Probing molecular spectral functions and unconventional pairing using Raman spectroscopy
O. K. Diessel, J. von Milczewski, A. Christianen, R. Schmidt
Physical Review Research 6 (2), 23239 (2024).
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.
Phase diagram for strong-coupling Bose polarons
A. Christianen, J. I. Cirac, R. Schmidt
Scipost Physics 16 (3), 67 (2024).
Important properties of complex quantum many-body systems and their phase diagrams can often already be inferred from the impurity limit. The Bose polaron problem describing an impurity atom immersed in a Bose-Einstein condensate is a paradigmatic example. The interplay between the impurity-mediated attraction between the bosons and their intrinsic repulsion makes this model rich and interesting, but also complex to describe theoretically. To tackle this challenge, we develop a quantum chemistry-inspired computational technique and compare two variational methods that fully include both the boson-impurity and interboson interactions. We find one regime where the impuritymediated interactions overcome the repulsion between the bosons, so that a sweep of the boson-impurity interaction strength leads to an instability of the polaron due to the formation of many-body clusters. If instead the interboson interactions dominate, the impurity will experience a crossover from a polaron into a few-body bound state. We achieve a unified understanding incorporating both of these regimes and show that they are experimentally accessible. Moreover, we develop an analytical model that allows us to interpret these phenomena in the Landau framework of phase transitions, revealing a deep connection of the Bose polaron model to both few- and many-body physics.
Probing Polaron Clouds by Rydberg Atom Spectroscopy
M. Gievers, M. Wagner, R. Schmidt
Physical Review Letters 132 (5), 53401 (2024).
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.
Transition from a polaronic condensate to a degenerate Fermi gas of heteronuclear molecules
M. Duda, X. Y. Chen, A. Schindewolf, R. Bause, J. von Milczewski, R. Schmidt, I. Bloch, X. Y. Luo
Nature Physics 19 (5), 17 (2023).
The interplay of quantum statistics and interactions in atomic Bose-Fermi mixtures leads to a phase diagram markedly different from pure fermionic or bosonic systems. However, investigating this phase diagram remains challenging when bosons condense due to the resulting fast interspecies loss. Here we report observations consistent with a phase transition from a polaronic to a molecular phase in a density-matched degenerate Bose-Fermi mixture. The condensate fraction, representing the order parameter of the transition, is depleted by interactions, and the build-up of strong correlations results in the emergence of a molecular Fermi gas. The features of the underlying quantum phase transition represent a new phenomenon complementary to the paradigmatic Bose-Einstein condensate/Bardeen-Cooper-Schrieffer crossover observed in Fermi systems. By driving the system through the transition, we produce a sample of sodium-potassium molecules exhibiting a large molecule-frame dipole moment in the quantum-degenerate regime. Tuning interspecies interactions in atomic Bose-Fermi mixtures is shown to drive the system through a quantum phase transition. This enables the generation of heteronuclear molecules in the quantum-degenerate regime.
Bose Polaron Interactions in a Cavity-Coupled Monolayer Semiconductor
L. B. Tan, O. K. Diessel, A. Popert, R. Schmidt, A. Imamoglu, M. Kroner
Physical Review X 13 (3), 31036 (2023).
The interaction between a mobile quantum impurity and a bosonic bath leads to the formation of quasiparticles, termed Bose polarons. The elementary properties of Bose polarons, such as their mutual interactions, can differ drastically from those of the bare impurities. Here, we explore Bose polaron physics in a two-dimensional nonequilibrium setting by injecting sigma- polarized exciton-polariton impurities into a bath of coherent sigma thorn polarized polaritons generated by resonant laser excitation of monolayer MoSe2 embedded in an optical cavity. By exploiting a biexciton Feshbach resonance between the impurity and the bath polaritons, we tune the interacting system to the strong-coupling regime and demonstrate the coexistence of two new quasiparticle branches. Using time-resolved pump-probe measurements, we observe how polaron dressing modifies the interaction between impurity polaritons. Remarkably, we find that the interactions between high-energy polaron quasiparticles, which are repulsive for small bath occupancy, can become attractive in the strong impurity-bath coupling regime. Our experiments provide the first direct measurement of Bose polaron-polaron interaction strength in any physical system and pave the way for exploration and control of many-body correlations in driven-dissipative settings.
Controlled Coherent Coupling in a Quantum Dot Molecule Revealed by Ultrafast Four-Wave Mixing Spectroscopy
D. Wigger, J. Schall, M. Deconinck, N. Bart, P. Mrowinski, M. Krzykowski, K. Gawarecki, M. von Helversen, R. Schmidt, L. Bremer, F. Bopp, D. Reuter, A. D. Wieck, S. Rodt, J. Renard, G. Nogues, A. Ludwig, P. Machnikowski, J. J. Finley, S. Reitzenstein, J. Kasprzak
Acs Photonics 10 (5), 1504-1511 (2023).
