Showing 1–26 of 26 results for author: Walther, V

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

Authors: Jonas Peterson, Shibalik Lahiri, Monique Tie, Shibin Deng, Jierong Wang, Minxue Wang, Luke Holtzman, James Hone, Takashi Taniguchi, Kenji Watanabe, Tony Heinz, Valentin Walther, Libai Huang

Abstract: 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… ▽ More 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. △ Less

Submitted 27 May, 2026; originally announced May 2026.

Low-Energy Purification of Crystal Defects by Rydberg Excitons

Authors: Shiva Kant Tiwari, Tijs Karman, Valentin Walther

Abstract: 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… ▽ More 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. △ Less

Submitted 29 April, 2026; originally announced April 2026.

Comments: 18 pages and 9 figures

Three-body interactions in Rydberg lattices

Authors: Rhine Samajdar, Mikhail D. Lukin, Valentin Walther

Abstract: 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 lattic… ▽ More 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. △ Less

Submitted 13 April, 2026; originally announced April 2026.

Comments: 8+8 pages, 5+5 figures

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

Authors: Tamara Šumarac, Emily H. Qiu, Shai Tsesses, Peiran Niu, Adrian J. Menssen, Wenchao Xu, Valentin Walther, Uroš Delić, Soonwon Choi, Mikhail D. Lukin, Vladan Vuletić

Abstract: 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 int… ▽ More 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. △ Less

Submitted 9 January, 2026; originally announced January 2026.

Optical signatures of interlayer electron coherence in a bilayer semiconductor

Authors: Xiaoling Liu, Nadine Leisgang, Pavel E. Dolgirev, Alexander A. Zibrov, Jiho Sung, Jue Wang, Takashi Taniguchi, Kenji Watanabe, Valentin Walther, Hongkun Park, Eugene Demler, Philip Kim, Mikhail D. Lukin

Abstract: 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,shi20… ▽ More 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. △ Less

Submitted 12 September, 2024; originally announced September 2024.

Dynamical Control of Excitons in Atomically Thin Semiconductors

Authors: Eric L. Peterson, Trond I. Andersen, Giovanni Scuri, Andrew Y. Joe, Andrés M. Mier Valdivia, Xiaoling Liu, Alexander A. Zibrov, Bumho Kim, Takashi Taniguchi, Kenji Watanabe, James Hone, Valentin Walther, Hongkun Park, Philip Kim, Mikhail D. Lukin

Abstract: 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 optoelectron… ▽ More 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. △ Less

Submitted 17 July, 2024; v1 submitted 15 July, 2024; originally announced July 2024.

Comments: 37 pages, 4 figures in main text, 6 figures in supplemental materials; (v2) corrected funding acknowledgements

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

Authors: Sambit Banerjee, Kai Zhou, Shiva Kant Tiwari, Hikaru Tamura, Rongjie Li, Panayotis Kevrekidis, Simeon I. Mistakidis, Valentin Walther, Chen-Lung Hung

Abstract: 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 Bo… ▽ More 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. △ Less

Submitted 28 June, 2025; v1 submitted 2 June, 2024; originally announced June 2024.

Comments: arXiv v3, 16 pages, 4 figures in main text, 8 in supplementary

Journal ref: Phys. Rev. Lett. 135, 073401 (2025)

Rydberg molecules bound by strong light fields

Authors: Simon Hollerith, Valentin Walther, Kritsana Srakaew, David Wei, Daniel Adler, Suchita Agrawal, Pascal Weckesser, Immanuel Bloch, Johannes Zeiher

Abstract: 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 mo… ▽ More 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. △ Less

Submitted 10 January, 2024; originally announced January 2024.

