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<p>“Fröknarna von Pahlen”, is a series of novels written by the author Agnes von Krusenstjerna. Especially the fourth and fifth parts, published in 1933, raised questions about sexuality, especially about what was conceived as perverse and provoking descriptions. “Fröknarna von Pahlen” became a part of heated debates about what is acceptable to write about. How can the so called Pahlen feud be understood from an intersectional perspective, and from a focus on values, and by discussing imagined communities? The purpose is to find out what is going on in these debates. Six different values are being pointed out; art and skill, truth, freedom of speech and freedom of the press, the value in the young, the value in female perspectives, and moral values. There is a number of knot points tied to these values, and differentiating processes such as sex, class, age, ethnicity, religion etc. are all intertwined in these debates. From an intersectional understanding, none of these processes are more primal than another. The knot points are both of an emotional nature and thematic. The individual voices that emerge in the feud are named small narratives, and the more intersubjective narratives are called grand narratives. These narratives are being investigated rhetorically; for instance how some stories can appear more as truths than others, and it is analyzed how they separate people in groups and create hierarchies. They are also being seen from an emotional perspective; how individual feelings are a part of emotions, larger contexts and meaning coherences. These feelings are also understood as actions. Throughout the investigation there is a hermeneutic will to make things intelligible, and respect and point out the many different perspectives. This is being made in a cultural relativistic attempt. By focusing on imagined communities, different comradeships and groups in the feud can be pointed out. People can consider themselves parts of these groups, but they can also, more or less involuntarily, be considered as parts of these groups. In the writers opinion, the most important question is how “extreme” sexual descriptions an author is allowed to bring forth.<em></em><em></em></p>

This thesis is about excitation, detection, properties and applications of multiple quantum coherences applied to different dipolar coupled spin systems. Major focus of the work is on spectral simplification, measurement of residual dipolar couplings and discrimination of enantiomers in chiral aligning media. The first chapter gives a brief account on the fundamentals of nuclear magnetic resonance spectroscopy and multiple quantum coherences. This includes a description of product operator and polarization operator formalisms of pulses and evolution of magnetization. Subsequently a detailed account of two dimensional multiple quantum – single quantum (MQ-SQ) correlation experiments is given. Demonstration of the homonuclear MQ-SQ pulse sequence on a weakly coupled spin system and analysis of the spectrum obtained are also discussed. Homo-nuclear multiple quantum studies carried out to obtain relative the signs of the couplings have been reported in the initial part of the second chapter. The technique has been applied on doubly labeled acetonitrile (13CH313C15N) aligned in a liquid crystalline medium. Special situations like ambiguity in the determination of relative signs of the couplings from the appearance of two dimensional MQ-SQ spectra and the explanation for the same are also discussed. Homo-nuclear MQ experiments on indistinguishable spins, like protons in a methyl group of 13CH313C15N oriented in liquid crystal, and distinguishable spins, like the two carbons in the same molecule, have been carried out. Different directions of approach in which these results need to be analyzed have been discussed. Subsequent part of the chapter is about the correlation of connected MQ-SQ coherences. These experiments are significant in reducing the cross-peaks further from the MQ-SQ spectra. This concept is extended for the discrimination of optical enantiomers dissolved in chiral aligning medium made of poly-Γ-benzyl-L-glutamate (PBLG) and CDCl3. In molecules of Chemical and biological interest one encounters several nuclei such as, 1H, 13C, 15N and 19F. It will be of general interest to determine magnitudes and relative signs of the couplings among these coupled nuclei by NMR experiments. Utilization of hetero-nuclear MQ Experiments in solving such problems is discussed in the third Chapter. Hetero-nuclear MQ experiments were carried out on dipolar coupled 13CH313C15N, with the aim of obtaining the values and signs of various hetero-nuclear couplings in the molecule. The splitting of transitions in the spectra of oriented molecules is always influenced by the sum of dipolar and scalar couplings. Hence precise determination of dipolar couplings requires the knowledge of scalar couplings. To determine the J couplings, experiments were carried out on the same molecule in isotropic medium. When many coupled nuclei are involved one has to carry out several experiments to derive all the spectral parameters. In circumventing this problem heteronuclear multiple quantum experiments involving more than two nuclei as active spins are advantageous. This reduces the number of experiments and thereby reducing the total experimental time. Second part of this chapter demonstrates how a triple resonance triple quantum experiment can provide