12% and 95% as the dot density is tuned from 102 to 105 dots/µm2 but is consistently ∼92% over that entire range for PAA-ligated PQDs. As temperature T decreases, initially, recombination is dominated by bound or trapped excitons, but below 80 K, spectral broadening, accompanied by free excitonic behavior, is observed. Our results indicate enhanced charge delocalization at lower values of T, which reduces the level of exciton confinement and recombination decay rates and underlines the importance of investigating PQD-ligand interactions at a fundamental level given the significant effect minute changes in ligand structures have on the optoelectronic properties of quantum dots.

9.
J Pain Res ; 13: 2313-2316, 2020.
Artigo em Inglês | MEDLINE | ID: mdl-32982394

RESUMO

A 62-year-old male diagnosed with cervical dystonia (CD) and chronic right-sided neck pain presented to the Pain Clinic after his pain and CD symptoms failed to resolve with botulinum toxin therapy. During clinical examination, right C3-C4 and C4-C5 facet arthropathy was suspected. After two sets of diagnostic right cervical, C3, C4, and C5 medial branch blocks provided >80% pain relief; cervical radiofrequency ablation (CRFA) was performed. Post CRFA, the patient was followed for 12 months. Till the last follow-up, he was not only experiencing 90% pain relief, but also had significant improvement in his CD symptoms to the point that he no longer needed botulinum toxin and other CD-related therapy. This report suggests that large-scale research is required to postulate whether CD patients, whose symptoms are refractory to botulinum toxin, should be routinely screened for cervical facet arthropathy. This is the first reported case of improvement in CD symptoms with CRFA. This effect could be explained by the fact that certain deep cervical muscles, which are affected in CD, are innervated by medial branch nerves.

10.
Opt Express ; 28(15): 22732-22747, 2020 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-32752530

RESUMO

The concept of "cloaking" an object is a very attractive one, especially in the visible (VIS) and near infra-red (NIR) regions of the electromagnetic spectrum, as that would reduce the visibility of an object to the eye. One possible route to achieving this goal is by leveraging the plasmonic property of metallic nanoparticles (NPs). We model and simulate light in the VIS and NIR scattered by a core of a homogeneous medium, covered by plasmonic cloak that is a spherical shell composed of gold nanoparticles (AuNPs). To consider realistic, scalable, and robust plasmonic cloaks that are comparable, or larger, in size to the wavelength, we introduce a multiscale simulation platform. This model uses the multiple scattering theory of Foldy and Lax to model interactions of light with AuNPs combined with the method of fundamental solutions to model interactions with the core. Numerical results of our simulations for the scattering cross-sections of core-shell composite indicate significant scattering suppression of up to 50% over a substantial portion of the desired spectral range (400 - 600 nm) for cores as large as 900 nm in diameter by a suitable combination of AuNP sizes and filling fractions of AuNPs in the shell.

11.
Comput Methods Programs Biomed ; 195: 105669, 2020 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-32763771

RESUMO

BACKGROUND AND OBJECTIVE: In this study, we have analysed pretreatment positron-emission tomography/ computed tomography (PET/CT) images of head and neck squamous cell carcinoma (HNSCC) patients. We have used a publicly available dataset for our analysis. The clinical features of the patient, PET quantitative parameters, and textural indices from pretreatment PET-CT images are selected for the study. The main objective of the study is to use classifiers to predict the outcome for HNSCC patients and compare the performance of the model with the conventional statistical model (CoxPH). METHODS: We have applied a 40% fixed SUV threshold method for tumour delineation. Clinical features of each patient are provided in the dataset, and other features are calculated using LIFEx software. For predicting the outcome, we have implemented three classifiers - Random Forest classifier, Gradient Boosted Decision tree (GBDT) and Decision tree classifier. We have trained each model using 93 data points and test the model performance using 39 data points. The best model - GBDT is chosen based on the performance metrics. RESULTS: It is observed that typically three features: MTV (Metabolic tumour Volume), primary tumour site and GLCM_correlation are significant for prediction of survival outcome. For testing cohort, GBDT achieves a balanced accuracy of 88%, where conventional statistical model reported a balanced accuracy of 81.5%. CONCLUSIONS: The proposed classifier achieves higher accuracy than the state of the art technique. Using this classifier we can estimate the HNSCC patient's outcome, and depending upon the outcome treatment policy can be selected.