The rise and fall of patterns in driven-dissipative Rydberg polaritons

Authors: H. Alaeian, V. Walther

Abstract: Spatial structures commonly emerge in interacting nonlinear systems. In this study, we focus on the out-of-equilibrium dynamics of the recently-established platform of Rydberg exciton-polaritons, fueled by their characteristic long-range non-local interactions, in the presence of an external drive and dissipation. Our work elucidates how modulational instability sets off spontaneous density patter… ▽ More Spatial structures commonly emerge in interacting nonlinear systems. In this study, we focus on the out-of-equilibrium dynamics of the recently-established platform of Rydberg exciton-polaritons, fueled by their characteristic long-range non-local interactions, in the presence of an external drive and dissipation. Our work elucidates how modulational instability sets off spontaneous density pattern formations in a Rydberg polariton system with characteristic scales in the micron range. Under conditions of an unstable flattop state, we track the evolution of the polariton ensemble, showing the emergence of meta-stable patterns and their collapse in the long-time limit. We trace this phenomenon back to the destructive interference between the polariton state and the pump in a driven ensemble. Finally, we map out conditions that allow stable patterns to form under incoherent pumping. These findings provide new opportunities for exploring the emerging field of long-range interacting gases through Rydberg exciton-polaritons. △ Less

Submitted 25 November, 2023; originally announced November 2023.

Comments: 6 pages and 4 figures

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

Authors: Martin Bergen, Valentin Walther, Binodbihari Panda, Mariam Harati, Simon Siegeroth, Julian Heckötter, Marc Aßmann

Abstract: 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… ▽ More 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. △ Less

Submitted 18 October, 2023; originally announced October 2023.

Comments: 13 pages, 7 figures

Quantum light from lossy semiconductor Rydberg excitons

Authors: Valentin Walther, Anders S. Sørensen

Abstract: 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 polarit… ▽ More 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. △ Less

Submitted 29 November, 2022; originally announced November 2022.

Comments: 11 pages, 6 figures

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

Authors: Simon Hollerith, Kritsana Srakaew, David Wei, Antonio Rubio-Abadal, Daniel Adler, Pascal Weckesser, Andreas Kruckenhauser, Valentin Walther, Rick van Bijnen, Jun Rui, Christian Gross, Immanuel Bloch, Johannes Zeiher

Abstract: 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 enginee… ▽ More 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. △ Less

Submitted 19 October, 2021; originally announced October 2021.

Comments: 5 pages, 4 figures + supplementary information

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

Authors: Stefan Ostermann, Valentin Walther, Susanne F. Yelin

Abstract: 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 ex… ▽ More 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. △ Less

Submitted 11 January, 2022; v1 submitted 29 September, 2021; originally announced September 2021.

Comments: new title, added references

Microwave-optical coupling via Rydberg excitons in cuprous oxide

Authors: Liam A. P. Gallagher, Joshua P. Rogers, Jon D. Pritchett, Rajan A. Mistry, Danielle Pizzey, Charles S. Adams, Matthew P. A Jones, Peter Grünwald, Valentin Walther, Chris Hodges, Wolfgang Langbein, Stephen A. Lynch

Abstract: 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 t… ▽ More 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. △ Less

Submitted 7 October, 2021; v1 submitted 20 September, 2021; originally announced September 2021.

Comments: 18 pages, 8 figures

Nonclassical Light from Exciton Interactions in a Two-Dimensional Quantum Mirror

Authors: Valentin Walther, Lida Zhang, Susanne F. Yelin, Thomas Pohl

Abstract: Excitons in a semiconductor monolayer form a collective resonance that can reflect resonant light with extraordinarily high efficiency. Here, we investigate the nonlinear optical properties of such atomistically thin mirrors and show that finite-range interactions between excitons can lead to the generation of highly non-classical light. We describe two scenarios, in which optical nonlinearities a… ▽ More Excitons in a semiconductor monolayer form a collective resonance that can reflect resonant light with extraordinarily high efficiency. Here, we investigate the nonlinear optical properties of such atomistically thin mirrors and show that finite-range interactions between excitons can lead to the generation of highly non-classical light. We describe two scenarios, in which optical nonlinearities arise either from direct photon coupling to excitons in excited Rydberg states or from resonant two-photon excitation of Rydberg excitons with finite-range interactions. The latter case yields conditions of electromagnetically induced transparency and thereby provides an efficient mechanism for single-photon switching between high transmission and reflectance of the monolayer, with a tunable dynamical timescale of the emerging photon-photon interactions. Remarkably, it turns out that the resulting high degree of photon correlations remains virtually unaffected by Rydberg-state decoherence, in excess of non-radiative decoherence observed for ground-state excitons in two-dimensional semiconductors. This robustness to imperfections suggests a promising new approach to quantum photonics at the level of individual photons. △ Less

Submitted 20 February, 2021; originally announced February 2021.

