Optical Two-dimensional Coherent Spectroscopy Research Articles

Optical two-dimensional coherent spectroscopy of cold atoms.

We report an experimental demonstration of optical two-dimensional coherent spectroscopy (2DCS) in cold atoms. The experiment integrates a collinear 2DCS setup with a magneto-optical trap (MOT), in which cold rubidium (Rb) atoms are prepared at a temperature of approximately 200 µK and a number density of 1010 cm-3. With a sequence of femtosecond laser pulses, we first obtain one-dimensional second- and fourth-order nonlinear signals and then acquire both one-quantum and zero-quantum 2D spectra of cold Rb atoms. The capability of performing optical 2DCS in cold atoms is an important step toward optical 2DCS study of many-body physics in cold atoms and ultimately in atom arrays and trapped ions. Optical 2DCS in cold atoms/molecules can also be a new avenue to probe chemical reaction dynamics in cold molecules.

Broadband optical two-dimensional coherent spectroscopy of a rubidium atomic vapor

Optical two-dimensional coherent spectroscopy (2DCS) has become a powerful tool for studying energy level structure, dynamics, and coupling in many systems including atomic ensembles. Various types of two-dimensional (2D) spectra, including the so-called single-quantum, zero-quantum, and double-quantum 2D spectra, of both D lines (D$_1$ and D$_2$ transitions) of potassium (K) atoms have been reported previously. For rubidium (Rb), a major difference is that the D-lines are about 15 nm apart as opposed to only about 3 nm for K. Simultaneously exciting both D-lines of Rb atoms requires a broader laser bandwidth for the experiment. Here, we report a broadband optical 2DCS experiment in an Rb atomic vapor. A complete set of single-quantum, zero-quantum, and double-quantum 2D spectra including both D-lines of Rb atoms were obtained. The experimental spectra were reproduced by simulated 2D spectra based on the perturbation solutions to the optical Bloch equations. This work in Rb atoms complements previous 2DCS studies of K and Rb with a narrower bandwidth that covers two D-lines of K or only a single D-line of Rb. The broadband excitation enables the capability to perform double-quantum and multi-quantum 2DCS of both D-lines of Rb to study many-body interactions and correlations in comparison with K atoms.

Optical two-dimensional coherent spectroscopy of many-body dipole-dipole interactions and correlations in atomic vapors.

Many-body interactions and correlations in atomic ensembles are fundamental in understanding many-body effects such as collective and emergent phenomena and also play an important role in various atom-based applications. Optical two-dimensional coherent spectroscopy (2DCS) provides a powerful tool to measure many-body interactions and correlations. Here, we present the study of many-body dipole-dipole interactions and correlations in potassium and rubidium atomic vapors by using double-quantum and multi-quantum 2DCS. The results show that double-quantum 2DCS provides sensitive and background-free detection of weak dipole-dipole interaction between atoms with a mean separation up to about 16 μm, and multi-quantum 2DCS can excite and detect multi-atom states (Dicke states) with up to eight correlated atoms. The technique of optical 2DCS can provide a new approach to study many-body physics in atomic ensembles and can be potentially implemented to measure many-body effects in cold atoms and other atomic/molecular systems.

Fast phase cycling in non-collinear optical two-dimensional coherent spectroscopy.

As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical 2DCS implementation by using liquid crystal phase retarders to modulate the phases of two excitation pulses. The background in the signal can be eliminated by combining either two or four interferograms measured with a proper phase configuration. The effectiveness of this method was validated in optical 2DCS measurements of an atomic vapor. This fast phase-cycling scheme will enable optical 2DCS in novel emerging applications that require enhanced detection sensitivity.

Ultrafast Carrier Dynamics of Dual Emissions from the Orthorhombic Phase in Methylammonium Lead Iodide Perovskites Revealed by Two-Dimensional Coherent Spectroscopy.

The fundamental understanding of photoexcitation landscape and dynamics in hybrid organic-inorganic perovskites is essential for improving their performance in solar cells and other applications. The dual emission features from the orthorhombic phase in perovskites have been the focus of numerous recent studies, and yet their underlying molecular origin remains elusive. We use optical two-dimensional coherent spectroscopy to study the carrier dynamics and coupling of the dual emissions in a methylammonium lead iodide film at 115 K. The two-dimensional spectra reveal an ultrafast redistribution of the photoexcited carriers into the two emission resonances within 250 fs. The high-energy resonance is a short-lived transient state, and the low-energy emission state interacts with coherent phonons. The observed carrier dynamics provide important experimental evidence that can be compared with potential theoretical models and contribute to the understanding of the dual emissions as well as the overall energy level structure in hybrid organic-inorganic perovskites.

Observation of scalable and deterministic multi-atom Dicke states in an atomic vapor

Dicke state, a coherent state of multiple particles, is fundamentally responsible for various intriguing collective behaviors of many-body systems. Experimental access to Dicke states with a scalable and deterministic number of particles is essential to study how many-body properties depend on the particle number. We report the observation of Dicke states consisting of two, three, four, five, six, and seven atoms in an atomic vapor. Quantum coherences between the ground state and multi-atom states are created and detected by using optical two-dimensional coherent spectroscopy. The signal originated from multi-atom states is manifested as correlation between the multi-quantum coherence and the emission signal, providing direct and unambiguous detection of Dicke states. The manipulation of deterministic atomic Dicke states has possible implications in quantum information processing and fundamental many-body physics.

Coherent and Incoherent Coupling Dynamics between Neutral and Charged Excitons in Monolayer MoSe2

The optical properties of semiconducting transition metal dichalcogenides are dominated by both neutral excitons (electron-hole pairs) and charged excitons (trions) that are stable even at room temperature. While trions directly influence charge transport properties in optoelectronic devices, excitons may be relevant through exciton-trion coupling and conversion phenomena. In this work, we reveal the coherent and incoherent nature of exciton-trion coupling and the relevant time scales in monolayer MoSe2 using optical two-dimensional coherent spectroscopy. Coherent interaction between excitons and trions is definitively identified as quantum beating of cross peaks in the spectra that persists for a few hundred femtoseconds. For longer times up to 10 ps, surprisingly, the relative intensity of the cross peaks increases, which is attributed to incoherent energy transfer likely due to phonon-assisted up-conversion and down-conversion processes that are efficient even at cryogenic temperature.

Coherent Excitonic Coupling in an Asymmetric Double InGaAs Quantum Well Arises from Many-Body Effects

We study an asymmetric double InGaAs quantum well using optical two-dimensional coherent spectroscopy. The collection of zero-quantum, one-quantum, and two-quantum two-dimensional spectra provides a unique and comprehensive picture of the double well coherent optical response. Coherent and incoherent contributions to the coupling between the two quantum well excitons are clearly separated. An excellent agreement with density matrix calculations reveals that coherent interwell coupling originates from many-body interactions.

Fatigue crack initiation and propagation in compact tension copper single crystals : Vinogradov, A., Hashimoto, S. and Miura, S. Z. Metallkunde (1996) 87 (2), 128–134

Optical two-dimensional coherent spectroscopy is an extremely useful tool for examining the structure and dynamics of semiconductors. The appeal of the technique is in its ability to resolve both individual-emitter and ensemble-averaged properties of disordered systems, reveal the nature of coupling between transitions, and elucidate many-body interactions. In this article, the basic principles of the technique are introduced, and its capabilities are illustrated with recent experiments that have examined optical decoherence, energy transfer, and multi-particle interactions in monolayer transition metal dichalcogenides.