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1.
ACS Photonics ; 10(6): 1859-1865, 2023 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-37363630

RESUMO

Magnetic imaging with nitrogen-vacancy (NV) spins in diamond is becoming an established tool for studying nanoscale physics in condensed matter systems. However, the optical access required for NV spin readout remains an important hurdle for operation in challenging environments such as millikelvin cryostats or biological systems. Here, we demonstrate a scanning-NV sensor consisting of a diamond nanobeam that is optically coupled to a tapered optical fiber. This nanobeam sensor combines a natural scanning-probe geometry with high-efficiency through-fiber optical excitation and readout of the NV spins. We demonstrate through-fiber optically interrogated electron spin resonance and proof-of-principle magnetometry operation by imaging spin waves in an yttrium-iron-garnet thin film. Our scanning-nanobeam sensor can be combined with nanophotonic structuring to control the light-matter interaction strength and has potential for applications that benefit from all-fiber sensor access, such as millikelvin systems.

2.
J Phys Chem A ; 127(6): 1532-1546, 2023 Feb 16.
Artigo em Inglês | MEDLINE | ID: mdl-36745871

RESUMO

We report on shock-tube experiments measuring the collisional excitation of atomic nitrogen using tunable diode laser absorption spectroscopy (TDLAS). Conditions behind the reflected shocks ranged from 8000 to 12000 K and 0.1 to 1.1 atm in mixtures of 1 or 2% molecular nitrogen (N2) in argon (Ar). Absorption from the transition between atomic nitrogen quantum states 4P to 4D at 868 nm was used to monitor the formation of electronically excited nitrogen. Population measurements of the 4P state were made at a rate of 50 kHz. In connection with these measurements, a multitemperature kinetic mechanism is proposed for nitrogen excitation. Measurements suggest a multistage process. In early test times, a period of induction due to N2 dissociation is followed by a rise via heavy particle excitation. The dominant channel causing this excitation is believed to be N + N ↔ N(4P) + N with a measured forward rate constant of 3.65 × 10-18 exp(-119892/T) [m3/s]. As test time evolves, the excitation of 4P, referred to as N*, is subsequently interrupted and then resumes, as the kinetic environment becomes increasingly electron-dominated. The most impactful reactions of the mechanism are optimized to reduce the residual between simulations and the measurements. The measured N* populations indicate strong, though indirect, sensitivity to adjacent processes, including the excitation of metastable nitrogen, and ionization channels.

3.
J Phys Chem A ; 127(9): 2148-2160, 2023 Mar 09.
Artigo em Inglês | MEDLINE | ID: mdl-36852653

RESUMO

We report the application of a multiwavelength speciation strategy to the study of n-pentane (nC5H12) pyrolysis behind reflected shock waves in a shock tube. Experiments were conducted with 2% nC5H12/0.8%CO2/Ar (by mole) between 1150 and 1520 K in the pressure range of 1-2 atm. Utilization of laser absorption spectroscopy at eight wavelengths allowed time-resolved measurements of n-pentane, ethylene, methane, heavy alkenes, and temperature. The measured time histories were compared against the predictions of four recently developed chemical kinetic models for heavy hydrocarbons. It was found that none of the models reconciled the measured species time histories simultaneously. Sensitivity analysis was conducted to identify key reactions influencing the evolution of ethylene and other major pyrolysis products. The analysis revealed that the unimolecular decomposition of n-pentane into n-propyl and ethyl radicals has a dominating influence over the evolution of ethylene in the temperature range of 1150-1450 K. The rate coefficient of this reaction was then adjusted to match the measured ethylene time histories for each experiment. The rate coefficients thus determined, were fit against temperature using an Arrhenius expression given by k1(T) = 3.5 × 1014 exp(-67.2 kcal/RT) s-1. The average overall 2σ uncertainty of the measured rate coefficient was found to be ±35%, resulting primarily from uncertainties in the rate coefficients of secondary reactions. The measured rate coefficient, when used with the models, leads to a significant improvement in the prediction of species time histories. Further improvements in the model are possible if the rate coefficients of relevant reactions pertaining to small hydrocarbon chemistry are determined with an improved accuracy, and less uncertainty. To the best knowledge of the authors, this is the first experimental determination of the rate coefficient of C5H12 → nC3H7 + C2H5.