Semiconductor quantum dot molecules are considered promising candidates for quantum technological applications due to their wide tunability of optical properties and coverage of different energy scales associated with charge and spin physics. While previous works have studied the tunnel-coupling of the different excitonic charge complexes shared by the two quantum dots by conventional optical spectroscopy, we here report on the first demonstration of a coherently controlled interdot tunnel-coupling focusing on the quantum coherence of the optically active trion transitions. We employ ultrafast four-wave mixing spectroscopy to resonantly generate a quantum coherence in one trion complex, transfer it to and probe it in another trion configuration. With the help of theoretical modeling on different levels of complexity, we give an instructive explanation of the underlying coupling mechanism and dynamical processes.
Impurity-induced pairing in two-dimensional Fermi gases
R. P. Li, J. von Milczewski, A. Imamoglu, R. Oldziejewski, R. Schmidt
Physical Review B 107 (15), 155135 (2023).
We study induced pairing between two identical fermions mediated by an attractively interacting quantum impurity in two-dimensional systems. Based on a stochastic variational method (SVM), we investigate the influence of confinement and finite interaction range effects on the mass ratio beyond which the ground state of the quantum three-body problem undergoes a transition from a composite bosonic trimer to an unbound dimer-fermion state. We find that confinement as well as a finite interaction range can greatly enhance trimer stability, bringing it within reach of experimental implementations such as found in ultracold atom systems. In the context of solid-state physics, our solution of the confined three-body problem shows that exciton-mediated interactions can become so dominant that they can even overcome detrimental Coulomb repulsion between electrons in atomically-thin semiconductors. Our paper thus paves the way towards a universal understanding of boson-induced pairing across various fermionic systems at finite density, and opens perspectives towards realizing unexplored forms of electron pairing beyond the conventional paradigm of Cooper pair formation.
Self-stabilized Bose polarons
R. Schmidt, T. Enss
Scipost Physics 13 (3), 54 (2022).
The mobile impurity in a Bose-Einstein condensate (BEC) is a paradigmatic many-body problem. For weak interaction between the impurity and the BEC, the impurity deforms the BEC only slightly and it is well described within the Fr??hlich model and the Bogoli-ubov approximation. For strong local attraction this standard approach, however, fails to balance the local attraction with the weak repulsion between the BEC particles and predicts an instability where an infinite number of bosons is attracted toward the im-purity. Here we present a solution of the Bose polaron problem beyond the Bogoliubov approximation which includes the local repulsion between bosons and thereby stabi-lizes the Bose polaron even near and beyond the scattering resonance. We show that the Bose polaron energy remains bounded from below across the resonance and the size of the polaron dressing cloud stays finite. Our results demonstrate how the dressing cloud replaces the attractive impurity potential with an effective many-body potential that excludes binding. We find that at resonance, including the effects of boson repul-sion, the polaron energy depends universally on the effective range. Moreover, while the impurity contact is strongly peaked at positive scattering length, it remains always finite. Our solution highlights how Bose polarons are self-stabilized by repulsion, pro-viding a mechanism to understand quench dynamics and nonequilibrium time evolution at strong coupling.
Excitonic Tonks-Girardeau and charge density wave phases in monolayer semiconductors
R. Oldziejewski, A. Chiocchetta, J. Knorzer, R. Schmidt
Physical Review B 106 (8), L081412 (2022).
Excitons in two-dimensional semiconductors provide a novel platform for fundamental studies of many-body interactions. In particular, dipolar interactions between spatially indirect excitons may give rise to strongly correlated phases of matter that so far have been out of reach of experiments. Here we show that excitonic few-body systems in atomically thin transition-metal dichalcogenides confined to a one-dimensional geometry undergo a crossover from a Tonks-Girardeau to a charge density wave regime. To this end, we take into account realistic system parameters and predict the effective exciton-exciton interaction potential. We find that the pair-correlation function contains key signatures of the many-body crossover already at small exciton numbers and show that photoluminescence spectra provide readily accessible experimental fingerprints of these strongly correlated quantum many-body states.
Tunable Feshbach Resonances and Their Spectral Signatures in Bilayer Semiconductors
C. Kuhlenkamp, M. Knap, M. Wagner, R. Schmidt, A. Imamoglu
Physical Review Letters 129 (3), 37401 (2022).
Feshbach resonances provide an invaluable tool in atomic physics, enabling precise control of interactionsand the preparation of complex quantum phases of matter. Here, we theoretically analyze a solid-state analogof a Feshbach resonance in two dimensional semiconductor heterostructures. In the presence of interlayerelectron tunneling, the scattering of excitons and electrons occupying different layers can be resonantlyenhanced by tuning an applied electric field. The emergence of an interlayer Feshbach molecule modifies theoptical excitation spectrum, and can be understood in terms of Fermi polaron formation. We discuss potentialimplications for the realization of correlated Bose-Fermi mixtures in bilayer semiconductors.
Dynamics of atoms within atoms
S. Tiwari, F. Engel, M. Wagner, R. Schmidt, F. Meinert, S. Wuster
New Journal of Physics 24 (7), 73005 (2022).
