Excitation Pulse Length Research Articles

Modulating lifetime distribution through variable excitation pulse length and power: a case study on colloidal PbS quantum dots

Modulating lifetime distribution through variable excitation pulse length and power: a case study on colloidal PbS quantum dots

Influence of Residual Quadrupolar Interaction on Quantitative Sodium Brain Magnetic Resonance Imaging of Patients With Multiple Sclerosis.

The purpose of this work was to evaluate the influence of residual quadrupolar interaction on the determination of human brain apparent tissue sodium concentrations (aTSCs) using quantitative sodium magnetic resonance imaging ( 23 Na MRI) in healthy controls (HCs) and patients with multiple sclerosis (MS). Especially, it was investigated if the more detailed examination of residual quadrupolar interaction effects enables further analysis of the observed 23 Na MRI signal increase in MS patients. 23 Na MRI with a 7 T MR system was performed on 21 HC and 50 MS patients covering all MS subtypes (25 patients with relapsing-remitting MS, 14 patients with secondary progressive MS, and 11 patients with primary progressive MS) using 2 different 23 Na pulse sequences for quantification: a commonly used standard sequence (aTSC Std ) as well as a sequence with shorter excitation pulse length and lower flip angle for minimizing signal loss resulting from residual quadrupolar interactions (aTSC SP ). Apparent tissue sodium concentration was determined using the same postprocessing pipeline including correction of the receive profile of the radiofrequency coil, partial volume correction, and relaxation correction. Spin dynamic simulations of spin-3/2 nuclei were performed to aid in the understanding of the measurement results and to get deeper insight in the underlying mechanisms. In normal-appearing white matter (NAWM) of HC and all MS subtypes, the aTSC SP values were approximately 20% higher than the aTSC Std values ( P < 0.001). In addition, the ratio aTSC SP /aTSC Std was significantly higher in NAWM than in normal-appearing gray matter (NAGM) for all subject cohorts ( P < 0.002). In NAWM, aTSC Std values were significantly higher in primary progressive MS compared with HC ( P = 0.01) as well as relapsing-remitting MS ( P = 0.03). However, in contrast, no significant differences between the subject cohorts were found for aTSC SP . Spin simulations assuming the occurrence of residual quadrupolar interaction in NAWM were in good accordance with the measurement results, in particular, the ratio aTSC SP /aTSC Std in NAWM and NAGM. Our results showed that residual quadrupolar interactions in white matter regions of the human brain have an influence on aTSC quantification and therefore must be considered, especially in pathologies with expected microstructural changes such as loss of myelin in MS. Furthermore, the more detailed examination of residual quadrupolar interactions may lead to a better understanding of the pathologies themselves.

The influence of Ce3+ codoping on upconversion in nanocrystalline NaYF4:Yb3+,Tm3+

Usually, to obtain multicolor upconversion in lanthanides, materials with different codopants, different size, chemical composition or compositional architecture are required. However, designing a material whose emission color can be tuned in-situ by an external stimulus, such as temperature, excitation pulse duration or photoexcitation density, is of great interest for many applications, but still remains a challenge. The possible solution for this issue can be achieved by intentional codoping the luminescent materials with optically active ions which can disturb or compete with other energy transfer processes, and in consequence lead to changes in relative emission intensity, thus the dominant emission color. Here we synthesized and investigated colloidal luminescent Yb3+ and Tm3+ doped NaYF4 nanoparticles which were codoped with optically active Ce3+ ions, whose relative emission intensity ratios between 1D2→3F4 (at 450 nm), 1G4→3H6 (at 475 nm), 1G4→3F4 (at 650 nm), and 3H4→3H6 (at 800 nm) were significantly dependent from external stimulus – namely temperature and/or excitation pulse length. Our results shows two fold increase in 450/800, 470/800 and 650/800 luminescence intensity bands ratios (LIR) only after incorporation of Ce3+ ions to the material, and even three-fold increase in those LIR after changing the excitation conditions (i.e. pulse width). Moreover, temperature dependent luminescence properties revealed relative sensitivity of 4%/K for the 450/800 and 470/800 bands ratio and almost 5.5%/K for the 650/800 band ratio close to 0 °C. By switching to physiological range of temperatures, the thermal sensitivity decreased to around 2%/K for the 450/800 and 470/800 bands ratio and to over 2.5%/K for 650/800 bands ratio, which should be considered as significant values and suitable for temperature sensing in practical applications. It is worth noting that the thermal sensitivity values can be further enhanced by applying different excitation pulse width. The proposed materials allows to tune its emissions as well as thermal properties by changing the dopant concentration or more importantly also in situ, through excitation scheme modifications.

