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    Ultrafast Transient Holographic Microscopy

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    Nanotechnology is increasingly being applied in many emerging technologies, ranging from metamaterials to next-generation nanodrugs. A key ingredient for its success is the ability to specifically tailor ultrafast nanoscale light–matter interactions over very large areas. Unfortunately, dynamic imaging by ultrafast nanoscopy so far remains limited to very small 2D areas. This shortcoming prevents connecting single-particle observations with large-scale functionality. Here, we address this experimental challenge by combining concepts of ultrafast spectroscopy, wide-field nanoscopy, and digital holography. We introduce an ultrafast holographic transient microscope for wide-field transient nanoscale imaging with high frequency all-optical signal demodulation. We simultaneously record ultrafast transient dynamics of many individual nano-objects and demonstrate time-resolved spectroscopy of gold nanoparticles over a large volume irrespective of their x–y–z position. Our results pave the way to single-shot 3D microscopy of 2D and 3D materials on arbitrary time scales from femtosecond carrier dynamics in optoelectronic materials to millisecond dynamics in complex tissues

    Widefield phototransient imaging for visualizing 3D motion of resonant particles in scattering environments

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    : Identifying, visualising and ultimately tracking dynamically moving non-fluorescent nanoparticles in the presence of non-specific scattering is a long-standing challenge across the nano- and life-sciences. In this work we demonstrate that our recently developed ultrafast holographic transient (UHT) microscope is ideally suited for meeting this challenge. We show that UHT microscopy allows reliably distinguishing off-resonant, dielectric, from resonant, metallic, nanoparticles, based on the phototransient signal: a pre-requisite for single-particle tracking in scattering environments. We then demonstrate the capability of UHT microscopy to holographically localize in 3D single particles over large volumes of view. Ultimately, we combine the two concepts to simultaneously track several tens of freely diffusing gold nanoparticles, within a 110 × 110 × 110 μm volume of view at an integration time of 10 ms per frame, while simultaneously recording their phototransient signals. The combined experimental concepts outlined and validated in this work lay the foundation for background-free 3D single-particle tracking applications or spectroscopy in scattering environments and are immediately applicable to systems as diverse as live cells and tissues or supported heterogeneous catalysts

    Ultrabroadband Optical Diffraction Tomography

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    Optical diffraction tomography (ODT) is a powerful noninvasive 3D imaging technique, but its combination with broadband light sources is difficult. In this study, we introduce ultrabroadband ODT, covering over 150 nm of visible spectral bandwidth with a lateral spatial resolution of 150 nm. Our work addresses a critical experimental gap by enabling the measurement of broadband refractive index changes in 3D samples, crucial information that is difficult to assess with existing methodologies. We present broadband, spectrally resolved ODT images of HeLa cells, obtained via pulse-shaping-based Fourier transform spectroscopy. The spectral observations enabled by ultrabroadband ODT, combined with material-dependent refractive index responses, allow for precise three-dimensional identification of nanoparticles within cellular structures. Our work represents a crucial step toward time and spectrally resolved tomography of complex 3D structures with implications for life and materials science applications.</p

    Understanding molecular dynamics with coherent vibrational spectroscopy in the time-domain

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    This thesis describes the development of several spectroscopic methods based on impulsive vibrational spectroscopy as well as of the technique itself. The first chapter describes the ultrafast time domain Raman spectrometer including the development of two noncollinear optical parametric amplifiers for sub-10 fs pulse generation with 343 or 515 nm pumping. In the first spectroscopic study we demonstrate, for the first time, that impulsive vibrational spectroscopy can be used for recording transient Raman spectra of molecules in excited electronic states. We obtain spectra of beta-carotene with comparable, or better, quality than established frequency domain based nonlinear Raman techniques. The following two chapters address the questions on the fate of vibrational coherences when generated on a reactive potential energy surface. We photoexcite bacteriorhodopsin and observe anharmonic coupling mediated vibrational coherence transfer to initially silent vibrational modes. Additionally, we are able to correlate the vibrational coherence activation with the efficiency of the isomerisation reaction in bR. Upon generation of vibrational coherence in the second excited electronic state of beta-carotene, by excitation from the ground electronic state, we are able to follow the wavepacket motion out of the Franck-Condon region. We observe vibrationally coherent internal conversion, through a conical intersection, into the first excited electronic state and are hence able to demonstrate that electronic surface crossings can occur in a vibrationally coherent fashion. Additionally, we find strong evidence for vibronic coupling mediated back and forth crossing between the two electronic states. As a combination of this work we develop a IVS based technique that allows for the direct recording of background and baseline free Raman spectra in the time domain. Several proof of principle experiments highlight the capabilities of this technique for time resolved Raman spectroscopy. In the final chapter we present work on weak-field coherent control. Here, we address the question of whether a photochemical reaction can be controlled by the phase term of an electric excitation field, in the one photon excitation limit. We study the systems rhodamine 101, bacteriorhodopsin, rhodopsin and isorhodopsin and, contrary to previous reports, find no evidence for one photon control

    Going Beyond Counting First Authors in Author Co-citation Analysis

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    The present study examines one of the fundamental aspects of author co-citation analysis (ACA) - the way co-citation counts are defined. Co-citation counting provides the data on which all subsequent statistical analyses and mappings are based, and we compare ACA results based on two different types of co-citation counting - the traditional type that only counts the first one among a cited work's authors on the one hand and a non-traditional type that takes into account the first 5 authors of a cited work on the other hand. Results indicate that the picture produced through this non-traditional author co-citation counting contains more coherent author groups and is therefore considerably clearer. However, this picture represents fewer specialties in the research field being studied than that produced through the traditional first-author co-citation counting when the same number of top-ranked authors is selected and analyzed. Reasons for these effects are discussed

    Variations on the Author

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    “Variations on the Author” discusses two of Eduardo Coutinho’s recent films (Um Dia na Vida, from 2010, and Últimas Conversas, posthumously released in 2015) and their contribution to the general question of documentary authorship. The director’s filmography is characterized by a consistent yet self-effacing form of authorial self-inscription: Coutinho often features as an interviewer that rather than express opinions propels discourses; an interviewer that is good at listening. This mode of self-inscription characterizes him as an author who is not expressive but who is nonetheless markedly present on the screen. In Um Dia na Vida, however, Coutinho is completely absent form the image, while Últimas Conversas, on the contrary, includes a confessional prologue that moves the director from the margins to the center of his films. This article examines the ways in which these works stand out in the filmography of a director who offers new insights into the notion of cinematic authorship

    Appropriate Similarity Measures for Author Cocitation Analysis

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    We provide a number of new insights into the methodological discussion about author cocitation analysis. We first argue that the use of the Pearson correlation for measuring the similarity between authors’ cocitation profiles is not very satisfactory. We then discuss what kind of similarity measures may be used as an alternative to the Pearson correlation. We consider three similarity measures in particular. One is the well-known cosine. The other two similarity measures have not been used before in the bibliometric literature. Finally, we show by means of an example that our findings have a high practical relevance.information science;Pearson correlation;cosine;similarity measure;author cocitation analysis
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