majority of the couplings from a given coupled system. The feasibility of the experiment is demonstrated even for molecules containing natural abundant isotopes. Application of multiple quantum j-resolved technique for chiral discrimination and obtaining complete one dimensional spectrum of each enantiomer from their racemic mixture is discussed in the fourth chapter. The two dimensional experiment consists of a selective double quantum excitation period followed by selective refocusing during indirect time domain, isotropic mixing and nonselective detection of SQ transitions. Hence this pulse sequence is named as DQSERF-COSY (Double Quantum Selective Refocused Correlation Spectroscopy). The experiment exploits the existence of different intra-methyl couplings between the enantiomers dissolved in chiral liquid crystal medium to separate the one dimensional spectra of each enantiomer in different cross sections. This is possible due to the fact that all the nuclei in any one of the enantiomers are coupled among themselves and there is no inter molecular interaction between the two enantiomers. Also one can extract all the couplings between protons in each enantiomer, which can subsequently be utilized for determination of the residual dipolar couplings, structure and orientation parameters.

<p>This dissertation focuses on a very special topic in the field of Nuclear Magnetic Resonance (NMR) in solution: Intermolecular Multiple Quantum Coherences, or iMQCs, which can only be created by intermolecular dipolar couplings. Since the very beginnings of NMR, it has been known that dipolar couplings dominate the solid-state linewidth for spin-1/2 nuclei, but the effects are still not fully understood. The angular dependency (1-3cos2&#952;ij) and distant dependency (rij-3) of dipolar coupling led to an oversimplified conclusion that it can be ignored in an isotropic liquid. Thus, it was surprising when COSY Revamped by Asymmetric Z-gradient Echo Detection (CRAZED) was first introduced in the early `90s and showed strong iMQC signals. Since then, CRAZED has inspired a wide range of applications for iMQCs and led to two different but equivalent mathematical frameworks to describes these effects, which we call the conventional DDF theory.</p><p>However, several disagreements between the conventional DDF theory and experiments have grasped our attention recently. This dissertation will: first, demonstrate how conventional picture fails by two examples, Multi-axis CRAZED (MAXCRAZED) and Gradient-embedded COSY Experiment (GRACE); second, provide a corrected DDF theory; and, third, discuss what impact this correction will bring.</p><p>Intermolecular double quantum coherences (iDQCs) are very sensitive to the local anisotropy (10&#956;m - 1mm) and can be used to create positive contrast highlighting superparamagnetic iron oxide nanoparticles (SPIONs). This dissertation will show the design and optimization of iDQC anisotropy by a series of phantom experiments. A set of numerical simulations will then be provided for a sub-voxel level explanation. We will also demonstrate how the newly corrected DDF theory can be quickly adapted to improve the iDQC anisotropy.</p><p>Finally, as a side product of this research, the mechanism of diacetyl hydration/dehydration as solved by NMR will be provided.</p> / Dissertation

“Fröknarna von Pahlen”, is a series of novels written by the author Agnes von Krusenstjerna. Especially the fourth and fifth parts, published in 1933, raised questions about sexuality, especially about what was conceived as perverse and provoking descriptions. “Fröknarna von Pahlen” became a part of heated debates about what is acceptable to write about. How can the so called Pahlen feud be understood from an intersectional perspective, and from a focus on values, and by discussing imagined communities? The purpose is to find out what is going on in these debates. Six different values are being pointed out; art and skill, truth, freedom of speech and freedom of the press, the value in the young, the value in female perspectives, and moral values. There is a number of knot points tied to these values, and differentiating processes such as sex, class, age, ethnicity, religion etc. are all intertwined in these debates. From an intersectional understanding, none of these processes are more primal than another. The knot points are both of an emotional nature and thematic. The individual voices that emerge in the feud are named small narratives, and the more intersubjective narratives are called grand narratives. These narratives are being investigated rhetorically; for instance how some stories can appear more as truths than others, and it is analyzed how they separate people in groups and create hierarchies. They are also being seen from an emotional perspective; how individual feelings are a part of emotions, larger contexts and meaning coherences. These feelings are also understood as actions. Throughout the investigation there is a hermeneutic will to make things intelligible, and respect and point out the many different perspectives. This is being made in a cultural relativistic attempt. By focusing on imagined communities, different comradeships and groups in the feud can be pointed out. People can consider themselves parts of these groups, but they can also, more or less involuntarily, be considered as parts of these groups. In the writers opinion, the most important question is how “extreme” sexual descriptions an author is allowed to bring forth.

