122 research outputs found

    Field-resolved studies of ultrafast light-matter interaction

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    Single-shot carrier-envelope-phase measurement in ambient air

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    The ability to measure and control the carrier envelope phase (CEP) of few-cycle laser pulses is of paramount importance for both frequency metrology and attosecond science. Here, we present a phase meter relying on the CEP-dependent photocurrents induced by circularly polarized few-cycle pulses focused between electrodes in ambient air. The new device facilitates compact single-shot, CEP measurements under ambient conditions and promises CEP tagging at repetition rates orders of magnitude higher than most conventional CEP detection schemes as well as straightforward implementation at longer wavelengths

    Low temperature dipolar echo in amorphous dielectrics: Significance of relaxation and decoherence free two level systems

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    The nature of dielectric echoes in amorphous solids at low temperatures is investigated. It is shown that at long delay times the echo amplitude is determined by a small subset of two level systems (TLS) having negligible relaxation and decoherence because of their weak coupling to phonons. The echo decay can then be described approximately by power law time dependencies with different powers at times longer and shorter than the typical TLS relaxation time. The theory is applied to recent measurements of two and three pulse dipolar echo in borosilicate glass BK7 and provides a perfect data fit in the broad time and temperature ranges under the assumption that there exist two TLS relaxation mechanisms due to TLS-phonons and TLS-TLS interaction. This interpretation is consistent with the previous experimental and theoretical investigations. Further experiments verifying the theory predictions are suggested.Comment: 10 pages, 8 figure

    A unified picture of aggregate formation in a model polymer semiconductor during solution processing

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    One grand challenge for printed organic electronics is the development of a knowledge platform that describes how polymer semiconductors assemble from solution, which requires a unified picture of the complex interplay of polymer solubility, mass transport, nucleation and, e.g., vitrification. One crucial aspect, thereby, is aggregate formation, i.e., the development of electronic coupling between adjacent chain segments. Here, it is shown that the critical aggregation temperatures in solution (no solvent evaporation allowed) and during film formation (solvent evaporation occurring) are excellent pointers to i) establish reliable criteria for polymer assembly into desired aggregates, and ii) advance mechanistic understanding of the overall polymer assembly. Indeed, important insights are provided on why aggregation occurs via a 1- or 2-step process depending on polymer solubility, deposition temperature and solvent evaporation rate; and the selection of deposition temperatures for specific scenarios (e.g., good vs bad solvent) is demystified. Collectively, it is demonstrated that relatively straightforward, concurrent in situ time-resolved absorbance and photoluminescence spectroscopies to monitor aggregate formation lead to highly useful and broadly applicable criteria for processing functional plastics. In turn, improved control over their properties and device performance can be obtained toward manufacturing sensors, energy-harvesting devices and, e.g., bioelectronics systems at high yield

    The emergence of macroscopic currents in photoconductive sampling of optical fields

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    Photoconductive field sampling enables petahertz-domain optoelectronic applications that advance our understanding of light-matter interaction. Despite the growing importance of ultrafast photoconductive measurements, a rigorous model for connecting the microscopic electron dynamics to the macroscopic external signal is lacking. This has caused conflicting interpretations about the origin of macroscopic currents. Here, we present systematic experimental studies on the signal formation in gas-phase photoconductive sampling. Our theoretical model, based on the Ramo–Shockley-theorem, overcomes the previously introduced artificial separation into dipole and current contributions. Extensive numerical particle-in-cell-type simulations permit a quantitative comparison with experimental results and help to identify the roles of electron-neutral scattering and mean-field charge interactions. The results show that the heuristic models utilized so far are valid only in a limited range and are affected by macroscopic effects. Our approach can aid in the design of more sensitive and more efficient photoconductive devices
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