arXiv subjects

Milan Delor

Publications and source records attributed to Milan Delor.

At least 19 recordsLinked to original sources

arXiv2026

Molecular spin qubits in a van der Waals bottle

Advancing quantum information technologies requires qubits whose coherence can be precisely engineered. Among the qubit platforms in development, molecular spin qubits (MSQs) stand out for their atomic scale tunability and chemical specificity, making them powerful candidates for sensing, simulation, and information processing. However, integrating MSQs into solid-state architectures without degrading their coherence remains a central challenge. Here, we introduce van der Waals (vdW) confinement within two-dimensional materials as a strategy for stabilizing quantum states in MSQs by engineering their local electronic, vibrational, and symmetry environments. Using cobaltocene as a model system, we show that confinement within vdW SnS2 and CdPS3 single crystals reorganizes the single-ion energy landscape and slows spin-lattice relaxation by over two orders of magnitude relative to unconfined cobaltocene. The confined MSQs adopt deterministic orientations and self-assemble into ordered, atomically precise superlattices, establishing vdW confinement as a pathway for integrating MSQs into functional quantum devices.

cond-mat.mtrl-sci↗

arXiv2026

Giant optical spin-orbit interactions in ferroelectric van der Waals waveguides

Optical spin-orbit interactions (SOI) link photonic spin to momentum, offering a route toward on-chip polarization control and beam steering. Nevertheless, achieving sufficient optical SOI and nonlinearities on sub-micrometer scales - a prerequisite for dense photonic integration - remains an outstanding challenge. Here, we show that highly birefringent van der Waals (vdW) waveguides provide an ideal, chip-compatible platform to address this limitation. We focus on the ferroelectric semiconductor NbOI2, which exhibits record optical nonlinearities and dielectric anisotropy. Using femtosecond optical microscopy, we image light propagation and harmonic conversion beyond the total internal reflection barrier over tens of micrometers in NbOI2 slab waveguides. We report giant optical spin-splitting through the optical spin Hall effect, which facilitates spatial separation of optical spin currents on sub-micrometer scales, in quantitative agreement with a microscopic light-matter interaction model. We further leverage optical spin-momentum locking to realize polarization-controlled waveguide steering. We generalize these observations across various vdW waveguides and empirically confirm a scaling law linking dielectric anisotropy to geometric spin-splitting. Our results establish highly anisotropic vdW waveguides as an ideal platform for densely integrated opto-spintronic technologies.

cond-mat.mtrl-sci↗

arXiv2026

On-demand steering of hyperbolic chiral polaritons

Control of light polarization and propagation in sub-wavelength architectures is foundational to nanophotonic technologies. A frontier direction is to leverage strong optical spin-orbit interactions to realize polarization-selective light steering, known as the photonic spin Hall effect. In this context, hyperbolic plasmon polaritons (HPPs) are of particular interest as they offer large optical spin-orbit coupling from strong confinement and dielectric anisotropy, as well as ray-like propagation. Despite theoretical predictions, however, the hyperbolic spin Hall effect in natural materials has remained elusive. Here, we demonstrate the hyperbolic spin Hall effect in the visible and near-infrared range in the natural hyperbolic van der Waals metal MoOCl2. Enabling this discovery is a novel far-field pump-probe microscope that facilitates the launching and imaging of HPPs with exceptional sensitivity through interference with a high-momentum reference field. This approach preserves excellent control over light polarization, overcoming a key barrier to polarization-selective interrogation of hyperbolic materials. We show that both hyperbolic and surface plasmons in MoOCl2 display chiral fields, and that their propagation direction can be completely switched upon light helicity reversal. Our results demonstrate on-demand steering of chiral plasmons, firmly establishing natural hyperbolic materials as ideal components for reconfigurable nanophotonics and chiral light-matter coupling.