4.
Appl Opt ; 61(16): 4857-4864, 2022 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-36255970

RESUMO

Schlieren imaging is widely adopted in applications where fluid dynamics features are of interest. However, traditional Z-type schlieren systems utilizing on-axis mirrors generally require large system footprints due to the need to use high f-number mirrors. In this context, off-axis parabolic (OAP) mirrors provide an attractive alternative for permitting the use of smaller f-number optics, but well-documented methodologies for designing schlieren systems with OAP mirrors are lacking. The present work outlines a ray-tracing-based workflow applied to the design of a modified Z-type schlieren system utilizing OAP mirrors. The ray-tracing analysis evaluates the defocus and distortion introduced by schlieren optics. The results are used along with system size and illumination efficiency considerations to inform the selection of optimal optical components capable of producing high-quality schlieren images while minimizing the system footprint. As a step-by-step demonstration of the design methodology, an example schlieren system design is presented. The example schlieren design achieved an image resolution of 1.1 lp/mm at 50% contrast, with a 60% reduction in system length compared to traditional Z-type systems with f/8 mirrors; distortion characterizations of the designed schlieren system showed good agreement with ray-tracing predictions, and the distortion can be corrected through image post-processing. The current work provides a systematic approach for the design of compact schlieren systems with OAP mirrors and demonstrates the utility of this underutilized option.

5.
J Phys Chem A ; 2022 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-35853207

RESUMO

High-temperature cyclopentadiene pyrolysis was examined behind reflected shock waves in a heated shock tube using several laser absorption diagnostic schemes. A two-color, online-offline sensor near 3335 cm-1 was used to measure time histories of acetylene, while a three-color scheme of diagnostics at 10.532, 10.675, and 11.345 µm yielded measurements of cyclopentadiene and ethylene. Species time histories of cyclopentadiene decomposition and acetylene formation as well as ethylene yields are reported from 1319 to 1678 K at 1.2-1.5 atm. In addition, the overall decomposition rate of cyclopentadiene is reported, and comparisons are made to a number of kinetic models.

6.
Laryngoscope ; 131(11): 2616-2624, 2021 11.
Artigo em Inglês | MEDLINE | ID: mdl-34626128

RESUMO

OBJECTIVES/HYPOTHESIS: To provide the ADHERE registry Upper Airway Stimulation (UAS) outcomes update, including analyses grouped by body mass index (BMI) and therapy discomfort. STUDY DESIGN: Prospective observational study. METHODS: ADHERE captures UAS outcomes including apnea-hypopnea index (AHI), Epworth sleepiness scale (ESS), therapy usage, patient satisfaction, clinician assessment, and safety over a 1-year period. BMI ≤32 kg/m2 (BMI32 ) and 32 < BMI ≤35 kg/m2 (BMI35 ) group outcomes were examined. RESULTS: One thousand eight hundred forty-nine patients enrolled in ADHERE, 1,019 reached final visit, 843 completed the visit. Significant changes in AHI (-20.9, P < .0001) and ESS (- 4.4, P < .0001) were demonstrated. Mean therapy usage was 5.6 ± 2.2 hr/day. Significant therapy use difference was present in patients with reported discomfort versus no discomfort (4.9 ± 2.5 vs. 5.7 ± 2.1 hr/day, P = .01). Patients with discomfort had higher final visit mean AHI versus without discomfort (18.9 ± 18.5 vs. 13.5 ± 13.7 events/hr, P = .01). Changes in AHI and ESS were not significantly different. Serious adverse events reported in 2.3% of patients. Device revision rate was 1.9%. Surgical success was less likely in BMI35 versus BMI32 patients (59.8% vs. 72.2%, P = .02). There was a significant therapy use difference: 5.8 ± 2.0 hr/day in BMI32 versus 5.2 ± 2.2 hr/day in BMI35 (P = .028). CONCLUSIONS: Data from ADHERE demonstrate high efficacy rates for UAS. Although surgical response rate differs between BMI32 and BMI35 patient groups, the AHI and ESS reduction is similar. Discomfort affects therapy adherence and efficacy. Thus, proper therapy settings adjustment to ensure comfort is imperative to improve outcomes. LEVEL OF EVIDENCE: 4 Laryngoscope, 131:2616-2624, 2021.