Assuntos
Carcinoma de Células Escamosas , Neoplasias de Cabeça e Pescoço , Carcinoma de Células Escamosas/diagnóstico por imagem , Fluordesoxiglucose F18 , Neoplasias de Cabeça e Pescoço/diagnóstico por imagem , Humanos , Tomografia por Emissão de Pósitrons combinada à Tomografia Computadorizada , Tomografia por Emissão de Pósitrons , Compostos Radiofarmacêuticos , Carcinoma de Células Escamosas de Cabeça e Pescoço/diagnóstico por imagem
12.
Sci Rep ; 9(1): 15784, 2019 10 31.
Artigo em Inglês | MEDLINE | ID: mdl-31673043

RESUMO

The ability to fabricate new materials using nanomaterials as building blocks, and with meta functionalities, is one of the most intriguing possibilities in the area of materials design and synthesis. Semiconducting quantum dots (QDs) and magnetic nanoparticles (MNPs) are co-dispersed in a liquid crystalline (LC) matrix and directed to form self-similar assemblies by leveraging the host's thermotropic phase transition. These co-assemblies, comprising 6 nm CdSe/ZnS QDs and 5-20 nm Fe3O4 MNPs, bridge nano- to micron length scales, and can be modulated in situ by applied magnetic fields <250 mT, resulting in an enhancement of QD photoluminescence (PL). This effect is reversible in co-assemblies with 5 and 10 nm MNPs but demonstrates hysteresis in those with 20 nm MNPs. Transmission electron microscopy (TEM) and energy dispersive spectroscopy reveal that at the nanoscale, while the QDs are densely packed into the center of the co-assemblies, the MNPs are relatively uniformly dispersed through the cluster volume. Using Lorentz TEM, it is observed that MNPs suspended in LC rotate to align with the applied field, which is attributed to be the cause of the observed PL increase at the micro-scale. This study highlights the critical role of correlating multiscale spectroscopy and microscopy characterization in order to clarify how interactions at the nanoscale manifest in microscale functionality.

13.
J Chem Phys ; 151(15): 154705, 2019 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-31640377

RESUMO

In this work, we studied the effects of particles' size and temperature on the photoluminescence (PL) of CH3NH3PbBr3 perovskite nanocrystals (PNCs), with the PNC size controlled by varying the surface passivating ligands. The structural and optical properties of the PNCs were investigated using UV-Vis and PL spectroscopy, revealing strong quantum confinement effects. Temperature dependent PL measurements showed the spectral blue shift of the PL peak for the small PNCs (3.1 ± 0.2 nm) with decreasing temperature from 300 K to 20 K, which is opposite to the red shift with decreasing temperature observed for large- (9.2 ± 0.5 nm) and middle-sized (5.1 ± 0.3 nm) PNCs. The PL lifetime also increased with increasing temperature for the larger PNCs, while it remained about the same for the small and middle-sized PNCs. This increase in lifetime with temperature is attributed to exciton dissociation to free carriers at higher temperatures and to the formation of polar domains in the PNCs. However, the small and middle-sized PNCs did not show such a trend, which may be due to efficient defect passivation as higher concentration of 3-aminopropyl trimethoxysilane (APTMS) was used and to the role of particle size in surface state delocalization. Cryo-X-ray diffraction showed no new peak formation or peak splitting as temperature was varied, which suggests efficient crystal phase stabilization in PNCs of all three sizes controlled by the concentration of APTMS. These results emphasize the importance of size and surface properties of PNCs in their optical properties such as PL quantum yield, PL lifetime, and crystal phase stability.

14.
Sci Adv ; 5(8): eaaw0706, 2019 08.
Artigo em Inglês | MEDLINE | ID: mdl-31457081

RESUMO

Foxp3 and its protein partners establish a regulatory T (Treg) cell transcription profile and promote immunological tolerance. However, molecular features contributing to a Treg-specific gene expression program are still incompletely understood. We find that the transcription factor Bcl11b is a prominent Foxp3 cofactor with multifaceted functions in Treg biology. Optimal genomic recruitment of Foxp3 and Bcl11b is critically interdependent. Genome-wide occupancy studies coupled with gene expression profiling reveal that Bcl11b, in association with Foxp3, is primarily responsible in establishing a Treg-specific gene activation program. Furthermore, Bcl11b restricts misdirected recruitment of Foxp3 to sites, which would otherwise result in an altered Treg transcriptome profile. Consequently, Treg-specific ablation of Bcl11b results in marked breakdown of immune tolerance, leading to aggressive systemic autoimmunity. Our study provides previously underappreciated mechanistic insights into molecular events contributing to basic aspects of Treg function. Furthermore, it establishes a therapeutic target with potential implications in autoimmunity and cancer.


