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arXiv:2210.01874 · Physical Review Letters

Driving Alkali Rydberg Transitions with a Phase-Modulated Optical Lattice

Ryan Cardman, Georg A. Raithel

Published Jul 11, 2023• 4 citations
arXivHTMLPDF

Abstract

We develop and demonstrate a spectroscopic method for Rydberg-Rydberg transitions using a phase-controlled and -modulated, standing-wave laser field focused on a cloud of cold ^{85}Rb Rydberg atoms. The method is based on the ponderomotive (A^{2}) interaction of the Rydberg electron, which has less-restrictive selection rules than electric-dipole couplings, allowing us to probe both nS_{1/2}→nP_{1/2} and nS_{1/2}→(n+1)S_{1/2} transitions in first order. Without increase in laser power, third- and fourth-order subharmonic drives are employed to access Rydberg transitions in the 40 to 70 GHz frequency range using widely available optical phase modulators in the Ku band (12 to 18 GHz). Measurements agree well with simulations based on the model we develop. The spectra have prominent Doppler-free components with linewidths ≲200 kHz. The method paves the way for optical Doppler-free high-precision spectroscopy of Rydberg-Rydberg transitions and for spatially selective qubit manipulation with μm-scale resolution in Rydberg-based simulators and quantum computers, provided that magic states are chosen and that the atoms are sufficiently cold.

DOI
10.1103/physrevlett.131.023201

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We develop and demonstrate a spectroscopic method for Rydberg-Rydberg transitions using a phase-controlled and -modulated, standing-wave laser field focused on a cloud of cold ^{85}Rb Rydberg atoms. The method is based on the ponderomotive (A^{2}) interaction of the Rydberg electron, which has less-restrictive selection rules than electric-dipole couplings, allowing us to probe both nS_{1/2}→nP_{1/2} and nS_{1/2}→(n+1)S_{1/2} transitions in first order. Without increase in laser power, third- and fourth-order subharmonic drives are employed to access Rydberg transitions in the 40 to 70 GHz frequency range using widely available optical phase modulators in the Ku band (12 to 18 GHz). Measurements agree well with simulations based on the model we develop. The spectra have prominent Doppler-free components with linewidths ≲200 kHz. The method paves the way for optical Doppler-free high-precision spectroscopy of Rydberg-Rydberg transitions and for spatially selective qubit manipulation with μm-scale resolution in Rydberg-based simulators and quantum computers, provided that magic states are chosen and that the atoms are sufficiently cold.
Spectroscopy is an essential tool in understanding and manipulating quantum systems, such as atoms and molecules. The model describing spectroscopy includes the multipole-field interaction, which leads to established spectroscopic selection rules, and an interaction that is quadratic in the field, which is not often employed. However, spectroscopy using the quadratic (ponderomotive) interaction promises two significant advantages over spectroscopy using the multipole-field interaction: flexible transition rules and vastly improved spatial addressability of the quantum system. Here we demonstrate ponderomotive spectroscopy by using optical-lattice-trapped Rydberg atoms, pulsating the lattice light and driving a microwave atomic transition that would otherwise be forbidden by established spectroscopic selection rules. This ability to measure frequencies of previously inaccessible transitions makes possible improved determinations of atomic characteristics and constants underlying physics. The spatial resolution of ponderomotive spectroscopy is orders of magnitude better than the transition frequency would suggest, promising single-site addressability in dense particle arrays for quantum computing applications. Atomic spectroscopy is typically based on multipole atom-field interactions that obey established selection rules. Using Rydberg atoms as an example, Moore et al. show that the quadratic (ponderomotive) interaction can provide both more flexible selection rules and greater spatial addressability.
In ponderomotive spectroscopy an amplitude-modulated optical standing wave is employed to probe Rydberg-atom transitions, utilizing a ponderomotive rather than a dipole-field interaction. Here, we engage nonlinearities in the modulation to drive dipole-forbidden transitions up to the fifth order. We reach transition frequencies approaching the sub-THz regime. We also demonstrate magic-wavelength conditions, which result in symmetric spectral lines with a Fourier-limited peak at the line center. Applicability to precision measurement is discussed.
In ponderomotive spectroscopy an amplitude-modulated optical standing wave is employed to probe Rydberg-atom transitions, utilizing a ponderomotive rather than a dipole-field interaction. Here, we engage nonlinearities in the modulation to drive dipole-forbidden transitions up to the fifth order. We reach transition frequencies approaching the sub-THz regime. We also demonstrate magic-wavelength conditions, which result in symmetric spectral lines with a Fourier-limited feature at the line center. Applicability to precision measurement is discussed.
Using cold atoms, I probe the energy-level intervals between Rydberg states to high spectroscopic precision. The focus of this work is to lay the groundwork for an updated, highly-controlled measurement of the Rydberg constant using circular-state Rydberg atoms, needed to resolve a recent conflict in proton-radius values that arose in 2010 (the so-called 'proton radius puzzle'). Toward this end, I have demonstrated a fundamentally-new mechanism with which to drive atomic (Rydberg-Rydberg) transitions, utilizing an inelastic (state-changing) ponderomotive interaction. Until now, the multipole-field interaction has been the sole mechanism on which spectroscopy of atomic transitions has been based. In this work, the state-changing ponderomotive interaction ('ponderomotive spectroscopy') is demonstrated by amplitude-modulating an optical standing wave at a transition resonance of a Rydberg atom. At the core of this new spectroscopic technique is the requirement that the light intensity must be modulated in space within the atomic volume, and in time at the desired atomic transition frequency. A Rydberg atom in a modulated optical lattice is very well-suited for a demonstration of this novel type of spectroscopy. Magic-wavelength conditions of this interaction are also identified, as well as a method to drive transitions at harmonics of the modulation. Both of these features of ponderomotive spectroscopy will be utilized to simultaneously trap and probe Rydberg atoms to perform the Rydberg constant measurement. I also present a high-precision measurement of the quantum defect of a high-angular-momentum state of rubidium, the atomic species that will be used in the Rydberg constant measurement. The quantum defects of high-angular-momentum states are needed to determine the effect of the rubidium core polarizability on the Rydberg constant measurement, which is anticipated to be a leading uncertainty. Finally, I present the background and design work for a measurement of the Rydberg constant specifically tailored to help resolve the proton radius puzzle, thereby completing the major preliminary work needed for the performance of that high-precision measurement.
In this dissertation, I explore several aspects of Rydberg physics with laser spectroscopy. The experiments center around the use of a very deep, cavity-generated, one-dimensional optical lattice in a cold atom sample. The optical lattice produces elongated clouds of dense, cold atoms via dipole trapping and is able to generate extreme light shifts in the atoms due to its high intensity. I describe experiments which may be divided into two main classes. In the first, I use the dipole trap to prepare a dense sample of atoms for photoassociation of Rb atom pairs into diatomic Rydberg molecules. The Rydberg molecules are formed by low-energy scattering of the Rydberg electron of one atom from the other atom, which is a ground-state atom. This novel binding mechanism also has relevance for chemical physics. I present binding energy measurements for eight different cases of Rydberg molecules. The binding energies reveal information about electron-atom collisions, such as their scattering lengths, and about the spin couplings present within the molecular system. In the second class of experiments, I introduce two proposed measurements in which the optical lattice is ramped to very high intensity during the laser excitation, creating AC Stark shifts in the transition frequencies. In one measurement, low-lying atomic states are probed. Measurements of the light shifts are expected to yield data on the dynamic polarizability and the photoionization cross section of the 5D3/2D_{3/2}D3/2​-state in rubidium in a 1064-nm light field. I show corresponding preliminary experimental data. The polarizability and photo-ionization cross-section measurements will provide tests of atomic structure theory, which is important both at a fundamental level and for applications such as atomic clocks. In another proposed measurement, Rydberg atoms in the lattice experience ponderomotive shifts and strong mixing of their angular-momentum states, allowing direct optical excitation of the lattice-mixed high-angular-momentum states. I describe the theoretical basis and experimental preparation for spectroscopically characterizing the lattice-mixed states. The ability to optically excite selected high-angular-momentum states without the use of static or RF fields may be useful for quantum information processing and simulation.
We develop and study quantum and semiclassical models of Rydberg-atom spectroscopy in amplitude-modulated optical lattices. Both initial- and target-state Rydberg atoms are trapped in the lattice. Unlike in other spectroscopic schemes, the modulation-induced ponderomotive coupling between the Rydberg states is spatially periodic and perfectly phase-locked to the lattice trapping potentials. This leads to a type of sub-Doppler mechanism which we explain in detail. In our exact quantum model, we solve the time-dependent Schr\"odinger equation in the product space of center-of-mass (COM) momentum states and the internal-state space. We also develop a perturbative model based on the band structure in the lattice and Fermi's golden rule, as well as a semiclassical trajectory model in which the COM is treated classically and the internal-state dynamics quantum-mechanically. In all models we obtain the spectrum of the target Rydberg-state population versus the lattice modulation frequency, averaged over the initial thermal COM momentum distribution of the atoms. We investigate the quantum-classical correspondence of the problem in several parameter regimes and exhibit spectral features that arise from vibrational COM coherences and rotary-echo effects. Applications in Rydberg-atom spectroscopy are discussed.