Assuntos
Índice de Massa Corporal , Terapia por Estimulação Elétrica/efeitos adversos , Neuroestimuladores Implantáveis/efeitos adversos , Cooperação do Paciente/estatística & dados numéricos , Apneia Obstrutiva do Sono/terapia , Idoso , Terapia por Estimulação Elétrica/instrumentação , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Estudos Prospectivos , Sistema de Registros/estatística & dados numéricos , Índice de Gravidade de Doença , Apneia Obstrutiva do Sono/diagnóstico , Resultado do Tratamento
7.
Phys Rev E ; 103(6-1): 063211, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-34271738

RESUMO

Collisional excitation kinetics for atomic oxygen is studied behind reflected shock waves in 1%O_{2}/Ar mixtures over 10 000-11 000K using laser absorption spectroscopy of the O(3s^{5}S^{o}) to O(3p^{5}P_{3}) transition at 777 nm and the O(3p^{5}P_{3}) to O(3d ^{5}D_{2,3,4}^{o}) transitions at 926 nm. Four time histories are inferred simultaneously from the absorbance of the two transitions: the population density of level 4 of atomic oxygen, i.e., the O(3s ^{5}S^{o}) state, n_{4}; the population density of level 6 of atomic oxygen, i.e., the O(3p^{5}P_{3}) state, n_{6}; the electron number density, n_{e}; and the heavy-particle translational temperature, T_{tr}. Atomic oxygen in the levels 4 and 6 are not in equilibrium with the ground-state atomic oxygen as the measurements of n_{4} and n_{6} are generally 3-20 times smaller than the corresponding values under Boltzmann equilibrium at T_{tr}. However, these two states are close to partial equilibrium with each other within the test time, indicating strong heavy-particle cross coupling between levels 4 and 6 of atomic oxygen. A simplified two-temperature collisional-radiative (CR) model is developed to study the thermal and chemical nonequilibrium of atomic oxygen following shock heating. The four measured time histories are used to optimize the 12 collisional rate constants in the CR model using a stochastic gradient descent (SGD) algorithm. The time-history results, diagnostic methods, and collisional-radiative model presented in the current study are potentially useful in studies of high-enthalpy air, plasma processing, or other applications involving weakly ionized oxygen.

8.
J Phys Chem A ; 124(19): 3687-3697, 2020 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-32306734

RESUMO

The collisional excitation kinetics of atomic oxygen was studied behind reflected shock waves using tunable diode laser absorption spectroscopy. A test gas mixture of 1% O2/Ar was shock-heated to temperatures between 8000 and 10,000 K and pressures between 0.15 and 1 atm. The time evolution of the atomic oxygen population in the 3 s 5S0 state was monitored by laser absorption at 777.2 nm. The measured O(3 s 5S0) population revealed multistage behavior that was not observed in previous measurements over a temperature range of 5300-7200 K. To interpret the multistage behavior, a three-level collisional-radiative model for atomic oxygen excitation kinetics was developed. The model utilized two independent temperatures, that is, heavy particle translational temperature Ttr and electron translational temperature Te, to describe the fundamental rate constants of atomic oxygen excitation because of collisions with heavy particles and electrons, respectively. The heavy particle excitation rate was inferred from the early stage of the measurement to be k(3P →5S0) = 3.4 × 10-27 (T/K)0.5(1.061 × 105 + 2 (T/K)) exp(-1.061 × 105 K/T) ± 50% m3 s-1. The electron impact excitation rate constant of oxygen, electron impact, and heavy particle impact ionization rate constants of Argon were modified in the model to match the experimental population time histories. The modified rate parameters are also reported for the temperature range explored in the current study.

