Impact of the terahertz and optical pump penetration depths on generated strain waves temporal profiles in a V2O3 thin film.

Triggering new stable macroscopic orders in materials by ultrafast optical or terahertz pump pulses is a difficult challenge, complicated by the interplay between multiscale microscopic mechanisms, and macroscopic excitation profiles in samples. In particular, the differences between the two types of excitations are still unclear. In this article, we compare the optical response on acoustic timescale of a V2O3 Paramagnetic Metallic (PM) thin film excited by a terahertz (THz) pump or an optical pump, at room temperature. We show that the penetration depth of the deposited energy has a strong influence on the shape of the optical transmission signal, consistent with the modulation of permittivity by the superposition of depth-dependent static strain, and dynamical strain waves travelling back and forth in the sample layer. In particular, the temporal modulation of the optical transmission directly reflects the excitation profile as a function of depth, as well as the sign of the acoustic reflection coefficient between the film and the substrate. The acoustic mismatch between the V2O3 layer and the substrate was also measured. The raw data were interpreted with a one-dimensional analytical model, using three fitting parameters only. These results are discussed in the context of triggering phase transitions by ultrafast pump pulses. To the best of our knowledge, this is the first report of the modulation of the optical transmission of V2O3 with a THz pump within the acoustic timescale.

Repetitive experiments of one or two-pulse sequences in NQR of spins I=3/2: Liouville space, steady-state, Ernst angle and optimum signal.

In NMR, the repetition of pulse sequences with a recycle time that does not allow the spin system to completely relax back to equilibrium is a well known and often used method to increase the signal to noise ratio at given total measuring time. For isolated spins I=1/2, the steady-state of a train of strictly identical pulse sequences separated by free evolution periods of same duration is described by the well known Ernst-Anderson model, and the optimum pulse angle is given by the Ernst angle. We showed recently that equivalent formula, but with super-operators in the Liouville space, can be obtained for general spins I. In this article, this formalism is generalized to pure NQR of spins I=3/2, and applied to calculate the signal resulting from single and solid-echo sequences, in the limit when the recycle time T>5T2q, where T2q is the transverse (coherence) quadrupolar relaxation time. In particular, we show that powder samples have a behaviour that is very close to NMR of spins I=1/2. For instance, the generalized Ernst angle ßM that maximizes the signal amplitude for a single pulse train is well described by the simple formula cos(1.52ßM)≈exp(-T/T1q), whatever the quadrupolar asymmetry parameter η, T1q being the longitudinal (population) quadrupolar relaxation time. Moreover, a simplified NMR-like formula that describes the overall behaviour of nutation curves is proposed, and it is shown that the signal to noise ratio (SNR) at given experimental time is exactly the same as in NMR of spins I=1/2 as a function of recycle time, when properly normalized. Some theoretical predictions for the single pulse and solid-echo sequence were compared to experiments, and validated, by performing 35Cl pure NQR experiment on chloranil (C6Cl4O2 tetrachloro-1,4-benzoquinone) powder.

Quadrupolar solid-state NMR and repetitive experiments: Some aspects in the Liouville space. Application to spins I=1.

The aim of this work is to generalize the Ernst-Anderson model developed to account of the steady-state regime of isolated spins I=1/2 subject to a train of strictly identical pulse sequences separated by free evolution periods of same duration. We generalize this model to the general case of spins I≥1 and general pulse sequence within the framework of the Liouville space. In particular, it is proved that under reasonable assumptions, a well defined steady-state regime is reached which is independent of the initial conditions. The general formal expressions obeyed by the steady-state density operator are given as a function of pulse propagators and relaxation operator for single and two-pulse sequences. In solid-state NMR where recycle time can be made, at the same time, much longer than typical coherence relaxation times and smaller than typical population relaxation times, further simplification leads to more tractable formula. As an example, the formalism is applied to I=1 spins with hard and soft single pulse sequence, or to the solid echo sequence. In particular, we were able to generalize the Ernst-Anderson formula to spins I=1. The pertinence of the theory is verified by comparing the theoretical and numerical simulations outputs to 2H single crystal experiments performed on nonadecane/urea C19D40/urea-H4 compound.

Evaluation of area-based collagen scoring by nonlinear microscopy in chronic hepatitis C-induced liver fibrosis.