Assuntos
Autoimunidade , Regulação da Expressão Gênica , Proteínas Repressoras/metabolismo , Linfócitos T Reguladores/metabolismo , Proteínas Supressoras de Tumor/metabolismo , Animais , Sítios de Ligação , Linfócitos T CD4-Positivos/citologia , Linfócitos T CD4-Positivos/imunologia , Linfócitos T CD4-Positivos/metabolismo , Colite/imunologia , Colite/patologia , Feminino , Fatores de Transcrição Forkhead/metabolismo , Masculino , Camundongos Endogâmicos C57BL , Camundongos Knockout , Ligação Proteica , Proteínas Repressoras/deficiência , Proteínas Repressoras/genética , Linfócitos T Reguladores/citologia , Linfócitos T Reguladores/imunologia , Proteínas Supressoras de Tumor/deficiência , Proteínas Supressoras de Tumor/genética
15.
Nat Commun ; 9(1): 4473, 2018 10 26.
Artigo em Inglês | MEDLINE | ID: mdl-30367168

RESUMO

Regulatory T (Treg) cells, which are broadly classified as thymically derived (tTreg) or extrathymically induced (iTreg), suppress immune responses and display stringent dependence to the transcription factor Foxp3. However precise understanding of molecular events that promote and preserve Foxp3 expression in Treg cells is still evolving. Here we show that Foxp1, a forkhead transcription factor and a sibling family member of Foxp3, is essential for sustaining optimal expression of Foxp3 specifically in iTreg cells. Deletion of Foxp1 renders iTreg cells to gradually lose Foxp3, resulting in dramatically reduced Nrp1-Helios- iTreg compartment as well as augmented intestinal inflammation in aged mice. Our finding underscores a mechanistic module in which evolutionarily related transcription factors establish a molecular program to ensure efficient immune homeostasis. Furthermore, it provides a novel target that can be potentially modulated to exclusively reinforce iTreg stability keeping their thymic counterpart unperturbed.


Assuntos
Fatores de Transcrição Forkhead/metabolismo , Proteínas Repressoras/metabolismo , Linfócitos T Reguladores/fisiologia , Animais , Diferenciação Celular/imunologia , Colite/imunologia , Colite/metabolismo , Proteínas de Ligação a DNA/metabolismo , Fatores de Transcrição Forkhead/genética , Deleção de Genes , Expressão Gênica , Histonas/metabolismo , Inflamação , Mucosa Intestinal/imunologia , Mucosa Intestinal/patologia , Camundongos , Camundongos Endogâmicos C57BL , Neuropilina-1/metabolismo , Sequências Reguladoras de Ácido Nucleico , Proteínas Repressoras/genética , Linfócitos T Reguladores/imunologia , Fatores de Transcrição/metabolismo
16.
Phys Rev E ; 97(6-1): 062704, 2018 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-30011549

RESUMO

We modeled the experimentally observed self-assembly of nanoparticles (NPs) into shells with diameters up to 10 µm, via segregation from growing nematic domains. Using field-based Monte Carlo simulations, we found the equilibrium configurations of the system by minimizing a free-energy functional that includes effects of excluded-volume interactions among NPs, orientational elasticity, and the isotropic-nematic phase-transition energy. We developed a Gaussian-profile approximation for the liquid crystal (LC) order-parameter field that provides accurate analytical values for the free energy of LC droplets and the associated microshells. This analytical model reveals a first-order transition between equilibrium states with and without microshells, governed mainly by the competition of excluded-volume and phase-transition energies. By contrast, the LC elasticity effects are much smaller and mostly confined to setting the size of the activation barrier for the transition. In conclusion, field-based thermodynamic methods provide a theoretical framework for the self-assembly of NP shells in liquid crystal hosts and suggest that field-based kinetic methods could be useful to simulate and model the time evolution of NP self-assembly coupled to phase separation.

