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arXiv:2003.12777 · New Journal of Physics

Two-dimensional spectroscopy of Rydberg gases

K. Mukherjee, Himangshu Prabal Goswami, S. Whitlock, Sebastian Wüster, Alexander Eisfeld

Published Jun 4, 2020• 8 citations
arXivHTMLPDF

Abstract

Abstract Two-dimensional (2D) spectroscopy uses multiple electromagnetic pulses to infer the properties of a complex system. A paradigmatic class of target systems are molecular aggregates, for which one can obtain information on the eigenstates, various types of static and dynamic disorder and on relaxation processes. However, two-dimensional spectra can be difficult to interpret without precise knowledge of how the signal components relate to microscopic Hamiltonian parameters and system-bath interactions. Here we show that two-dimensional spectroscopy can be mapped in the microwave domain to highly controllable Rydberg quantum simulators. By porting 2D spectroscopy to Rydberg atoms, we firstly open the possibility of its experimental quantum simulation, in a case where parameters and interactions are very well known. Secondly, the technique may provide additional handles for experimental access to coherences between system states and the ability to discriminate different types of decoherence mechanisms in Rydberg gases. We investigate the requirements for a specific implementation utilizing multiple phase coherent microwave pulses and a phase cycling technique to isolate signal components.

DOI
10.1088/1367-2630/ab9984

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Abstract Two-dimensional (2D) spectroscopy uses multiple electromagnetic pulses to infer the properties of a complex system. A paradigmatic class of target systems are molecular aggregates, for which one can obtain information on the eigenstates, various types of static and dynamic disorder and on relaxation processes. However, two-dimensional spectra can be difficult to interpret without precise knowledge of how the signal components relate to microscopic Hamiltonian parameters and system-bath interactions. Here we show that two-dimensional spectroscopy can be mapped in the microwave domain to highly controllable Rydberg quantum simulators. By porting 2D spectroscopy to Rydberg atoms, we firstly open the possibility of its experimental quantum simulation, in a case where parameters and interactions are very well known. Secondly, the technique may provide additional handles for experimental access to coherences between system states and the ability to discriminate different types of decoherence mechanisms in Rydberg gases. We investigate the requirements for a specific implementation utilizing multiple phase coherent microwave pulses and a phase cycling technique to isolate signal components.
Optical multidimensional coherent spectroscopy is a powerful tool for studying structure and dynamics in complex systems, such as semiconductors. In optical two-dimensional coherent spectroscopy (2DCS), where the spectrum is presented in a two-dimensional (2D) plane with two frequency axes, an important advantage is the ability to isolate quantum pathways by unfolding a one-dimensional spectrum onto a 2D plane. For many systems, however, the quantum pathways are only partially separated in a 2D spectrum. In order to completely isolate the quantum pathways, we extend 2DCS into a third dimension to generate three-dimensional (3D) spectra in which the spectrum is further unfolded. A 3D spectrum provides complete and well-isolated information of the third-order optical response of the system. The information can be used to fully characterize the quantum pathways and to determine the system’s Hamiltonian. Quantitative knowledge of the Hamiltonian enables prediction and control of quantum processes. For instance, such information is essential for deterministic control and improved performance of coherent control schemes.
Nonequilibrium dynamics are closely related to various fields of research, in which vastly different phases emerge when parameters are changed. However, it is difficult to construct nonequilibrium systems that have sufficiently tunable controllable parameters. Using microwave field coupling induced optical bistability, Rydberg gases exhibit a range of significantly different optical responses. In conjunction with electromagnetically induced transparency, the microwave coupling can create versatile nonequilibrium dynamics. In particular, the microwave coupling of two Rydberg states provides an additional handle for controlling the dynamics. And the microwave-controlled nonequilibrium phase transition has the potential to be applied in microwave field measurement. This study opens a new avenue to exploring bistable dynamics using microwave-coupled Rydberg gases, and developing quantum technological applications.
Abstract As was recently shown in Abumwis et al (2020 Phys. Rev. Lett. 124 193401), many eigenstates of a random Rydberg gas with resonant dipole–dipole interactions are highly delocalized. Although the high degree of delocalization is generic to various types of power-law interactions and to both two and three-dimensional systems, in their detailed aspects the coherence distributions are sensitive to these parameters and vary dramatically between different systems. We calculate the eigenstates of both two and three-dimensional gases and quantify their delocalization throughout the atoms in the gas using a coherence measure. By contrasting the angular dependence of the dipole–dipole interaction with an isotropic interaction we obtain additional information about the generic physical principles underlying random interacting systems. We also investigate the density of states and microwave absorption spectra to obtain information about the types of measurements where these delocalized states play a role, and to check that these delocalized eigenstates are robust against various types of perturbation.
Two-dimensional (2D) spectroscopy has been intensively used to study electronic and vibronic coherences in biological systems and semiconductors. This technique studies coherent as well as incoherent signals that arise from the nonlinear interaction of a sequence of laser pulses. In this paper we present a direct evaluation of the 2D signal based on elementary quantum kinetics in order to compare with the common approximate diagrammatic approaches. Here we consider incoherent action signals such as fluorescence or photocurrent as the observable, which is easily accessible in a measurement. These observables are calculated by solving the time evolution of the density matrix in the Lindblad form, which can take into account all possible decoherence processes. The phase modulation technique is used to separate the relevant nonlinear signals from the other possible interaction pathways. The approach can be used to calculate 2D spectra of any quantum system. For our model system we find a good agreement for the quantum beating between the coupled states.
The field of coherent control has today been seeing significant progress, in a wide array of physical systems. One such system is the Rydberg atom. The long lifetime, strong dipole interactions, multiple degrees of freedom, and simple atomic structure make Rydberg atoms particularly appealing for experiments involving coherent control. The same properties have led to the exploration of Rydberg atoms as candidates for quantum information storage, processing and retrieval. Quantum information processing is a particular application of coherent control. Rather than being disparate subjects of study, coherent control of Rydberg atoms and processing of information stored as phase in different Rydberg levels are two sides of the same coin. In this dissertation, we experimentally characterize the effect of a half-cycle pulse on the phases of the states of a Rydberg wave packet and their mutual coherence. This has bearing both on our ability to control the states of the atom and on our ability to measure the information stored as quantum phase. We observe delay dependent phase shifts and losses of coherence. Despite a loss of information due to transfer of quantum amplitude to states outside the data register, we demonstrate partial retrieval of that information by the application of a second half cycle pulse. We also present an essential states model of the interaction, and we compare results from the model to experimental features observed. Although the particulars may vary, the concepts involved are quite general and may be applied to multilevel systems other than Rydberg atoms.
We introduce molecular coherent three-quantum (3Q) two-dimensional (2D) fluorescence spectroscopy with phase cycling via shot-to-shot pulse shaping at a 1 kHz repetition rate. This allows us to acquire simultaneously, within a single scan, three fourth-order and six sixth-order signals correlating various one-quantum, two-quantum, and 3Q coherences. We demonstrate the approach on the dye molecule rhodamine 700 and reproduce all nine 2D data sets, including their absolute signal strengths, with simulations using a single, consistent set of model parameters. We observe a linear concentration dependence of all nonlinear signals, evidencing the absence of cascades and many-particle signals of noninteracting molecules. The single-beam, background-free implementation allows direct comparability between various nonlinear signal types and provides information about multiple excited states. Apart from molecules, the method is expected to be applicable to supramolecular systems, polymers, and solid-state materials with the prospect of revealing signatures of bi- and triexcitonic states.