arXiv subjects

M. Kroner

Publications and source records attributed to M. Kroner.

16 recordsLinked to original sources

arXiv2024

Cavity-Driven Attractive Interactions in Quantum Materials

Many-body phenomena in quantum materials emerge from the interplay among a broad continuum of electronic states, and controlling these interactions is critical for engineering novel phases. One promising approach exploits fluctuations of the vacuum electromagnetic field confined within optical cavities to tailor electronic properties. Here, we demonstrate that cavity photons can mediate attractive interactions in a tunable van der Waals material and reorganize a continuum of electron-hole transitions into an exciton-like state. We introduce a broadband, sub-wavelength time-domain microscope that integrates exfoliated, dual-gated two-dimensional quantum materials into a terahertz cavity. This approach enables the first-ever measurement of the field-tunable bandgap of bilayer graphene at terahertz frequencies while revealing ultrastrong coupling with a vacuum Rabi frequency exceeding $\Omega_{Rabi}/\omega\approx 40\%$ of the bare photon energy. Crucially, we identify a novel cavity-induced resonance emerging from the interband continuum that resembles Coulomb-bound excitons and remains stable across a broad temperature range. By uniting longstanding theoretical predictions with advanced experimental techniques, our findings open new avenues for designing and probing unique light-matter states and realizing hybrid correlated phases in quantum materials.

cond-mat.mtrl-sci↗

arXiv2024

AC-Stark Spectroscopy of Interactions between Moir\'e Excitons and Polarons

We use nonlinear pump-probe spectroscopy to study optical excitations in a charge-tunable MoSe$_2$\WS$_2$ moir\'e heterostructure. An intense red-detuned laser pulse creates a photonic dressing of the material by introducing a large virtual population of excitons or exciton polarons in a deep moir\'e potential. By measuring the resulting ac Stark effect with a weak resonant laser pulse, we gain access to the nature and mutual interactions of the elementary optical excitations. At charge neutrality, our measurements reveal that different exciton resonances, associated with confinement of their center-of-mass motion in the moir\'e potential, have a significant spatial overlap. The resulting short-range interactions manifest themselves as a density-dependent blueshift for same-valley excitons and bound biexciton states for opposite-valley excitons. The attractive polaron resonance that appears upon injection of electrons into the heterostructure shows a contrasting behavior: Here, we observe an electron-density-independent light shift and a clear pump-power-dependent saturation. These features are equivalent to that of an ensemble of independent two-level emitters and indicate a breakdown of the Fermi-polaron picture for optical excitations of electrons subject to a strong moir\'e potential. Our work establishes an experimental approach to elucidate the elementary optical excitations of semiconductor moir\'e heterostructures, providing a solid ground for the spectroscopy of correlated electronic and excitonic states in such materials.

cond-mat.str-el↗

arXiv2021

Optical sensing of fractional quantum Hall effect in graphene

Graphene and its van der Waals (vdW) heterostructures provide a unique and versatile playground for explorations of strongly correlated electronic phases, ranging from unconventional fractional quantum Hall (FQH) states in a monolayer system to a plethora of superconducting and insulating states in twisted bilayers. However, the access to those fascinating phases has been thus far entirely restricted to transport techniques, due to the lack of a robust energy bandgap that makes graphene hard to access optically. Here we demonstrate an all-optical, non-invasive spectroscopic tool for probing electronic correlations in graphene using excited Rydberg excitons in an adjacent transition metal dichalcogenide monolayer. Due to their large Bohr radii, Rydberg states are highly susceptible to the compressibility of graphene electrons, allowing us to detect the formation of odd-denominator FQH states at high magnetic fields. Owing to its sub-micron spatial resolution, the technique we demonstrate circumvents spatial inhomogeneities in vdW structures, and paves the way for optical studies of correlated states in twisted bilayer graphene and other optically inactive atomically-thin materials.

cond-mat.mes-hall↗

arXiv2021

Spin-valley relaxation dynamics of Landau-quantized electrons in MoSe$_2$ monolayer

Non-equilibrium dynamics of strongly correlated systems constitutes a fascinating problem of condensed matter physics with many open questions. Here we investigate the relaxation dynamics of Landau-quantized electron system into spin-valley polarized ground state in a gate-tunable MoSe$_2$ monolayer subjected to a strong magnetic field. The system is driven out of equilibrium with optically injected excitons that depolarize the electron spins and the subsequent electron spin-valley relaxation is probed in time-resolved experiments. We demonstrate that the relaxation rate at millikelvin temperatures sensitively depends on the Landau level filling factor: it becomes faster whenever the electrons form an integer quantum Hall liquid and slows down appreciably at non-integer fillings. Our findings evidence that valley relaxation dynamics may be used as a tool to investigate the interplay between the effects of disorder and strong interactions in the electronic ground state.

