Strong Many-body Interactions Research Articles

Dispersion kinks from electronic correlations in an unconventional iron-based superconductor

The attractive interaction in conventional BCS superconductors is provided by a bosonic mode. However, the pairing glue of most unconventional superconductors is unknown. The effect of electron-boson coupling is therefore extensively studied in these materials. A key signature is dispersion kinks that can be observed in the spectral function as abrupt changes in velocity and lifetime of quasiparticles. Here, we show the existence of two kinks in the unconventional iron-based superconductor RbFe2As2 using angle-resolved photoemission spectroscopy (ARPES) and dynamical mean field theory (DMFT). In addition, we observe the formation of a Hubbard band multiplet due to the combination of Coulomb interaction and Hund’s rule coupling in this multiorbital system. We demonstrate that the two dispersion kinks are a consequence of these strong many-body interactions. This interpretation is in line with a growing number of theoretical predictions for kinks in various general models of correlated materials. Our results provide a unifying link between iron-based superconductors and different classes of correlated, unconventional superconductors such as cuprates and heavy-fermion materials.

Floquet Engineering of Excitons in Two-Dimensional Halide Perovskites via Biexciton States.

Layered two-dimensional halide perovskites (2DHPs) exhibit exciting non-equilibrium properties that allow the manipulation of energy levels through coherent light-matter interactions. Under the Floquet picture, novel quantum states manifest through the optical Stark effect (OSE) following intense subresonant photoexcitation. Nevertheless, a detailed understanding of the influence of strong many-body interactions between excitons on the OSE in 2DHPs remains unclear. Herein, we uncover the crucial role of biexcitons in photon-dressed states and demonstrate precise optical control of the excitonic states via the biexcitonic OSE in 2DHPs. With fine step tuning of the driven energy, we fully parametrize the evolution of exciton resonance modulation. The biexcitonic OSE enables Floquet engineering of the exciton resonance with either a blue-shift or a red-shift of the energy levels. Our findings shed new light on the intricate nature of coherent light-matter interactions in 2DHPs and extend the degree of freedom for ultrafast coherent optical control over excitonic states.

Plasmonic-hot-electron mediated room-temperature generation of charged biexciton in monolayer WS2

Transition-metal dichalcogenide (TMDC) monolayers exhibit strong many-body Coulomb interaction, which induces rich excitonic states, including neutral exciton, trion (charged exciton), biexciton, and even charged biexciton. Despite the fact that the biexcitons in pristine two-dimensional (2D) TMDCs have great potential in forming correlated exciton pairs at distinct valleys, they lack efficient emission and optical tunability at room temperature, hindering their applications in photonic and optoelectronic devices. Here, we report room-temperature strong emission of the charged biexcitons from a gold nanosphere capped ${\mathrm{WS}}_{2}$ monolayer through localized surface plasmon (LSP) induced hot-electron injection, and demonstrate all-optical control of the emission intensity through on- or off-resonant LSP excitation. Under on-resonant LSP excitation at 2.08 eV, the photoluminescence (PL) intensity shows a superlinear scaling with the laser power density, signifying the existence of charged biexcitons; On the contrary, the off-resonant LSP excitation at 2.33 eV results in no detectable PL signal of the charged biexcitons. By calculating the energy difference between the charged biexciton and trion, we further determine the binding energy of the former to be 25 meV. Our findings offer an opportunity for understanding the many-body effect associated with the charged biexcitons of 2D TMDCs, and could facilitate their potential quantum and optoelectronic applications under ambient environment.

Nanoscale heterogeneity of ultrafast many-body carrier dynamics in triple cation perovskites

In high fluence applications of lead halide perovskites for light-emitting diodes and lasers, multi-polaron interactions and associated Auger recombination limit the device performance. However, the relationship of the ultrafast and strongly lattice coupled carrier dynamics to nanoscale heterogeneities has remained elusive. Here, in ultrafast visible-pump infrared-probe nano-imaging of the photoinduced carrier dynamics in triple cation perovskite films, a ~20 % variation in sub-ns relaxation dynamics with spatial disorder on tens to hundreds of nanometer is resolved. We attribute the non-uniform relaxation dynamics to the heterogeneous evolution of polaron delocalization and increasing scattering time. The initial high-density excitation results in faster relaxation due to strong many-body interactions, followed by extended carrier lifetimes at lower densities. These results point towards the missing link between the optoelectronic heterogeneity and associated carrier dynamics to guide synthesis and device engineering for improved perovskites device performance.