Comments: 11 pages, 7 figures

Self-bound droplet clusters in laser-driven Bose-Einstein condensates

Authors: Yong-Chang Zhang, Valentin Walther, Thomas Pohl

Abstract: We investigate a two-dimensional Bose-Einstein condensate that is optically driven via a retro-reflecting mirror, forming a single optical feedback loop. This induces a peculiar type of long-range atomic interaction with highly oscillatory behavior, and we show here how the sign of the underlying interaction potential can be controlled by additional optical elements and external fields. This addit… ▽ More We investigate a two-dimensional Bose-Einstein condensate that is optically driven via a retro-reflecting mirror, forming a single optical feedback loop. This induces a peculiar type of long-range atomic interaction with highly oscillatory behavior, and we show here how the sign of the underlying interaction potential can be controlled by additional optical elements and external fields. This additional tunability enriches the behavior of the system substantially, and gives rise to a surprising range of new ground states of the condensate. In particular, we find the emergence of self-bound crystals of quantum droplets with various lattice structures, from simple and familiar triangular arrays to complex superlattice structures and crystals with entirely broken rotational symmetry. This includes mesoscopic clusters composed of small numbers of quantum droplets as well as extended crystalline structures. Importantly, such ordered states are entirely self-bound and stable without any external in-plane confinement, having no counterpart to other quantum-gas settings with long-range atomic interactions. △ Less

Submitted 9 November, 2020; originally announced November 2020.

Comments: 7 pages, 6 figures

Journal ref: Phys. Rev. A 103, 023308 (2021)

Asymmetric Rydberg blockade of giant excitons in Cuprous Oxide

Authors: Julian Heckötter, Valentin Walther, Stefan Scheel, Manfred Bayer, Thomas Pohl, Marc Aßmann

Abstract: The ability to generate and control strong long-range interactions via highly excited electronic states has been the foundation for recent breakthroughs in a host of areas, from atomic and molecular physics [1, 2] to quantum optics [3, 4] and technology [5-7]. Rydberg excitons provide a promising solid-state realization of such highly excited states, for which record-breaking orbital sizes of up t… ▽ More The ability to generate and control strong long-range interactions via highly excited electronic states has been the foundation for recent breakthroughs in a host of areas, from atomic and molecular physics [1, 2] to quantum optics [3, 4] and technology [5-7]. Rydberg excitons provide a promising solid-state realization of such highly excited states, for which record-breaking orbital sizes of up to a micrometer have indeed been observed in cuprous oxide semiconductors [8]. Here, we demonstrate the generation and control of strong exciton interactions in this material by optically producing two distinct quantum states of Rydberg excitons. This makes two-color pump-probe experiments possible that allow for a detailed probing of the interactions. Our experiments reveal the emergence of strong spatial correlations and an inter-state Rydberg blockade that extends over remarkably large distances of several micrometers. The generated many-body states of semiconductor excitons exhibit universal properties that only depend on the shape of the interaction potential and yield clear evidence for its vastly extended-range and power-law character. △ Less

Submitted 29 October, 2020; originally announced October 2020.

Comments: Main script: 7 pages, 3 figures. Supplementary file 15 pages, 5 figures

Electromagnetically induced transparency with Cu$_2$O excitons in the presence of phonon coupling

