Investigation of Dielectric Properties of Polymers and their Discrimination Using Terahertz Time-Domain Spectroscopy with Principal Component Analysis.

Polymers are among the most commonly used materials in our everyday life. They are generally transparent to terahertz (THz) radiation, but are quite difficult to differentiate using optical techniques as few or no characteristic features exist in the spectral range of <2.0 THz for small and portable radiation systems. In this work, we report experimental measurement of refractive indices and absorption coefficients of styrene acrylonitrile (SAN) and Bakelite in the spectral range of 0.2-2.0 THz for the first time. Additionally, we demonstrate that by combining principle component analysis (PCA) with THz time-domain spectroscopy one can differentiate such polymers. In this analysis, the first three principle components PC1, PC2, and PC3 depict >94% variance with a distribution of 72.45%, 11.52%, and 9.38%, respectively.

Isolated attosecond pulse generation without the need to stabilize the carrier-envelope phase of driving lasers.

Single isolated attosecond pulses can be extracted from a pulse train with an ultrafast gate in the generation target. By setting the gate width sufficiently narrow with the generalized double optical gating, we demonstrate that single isolated attosecond pulses can be generated with any arbitrary carrier-envelope phase value of the driving laser. The carrier-envelope phase only affects the photon flux, not the pulse duration or contrast. Our results show that isolated attosecond pulses can be generated using carrier-envelope phase unstabilized 23 fs pulses directly from chirped pulse amplifiers.

Characterizing ultrabroadband attosecond lasers.

Recent progress in sub-laser-cycle gating of high-order harmonic generation promises to push the limits on optical pulse durations below the atomic unit of time, 24 as, which corresponds to a bandwidth broader than 75 eV. However, the available techniques for attosecond pulse measurement are valid only for narrow-bandwidth spectra, due to one of the key approximations made in the phase retrieval. Here we report a new technique for characterizing attosecond pulses, whereby the spectral phase of the attosecond pulse is extracted from the oscillation component with the dressing laser frequency in the photoelectron spectrogram. This technique, termed PROOF (Phase Retrieval by Omega Oscillation Filtering), can be applied to characterizing attosecond pulses with ultrabroad bandwidths.

Calibration of electron spectrometer resolution in attosecond streak camera.

We report a new method for determining the energy resolution of time-of-flight spectrometers for detecting photoelectrons produced with attosecond XUV pulses. By measuring the width of the 2s2p autoionization line of helium, we found the resolution of our spectrometer to be approximately 0.6 eV for electrons at 35.5 eV. Furthermore, the resolution in the 10 to 35 eV range was determined by applying a retarding potential at the entrance of the drift tube.

Extreme ultraviolet supercontinua supporting pulse durations of less than one atomic unit of time.

Double optical gating of high-harmonic generation was used to obtain supercontinuous spectra in the extreme UV (XUV) region including the water window. The spectra supported a 16 as pulse duration that is below one atomic unit of time (24 as). The dependence of the gated spectra on the carrier-envelope phase of the laser provided evidence that isolated attosecond pulses were generated. In addition, to ensure the temporal coherence of the XUV light, the pulse shape and phase of isolated 107 as XUV pulses using a portion of the spectrum were characterized by attosecond streaking.

Generation of isolated attosecond pulses with 20 to 28 femtosecond lasers.

Isolated attosecond pulses are powerful tools for exploring electron dynamics in matter. So far, such extreme ultraviolet pulses have only been generated using high power, few-cycle lasers, which are very difficult to construct and operate. We propose and demonstrate a technique called generalized double optical gating for generating isolated attosecond pulses with 20 fs lasers from a hollow-core fiber and 28 fs lasers directly from an amplifier. These pulses, generated from argon gas, are measured to be 260 and 148 as by reconstructing the streaked photoelectron spectrograms. This scheme, with a relaxed requirement on laser pulse duration, makes attophysics more accessible to many laboratories that are capable of producing such multicycle laser pulses.

Double optical gating of high-order harmonic generation with carrier-envelope phase stabilized lasers.

We demonstrated a novel optical switch to control the high-order harmonic generation process so that single attosecond pulses can be generated with multiple-cycle pulses. The technique combines two powerful optical gating methods: polarization gating and two-color gating. An extreme ultraviolet supercontinuum supporting 130 as was generated with neon gas using 9 fs laser pulses. We discovered a unique dependence of the harmonic spectra on the carrier-envelope phase of the laser fields, which repeats every 2 pi radians.

Modelling of C(2) addition route to the formation of C(60).

To understand the phenomenon of fullerene growth during its synthesis, an attempt is made to model a minimum energy growth route using a semi-empirical quantum mechanics code. C(2) addition leading to C(60) was modelled and three main routes, i.e. cyclic ring growth, pentagon and fullerene road, were studied. The growth starts with linear chains and, at n = 10, ring structures begins to dominate. The rings continue to grow and, at some point n>30, they transform into close-cage fullerenes and the growth is shown to progress by the fullerene road until C(60) is formed. The computer simulations predict a transition from a C(38) ring to fullerene. Other growth mechanisms could also occur in the energetic environment commonly encountered in fullerene synthesis, but our purpose was to identify a minimal energy route which is the most probable structure. Our results also indicate that, at n = 20, the corannulene structure is energetically more stable than the corresponding fullerene and graphene sheet, however a ring structure has lower energy among all the structures up to n≤40. Additionally, we have also proved that the fullerene road is energetically more favoured than the pentagon road. The overall growth leading to cage closure for n = 60 may not occur by a single route but by a combination of more than one route.

The degenerate Fermi gas of π electrons in fullerenes and the σ surface instabilities.

The departure from perfect spherical symmetry in the case of fullerenes (C60 being the sole exception) induces instabilities due to the stresses generated by the pentagonal protrusions in the σ-bonded surfaces. By assuming σ-π separability and treating π electrons as a degenerate Fermi gas in the two shells around the central σ structure, the resulting degeneracy pressures can further enhance the σ-surface initiated instabilities for non-icosahedral structures (especially for those C60) with large protrusions. Under certain circumstances the net degeneracy pressure across the σ surface may have a structure stabilizing effect. The role of the π-electron degeneracy in a broad range of fullerenes from C20 to C1500 and its effects on fullerene stability are investigated.