Probe Delays Research Articles

Factors influencing false-positive results of rifampicin resistance detected by Xpert MTB/RIF: A retrospective study in Zhejiang, China

ObjectiveThis study aimed to explore the factors influencing false-positive results for rifampicin resistance (RIF-R) detected using Xpert MTB/RIF (Xpert). MethodsThis retrospective analysis included the clinical data of patients from September 2019 to February 2023. The chi-square and rank sum tests were used to compare differences in patient characteristics between the true-positive and false-positive groups. Logistic regression was used to analyze the factors influencing false positives in the detection of RIF-R by Xpert. ResultsA total of 384 patients were included. Logistic regression analysis revealed that, with mutation of probe E as the reference, mutations on probe A or C (OR = 72.68, P < 0.001), probe D (OR = 6.44, P < 0.001), and multiple probes (OR = 5.94, P = 0.002) were associated with false-positive results in Xpert detection of RIF-R. Taking probe delay ΔCt <4 as the reference, ΔCt (4–5.9) (OR = 13.54, P < 0.001), ΔCt (6–7.9) (OR = 48.08, P < 0.001) probe delays were associated with false positives in Xpert detection of RIF-R. When very low quantification is accompanied by a probe delay, the probability of false-positive RIF-R detection can reach 80 %. ConclusionsClinicians should consider factors such as probe mutation type, probe delay, and very low quantification accompanied by probe delay when interpreting Xpert results, which can reduce the misdiagnosis of tuberculosis drug resistance.

Hybrid time-frequency domain dual-probe coherent anti-Stokes Raman scattering for simultaneous temperature and pressure measurements in compressible flows via spectral fitting.

We demonstrate a hybrid time-frequency spectroscopic method for simultaneous temperature/pressure measurements in nonreacting compressible flows with known gas composition. Hybrid femtosecond-picosecond, pure-rotational coherent anti-Stokes Raman scattering (CARS), with two independent, time-delayed probe pulses, is deployed for single-laser-shot measurements of temperature and pressure profiles along an ∼5-mm line. The theory of dual-probe CARS is presented, along with a discussion of the iterative fitting of experimental spectra. Temperature is obtained from spectra acquired with an early, near-collision-free probe time delay (τ 1=0p s) and pressure from spectra obtained at probe delays of τ 2=150-1000p s, where collisions significantly impact the spectral profile. Unique solutions for temperature and pressure are obtained by iteratively fitting the two spectra to account for small collisional effects observed for the near zero probe delay spectrum. A dual-probe pure-rotational CARS system, in a 1D line-imaging configuration, is developed to demonstrate effectively the simultaneous temperature and pressure profiles recorded along the axial centerline of a highly underexpanded jet. The underexpanded air jet permits evaluation of this hybrid time-frequency domain approach for temperature and pressure measurements across a wide range of low-temperature-low-pressure conditions of interest in supersonic ground-test facilities. Single-laser-shot measurement precisions in both quantities and pressure measurement accuracy are systematically evaluated in the quiet zone upstream of the Mach disk. Precise thermometry approaching 1%-2% is observed in regions of high CARS signal-to-noise ratios. Pressure measurements are optimized at probe time delays where the ratio of the late probe delay to the Raman lifetime exceeds four (τ 2/τ R>4). The impact of low-temperature Raman linewidths on CARS pressure measurements is evaluated, and comparisons of CARS pressures obtained with our recent low-temperature pure-rotational Raman linewidth data and extrapolated high-temperature Q-branch linewidths are presented. Considering all measurements with τ 2/τ R≥4.0, measured pressures were on average 7.9% of the computed isentropic values with average shot-to-shot deviations representing a combination of instrument noise and fluid fluctuations of 5.0%.

Numerical study of pure rotational fs/ps CARS coherence beating at high pressure and for multi-species rotation-vibration non-equilibrium thermometry

Coherent anti-Stokes Raman scattering (CARS) has long been the gold standard for non-intrusively measuring gas temperature in reacting flows such as flames and plasmas. Recently, the development of ultrafast hybrid fs/ps CARS has enabled the exploitation of coherence beating between neighboring spectral lines to simultaneously measure rotational and vibrational temperatures from a single pure rotational spectrum. However, the influence of non-Boltzmann vibrational state distributions and limitations due to collisional dephasing at pressures greater than 1 atm remains unclear. In this work, we use spectral simulations to investigate the effects of non-Boltzmann vibrational state distributions and the applicability of coherence beating at pressures up to 10 atm. We show that short probe pulses can be leveraged to quantify non-Boltzmann vibrational state distributions of N2. Furthermore, we demonstrate that fs/ps CARS coherence beating can simultaneously provide sensitive measurements of rotational and vibrational temperatures of both O2 and N2 in air. A sensitivity analysis was conducted to qualitatively explain the accuracy and precision comparisons between probe delays.

