Probing the interplay between lattice dynamics and short-range magnetic correlations in CuGeO3 with femtosecond RIXS
E. ParisC. W. NicholsonSteven JohnstonYi TsengM. RumoGiacomo CoslovichS. ZoharMing‐Fu LinVladimir N. StrocovR. Saint-MartinA. RevcolevschiAlexander F. KemperW. F. SchlotterGeorgi L. DakovskiClaude MonneyThorsten Schmitt
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Abstract Investigations of magnetically ordered phases on the femtosecond timescale have provided significant insights into the influence of charge and lattice degrees of freedom on the magnetic sub-system. However, short-range magnetic correlations occurring in the absence of long-range order, for example in spin-frustrated systems, are inaccessible to many ultrafast techniques. Here, we show how time-resolved resonant inelastic X-ray scattering (trRIXS) is capable of probing such short-ranged magnetic dynamics in a charge-transfer insulator through the detection of a Zhang–Rice singlet exciton. Utilizing trRIXS measurements at the O K -edge, and in combination with model calculations, we probe the short-range spin correlations in the frustrated spin chain material CuGeO 3 following photo-excitation, revealing a strong coupling between the local lattice and spin sub-systems.Keywords:
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This chapter contains sections titled: Introduction Reaction Dynamics Time-Resolved Femtosecond Dynamics Coherence Representative Femtosecond Dynamics Studies Femtosecond Structural Determinations More Complex Reactions Conclusion and Outlook Suggested Reading References
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Femtosecond spectral holography is a very important technique of femtosecond pulse shaping, which permits storage, recalling and processing of femtosecond pulse signals. Femtosecond spectral holography technique and new applications of femtosecond pulse shaping with space-time conversion in femtosecond chemistry are presented
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Even in this day of proliferation of widely tunable femtosecond laser sources, severe limitations exist when one tries to perform two color femtosecond experiments with two independently tunable femtosecond lasers, One can generate, by clever cavity manipulation, two perfectly synchronized femtosecond pulses, but with very limited tunability. On the other hand, commercially available systems deliver completely independent tunability over the entire tuning range, but with timing jitters in the range of 5-10 ps. Here, we have developed a novel scheme which allows true two color femtosecond experiments with independent tunability of the two lasers.
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Abstract The binding of two free excitons into a bi‐exciton due to direct exciton‐exciton interaction is studied. The process of bi‐exciton formation via exciton–phonon interaction is not taken into account. By group theory methods the wave functions of two interacting excitons are constructed for a model applicable to CuCl and Cu 2 O crystals. Making use of these functions, the Fourier transform of exciton‐exciton interaction energy is calculated. By the Green's function method the dissociation energy of the bi‐exciton is obtained in the adiabatic approximation (the exciton‐exciton interaction energy is much smaller than the ionization energy of the exciton). A numerical estimate and comparison with experimental values is made for CuCl crystals.
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Abstract In first order of perturbation theory the probability of binding of two excitons into a bi‐exciton accompanied by light emission and caused by exciton–exciton collisions is calculated. Firstly the case is considered where two excitons of 1s‐type and n ‐p‐type form a bi‐exciton in the ground state consisting of two excitons of 1s‐type. The binding is accompanied by light emission. The luminescence begins with a threshold and the luminescence band has the form of a sharp asymmetrical peak. The exciton–exciton collisions lead to the binding of two excitons of 1s‐type with no internal excitation. Numerical estimations of the processes under consideration are made for a set of crystals.
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Abstract Femtosecond laser fabrication has grown to be a major method of extreme manufacturing because of the extreme energy density and spatial and temporal scales of femtosecond lasers. The physical effects and the mechanism of interaction between femtosecond lasers and materials are distinct from those in traditional processes. The nonlinear and nonequilibrium effects of the interaction have given rise to new concepts, principles, and methods, such as femtosecond pulse durations are shorter than many physical/chemical characteristic times, which permits manipulating, adjusting, or interfering with electron dynamics. These new concepts and methods have broad application prospects in micro/nanofabrication, chemical synthesis, material processing, quantum control, and other related fields. This review discusses the cutting-edge theories, methods, measurements, and applications of femtosecond lasers to micro/nano-manufacturing. The key to future development of femtosecond laser manufacturing lies in revealing its fabrication mechanism from the electronic level and precisely regulating the electronic dynamics.
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A comparison of two femtosecond coherent anti-Stokes Raman scattering (CARS) thermometry techniques is presented. While similar accuracies can be obtained with each technique, the hybrid femtosecond/picosecond technique was found to be less complex.
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