Filament damage formation in fused silica glass as a result of 1-50 ps near-infrared laser pulses.

We measure filament damage due to self-focusing in fused silica glass using short laser pulses of 1-50ps of 1053nm wavelength. We examine the dependence of the effect on the excitation fluence and pulse length. A beam propagation model adjusted to picosecond pulse lengths shows a good fit to the measurements. Whereas for longer pulses a filament appears within the bulk, for the shorter pulses surface damage appears due to the high nonlinearity of the system.

Environmental and Excitation Power Effects on the Ratiometric Upconversion Luminescence Based Temperature Sensing Using Nanocrystalline NaYF4 :Yb3+ ,Er3.

The luminescence intensity ratio (LIR) of the green emissions of the near-infrared excited NaYF4 :Yb3+ ,Er3+ nanocrystals is a promising method for temperature sensing. Here, the influence of excitation power density, excitation pulse length, excitation wavelength, silica shell, and solvent on the LIR and its temperature response is reported. The primary objective is to study the LIR mechanism and the impact of measurement and environmental parameters on the calibration and precision of the LIR. The LIR value is demonstrated to be unaffected by the excitation intensity in the studied range. This result is essential, considering the application feasibility of the LIR method as temperature sensor, where the effective excitation power density depends on the sample matrix and the distance excitation light travels in the sample. The pulsed excitation, however, results in an increase in the LIR value upon short pulse width. Silanization of bare nanocrystals has no effect on the LIR values, but the local warming of H2 O samples under laser exposure results in slightly increased LIR values compared to other solvents; D2 O, oleic acid, and dimethyl sulfoxide. The thermal quenching of luminescence lifetimes of Er3+ emission is proved to be too weak for sensing applications.

Note: On the choice of the appropriate excitation-pulse-length for assessment of slow luminescence decays.

The decay-time distribution deduced from luminescence kinetics experiments is, in general, dependent on the excitation pulse length as a direct consequence of different onset dynamics. We demonstrate this effect for the case of square excitation pulses applied to study the luminescence kinetics in Si nanocrystals. The short- and long-pulse limits are defined as 0.1 times the shortest lifetime in the distribution and 3 times the longest time, respectively. Outside these limits the decay-time distribution is independent on the pulse duration. In addition, we describe experimental conditions required to obtain a correct depiction of slow luminescence decay in the μs to ms time range.

Dynamical modeling of pulsed two-photon interference

Single-photon sources are at the heart of quantum-optical networks, with their uniquely quantum emission and phenomenon of two-photon interference allowing for the generation and transfer of nonclassical states. Although a few analytical methods have been briefly investigated for describing pulsed single-photon sources, these methods apply only to either perfectly ideal or at least extremely idealized sources. Here, we present the first complete picture of pulsed single-photon sources by elaborating how to numerically and fully characterize non-ideal single-photon sources operating in a pulsed regime. In order to achieve this result, we make the connection between quantum Monte-Carlo simulations, experimental characterizations, and an extended form of the quantum regression theorem. We elaborate on how an ideal pulsed single-photon source is connected to its photocount distribution and its measured degree of second- and first-order optical coherence. By doing so, we provide a description of the relationship between instantaneous source correlations and the typical experimental interferometers (Hanbury-Brown and Twiss, Hong–Ou–Mandel, and Mach–Zehnder) used to characterize such sources. Then, we use these techniques to explore several prototypical quantum systems and their non-ideal behaviors. As an example numerical result, we show that for the most popular single-photon source—a resonantly excited two-level system—its error probability is directly related to its excitation pulse length. We believe that the intuition gained from these representative systems and characters can be used to interpret future results with more complicated source Hamiltonians and behaviors. Finally, we have thoroughly documented our simulation methods with contributions to the Quantum Optics Toolbox in Python in order to make our work easily accessible to other scientists and engineers.

