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1.
Physiol Rep ; 12(17): e70031, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39218618

RESUMO

Previous studies report contradicting age-related neurovascular coupling (NVC). Few studies assess postural effects, but less investigate relationships between age and NVC within different postures. Therefore, this study investigated the effect of age on NVC in different postures with varying cognitive stimuli. Beat-to-beat blood pressure, heart rate and end-tidal carbon dioxide were assessed alongside middle and posterior cerebral artery velocities (MCAv and PCAv, respectively) using transcranial Doppler ultrasonography in 78 participants (31 young-, 23 middle- and 24 older-aged) with visuospatial (VST) and attention tasks (AT) in various postures at two timepoints (T2 and T3). Between-group significance testing utilized one-way analysis-of-variance (ANOVA) (Tukey post-hoc). Mixed three-way/one-way ANOVAs explored task, posture, and age interactions. Significant effects of posture on NVC were driven by a 3.8% increase from seated to supine. For AT, mean supine %MCAv increase was greatest in younger (5.44%) versus middle (0.12%) and older-age (0.09%) at T3 (p = 0.005). For VST, mean supine %PCAv increase was greatest at T2 and T3 in middle (10.99%/10.12%) and older-age (17.36%/17.26%) versus younger (9.44%/8.89%) (p = 0.004/p = 0.002). We identified significant age-related NVC effects with VST-induced hyperactivation. This may reflect age-related compensatory processes in supine. Further work is required, using complex stimuli while standing/walking, examining NVC, aging and falls.


Assuntos
Envelhecimento , Acoplamento Neurovascular , Postura , Humanos , Masculino , Feminino , Acoplamento Neurovascular/fisiologia , Adulto , Pessoa de Meia-Idade , Idoso , Postura/fisiologia , Envelhecimento/fisiologia , Adulto Jovem , Atenção/fisiologia , Ultrassonografia Doppler Transcraniana/métodos , Pressão Sanguínea/fisiologia , Circulação Cerebrovascular/fisiologia , Velocidade do Fluxo Sanguíneo/fisiologia , Frequência Cardíaca/fisiologia , Artéria Cerebral Média/fisiologia , Artéria Cerebral Média/diagnóstico por imagem
2.
Nat Commun ; 15(1): 7584, 2024 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-39217171

RESUMO

Heparan sulfate (HS) regulation of FGFR function, which is essential for salivary gland (SG) development, is determined by the immense structural diversity of sulfated HS domains. 3-O-sulfotransferases generate highly 3-O-sulfated HS domains (3-O-HS), and Hs3st3a1 and Hs3st3b1 are enriched in myoepithelial cells (MECs) that produce basement membrane (BM) and are a growth factor signaling hub. Hs3st3a1;Hs3st3b1 double-knockout (DKO) mice generated to investigate 3-O-HS regulation of MEC function and growth factor signaling show loss of specific highly 3-O-HS and increased FGF/FGFR complex binding to HS. During development, this increases FGFR-, BM- and MEC-related gene expression, while in adult, it reduces MECs, increases BM and disrupts acinar polarity, resulting in salivary hypofunction. Defined 3-O-HS added to FGFR pulldown assays and primary organ cultures modulates FGFR signaling to regulate MEC BM synthesis, which is critical for secretory unit homeostasis and acinar function. Understanding how sulfated HS regulates development will inform the use of HS mimetics in organ regeneration.


Assuntos
Membrana Basal , Diferenciação Celular , Células Epiteliais , Heparitina Sulfato , Camundongos Knockout , Glândulas Salivares , Transdução de Sinais , Sulfotransferases , Animais , Heparitina Sulfato/metabolismo , Membrana Basal/metabolismo , Glândulas Salivares/metabolismo , Glândulas Salivares/citologia , Sulfotransferases/metabolismo , Sulfotransferases/genética , Camundongos , Células Epiteliais/metabolismo , Células Epiteliais/citologia , Receptores de Fatores de Crescimento de Fibroblastos/metabolismo , Receptores de Fatores de Crescimento de Fibroblastos/genética , Masculino , Fatores de Crescimento de Fibroblastos/metabolismo
3.
J Cereb Blood Flow Metab ; : 271678X241270452, 2024 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-39113406