In this paper we analyze a fibrosis scoring method based on measurement of the fibrillar collagen area from second harmonic generation (SHG) microscopy images of unstained histological slices from human liver biopsies. The study is conducted on a cohort of one hundred chronic hepatitis C patients with intermediate to strong Metavir and Ishak stages of liver fibrosis. We highlight a key parameter of our scoring method to discriminate between high and low fibrosis stages. Moreover, according to the intensity histograms of the SHG images and simple mathematical arguments, we show that our area-based method is equivalent to an intensity-based method, despite saturation of the images. Finally we propose an improvement of our scoring method using very simple image processing tools.

Comparison between two treatment planning systems for volumetric modulated arc therapy optimization for prostate cancer.

PURPOSE: To investigate the performances of two commercial treatment planning systems (TPS) for Volumetric Modulated Arc Therapy (VMAT) optimization regarding prostate cancer. The TPS were compared in terms of dose distributions, treatment delivery parameters and quality control results. MATERIALS AND METHODS: For ten patients, two VMAT plans were generated: one with Monaco TPS (Elekta) and one with Pinnacle TPS (Philips Medical Systems). The total prescribed dose was 78 Gy delivered in one 360° arc with a Synergy(®) linear accelerator equipped with a MLCi2(®). RESULTS: VMAT with Monaco provided better homogeneity and conformity indexes but lower mean dose to PTVs than Pinnacle. For the bladder wall (p = 0.019), the femoral heads (p = 0.017), and healthy tissues (p = 0.005), significantly lower mean doses were found using Monaco. For the rectal wall, VMAT with Pinnacle provided a significantly (p = 0.047) lower mean dose, and lower dose into 50% of the volume (p = 0.047) compared to Monaco. Despite a greater number of monitor units (factor 1.5) for Monaco TPS, the total treatment time was equivalent to that of Pinnacle. The treatment delivery parameter analysis showed larger mean MLC area for Pinnacle and lower mean dose rate compared to Monaco. The quality control results gave a high passing rate (>97.4%) for the gamma index for both TPS but Monaco provided slightly better results. CONCLUSION: For prostate cancer patients, VMAT treatment plans obtained with Monaco and Pinnacle offered clinically acceptable dose distributions. Further investigations are in progress to confirm the performances of the two TPS for irradiating more complex volumes.

Measuring the scattering coefficient of turbid media from two-photon microscopy.

In this paper, we propose a new and simple method based on two-photon excitation fluorescence (TPEF) microscopy to measure the scattering coefficient µ(s) of thick turbid media. We show, from Monte Carlo simulations, that µ(s) can be derived from the axial profile of the ratio of the TPEF signals epi-collected by the confocal and the non-descanned ports of a scanning microscope, independently of the anisotropy factor g and of the absorption coefficient µ(a) of the medium. The method is validated experimentally on tissue-mimicking optical phantoms, and is shown to have potential for imaging the scattering coefficient of heterogeneous media.

A robust collagen scoring method for human liver fibrosis by second harmonic microscopy.

Second Harmonic Generation (SHG) microscopy offers the opportunity to image collagen of type I without staining. We recently showed that a simple scoring method, based on SHG images of histological human liver biopsies, correlates well with the Metavir assessment of fibrosis level (Gailhouste et al., J. Hepatol., 2010). In this article, we present a detailed study of this new scoring method with two different objective lenses. By using measurements of the objectives point spread functions and of the photomultiplier gain, and a simple model of the SHG intensity, we show that our scoring method, applied to human liver biopsies, is robust to the objective's numerical aperture (NA) for low NA, the choice of the reference sample and laser power, and the spatial sampling rate. The simplicity and robustness of our collagen scoring method may open new opportunities in the quantification of collagen content in different organs, which is of main importance in providing diagnostic information and evaluation of therapeutic efficiency.

Fibrillar collagen scoring by second harmonic microscopy: a new tool in the assessment of liver fibrosis.