Multi-Frequency Pulsed Overhauser DNP at 1.2 Tesla

Abstract Dynamic nuclear polarization (DNP) is a methodology to increase the sensitivity of nuclear magnetic resonance (NMR) spectroscopy. It relies on the transfer of the electron spin polarization from a radical to coupled nuclear spins, driven by microwave excitation resonant with the electron spin transitions. In this work we explore the potential of pulsed multi-frequency microwave excitation in liquids. Here, the relevant DNP mechanism is the Overhauser effect. The experiments were performed with TEMPOL radicals in aqueous solution at room temperature using a Q-band frequency (1.2 T) electron paramagnetic resonance (EPR) spectrometer combined with a Minispec NMR spectrometer. A fast arbitrary waveform generator (AWG) enabled the generation of multi-frequency pulses used to either sequentially or simultaneously excite all three 14N-hyperfine lines of the nitroxide radical. The multi-frequency excitation resulted in a doubling of the observed DNP enhancements compared to single-frequency microwave excitation. Q-band free induction decay (FID) signals of TEMPOL were measured as a function of the excitation pulse length allowing the efficiency of the electron spin manipulation by the microwave pulses to be extracted. Based on this knowledge we could quantitatively model our pulsed DNP enhancements at 1.2 T by numerical solution of the Bloch equations, including electron spin relaxation and experimental parameters. Our results are in good agreement with theoretical predictions. Whereas for a narrow and homogeneous single EPR line continuous wave excitation leads to more efficient DNP enhancements compared to pulsed excitation for the same amount of averaged microwave power. The situation is different for radicals with several hyperfine lines or in the presence of inhomogeneous line broadening. In such cases pulsed single/multi-frequency excitation can lead to larger DNP enhancements.

Effects of acoustic parameters on nanodroplet vaporization

Phase shift nanodroplets offer a number of advantages over ordinary microbubbles due to their enhanced stability and smaller size distribution. These nanodroplets undergo a phase transition from liquid to highly echogenic gaseous state when activated by sufficient acoustic energy through a process termed acoustic droplet vaporization (ADV). In this study, we synthesized lipid-coated perfluoropentane (PFP) filled nanodroplets via sonication method. We investigated the ADV threshold of these nanodroplets as a function of acoustic parameters such as excitation pressure, frequency, pulse length, and pulse repetition period (PRP). Our results indicate that ADV threshold varies significantly with PRP; while at PRP of 10 ms, the ADV threshold was found to be 3.6 MPa (pk-pk), for PRP of 1 ms, 100 μs, and 500 μs, ADV was not observed even at 10 MPa. At ADV, fundamental and odd harmonics were found to be significantly higher than the background noise. The acoustic response of ordinary perfluorobutane (PFB) filled microbubbles with the same lipid composition is compared to that of PFP nanodroplets when both were excited with the same excitation pressures (450 kPa to 10 MPa). Above ADV threshold both showed a similar response.

The influence of the excitation pulse length on ultrafast magnetization dynamics in nickel.

The laser-induced demagnetization of a ferromagnet is caused by the temperature of the electron gas as well as the lattice temperature. For long excitation pulses, the two reservoirs are in thermal equilibrium. In contrast to a picosecond laser pulse, a femtosecond pulse causes a non-equilibrium between the electron gas and the lattice. By pump pulse length dependent optical measurements, we find that the magnetodynamics in Ni caused by a picosecond laser pulse can be reconstructed from the response to a femtosecond pulse. The mechanism responsible for demagnetization on the picosecond time scale is therefore contained in the femtosecond demagnetization experiment.