cond-mat.mes-hall↗

arXiv2020

Observation of Wigner crystal of electrons in a monolayer semiconductor

When the Coulomb repulsion between electrons dominates over their kinetic energy, electrons in two dimensional systems were predicted to spontaneously break continuous translation symmetry and form a quantum crystal. Efforts to observe this elusive state of matter, termed a Wigner crystal (WC), in two dimensional extended systems have primarily focused on electrons confined to a single Landau level at high magnetic fields, but have not provided a conclusive experimental signature of the emerging charge order. Here, we use optical spectroscopy to demonstrate that electrons in a pristine monolayer semiconductor with density $ \lesssim 3 \cdot 10^{11}$ cm$^{-2}$ form a WC. The interactions between resonantly injected excitons and electrons arranged in a periodic lattice modify the exciton band structure so that it exhibits a new umklapp resonance, heralding the presence of charge order. Remarkably, the combination of a relatively high electron mass and reduced dielectric screening allows us to observe an electronic WC state even in the absence of magnetic field. The tentative phase diagram obtained from our Hartree-Fock calculations provides an explanation of the striking experimental signatures obtained up to $B = 16$ T. Our findings demonstrate that charge-tunable transition metal dichalcogenide (TMD) monolayers enable the investigation of previously uncharted territory for many-body physics where interaction energy dominates over kinetic energy, even in the absence of a moire potential or external fields.

cond-mat.mes-hall↗

arXiv2018

Shubnikov-de Haas oscillations in optical conductivity of monolayer MoSe$_2$

We report polarization-resolved resonant reflection spectroscopy of a charge-tunable atomically-thin valley semiconductor hosting tightly bound excitons coupled to a dilute system of fully spin- and valley-polarized holes in the presence of a strong magnetic field. We find that exciton-hole interactions manifest themselves in hole-density dependent, Shubnikov-de Haas-like oscillations in the energy and line broadening of the excitonic resonances. These oscillations are evidenced to be precisely correlated with the occupation of Landau levels, thus demonstrating that strong interactions between the excitons and Landau-quantized itinerant carriers enable optical investigation of quantum-Hall physics in transition metal dichalcogenides.

cond-mat.mes-hall↗

arXiv2015

Spin measurement using cycling transitions of a two-electron quantum dot molecule

Two-electron charged self-assembled quantum dot molecules exhibit a decoherence-avoiding singlet-triplet qubit subspace and an efficient spin-photon interface. Here, we demonstrate that the cycling transitions originating from auxiliary ground states in the same system allow for an efficient optical read-out of a singlet-triplet qubit. By implementing a spin-selective state transfer to the auxiliary state using a resonant laser field, we observe an improvement approaching two orders of magnitude in fidelity as compared to spin measurement by light scattering directly from the qubit states. Embedding the quantum dot molecule inside a low quality-factor micro-cavity structure should enable single-shot qubit read-out.

cond-mat.mes-hall↗

arXiv2011

Dynamic nuclear spin polarization in resonant laser spectroscopy of a quantum dot

Resonant optical excitation of lowest-energy excitonic transitions in self-assembled quantum dots lead to nuclear spin polarization that is qualitatively different from the well known optical orientation phenomena. By carrying out a comprehensive set of experiments, we demonstrate that nuclear spin polarization manifests itself in quantum dots subjected to finite external magnetic field as locking of the higher energy Zeeman transition to the driving laser field, as well as the avoidance of the resonance condition for the lower energy Zeeman branch. We interpret our findings on the basis of dynamic nuclear spin polarization originating from non-collinear hyperfine interaction and find an excellent agreement between the experimental results and the theoretical model.

cond-mat.mes-hall↗

arXiv2009

Demagnetization of Quantum Dot Nuclear Spins: Breakdown of the Nuclear Spin Temperature Approach

The physics of interacting nuclear spins arranged in a crystalline lattice is typically described using a thermodynamic framework: a variety of experimental studies in bulk solid-state systems have proven the concept of a spin temperature to be not only correct but also vital for the understanding of experimental observations. Using demagnetization experiments we demonstrate that the mesoscopic nuclear spin ensemble of a quantum dot (QD) can in general not be described by a spin temperature. We associate the observed deviations from a thermal spin state with the presence of strong quadrupolar interactions within the QD that cause significant anharmonicity in the spectrum of the nuclear spins. Strain-induced, inhomogeneous quadrupolar shifts also lead to a complete suppression of angular momentum exchange between the nuclear spin ensemble and its environment, resulting in nuclear spin relaxation times exceeding an hour. Remarkably, the position dependent axes of quadrupolar interactions render magnetic field sweeps inherently non-adiabatic, thereby causing an irreversible loss of nuclear spin polarization.