Transient Super‐/Sub‐Linear Nonlinearities in Silicon Nanostructures (Advanced Optical Materials 5/2022)

In article number 2101711, Kung-Hsuan Lin, Shi-Wei Chu, and co-workers demonstrate a temporally tunable transient nonlinearity based on fluence-dependent carrier dynamics. This is exemplified via Auger recombination on silicon nanostructures. By combining spatial confocal x-scan and temporal pump–probe techniques, the fluence dependence is analyzed at different pump–probe delays and various transient nonlinearities are found, including sub-linear, super-linear, and surprisingly full saturation behaviors. [Cover image: artwork by Guan-Jie Huang.]

Broadband femtosecond spectroscopic ellipsometry.

We present a setup for time-resolved spectroscopic ellipsometry in a pump-probe scheme using femtosecond laser pulses. As a probe, the system deploys supercontinuum white light pulses that are delayed with respect to single-wavelength pump pulses. A polarizer-sample-compensator-analyzer configuration allows ellipsometric measurements by scanning the compensator azimuthal angle. The transient ellipsometric parameters are obtained from a series of reflectance-difference spectra that are measured for various pump-probe delays and polarization (compensator) settings. The setup is capable of performing time-resolved spectroscopic ellipsometry from the near-infrared through the visible to the near-ultraviolet spectral range at 1.3 eV-3.6 eV. The temporal resolution is on the order of 100 fs within a delay range of more than 5 ns. We analyze and discuss critical aspects such as fluctuations of the probe pulses and imperfections of the polarization optics and present strategies deployed for circumventing related issues.

Ultrafast demagnetization of Pt magnetic moment in L10-FePt probed by magnetic circular dichroism at a hard x-ray free electron laser

Unraveling the origin of ultrafast demagnetization in multisublattice ferromagnetic materials requires femtosecond x-ray techniques to trace the magnetic moment dynamics on individual elements, but this could not yet be achieved in the hard x-ray regime. We demonstrate here the first ultrafast demagnetization dynamics in the ferromagnetic heavy 5d-transition metal Pt using circularly-polarized hard x-rays at an x-ray free electron laser (XFEL). The decay time of laser-induced demagnetization of L10-FePt is determined to be using time-resolved x-ray magnetic circular dichroism at the Pt L3 edge, whereas magneto-optical Kerr measurements indicate the decay time for the total magnetization as . A transient magnetic state with a photo-modulated ratio of the 3d and 5d magnetic moments is demonstrated for pump–probe delays larger than 1 ps. We explain this distinct photo-modulated transient magnetic state by the induced-moment behavior of the Pt atom and the x-ray probing depth. Our findings pave the way for the future use of XFELs to disentangle atomic spin dynamics contributions.

Rotational coherence beating in molecular oxygen: Coupling between electronic spin and nuclear angular momenta.

Time-resolved pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman spectroscopy (fs/ps RCARS) of oxygen (O2) is performed at pressures from ∼0.04 to 0.4 atm. As the RCARS spectra evolve with probe delay, they exhibit coherence beating between unresolved S-branch triplet transitions (ΔN = 2, ΔJ = 2). The time-domain fitting of the RCARS signal intensity enables the determination of these transition frequency separations, which are as low as 480 MHz (0.016 cm-1). Additionally, we study the underlying pressure-dependent dynamics and the signatures of the time-domain triplet signals compared to the simple decays associated with the O2 self-broadened linewidths. Pressure- and N-dependent O2 linewidths are compared to literature coefficients obtained from experiments and models that have not incorporated the triplet splitting. Our findings are incorporated into a time-domain model for rotational CARS thermometry of O2 and have significant impact for spectral evaluations at probe delays greater than 100 ps for temperature or species concentration determination. The time- and frequency-resolved experiments presented in this work provide insight into the spectroscopic complexities introduced by the electronic ground state of O2 for accurate evaluation of time-resolved coherent Raman spectra.

Interference-free hybrid fs/ps vibrational CARS thermometry in high-pressure flames.