RESUMO

Neurovascular coupling (NVC) is the perturbation of cerebral blood flow (CBF) to meet varying metabolic demands induced by various levels of neural activity. NVC may be assessed by Transcranial Doppler ultrasonography (TCD), using task activation protocols, but with significant methodological heterogeneity between studies, hindering cross-study comparisons. Therefore, this review aimed to summarise and compare available methods for TCD-based healthy NVC assessments. Medline (Ovid), Scopus, Web of Science, EMBASE (Ovid) and CINAHL were searched using a predefined search strategy (PROSPERO: CRD42019153228), generating 6006 articles. Included studies contained TCD-based assessments of NVC in healthy adults. Study quality was assessed using a checklist, and findings were synthesised narratively. 76 studies (2697 participants) met the review criteria. There was significant heterogeneity in the participant position used (e.g., seated vs supine), in TCD equipment, and vessel insonated (e.g. middle, posterior, and anterior cerebral arteries). Larger, more significant, TCD-based NVC responses typically included a seated position, baseline durations >one-minute, extraneous light control, and implementation of previously validated protocols. In addition, complementary, combined position, vessel insonated and stimulation type protocols were associated with more significant NVC results. Recommendations are detailed here, but further investigation is required in patient populations, for further optimisation of TCD-based NVC assessments.

4.
Blood Press Monit ; 2024 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-39133561

RESUMO

OBJECTIVE: Remote patient monitoring (RPM) beat-to-beat blood pressure (BP) provides an opportunity to measure poststroke BP variability (BPV), which is associated with clinical stroke outcomes. BP sampling interval (SI) influences ambulatory BPV, but RPM BP SI optimisation research is limited. SI and RPM device capabilities require compromises, meaning SI impact requires investigation. Therefore, this study assessed healthy and stroke subtype BPV via optimised BP sampling, aiding sudden BP change identification and potentially assisting cardiovascular event (recurrent stroke) prediction. METHODS: Leicester Cerebral Haemodynamic Database ischaemic [acute ischaemic stroke (AIS), n = 68] and haemorrhagic stroke (intracerebral haemorrhage, n = 12) patient and healthy control (HC, n = 40) baseline BP data were analysed. Intrasubject and interpatient SD (SDi/SDp) represented individual/population variability with synthetically altered SIs. Matched-filter approaches using cross-correlation function detected sudden BP changes. RESULTS: At SIs between 1 and 180 s, SBP and DBP SDi staticised while SDp increased at SI < 30 s. Mean BP and HR SDi and SDp increased at SI < 60s. AIS BPV, normalised to SI1s, increased at SI30s (26%-131%) and SI120s (1%-274%). BPV increased concomitantly with SI. Cross-correlation analysis showed HC and AIS BP sudden change detection accuracy reductions with increasing SI. Positive BP deviation detection fell 48.48% (SI10s) to 78.79% (SI75s) in HC and 67.5% (SI10s) to 100% (SI75s) in AIS. Negative BP deviation detection fell 50% (SI10s) to 82.35% (SI75s) in HC and 52.27% (SI10s) to 95.45% (SI75s) in AIS. CONCLUSION: Sudden BP change detection and BPV are relatively robust to SI increases within certain limits, but accuracy reductions generate unacceptable estimates, considerable within RPM device design. This research warrants further SI optimisation.