Recent experiments with Bose-Einstein condensates have entered a regime in which thousands of ground-state condensate atoms fill the Rydberg-electron orbit. After the excitation of a single atom into a highly excited Rydberg state, scattering off the Rydberg electron sets ground-state atoms into motion, such that one can study the quantum-many-body dynamics of atoms moving within the Rydberg atom. Here we study this many-body dynamics using Gross-Pitaevskii and truncated Wigner theory. Our simulations focus in particular on the scenario of multiple sequential Rydberg excitations on the same rubidium condensate which has become the standard tool to observe quantum impurity dynamics in Rydberg experiments. We investigate to what extent such experiments can be sensitive to details in the electron-atom interaction potential, such as the rapid radial modulation of the Rydberg molecular potential, or p-wave shape resonance. We demonstrate that both effects are crucial for the initial condensate response within the Rydberg orbit, but become less relevant for the density waves emerging outside the Rydberg excitation region at later times. Finally we explore the local dynamics of condensate heating. We find that it provides only minor corrections to the mean-field dynamics. Combining all these insights, our results suggest Bose-Einstein condensates as a viable platform for the in situ and real time interrogation of ultra-cold chemistry dynamics involving Rydberg states.
Bose polaron and the Efimov effect: A Gaussian-state approach
A. Christianen, J. I. Cirac, R. Schmidt
Physical Review A 105 (5), 53302 (2022).
Since the Efimov effect was introduced, a detailed theoretical understanding of Efimov physics has been developed in the few-body context. However, it has proven challenging to describe the role Efimov correlations play in many-body systems such as quenched or collapsing Bose-Einstein condensates (BECs). To study the impact the Efimov effect has in such scenarios, we consider a light impurity immersed in a weakly interacting BEC, forming a Bose polaron. In this case, correlations are localized around the impurity, making it more feasible to develop a theoretical description. Specifically, we employ a variational Gaussian state Ansatz in the reference frame of the impurity, capable of capturing both the Efimov effect and the formation of a polaron cloud consisting of a macroscopic number of particles. We find that the Efimov effect entails cooperative binding of bosons to the impurity, leading to the formation of large clusters. These many-particle Efimov states exist for a wide range of scattering lengths, with energies significantly below the polaron energy. As a result, the polaron is not the ground state, but rendered a metastable excited state which can decay into these clusters. While this decay is slow for small interaction strengths, it becomes more prominent as the attraction increases, up to a point where the polaron becomes completely unstable. We show that the critical scattering length where this happens can be interpreted as a many-body shifted Efimov resonance, where the scattering of two excitations of the bath with the polaron can lead to polaron-cloud assisted bound-state formation. Compared to the few-body case, the resonance is shifted to weaker attraction due to the participation of the polaron cloud in the cooperative binding process. This represents an intriguing example of chemistry in a quantum medium [A. Christianen et al., Phys. Rev. Lett. 128, 183401 (2022)], where many-body effects lead to a shift in the resonances of the chemical recombination, which can be directly probed in state-of-the-art experiments.
Chemistry of a Light Impurity in a Bose-Einstein Condensate
A. Christianen, J. I. Cirac, R. Schmidt
Physical Review Letters 128 (18), 183401 (2022).
Similar to an electron in a solid, an impurity in an atomic Bose-Einstein condensate (BEC) is dressed by excitations from the medium, forming a polaron quasiparticle with modified properties. This impurity can also undergo chemical recombination with atoms from the BEC, a process resonantly enhanced when universal three-body Efimov bound states cross the continuum. To study the interplay between these phenomena, we use a Gaussian state variational method able to describe both Efimov physics and arbitrarily many excitations of the BEC. We show that the polaron cloud contributes to bound state formation, leading to a shift of the Efimov resonance to smaller interaction strengths. This shifted scattering resonance marks the onset of a polaronic instability towards the decay into large Efimov clusters and fast recombination, offering a remarkable example of chemistry in a quantum medium.
Functional-renormalization-group approach to strongly coupled Bose-Fermi mixtures in two dimensions
J. von Milczewski, F. Rose, R. Schmidt
Physical Review A 105 (1), 13317 (2022).
We study theoretically the phase diagram of strongly coupled two-dimensional Bose-Fermi mixtures interacting with attractive short-range potentials as a function of the particle densities. We focus on the limit where the size of the bound state between a boson and a fermion is small compared to the average interboson separation and develop a functional-renormalization-group approach that accounts for the bound-state physics arising from the extended Frohlich Hamiltonian. By including three-body correlations we are able to reproduce the polaron-to-molecule transition in two-dimensional Fermi gases in the extreme limit of vanishing boson density. We predict frequency- and momentum-resolved spectral functions and study the impact of three-body correlations on quasiparticle properties. At finite boson density, we find that when the bound-state energy exceeds the Fermi energy by a critical value, the fermions and bosons can form a fermionic composite with a well-defined Fermi surface. These composites constitute a Fermi sea of dressed Feshbach molecules in the case of ultracold atoms, while in the case of atomically thin semiconductors a trion liquid emerges. As the boson density is increased further, the effective energy gap of the composites decreases, leading to a transition into a strongly correlated phase where polarons are hybridized with molecular degrees of freedom. We highlight the universal connection between two-dimensional semiconductors and ultracold atoms, and we discuss perspectives for further exploring the rich structure of strongly coupled Bose-Fermi mixtures in these complementary systems.