Theoretical study of time-resolved luminescence in semiconductors. II. Pulsed excitation

In the second part of this series, we studied TRL decay on semiconductor layers and thin film homostructures after a pulsed excitation by simulation with Synopsys TCAD® and by mathematical approximation. Again, our working example is Cu(In,Ga)Se2. We investigate the influence of the excitation pulse length, axial diffusion, bulk-defects, and defects at the contacts, as well as space charge on the TRL-decay separately by quasi one-dimensional simulations of semiconductor layers and semiconductor homostructures. Material parameters like defect density, carrier mobility, and surface recombination velocity are varied in a wide range, such that the calculations are applicable to other semiconductors. We further study the influence of multi-pulse excitation. We show how material parameters such as carrier lifetime and carrier mobility can be extracted from the TRL transients and how the samples can be characterized by excitation dependent measurements in the open circuit case. We can explain some effects found in luminescence experiments, like an increased decay in semiconductor junctions due to the electric field in the space charge region. However, we also discuss the effect of charge storage which may lead to decreased decay. It is revealed that under high injection conditions single layers within a semiconductor stack can be characterized in terms of carrier lifetime.

Investigation on the relationship between overpressure and sub-harmonic response from encapsulated microbubbles

Sub-harmonic component generated from microbubbles is proven to be potentially used in noninvasive blood pressure measurement. Both theoretical and experimental studies are performed in the present work to investigate the dependence of the sub-harmonic generation on the overpressure with different excitation pressure amplitudes and pulse lengths. With 4-MHz ultrasound excitation at an applied acoustic pressure amplitude of 0.24 MPa, the measured sub-harmonic amplitude exhibits a decreasing change as overpressure increases; while non-monotonic change is observed for the applied acoustic pressures of 0.36 MPa and 0.48 MPa, and the peak position in the curve of the sub-harmonic response versus the overpressure shifts toward higher overpressure as the excitation pressure amplitude increases. Furthermore, the exciting pulse with long duration could lead to a better sensitivity of the sub-harmonic response to overpressure. The measured results are explained by the numerical simulations based on the Marmottant model. The numerical simulations qualitatively accord with the measured results. This work might provide a preliminary proof for the optimization of the noninvasive blood pressure measurement through using sub-harmonic generation from microbubbles.

Transient Analysis of THz-QCL Pulses Using NbN and YBCO Superconducting Detectors

We report the time-domain analysis of fast pulses emitted by a quantum cascade laser (QCL) operating at ~ 3.1 THz using superconducting THz detectors made from either NbN or YBa2Cu3O7-δ (YBCO) thin films. The ultrafast response from these detectors allows resolution of emission features occurring on a nanosecond time-scale, which is not possible with commercially available Ge or InSb bolometers owing to their much larger time constants. We demonstrate that the time-dependent emission can be strongly affected by relatively small variations in the driving pulse. The QCL output power-current relationship was determined, based on correlation of the time-dependent emission of radiation with current flow in the QCL, under different QCL bias conditions. We show that this relationship differs from that obtained using bolometric detectors that respond only to the integrated pulse energy. The linearity of the detectors, and their agreement with measurements using a Ge bolometer, was also established by studying the QCL emission as a function of bias voltage and excitation pulse length. This measurement scheme could be readily applied to the study of ultrafast modulation and mode-locking of THz-QCLs.

Diagnostic potential of chronoaximetric electrodiagnostics in the assessment of denervation-induced defects of m. soleus in patients with diabetic neuropathy

The study was designed to elucidate the informative value of chronaximetry for the quantitative assessment of denervation-induced defects of m. soleus in patients with diabetic neuropathy. Conditions are clarified under which chronaximetric measurements disagree with the position of the IT hyperbola; this discrepancy lowers substantially the informative value of these characteristics as a measure of the degree of manifestation of diabetic neuropathy. The value of chronaximetry for this purpose is markedly surpassed by that of the position of the vertex of IT hyperbola. Two approaches are proposed to the simplified and exact calculation of the position of the vertex of IT hyperbola. The length of the excitation pulse obtained by these methods (CRP6 and TGT parameters) may be used, similar to chronaximetric measurements, both for the evaluation of neuropathic changes and for the choice of optimal electrostimulation technique.

