arXiv subjects

Valentin Walther

Publications and source records attributed to Valentin Walther.

At least 19 recordsLinked to original sources

arXiv2026

Long-Range Fermi-Polaron Blockade in Monolayer MoSe$_2$

Strong optical nonlinearities at the few-photon level are a central goal for quantum photonics, yet they remain difficult to realize in solid-state systems. In doped two-dimensional semiconductors, coupling between excitons and a degenerate Fermi sea gives rise to exciton-Fermi polarons, many-body quasiparticles whose optical response is governed by fermionic correlations. Here, using femtosecond pump-probe transient absorption microscopy, we directly image the spatially resolved nonlinear optical response of exciton-Fermi polarons in monolayer MoSe$_2$. We observe a pronounced spatial suppression of resonant absorption associated with the attractive Fermi polaron, from which we extract an optical blockade radius that is more than ten times larger than that of the neutral exciton. Microscopic analysis indicates that this extended nonlinearity arises primarily from fermion-mediated interactions between exciton-Fermi polarons. Our results establish exciton-Fermi polarons in two-dimensional semiconductors as electrically tunable, strongly interacting optical quasiparticles, and identify them as a promising platform for ultralow-power nonlinear optical devices.

cond-mat.mes-hall↗

arXiv2026

Low-Energy Purification of Crystal Defects by Rydberg Excitons

Recent experiments show that optically generated Rydberg excitons in cuprous oxide can neutralize charged impurities, strongly reducing stray electric fields and effectively purifying the crystal. Here, we develop a multichannel theory of Rydberg exciton-impurity scattering that resolves the competing roles of capture, elastic scattering, and inelastic transitions between excitonic states. We find that at high collision energies, as effective under conventional single-photon excitation, purification is reduced relative to Langevin capture. These collisions are accompanied by inelastic redistribution and dominant elastic scattering, including pronounced glory scattering, which suppress purification efficiency. We identify a quantum regime at ultralow collision energies favorable for purification, where only the s-wave contributes: capture is enhanced while elastic and inelastic channels are strongly suppressed. This regime can be accessed via degenerate two-photon excitation of even-parity Rydberg excitons with tunable recoil, additionally enabling the systematic exploration of exciton-impurity scattering over a wide range of collision energies beyond what is readily achievable in atomic counterparts in atomic gas experiments.

cond-mat.mes-hall↗

arXiv2026

Three-body interactions in Rydberg lattices

Programmable arrays of neutral Rydberg atoms are one of the leading platforms today for scalable quantum simulation and computation. In these systems, the dipole-dipole interactions between the individual atoms, or qubits, typically result in binary -- i.e., two-body -- couplings. In this work, we develop an experimentally accessible scheme for engineering three-body interactions in Rydberg lattices. Such strong three-body couplings can fundamentally modify the underlying physics compared to systems with only two-body interactions: we demonstrate this, in particular, by systematically investigating the effective many-body Hamiltonian and its emergent quantum phases. This capability paves the way for the quantum simulation of a broader class of correlated models of condensed matter and high-energy physics.

cond-mat.quant-gas↗

arXiv2026

Controlling Rydberg atom-polariton interactions: from exceptional points to fast readout

Rydberg atoms represent a platform underpinning many recent developments in quantum computation, simulation, sensing, and metrology. They further facilitate optical nonlinearity at the single-photon level when coupled to photons propagating in atomic clouds, which form collective atomic excitations called Rydberg polaritons, strongly interacting with each other. Here, we experimentally explore interactions between a Rydberg polariton in an atomic ensemble and a single, adjacent, Rydberg atom. We discover three different regimes of quantum dynamics corresponding to polariton blockade, coherent exchange, and probabilistic hopping, which are defined by their distinct transmission characteristics, with a transition through an exceptional point occurring between blockade and coherent exchange. We investigate the applications of such interactions for fast, non-destructive detection of Rydberg atoms and present proof-of-principle demonstrations for their potential application in nonlinear photonic networks.

physics.atom-ph↗

arXiv2025

Attosecond Control of Squeezed Light

Squeezed light is a key resource in quantum metrology and quantum information science. It is primarily generated through nonlinear optical interactions, where the degree of squeezing is set by the nonlinearity of the medium. Here, we modulate the third-order nonlinear response of a dielectric with strong ultrafast laser fields to control squeezed light generation on attosecond time scales. By tuning a sub-cycle phase delay between the input femtosecond pulses, we switch the generated light between amplitude-squeezed and phase-squeezed states. We measure the quantum noise using a frequency-resolved balanced homodyne detection scheme that extracts field quadratures in many frequency modes simultaneously. From these measurements we obtain the complete coherency matrix containing quadrature correlations across the frequency modes of the pulse. These results enable quantum light sources with sub-cycle control of squeezing and open a route to transduction of dynamical quantum correlations in matter to quantum correlations in electric fields.