Disorder in order: Localization without randomness in a cold-atom system
F. Rose, R. Schmidt
Physical Review A 105 (1), 13324 (2022).
We present a mapping between the Edwards model of disorder describing the motion of a single particle subject to randomly positioned static scatterers and the Bose polaron problem of a light quantum impurity interacting with a Bose-Einstein condensate (BEC) of heavy atoms. The mapping offers an experimental setting to investigate the physics of Anderson localization where, by exploiting the quantum nature of the BEC, the time evolution of the quantum impurity emulates the disorder-averaged dynamics of the Edwards model. Valid in any space dimension, the mapping can be extended to include interacting particles, arbitrary disorder, or confinement and can be generalized to study many-body localization. Moreover, the corresponding exactly solvable disorder model offers means to benchmark variational approaches used to study polaron physics. Here we illustrate the mapping by focusing on the case of an impurity interacting with a one-dimensional BEC through a contact interaction. While a simple wave function based on the expansion in the number of bath excitations misses the localization physics entirely, a coherent state Ansatz combined with a canonical transformation captures the physics of disorder and Anderson localization.
Exciton-polarons in two-dimensional semiconductors and the Tavis-Cummings model
A. Imamoglu, O. Cotlet, R. Schmidt
Comptes Rendus Physique 22, 89-96 (2021).
The elementary optical excitations of a two-dimensional electron or hole system have been identified as exciton-Fermi-polarons. Nevertheless, the connection between the bound state of an exciton and an electron, termed trion, and exciton-polarons is subject of ongoing debate. Here, we use an analogy to the Tavis-Cummings model of quantum optics to show that an exciton-polaron can be understood as a hybrid quasiparticle-a coherent superposition of a bare exciton in an unperturbed Fermi sea and a bright collective excitation of many trions. The analogy is valid to the extent that the Chevy Ansatz provides a good description of dynamical screening of excitons and provided the Fermi energy is much smaller than the trion binding energy. We anticipate our results to bring new insight that could help to explain the striking differences between absorption and emission spectra of two-dimensional semiconductors.
Lossy quantum defect theory of ultracold molecular collisions
A. Christianen, G. C. Groenenboom, T. Karman
Physical Review A 104 (4), 43327 (2021).
We consider losses in collisions of ultracold molecules described by a simple statistical short-range model that explicitly accounts for the limited lifetime of classically chaotic collision complexes. This confirms that thermally sampling many isolated resonances leads to a loss cross section equal to the elastic cross section derived by Mayle et al. [Phys. Rev. A 85, 062712 (2012)] and this makes precise the conditions under which this is the case. Surprisingly, we find that the loss is nonuniversal. We also consider the case that loss broadens the short-range resonances to the point that they become overlapping. The overlapping resonances can be treated statistically even if the resonances are sparse compared to kBT, which may be the case for many molecules. The overlap results in Ericson fluctuations which yield a nonuniversal short-range boundary condition that is independent of energy over a range much wider than is sampled thermally. Deviations of experimental loss rates from the present theory beyond statistical fluctuations and the dependence on a background phase shift are interpreted as nonchaotic dynamics of short-range collision complexes.
Dispersion forces between weakly disordered van der Waals crystals
J. von Milczewski, J. R. Tolsma
Physical Review B 104 (12), 125111 (2021).
We describe a many-body theory for interlayer dispersion forces between weakly disordered atomically thin crystals and numerically investigate the role of disorder for different layer-separation distances and for different densities of induced electrons and holes. In contrast to the common wisdom that disorder tends to enhance the importance of Coulomb interactions in Fermi liquids, we find that short-range disorder tends to weaken interlayer dispersion forces. This is in line with previous findings that suggest that transitioning from metallic to insulating propagation weakens interlayer dispersion forces. We demonstrate that disorder alters the scaling laws of dispersion forces and we comment on the role of the maximally crossed vertex-correction diagrams responsible for logarithmic divergences in the resistivity of two-dimensional metals.
Ionic polaron in a Bose-Einstein condensate
G. E. Astrakharchik, L. A. P. Ardila, R. Schmidt, K. Jachymski, A. Negretti
Communications Physics 4 (1), 94 (2021).
An impurity introduced to a many-body quantum environment gets dressed by excitations and it is of a particular interest to understand the limits of the quasi-particle description. The authors theoretically and numerically study an ionic impurity immersed in a weakly interacting gas of bosonic atoms and demonstrate the existence of two main phases of a polaronic regime for weak interactions, and a strongly correlated state with many bosons bound to the ion. The presence of strong interactions in a many-body quantum system can lead to a variety of exotic effects. Here we show that even in a comparatively simple setup consisting of a charged impurity in a weakly interacting bosonic medium the competition of length scales gives rise to a highly correlated mesoscopic state. Using quantum Monte Carlo simulations, we unravel its vastly different polaronic properties compared to neutral quantum impurities. Moreover, we identify a transition between the regime amenable to conventional perturbative treatment in the limit of weak atom-ion interactions and a many-body bound state with vanishing quasi-particle residue composed of hundreds of atoms. In order to analyze the structure of the corresponding states, we examine the atom-ion and atom-atom correlation functions which both show nontrivial properties. Our findings are directly relevant to experiments using hybrid atom-ion setups that have recently attained the ultracold regime.