5.
Matrix Biol ; 2024 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-38944161

RESUMO

Heparan sulfate (HS) is an important component of the kidney anionic filtration barrier, the glomerular basement membrane (GBM). HS chains attached to proteoglycan protein cores are modified by sulfotransferases in a highly ordered series of biosynthetic steps resulting in immense structural diversity due to negatively charged sulfate modifications. 3-O-sulfation is the least abundant modification generated by a family of seven isoforms but creates the most highly sulfated HS domains. We analyzed the kidney phenotypes in the Hs3st3a1, Hs3st3b1 and Hs3st6 -knockout (KO) mice, the isoforms enriched in kidney podocytes. Individual KO mice show no overt kidney phenotype, although Hs3st3b1 kidneys were smaller than wildtype (WT). Furthermore, Hs3st3a1-/-; Hs3st3b1-/- double knockout (DKO) kidneys were smaller but also had a reduction in glomerular size relative to wildtype (WT). Mass spectrometry analysis of kidney HS showed reduced 3-O-sulfation in Hs3st3a1-/- and Hs3st3b1-/-, but not in Hs3st6-/- kidneys. Glomerular HS showed reduced HS staining and reduced ligand-and-carbohydrate engagement (LACE) assay, a tool that detects changes in binding of growth factor receptor-ligand complexes to HS. Interestingly, DKO mice have increased levels of blood urea nitrogen, although no differences were detected in urinary levels of albumin, creatinine and nephrin. Finally, transmission electron microscopy showed irregular and thickened GBM and podocyte foot process effacement in the DKO compared to WT. Together, our data suggest that loss of 3-O-HS domains disrupts the kidney glomerular architecture without affecting the glomerular filtration barrier and overall kidney function.

8.
Nature ; 620(7975): 807-812, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37612395

RESUMO

The United Nations recently agreed to major expansions of global protected areas (PAs) to slow biodiversity declines1. However, although reserves often reduce habitat loss, their efficacy at preserving animal diversity and their influence on biodiversity in surrounding unprotected areas remain unclear2-5. Unregulated hunting can empty PAs of large animals6, illegal tree felling can degrade habitat quality7, and parks can simply displace disturbances such as logging and hunting to unprotected areas of the landscape8 (a phenomenon called leakage). Alternatively, well-functioning PAs could enhance animal diversity within reserves as well as in nearby unprotected sites9 (an effect called spillover). Here we test whether PAs across mega-diverse Southeast Asia contribute to vertebrate conservation inside and outside their boundaries. Reserves increased all facets of bird diversity. Large reserves were also associated with substantially enhanced mammal diversity in the adjacent unprotected landscape. Rather than PAs generating leakage that deteriorated ecological conditions elsewhere, our results are consistent with PAs inducing spillover that benefits biodiversity in surrounding areas. These findings support the United Nations goal of achieving 30% PA coverage by 2030 by demonstrating that PAs are associated with higher vertebrate diversity both inside their boundaries and in the broader landscape.


Assuntos
Biodiversidade , Conservação dos Recursos Naturais , Objetivos , Clima Tropical , Nações Unidas , Animais , Conservação dos Recursos Naturais/legislação & jurisprudência , Conservação dos Recursos Naturais/métodos , Conservação dos Recursos Naturais/tendências , Mamíferos , Agricultura Florestal/legislação & jurisprudência , Agricultura Florestal/métodos , Agricultura Florestal/tendências
9.
J Magn Reson ; 354: 107521, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37487304

RESUMO

We report on hyperpolarization of quadrupolar (I=3/2) 131Xe via spin-exchange optical pumping. Observations of the 131Xe polarization dynamics via in situ low-field NMR show that the estimated alkali-metal/131Xe spin-exchange rates can be large enough to compete with 131Xe spin relaxation. 131Xe polarization up to 7.6±1.5% was achieved in ∼8.5×1020 spins-a ∼100-fold improvement in the total spin angular momentum-potentially enabling various applications, including: measurement of spin-dependent neutron-131Xe s-wave scattering; sensitive searches for time-reversal violation in neutron-131Xe interactions beyond the Standard Model; and surface-sensitive pulmonary MRI.