Excitonic Bloch–Siegert shift in CsPbI3 perovskite quantum dots

Coherent interaction between matter and light field induces both optical Stark effect and Bloch–Siegert shift. Observing the latter has been historically challenging, because it is weak and is often accompanied by a much stronger Stark shift. Herein, by controlling the light helicity, we can largely restrict these two effects to different spin-transitions in CsPbI3 perovskite quantum dots, achieving room-temperature Bloch–Siegert shift as strong as 4 meV with near-infrared pulses. The ratio between the Bloch–Siegert and optical Stark shifts is however systematically higher than the prediction by the non-interacting, quasi-particle model. With a model that explicitly accounts for excitonic effects, we quantitatively reproduce the experimental observations. This model depicts a unified physical picture of the optical Stark effect, biexcitonic optical Stark effect and Bloch–Siegert shift in low-dimensional materials displaying strong many-body interactions, forming the basis for the implementation of these effects to information processing, optical modulation and Floquet engineering.

Geometric energy transport and refrigeration with driven quantum dots

Geometric energy transport is of high interest both for spectroscopy of quantum devices and as a way to realize cyclic thermal machines at the nanoscale. Using a recently discovered dissipative symmetry, this work derives compact and insightful analytical expressions characterizing energy pumping with a slowly driven quantum dot subject to strong many-body interactions. Equipped with these results, the authors analyze the dot as a refrigerator or a heat pump, revealing a direct link between its efficiency and its well-known steady-state thermoelectric properties.

A simple and efficient parallel immersed boundary-lattice Boltzmann method for fully resolved simulations of incompressible settling suspensions

This study presents an efficient and parallel fully resolved direct numerical simulation (FR-DNS) of settling suspensions on multiple CPU cores based on the boundary-thickening direct forcing immersed boundary method (BTDF-IBM) and incompressible lattice Boltzmann method (LBM). The simple BTDF-IBM is used to meet the no-slip and no-penetration conditions on particle boundaries, and the incompressible LBM is used to achieve the capability of large pressure fluctuations in suspensions. In addition, a theoretical force model is used to compensate for the unresolved lubrication force between the two approaching particles. A swap strategy for the streaming step is used to reduce the memory storage of the LBM particle density functions to half. A distribution and communication strategy is proposed to handle the IBM computing and complete the immersed boundary (IB) force of the particles residing in the interface region between adjacent subdomains. The developed BTDF-IBM-LBM solver “PFlows” can simulate large particle-laden flows with more than O(106) particles and with a particle volume fraction of up to 0.4. An almost linear parallel speedup and efficiency of higher than 0.8 are obtained by testing three-dimensional (3D) cases (up to 1.0 billion fluid grids and 0.45 million particles) and two-dimensional (2D) cases (up to 1.2 billion fluid grids and 2.39 million particles). Finally, the framework is applied to three large-scale real simulations involving 50,000 particles settling in 2D and 3D bounded and unbounded domains for qualitative and quantitative validations. The particle settling behaviors and disturbed complex fluid flows in the vertical channel are demonstrated. The Boycott effect in the inclined channel is uncovered by a new mechanism that combines particle sliding at the lower sidewall with fluid convection in the upper region. The hindered settling of particles in the 3D periodic domain, which is affected by the strong particle-fluid hydrodynamic interactions and particle-particle many-body interactions at a high solid volume fraction, are analyzed. The complex behaviors and statistical characteristics of the suspensions are preliminarily revealed and analyzed, which demonstrates the prospective capability of the present framework for FR-DNS of large-scale 2D and 3D suspension flows that are relevant to many industrial applications by IB-LBM.