quant-ph↗

arXiv2025

Many-Body Entanglement in Solid-State Emitters

The preparation and control of quantum states lie at the heart of quantum information science (QIS). Recent advances in solid-state quantum emitters (QEs) and nanophotonics have transformed the landscape of quantum photonic technologies, enabling scalable generation of quantum states of light and matter. A new frontier in solid-state quantum photonics is the engineering of many-body interactions between QEs and photons to achieve robust coherence and controllable many-body entanglement. These entangled states, including photonic graph and cluster states, superradiant emission, and emergent quantum phases, are promising for quantum computation, sensing, and simulation. However, intrinsic inhomogeneities and decoherence in solid-state platforms pose significant challenges to realize such complex entangled states. This review provides an overview of the fundamental many-body interactions and dynamics at the light-matter interfaces of solid-state QEs, and discusses recent advances in mitigating decoherence and harnessing robust many-body coherence.

quant-ph↗

arXiv2025

Universal two-excitation scattering in two-dimensional subwavelength atomic arrays

Subwavelength atomic arrays are a leading platform for engineering strong light-matter interactions, presenting exciting opportunities for quantum science. However, a full understanding of their multi-excitation dynamics remains a significant challenge. In this work, we uncover a remarkable universal phenomenon that emerges in these arrays. Using scattering theory to analyze two-excitation interactions, we reveal a profound simplification near critical points of the collective atomic excitation band structure, determined solely from single-excitation properties. At these critical points, scattering becomes universal and the full two-excitation scattering matrix decomposes into a block-diagonal form. Remarkably, all scattering processes involving the photon field are completely suppressed, resulting in the perfect isolation of a unitary, nonlinear interaction channel between collective dark spin waves. Our findings provide exact analytical insights into few-body nonlinearities and establish a universal framework for analyzing complex scattering phenomena in ordered atomic systems.

quant-ph↗

arXiv2025

Multi-excitation scattering in subwavelength atomic arrays

Subwavelength atomic arrays are a leading platform for engineering light-matter interactions, enabling near-perfect single-photon mirrors and robust quantum memories based on long-lived dark spin waves. However, a comprehensive theory of their nonlinear, multi-excitation dynamics has remained a significant challenge. We present a unified quantum scattering theory that treats both photons and collective atomic spin waves as distinct propagating excitations interacting across different spatial dimensions. Our central result is a powerful analytical reduction: we demonstrate that the complete multi-channel S-matrix and the associated scattering cross sections are exactly determined by the effective scattering dynamics solely within the atomic spin wave subspace. This maps the complex physical problem of photon-atom interactions to a conceptually simpler one involving only atomic modes. We apply this formalism to the two-excitation case, deriving the complete analytical S-matrix and scattering cross sections for systems with two-level nonlinearities. Our work provides a versatile analytic tool for analyzing and engineering complex quantum nonlinear phenomena, including multi-excitation subradiance, in large-scale atomic systems.

quant-ph↗

arXiv2024

Optical signatures of interlayer electron coherence in a bilayer semiconductor

Emergent strongly-correlated electronic phenomena in atomically-thin transition metal dichalcogenides are an exciting frontier in condensed matter physics, with examples ranging from bilayer superconductivity~\cite{zhao2023evidence} and electronic Wigner crystals~\cite{smolenski2021signatures,zhou2021bilayer} to the ongoing quest for exciton condensation~\cite{wang2019evidence,ma2021strongly,shi2022bilayer}. Here, we experimentally investigate the properties of indirect excitons in naturally-grown MoS$_2$-homobilayer, integrated in a dual-gate device structure allowing independent control of the electron density and out-of-plane electric field. Under conditions when electron tunneling between the layers is negligible~\cite{pisoni2019absence}, upon electron doping the sample, we observe that the two excitons with opposing dipoles hybridize, displaying unusual behavior distinct from both conventional level crossing and anti-crossing. We show that these observations can be explained by static random coupling between the excitons, which increases with electron density and decreases with temperature. We argue that this phenomenon is indicative of a spatially fluctuating order parameter in the form of interlayer electron coherence, a theoretically predicted many-body state~\cite{zheng1997exchange} that has yet to be unambiguously established experimentally outside of the quantum Hall regime~\cite{sarma2008perspectives,spielman2000resonantly,kellogg2004vanishing,kellogg2002observation,spielman2001observation,fertig1989energy,shi2022bilayer}. Implications of our findings for future experiments and quantum optics applications are discussed.