Authors: Valentin Walther, Peter Grünwald, Thomas Pohl

Abstract: Highly excited Rydberg states of excitons in Cu$_2$O semiconductors provide a promising approach to explore and control strong particle interactions in a solid-state environment. A major obstacle has been the substantial absorption background that stems from exciton-phonon coupling and lies under the Rydberg excitation spectrum, weakening the effects of exciton interactions. Here, we demonstrate t… ▽ More Highly excited Rydberg states of excitons in Cu$_2$O semiconductors provide a promising approach to explore and control strong particle interactions in a solid-state environment. A major obstacle has been the substantial absorption background that stems from exciton-phonon coupling and lies under the Rydberg excitation spectrum, weakening the effects of exciton interactions. Here, we demonstrate that two-photon excitation of Rydberg excitons under conditions of electromagnetically induced transparency (EIT) can be used to control this background. Based on a microscopic theory that describes the known single-photon absorption spectrum, we analyze the conditions under which two-photon EIT permits separating the optical Rydberg excitation from the phonon-induced absorption background, and even suppressing it entirely. Our findings thereby pave the way for the exploitation of Rydberg blockade with Cu$_2$O excitons in nonlinear optics and other applications. △ Less

Submitted 14 July, 2020; originally announced July 2020.

Comments: 11 pages, 6 figures

Journal ref: Phys. Rev. Lett. 125, 173601 (2020)

Plasma-enhanced interaction and optical nonlinearities of Cu$_2$O Rydberg excitons

Authors: Valentin Walther, Thomas Pohl

Abstract: We theoretically investigate the nonlinear optical transmission through a cuprous oxide crystal for wavelengths that cover the series of highly excited excitons, observed in recent experiments. Since such Rydberg excitons have strong van der Waals interactions, they can dynamically break the conditions for resonant exciton creation and dramatically modify the refractive index of the material in a… ▽ More We theoretically investigate the nonlinear optical transmission through a cuprous oxide crystal for wavelengths that cover the series of highly excited excitons, observed in recent experiments. Since such Rydberg excitons have strong van der Waals interactions, they can dynamically break the conditions for resonant exciton creation and dramatically modify the refractive index of the material in a nonlinear manner. We explore this mechanism theoretically and determine its effects on the optical properties of a semiconductor for the case of degenerate pair-state asymptotes of Rydberg excitons in Cu$_2$O. Upon analyzing the additional effects of a dilute residual electron-hole plasma, we find quantitative agreement with previous transmission measurements, which provides strong indications for the enhancement of Rydberg-induced nonlinearities by surrounding free charges. △ Less

Submitted 30 March, 2020; originally announced March 2020.

Comments: 12 pages, 7 figures

Journal ref: Phys. Rev. Lett. 125, 097401 (2020)

Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2

Authors: Jie Gu, Valentin Walther, Lutz Waldecker, Daniel Rhodes, Archana Raja, James C. Hone, Tony F. Heinz, Stephane Kena-Cohen, Thomas Pohl, Vinod M. Menon

Abstract: Strong optical nonlinearities play a central role in realizing quantum photonic technologies. In solid state systems, exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. Here, the interaction between excitons forms the basis of the polaritonic nonlinearity. While the interaction between grou… ▽ More Strong optical nonlinearities play a central role in realizing quantum photonic technologies. In solid state systems, exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. Here, the interaction between excitons forms the basis of the polaritonic nonlinearity. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such ground state interactions is generally not sufficient to reach the regime of quantum nonlinear optics and strong single-polariton interactions. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities, as demonstrated with high-lying Rydberg states of cold atomic systems. Excitons in excited states have recently been observed in monolayer transition metal dichalcogenides. Here we demonstrate the formation of exciton-polaritons using the first excited excitonic state in monolayer tungsten diselenide (WSe2) embedded in a microcavity. Owing to the larger exciton size compared to their ground state counterpart, the realized polaritons exhibit an enhanced nonlinear response by more than an order of magnitude, as evidenced through a modification of the cavity Rabi splitting. The demonstration of excited exciton-polaritons in two-dimensional semiconductors and their enhanced nonlinear response presents the first step towards the generation of strong photon interactions in solid state systems, a necessary building block for quantum photonic technologies. △ Less

Submitted 28 December, 2019; originally announced December 2019.