cond-mat.mes-hall↗

arXiv2009

Confluence of resonant laser excitation and bi-directional quantum dot nuclear spin polarization

Resonant laser scattering along with photon correlation measurements have established the atom-like character of quantum dots. Here, we present measurements which challenge this identification for a wide range of experimental parameters: the absorption lineshapes that we measure at magnetic fields exceeding 1 Tesla indicate that the nuclear spins polarize by an amount that ensures locking of the quantum dot resonances to the incident laser frequency. In contrast to earlier experiments, this nuclear spin polarization is bi-directional, allowing the electron+nuclear spin system to track the changes in laser frequency dynamically on both sides of the quantum dot resonance. Our measurements reveal that the confluence of the laser excitation and nuclear spin polarization suppresses the fluctuations in the resonant absorption signal. A master equation analysis shows narrowing of the nuclear Overhauser field variance, pointing to potential applications in quantum information processing.

cond-mat.mes-hall↗

arXiv2007

Absorptive and dispersive optical responses of excitons in a single quantum dot

We have determined both the real and imaginary parts of the dielectric polarizability of a single quantum dot. The experiment is based on the observation and the manipulation of Rayleigh scattering at photon frequencies near the resonance of an optical exciton transition in single self-assembled InAs and InGaAs quantum dots. The interference between the narrow-band laser field and the weak electromagnetic field coherently scattered by the quantum dot is detected with a cryogenic Fabry-Perot setup by combined differential transmission and reflectivity measurements.

cond-mat.mes-hall↗

arXiv2007

Contrast in transmission spectroscopy of a single quantum dot

We perform transmission spectroscopy on single quantum dots and examine the effects of a resident carriers spin, the incident laser spot size, polarization, and power on the experimental contrast. We demonstrate a factor of 4 improvement in the maximum contrast by using a solid immersion lens to decrease the spot area. This increase yields a maximum signal to noise ratio of 2000 Hz-1/2, which will allow for MHz detection frequencies. We anticipate that this improvement will allow further investigation of spectral fluctuation and open up the feasibility for an all-optical read-out of an electron spin in a quantum dot.

cond-mat.mes-hall↗

arXiv2005

Absorption and photoluminescence spectroscopy on a single self-assembled charge-tunable quantum dot

We have performed detailed photoluminescence (PL) and absorption spectroscopy on the same single self-assembled quantum dot in a charge-tunable device. The transition from neutral to charged exciton in the PL occurs at a more negative voltage than the corresponding transition in absorption. We have developed a model of the Coulomb blockade to account for this observation. At large negative bias, the absorption broadens as a result of electron and hole tunneling. We observe resonant features in this regime whenever the quantum dot hole level is resonant with two-dimensional hole states located at the capping layer-blocking barrier interface in our structure.

cond-mat.mes-hall↗

arXiv2005

Voltage-controlled electron-hole interaction in a single quantum dot

The ground state of neutral and negatively charged excitons confined to a single self-assembled InGaAs quantum dot is probed in a direct absorption experiment by high resolution laser spectroscopy. We show how the anisotropic electron-hole exchange interaction depends on the exciton charge and demonstrate how the interaction can be switched on and off with a small dc voltage. Furthermore, we report polarization sensitive analysis of the excitonic interband transition in a single quantum dot as a function of charge with and without magnetic field.

cond-mat.mes-hall↗

arXiv2005

Spin-selective optical absorption of singly charged excitons in a quantum dot

We investigate high resolution laser absorption spectroscopy of a single InGaAs/GaAs self-assembled quantum dot embedded in a field-effect structure. We show experimentally that the interband optical absorption to the lower Zeeman branch of the singly charged exciton is strongly inhibited due to spin (Pauli) blockade of the optical transition. At high magnetic fields the optical absorption to the upper Zeeman branch dominates the absorption spectrum. We find however that the spin blockade is not complete and a 10% leakage remains at high magnetic fields. Applying a gate voltage to empty the dot of its resident electron turns off the spin blockade. This effect is observed at 1.5 K and up to 9 Tesla.

cond-mat.mes-hall↗

arXiv2004

Voltage-Controlled Optics of a Quantum Dot

We show how the optical properties of a single semiconductor quantum dot can be controlled with a small dc voltage applied to a gate electrode. We find that the transmission spectrum of the neutral exciton exhibits two narrow lines with $\sim 2$ $μ$eV linewidth. The splitting into two linearly polarized components arises through an exchange interaction within the exciton. The exchange interaction can be turned off by choosing a gate voltage where the dot is occupied with an additional electron. Saturation spectroscopy demonstrates that the neutral exciton behaves as a two-level system. Our experiments show that the remaining problem for manipulating excitonic quantum states in this system is spectral fluctuation on a $μ$eV energy scale.

cond-mat.mes-hall↗