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1.
Nat Mater ; 23(4): 512-518, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38347119

RESUMO

High-contrast optically detected magnetic resonance is a valuable property for reading out the spin of isolated defect colour centres at room temperature. Spin-active single defect centres have been studied in wide bandgap materials including diamond, SiC and hexagonal boron nitride, each with associated advantages for applications. We report the discovery of optically detected magnetic resonance in two distinct species of bright, isolated defect centres hosted in GaN. In one group, we find negative optically detected magnetic resonance of a few percent associated with a metastable electronic state, whereas in the other, we find positive optically detected magnetic resonance of up to 30% associated with the ground and optically excited electronic states. We examine the spin symmetry axis of each defect species and establish coherent control over a single defect's ground-state spin. Given the maturity of the semiconductor host, these results are promising for scalable and integrated quantum sensing applications.

2.
J Chem Phys ; 157(21): 211101, 2022 Dec 07.
Artigo em Inglês | MEDLINE | ID: mdl-36511560

RESUMO

The optical spectra of transition metal dichalcogenide monolayers are dominated by excitons and trions. Here, we establish the dependence of these optical transitions on the disorder from hyperspectral imaging of h-BN encapsulated monolayer MoSe2. While both exciton and trion energies vary spatially, these two quantities are almost perfectly correlated, with spatial variation in the trion binding energy of only ∼0.18 meV. In contrast, variation in the energy splitting between the two lowest energy exciton states is one order of magnitude larger at ∼1.7 meV. Statistical analysis and theoretical modeling reveal that disorder results from dielectric and bandgap fluctuations, not electrostatic fluctuations. Our results shed light on disorder in high quality TMDC monolayers, its impact on optical transitions, and the many-body nature of excitons and trions.

3.
Phys Rev Lett ; 126(12): 127402, 2021 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-33834815

RESUMO

We present a many-body theory of exciton-trion polaritons (ETPs) in doped two-dimensional semiconductor materials. ETPs are robust coherent hybrid excitations involving excitons, trions, and photons. In ETPs, the 2-body exciton states are coupled to the material ground state via exciton-photon interaction, and the 4-body trion states are coupled to the exciton states via Coulomb interaction. The trion states are not directly optically coupled to the material ground state. The energy-momentum dispersion of ETPs exhibit three bands. We calculate the energy band dispersions and the compositions of ETPs at different doping densities using Green's functions. The energy splittings between the polariton bands, as well as the spectral weights of the polariton bands, depend on the strength of the Coulomb coupling between the excitons and the trions, which in turn depends sensitively on the doping density. The doping density dependence of the ETP bands and the charged nature of the trion states could enable novel electrical and optical control of ETPs.

5.
Nano Lett ; 15(12): 8204-10, 2015 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-26535607

RESUMO

We present results on photoexcited carrier lifetimes in few-layer transition metal dichalcogenide MoS2 using nondegenerate ultrafast optical pump-probe technique. Our results show a sharp increase of the carrier lifetimes with the number of layers in the sample. Carrier lifetimes increase from few tens of picoseconds in monolayer samples to more than a nanosecond in 10-layer samples. The inverse carrier lifetime was found to scale according to the probability of the carriers being present at the surface layers, as given by the carrier wave function in few layer samples, which can be treated as quantum wells. The carrier lifetimes were found to be largely independent of the temperature, and the inverse carrier lifetimes scaled linearly with the photoexcited carrier density. These observations are consistent with defect-assisted carrier recombination, in which the capture of electrons and holes by defects occurs via Auger scatterings. Our results suggest that carrier lifetimes in few-layer samples are surface recombination limited due to the much larger defect densities at surface layers compared with the inner layers.