10.
Chest ; 164(3): 700-716, 2023 09.
Artigo em Inglês | MEDLINE | ID: mdl-36965765

RESUMO

BACKGROUND: Microvascular abnormalities and impaired gas transfer have been observed in patients with COVID-19. The progression of pulmonary changes in these patients remains unclear. RESEARCH QUESTION: Do patients hospitalized with COVID-19 without evidence of architectural distortion on structural imaging exhibit longitudinal improvements in lung function measured by using 1H and 129Xe MRI between 6 and 52 weeks following hospitalization? STUDY DESIGN AND METHODS: Patients who were hospitalized with COVID-19 pneumonia underwent a pulmonary 1H and 129Xe MRI protocol at 6, 12, 25, and 51 weeks following hospital admission in a prospective cohort study between November 2020 and February 2022. The imaging protocol was as follows: 1H ultra-short echo time, contrast-enhanced lung perfusion, 129Xe ventilation, 129Xe diffusion-weighted, and 129Xe spectroscopic imaging of gas exchange. RESULTS: Nine patients were recruited (age 57 ± 14 [median ± interquartile range] years; six of nine patients were male). Patients underwent MRI at 6 (n = 9), 12 (n = 9), 25 (n = 6), and 51 (n = 8) weeks following hospital admission. Patients with signs of interstitial lung damage were excluded. At 6 weeks, patients exhibited impaired 129Xe gas transfer (RBC to membrane fraction), but lung microstructure was not increased (apparent diffusion coefficient and mean acinar airway dimensions). Minor ventilation abnormalities present in four patients were largely resolved in the 6- to 25-week period. At 12 weeks, all patients with lung perfusion data (n = 6) showed an increase in both pulmonary blood volume and flow compared with 6 weeks, although this was not statistically significant. At 12 weeks, significant improvements in 129Xe gas transfer were observed compared with 6-week examinations; however, 129Xe gas transfer remained abnormally low at weeks 12, 25, and 51. INTERPRETATION: 129Xe gas transfer was impaired up to 1 year following hospitalization in patients who were hospitalized with COVID-19 pneumonia, without evidence of architectural distortion on structural imaging, whereas lung ventilation was normal at 52 weeks.


Assuntos
COVID-19 , Isótopos de Xenônio , Humanos , Masculino , Adulto , Pessoa de Meia-Idade , Idoso , Feminino , Estudos Prospectivos , Imageamento por Ressonância Magnética/métodos , Pulmão/diagnóstico por imagem
11.
Nat Commun ; 14(1): 932, 2023 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-36805448

RESUMO

In this work, we couple theoretical and experimental approaches to understand and reduce the losses of wide bandgap Br-rich perovskite pin devices at open-circuit voltage (VOC) and short-circuit current (JSC) conditions. A mismatch between the internal quasi-Fermi level splitting (QFLS) and the external VOC is detrimental for these devices. We demonstrate that modifying the perovskite top-surface with guanidinium-Br and imidazolium-Br forms a low-dimensional perovskite phase at the n-interface, suppressing the QFLS-VOC mismatch, and boosting the VOC. Concurrently, the use of an ionic interlayer or a self-assembled monolayer at the p-interface reduces the inferred field screening induced by mobile ions at JSC, promoting charge extraction and raising the JSC. The combination of the n- and p-type optimizations allows us to approach the thermodynamic potential of the perovskite absorber layer, resulting in 1 cm2 devices with performance parameters of VOCs up to 1.29 V, fill factors above 80% and JSCs up to 17 mA/cm2, in addition to a thermal stability T80 lifetime of more than 3500 h at 85 °C.

12.
Magn Reson Med ; 89(6): 2217-2226, 2023 06.
Artigo em Inglês | MEDLINE | ID: mdl-36744585

RESUMO

PURPOSE: Imaging of the different resonances of hyperpolarized 129 Xe in the brain and lungs was performed using a 3D sampling density-weighted MRSI technique in healthy volunteers. METHODS: Four volunteers underwent dissolved-phase hyperpolarized 129 Xe imaging in the lung with the MRSI technique, which was designed to improve the point-spread function while preserving SNR (1799 phase-encoding steps, 14-s breath hold, 2.1-cm isotropic resolution). A frequency-tailored RF excitation pulse was implemented to reliably excite both the 129 Xe gas and dissolved phase (tissue/blood signal) with 0.1° and 10° flip angles, respectively. Images of xenon gas in the lung airspaces and xenon dissolved in lung tissue/blood were used to generate quantitative signal ratio maps. The method was also optimized and used for imaging dissolved resonances of 129 Xe in the brain in 2 additional volunteers. RESULTS: High-quality regional spectra of hyperpolarized 129 Xe were achieved in both the lung and the brain. Ratio maps of the different xenon resonances were obtained in the lung with sufficient SNR (> 10) at both 1.5 T and 3 T, making a triple Lorentzian fit possible and enabling the measurement of relaxation times and xenon frequency shifts on a voxel-wise basis. The imaging technique was successfully adapted for brain imaging, resulting in the first demonstration of 3D xenon brain images with a 2-cm isotropic resolution. CONCLUSION: Density-weighted MRSI is an SNR and encoding-efficient way to image 129 Xe resonances in the lung and the brain, providing a valuable tool to quantify regional spectroscopic information.