Optical Signatures of Periodic Charge Distribution in a Mott-like Correlated Insulator State
Y. Shimazaki, C. Kuhlenkamp, I. Schwartz, T. Smolenski, K. Watanabe, T. Taniguchi, M. Kroner, R. Schmidt, M. Knap, A. Imamoglu
Physical Review X 11 (2), 21027 (2021).
The elementary optical excitations in two-dimensional semiconductors hosting itinerant electrons are attractive and repulsive polarons-excitons that are dynamically screened by electrons. Exciton polarons have hitherto been studied in translationally invariant degenerate Fermi systems. Here, we show that periodic distribution of electrons breaks the excitonic translational invariance and leads to a direct optical signature in the exciton-polaron spectrum. Specifically, we demonstrate that new optical resonances appear due to spatially modulated interactions between excitons and electrons in an incompressible Mott-like correlated state. Our observations demonstrate that resonant optical spectroscopy provides an invaluable tool for studying strongly correlated states, such as Wigner crystals and density waves, where exciton-electron interactions are modified by the emergence of charge order.
Quantum-Zeno Fermi polaron in the strong dissipation limit
T. Wasak, R. Schmidt, F. Piazza
Physical Review Research 3, 13086 (2021).
The interplay between measurement and quantum correlations in many-body systems can lead to novel types of collective phenomena which are not accessible in isolated systems. In this work, we merge the Zeno paradigm of quantum measurement theory with the concept of polarons in condensed-matter physics. The resulting quantum-Zeno Fermi polaron is a quasiparticle which emerges for lossy impurities interacting with a quantum-degenerate bath of fermions. For loss rates of the order of the impurity-fermion binding energy, the quasiparticle is short lived. However, we show that in the strongly dissipative regime of large loss rates a long-lived polaron branch reemerges. This quantum-Zeno Fermi polaron originates from the nontrivial interplay between the Fermi surface and the surface of the momentum region forbidden by the quantum-Zeno projection. The situation we consider here is realized naturally for polaritonic impurities in charge-tunable semiconductors and can be also implemented using dressed atomic states in ultracold gases.
Mobile impurity in a Bose-Einstein condensate and the orthogonality catastrophe
N. E. Guenther, R. Schmidt, G. M. Bruun, V. Gurarie, P. Massignan
Physical Review A 103 (1), 13317 (2021).
We analyze the properties of an impurity in a dilute Bose-Einstein condensate (BEC). The quasiparticle residue of a static impurity in an ideal BEC is known to vanish exponentially with increasing particle number, leading to a bosonic orthogonality catastrophe. Here we introduce a conceptually simple variational ansatz for mobile impurities which accurately describes their macroscopic dressing in the regime close to orthogonality, including back-action onto the BEC as well as boson-boson repulsion beyond the Bogoliubov approximation. This ansatz predicts that the orthogonality catastrophe also occurs in the mobile case, whenever the BEC becomes ideal. Finally, we show that our ansatz agrees well with recent experimental results.
Observation of a Smooth Polaron-Molecule Transition in a Degenerate Fermi Gas
G. Ness, C. Shkedrov, Y. Florshaim, O. K. Diessel, J. von Milczewski, R. Schmidt, Y. Sagi
Physical Review X 10 (4), 41019 (2020).
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. Our findings establish Raman spectroscopy as a powerful experimental tool for probing the physics of mobile quantum impurities and shed new light on the competition between emerging fermionic and bosonic quasiparticles in non-Fermi-liquid phases.
Vibrational Dressing in Kinetically Constrained Rydberg Spin Systems
P. P. Mazza, R. Schmidt, I. Lesanovsky
Physical Review Letters 125 (3), 33602 (2020).
Quantum spin systems with kinetic constraints have become paradigmatic for exploring collective dynamical behavior in many-body systems. Here we discuss a facilitated spin system which is inspired by recent progress in the realization of Rydberg quantum simulators. This platform allows to control and investigate the interplay between facilitation dynamics and the coupling of spin degrees of freedom to lattice vibrations. Developing a minimal model, we show that this leads to the formation of polaronic quasiparticle excitations which are formed by many-body spin states dressed by phonons. We investigate in detail the properties of these quasiparticles, such as their dispersion relation, effective mass, and the quasiparticle weight. Rydberg lattice quantum simulators are particularly suited for studying this phonon-dressed kinetically constrained dynamics as their exaggerated length scales permit the site-resolved monitoring of spin and phonon degrees of freedom.