Interference-free hybrid femtosecond/picosecond vibrational coherent anti-Stokes Raman scattering (CARS) of nitrogen is reported for temperature measurements of 1300-2300K in high-pressure, laminar H2-air and CH4-air diffusion flames up to 10bar. Following coherent Raman excitation by 100fs duration pump and Stokes pulses, a time-asymmetric probe pulse is used for the detection of spectrally resolved N2 CARS signals at probe delays as early as ∼200-300 fs. This allows for full rejection of nonresonant contributions while being independent of collisions for single-shot precision of ±2% at elevated pressures. The effects of collisions at longer probe-pulse delays are also investigated to determine the feasibility of varying the detection timing from 200fs to 100ps.

Dielectric-barrier-discharge plasma-assisted hydrogen diffusion flame. Part 1: Temperature, oxygen, and fuel measurements by one-dimensional fs/ps rotational CARS imaging

One-dimensional hybrid fs/ps CARS imaging provides single-laser-shot measurements of temperature, oxygen, and hydrogen in a plasma-assisted hydrogen diffusion flame. The coaxial dielectric-barrier-discharge burner collapses the Re ∼50 hydrogen diffusion flame to within ∼5 mm of the burner surface at an applied AC potential of 8.75 kV at 18 kHz, coinciding nicely with the full spatial extent of the 1D CARS measurements. Translating the burner through the measurement volume allowed for measurements at numerous radial locations in increments of 1 mm with a resolution of 140 µm × 30 µm × 600 µm, sufficient to resolve spatial gradients in this unsteady flame. Longer probe delays, required for improved dynamic range in regions of high temperature fluctuations, proved difficult to model as a result of a nontrivial decay in the O2 Raman coherence arising from complexities associated with the triplet ground electronic state of the O2 molecule. Oxygen linewidths were treated empirically using the observed O2 coherence decay in spectra acquired from the product gases of lean, near-adiabatic H2/air flames stabilized on a Hencken flat-flame burner. While still leading to errors up to 10% at worst, the empirically determined Raman linewidth factors eliminated any systematic error in the O2/N2 measurements with probe delay. Temperature measurements in the Hencken Burner flames proved to be insensitive to probe pulse delay, providing robust thermometry. Demonstration of this technique in both the canonical Hencken burner flames and a new DBD burner validates its effectiveness in producing multiple spatially resolved measurements in combustion environments. Measurements in the DBD burner revealed an unsteady, counterflow flattened flame structure near the fuel orifice which became unsteady as the reaction zone curves towards the surface for larger radial positions. Fluctuations in the fuel concentration were largest at the source, as the large, plasma-generated, unsteady external toroidal vortex that dominates the transport in this flame provides enhanced ventilation of the flame surface in close proximity to the fuel tube.

Ultrafast optical Faraday effect in transparent solids

We predict a strong-field ultrafast optical Faraday effect, where a circularly polarized ultrashort optical pulse induces transient chirality in an achiral transparent dielectric. This effect is attractive for time-resolved measurements because it gives access to the non-instantaneity of the nonlinear medium response, and also because it represents relaxation of time-reversal symmetry by all-optical means. We propose probing the induced transient chirality with a weak linearly polarized ultraviolet pulse that is shorter than the near-infrared pump pulse. The predicted effects are ultrafast: the induced chirality vanishes for probe delays exceeding the duration of the near-infrared pulse. This opens up possibilities for applications in ultrafast circular-polarization modulators and analyzers.

Hybrid femtosecond/picosecond pure‐rotational coherent anti‐Stokes Raman scattering with chirped probe pulses

AbstractThe influence of probe laser chirp on hybrid femtosecond/picosecond pure‐rotational coherent anti‐Stokes Raman scattering is studied theoretically and experimentally. Experiments of N2(hybrid fs/ps pure‐rotational coherent anti‐Stokes Raman scattering) are carried out using an in‐house built second harmonic bandwidth compressor, results with different probe chirps of are reported. The experimental spectra are fitted with and without considering probe chirp. Including the chirp improves the fit to experimental spectra at all probe delays. The effect of probe pulse chirp is evaluated through a quantitative analysis of matching residuals.

Towards efficient time-resolved X-ray absorption studies of electron dynamics at photocatalytic interfaces.

