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Figure 7 shows also that PET, when under irradiation, becomes unstable [20] and [21]. In zone 2, an exothermic peak characteristic of the crystallization of a material is seen. The irradiated PET which has a semi crystalline structure with Xc equal to Figure 7. The decrease in Tg could be the result of chain breaks which have the effect of reducing the number of junction points and thus increasing molecular mobility [22].

In fact, irradiation in the presence of oxygen generally leads to more chain splitting than under neutral gas [23].

The cross linking involves radical coupling, and in a medium rich in oxygen, these molecules react rapidly with the radicals and prevent recombination and therefore the cross linking of the polymer [24]. The appearance of an endothermic peak near the glass transition temperature reflects the physical aging of the irradiated PET as exposed by Vigier [20].

This aging is attributed to the formation of radicals within the amorphous material after irradiation. These radicals are trapped in the vitreous material and can cause slow and gradual changes in the network when maintained at a temperature below the glass transition temperature [25]. We present now the main results obtained by comparing the two types of samples from the BDS analysis.

Figure 8 shows the loss factor as a function of frequency for temperatures below the glass transition temperature for irradiated PET. Figure 8. These values are the consequence of the existence of an extrinsic parasitic series resistance to the sample as suggested by Runt [12].

This increase does not exist for non-irradiated PET as shown in Figure 4. Comparison of the two figures shows closer spectra for irradiated PET that could be associated with a dehydration of PET during irradiation. Figure 9 shows the relaxation time temperature dependence.

We have an Arrhenius trend characterizing molecular localized mobility for the blank PET. And a tendency Vogel-Fulcher-Tammann law characterizing a cooperative mobility of molecules and so a large molecular mobility in the irradiated PET.

It would reveal a molecular chain scission due to irradiation. Figure 9. Electric field irradiation affects structural properties of PET so that it is characterized in this case by semi-crystalline and heterogeneous structure depending on the phenomenon of charge injection into the volume because it presents a place of trapping for the load to inject.

The closer thermal spectra of loss factor for irradiated PET could be associated with a dehydration of PET during irradiation. The tendency Vogel Fulcher - Tammann law in the irradiated PET characterize a cooperative mobility of molecules; it would reveal a molecular chain scission due to electric field irradiation.

Graphical method for the Debye-like relaxation spectra analysis. Journal of Non-Crystalline Solids, vol. Part II. Low temperature thermal oxidation," Polymer Degradation and Stability, vol. Interfaces, vol. Doctorat thesis," Joseph Fourrier University , Grenoble, vol. The ultrafast reversibility of the at the photon energy BvXUV , and d is the thickness of the sample. We effects implies that the physical properties of a dielectric can be first discuss XUV absorption near the edge of the conduction band.

NIR field plotted in Fig. It reveals a large. The ial. When the strength of the electric field F approaches the criti- measurement resolves condensed-matter processes driven by the cal field strength, inducing a change in electron potential energy by instantaneous field of visible light.

Briefly, it is based on the time- trics calls for sub-femtosecond temporal resolution. For a detailed description, see Supplementary few-femtosecond near-infrared NIR laser pulses.

The model accurately predicts the magnitude and the In a first set of experiments, the waveform-controlled linearly pola- sub-femtosecond temporal structure of the observed modulation in rized field, FL t , of NIR laser pulses of less than 4 fs carrier wave- strength Fig.

Agreement in the phase of these parallel to the laser field, impinged collinearly on a free-standing modulations with respect to the oscillating laser field Fig. TOF, time of flight. Supplementary Information. To ensure the highest contrast for the subsequent pump— —1 probe study see below , this measurement was implemented with —2 2. The inset shows the evolution of A in a more extended delay range, Delay fs 1.

The error bar in b represents LDOS the standard error of the average over 15 spectral lineouts within the energy 0. The dashed c The process is fully reversible for several thousand laser shots before SiO2 irreversible damage occurs owing to self-focusing inside the sample rather than wedge on the surface. The data points are averaged over 3, laser pulses error bars Pump represent the standard deviation.

Inset, schematic illustration of the pump— 0. The curve is the result of an average of ten scans; for representative 1 2 2.

The grey shading represents the experimental value of the optical breakdown threshold, as S —TL determined from the reflectance measurement yielding the data shown in a. Our observation thus provides com- pelling evidence, in a model-independent manner, for the substantial Maximum conduction-band —1 e 20 reversibility of the strong-field-induced increase in polarizability on the Measured timescale of the optical wave cycle.

This effect is accompanied by a field-induced transient 0 population and subsequent depopulation of the conduction band, —6 —4 —2 0 2 4 6 confined, again, to several femtoseconds see Fig. Thus, our model also correctly predicts the incidence p-polarized. The dependence on the field strength was extremely nonlinear, closely resembling that of the field-induced threshold for optical breakdown Fig.

Both the nonlinear polari- current Our model is not yet applicable to an oblique angle of zation and the conduction band population induced by the strong incidence but did correctly predict the field-strength-dependence of field return to near-zero immediately after the laser pulse for the current This is fully consistent with the abrupt decay of current and reflectivity points to their common physical origin: the field-induced transient NIR reflectivity and XUV absorption bleach- field-enhanced polarizability.

This points towards the also turned off by the field? Although the XUV bleaching already sug- reversible, Hamiltonian nature of the laser-induced dynamics up to the gests that the latter is more likely, we sought additional evidence using critical field strength. To this end, we split the incident Our quantum mechanical model identifies light-field-induced re- pulse into a strong pump and a weak probe beam, with the sum of the versible changes of the local density of states Fig.

The probe beam was isolated with an iris in front of the detector mea- without parameter adjustment provides convincing evidence of the suring the reflected probe pulse energy as a function of pump—probe delay.

Considerations presented in ref. The field-induced strong transient localization of states is expected to occur in all bands, 1. Zener, C. A theory of the electrical breakdown of solid dielectrics. A , — Wannier, G. Wave functions and effective Hamiltonian for Bloch electrons in an localized at the same site of the lattice. The energy levels of such electric field.

Franz, W. A 13, Keldysh, L. Behavior of non-metallic crystals in strong electric fields. L-band and conduction band nearly unchanged.

Hence, XUV prob- Theor. Mizumoto, Y. Dressed-band shifts observed in Fig.