17.
Sci Rep ; 7(1): 17788, 2017 12 19.
Artigo em Inglês | MEDLINE | ID: mdl-29259223

RESUMO

We present three-dimensional microshells formed by self-assembly of densely-packed 5 nm gold nanoparticles (AuNPs). Surface functionalization of the AuNPs with custom-designed mesogenic molecules drives the formation of a stable and rigid shell wall, and these unique structures allow encapsulation of cargo that can be contained, virtually leakage-free, over several months. Further, by leveraging the plasmonic response of AuNPs, we can rupture the microshells using optical excitation with ultralow power (<2 mW), controllably and rapidly releasing the encapsulated contents in less than 5 s. The optimal AuNP packing in the wall, moderated by the custom ligands and verified using small angle x-ray spectroscopy, allows us to calculate the heat released in this process, and to simulate the temperature increase originating from the photothermal heating, with great accuracy. Atypically, we find the local heating does not cause a rise of more than 50 °C, which addresses a major shortcoming in plasmon actuated cargo delivery systems. This combination of spectral selectivity, low power requirements, low heat production, and fast release times, along with the versatility in terms of identity of the enclosed cargo, makes these hierarchical microshells suitable for wide-ranging applications, including biological ones.

18.
J Phys Chem Lett ; 8(21): 5378-5384, 2017 Nov 02.
Artigo em Inglês | MEDLINE | ID: mdl-29043800

RESUMO

Surface functionalization of nanoscale materials has a significant impact on their properties. We have demonstrated the effect of different passivating ligands on the crystal phase of organometal halide perovskite quantum dots (PQDs). Using static and dynamic spectroscopy, we studied phase transitions in CH3NH3PbBr3 PQDs ligated with either octylaminebromide (P-OABr) or 3-aminopropyl triethoxysilane (P-APTES). Around 140 K, P-OABr underwent a structural phase transition from tetragonal to orthorhombic, established by the emergence of a higher energy band in the photoluminescence (PL) spectrum. This was not observed in P-APTES, despite cooling down to 20 K. Additionally, time-resolved and excitation power-dependent PL, as well as Raman spectroscopy over a range of 300-20 K, revealed that recombination rates and types of charge carriers involved are significantly different in P-APTES and P-OABr. Our findings highlight how aspects of PQD phase stabilization are linked to nanoscale morphology and the crystal phase diagram.

19.
Phys Chem Chem Phys ; 18(41): 28428-28433, 2016 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-27471170

RESUMO

We have developed a framework for using temperature dependent static and dynamic photoluminescence (PL) of hybrid organic-inorganic perovskites (PVSKs) to characterize lattice defects in thin films, based on the presence of nanodomains at low temperature. Our high-stability PVSK films are fabricated using a novel continuous liquid interface propagation technique, and in the tetragonal phase (T > 120 K), they exhibit bi-exponential recombination from free charge carriers with an average PL lifetime of ∼200 ns. Below 120 K, the emergence of the orthorhombic phase is accompanied by a reduction in lifetimes by an order of magnitude, which we establish to be the result of a crossover from free carrier to exciton-dominated radiative recombination. Analysis of the PL as a function of excitation power at different temperatures provides direct evidence that the exciton binding energy is different in the two phases, and using these results, we present a theoretical approach to estimate this variable binding energy. Our findings explain this anomalous low temperature behavior for the first time, attributing it to an inherent fundamental property of the hybrid PVSKs that can be used as an effective probe of thin film quality.

20.
Opt Express ; 23(5): 6888-95, 2015 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-25836908

RESUMO

We have demonstrated an all-optical technique for reversible in-plane and out-of-plane switching of nematic liquid crystal molecules in few micron thick films. Our method leverages the highly localized electric fields ("hot spots") and plasmonic heating that are generated in the near-field region of densely packed gold nanoparticle layers optically excited on-resonance with the localized surface plasmon absorption. Using polarized microscopy and transmission measurements, we observe this switching from homeotropic to planar over a temperature range starting at room temperature to just below the isotropic transition, and at on-resonance excitation intensity less than 0.03 W/cm(2). In addition, we controllably vary the in-plane directionality of the liquid crystal molecules in the planar state by altering the linear polarization of the incident excitation. Using discrete dipole simulations and control measurements, we establish spectral selectivity in this new and interesting perspective for photonic application using low light power.

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