We present a picosecond time-resolved X-ray absorption spectroscopy (tr-XAS) setup designed for synchrotron-based studies of interfacial photochemical dynamics. The apparatus combines a high power, variable repetition rate picosecond laser system with a time-resolved X-ray fluorescence yield detection technique. Time-tagging of the detected fluorescence signals enables the parallel acquisition of X-ray absorption spectra at a variety of pump-probe delays employing the well-defined time structure of the X-ray pulse trains. The viability of the setup is demonstrated by resolving dynamic changes in the fine structure near the O1s X-ray absorption edge of cuprous oxide (Cu2O) after photo-excitation with a 355 nm laser pulse. Two distinct responses are detected. A pronounced, quasi-static, reversible change of the Cu2O O1s X-ray absorption spectrum by up to ∼30% compared to its static line shape corresponds to a redshift of the absorption edge by ∼1 eV. This value is small compared to the 2.2 eV band gap of Cu2O but in agreement with previously published results. The lifetime of this effect exceeds the laser pulse-to-pulse period of 8 μs, resulting in a quasi-static spectral change that persists as long as the sample is exposed to the laser light, and completely vanishes once the laser is blocked. Additionally, a short-lived response corresponding to a laser-induced shift of the main absorption line by ∼2 eV to lower energies appears within <200 ps and decays with a characteristic timescale of 43 ± 5 ns. Both the picosecond rise and nanosecond decay of this X-ray response are simultaneously captured by making use of a time-tagging approach - highlighting the prospects of the experimental setup for efficient probing of the electronic and structural dynamics in photocatalytic systems on multiple timescales.

Reflectivity kinetics of saturable absorbers for laser mirrors

The reflectivity kinetics of saturable absorbers based on semiconductor quantum wells was investigated with differential reflectivity accuracy by the pump–probe technique for energy fluxes (0.27–5.40) photons cm−2 using a femtosecond Yb3+ :KY(WO4)2 laser. Three kinds of saturable absorbers were investigated: absorbers based on multiple quantum wells with nano-structured barriers grown over a mirror; the same absorber grown over the substrate; absorbers on multiple quantum wells separated by thick barriers grown over the substrate. The substrate contribution gives a stationary background and a two-photon absorption peak for small probe delays, which complicates the kinetics of the samples grown over the substrate. For absorbers grown over the mirror two exponential decays with a short relaxation time –0.4 ps and with a long relaxation time ps were obtained. The last relaxation time is remarkably shorter than in quantum wells with thick barriers.

Pressure measurements using hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman scattering.

We investigate the feasibility of gas-phase pressure measurements using fs/ps rotational CARS. Femtosecond pump and Stokes pulses impulsively prepare a rotational Raman coherence, which is probed by a high-energy 5-ps pulse introduced at a time delay from the Raman preparation. These ultrafast laser pulses are shorter than collisional-dephasing time scales, enabling a new hybrid time- and frequency-domain detection scheme for pressure. Single-laser-shot rotational CARS spectra were recorded from N2 contained in a room-temperature gas cell for pressures from 0.4 to 3 atm and probe delays ranging from 16 to 298 ps. Sensitivity of the accuracy and precision of the pressure data to probe delay was investigated. The technique exhibits superior precision and comparable accuracy to previous laser-diagnostic pressure measurements.

Unambiguous determination of spin dephasing times in ZnO by time‐resolved magneto‐optical pump–probe experiments

Time‐resolved magneto‐optics is a well‐established optical pump–probe technique to generate and to probe spin coherence in semiconductors. By this method, spin dephasing times can easily be determined if their values are comparable to the available pump–probe delays. If exceeds the laser repetition time, however, resonant spin amplification (RSA) can equally be used to extract . We demonstrate that in ZnO these techniques have several tripping hazards resulting in deceptive values for and show how to avoid them. We show that the temperature dependence of the amplitude ratio of two separate spin species can easily be misinterpreted as a strongly temperature‐dependent of a single spin ensemble, while the two spin species have values, which are nearly independent of temperature. Additionally, consecutive pump pulses can significantly diminish the spin polarization, which remains from previous pump pulses. While this barely affects values extracted from delay line scans, it results in seemingly shorter values in RSA.

The Study of the Delay Kerr Loops Induced by Femtosecond Laser Pulses in GdFeCo Film

To study the evolution of the coercivity and magnetization induced by femtosecond laser pulses in GdFeCo film at distinct pump–probe delays and reveal the laser-induced magnetization reversal process, the static delay Kerr loops were measured by the traditional time-resolved magneto-optical Kerr effect technique. The results showed that the loops contained memory effect from external field history and could not reflect the real change of coercivity and magnetization after laser pump. To eliminate the memory effect, a home-made experimental setup of photomagnetic synchronized time-resolved magneto-optical Kerr effect technology was used to measure the dynamic delay Kerr loops and reveal the real evolution of the coercivity and magnetization after laser pump, whose results are of great importance in real magneto-optical recording application.

