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Long-lived polaritonic coherence and polaron decoupling effects in 2D electronic spectra

Molecular polaritons, formed by coupling molecular excitons with cavity photons, offer a promising platform for exploring quantum phenomena. A key challenge is understanding how these hybrid states maintain coherence in the presence of environmental vibrations. Here, we show theoretically that collective coupling of many molecular excitons in a cavity can protect polariton coherence from phonon-induced decoherence. Under realistic conditions, the coherence time can extend up to 200 fs at room temperature, compared with 15 fs for typical molecular systems. Simulations of two-dimensional electronic spectra reveal prolonged oscillations between upper and lower polariton states, and reduced vibrational coupling as indicated by changes in the nodal line slope of the lower polariton peak. These findings provide guidance for experimental efforts to realize long-lived polaritons, such as coupling CdSe nanoplatelets to optical cavities.

2D electronic spectroscopy

Polariton spectra under the collective coupling regime. II. 2D non-linear spectra

In our previous work [Mondal et al., J. Chem. Phys. 162, 014114 (2025)], we developed several efficient computational approaches to simulate exciton–polariton dynamics described by the Holstein–Tavis–Cummings (HTC) Hamiltonian under the collective coupling regime. Here, we incorporated these strategies into the previously developed Lindblad-partially linearized density matrix (⁠$\mathscr{L}$-PLDM) approach for simulating 2D electronic spectroscopy (2DES) of exciton–polariton under the collective coupling regime. In particular, we apply the efficient quantum dynamics propagation scheme developed in Paper I to both the forward and the backward propagations in the PLDM and develop an efficient importance sampling scheme and graphics processing unit vectorization scheme that allow us to reduce the computational costs from $\mathscr{O}$($\mathscr{K}$ 2 )$\mathscr{O}$(T 3 ) to $\mathscr{O}$($\mathscr{K}$)$\mathscr{O}$(T 0 ) for the 2DES simulation, where $\mathscr{K}$ is the number of states and T is the number of time steps of propagation. As a result, we further simulated the 2DES for an HTC Hamiltonian under the collective coupling regime and analyzed the signal from both rephasing and non-rephasing contributions of the ground state bleaching, excited state emission, and stimulated emission pathways.

2D non-linear spectra

Roadmap for Photonics with 2D Materials

Triggered by advances in atomic-layer exfoliation and growth techniques, along with the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or a few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals now constitute a broad research field expanding in multiple directions through the combination of layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary subset of those directions, where 2D materials contribute remarkable nonlinearities, long-lived and ultraconfined polaritons, strong excitons, topological and chiral effects, susceptibility to external stimuli, accessibility, robustness, and a completely new range of photonic materials based on layer stacking, gating, and the formation of moiré patterns. These properties are being leveraged to develop applications in electro-optical modulation, light emission and detection, imaging and metasurfaces, integrated optics, sensing, and quantum physics across a broad spectral range extending from the far-infrared to the ultraviolet, as well as enabling hybridization with spin and momentum textures of electronic band structures and magnetic degrees of freedom. The rapid expansion of photonics with 2D materials as a dynamic research arena is yielding breakthroughs, which this Roadmap summarizes while identifying challenges and opportunities for future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

2D materials

Engineering anisotropic electrodynamics at the graphene/CrSBr interface

Abstract Graphene is a privileged 2D platform for hosting confined light-matter excitations known as surface plasmon polaritons (SPPs), as it possesses low intrinsic losses and a high degree of optical confinement. However, the isotropic nature of graphene limits its ability to guide and focus SPPs, making it less suitable than anisotropic elliptical and hyperbolic materials for polaritonic lensing and canalization. Here, we present graphene/CrSBr as an engineered 2D interface that hosts highly anisotropic SPP propagation across mid-infrared and terahertz energies. Using scanning tunneling microscopy, scattering-type scanning near-field optical microscopy, and first-principles calculations, we demonstrate mutual doping in excess of 10 13 cm –2 holes/electrons between the interfacial layers of graphene/CrSBr. SPPs in graphene activated by charge transfer interact with charge-induced electronic anisotropy in the interfacial doped CrSBr, leading to preferential SPP propagation along the quasi-1D chains that compose each CrSBr layer. This multifaceted proximity effect both creates SPPs and endows them with anisotropic propagation lengths that differ by an order-of-magnitude between the in-plane crystallographic axes of CrSBr.

Science & Technology - Other Topics

Real-space simulations of the hyperbolic plasmon polaritons in 1T′ tungsten ditelluride

Recent discoveries of hyperbolic surface plasmon polaritons (SPPs) in 1T′ WTe 2 have garnered significant attention in 2D materials and nanophotonics. In this study, we employ finite-element simulations to investigate the real-space characteristics of hyperbolic SPPs in thin WTe 2 flakes. Our results show that the SPPs exhibit a pronounced sensitivity to excitation energy and sample thickness. By analyzing the plasmonic field patterns, we extract key plasmonic parameters including plasmon wavelengths, hyperbolic angles, and plasmonic figures of merit. In addition, we examine SPP modes in stacked WTe 2 flakes with varying twist angles, demonstrating that the plasmonic field patterns can be effectively tuned by adjusting the twist angle. Notably, as the twist angle increases, the SPPs undergo a topological transition from open hyperbolic modes to closed elliptic modes. This twist-engineering capability offers promising potential for the development of tunable plasmonic devices based on WTe 2 .

2D materials

Low‐Loss Far‐Infrared Surface Phonon Polaritons in Suspended SrTiO 3 Nanomembranes

Phonon polaritons (PhPs), excitations arising from the coupling of light with lattice vibrations, enable light confinement and local field enhancement, which is essential for various photonic and thermal applications. To date, PhPs with high confinement and low loss are mainly observed in the mid-infrared regime and mostly in manually exfoliated flakes of van der Waals (vdW) materials. In this work, the existence of low-loss, thickness-tunable phonon polaritons in the far-infrared regime within transferable freestanding SrTiO 3 membranes synthesized through a scalable approach, achieving high figures of merit is demonstrated, which are comparable to the previous record values from the vdW materials. Leveraging atomic precision in thickness control, large dimensions, and compatibility with mature oxide electronics, functional oxide membranes present a promising large-scale 2D platform alternative to vdW materials for on-chip polaritonic technologies in the infrared regime.

functional oxide membranes

Interfacial Strong Coupling and Negative Dispersion of Propagating Polaritons in Freestanding Oxide Membranes

Membranes of complex oxides like perovskite SrTiO3 extend the multi-functional promise of oxide electronics into the nanoscale regime of 2D materials. Here, it is demonstrated that freestanding oxide membranes supply a reconfigurable platform for nano-photonics based on propagating surface phonon polaritons. Infrared near-field imaging and spectroscopy enabled by a tunable ultrafast laser are applied to study pristine nano-thick SrTiO3 membranes prepared by hybrid molecular beam epitaxy. As predicted by coupled mode theory, it is found that strong coupling of interfacial polaritons realizes symmetric and antisymmetric hybridized modes with simultaneously tunable negative and positive group velocities. By resolving reflection of these propagating modes from membrane edges, defects, and substrate structures, their dispersion is quantified with position-resolved nano-spectroscopy. