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arXiv:2209.11758 · Physical Review Research

Probing molecular spectral functions and unconventional pairing using Raman spectroscopy

Oriana K. Diessel, Jonas von Milczewski, Arthur Christianen, Richard Schmidt

Published Jun 3, 2024• 10 citations
arXivHTMLPDF

Abstract

An impurity interacting with an ultracold Fermi gas can form either a polaron state or a dressed molecular state, the molaron, in which the impurity forms a bound state with one gas particle. This molaron state features rich physics, including a negative effective mass around unitarity and a first-order transition to the polaron state. However, these features have remained so far experimentally inaccessible. In this work we show theoretically how the molaron state can be directly prepared experimentally even in its excited states using Raman spectroscopy techniques. Initializing the system in the ultrastrong coupling limit, where the binding energy of the molaron is much larger than the Fermi energy, our protocol maps out the momentum-dependent spectral function of the molecule. Using a diagrammatic approach we furthermore show that the molecular spectral function serves as a direct precursor of the elusive Fulde-Ferell-Larkin-Ovchinnikov phase, which is realized for a finite density of fermionic impurity particles. Our results pave the way to a systematic understanding of how composite particles form in quantum many-body environments and provide a basis to develop new schemes for the observation of exotic phases of quantum many-body systems. Published by the American Physical Society 2024