Assuntos
Imageamento por Ressonância Magnética , Isótopos de Xenônio , Humanos , Isótopos de Xenônio/química , Imageamento por Ressonância Magnética/métodos , Pulmão/diagnóstico por imagem , Xenônio , Imageamento Tridimensional/métodos
13.
Environ Sci Pollut Res Int ; 30(10): 27912-27935, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36385346

RESUMO

This study aimed to predict evaporation from dam reservoirs using artificial intelligence considering climate change. Mahabad Dam, near Lake Urmia, in northwestern Iran, is used to investigate the proposed approach. There are three parts to the study presented herein. In the first part, two machine learning models, namely group method of data handling (GMDH) and least squares support vector regression (LS-SVR), were used to model the inflow to the dam reservoir. Temperature, precipitation, and inflow during the previous month from 1990 to 2017 were used as input data. In the second part, the evaporation from the dam reservoir was modeled using the adaptive neuro-fuzzy inference system (ANFIS) and optimized ANFIS using Harris hawks optimization (HHO) and the arithmetic optimization algorithm (AOA) optimization algorithms. The input parameters in this part were temperature, precipitation, inflow to the dam reservoir, along with evaporation from the dam reservoir in the previous month. In the third part, precipitation and temperature were predicted using the fifth report of IPCC based on RCP2.6, RCP4.5, and RCP8.5 scenarios for the period 2020-2040. Out of 28 models presented in the fifth report, EC-ERATH and FIO-ESM had the greatest similarity with observational data of temperature and precipitation, respectively. The results of scatter plots and Taylor's diagram showed the higher performance of LS-SVR (root mean square error (RMSE), mean absolute percentage error (MAPE), and Nash-Sutcliffe efficiency (NSE) of 8.65, 4.69, and 0.96) compared to GMDH (RMSE, MAPE, and NSE of 11.65, 7.81, and 0.93) in modeling the inflow. Moreover, both hybrid modes (AOA-ANFIS and HHO-ANFIS) improved the performance of ANFIS in modeling the evaporation from the dam reservoir. The RMSE, MAPE, and NSE values for ANFIS were 0.56, 0.52, and 0.89, respectively, while these values for the AOA-ANFIS (RMSE, MAPE, and NSE of 0.31, 0.24, and 0.93) and HHO-ANFIS (RMSE, MAPE, and NSE of 0.20, 0.30, and 0.96) were improved remarkably. The impact of climate change reduced the inflow to the dam reservoir by about 0.45, 0.80, and 1.7 MCM in RCP2.6, RCP4.5, and RCP8.5 scenarios, respectively. Also, the effect of climate change caused the evaporation from the dam reservoir to increase by about 0.2, 0.9, and 1 MCM in RCP2.6, RCP4.5, and RCP8.5 scenarios, respectively. The findings of this study show that the correct management of dam reservoirs needs to consider the potential effects of climate change in the future. Moreover, the hybrid machine learning models used in this study can be used to predict the amount of evaporation in other reservoirs.


Assuntos
Inteligência Artificial , Lógica Fuzzy , Mudança Climática , Algoritmos , Aprendizado de Máquina
14.
ACS Appl Mater Interfaces ; 15(1): 772-781, 2023 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-36563084