Dynamical Variational Approach to Bose Polarons at Finite Temperatures
D. Dzsotjan, R. Schmidt, M. Fleischhauer
Physical Review Letters 124 (22), 223401 (2020).
We discuss the interaction of a mobile quantum impurity with a Bose-Einstein condensate of atoms at finite temperature. To describe the resulting Bose polaron formation we develop a dynamical variational approach applicable to an initial thermal gas of Bogoliubov phonons. We study the polaron formation after switching on the interaction, e.g., by a radio-frequency (rf) pulse from a noninteracting to an interacting state. To treat also the strongly interacting regime, interaction terms beyond the Frohlich model are taken into account. We calculate the real-time impurity Green's function and discuss its temperature dependence. Furthermore we determine the rf absorption spectrum and find good agreement with recent experimental observations. We predict temperature-induced shifts and a substantial broadening of spectral lines. The analysis of the real-time Green's function reveals a crossover to a linear temperature dependence of the thermal decay rate of Bose polarons as unitary interactions are approached.
Theory of exciton-electron scattering in atomically thin semiconductors
C. Fey, P. Schmelcher, A. Imamoglu, R. Schmidt
Physical Review B 101 (19), 195417 (2020).
The realization of mixtures of excitons and charge carriers in van der Waals materials presents a frontier for the study of the many-body physics of strongly interacting Bose-Fermi mixtures. In order to derive an effective low-energy model for such systems, we develop an exact diagonalization approach based on a discrete variable representation that predicts the scattering and bound state properties of three charges in two-dimensional transition metal dichalcogenides. From the solution of the quantum mechanical three-body problem we thus obtain the bound state energies of excitons and trions within an effective mass model which are in excellent agreement with quantum Monte Carlo predictions. The diagonalization approach also gives access to excited states of the three-body system. This allows us to predict the scattering phase shifts of electrons and excitons that serve as input for a low-energy theory of interacting mixtures of excitons and charge carriers at finite density. To this end we derive an effective exciton-electron scattering potential that is directly applicable for quantum Monte Carlo or diagrammatic many-body techniques. As an example, we demonstrate the approach by studying the many-body physics of exciton Fermi polarons in transition-metal dichalcogenides, and we show that finite-range corrections have a substantial impact on the optical absorption spectrum. Our approach can be applied to a plethora of many-body phenomena realizable in atomically thin semiconductors ranging from exciton localization to induced superconductivity.
Interacting Polaron-Polaritons
L. Tan, O. Cotlet, A. Bergschneider, R. Schmidt, P. Back, Y. Shimazaki, M. Kroner, A. Imamoglu
Physical Review X 10 (2), 21011 (2020).
Two-dimensional semiconductors provide an ideal platform for exploration of linear exciton and polariton physics, primarily due to large exciton binding energy and strong light-matter coupling. These features, however, generically imply reduced exciton-exciton interactions, hindering the realization of active optical devices such as lasers or parametric oscillators. Here, we show that electrical injection of itinerant electrons into monolayer molybdenum diselenide allows us to overcome this limitation: dynamical screening of exciton-polaritons by electrons leads to the formation of new quasiparticles termed polaron-polaritons that exhibit unexpectedly strong interactions as well as optical amplification by Bose-enhanced polaron-electron scattering. To measure the nonlinear optical response, we carry out timeresolved pump-probe measurements and observe polaron-polariton interaction enhancement by a factor of 50 (0.5 mu eV mu m(2)) as compared to exciton-polaritons. Concurrently, we measure a spectrally integrated transmission gain of the probe field of greater than or similar to 2 stemming from stimulated scattering of polaron-polaritons. We show theoretically that the nonequilibrium nature of optically excited quasiparticles favors a previously unexplored interaction mechanism stemming from a phase-space filling in the screening cloud, which provides an accurate explanation of the strong repulsive interactions observed experimentally. Our findings show that itinerant electron-exciton interactions provide an invaluable tool for electronic manipulation of optical properties, demonstrate a new mechanism for dramatically enhancing polariton-polariton interactions, and pave the way for realization of nonequilibrium polariton condensates.
Rydberg impurity in a Fermi gas: Quantum statistics and rotational blockade
J. Sous, H. R. Sadeghpour, T. C. Killian, E. Demler, R. Schmidt
Physical Review Research 2 (2), 23021 (2020).
We consider the quench of an atomic impurity via a single Rydberg excitation in a degenerate Fermi gas. The Rydberg interaction with the background gas particles induces an ultralong-range potential that binds particles to form dimers, trimers, tetramers, etc. Such oligomeric molecules were recently observed in atomic Bose-Einstein condensates. Understanding the effects of a correlated background on molecule formation, absent in bosonic baths, is crucial to explain ongoing experiments with Fermi gases. In this work we demonstrate with a functional determinant approach that quantum statistics and fluctuations have clear observable consequences. We show that the occupation of molecular states is predicated on the Fermi statistics, which suppresses molecular formation in an emergent molecular shell structure. At high gas densities this leads to spectral narrowing, which can serve as a probe of the quantum gas thermodynamic properties. Rydberg excitations in Fermi gases go beyond traditional impurity problems, creating an opportunity for studies of mesoscopic interactions in synthetic quantum matter.