DOI
10.1103/physrevresearch.6.023239

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An impurity interacting with an ultracold Fermi gas can form either a polaron state or a dressed molecular state, the molaron, in which the impurity forms a bound state with one gas particle. This molaron state features rich physics, including a negative effective mass around unitarity and a first-order transition to the polaron state. However, these features have remained so far experimentally inaccessible. In this work we show theoretically how the molaron state can be directly prepared experimentally even in its excited states using Raman spectroscopy techniques. Initializing the system in the ultrastrong coupling limit, where the binding energy of the molaron is much larger than the Fermi energy, our protocol maps out the momentum-dependent spectral function of the molecule. Using a diagrammatic approach we furthermore show that the molecular spectral function serves as a direct precursor of the elusive Fulde-Ferell-Larkin-Ovchinnikov phase, which is realized for a finite density of fermionic impurity particles. Our results pave the way to a systematic understanding of how composite particles form in quantum many-body environments and provide a basis to develop new schemes for the observation of exotic phases of quantum many-body systems. Published by the American Physical Society 2024
Understanding the behavior of an impurity strongly interacting with a Fermi sea is a long-standing challenge in many-body physics. When the interactions are short-ranged, two vastly different ground states exist: a polaron quasiparticle and a molecule dressed by the majority atoms. In the single-impurity limit, it is predicted that at a critical interaction strength, a first-order transition occurs between these two states. Experiments, however, are always conducted in the finite temperature and impurity density regime. The fate of the polaron-to-molecule transition under these conditions, where the statistics of quantum impurities and thermal effects become relevant, is still unknown. Here, we address this question experimentally and theoretically. Our experiments are performed with a spin-imbalanced ultracold Fermi gas with tunable interactions. Utilizing a novel Raman spectroscopy combined with a high-sensitivity fluorescence detection technique, we isolate the quasiparticle contribution and extract the polaron energy, spectral weight, and the contact parameter. As the interaction strength is increased, we observe a continuous variation of all observables, in particular a smooth reduction of the quasiparticle weight as it goes to zero beyond the transition point. Our observation is in good agreement with a theoretical model where polaron and molecule quasiparticle states are thermally occupied according to their quantum statistics. At the experimental conditions, polaron states are hence populated even at interactions where the molecule is the ground state and vice versa. The emerging physical picture is thus that of a smooth transition between polarons and molecules and a coexistence of both in the region around the expected transition.
Immersing a mobile impurity into a many-body quantum system represents a theoretically intriguing and experimentally effective way of probing its properties. In this work, we study the polaron spectral function in various environments, within the framework of Fermi-Hubbard models. Inspired by possible realizations in cold atoms and semiconductor heterostructures, we consider different configurations for the background Fermi gas, including charge density waves, multiple Fermi seas and pair superfluids. While our calculations are performed using an exact-diagonalization approach, hence limiting our analysis to systems of few interacting Fermi particles, we identify robust spectral features supported by theoretical results. Our work provides a benchmark for computations based on mean-field approaches and reveal surprising features of polaron spectra, inspiring new theoretical investigations.
In recent years, Rydberg excitations in atomic quantum gases have become a successful platform to explore quantum impurity problems. A single impurity immersed in a Fermi gas leads to the formation of a polaron, a quasiparticle consisting of the impurity being dressed by the surrounding medium. With a radius of about the Fermi wavelength, the density profile of a polaron cannot be explored using in situ optical imaging techniques. In this Letter, we propose a new experimental measurement technique that enables the in situ imaging of the polaron cloud in ultracold quantum gases. The impurity atom induces the formation of a polaron cloud and is then excited to a Rydberg state. Because of the mesoscopic interaction range of Rydberg excitations, which can be tuned by the principal numbers of the Rydberg state, atoms extracted from the polaron cloud form dimers with the impurity. By performing first principle calculations of the absorption spectrum based on a functional determinant approach, we show how the occupation of the dimer state can be directly observed in spectroscopy experiments and can be mapped onto the density profile of the gas particles, hence providing a direct, real-time, and in situ measure of the polaron cloud.
Ultracold Fermi gas is an exciting field benefiting from atomic physics, optical physics and condensed matter physics. It covers many aspects of quantum mechanics. Here I introduce some of my work during my graduate study. We proposed an optical spectroscopic method based on electromagnetically-induced transparency (EIT) as a generic probing tool that provides valuable insights into the nature of Fermi paring in ultracold Fermi gases of two hyperfine states. This technique has the capability of allowing spectroscopic response to be determined in a nearly non-destructive manner and the whole spectrum may be obtained by scanning the probe laser frequency faster than the lifetime of the sample without re-preparing the atomic sample repeatedly. Both quasiparticle picture and pseudogap picture are constructed to facilitate the physical explanation of the pairing signature in the EIT spectra. Motivated by the prospect of realizing a Fermi gas of 40 K atoms with a synthetic non-Abelian gauge field, we investigated theoretically BEC-HCS crossover physics in the presence of a Rashba spin-orbit coupling in a system of two-component Fermi gas with and without a Zeeman field that breaks the population balance. A new bound state (Rashba pair) emerges because of the spin-orbit interaction. We studied the properties of Rashba pairs using a standard pair fluctuation theory. As the two-fold spin degeneracy is lifted by spin-orbit interaction, bound pairs with mixed singlet and triplet pairings (referred to as rashbons) emerge, leading to an anisotropic superfluid. We discussed in detail the experimental signatures for observing the condensation of Rashba pairs by calculating various physical observables which characterize the properties of the system and can be measured in experiment. The role of impurities as experimental probes in the detection of quantum material properties is well appreciated. Here we studied the effect of a single classical impurity in trapped ultracold Fermi superfluids. Although a non-magnetic impurity does not change macroscopic properties of s-wave Fermi superfluids, depending on its shape and strength, a magnetic impurity can induce single or multiple mid-gap bound states. The multiple mid-gap states could coincide with the development of a Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) phase within the superfluid. As an analog of the Scanning Tunneling Microscope, we proposed a modified radio frequency spectroscopic method to measure the focal density of states which can be employed to detect these states and other quantum phases of cold atoms. A key result of our self consistent Bogoliubov-de Gennes calculations is that a magnetic impurity can controllably induce an FFLO state at currently accessible experimental parameters.
We investigate the pairing physics in a three-component Fermi-Fermi mixture, where a few fermionic impurities are immersed in a noninteracting two-component Fermi gas with synthetic spin-orbit coupling (SOC), and interact attractively with one spin species in the Fermi gas. Because of the interplay of SOC and the spin-selective interaction, the molecular state intrinsically acquires a nonzero center-of-mass momentum, which results in a new type of Fulde-Ferrell (FF) pairing in spin-orbit coupled Fermi systems. The existence of the Fermi sea can also lead to the competition between FF-like molecular states with different center-of-mass momenta, which corresponds to a first-order transition between FF phases in the thermodynamic limit. As the interaction strength is tuned, a polaron-molecule transition occurs in the highly imbalanced system, where the boundary varies nonmonotonically with SOC parameters and gives rise to the reentrance of polaron states. The rich physics in this system can be probed using existing experimental techniques.
The Fermi polaron, formed by an impurity interacting with a surrounding Fermi sea, exemplifies the canonical quasiparticle concept as a cornerstone in our description of quantum many-body systems across a wide range of energy scales. Experiments on atomic quantum gases have provided profound insights into the universal nature of the Fermi polaron. While most previous studies have focused on the case of zero impurity momentum, finite-momentum properties have remained largely uncharted. Here, we investigate the moving Fermi polaron by combining a novel Raman acceleration scheme with high-precision radio-frequency spectroscopy, exploring the quasiparticle dispersion relation over a wide range of momenta. We compare our measurements of energy shifts and spectral linewidths with a microscopic theory and reach quantitative agreement for all momenta. For low momenta, we find the energy of the moving polaron to be fully consistent with the Fermi liquid picture of a dressed particle with a constant effective mass. At high momenta, the polaron approaches the behavior of a weakly interacting bare particle, featuring small energy shifts and weak broadening. For intermediate momenta, broadening is generally larger and, most strikingly, the behavior differs for attractive and repulsive polarons. While the repulsive polaron exhibits a smooth connection between both regimes along with a monotonic change of the energy shift, the attractive case shows a peculiar non-monotonic behavior. With increasing momentum, the attractive polaron enters a regime where its energy deviates from the constant effective mass expression and broadening suddenly increases. By comparing this observation with theory, we show that this abrupt behavior coincides with the attractive polaron entering a molecule-hole continuum, where it is no longer the ground state. We interpret this as a motion-induced polaron-molecule transition.