RESUMO

Vacuum deposition is a solvent-free method suitable for growing thin films of metal halide perovskite (MHP) semiconductors. However, most reports of high-efficiency solar cells based on such vacuum-deposited MHP films incorporate solution-processed hole transport layers (HTLs), thereby complicating prospects of industrial upscaling and potentially affecting the overall device stability. In this work, we investigate organometallic copper phthalocyanine (CuPc) and zinc phthalocyanine (ZnPc) as alternative, low-cost, and durable HTLs in all-vacuum-deposited solvent-free formamidinium-cesium lead triodide [CH(NH2)2]0.83Cs0.17PbI3 (FACsPbI3) perovskite solar cells. We elucidate that the CuPc HTL, when employed in an "inverted" p-i-n solar cell configuration, attains a solar-to-electrical power conversion efficiency of up to 13.9%. Importantly, unencapsulated devices as large as 1 cm2 exhibited excellent long-term stability, demonstrating no observable degradation in efficiency after more than 5000 h in storage and 3700 h under 85 °C thermal stressing in N2 atmosphere.

15.
Nat Mater ; 22(1): 73-83, 2023 01.
Artigo em Inglês | MEDLINE | ID: mdl-36456873

RESUMO

Achieving the long-term stability of perovskite solar cells is arguably the most important challenge required to enable widespread commercialization. Understanding the perovskite crystallization process and its direct impact on device stability is critical to achieving this goal. The commonly employed dimethyl-formamide/dimethyl-sulfoxide solvent preparation method results in a poor crystal quality and microstructure of the polycrystalline perovskite films. In this work, we introduce a high-temperature dimethyl-sulfoxide-free processing method that utilizes dimethylammonium chloride as an additive to control the perovskite intermediate precursor phases. By controlling the crystallization sequence, we tune the grain size, texturing, orientation (corner-up versus face-up) and crystallinity of the formamidinium (FA)/caesium (FA)yCs1-yPb(IxBr1-x)3 perovskite system. A population of encapsulated devices showed improved operational stability, with a median T80 lifetime (the time over which the device power conversion efficiency decreases to 80% of its initial value) for the steady-state power conversion efficiency of 1,190 hours, and a champion device showed a T80 of 1,410 hours, under simulated sunlight at 65 °C in air, under open-circuit conditions. This work highlights the importance of material quality in achieving the long-term operational stability of perovskite optoelectronic devices.


Assuntos
Amidinas , Luz Solar , Cátions , Dimetil Sulfóxido
16.
Cereb Circ Cogn Behav ; 3: 100039, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36324414

RESUMO

Background: Consensus on the optimal metrics for neurovascular coupling (NVC) is lacking. The aim of this study was to use principal component analysis (PCA) to determine the most significant contributors to NVC responses in healthy adults (HC), Alzheimer's disease (AD), and mild cognitive impairment (MCI). New method: PCA was applied to three datasets: 1) 69 HC, 2) 30 older HC, 34 AD, and 22 MCI, 3) 1&2 combined. Data were extracted on peak percentage change in cerebral blood flow velocity (CBFv), variance ratio (VR), cross-correlation function peak (CCF), and blood pressure, for five cognitive tasks. An equamax rotation was applied and factors were significant where the eignevalue was ≥1. Rotated factor loadings ≥0.4 determined significant NVC variables. Results: PCA identified 12 significant factors accounting for 78% of variance (all datasets). Contributing variables loaded differently on the factors across the datasets. In datasets 1&2, peak percentage change in CBFv contributed to factors explaining the most variance (45-58%), whereas cognitive test scores, fluency and memory domains contributed the least (15-37%). In the combined dataset, CBFv, CCF and fluency domain contributed the majority (33-43%), whereas VR and attention the least (6-24%). Conclusions: Peak percentage change in CBFv and the visuospatial task consistently accounted for a large proportion of the variance, suggesting these are robust NVC markers for future studies.

17.
Science ; 378(6616): 186-192, 2022 10 14.
Artigo em Inglês | MEDLINE | ID: mdl-36227977

RESUMO

Studies of the proteome would benefit greatly from methods to directly sequence and digitally quantify proteins and detect posttranslational modifications with single-molecule sensitivity. Here, we demonstrate single-molecule protein sequencing using a dynamic approach in which single peptides are probed in real time by a mixture of dye-labeled N-terminal amino acid recognizers and simultaneously cleaved by aminopeptidases. We annotate amino acids and identify the peptide sequence by measuring fluorescence intensity, lifetime, and binding kinetics on an integrated semiconductor chip. Our results demonstrate the kinetic principles that allow recognizers to identify multiple amino acids in an information-rich manner that enables discrimination of single amino acid substitutions and posttranslational modifications. With further development, we anticipate that this approach will offer a sensitive, scalable, and accessible platform for single-molecule proteomic studies and applications.