Intermolecular forces and correlations mediated by a phonon bath
X. Li, E. Yakaboylu, G. Bighin, R. Schmidt, M. Lemeshko, A. Deuchert
Journal of Chemical Physics 152 (16), 164302 (2020).
Inspired by the possibility to experimentally manipulate and enhance chemical reactivity in helium nanodroplets, we investigate the effective interaction and the resulting correlations between two diatomic molecules immersed in a bath of bosons. By analogy with the bipolaron, we introduce the biangulon quasiparticle describing two rotating molecules that align with respect to each other due to the effective attractive interaction mediated by the excitations of the bath. We study this system in different parameter regimes and apply several theoretical approaches to describe its properties. Using a Born-Oppenheimer approximation, we investigate the dependence of the effective intermolecular interaction on the rotational state of the two molecules. In the strong-coupling regime, a product-state ansatz shows that the molecules tend to have a strong alignment in the ground state. To investigate the system in the weak-coupling regime, we apply a one-phonon excitation variational ansatz, which allows us to access the energy spectrum. In comparison to the angulon quasiparticle, the biangulon shows shifted angulon instabilities and an additional spectral instability, where resonant angular momentum transfer between the molecules and the bath takes place. These features are proposed as an experimentally observable signature for the formation of the biangulon quasiparticle. Finally, by using products of single angulon and bare impurity wave functions as basis states, we introduce a diagonalization scheme that allows us to describe the transition from two separated angulons to a biangulon as a function of the distance between the two molecules.
Wigner crystals in two-dimensional transition-metal dichalcogenides: Spin physics and readout
J. Knorzer, M. J. A. Schuetz, G. Giedke, D. S. Wild, K. De Greve, R. Schmidt, M. D. Lukin, J. I. Cirac
Physical Review B 101 (12), 125101 (2020).
Wigner crystals are prime candidates for the realization of regular electron lattices under minimal requirements on external control and electronics. However, several technical challenges have prevented their detailed experimental investigation and applications to date. We propose an implementation of two-dimensional electron lattices for quantum simulation of Ising spin systems based on self-assembled Wigner crystals in transition-metal dichalcogenides. We show that these semiconductors allow for minimally invasive all-optical detection schemes of charge ordering and total spin. For incident light with optimally chosen beam parameters and polarization, we predict a strong dependence of the transmitted and reflected signals on the underlying lattice periodicity, thus revealing the charge order inherent in Wigner crystals. At the same time, the selection rules in transition-metal dichalcogenides provide direct access to the spin degree of freedom via Faraday rotation measurements.
Transport of Neutral Optical Excitations Using Electric Fields
O. Cotlet, F. Pientka, R. Schmidt, G. Zarand, E. Demler, A. Imamoglu,
Physical Review X 9, 214505 (2019).
Mobile quantum impurities interacting with a fermionic bath form quasiparticles known as Fermi polarons. We demonstrate that a force applied to the bath particles can generate a drag force of similar magnitude acting on the impurities, realizing a novel, nonperturbative Coulomb drag effect. To prove this, we calculate the fully self-consistent, frequency-dependent transconductivity at zero temperature in the Baym-Kadanoff conserving approximation. We apply our theory to excitons and exciton polaritons interacting with a bath of charge carriers in a doped semiconductor embedded in a microcavity. In external electric and magnetic fields, the drag effect enables electrical control of excitons and may pave the way for the implementation of gauge fields for excitons and polaritons. Moreover, a reciprocal effect may facilitate optical manipulation of electron transport. Our findings establish transport measurements as a novel, powerful tool for probing the many-body physics of mobile quantum impurities.
Efficient variational approach to dynamics of a spatially extended bosonic Kondo model
Y. Ashida, T. Shi, R. Schmidt, H. R. Sadeghpour, J. I. Cirac, E. Demler
Physical Review A 100 (4), 43618 (2019).
We develop an efficient variational approach to studying dynamics of a localized quantum spin coupled to a bath of mobile spinful bosons. We use parity symmetry to decouple the impurity spin from the environment via a canonical transformation and reduce the problem to a model of the interacting bosonic bath. We describe coherent time evolution of the latter using bosonic Gaussian states as a variational ansatz. We provide full analytical expressions for equations describing variational time evolution that can be applied to study in- and out-of-equilibrium phenomena in a wide class of quantum impurity problems. In the accompanying paper [Ashida et al., Phys. Rev. Lett. 123, 183001 (2019)], we present a concrete application of this general formalism to the analysis of the Rydberg central spin model, in which the spin-1/2 Rydberg impurity undergoes spin-changing collisions in a dense cloud of two-component ultracold bosons. To illustrate new features arising from orbital motion of the bath atoms, we compare our results to the Monte Carlo study of the model with spatially localized bosons in the bath, in which random positions of the atoms give rise to random couplings of the standard central spin model.