BACKGROUND & AIMS: Imaging of supramolecular structures by multiphoton microscopy offers significant advantages for studying specific fibrillar compounds in biological tissues. In this study, we aimed to demonstrate the relevance of Second Harmonic Generation (SHG) for assessing and quantifying, without staining, fibrillar collagen in liver fibrosis. METHODS: We first showed the relationship between SHG signal and collagen forms over-produced and accumulated during fibrosis progression. Taking this property into consideration, we developed an innovative method to precisely quantify the fibrosis area in histological slices by scoring of fibrillar collagen deposits (Fibrosis-SHG index). RESULTS: The scoring method was routinely applied to 119 biopsies from patients with chronic liver disease allowing a fast and accurate measurement of fibrosis correlated with the Fibrosis-Metavir score (rho=0.75, p<0.0001). The technique allowed discriminating patients with advanced (moderate to severe) fibrosis (AUROC=0.88, p<0.0001) and cirrhosis (AUROC=0.89, p<0.0001). Taking advantage of its continuous gradation, the Fibrosis-SHG index also allowed the discrimination of several levels of fibrosis within the same F-Metavir stage. The SHG process presented several advantages such as a high reliability and sensitivity that lead to a standardized evaluation of hepatic fibrosis in liver biopsies without staining and pathological examination. CONCLUSIONS: Second harmonic microscopy emerges as an original and powerful tool in the assessment of liver fibrosis and offers new possibilities for the evaluation of experimental protocols. We expect that this technology could easily be applicable in the study of other fibro-proliferative pathologies.

Second harmonic microscopy of axonemes.

We performed Second Harmonic Microscopy of axonemes obtained from sea urchin sperm. Using polarization analysis and a trade-off between signal and photodamage, we were able to determine, for the first time to our knowledge, the nonlinear susceptibility chizxx/chixzx = 1.1+/-0.2 and chizzz/chixzx = 4+/-0.5 of axonemes.

Collagen and myosin characterization by orientation field second harmonic microscopy.

Collagen and myosin fibrils are endogenous harmonophores that both give rise to Second Harmonic Generation (SHG). By combining four polarization SHG images provided by a scanning microscope, we show that the orientation of the principal axis of the nonlinear susceptibility tensor chi(2) can be determined for each pixel of the image. The ratio rho = chi33/chi15 of the principal components of chi(2) of collagen and myosin was obtained with the same method, and found within the range 1.6-1.8 and 0.5-0.6 respectively. The orientation of the principal axis of chi(2) is shown to be correlated to the orientation of the fibrils themselves. This provides a straightforward method, which we call Orientation Field-Second Harmonic Microscopy (OF-SHM), to reconstruct orientation fields of fibrils at various scales and resolutions in different biological systems (from muscle sarcomere to the whole embryo).

Hidden degrees of freedom in aperiodic materials.

Numerous crystalline materials, including those of bioorganic origin, comprise incommensurate sublattices whose mutual arrangement is described in a superspace framework exceeding three dimensions. We report direct observation by neutron diffraction of superspace symmetry breaking in a solid-solid phase transition of an incommensurate host-guest system: the channel inclusion compound of nonadecane/urea. Strikingly, this phase transition generates a unit cell doubling that concerns only the modulation of one substructure by the other-an internal variable available only in superspace. This unanticipated pathway for degrees of freedom to rearrange leads to a second phase transition, which again is controlled by the higher dimensionality of superspace. These results reveal nature's capacity to explore the increased number of phases allowed in aperiodic crystals.

Critical behavior of KDCO3 from 2H and 39K single crystal NMR.

Potassium hydrogenocarbonate KDCO3 presents an order/disorder phase transition at Tc approximately 353 K. The critical behavior of this phase transition was studied by single crystal 2H and 39K NMR. The evolution of the order parameter as a function of temperature is quantified, and the critical exponent was determined, indicating a transition close to a tricritical point. The 2H Zeeman relaxation rate is strongly increased near the transition temperature. By calculating the noncritical contribution to the Zeeman relaxation rate, we show that the observed relaxation rate clearly presents a pseudo-divergent behavior near Tc, with a logarithmic singularity. The nature of the phase transition is discussed in the light of these results.

Evidence of a phase transition of RbHCO3 from high-resolution solid-state 13C and 87Rb NMR by comparison with KHCO3.

A variable-temperature high-resolution 13C and 87Rb solid-state NMR study of powder rubidium hydrogencarbonate, RbHCO3, is presented for the first time. At ambient temperature, RbHCO3 is formed by centrosymmetric dimers linked by hydrogen bonds, but almost no information is available on this compound concerning proton disorder and the low-temperature phase. However, potassium hydrogencarbonate, KHCO3, which has an isomorphic structure for the high temperature phase, was well studied: it undergoes a non-ferroic, non-ferroelectric phase transition at Tc = 318 K between two monoclinic structures. The protons are disordered in an asymmetric double-well potential in the low-temperature phase, and the double-well potential becomes symmetric in the high-temperature phase. By comparison with recent solid-state NMR experimental results on KHCO3, we show that RbHCO3 undergoes a phase transition at Tc approximately 245 K, and give evidence that the proton dynamic disorder in both compounds is very similar.