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488210 Supplemental Document

We demonstrate a double Rabi splitting totaling 348 meV in an Ag nanocavity embedding of methylene blue (MB) dye layer, which is ascribed to the equilibrium state of monomer and dimer coexistence in MB dye. At low dye concentration, the single-mode strong coupling between the monomer exciton in MB dye and the Ag nanocavity is observed. As the dye concentration is increased, three hybridized plexciton states are observed, indicating a double Rabi splitting (178 and 170 meV). Furthermore, the double anti-crossing behavior of the three hybrid states is observed by tuning the Ag nanocube size, which validates the multi-mode strong coupling regime. It shows clear evidence on the diverse exciton forms of dye molecules, both of which can interact with plasmonic nanocavity, effectively. Therefore, it provides a good candidate for realizing the multi-mode strong coupling.

supplemental document

In strong laser fields, the electron density in solids can show up tidal motions caused by the laser ``pulling'' on the electrons, which forms an electron density tide (EDT). However, the strong field processes in solids are always explained by the single-active-electron (SAE) model and the fluctuation of background electrons is neglected previously. Here, we demonstrate the strong field induced EDT effect and propose a model for revealing its role in high harmoinc generation (HHG) from solids. We show that the EDT effect induces an additional polarization current beyond the SAE approximation. It gives a new mechanism for HHG and leads to new anisotropic structures, which are experimentally observed with MgO. Our experiment indicates that the EDT effect becomes more obvious with increasing the laser intensity. Our work establishes the bridge between the HHG and the microscopic EDT in solids induced by the strong laser field, which paves the way to probe the ultrafast electron dynamics.

Direct imaging of molecular dynamics is a long-standing goal in physics and chemistry. As an emerging tool, high-harmonic spectroscopy (HHS) enables accessing molecular dynamics on femtosecond to attosecond time scales. However, decoding information from the harmonic signals is usually painstaking due to the coherent nature of high-harmonic generation (HHG). Here we show that this obstacle can be effectively overcome by exploiting machine learning in HHS. Combining the machine learning with an angle-resolved HHS method, we demonstrate that the rich dynamics of molecular rotational wave packet is fully reconstructed from the angular distributions of HHG measured at various time delays of the probe pulse. The experimental retrievals are in good agreement with the numerical simulations. These findings provide a comprehensive picture of molecular rotation in space and time which will facilitate the development of related researches on molecular dynamics imaging., Comment: 8 pages, 6 figures

Interferometry, as the key technique in modern precision measurements, has been used for length diagnosis in the fields of engineering metrology and astronomy. Analogous interferometric technique for time domain precision measurement is a significant complement to the spatial domain applications and requires the manipulation of the interference on the extreme time and energy scale. Here we present an all-optical interferometry for high precision measurement with attosecond temporal and hundreds of meV energy resolution. The interferometer is based on laser driven high order harmonics which provide a robust sequence of attosecond temporal slits. As applications, we reconstruct the waveform of an arbitrarily polarized optical pulse using the time resolving capability, and capture the abnormal character of the transition dipole near a Cooper minimum in argon using the energy resolution provided. This novel attosecond interferometry opens the possibility for high precision measurement in time energy domain using an all-optical approach., Comment: 12 pages, 5 figures in main text and 9 pages, 7 figures in supplementary material

Bloch oscillations (BOs) refer to a periodically oscillatory motion of particle in lattice systems driven by a constant force. By temporally modulating acoustic waveguides, BOs can be generalized from spatial to frequency domain, opening new possibilities for spectrum manipulations. The modulation can induce mode transitions in the waveguide band and form an artificial frequency lattice, with the mismatched wave vector during transitions acting as a constant force that drives frequency Bloch oscillations (FBOs). Furthermore, the modulation phase accompanying transitions serves as a gauge potential that controls the initial oscillation phase, providing an additional degree of freedom to tailor FBOs. We report that multiple FBOs with judiciously designed oscillation phases can be further cascaded to realize acoustic spectrum self-imaging, unidirectional transduction and bandwidth engineering. The study proposes the concept of FBOs in acoustic systems and functionalizes its cascade configurations for advanced control of sound spectrum. This paradigm may find versatile applications in underwater secure communication, voice encryption and signal processing., Comment: 4 figures

We investigate the high harmonic generation (HHG) in solids driven by laser fields with different ellipticities. The HHG spectra show a two-plateau structure within the energy gap between the valence band and the first conduction band. These two plateaus depend distinctly on the laser ellipticity. The first plateau is decreased while the second plateau is enhanced with increasing the laser ellipticity. To understand these phenomena, we develop an intuitive Reciprocal-Space- Trajectory (RST) method, with which HHG in solids is explained by a trajectory-ensemble from different initial states and different ionization times in the reciprocal space. In the framework of RST, we can not only quantitatively reproduce the HHG spectra, but also well understand the underlying physics of these phenomena, providing a deep insight into the mechanism of HHG in solids.

We propose an intuitive method, called time-dependent population imaging (TDPI), to map the dynamical processes of high harmonic generation (HHG) in solids by solving the time-dependent Schr\"{o}dinger equation (TDSE). It is shown that the real-time dynamical characteristics of HHG in solids, such as the instantaneous photon energies of emitted harmonics, can be read directly from the energy-resolved population oscillations of electrons in the TDPIs. Meanwhile, the short and long trajectories of solid HHG are illustrated clearly from TDPI. By using the TDPI, we also investigate the effects of carrier-envelope phase (CEP) in few-cycle pulses and intuitively demonstrate the HHG dynamics driven by two-color fields. Our results show that the TDPI provides a powerful tool to study the ultrafast dynamics in strong fields for various laser-solid configurations and gain an insight into HHG processes in solids.

The present work reports an investigation of plasma expansion produced by Nd:YAG laser irradiating tin droplets. An intensified charged coupled device camera was used to record the plasma plume images, and the temporal evolution of the plasma plume was studied at various laser intensities. Our results demonstrate that the shape of the plasma plume develops from an approximate circle to an ellipse. The temporal evolutions of plasma boundary and plasma centroid were calculated by the secondary moment of plasma image intensity. The angle distributions of the plasma expanding velocity were obtained; the results show that the plasma expanding velocity decreases with increase of the angle to the incoming laser axis. In addition, the eccentricity of the plasma ellipse decreases with time. Meanwhile, we found that the centroid of plasma clusters moves toward the laser incoming direction during the expansion stage and the velocity of this motion is independent of laser intensity.