Assuntos
Calcogênios/química , Elementos de Transição/química , Fotoquímica , Propriedades de Superfície
6.
Nano Lett ; 15(1): 339-45, 2015 Jan 14.
Artigo em Inglês | MEDLINE | ID: mdl-25546602

RESUMO

In this Letter, we present nondegenerate ultrafast optical pump-probe studies of the carrier recombination dynamics in MoS2 monolayers. By tuning the probe to wavelengths much longer than the exciton line, we make the probe transmission sensitive to the total population of photoexcited electrons and holes. Our measurement reveals two distinct time scales over which the photoexcited electrons and holes recombine; a fast time scale that lasts ∼ 2 ps and a slow time scale that lasts longer than ∼ 100 ps. The temperature and the pump fluence dependence of the observed carrier dynamics are consistent with defect-assisted recombination as being the dominant mechanism for electron-hole recombination in which the electrons and holes are captured by defects via Auger processes. Strong Coulomb interactions in two-dimensional atomic materials, together with strong electron and hole correlations in two-dimensional metal dichalcogenides, make Auger processes particularly effective for carrier capture by defects. We present a model for carrier recombination dynamics that quantitatively explains all features of our data for different temperatures and pump fluences. The theoretical estimates for the rate constants for Auger carrier capture are in good agreement with the experimentally determined values. Our results underscore the important role played by Auger processes in two-dimensional atomic materials.


Assuntos
Dissulfetos/química , Elétrons , Modelos Químicos , Molibdênio/química
7.
Sci Rep ; 13(1): 8678, 2023 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-37248283

RESUMO

Single-photon defect emitters (SPEs), especially those with magnetically and optically addressable spin states, in technologically mature wide bandgap semiconductors are attractive for realizing integrated platforms for quantum applications. Broadening of the zero phonon line (ZPL) caused by dephasing in solid state SPEs limits the indistinguishability of the emitted photons. Dephasing also limits the use of defect states in quantum information processing, sensing, and metrology. In most defect emitters, such as those in SiC and diamond, interaction with low-energy acoustic phonons determines the temperature dependence of the dephasing rate and the resulting broadening of the ZPL with the temperature obeys a power law. GaN hosts bright and stable single-photon emitters in the 600-700 nm wavelength range with strong ZPLs even at room temperature. In this work, we study the temperature dependence of the ZPL spectra of GaN SPEs integrated with solid immersion lenses with the goal of understanding the relevant dephasing mechanisms. At temperatures below ~ 50 K, the ZPL lineshape is found to be Gaussian and the ZPL linewidth is temperature independent and dominated by spectral diffusion. Above ~ 50 K, the linewidth increases monotonically with the temperature and the lineshape evolves into a Lorentzian. Quite remarkably, the temperature dependence of the linewidth does not follow a power law. We propose a model in which dephasing caused by absorption/emission of optical phonons in an elastic Raman process determines the temperature dependence of the lineshape and the linewidth. Our model explains the temperature dependence of the ZPL linewidth and lineshape in the entire 10-270 K temperature range explored in this work. The ~ 19 meV optical phonon energy extracted by fitting the model to the data matches remarkably well the ~ 18 meV zone center energy of the lowest optical phonon band ([Formula: see text]) in GaN. Our work sheds light on the mechanisms responsible for linewidth broadening in GaN SPEs. Since a low energy optical phonon band ([Formula: see text]) is a feature of most group III-V nitrides with a wurtzite crystal structure, including hBN and AlN, we expect our proposed mechanism to play an important role in defect emitters in these materials as well.