Blockade-induced resonant enhancement of the optical nonlinearity in a Rydberg medium

Authors: Annika Tebben, Clément Hainaut, Valentin Walther, Yong-Chang Zhang, Gerhard Zürn, Thomas Pohl, Matthias Weidemüller

Abstract: We predict a resonant enhancement of the nonlinear optical response of an interacting Rydberg gas under conditions of electromagnetically induced transparency. The enhancement originates from a two-photon process which resonantly couples electronic states of a pair of atoms dressed by a strong control field. We calculate the optical response for the three-level system by explicitly including the d… ▽ More We predict a resonant enhancement of the nonlinear optical response of an interacting Rydberg gas under conditions of electromagnetically induced transparency. The enhancement originates from a two-photon process which resonantly couples electronic states of a pair of atoms dressed by a strong control field. We calculate the optical response for the three-level system by explicitly including the dynamics of the intermediate state. We find an analytical expression for the third order susceptibility for a weak classical probe field. The nonlinear absorption displays the strongest resonant behavior on two-photon resonance where the detuning of the probe field equals the Rabi frequency of the control field. The nonlinear dispersion of the medium exhibits various spatial shapes depending on the interaction strength. Based on the developed model, we propose a realistic experimental scenario to observe the resonance by performing transmission measurements. △ Less

Submitted 15 September, 2019; originally announced September 2019.

Comments: 8 pages, 5 figures

Journal ref: Phys. Rev. A 100, 063812 (2019)

Quantum gas microscopy of Rydberg macrodimers

Authors: Simon Hollerith, Johannes Zeiher, Jun Rui, Antonio Rubio-Abadal, Valentin Walther, Thomas Pohl, Dan M. Stamper-Kurn, Immanuel Bloch, Christian Gross

Abstract: A microscopic understanding of molecules is essential for many fields of natural sciences but their tiny size hinders direct optical access to their constituents. Rydberg macrodimers - bound states of two highly-excited Rydberg atoms - feature bond lengths easily exceeding optical wavelengths. Here we report on the direct microscopic observation and detailed characterization of such macrodimers in… ▽ More A microscopic understanding of molecules is essential for many fields of natural sciences but their tiny size hinders direct optical access to their constituents. Rydberg macrodimers - bound states of two highly-excited Rydberg atoms - feature bond lengths easily exceeding optical wavelengths. Here we report on the direct microscopic observation and detailed characterization of such macrodimers in a gas of ultracold atoms in an optical lattice. The size of about 0.7 micrometers, comparable to the size of small bacteria, matches the diagonal distance of the lattice. By exciting pairs in the initial two-dimensional atom array, we resolve more than 50 vibrational resonances. Using our spatially resolved detection, we observe the macrodimers by correlated atom loss and demonstrate control of the molecular alignment by the choice of the vibrational state. Our results allow for precision testing of Rydberg interaction potentials and establish quantum gas microscopy as a powerful new tool for quantum chemistry. △ Less

Submitted 17 May, 2019; v1 submitted 18 December, 2018; originally announced December 2018.

Comments: 13 pages, 9 figures

Interactions between Rydberg excitons in Cu$_2$O

Authors: Valentin Walther, Sjard Ole Krüger, Stefan Scheel, Thomas Pohl

Abstract: Highly-excited states of excitons in cuprous oxide have recently been observed at a record quantum number of up to $n=25$. Here, we evaluate the long-range interactions between pairs of Rydberg excitons in Cu$_2$O, which are due to direct Coulomb forces rather than short-range collisions typically considered for ground state excitons. A full numerical analysis is supplemented by the van der Waals… ▽ More Highly-excited states of excitons in cuprous oxide have recently been observed at a record quantum number of up to $n=25$. Here, we evaluate the long-range interactions between pairs of Rydberg excitons in Cu$_2$O, which are due to direct Coulomb forces rather than short-range collisions typically considered for ground state excitons. A full numerical analysis is supplemented by the van der Waals asymptotics at large exciton separations, including the angular dependence of the potential surfaces. △ Less

Submitted 16 July, 2018; originally announced July 2018.