9.
J Phys Chem A ; 124(16): 3026-3030, 2020 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-32178517

RESUMO

The overall reaction rate for JP10 + OH → products was measured directly via laser absorption of OH in shock tube experiments from 931 to 1308 K and 0.94 to 1.44 atm. The JP10 concentration of test gas mixtures was measured in the shock tube for several experiments using a 3.39 µm laser fuel diagnostic. The measured JP10 concentrations indicated fuel losses due to adsorption of 11-31% compared to values calculated manometrically from mixture preparation. OH was generated via rapid thermal decomposition of tert-butyl hydroperoxide behind reflected shock waves, and post-shock OH profiles were measured via laser absorption at 308.6 nm. The measured OH profiles were fit with a chemical kinetic model for JP10 chemistry to determine the overall JP10 + OH reaction rate. A recommendation is made for the JP10 + OH overall reaction rate over the temperature range explored in this study as k1 (931-1308 K) = 1.622 × 1014 exp(-1826/T [K]) ± 12%. To the authors' knowledge, these data are the first direct measurements of the overall reaction rate for JP10 + OH.

10.
Phys Rev Lett ; 123(6): 063601, 2019 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-31491180

RESUMO

We report on the realization and verification of quantum entanglement between a nitrogen-vacancy electron spin qubit and a telecom-band photonic qubit. First we generate entanglement between the spin qubit and a 637 nm photonic time-bin qubit, followed by photonic quantum frequency conversion that transfers the entanglement to a 1588 nm photon. We characterize the resulting state by correlation measurements in different bases and find a lower bound to the Bell state fidelity of ≥0.77±0.03. This result presents an important step towards extending quantum networks via optical fiber infrastructure.

11.
J Phys Chem A ; 123(42): 9096-9101, 2019 Oct 24.
Artigo em Inglês | MEDLINE | ID: mdl-31557027

RESUMO

The rate constant for the CH3 + C2H6 → CH4 + C2H5 reaction was studied behind reflected shock waves at temperatures between 1369 and 1626 K and pressures from 8.6 to 47.4 atm in mixtures of methane, ethane, and argon. Ethylene time histories were measured using laser absorption of radiation from a carbon dioxide gas laser near 10.532 µm. The resulting rate constant data can be represented by the Arrhenius equation k (T) = 3.90 × 1013 exp(-16670 cal/mol/RT) cm3 mol-1 s-1. We believe this is the first study to extend experimental data for this rate constant to temperatures above 1400 K. The overall 2σ uncertainty of the current data is +18%/-21% resulting primarily from uncertainties associated with the influence of secondary reactions and the fitting of rapidly changing species time histories at the higher temperatures.

12.
Nano Lett ; 19(6): 3987-3992, 2019 06 12.
Artigo em Inglês | MEDLINE | ID: mdl-31136192

RESUMO

Diamond membrane devices containing optically coherent nitrogen-vacancy (NV) centers are key to enable novel cryogenic experiments such as optical ground-state cooling of hybrid spin-mechanical systems and efficient entanglement distribution in quantum networks. Here, we report on the fabrication of a (3.4 ± 0.2) µm thin, smooth (surface roughness rq < 0.4 nm over an area of 20 µm by 30 µm) diamond membrane containing individually resolvable, narrow linewidth (< 100 MHz) NV centers. We fabricate this sample via a combination of high-energy electron irradiation, high-temperature annealing, and an optimized etching sequence found via a systematic study of the diamond surface evolution on the microscopic level in different etch chemistries. Although our particular device dimensions are optimized for cavity-enhanced entanglement generation between distant NV centers in open, tunable microcavities, our results have implications for a broad range of quantum experiments that require the combination of narrow optical transitions and micrometer-scale device geometry.

13.
Opt Lett ; 44(3): 578-581, 2019 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-30702683

RESUMO

A novel method is presented for quantitative two-dimensional temperature measurement in combustion gases. This method, namely spectrally resolved planar laser-induced fluorescence thermometry, utilizes a high-power, wavelength-tunable and narrow-linewidth CW laser to access the spectral lineshapes of a key combustion intermediate, the hydroxyl radical (OH), and enables high-fidelity and calibration-free quantification of non-uniform temperature fields in complex reacting flows. Specifically, the R1(11)/R1(7) line pair of the OH A2Σ+-X2Π(0,0) rovibronic band was probed with laser radiation near 306.5 nm, and their fluorescence ratios were used to infer temperature. Preliminary demonstrations of this thermometry method were performed in a series of burner-stabilized CH4-air flames.