8.
medRxiv ; 2023 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-36865094

RESUMO

Background: Acute decompensation is associated with increased mortality in heart failure (HF) patients, though the underlying etiology remains unclear. Extracellular vesicles (EVs) and their cargo may mark specific cardiovascular physiologic states. We hypothesized that EV transcriptomic cargo, including long non-coding RNAs (lncRNAs) and mRNAs, is dynamic from the decompensated to recompensated HF state, reflecting molecular pathways relevant to adverse remodeling. Methods: We examined differential RNA expression from circulating plasma extracellular RNA in acute HF patients at hospital admission and discharge alongside healthy controls. We leveraged different exRNA carrier isolation methods, publicly available tissue banks, and single nuclear deconvolution of human cardiac tissue to identify cell and compartment specificity of the topmost significantly differentially expressed targets. EV-derived transcript fragments were prioritized by fold change (-1.5 to + 1.5) and significance (<5% false discovery rate), and their expression in EVs was subsequently validated in 182 additional patients (24 control; 86 HFpEF; 72 HFrEF) by qRT-PCR. We finally examined the regulation of EV-derived lncRNA transcripts in human cardiac cellular stress models. Results: We identified 138 lncRNAs and 147 mRNAs (present mostly as fragments in EVs) differentially expressed between HF and control. Differentially expressed transcripts between HFrEF vs. control were primarily cardiomyocyte derived, while those between HFpEF vs. control originated from multiple organs and different (non-cardiomyocyte) cell types within the myocardium. We validated 5 lncRNAs and 6 mRNAs to differentiate between HF and control. Of those, 4 lncRNAs (AC092656.1, lnc-CALML5-7, LINC00989, RMRP) were altered by decongestion, with their levels independent of weight changes during hospitalization. Further, these 4 lncRNAs dynamically responded to stress in cardiomyocytes and pericytes in vitro , with a directionality mirroring the acute congested state. Conclusion: Circulating EV transcriptome is significantly altered during acute HF, with distinct cell and organ specificity in HFpEF vs. HFrEF consistent with a multi-organ vs. cardiac origin, respectively. Plasma EV-derived lncRNA fragments were more dynamically regulated with acute HF therapy independent of weight change (relative to mRNAs). This dynamicity was further demonstrated with cellular stress in vitro . Prioritizing transcriptional changes in plasma circulating EVs with HF therapy may be a fruitful approach to HF subtype-specific mechanistic discovery. CLINICAL PERSPECTIVE: What is new?: We performed extracellular transcriptomic analysis on the plasma of patients with acute decompensated heart failure (HFrEF and HFpEF) before and after decongestive efforts.Long non-coding RNAs (lncRNAs) within extracellular vesicles (EVs) changed dynamically upon decongestion in concordance with changes within human iPSC-derived cardiomyocytes under stress.In acute decompensated HFrEF, EV RNAs are mainly derived from cardiomyocytes, whereas in HFpEF, EV RNAs appear to have broader, non-cardiomyocyte origins.What are the clinical implications?: Given their concordance between human expression profiles and dynamic in vitro responses, lncRNAs within EVs during acute HF may provide insight into potential therapeutic targets and mechanistically relevant pathways. These findings provide a "liquid biopsy" support for the burgeoning concept of HFpEF as a systemic disorder extending beyond the heart, as opposed to a more cardiac-focused physiology in HFrEF.

9.
Nano Lett ; 11(11): 4902-6, 2011 Nov 09.
Artigo em Inglês | MEDLINE | ID: mdl-21973122

RESUMO

Using optical-pump terahertz-probe spectroscopy, we study the relaxation dynamics of photoexcited carriers in graphene at different substrate temperatures. We find that at lower temperatures the tail of the relaxation transients measured by the differential probe transmission become slower, extending beyond several hundred picoseconds below 50 K. We interpret the observed relaxation transients as resulting from the cooling of the photoexcited carriers via phonon emission. The slow cooling of the photoexcited carriers at low temperatures is attributed to the bulk of the electron and hole energy distributions moving close enough to the Dirac point that both intraband and interband scattering of carriers via optical phonon emission become inefficient for removing heat from the carriers. Our model, which includes intraband carrier scattering and interband carrier recombination and generation, agrees very well with the experimental observations.