Quantum Rydberg Central Spin Model
Y. Ashida, T. Shi, R. Schmidt, H. R. Sadeghpour, J. I. Cirac, E. Demler
Physical Review Letters 123 (18), 183001 (2019).
We consider dynamics of a Rydberg impurity in a cloud of ultracold bosonic atoms in which the Rydberg electron undergoes spin-changing collisions with surrounding atoms. This system realizes a new type of quantum impurity problems that compounds essential features of the Kondo model, the Bose polaron, and the central spin model. To capture the interplay of the Rydberg-electron spin dynamics and the orbital motion of atoms, we employ a new variational method that combines an impurity-decoupling transformation with a Gaussian ansatz for the bath particles. We find several unexpected features of this model that are not present in traditional impurity problems, including interaction-induced renormalization of the absorption spectrum that eludes simple explanations from molecular bound states, and long-lasting oscillations of the Rydberg-electron spin. We discuss generalizations of our analysis to other systems in atomic physics and quantum chemistry, where an electron excitation of high orbital quantum number interacts with a spinful quantum bath.
Probing nonlocal spatial correlations in quantum gases with ultra-long-range Rydberg molecules
J. D. Whalen, S. K. Kanungo, R. Ding, M. Wagner, R. Schmidt, H. R. Sadeghpour, S. Yoshida, J. Burgdorfer, F. B. Dunning, T. C. Killian
Physical Review A 100 (1), 11402 (2019).
We present photoexcitation of ultra-long-range Rydberg molecules as a probe of spatial correlations in bosonic and fermionic quantum gases. Rydberg molecules can be created with well-defined internuclear spacing, set by the radius of the outer lobe of the Rydberg electron wave function R-n. By varying the principal quantum number n of the target Rydberg state, the molecular excitation rate can be used to map the pair-correlation function of the trapped gas g((2)) (R-n). We demonstrate this with ultracold Sr gases and probe pair-separation length scales in the range R-n= 1400-3200 a(0), which are on the order of the thermal de Broglie wavelength for temperatures around 1 mu K. We observe bunching for a single-component Bose gas of Sr-84 and antibunching due to Pauli exclusion at short distances for a polarized Fermi gas of Sr-87, revealing the effects of quantum statistics.
Site-selectively generated photon emitters in monolayer MoS2 via local helium ion irradiation
J. Klein, M. Lorke, M. Florian, F. Sigger, L. Sigl, S. Rey, J. Wierzbowski, J. Cerne, K. Müller, E. Mitterreiter, P. Zimmermann, T. Taniguchi, K. Watanabe, U. Wurstbauer, M. Kaniber, M. Knap, R. Schmidt, J. J. Finley, A. W. Holleitner
Nature Communications 10, 2755 (2019).
Quantum light sources in solid-state systems are of major interest as a basic ingredient for integrated quantum photonic technologies. The ability to tailor quantum emitters via site-selective defect engineering is essential for realizing scalable architectures. However, a major difficulty is that defects need to be controllably positioned within the material. Here, we overcome this challenge by controllably irradiating monolayer MoS2 using a sub-nm focused helium ion beam to deterministically create defects. Subsequent encapsulation of the ion exposed MoS2 flake with high-quality hBN reveals spectrally narrow emission lines that produce photons in the visible spectral range. Based on ab-initio calculations we interpret these emission lines as stemming from the recombination of highly localized electron-hole complexes at defect states generated by the local helium ion exposure. Our approach to deterministically write optically active defect states in a single transition metal dichalcogenide layer provides a platform for realizing exotic many-body systems, including coupled single-photon sources and interacting exciton lattices that may allow the exploration of Hubbard physics.
Atomtronics with a spin: Statistics of spin transport and nonequilibrium orthogonality catastrophe in cold quantum gases
J. S. You, R. Schmidt, D. A. Ivanov, M. Knap, E. Demler
Physical Review B 99 (21), 214505 (2019).
We propose to investigate the full counting statistics of nonequilibrium spin transport with an ultracold atomic quantum gas. The setup makes use of the spin control available in atomic systems to generate spin transport induced by an impurity atom immersed in a spin-imbalanced two-component Fermi gas. In contrast to solid-state realizations, in ultracold atoms spin relaxation and the decoherence from external sources is largely suppressed. As a consequence, once the spin current is turned off by manipulating the internal spin degrees of freedom of the Fermi system, the nonequilibrium spin population remains constant. Thus one can directly count the number of spins in each reservoir to investigate the full counting statistics of spin flips, which is notoriously challenging in solid-state devices. Moreover, using Ramsey interferometry, the dynamical impurity response can be measured. Since the impurity interacts with a many-body environment that is out of equilibrium, our setup provides a way to realize the nonequilibrium orthogonality catastrophe. Here, even for spin reservoirs initially prepared in a zero-temperature state, the Ramsey response exhibits an exponential decay, which is in contrast to the conventional power-law decay of Anderson's orthogonality catastrophe. By mapping our system to a multistep Fermi sea, we are able to derive analytical expressions for the impurity response at late times. This allows us to reveal an intimate connection of the decay rate of the Ramsey contrast and the full counting statistics of spin flips.