Assuntos
Proteoma , Proteômica , Aminoácidos/química , Aminopeptidases , Peptídeos/química , Proteômica/métodos , Semicondutores , Análise de Sequência de Proteína/métodos
18.
Nat Commun ; 13(1): 4201, 2022 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-35859149

RESUMO

Charge carrier mobility is a fundamental property of semiconductor materials that governs many electronic device characteristics. For metal halide perovskites, a wide range of charge carrier mobilities have been reported using different techniques. Mobilities are often estimated via transient methods assuming an initial charge carrier population after pulsed photoexcitation and measurement of photoconductivity via non-contact or contact techniques. For nanosecond to millisecond transient methods, early-time recombination and exciton-to-free-carrier ratio hinder accurate determination of free-carrier population after photoexcitation. By considering both effects, we estimate long-range charge carrier mobilities over a wide range of photoexcitation densities via transient photoconductivity measurements. We determine long-range mobilities for FA0.83Cs0.17Pb(I0.9Br0.1)3, (FA0.83MA0.17)0.95Cs0.05Pb(I0.9Br0.1)3 and CH3NH3PbI3-xClx polycrystalline films in the range of 0.3 to 6.7 cm2 V-1 s-1. We demonstrate how our data-processing technique can also reveal more precise mobility estimates from non-contact time-resolved microwave conductivity measurements. Importantly, our results indicate that the processing of polycrystalline films significantly affects their long-range mobility.

19.
J Synchrotron Radiat ; 29(Pt 4): 1043-1053, 2022 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-35787572

RESUMO

Three-dimensional X-ray diffraction (3DXRD) is shown to be feasible at the I12 Joint Engineering, Environmental and Processing (JEEP) beamline of Diamond Light Source. As a demonstration, a microstructually simple low-carbon ferritic steel was studied in a highly textured and annealed state. A processing pipeline suited to this beamline was created, using software already established in the 3DXRD user community, enabling grain centre-of-mass positions, orientations and strain tensor elements to be determined. Orientations, with texture measurements independently validated from electron backscatter diffraction (EBSD) data, possessed a ∼0.1° uncertainty, comparable with other 3DXRD instruments. The spatial resolution was limited by the far-field detector pixel size; the average of the grain centre of mass position errors was determined as ±âˆ¼80 µm. An average per-grain error of ∼1 × 10-3 for the elastic strains was also measured; this could be reduced in future experiments by improving sample preparation, geometry calibration, data collection and analysis techniques. Application of 3DXRD onto I12 shows great potential, where its implementation is highly desirable due to the flexible, open architecture of the beamline. User-owned or designed sample environments can be used, thus 3DXRD could be applied to previously unexplored scientific areas.

20.
ACS Energy Lett ; 7(6): 1903-1911, 2022 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-35719271

RESUMO

As perovskite-based photovoltaics near commercialization, it is imperative to develop industrial-scale defect-passivation techniques. Vapor deposition is a solvent-free fabrication technique that is widely implemented in industry and can be used to fabricate metal-halide perovskite thin films. We demonstrate markably improved growth and optoelectronic properties for vapor-deposited [CH(NH2)2]0.83Cs0.17PbI3 perovskite solar cells by partially substituting PbI2 for PbCl2 as the inorganic precursor. We find the partial substitution of PbI2 for PbCl2 enhances photoluminescence lifetimes from 5.6 ns to over 100 ns, photoluminescence quantum yields by more than an order of magnitude, and charge-carrier mobility from 46 cm2/(V s) to 56 cm2/(V s). This results in improved solar-cell power conversion efficiency, from 16.4% to 19.3% for the devices employing perovskite films deposited with 20% substitution of PbI2 for PbCl2. Our method presents a scalable, dry, and solvent-free route to reducing nonradiative recombination centers and hence improving the performance of vapor-deposited metal-halide perovskite solar cells.

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