cond-mat.str-el↗

arXiv2024

Dynamical Control of Excitons in Atomically Thin Semiconductors

Excitons in transition metal dichalcogenides (TMDs) have emerged as a promising platform for novel applications ranging from optoelectronic devices to quantum optics and solid state quantum simulators. While much progress has been made towards characterizing and controlling excitons in TMDs, manipulating their properties during the course of their lifetime - a key requirement for many optoelectronic device and information processing modalities - remains an outstanding challenge. Here we combine long-lived interlayer excitons in angle-aligned MoSe$_2$/WSe$_2$ heterostructures with fast electrical control to realize dynamical control schemes, in which exciton properties are not predetermined at the time of excitation but can be dynamically manipulated during their lifetime. Leveraging the out-of-plane exciton dipole moment, we use electric fields to demonstrate dynamical control over the exciton emission wavelength. Moreover, employing a patterned gate geometry, we demonstrate rapid local sample doping and toggling of the radiative decay rate through exciton-charge interactions during the exciton lifetime. Spatially mapping the exciton response reveals charge redistribution, offering a novel probe of electronic transport in twisted TMD heterostructures. Our results establish the feasibility of dynamical exciton control schemes, unlocking new directions for exciton-based information processing and optoelectronic devices, and the realization of excitonic phenomena in TMDs.

cond-mat.mes-hall↗

arXiv2024

Collapse of a quantum vortex in an attractive two-dimensional Bose gas

We experimentally and numerically study the collapse dynamics of a quantum vortex in a two-dimensional atomic superfluid following a fast interaction ramp from repulsion to attraction. We find the conditions and time scales for a superfluid vortex to radially converge into a quasi-stationary density profile, demonstrating the spontaneous formation of a vortex soliton-like structure in an atomic Bose gas. We record an emergent self-similar dynamics caused by an azimuthal modulational instability, which amplifies initial density perturbations and leads to the eventual splitting of a solitonic ring profile or direct fragmentation of a superfluid into disordered, but roughly circular arrays of Townes soliton-like wavepackets. These dynamics are qualitatively reproduced by simulations based on the Gross-Pitaevskii equation. However, a discrepancy in the magnitude of amplified density fluctuations predicted by our mean-field analysis suggests the presence of effects beyond the mean-field approximation. Our study sets the stage for exploring out-of-equilibrium dynamics of vortex quantum matter quenched to attractive interactions and their universal characteristics.

cond-mat.quant-gas↗

arXiv2024

Rydberg molecules bound by strong light fields

The coupling of an isolated quantum state to a continuum is typically associated with decoherence and decreased lifetime. Here, we demonstrate that Rydberg macrodimers, weakly bound pairs of Rydberg atoms, can overcome this dissipative mechanism and instead form bound states with the continuum of free motional states. This is enabled by the unique combination of extraordinarily slow vibrational motion in the molecular state and the optical coupling to a non-interacting continuum. Under conditions of strong coupling, we observe the emergence of distinct resonances and explain them within a Fano model. For atoms arranged on a lattice, we predict the strong continuum coupling to even stabilize molecules consisting of more than two atoms and find first signatures of these by observing atom loss correlations using a quantum gas microscope. Our results present an intriguing mechanism to control decoherence and bind multiatomic molecules using strong light-matter interactions.

quant-ph↗

arXiv2023

Taming Charged Defects: Large Scale Purification in Semiconductors using Rydberg Excitons

We investigate the interaction between highly excited Rydberg excitons and charged impurities in the semiconductor Cuprous Oxide. We find that it is long-ranged and based on charge-induced dipole interactions. We demonstrate that we can utilize this interaction to neutralize impurities throughout the whole crystal - an effect we call purification. Purification reduces detrimental electrical stray fields drastically. We find that the absorption of the purified crystal increases by up to 25 % and that the purification effect is long-lived and may persist for hundreds of microseconds or even longer. Using a time-resolved pump-probe technique, we can discriminate purification from Rydberg blockade, which has been a long-standing goal in excitonic Rydberg systems.

cond-mat.mes-hall↗

arXiv2023

Superradiant and subradiant states in lifetime-limited organic molecules through laser-induced tuning

