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Zi-Qian Cheng

Publications and source records attributed to Zi-Qian Cheng.

3 recordsLinked to original sources

Frequency-resolved Transient Absorption Spectroscopy for High Pressure System

Dynamics of materials under high-pressure conditions has been an important focus of materials science, especially in the timescale of pico- and femto-second of electronic and vibrational motion, which is typically probed by ultrafast laser pulses. To probe such dynamics, it requires an integration of high-pressure devices with the ultrafast laser system. In this work, we construct a frequency-resolved high-pressure transient absorption spectroscopy system based on a diamond anvil cell (DAC) with transmissive detection. In this setup, we use the narrowband laser as the pump beam and the supercontinuum white light as the probe beam. To effectively eliminate the scattering noise from the pump light, we design a double-chopper operating mode, which allows us to obtain signals in the complete frequency domain including the overlap region with the pump pulse. And we test system with Rhodamine B solution with the probe wavelength range of 450-750 nm and the 550nm pump, and observe that the intensity of the signal peak corresponding to the monomer at 560 nm continuously decreased relative to the signal peak corresponding to the dimer at 530 nm. This indicates that the portion of Rhodamine B molecules in the dimer form increases under increasing pressure. Additionally, we find two dynamic components of the signal peaks for both monomer and dimer, and the short-lifetime component increases as the pressure is increased, and the long-lifetime component decreases.

physics.optics

Extracting double-quantum coherence in two-dimensional electronic spectroscopy under pump-probe geometry

Two-dimensional electronic spectroscopy (2DES) can be implemented with different geometries, e.g., BOXCARS, collinear and pump-probe geometries. The pump-probe geometry has its advantage of overlapping only two beams and reducing phase cycling steps. However, its applications are typically limited to observe the dynamics with single-quantum coherence and population, leaving the challenge to measure the dynamics of the double-quantum (2Q) coherence, which reflects the many-body interactions. We propose an experimental technique in 2DES under pump-probe geometry with a designed pulse sequence and the signal processing method to extract 2Q coherence. In the designed pulse sequence with the probe pulse arriving earlier than pump pulses, our measured signal includes the 2Q signal as well as the zero-quantum (0Q) signal. With phase cycling and the data processing using causality enforcement, we extract the 2Q signal. The proposal is demonstrated with the rubidium atoms. And we observe the collective resonances of two-body dipole-dipole interactions of both $D_{1}$ and $D_{2}$ lines.

quant-ph

Cross-phase modulation in the two dimensional spectroscopy

Developing from the transient absorption (TA) spectroscopy, the two dimensional (2D) spectroscopy with pump-probe geometry has emerged as a versatile approach for alleviating the difficulty on implementing the 2D spectroscopy with other geometries. However, the presence of cross-phase modulation (XPM) in TA spectroscopy introduces significant spectral distortions, particularly when the pump and probe pulses overlap. We demonstrate that this phenomenon is extended to the 2D spectroscopy with pump-probe geometry and the XPM is induced by the interference of the two pump pulse. We present the oscillatory behavior of XPM in the 2D spectrum and its displacement with respect to the waiting time delay through both experimental measurements and numerical simulations. Additionally, we explore the influence of probe pulse chirp on XPM and discover that by compressing the chirp, the impact of XPM on the desired signal can be reduced.

physics.optics