Assuntos
Grafite/química , Nanoestruturas/química , Nanoestruturas/ultraestrutura , Espectroscopia Terahertz/métodos , Transporte de Elétrons , Teste de Materiais , Tamanho da Partícula
10.
Artigo em Inglês | MEDLINE | ID: mdl-35712686

RESUMO

Background and objectives: In recent years, immune-checkpoint inhibitors (ICIs) particularly atezolizumab is on the rise in treating advanced malignancies. With its increased clinical use, various electrolyte abnormalities have been reported in the literature. In this review, we have addressed the question of significant electrolyte abnormalities associated with atezolizumab. Materials and methods: Following PRISMA guidelines, we performed a thorough literature search in four databases including PubMed, Cochrane Library, Embase, and Clinicaltrials.gov. We included only randomized controlled trials from 2010 till March 2021. After a comprehensive screening of 1587 articles, we selected 14 articles for our review and tabulated the results. Following MeSH terms were used: "electrolyte abnormalities", "immune checkpoint inhibitors", "atezolizumab". Results: Non-small cell lung cancer (n = 1270) and metastatic urothelial carcinoma (n = 1164) were the most common malignancies among 3160 patients. The most common electrolyte abnormality was hypomagnesemia (4.7%). Hyponatremia, hypophosphatemia, hypercalcemia and hypokalemia were found in 2.3%, 0.63%, 0.25% and 0.06% patients respectively. For patients taking atezolizumab, hypomagnesemia was most frequently found in non-small cell lung carcinoma patients (9.4%), while urothelial metastatic carcinoma patients most commonly had hyponatremia (5.15%). Hypokalemia though insignificant was observed only in patients with metastatic renal cell carcinoma (2.85%). Conclusion: Since the use of atezolizumab is on the rise for the treatment of various cancers, more studies need to be conducted to better understand its safety and toxicity profile.

11.
Am J Cardiol ; 174: 68-75, 2022 07 01.
Artigo em Inglês | MEDLINE | ID: mdl-35473782

RESUMO

In this study, we investigated the baseline characteristics and "trajectories" of clinical response in men and women after cardiac resynchronization therapy (CRT) implantation. Although women enjoy improved echocardiographic response after CRT compared with men, the kinetics of this response and its relation to functional performance and outcomes are less clear. We identified 592 patients who underwent CRT implantation at our center between 2004 and 2017 and were serially followed in a multidisciplinary clinic. Longitudinal linear mixed effects regression for cardiac response was specified, including interaction terms between time after CRT and sex , and Cox regression models were used to assess differences in all-cause mortality by gender after CRT. Women in our cohort were younger than men, had less frequent ischemic etiology of heart failure (24% vs 60% in men), a shorter QRS (151 vs 161 ms) and more frequent left bundle branch block (77% vs 52%) at baseline. Women had a greater improvement in left ventricular ejection fraction that was evident starting at approximately 1-month after CRT. We did not observe effect modification by gender in New York Heart Association class or 6-minute walk distance after CRT. Although women had improved mortality after CRT, after adjustment for potential confounders, gender was not associated with mortality after CRT. In conclusion, women were more likely to have CRT implantation for left bundle branch block and exhibited improved echocardiographic but not functional response within the first year after CRT. Clinical outcomes after CRT were not associated with gender in adjusted analysis.


Assuntos
Terapia de Ressincronização Cardíaca , Insuficiência Cardíaca , Arritmias Cardíacas/terapia , Bloqueio de Ramo , Terapia de Ressincronização Cardíaca/efeitos adversos , Eletrocardiografia , Feminino , Humanos , Masculino , Volume Sistólico , Resultado do Tratamento , Função Ventricular Esquerda , Remodelação Ventricular
12.
iScience ; 25(8): 104833, 2022 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-35937088

RESUMO

Patients with SARS-CoV-2 infection (COVID-19) risk developing long-term neurologic symptoms after infection. Here, we identify biomarkers associated with neurologic sequelae one year after hospitalization for SARS-CoV-2 infection. SARS-CoV-2-positive patients were followed using post-SARS-CoV-2 online questionnaires and virtual visits. Hospitalized adults from the pre-SARS-CoV-2 era served as historical controls. 40% of hospitalized patients develop neurological sequelae in the year after recovery from acute COVID-19 infection. Age, disease severity, and COVID-19 infection itself was associated with additional risk for neurological sequelae in our cohorts. Glial fibrillary astrocytic protein (GFAP) and neurofilament light chain (NF-L) were significantly elevated in SARS-CoV-2 infection. After adjusting for age, sex, and disease severity, GFAP and NF-L remained significantly associated with longer term neurological symptoms in patients with SARS-CoV-2 infection. GFAP and NF-L warrant exploration as biomarkers for long-term neurologic complications after SARS-CoV-2 infection.

