We demonstrate the use of spectrograms of the field-induced second-harmonic (FISH) signal generated in ambient air, to reconstruct the absolute temporal electric field of ultra-broadband terahertz-infrared (THz-IR) pulses with bandwidths exceeding 100 THz. The approach is applicable even with relatively long (150-femtosecond) optical detection pulses, where the relative intensity and phase can be extracted from the moments of the spectrogram, as demonstrated by transmission spectroscopy of very thin samples. Auxiliary EFISH/ABCD measurements are used to provide the absolute field and phase calibration, respectively. We take into account the beam-shape/propagation effects about the detection focus on the measured FISH signals, which affect the field calibration, and show how an analysis of a set of measurements vs. truncation of the unfocused THz-IR beam can be used to correct for these. This approach could also be applied to the field calibration of ABCD measurements of conventional THz pulses.
We investigate experimentally both the amplitude and phase channels of the collective modes in the quasi-1D charge-density-wave (CDW) system, K0.3MoO3, by combining (i) optical impulsive-Raman pump-probe and (ii) terahertz time-domain spectroscopy (THz-TDS), with high resolution and a detailed analysis of the full complex-valued spectra in both cases. This allows an unequivocal assignment of the observed bands to CDW modes across the THz range up to 9 THz. We revise and extend a time-dependent Ginzburg-Landau model to account for the observed temperature dependence of the modes, where the combination of both amplitude and phase modes allows one to robustly determine the bare-phonon and electron-phonon coupling parameters. While the coupling is indeed strongest for the lowest-energy phonon, dropping sharply for the immediately subsequent phonons, it grows back significantly for the higher-energy phonons, demonstrating their important role in driving the CDW formation. We also include a reassessment of our previous analysis of the lowest-lying phase modes, whereby assuming weaker electronic damping for the phase channel results in a qualitative picture more consistent with quantum-mechanical treatments of the collective modes, with a strongly coupled amplitudon and phason as the lowest modes.
We re-examine the effect of long-range Coulomb interactions on the collective amplitude and phase modes in the incommensurate charge-density wave ground state of quasi-one-dimensional conductors. Using an effective action approach we show that the longitudinal acoustic phonon protects the gapless linear dispersion of the lowest phase mode in the presence of long-range Coulomb interactions. Moreover, in Gaussian approximation amplitude fluctuations are not affected by longrange Coulomb interactions. We also calculate the collective mode dispersions at finite temperatures and compare our results with the measured energies of amplitude and phase modes in K0.3MoO3. With the exception of the lowest phase mode, the temperature dependence of the measured mode energies can be quantitatively described within a multi-phonon Fröhlich model neglecting long-range Coulomb interactions.
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