cond-mat.mtrl-sci↗

arXiv2026

Plasmon dynamics in graphene

Plasmon are collective oscillations of mobile electrons with dynamics controlled by their charge stiffness("Drude weight"). Using terahertz spacetime metrology, we probe Plasmon dynamics of mono- and bi-layer graphene. In both systems, the experimentally measured Drude weight systematically exceeds the prediction based on non-interacting electronic system. The relative enhancement increases as the carrier density decreases. We attribute the observed deviation to the interplay of interactions and wave function structure of the Dirac fermions in multi-layer graphene. Our results establish that pseudospin structure of the single-particle electronic wave function can directly influence collective excitations, with implications that extend beyond graphene to a broad class of quantum materials.

cond-mat.mes-hall↗

arXiv2025

Flat band excitons in a three-dimensional supertwisted spiral transition metal dichalcogenide

A new frontier in van der Waals twistronics is the development of three-dimensional (3D) supertwisted materials, where each successive atomic layer rotates by the same angle. While two-dimensional (2D) moire systems have been extensively studied, the unique phenomena arising from 3D twistronics remain largely unexplored. In this work, we report the discovery of flat-band excitons in 3D supertwisted WS2, revealed by systematic photoluminescence (PL) experiments and electronic structure calculations. These excitons retain key features of 2D moire transition metal dichalcogenides (TMDs)-such as layer confinement, moire-driven localization, and strong Coulomb interactions-while also offering advantages in scalability and enhanced optical responses in three dimensions. Beyond the PL signatures reminiscent of 2D A excitons, we observe novel direct and indirect exciton emission uniquely tied to the supertwist geometry. Using generalized Bloch band theory and local density of states calculations that incorporate screw rotational symmetry, we uncovered the coexistence of 2D and 3D flatband gaps. These flat-band excitons serve as sensitive probes of the electronic properties of 3D supertwisted semiconductors and open new pathways for applications in quantum optoelectronics.

physics.app-ph↗

arXiv2025

Van der Waals waveguide quantum electrodynamics probed by infrared nano-photoluminescence

Atomically layered van der Waals (vdW) materials exhibit remarkable properties, including highly-confined infrared waveguide modes and the capacity for infrared emission in the monolayer limit. Here, we engineered structures that leverage both of these nano-optical functionalities. Specifically, we encased a photoluminescing atomic sheet of MoTe2 within two bulk crystals of WSe2, forming a vdW waveguide for the embedded light-emitting monolayer. The modified electromagnetic environment offered by the WSe2 waveguide alters MoTe2 spontaneous emission, a phenomenon we directly image with our interferometric nano-photoluminescence technique. We captured spatially-oscillating nanoscale patterns prompted by spontaneous emission from MoTe2 into waveguide modes of WSe2 slabs. We quantify the resulting Purcell-enhanced emission rate within the framework of a waveguide quantum electrodynamics (QED) model, relating the MoTe2 spontaneous emission rate to the measured waveguide dispersion. Our work marks a significant advance in the implementation of all-vdW QED waveguides.

physics.optics↗

arXiv2025

Exciton Delocalization Suppresses Polariton Scattering

Exciton-polaritons (EPs) are part-light part-matter quasiparticles that combine large exciton-mediated nonlinearities with long-range coherence, ideal for energy harvesting and nonlinear optics. Optimizing EPs for these applications is predicated on a still-elusive understanding of how disorder affects their propagation and dephasing times. Here, using cutting-edge femtosecond spatiotemporal microscopy, we directly image EP propagation at light-like speeds in systems ranging from two-dimensional semiconductors to amorphous molecular films with systematically varied exciton-phonon coupling, exciton delocalization, and static disorder. Despite possessing similar EP dispersions, we observe dramatically different transport velocities and scattering times across systems. We establish a robust scaling law linking EP scattering to exciton transfer integral, demonstrating that polaritons based on materials with large exciton bandwidths are immune to disorder even for highly excitonic EPs. This observation cannot be deduced from the systems' linear optical properties, including EP dispersion and linewidth disorder. Our work highlights the critical and often-overlooked role of the matter component in dictating polariton properties, and provides precise guidelines for simultaneously optimizing EP propagation and nonlinearities.