Interaction-enhanced transmission imaging with Rydberg atoms

Atomic-scale imaging offers a reliable tool to directly measure the movement of microscopic particles. We present a scheme for achieving a nondestructive and ultrasensitive imaging of Rydberg atoms within an ensemble of cold probe atoms. This is made possible by the interaction-enhanced electromagnetically induced transparency at off-resonance which enables an extremely narrow absorption dip for an enhanced transmission. Through the transmission of a probe beam, we obtain the distribution of Rydberg atoms with both high spatial resolution and fast response, which ensures a more precise real-time imaging. Increased resolution compared to the prior interaction-enhanced imaging technique allows us to accurately locate the atoms by adjusting the probe detuning only. This new type of interaction-enhanced transmission imaging can be utilized to other impure systems containing strong many-body interactions, and is promising to develop super-resolution microscopy of cold atoms.

Computational design of quantum defects in two-dimensional materials.

Missing atoms or atom substitutions (point defects) in crystal lattices in two-dimensional (2D) materials are potential hosts for emerging quantum technologies, such as single-photon emitters and spin quantum bits (qubits). First-principles-guided design of quantum defects in 2D materials is paving the way for rational spin qubit discovery. Here we discuss the frontier of first-principles theory development and the challenges in predicting the critical physical properties of point defects in 2D materials for quantum information technology, in particular for optoelectronic and spin-optotronic properties. Strong many-body interactions at reduced dimensionality require advanced electronic structure methods beyond mean-field theory. The great challenges for developing theoretical methods that are appropriate for strongly correlated defect states, as well as general approaches for predicting spin relaxation and the decoherence time of spin defects, are yet to be addressed.

Observation of Strong Valley Magnetic Response in Monolayer Transition Metal Dichalcogenide Alloys of Mo0.5W0.5Se2 and Mo0.5W0.5Se2/WS2 Heterostructures.

Monolayer transition metal dichalcogenide (TMD) alloys have emerged as a unique material system for promising applications in electronics, optoelectronics, and spintronics due to their tunable electronic structures, effective masses of carriers, and valley polarization with various alloy compositions. Although spin-orbit engineering has been extensively studied in monolayer TMD alloys, the valley Zeeman effect in these alloys still remains largely unexplored. Here we demonstrate the enhanced valley magnetic response in Mo0.5W0.5Se2 alloy monolayers and Mo0.5W0.5Se2/WS2 heterostructures probed by magneto-photoluminescence spectroscopy. The large g factors of negatively charged excitons (trions) of Mo0.5W0.5Se2 have been extracted for both pure Mo0.5W0.5Se2 monolayers and Mo0.5W0.5Se2/WS2 heterostructures, which are attributed to the significant impact of doping-induced strong many-body Coulomb interactions on trion emissions under an out-of-plane magnetic field. Moreover, compared with the monolayer Mo0.5W0.5Se2, the slightly reduced valley Zeeman splitting in Mo0.5W0.5Se2/WS2 is a consequence of the weakened exchange interaction arising from p-doping in Mo0.5W0.5Se2 via interlayer charge transfer between Mo0.5W0.5Se2 and WS2. Such interlayer charge transfer further evidences the formation of type-II band alignment, in agreement with the density functional theory calculations. Our findings give insights into the spin-valley and interlayer coupling effects in monolayer TMD alloys and their heterostructures, which are essential to develop valleytronic applications based on the emerging family of TMD alloys.

Large Zeeman Splitting in Out-of-Plane Magnetic Field in a Double-Layer Quantum Point Contact

In this study, we observe that the conductance of a quantum point contact on a GaAs/AlGaAs double quantum well depends significantly on the magnetic field perpendicular to the two-dimensional electron gas. In the presence of the magnetic field, the subband edge splitting due to the Zeeman energy reaches 0.09 meV at 0.16 T, thereby suggesting an enhanced g-factor. The estimated g-factor enhancement is 17.5 times that of the bare value. It is considered that a low electron density and high mobility makes it possible to reach a strong many-body interaction regime in which this type of strong enhancement in g-factor can be observed.