14.
J Phys Chem A ; 123(1): 15-20, 2019 Jan 10.
Artigo em Inglês | MEDLINE | ID: mdl-30537818

RESUMO

The rate constant for the reaction C2H4 + H ⇔ C2H3 + H2 was studied behind reflected shock waves at temperatures between 1619 and 1948 K and pressures near 10 atm in a mixture of C2H4, CH4, H2, and argon. C2H4 time histories were measured using laser absorption of a CO2 gas laser near 10.53 µm. Experimental mixtures were designed to optimize sensitivity to the title reaction with only weak sensitivity to secondary reactions. Two mechanisms, FFCM1 and ARAMCO v2, are used for data analysis. The well-selected operating conditions and Monte Carlo sampling data analysis procedure resulted in mechanism-independent reaction rate constant measurements with a 2σ uncertainty of ±35%. The current data disagree with a broadly used theoretical calculation (Knyazev et al. (1996)), but they are in good consensus with one of the review studies (Baulch et al. (2005)), k = (3.9 × 1022) T3.62 exp(-5670/ T) cm3 molecule-1 s-1. To the best of our knowledge, this work provides the first high-temperature study of the C2H4 + H ⇔ C2H3 + H2 reaction rate constant with well-defined uncertainty.

15.
Science ; 362(6412)2018 10 19.
Artigo em Inglês | MEDLINE | ID: mdl-30337383

RESUMO

The internet-a vast network that enables simultaneous long-range classical communication-has had a revolutionary impact on our world. The vision of a quantum internet is to fundamentally enhance internet technology by enabling quantum communication between any two points on Earth. Such a quantum internet may operate in parallel to the internet that we have today and connect quantum processors in order to achieve capabilities that are provably impossible by using only classical means. Here, we propose stages of development toward a full-blown quantum internet and highlight experimental and theoretical progress needed to attain them.

16.
Opt Lett ; 43(15): 3518-3521, 2018 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-30067624

RESUMO

The hydroxyl (OH) radical is arguably the most important transient radical in high-temperature gas-phase combustion reactions, yet it is very difficult to measure because of its high reactivity and, thus, short lifetime and low concentration. This work reports the development of a novel method for ultra-sensitive, quantitative, and microsecond-resolved detection of OH based on UV frequency-modulation spectroscopy (FMS). To the best of the authors' knowledge, this is the first FMS demonstration in the near-UV spectral region for detection of short-lived radical species. Shot-noise-limited detection was achieved at an optical power of 25 mW. A proof-of-concept experiment in a tabletop H2O/He microwave discharge cell has reached a 1σ minimum detectable absorbance (MDA) of less than 2×10-4 over 1 MHz measurement bandwidth. High-temperature OH measurement was demonstrated in a 15 cm diameter shock tube, where a typical MDA of 3.0×10-4 was achieved at 1330 K, 0.38 atm, and 1 MHz. These preliminary results have outperformed the previous best MDA by more than a factor of 3; further improvement by another order of magnitude is anticipated, following the strategies outlined at the end of this Letter. The current method paves the path to parts per billion (ppb) -level OH detection capability and offers prospects to significantly advance fundamental combustion research by enabling direct observation of OH formation and scavenging kinetics during key stages of fuel oxidation that were inaccessible with previous methods.

