arXiv subjects

Mao-Rui Cai

Publications and source records attributed to Mao-Rui Cai.

5 recordsLinked to original sources

arXiv2024

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↗

arXiv2023

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↗

arXiv2023

Enantiodetection via the 2D spectroscopy: extending the methodology to general experimental conditions

Developing effective methods to measure the enantiomeric excess of the chiral mixture is one of the major topics in chiral molecular researches, yet remains challenging. Enantiodetection method via two-dimensional (2D) spectroscopy based on a four level model, containing a cyclic three-level system (CTLS), of chiral molecules was recently proposed and demonstrated, yet with a strict condition of the one-photon resonance (where three driving fields are exactly resonantly coupled to the three electric-dipole transitions, respectively) in the CTLS and narrowband probe pulse assumption. Here, we extend the 2D spectroscopy method to more general experimental conditions, with three-photon resonance (where the sum of the two smaller frequencies among the three driving fields equals to the third one) and broadband probe pulse. Our method remains effective on enantiodetection with the help of experimental techniques, such as the chop detection method, which is used to eliminate the influence of the other redundant levels existing in the real system of chiral molecules. Under these more general conditions, the enantiomeric excess of the chiral mixture is estimated by taking an easily available standard sample (usually the racemic mixture) as the reference.

physics.chem-ph↗

arXiv2021

Enantiodetection of chiral molecules via two-dimensional spectroscopy

Enantiodetection of chiral molecules is important to pharmaceutical drug production, chemical reaction control, and biological function designs. Traditional optical methods of enantiodetection rely on the weak magnetic-dipole or electric-quadrupole interactions, and in turn suffer from the weak signal and low sensitivity. We propose a new optical enantiodetection method to determine the enantiomeric excess via two-dimensional (2D) spectroscopy of the chiral mixture driven by three electromagnetic fields. The quantities of left- and right- handed chiral molecules are reflected by the intensities of different peaks on the 2D spectrum, separated by the chirality-dependent frequency shifts resulting from the relative strong electric-dipole interactions between the chiral molecules and the driving fields. Thus, the enantiomeric excess can be determined via the intensity ratio of the peaks for the two enantiomers.

physics.chem-ph↗

arXiv2021

Single-photon nonreciprocal excitation transfer with non-Markovian retarded effects

We study at the single-photon level the nonreciprocal excitation transfer between emitters coupled with a common waveguide. Non-Markovian retarded effects are taken into account due to the large separation distance between different emitter-waveguide coupling ports. It is shown that the excitation transfer between the emitters of a small-atom dimer can be obviously nonreciprocal by introducing between them a coherent coupling channel with nontrivial coupling phase. We prove that for dimer models the nonreciprocity cannot coexist with the decoherence-free giant-atom structure although the latter markedly lengthens the lifetime of the emitters. In view of this, we further propose a giant-atom trimer which supports both nonreciprocal transfer (directional circulation) of the excitation and greatly lengthened lifetime. Such a trimer model also exhibits incommensurate emitter-waveguide entanglement for different initial states in which case the excitation transfer is however reciprocal. We believe that the proposals in this paper are of potential applications in large-scale quantum networks and quantum information processing.

quant-ph↗