In the first part of this dissertation, recent efforts to understand quantum mechanical effects in biological systems are discussed. Especially, long-lived quantum coherences observed during the electronic energy transfer process in the Fenna-Matthews-Olson complex at physiological condition are studied extensively using theories of open quantum systems. In addition to the usual master equation based approaches, the effect of the protein structure is investigated in atomistic detail through the combined application of quantum chemistry and molecular dynamics simulations. To evaluate the thermalized reduced density matrix, a path-integral Monte Carlo method with a novel importance sampling approach is developed for excitons coupled to an arbitrary phonon bath at a finite temperature. In the second part of the thesis, simulations of molecular systems and applications to vibrational spectra are discussed. First, the quantum dynamics of a molecule is simulated by combining semiclassical initial value representation and density funcitonal theory with analytic derivatives. A computationally-tractable approximation to the sum-of-states formalism of Raman spectra is subsequently discussed.

Zum ersten Mal konnte die kohärente Erzeugung von ultrakurzen Pulsen mit Feld stärken im MV/cm Bereich mit einem Spektralbereich von 0.1-30 THz im organischen Kristall DSTMS. Kohärente mehrdimensionale Terahertzspektroskopie (CMTS) hat sich zu einer wichtigen Methode zur Untersuchung der niederenergetischen Anregungen von Halbleitern and deren kohärenter Dynamik entwickelt. Eine neuartige CMTS Methode mit drei phasenstarren, zueinander zeitverzögerten Terahertzpulsen wurde entwickelt. Sie beruht auf der kollinearen Wechselwirkung der Pulse mit der Probe, sodass verschiedene Ordnungen des nichtlinearen Signals in gleicher Richtung emittiert werden und deshalb gleichzeitig gemessen werden können. Amplitude und Phase des nichtlinearen Signals können durch elektro-optisches Abtasten vermessen werden, wodurch die zeitliche Entwicklung der kohärenten Wechselwirkungen in Echtzeit untersucht werden kann. CMTS erlaubt zusätzlich die eindeutige Zerlegung des nichtlinearen Signals in die verschiedenen nichtlinearen Ordnungen in der jeweiligen mehrdimensionalen Frequenzdomäne. Die nichtlineare, nicht-resonante Antwort zweier undotierter Halbleiter, des Ferroelektrikums Lithiumniobat (LiNbO3) und Indiumantimonids (InSb) kann mit dieser neuartigen Methode untersucht werden. In LiNbO3 wird das nichtlineare Signal durch einen Femtosekunden nichtlinearen Verschiebestrom (SC) hervorgerufen. SC wird durch die gebrochene Inversionssymmetrie des Kristalls in Verbindung mit einer ultraschnellen Dephasierung der feldinduzierten, kohärenten interband-Polarisation hervorgerufen. Die Dephasierung der interband-Polarisation erlaubt das Tunneln von Elektronen vom Valenzband in das Leitungsband. In InSb wird das kohärente Signal durch sowohl zwei-Phonen als auch zwei-Photonen interband-Anregungen erzeugt. Die impulsive Anregung einer kohärenten zwei-Phononen Polarisation wird durch das große Übergangsdipolmoment von InSb verstärkt, was zu deutlich größeren Amplituden der Polarisation als im linearem Regime führt. / For the first time, the coherent generation of ultrashort MV/cm field pulses with a spectrum covering the frequency range 0.1-30 THz is demonstrated in the organic crystal DSTMS. Coherent multidimensional terahertz spectroscopy (CMTS) has become a prominent technique for, e.g., driving low-energy excitations in semiconductors and monitoring their coherent dynamics. A novel CMTS technique using three phase-locked inter-delayed THz pulses is implemented. It relies on a collinear interaction of the pulses with a sample, so that different contributions to the nonlinear signal are emitted in the same direction, and thus can be measured all at once. Phase-resolved detection by electro-optic sampling allows for measuring amplitude and absolute phase of the nonlinear signal, thereby enabling to investigate the evolution of coherent interactions between quantum excitations in real time. In CMTS, the nonlinear signal is dissected into the distinct nonlinear contributions in the corresponding multidimensional frequency