17.
Nature ; 558(7709): 268-273, 2018 06.
Artigo em Inglês | MEDLINE | ID: mdl-29899475

RESUMO

Large-scale quantum networks promise to enable secure communication, distributed quantum computing, enhanced sensing and fundamental tests of quantum mechanics through the distribution of entanglement across nodes1-7. Moving beyond current two-node networks8-13 requires the rate of entanglement generation between nodes to exceed the decoherence (loss) rate of the entanglement. If this criterion is met, intrinsically probabilistic entangling protocols can be used to provide deterministic remote entanglement at pre-specified times. Here we demonstrate this using diamond spin qubit nodes separated by two metres. We realize a fully heralded single-photon entanglement protocol that achieves entangling rates of up to 39 hertz, three orders of magnitude higher than previously demonstrated two-photon protocols on this platform 14 . At the same time, we suppress the decoherence rate of remote-entangled states to five hertz through dynamical decoupling. By combining these results with efficient charge-state control and mitigation of spectral diffusion, we deterministically deliver a fresh remote state with an average entanglement fidelity of more than 0.5 at every clock cycle of about 100 milliseconds without any pre- or post-selection. These results demonstrate a key building block for extended quantum networks and open the door to entanglement distribution across multiple remote nodes.

18.
Nature ; 562(7725): E2, 2018 10.
Artigo em Inglês | MEDLINE | ID: mdl-29946170

RESUMO

Change history: In this Letter, the received date should be 20 December 2017, instead of 27 April 2018. This has been corrected online.

19.
J Phys Chem A ; 121(45): 8561-8568, 2017 Nov 16.
Artigo em Inglês | MEDLINE | ID: mdl-29065683

RESUMO

The oxidation of Ar-diluted stoichiometric CH2O-O2 mixtures was studied behind reflected shock waves over temperatures of 1332-1685 K, at pressures of about 1.5 atm and initial CH2O mole fractions of 500, 1500, and 5000 ppm. Quantitative and time-resolved concentration histories of OH and CO (at both v″ = 0 and v″ = 1) were measured by narrow-linewidth laser absorption at 306.7 and 4854 nm, respectively. A time delay was observed between the formation of v″ = 0 and v″ = 1 states of CO, suggesting that CO was kinetically generated primarily in the ground state and then collisionally relaxed toward vibrational equilibrium. The measured CO and OH time-histories were used to evaluate the performance of four detailed reaction mechanisms regarding the oxidation chemistry of CH2O. Further analyses of these time-history data have also led to improved determination for the rate constants of two key reactions, namely H + O2 = O + OH (R1) and OH + CO = CO2 + H (R2), as follows: k1 = 8.04 × 1013 exp(-7370 K/T) cm3 mol-1 s-1, k2 = 1.90 × 1012 exp(-2760 K/T) cm3 mol-1 s-1; both expressions are valid over 1428-1685 K and have 1σ uncertainties of approximately ±10%.

20.
J Phys Chem A ; 121(35): 6568-6579, 2017 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-28792750

RESUMO

The potential energy surfaces (PESs) and reaction rate constants of the unimolecular decomposition of ethyl formate (EF) were investigated using high-precision theoretical methods at the CCSD(T)/CBS(T-Q)//M06-2X/6-311++G(d,p) level of theory. The calculated PESs of EF dissociation and molecular decomposition reactions indicate that the intramolecular H-shift to produce formic acid and ethylene is the dominant decomposition pathway. A detailed chemical kinetic mechanism for EF pyrolysis was constructed by incorporating the important reactions of EF and its radicals into an existing mechanism previously developed for small methyl esters. The updated mechanism was first used to reproduce CO, CO2, and H2O concentration time histories during EF pyrolysis in the shock tube reported by Ren et al. [ Ren , W. , Mitchell Spearrin , R. , Davidson , D. F. , and Hanson , R. K. J. Phys. Chem. A 2014 , 118 , 1785 - 1798 ]. The rate of production and sensitivity analyses show that the competing dehydration and decarboxylation channels of the intermediate formic acid control the final product yields of EF pyrolysis. The EF mechanism was further validated against the shock tube data of OH, CO, CO2, and H2O time histories measured during EF oxidation (equivalence ratio Φ = 1.0) at 1331-1615 K and 1.52-1.74 atm. This revised EF mechanism captured all of the species' time histories over the entire temperature range. Such modeling capability was due to the more accurate rate constants of EF reactions determined by high-precision theoretical calculations and a high-fidelity C0-C2 basis mechanism.

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