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This thesis describes how the rich internal degrees of freedom of molecules can be exploited to construct the first “clock” based on ultracold molecules, rather than atoms. By holding the molecules in an optical lattice trap, the vibrational clock is engineered to have a high oscillation quality factor, facilitating the full characterization of frequency shifts affecting the clock at the hertz level. The prototypical vibrational molecular clock is shown to have a systematic fractional uncertainty at the 14th decimal place, matching the performance of the earliest optical atomic lattice clocks. As part of this effort, deeply bound strontium dimers are coherently created, and ultracold collisions of these Van der Waals molecules are studied for the first time, revealing inelastic losses at the universal rate. The thesis reports one of the most accurate measurements of a molecule’s vibrational transition frequency to date. The molecular clock lays the groundwork for explorations into terahertz metrology, quantum chemistry, and fundamental interactions at atomic length scales.

Atoms. --- Molecules. --- Metrology. --- Molecular spectroscopy. --- Lasers. --- Measurement. --- Measuring instruments. --- Quantum chemistry. --- Atoms and molecules in external fields. --- Metrology and Fundamental Constants. --- Molecular Spectroscopy. --- Laser. --- Measurement Science and Instrumentation. --- Quantum Chemistry.

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This book introduces the ideas and concepts of nonlinear dielectric spectroscopy, outlines its history, and provides insight into the present state of the art of the experimental technology and understanding of nonlinear dielectric effects. Emphasis is on what can be learned from nonlinear experiments that could not be derived from the linear counterparts. The book explains that nonlinear dielectric spectroscopy can be used as a tool to measure structural recovery or physical aging, as well as connections between dynamics and thermodynamic variables such as enthalpy and entropy. Supercooled liquids in their viscous regime are ideal candidates for investigating nonlinear effects, because they are particularly sensitive to changes in temperature, and thus also to changes in the electric field. Other interesting materials covered are plastic crystals and complex liquids near criticality. The book also points out that, compared with other techniques such as mechanical shear experiments, the nonlinear regime of dielectric spectroscopy is special in the sense that the energies involved always remain small compared with thermal energies. To demonstrate this, nonlinear features of mechanical experiments are discussed. Theoretical approaches to nonlinear effects are particularly complicated because the tools available for the linear regime no longer apply. As a result, there is no single generally accepted theory to nonlinear dielectric responses of real liquids. Various approaches to nonlinear dielectric features have been reported, and the different aspects are communicated in several chapters. The book communicates recent progress most effectively through individual contributions from specialists in their respective fields. Chapter 'Third and Fifth Harmonic Responses in Viscous Liquids' is available open access under a Creative Commons Attribution 4.0 International License via link.springer.com.

Broadband dielectric spectroscopy. --- Nonlinear systems. --- Chemistry. --- Spectroscopy. --- Electrochemistry. --- Atoms. --- Physics. --- Matter. --- Amorphous substances. --- Complex fluids. --- Materials science. --- Spectroscopy/Spectrometry. --- Atoms and Molecules in Strong Fields, Laser Matter Interaction. --- Characterization and Evaluation of Materials. --- Soft and Granular Matter, Complex Fluids and Microfluidics. --- Systems, Nonlinear --- System theory --- BDS (Spectrum analysis) --- Dielectric spectroscopy, Broadband --- Spectrum analysis --- Surfaces (Physics). --- Physical sciences --- Physics --- Surface chemistry --- Surfaces (Technology) --- Analysis, Spectrum --- Spectra --- Spectrochemical analysis --- Spectrochemistry --- Spectroscopy --- Chemistry, Analytic --- Interferometry --- Optics --- Radiation --- Wave-motion, Theory of --- Absorption spectra --- Light --- Spectroscope --- Qualitative --- Complex liquids --- Fluids, Complex --- Amorphous substances --- Liquids --- Soft condensed matter --- Chemistry, Physical and theoretical --- Material science --- Natural philosophy --- Philosophy, Natural --- Dynamics --- Matter --- Stereochemistry --- Spectrometry --- Constitution --- Analytical chemistry --- Spectrum analysis. --- Molecules. --- Materials --- Soft condensed matter. --- Atoms and molecules in external fields. --- Characterization and Analytical Technique. --- Soft and Granular Matter. --- Analysis. --- Matter, Soft (Condensed matter) --- Matter, Soft condensed --- Soft matter (Condensed matter) --- Condensed matter --- Complex fluids