domain. This novel technique is applied to study the nonlinear off-resonant response of two undoped bulk semiconductors, the wide-bandgap ferroelectric lithium niobate (LiNbO3) and the narrow-bandgap indium antimonide (InSb). In LiNbO3, the nonlinear signal is generated by a femtosecond nonlinear shift current (SC), a distinctive characteristic of the bulk photovoltaic effect. The SC stems from the lack of inversion symmetry and the ultrafast dephasing of the field-induced interband coherent polarization due to a sufficiently high decoherence rate, which enables tunneling of electrons from the valence to the conduction band. In InSb, the nonlinear signal is caused by the coherent response on both the two-phonon and two-photon interband excitations. The impulsive generation of the two-phonon coherent polarization is enhanced by the large interband transition dipole of InSb, resulting in much larger polarization amplitudes than in the regime of linear response.

We investigate two different coupling schemes between a nano-scale mechanical resonator and one-electron atoms. In these schemes, classical electromagnetic radiation mediates a mutual communication between the mechanical resonator and the atoms. In the process it generates atomic coherences, quantum superpositions of excited electronic levels of the atoms. An atomic coherence is highly responsive to subtle variations in the relative frequencies of the levels participating in such superposition state. By exposing the atoms to electromagnetic radiation modulated by the motion of the mechanical resonator, we show how the response of an atomic coherence can, under appropriate conditions, be used to affect on demand the dynamical state of the mechanical resonator. The first scheme realizes a long range interface between a mechanical resonator and an ensemble of three-level atoms. Here, mechanically modulated electromagnetic radiation comes from a laser beam reflected off an oscillating mirror, the mechanical resonator. This light beam drives the transition between an excited level and a hyperfine sublevel of the atoms with a certain detuning. A weaker light beam resonantly couples to the transition between the excited level and another hyperfine sublevel. On full resonance, the atoms evolve into a stationary coherence of the above (non-absorbing) hyperfine sublevels only. The atoms then become transparent to the weaker light beam, in a phenomenon called electromagnetically induced transparency. Off resonance, we find that this transparency is modulated at the mirror frequency with some phase shift, which allows the weaker beam to cause resonant backaction onto the moving mirror. The strength of this backaction is enhanced near atomic resonances and its character can be switched between amplification or damping of mirror vibrations by adjusting the detuning. In contrast, the second scheme accomplishes a closer range interface between a torsion pendulum and guided two level Rydberg atoms. Attaching a point electric dipole to the torsion pendulum allows electromagnetic coupling to two Rydberg levels of a passing atom. This coupling modifies the eigenfrequencies of the Rydberg levels such that they become dependent on the phonon number of the torsion pendulum. Via Ramsey interferometry, we may readout this effect and thus measure the phonon number. We show that, by subjecting several atoms, one by one, to a Ramsey measurement, a quantum non-demolition detection of the phonon number is feasible. Likewise, we show coherent oscillator displacements possible, by driving the atoms with external fields while they interact with the torsion pendulum. We propose a protocol to reconstruct the quantum state of motion of the torsion pendulum, combining these two techniques, Ramsey measurements and oscillator displacements. Our interfaces between a mechanical resonator and atoms provide alternative routes for the control of the state of motion, ultimately quantum mechanical, of a mechanical resonator, in which the latter is not restricted to be part of a cavity. We will thus ease quantum dynamical manipulations of mechanical resonators of sub micron scales, for which an efficient design of cavity opto- and electro-mechanical systems is hard.