physics.optics↗

arXiv2025

Observation of Coherent Ferron Emission and Propagation

Excitation of ordered quantum phases gives rise to collective modes and quasiparticles, as exemplified by spin waves and magnons emerging from magnetic order. Extending this paradigm to ferroelectric materials suggests the existence of polarization waves and their fundamental quanta, ferrons. Here, we report the generation and transport of polarization waves, i.e., coherent ferrons, in the van der Waals ferroelectric material NbOI2. Upon excitation by a short laser pulse, the polarization wave emits intense and narrow-band terahertz (THz) radiation at the ferroelectric transverse optical phonon frequency, modulates the ferroelectric order parameter, and propagates uniaxially along the polar axis at hypersonic velocities of ~105 m/s. These long-lived, uniaxial, and dipole-carrying polarization waves may find applications in narrow-band THz emission, ferronic information processing, and coherent electric control.

cond-mat.mtrl-sci↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2024

Spatiotemporal imaging of nonlinear optics in van der Waals waveguides

Van der Waals (vdW) semiconductors have emerged as promising platforms for efficient nonlinear optical conversion, including harmonic and entangled photon generation. Although major efforts are devoted to integrating vdW materials in nanoscale waveguides for miniaturization, the realization of efficient, phase-matched conversion in these platforms remains challenging. To address this challenge, we develop a far-field ultrafast imaging method to track the propagation of both fundamental and harmonic waves within vdW waveguides with extreme spatiotemporal resolution. Our approach allows systematic optimization of nonlinear conversion by determining the phase-matching angles, mode profiles, and losses in waveguides without a priori knowledge of material properties. We focus on light propagation in slab waveguides of rhombohedral-stacked MoS2, an emerging vdW semiconductor with giant nonlinear susceptibility. Our results reveal that these waveguides support birefringent phase-matching, demonstrating the material's potential for efficient on-chip nonlinear optics. This work establishes spatiotemporal imaging of light propagation in waveguides as an incisive and general method to identify new materials and architectures for efficient nonlinear nanophotonics.

cond-mat.mtrl-sci↗

arXiv2024

Microscopic Theory of Polariton Group Velocity Renormalization

Cavity exciton-polaritons exhibit ballistic transport and can achieve a distance of 100 $\mu $m in one picosecond. This ballistic transport significantly enhances mobility compared to that of bare excitons, which often move diffusively and become the bottleneck for energy conversion and transfer devices. Despite being robustly reproduced in experiments and simulations, there is no comprehensive microscopic theory addressing the group velocity of polariton transport, and its renormalization due to phonon scattering while still preserving this ballistic behavior. In this work, we develop a microscopic theory to describe the group velocity renormalization using a finite-temperature Green's function approach. Utilizing the generalized Holstein-Tavis-Cummings Hamiltonian, we analytically derive an expression for the group velocity renormalization and find that it is caused by phonon-mediated transitions from the lower polariton (LP) states to the dark states, then scattering from dark states back to LP. The dark states do not have to be populated in this process, serving as the virtual state for super-exchange (especially true for a large light-matter detuning). The theory predicts that the magnitude of group velocity renormalization scales linearly with the phonon bath reorganization energy under weak coupling conditions (perturbative regime for exciton-phonon coupling) and also linearly depends on the temperature in the high-temperature regime. These predictions are numerically verified using quantum dynamics simulations, demonstrating quantitative agreement. Our findings provide theoretical insights and a predictive analytical framework that advance the understanding and design of cavity-modified semiconductors and molecular ensembles, opening new avenues for engineered polaritonic devices.

quant-ph↗

arXiv2024

Frustrated hopping from orbital decoration of a primitive two-dimensional lattice

