Raum: Seminar Room V, O1.109

Matteo Lucchini - Attosecond dynamics in polycrystalline diamond

MPSD Seminar
The possibility to manipulate the electrical properties of matter with very short opticalpulses is a fascinating field of research with possible far reaching applications inmany relevant technological fields. The first step towards the realization of this goal is to understand the ultrafast dynamics at the basis of light-matter interaction. Short and intense pulses allowed us to investigate a very interesting regime where the photon energy becomes comparable to the cycle-averaged kinetic energy of the electrons in the field. As the optical response of the material transitions from a classical to quantum-mechanical description many intriguing effects co-exist in this regime and the importance of inter- versus intra-band transitions is still debated. We used attosecond transient absorption spectroscopy (ATAS) to study the optical response of polycrystalline diamond driven by few-femtosecond, intense (IIR ~1012 W/cm2) infrared (IR) pulses. We monitored the system response by looking at the induced change in the absorbance with a 250-as pulse centred around 40 eV. We observed the appearance of oscillating features which modulate at twice the IR frequency, ωIR, and fully recover after the interaction. Simultaneous photoelectron acquisition from a gas nozzle placed in front of the diamond target allowed us to study the phase relation of the oscillating features and the pumping IR field. We found that the timing of the diamond response changes significantly with the probing energy and does not always follow the IR field adiabatically. Ab initio calculations performed by coupling time-dependent density functional theory (TDDFT) in real time with Maxwell’s equations reproduced the experimental observations. Further comparison with a numerical two-band model allowed us to conclude that intra-band motion dominates over inter-band transitions, thus identifying the dynamical Franz- Keldysh effect as the dominant mechanism in this regime. Our analysis constitutes an important step towards a full understanding of the optical properties of dielectrics in the Petahertz regime. [mehr]

Quantum control and dynamics with x-rays

MPSD Seminar
More than fifty years ago, it was the invention of the laser that revolutionized atomic physics and laid the foundations for quantum optics and coherent control. With only optical frequencies available, the interaction of coherent light with matter was for a long time mainly restricted to atomic transitions. Only recently have novelhigh-frequency light sources rendered x-ray quantum optics possible. In this higher frequency regime, atomic nuclei rise as natural candidates for the interaction with coherent light creating a new bridge between atomic physics, quantum optics and nuclear condensed matter physics. Nuclei are very clean quantum systems, well isolated from the environment and benefiting from long coherence times. Combining the advantages of x-rays and nuclei, a prominent incentive is to exploit x-rays as the future quantum information carriers or for novel probing technologies based on quantum effects. Furthermore, the control of nuclear transitions would open the possibility to use long-lived nuclear excited states as a compact and clean energy storage solution. The lecture will follow the developments on the emerging field of x-ray quantum optics and focus on the mutual control of coherent x-ray radiation and nuclear transitions in this new regime of laser-matter interactions. [mehr]

Gapless excitations in the ground state of 1T-TaS2

MPSD Seminar
1T-TaS2 is a layered transition metal dichalcogenide with a very rich phase diagram, which was investigated since the early 1970s. At T=180K it undergoes a metal to Mott insulator transition. Mott insulators usually display anti-ferromagnetic ordering in the insulating phase but 1T-TaS2 was never shown to order magnetically. We have shown that 1T-TaS2 has a large paramagnetic contribution to the magnetic susceptibility but it does not show any sign of magnetic ordering or freezing down to 20mK, as probed by muSR, possibly indicating a quantum spin liquid ground state. Although 1T-TaS2 exhibits a strong resistive behavior both in and out of plane at low temperatures we find a linear term in the heat capacity suggesting the existence of a Fermi-surface, which has an anomalously strong magnetic field dependence. [mehr]

Electronic and Vibrational Properties of Colloidal Nanocrystals

MPSD Seminar
Colloidal nanocrystals (CNCs) are nanometer sized crystals grown in solution. Due to their size-tunable optical properties, CNCs have emerged as a novel material platform for numerous applications such as displays, photovoltaics, and biological tagging. However, the colloidal growth process results in an unavoidable distribution of CNC size that inhomogeneously broadens optical absorption/luminescence lineshapes. 2-D spectroscopy is a technique capable of circumventing inhomogeneous broadening by correlating absorption and emission dynamics. In this talk I will present our results from applying 2-D spectroscopy to CNCs at cryogenic temperatures. I will first discuss our experiments on conventional CdSe CNCs, in which we have simultaneously observed both bulk-like acoustic phonons and acoustic vibrations discretized by the nanocrystal geometry for the first time. Next, I discuss our experiments on perovskite CNCs, which are a new class of materials first synthesized in 2015. We demonstrate that coherences due to vibrational coupling exhibit anomalous dephasing dynamics, which we attribute to a cascaded coherence transfer process. Finally, I discuss our observations of coherences between so-called bright-triplet exciton states, which are robust at high temperatures and polarization-selective. [mehr]
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