An array of radiatively coupled emitters is an exciting new platform for generating, storing, and manipulating quantum light. However, the simultaneous positioning and tuning of multiple lifetime-limited emitters into resonance remains a significant challenge. Here we report the creation of superradiant and subradiant entangled states in pairs of lifetime-limited and sub-wavelength spaced organic molecules by permanently shifting them into resonance with laser-induced tuning. The molecules are embedded as defects in an organic nanocrystal. The pump light redistributes charges in the nanocrystal and dramatically increases the likelihood of resonant molecules. The frequency spectra, lifetimes, and second-order correlation agree with a simple quantum model. This scalable tuning approach with organic molecules provides a pathway for observing collective quantum phenomena in sub-wavelength arrays of quantum emitters.

quant-ph↗

arXiv2022

Quantum light from lossy semiconductor Rydberg excitons

The emergence of photonic quantum correlations is typically associated with emitters strongly coupled to a photonic mode. Here, we show that semiconductor Rydberg excitons, which are only weakly coupled to a free-space light mode can produce strongly antibunched fields, i.e. quantum light. This effect is fueled by micron-scale excitation blockade between Rydberg excitons inducing pair-wise polariton scattering events. Photons incident on an exciton resonance are scatted into blue- and red-detuned pairs, which enjoy relative protection from absorption and thus dominate the transmitted light. We demonstrate that this effect persists in the presence of additional phonon coupling, strong non-radiative decay and across a wide range of experimental parameters. Our results pave the way for the observation of quantum statistics from weakly coupled semiconductor excitons.

cond-mat.mes-hall↗

arXiv2021

Realizing distance-selective interactions in a Rydberg-dressed atom array

Measurement-based quantum computing relies on the rapid creation of large-scale entanglement in a register of stable qubits. Atomic arrays are well suited to store quantum information, and entanglement can be created using highly-excited Rydberg states. Typically, isolating pairs during gate operation is difficult because Rydberg interactions feature long tails at large distances. Here, we engineer distance-selective interactions that are strongly peaked in distance through off-resonant laser coupling of molecular potentials between Rydberg atom pairs. Employing quantum gas microscopy, we verify the dressed interactions by observing correlated phase evolution using many-body Ramsey interferometry. We identify atom loss and coupling to continuum modes as a limitation of our present scheme and outline paths to mitigate these effects, paving the way towards the creation of large-scale entanglement.

cond-mat.quant-gas↗

arXiv2021

Superglass formation in an atomic BEC with competing long-range interactions

The complex dynamical phases of quantum systems are dictated by atomic interactions that usually evoke an emergent periodic order. Here, we study a quantum many-body system with two competing and substantially different long-range interaction potentials where the dynamical instability towards density order can give way to a superglass phase, i. e., a superfluid disordered amorphous solid, which exhibits local density modulations but no long-range periodic order. We consider a two-dimensional BEC in the Rydberg-dressing regime coupled to an optical standing wave resonator. The dynamic pattern formation in this system is governed by the competition between the two involved interaction potentials: repulsive soft-core interactions arising due to Rydberg dressing and infinite-range sign changing interactions induced by the cavity photons. The superglass phase is found when the two interaction potentials introduce incommensurate length scales. The dynamic formation of this peculiar phase without any externally added disorder is driven by quantum fluctuations and can be attributed to frustration induced by the two competing interaction energies and length scales.

cond-mat.quant-gas↗

arXiv2021

Microwave-optical coupling via Rydberg excitons in cuprous oxide

We report exciton-mediated coupling between microwave and optical fields in cuprous oxide (Cu$_2$O) at low temperatures. Rydberg excitonic states with principal quantum number up to $n=12$ were observed at 4~K using both one-photon (absorption) and two-photon (second harmonic generation) spectroscopy. Near resonance with an excitonic state, the addition of a microwave field significantly changed the absorption lineshape, and added sidebands at the microwave frequency to the coherent second harmonic. Both effects showed a complex dependence on $n$ and angular momentum, $l$. All of these features are in semi-quantitative agreement with a model based on intraband electric dipole transitions between Rydberg exciton states. With a simple microwave antenna we already reach a regime where the microwave coupling (Rabi frequency) is comparable to the nonradiatively broadened linewidth of the Rydberg excitons. The results provide a new way to manipulate excitonic states, and open up the possibility of a cryogenic microwave to optical transducer based on Rydberg excitons.

cond-mat.mes-hall↗