Parity-time symmetry and coherent perfect absorption in a cooperative atom response

Abstract Parity-Time ( P T $\mathcal{P}\mathcal{T}$ ) symmetry has become an important concept in the design of synthetic optical materials, with exotic functionalities such as unidirectional transport and nonreciprocal reflection. At exceptional points, this symmetry is spontaneously broken, and solutions transition from those with conserved intensity to exponential growth or decay. Here, we analyze a quantum-photonic surface formed by a single layer of atoms in an array with light mediating strong cooperative many-body interactions. We show how delocalized collective excitation eigenmodes can exhibit an effective P T $\mathcal{P}\mathcal{T}$ symmetry and nonexponential decay. This effective symmetry is achieved in a passive system without gain by balancing the scattering of a bright mode with the loss from a subradiant dark mode. These modes coalesce at exceptional points, evidenced by the emergence of coherent perfect absorption where coherent incoming light is perfectly absorbed and scattered only incoherently. We also show how P T $\mathcal{P}\mathcal{T}$ symmetry can be generated in total reflection and by balancing scattering and loss between different polarizations of collective modes.

Controlled melting of a Wigner ion crystal with atomic resolution

The solid-liquid phase transition (melting) is a long-standing problem for which a complete understanding is challenging because of the strong many-body interactions. A trapped-ion Wigner crystal is a suitable platform for a controlled study of this phase transition with its unprecedented resolution of individual atomic ions. Here we study the melting dynamics of a linear chain of $^{174}\mathrm{Yb}^{+}$ ions, which is initially cooled to the Doppler temperature and is then periodically heated and detected by a focused laser beam. We achieve controlled melting of the ion chain and observe unusual partial melting of long chains (coexistence of solid and liquid phases). We also observe a counterintuitive nonuniform energy distribution over the chain under localized heating. These results are further confirmed by molecular dynamics simulations to rule out other heating mechanisms.

Phonon-exciton Interactions in WSe2 under a quantizing magnetic field

Strong many-body interaction in two-dimensional transitional metal dichalcogenides provides a unique platform to study the interplay between different quasiparticles, such as prominent phonon replica emission and modified valley-selection rules. A large out-of-plane magnetic field is expected to modify the exciton-phonon interactions by quantizing excitons into discrete Landau levels, which is largely unexplored. Here, we observe the Landau levels originating from phonon-exciton complexes and directly probe exciton-phonon interaction under a quantizing magnetic field. Phonon-exciton interaction lifts the inter-Landau-level transition selection rules for dark trions, manifested by a distinctively different Landau fan pattern compared to bright trions. This allows us to experimentally extract the effective mass of both holes and electrons. The onset of Landau quantization coincides with a significant increase of the valley-Zeeman shift, suggesting strong many-body effects on the phonon-exciton interaction. Our work demonstrates monolayer WSe2 as an intriguing playground to study phonon-exciton interactions and their interplay with charge, spin, and valley.

Emergent quantum materials

Abstract

Landau-Quantized Excitonic Absorption and Luminescence in a Monolayer Valley Semiconductor.

We investigate Landau-quantized excitonic absorption and luminescence of monolayer WSe_{2} under magnetic field. We observe gate-dependent quantum oscillations in the bright exciton and trions (or exciton polarons) as well as the dark trions and their phonon replicas. Our results reveal spin- and valley-polarized Landau levels (LLs) with filling factors n=+0, +1 in the bottom conduction band and n=-0 to -6 in the top valence band, including the Berry-curvature-induced n=±0 LLs of massive Dirac fermions. The LL filling produces periodic plateaus in the exciton energy shift accompanied by sharp oscillations in the exciton absorption width and magnitude. This peculiar exciton behavior can be simulated by semiempirical calculations. The experimentally deduced g factors of the conduction band (g∼2.5) and valence band (g∼15) exceed those predicted in a single-particle model (g=1.5, 5.5, respectively). Such g-factor enhancement implies strong many-body interactions in gated monolayer WSe_{2}. The complex interplay between Landau quantization, excitonic effects, and many-body interactions makes monolayer WSe_{2} a promising platform to explore novel correlated quantum phenomena.

Harnessing Exciton-Exciton Annihilation in Two-Dimensional Semiconductors.