2D NMR Nutation Analysis of Non-Thermal Polarization of Coupled Multi-Spin Systems

Abstract A new, convenient method of analyzing the spin polarization of a non-equilibrium system of N coupled nuclei is described and applied to photo-reactions exhibiting chemically induced dynamic nuclear polarization (CIDNP). It is based on the Fourier analysis of the variation of NMR line intensities as a function of the radio frequency excitation pulse length. A relationship between the spectral components at various harmonic order and the alignment in the spin multiplet is established. In application to the Norrish type I photolysis of cyclodecanone we demonstrate that at low magnetic field the rate determining step in the reaction kinetics depends on the mutual orientation of at least four pairs of non-equivalent spins.

A novel approach to the aperture windowing in medical imaging

A new technique is proposed to improve the lateral resolution in the conventional B-mode imaging systems, which enables a simple array aperture windowing in the transmitting mode. Amplitude shaping is performed without modifying the transmitting voltage of the array elements, but only varying the excitation pulse length from one element to another. This method presents some attractive practical advantages, and the reduction of the sidelobe energy is comparable to that attainable with a conventional aperture windowing. Parametric plots are given, which transform an amplitude apodization into a `time apodization' for any type of transducer array.

Optimized multiple-quantum magic-angle spinning NMR experiments on half-integer quadrupoles

It has been recently shown that second-order anisotropies can be removed from solid phase NMR spectra of quadrupolar nuclei via the combined use of magic-angle spinning (MAS) and bidimensional multiple-quantum (MQ) spectroscopy. The present study investigates the conditions under which the acquisition of such high-resolution MQMAS NMR spectra are optimized. The excitation and conversion pulse lengths that maximize 0 → ±3( t 1) → − 1 ( t) 2) coherence transfer pathway signals for arbitrary spin numbers were calculated, as were the pulse lengths that provide NMR spectra free from dispersive line shape distortions. For the case of spin-5/2 nuclei, the conditions which optimize experiments involving quintuplequantum coherences were also determined.

Application of the three-level model: Rise and decay kinetics of the temperature-dependent emission of metal ions withs 2-valence electron configuration

Temperature-dependent rise time and lifetime results, by measuring the photon emission in the temperature range 10–200 K, were obtained on cis-(NEt4)2[TeCl4Br2]2-(C2v) and [SeCl6]2-(Oh). The kinetics of excitation and relaxation are described by a three-level model containing transition rate constants which are related to different symmetry selection rules between corresponding electronic levels. The transient emission can be modified by varying the excitation pulse length. Besides a slow component in the luminescence decay-curve (0.5 ms atT = 12 K) a second, faster component can be detected. The amplitude ratio of these components can be increased by decreasing the excitation pulse length, which can be explained by assuming non-thermally equilibrated excited states. The results allow the assignment of the lowest levels which arise from the excitedsp electron configuration of the central ion.

Pure rotational spectra of the mixed rare gas van der Waals complexes Ne–Xe, Ar–Xe, and Kr–Xe

Pure rotational transitions in the vibrational ground states of various isotopomers of the heteronuclear rare gas dimers Ne–Xe, Ar–Xe, and Kr–Xe have been measured using a pulsed molecular beam cavity microwave Fourier transform spectrometer. Rotational and centrifugal distortion constants have been obtained, and have yielded estimates of the lengths of the van der Waals bonds and of their harmonic vibration frequencies. Effects due to nuclear quadrupole coupling have been observed in 131Xe-containing complexes and have yielded the corresponding nuclear quadrupole coupling constants. The electric molecular dipole moments of the complexes have been estimated from the excitation pulse lengths, optimized for maximum signal strength (π/2 condition).

Extra resonances in time-domain four-wave mixing

We show that extra resonances, such as those caused in frequency-domain nonlinear wave mixing by pure dephasing or laser fluctuations, can also be induced by operation in the time domain. These pulse-length-induced extra resonances arise in transient-grating experiments when the laser pulses are short enough that a steady state cannot be achieved during the excitation process. We show theoretically that these resonances increase in strength with decreasing excitation pulse length until the pulse length becomes shorter than the dephasing time of the medium and quote an experimental example to support this interpretation.