Journal ref: Phys. Rev. B 98, 165201 (2018)

Giant optical nonlinearities from Rydberg-excitons in semiconductor microcavities

Authors: Valentin Walther, Robert Johne, Thomas Pohl

Abstract: The realization of exciton-polaritons -- hybrid excitations of semiconductor quantum well excitons and cavity photons -- has been of great technological and scientific significance. In particular, the short-range collisional interaction between excitons has enabled explorations into a wealth of nonequilibrium and hydrodynamical effects that arise in weakly nonlinear polariton condensates. Yet, the… ▽ More The realization of exciton-polaritons -- hybrid excitations of semiconductor quantum well excitons and cavity photons -- has been of great technological and scientific significance. In particular, the short-range collisional interaction between excitons has enabled explorations into a wealth of nonequilibrium and hydrodynamical effects that arise in weakly nonlinear polariton condensates. Yet, the ability to enhance optical nonlinearities would enable quantum photonics applications and open up a new realm of photonic many-body physics in a scalable and engineerable solid-state environment. Here we outline a route to such capabilities in cavity-coupled semiconductors by exploiting the giant interactions between excitons in Rydberg-states. We demonstrate that optical nonlinearities in such systems can be vastly enhanced by several orders of magnitude and induce nonlinear processes at the level of single photons. △ Less

Submitted 5 November, 2017; originally announced November 2017.

Comments: 17 pages, 5 figures

Journal ref: Nat. Comm. 9, 1309 (2018)

Maximum caliber is a general variational principle for nonequilibrium statistical mechanics

Authors: Michael J. Hazoglou, Valentin Walther, Purushottam D. Dixit, Ken A. Dill

Abstract: There has been interest in finding a general variational principle for non-equilibrium statistical mechanics. We give evidence that Maximum Caliber (Max Cal) is such a principle. Max Cal, a variant of Maximum Entropy, predicts dynamical distribution functions by maximizing a path entropy subject to dynamical constraints, such as average fluxes. We first show that Max Cal leads to standard near-equ… ▽ More There has been interest in finding a general variational principle for non-equilibrium statistical mechanics. We give evidence that Maximum Caliber (Max Cal) is such a principle. Max Cal, a variant of Maximum Entropy, predicts dynamical distribution functions by maximizing a path entropy subject to dynamical constraints, such as average fluxes. We first show that Max Cal leads to standard near-equilibrium results -including the Green-Kubo relations, Onsager's reciprocal relations of coupled flows, and Prigogine's principle of minimum entropy production -in a way that is particularly simple. More importantly, because Max Cal does not require any notion of 'local equilibrium', or any notion of entropy dissipation, or even any restriction to material physics, it is more general than many traditional approaches. We develop some generalizations of the Onsager and Prigogine results that apply arbitrarily far from equilibrium. Max Cal is not limited to materials and fluids; it also applies, for example, to flows and trafficking on networks more broadly. △ Less

Submitted 20 May, 2015; originally announced May 2015.

Attractor Metadynamics in Adapting Neural Networks

Authors: Claudius Gros, Mathias Linkerhand, Valentin Walther

Abstract: Slow adaption processes, like synaptic and intrinsic plasticity, abound in the brain and shape the landscape for the neural dynamics occurring on substantially faster timescales. At any given time the network is characterized by a set of internal parameters, which are adapting continuously, albeit slowly. This set of parameters defines the number and the location of the respective adiabatic attrac… ▽ More Slow adaption processes, like synaptic and intrinsic plasticity, abound in the brain and shape the landscape for the neural dynamics occurring on substantially faster timescales. At any given time the network is characterized by a set of internal parameters, which are adapting continuously, albeit slowly. This set of parameters defines the number and the location of the respective adiabatic attractors. The slow evolution of network parameters hence induces an evolving attractor landscape, a process which we term attractor metadynamics. We study the nature of the metadynamics of the attractor landscape for several continuous-time autonomous model networks. We find both first- and second-order changes in the location of adiabatic attractors and argue that the study of the continuously evolving attractor landscape constitutes a powerful tool for understanding the overall development of the neural dynamics. △ Less

Submitted 22 April, 2014; originally announced April 2014.

Journal ref: Artificial Neural Networks and Machine Learning-ICANN 2014 , S. Wermter et al. (Eds), pp. 65-72. Springer (2014)