Materials hosting flat electronic bands are a central focus of condensed matter physics as promising venues for novel electronic ground states. Two-dimensional (2D) geometrically frustrated lattices such as the kagome, dice, and Lieb lattices are attractive targets in this direction, anticipated to realize perfectly flat bands. Synthesizing these special structures, however, poses a formidable challenge, exemplified by the absence of solid-state materials realizing the dice and Lieb lattices. An alternative route leverages atomic orbitals to create the characteristic electron hopping of geometrically frustrated lattices. This strategy promises to expand the list of candidate materials to simpler structures, but is yet to be demonstrated experimentally. Here, we report the realization of frustrated hopping in the van der Waals (vdW) intermetallic Pd$_5$AlI$_2$, emerging from orbital decoration of a primitive square lattice. Using angle-resolved photoemission spectroscopy and quantum oscillations measurements, we demonstrate that the band structure of Pd$_5$AlI$_2$ includes linear Dirac-like bands intersected at their crossing point by a flat band, essential characteristics of frustrated hopping in the Lieb and dice lattices. Moreover, Pd$_5$AlI$_2$ is exceptionally stable, with the unusual bulk band structure and metallicity persisting in ambient conditions down to the monolayer limit. Our ability to realize an electronic structure characteristic of geometrically frustrated lattices establishes orbital decoration of primitive lattices as a new approach towards electronic structures that remain elusive to prevailing lattice-centric searches.

cond-mat.str-el↗

arXiv2023

Quasi-phase-matched up- and down-conversion in periodically poled layered semiconductors

Nonlinear optics lies at the heart of classical and quantum light generation. The invention of periodic poling revolutionized nonlinear optics and its commercial applications by enabling robust quasi-phase-matching in crystals such as lithium niobate. However, reaching useful frequency conversion efficiencies requires macroscopic dimensions, limiting further technology development and integration. Here we realize a periodically poled van der Waals semiconductor (3R-MoS$_2$). Due to its exceptional nonlinearity, we achieve macroscopic frequency conversion efficiency of 0.03% at the relevant telecom wavelength over a microscopic thickness of 3.4${\mu}$m (that is, 3 poling periods), $10-100\times$ thinner than current systems with similar performances. Due to unique intrinsic cavity effects, the thickness-dependent quasi-phase-matched second harmonic signal surpasses the usual quadratic enhancement by $50\%$. Further, we report the broadband generation of photon pairs at telecom wavelengths via quasi-phase-matched spontaneous parametric down-conversion, showing a maximum coincidence-to-accidental-ratio of $638 \pm 75$. This work opens the new and unexplored field of phase-matched nonlinear optics with microscopic van der Waals crystals, unlocking applications that require simple, ultra-compact technologies such as on-chip entangled photon-pair sources for integrated quantum circuitry and sensing.

physics.optics↗

arXiv2023

Electronic interactions in Dirac fluids visualized by nano-terahertz spacetime interference of electron-photon quasiparticles

Ultraclean graphene at charge neutrality hosts a quantum critical Dirac fluid of interacting electrons and holes. Interactions profoundly affect the charge dynamics of graphene, which is encoded in the properties of its electron-photon collective modes: surface plasmon polaritons (SPPs). Here we show that polaritonic interference patterns are particularly well suited to unveil the interactions in Dirac fluids by tracking polaritonic interference in time at temporal scales commensurate with the electronic scattering. Spacetime SPP interference patterns recorded in tera-hertz (THz) frequency range provided unobstructed readouts of the group velocity and lifetime of polariton that can be directly mapped onto the electronic spectral weight and the relaxation rate. Our data uncovered prominent departures of the electron dynamics from the predictions of the conventional Fermi-liquid theory. The deviations are particularly strong when the densities of electrons and holes are approximately equal. The proposed spacetime imaging methodology can be broadly applied to probe the electrodynamics of quantum materials.

cond-mat.str-el↗

arXiv2023

Room temperature wavelike exciton transport in a van der Waals superatomic semiconductor