Electron Correlation Effects on the Femtosecond Dephasing Dynamics ofE22Excitons in (6,5) Carbon Nanotubes

Highly nonlinear pump fluence dependence was observed in the ultrafast one-color pump-probe responses excited by 38 fs pulses resonant with the E(22) transition in a room-temperature solution of (6,5) carbon nanotubes. The differential probe transmission (ΔT/T) at the peak of the pump-probe response (τ = 20 fs) was measured for pump fluences from ∼10(13) to 10(17) photons/pulse cm(2). The onset of saturation is observed at ∼2 × 10(15) photons/pulse cm(2) (∼8 × 10(5) excitons/cm). At pump fluences >4 × 10(16) photons/pulse cm(2) (∼1.6 × 10(6) excitons/cm), ΔT/T decreases as the pump fluence increases. Analogous signal saturation behavior was observed for all measured probe delays. Despite the high exciton density at saturation, no change in the E(22) population decay rate was observed at short times (<300 fs). The pump probe signal was modeled by a third-order perturbation theory treatment that includes the effects of inhomogeneous broadening. The observed ΔT/T signal is well-fit by a pump-fluence-dependent dephasing rate linearly dependent on the number of excitons created by the pump pulse. Therefore, the observed nonlinear pump intensity dependence is attributed to the effects of quasi-elastic exciton-exciton interactions on the dephasing rates of single carbon nanotubes. The low fluence total dephasing time is 36 fs, corresponding to a homogeneous width of 36 meV (290 cm(-1)), and the derived E(22) inhomogeneous width is 68 meV (545 cm(-1)). These results are contrasted with photon-echo-derived parameters for the E(11) transition.

Time-dependent depolarization of aligned D2 caused by hyperfine coupling

Molecular deuterium is prepared in the J = 2, M = 0 sublevel of ν = 1 by stimulated Raman pumping of the ν = 0 S(0) line. Following optical excitation, the degree of alignment of the rotational angular momentum J oscillates in time caused by the coupling of J to the total nuclear spin angular momentum I(T). This coupling is of two kinds, the interaction of J with the magnetic moments and the quadrupole fields of the two I = 1 deuterium nuclei. The alignment is monitored via the O(2) line of the E,F(1)Σ(g)(+)-X(1)Σ(g)(+) (0,1) band using [2+1] resonance enhanced multiphoton ionization for pump-probe delays from 0 to 20 μs. Using the hyperfine coupling constants found previously for the ν = 0 state (R. F. Code and N. F. Ramsey, Phys. Rev. A, 1971, 4, 1945), we are able to fit the time dependence essentially within our experimental error, but this requires that the presence of both I(T) = 0 and I(T) = 2 nuclear spin states for this o-deuterium level is properly weighted and taken into account.

Gas-phase single-shot thermometry at 1 kHz using fs-CARS spectroscopy

Single-laser-shot temperature measurements at a data rate of 1 kHz employing femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy of N(2) are demonstrated. The measurements are performed using a chirped-probe pulse to map the time-dependent frequency-spread dephasing of the Raman coherence, which is created by approximately 80-fs pump and Stokes beams, into the spectrum of the coherent anti-Stokes Raman scattering signal pulse. Temperature is determined from the spectral shape of the fs-CARS signal for probe delays of approximately 2 ps with respect to the pump-Stokes excitation. The accuracy and precision of the measurements for the 300-2400 K range are found to be approximately 1%-6% and approximately 1.5%-3%, respectively.

Soot particle sizing during high-pressure Diesel spray combustion via time-resolved laser-induced incandescence

Single-pulse time-resolved laser-induced incandescence (TiRe-LII) signal transients from soot particulates were acquired during unsteady high pressure Diesel combustion in a constant volume cell for typical top dead center conditions during a Diesel engine cycle. Measurements were performed for initial gas pressures between 1 and 3 MPa, injection pressures between 50 and 130 MPa and laser probe timings between 5 and 16 ms after start of fuel injection. In separate experiments and for the same cell operating conditions gas temperatures were deduced from spectrally resolved soot pyrometry measurements. Implementing the LII model of Kock et al. [Combust. Flame 147 (2006) 79–92] ensemble mean soot particle diameters were evaluated from least-squares fitting of theoretical cooling curves to experimental TiRe-LII signal transients. Since in the experiments the environmental gas temperature and the width of an assumed particle size distribution were not known, the effects of the initial choice of these parameters on retrieved particle diameters were investigated. It is shown that evaluated mean particle diameters are only slightly biased by the choice of typical size distribution widths and gas temperatures. For a fixed combustion phase mean particle diameters are not much affected by gas pressure, however they become smaller at high fuel injection pressure. At a mean chamber pressure of 1.39 MPa evaluated mean particle diameters increased by a factor of two for probe delays between 5 and 16 ms after start of injection irrespective of the choices of first-guess fitting variables, indicating a certain robustness of data analysis procedure.