13.
Nano Lett ; 9(8): 2967-72, 2009 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-19594164

RESUMO

We have measured the terahertz response of oriented Germanium nanowires using ultrafast optical-pump terahertz-probe spectroscopy. We present results on the time, frequency, and polarization dependence of the terahertz response. Our results indicate intraband energy relaxation times of photoexcited carriers in the 1.5-2.0 ps range, carrier density dependent interband electron-hole recombination times in the 75-125 ps range, and carrier momentum scattering rates in the 60-90 fs range. Additionally, the terahertz response of the nanowires is strongly polarization dependent despite the subwavelength dimensions of the nanowires. The differential terahertz transmission is found to be large when the field is polarized parallel to the nanowires and very small when the field is polarized perpendicular to the nanowires. This polarization dependence of the terahertz response can be explained in terms of the induced depolarization fields and the resulting magnitudes of the surface plasmon frequencies.


Assuntos
Germânio/química , Nanofios/química , Dispositivos Ópticos , Espectroscopia Terahertz
14.
Nat Commun ; 11(1): 2941, 2020 Jun 10.
Artigo em Inglês | MEDLINE | ID: mdl-32523020

RESUMO

Selection rules are of vital importance in determining the basic optical properties of atoms, molecules and semiconductors. They provide general insights into the symmetry of the system and the nature of relevant electronic states. A two-dimensional electron gas in a magnetic field is a model system where optical transitions between Landau levels (LLs) are described by simple selection rules associated with the LL index N. Here we examine the inter-LL optical transitions of high-quality bilayer graphene by photocurrent spectroscopy measurement. We observed valley-dependent optical transitions that violate the conventional selection rules Δ|N| = ± 1. Moreover, we can tune the relative oscillator strength by tuning the bilayer graphene bandgap. Our findings provide insights into the interplay between magnetic field, band structure and many-body interactions in tunable semiconductor systems, and the experimental technique can be generalized to study symmetry-broken states and low energy magneto-optical properties of other nano and quantum materials.

15.
Nat Commun ; 11(1): 3271, 2020 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-32581218

RESUMO

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

16.
J Phys Condens Matter ; 21(17): 174208, 2009 Apr 29.
Artigo em Inglês | MEDLINE | ID: mdl-21825412

RESUMO

We review our recent progress on the fabrication of near-infrared photodetectors based on intersubband transitions in AlN/GaN superlattice structures. Such devices were first demonstrated in 2003, and have since then seen a quite substantial development both in terms of detector responsivity and high speed operation. Nowadays, the most impressive results include characterization up to 3 GHz using a directly modulated semiconductor laser and up to 13.3 GHz using an ultra-short pulse solid state laser.

17.
PLoS One ; 14(11): e0224161, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-31689316

RESUMO

BACKGROUND: Recognizing the need for improving maternal and newborn care, the Punjab public health department (Pakistan) launched emergency obstetric neonatal care (EmONC) services under WHO guideline. Unfortunately, the program implementation is facing some serious problems. The purpose of this study was to identify barriers to implementation of EmONC in district Bahawalnagar (Pakistan). METHODS: This study used sequential exploratory design. Specifically, a qualitative study was conducted to identify barriers to EmONC. Subsequently, the relative importance of these barriers was determined in a quantitative study. Participants were health service providers involved in 24-hours basic EmONC services in the basic health units of district Bahawalnagar (Pakistan). Qualitative data were gathered by interviewing the participants using key informant guide. Quantitative data were collected in a rank order survey of the same participants. The methodological quality was assessed using mixed methods appraisal tool (MMAT) version 2011. RESULTS: The results indicate that lack of teamwork, conflict management, communication, and improper power distribution are important interpersonal barriers. The significant organizational-level barriers include job insecurity, lack of organizational culture, human resource deployment issues, and lack of role clarity. Lack of target management, lack of resource availability, house job requirement, and dual practice issues were identified as major system-level barriers. CONCLUSION: Barriers to EmONC implementation must be addressed for improving maternal and neonatal care in district Bahawalnagar.