Strong many-body interactions in two-dimensional (2D) semiconductors give rise to efficient exciton-exciton annihilation (EEA). This process is expected to result in the generation of unbound high energy carriers. Here, we report an unconventional photoresponse of van der Waals heterostructure devices resulting from efficient EEA. Our heterostructures, which consist of monolayer transition metal dichalcogenide (TMD), hexagonal boron nitride (hBN), and few-layer graphene, exhibit photocurrent when photoexcited carriers possess sufficient energy to overcome the high energy barrier of hBN. Interestingly, we find that the device exhibits moderate photocurrent quantum efficiency even when the semiconducting TMD layer is excited at its ground exciton resonance despite the high exciton binding energy and large transport barrier. Using ab initio calculations, we show that EEA yields highly energetic electrons and holes with unevenly distributed energies depending on the scattering condition. Our findings highlight the dominant role of EEA in determining the photoresponse of 2D semiconductor optoelectronic devices.

Light-Induced Defect Healing and Strong Many-Body Interactions in Formamidinium Lead Bromide Perovskite Nanocrystals.

Organic lead halide perovskite (OLHP) nanocrystals (NCs) have paved the way to advanced optoelectronic devices through their extraordinary electrical and optical properties. However, understanding of the light-induced complex dynamic phenomena in OLHP NCs remains a subject of debate. Here we used wide field microscopy and time-resolved spectroscopy to correlate the local changes in photophysics and the dynamical behavior of photocarriers. We demonstrate that light-induced brightening of the photoluminescence from the formamidinium lead bromide NC films is related to the film preparation condition and reduction of trap density. The density of trap states is reduced via halide ion migration from interstitial position. Our femtosecond transient absorption study identifies transient Stark effect due to the generation of hot carriers. Because of slow carrier trapping, Auger recombination through many-body carrier-carrier interactions dominates over trion recombination. This work presents unprecedented insights into the light-driven processes enabling better device design in the future.

Enhancing and controlling valley magnetic response in MoS2/WS2 heterostructures by all-optical route

Van der Waals heterostructures of transition metal dichalcogenides with interlayer coupling offer an exotic platform to realize fascinating phenomena. Due to the type II band alignment of these heterostructures, electrons and holes are separated into different layers. The localized electrons induced doping in one layer, in principle, would lift the Fermi level to cross the spin-polarized upper conduction band and lead to strong manipulation of valley magnetic response. Here, we report the significantly enhanced valley Zeeman splitting and magnetic tuning of polarization for the direct optical transition of MoS2 in MoS2/WS2 heterostructures. Such strong enhancement of valley magnetic response in MoS2 stems from the change of the spin-valley degeneracy from 2 to 4 and strong many-body Coulomb interactions induced by ultrafast charge transfer. Moreover, the magnetic splitting can be tuned monotonically by laser power, providing an effective all-optical route towards engineering and manipulating of valleytronic devices and quantum-computation.

In-Plane Isotropic/Anisotropic 2D van der Waals Heterostructures for Future Devices.

Mono- to few-layers of 2D semiconducting materials have uniquely inherent optical, electronic, and magnetic properties that make them ideal for probing fundamental scientific phenomena up to the 2D quantum limit and exploring their emerging technological applications. This Review focuses on the fundamental optoelectronic studies and potential applications of in-plane isotropic/anisotropic 2D semiconducting heterostructures. Strong light-matter interaction, reduced dimensionality, and dielectric screening in mono- to few-layers of 2D semiconducting materials result in strong many-body interactions, leading to the formation of robust quasiparticles such as excitons, trions, and biexcitons. An in-plane isotropic nature leads to the quasi-2D particles, whereas, an anisotropic nature leads to quasi-1D particles. Hence, in-plane isotropic/anisotropic 2D heterostructures lead to the formation of quasi-1D/2D particle systems allowing for the manipulation of high binding energy quasi-1D particle populations for use in a wide variety of applications. This Review emphasizes an exciting 1D-2D particles dynamic in such heterostructures and their potential for high-performance photoemitters and exciton-polariton lasers. Moreover, their scopes are also broadened in thermoelectricity, piezoelectricity, photostriction, energy storage, hydrogen evolution reactions, and chemical sensor fields. The unique in-plane isotropic/anisotropic 2D heterostructures may open the possibility of engineering smart devices in the nanodomain with complex opto-electromechanical functions.