The transport of energy and information in semiconductors is limited by scattering between electronic carriers and lattice phonons, resulting in diffusive and lossy transport that curtails all semiconductor technologies. Using Re6Se8Cl2, a van der Waals (vdW) superatomic semiconductor, we demonstrate the formation of acoustic exciton-polarons, an electronic quasiparticle shielded from phonon scattering. We directly image polaron transport in Re6Se8Cl2 at room temperature and reveal quasi-ballistic, wavelike propagation sustained for nanoseconds and several microns. Shielded polaron transport leads to electronic energy propagation orders of magnitude greater than in other vdW semiconductors, exceeding even silicon over nanoseconds. We propose that, counterintuitively, quasi-flat electronic bands and strong exciton-acoustic phonon coupling are together responsible for the remarkable transport properties of Re6Se8Cl2, establishing a new path to ballistic room-temperature semiconductors.

cond-mat.mtrl-sci↗

arXiv2022

Ultrafast imaging of polariton propagation and interactions

Semiconductor excitations can hybridize with cavity photons to form exciton-polaritons (EPs) with remarkable properties, including light-like energy flow combined with matter-like interactions. To fully harness these properties, EPs must retain ballistic, coherent transport despite matter-mediated interactions with lattice phonons. Here we develop a nonlinear momentum-resolved optical approach that directly images EPs in real space on femtosecond scales in a range of polaritonic architectures. We focus our analysis on EP propagation in layered halide perovskite microcavities. We reveal that EP-phonon interactions lead to a large renormalization of EP velocities at high excitonic fractions at room temperature. Despite these strong EP-phonon interactions, ballistic transport is maintained for up to half-exciton EPs, in agreement with quantum simulations of dynamic disorder shielding through light-matter hybridization. Above 50% excitonic character, rapid decoherence leads to diffusive transport. Our work provides a general framework to precisely balance EP coherence, velocity, and nonlinear interactions.

cond-mat.mtrl-sci↗

arXiv2022

Exciton-Coupled Coherent Magnons in a 2D Semiconductor

Two-dimensional (2D) magnetic semiconductors feature both tightly-bound excitons with large oscillator strength and potentially long-lived coherent magnons due to the presence of bandgap and spatial confinement. While magnons and excitons are energetically mismatched by orders of magnitude, their coupling can lead to efficient optical access to spin information. Here we report strong magnon-exciton coupling in the 2D van der Waals (vdW) antiferromagnetic (AFM) semiconductor CrSBr. Coherent magnons launched by above-gap excitation modulate the interlayer hybridization, which leads to dynamic modulation of excitonic energies. Time-resolved exciton sensing reveals magnons that can coherently travel beyond 7 micrometer, with coherence time above 5 ns. We observe this exciton-coupled coherent magnons in both even and odd number of layers, with and without compensated magnetization, down to the bilayer limit. Given the versatility of vdW heterostructures, these coherent 2D magnons may be basis for optically accessible magnonics and quantum interconnects.

cond-mat.mes-hall↗

arXiv2022

Dark-exciton driven energy funneling into dielectric inhomogeneities in two-dimensional semiconductors

The optoelectronic and transport properties of two-dimensional transition metal dichalcogenide semiconductors (2D TMDs) are highly susceptible to external perturbation, enabling precise tailoring of material function through post-synthetic modifications. Here we show that nanoscale inhomogeneities known as nanobubbles can be used for both strain and, less invasively, dielectric tuning of exciton transport in bilayer tungsten disulfide (WSe2). We use ultrasensitive spatiotemporally resolved optical scattering microscopy to directly image exciton transport, revealing that dielectric nanobubbles are surprisingly efficient at funneling and trapping excitons at room temperature, even though the energies of the bright excitons are negligibly affected. Our observations suggest that exciton funneling in dielectric inhomogeneities is driven by momentum-indirect (dark) excitons whose energies are more sensitive to dielectric perturbations than bright excitons. These results reveal a new pathway to control exciton transport in 2D semiconductors with exceptional spatial and energetic precision using dielectric engineering of dark state energetic landscapes.

cond-mat.mes-hall↗