Assuntos
Serviços Médicos de Emergência/organização & administração , Implementação de Plano de Saúde/organização & administração , Acessibilidade aos Serviços de Saúde/organização & administração , Serviços de Saúde Materno-Infantil/organização & administração , Serviços de Saúde Rural/organização & administração , Feminino , Humanos , Saúde do Lactente , Recém-Nascido , Saúde Materna , Paquistão , Gravidez , Indicadores de Qualidade em Assistência à Saúde
18.
Opt Express ; 16(3): 1577-82, 2008 Feb 04.
Artigo em Inglês | MEDLINE | ID: mdl-18542235

RESUMO

We demonstrate microfluidic devices for terahertz spectroscopy of biomolecules in aqueous solutions. The devices are fabricated out of a plastic material that is both mechanically rigid and optically transparent with near-zero dispersion in the terahertz frequency range. Using a lowpower terahertz time-domain spectrometer, we experimentally measure the absorption spectra of the vibrational modes of bovine serum albumin from 0.5 - 2.5 THz and find good agreement with previously reported data obtained using large-volume solutions and a high-power free-electron laser. Our results demonstrate the feasibility of performing high sensitivity terahertz spectroscopy of biomolecules in aqueous solutions with detectable molecular quantities as small as 10 picomoles using microfluidic devices.


Assuntos
Biopolímeros/análise , Microfluídica/instrumentação , Espectrofotometria Infravermelho/instrumentação , Água/química , Biopolímeros/química , Desenho de Equipamento , Análise de Falha de Equipamento , Raios Infravermelhos , Microfluídica/métodos , Micro-Ondas , Reprodutibilidade dos Testes , Sensibilidade e Especificidade , Espectrofotometria Infravermelho/métodos
19.
Science ; 358(6365): 907-910, 2017 11 17.
Artigo em Inglês | MEDLINE | ID: mdl-29146807

RESUMO

Excitons, the bound states of an electron and a hole in a solid material, play a key role in the optical properties of insulators and semiconductors. Here, we report the observation of excitons in bilayer graphene (BLG) using photocurrent spectroscopy of high-quality BLG encapsulated in hexagonal boron nitride. We observed two prominent excitonic resonances with narrow line widths that are tunable from the mid-infrared to the terahertz range. These excitons obey optical selection rules distinct from those in conventional semiconductors and feature an electron pseudospin winding number of 2. An external magnetic field induces a large splitting of the valley excitons, corresponding to a g-factor of about 20. These findings open up opportunities to explore exciton physics with pseudospin texture in electrically tunable graphene systems​.

20.
Nat Commun ; 6: 8831, 2015 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-26572726

RESUMO

The strong light emission and absorption exhibited by single atomic layer transitional metal dichalcogenides in the visible to near-infrared wavelength range make them attractive for optoelectronic applications. In this work, using two-pulse photovoltage correlation technique, we show that monolayer molybdenum disulfide photodetector can have intrinsic response times as short as 3 ps implying photodetection bandwidths as wide as 300 GHz. The fast photodetector response is a result of the short electron-hole and exciton lifetimes in this material. Recombination of photoexcited carriers in most two-dimensional metal dichalcogenides is dominated by nonradiative processes, most notable among which is Auger scattering. The fast response time, and the ease of fabrication of these devices, make them interesting for low-cost ultrafast optical communication links.

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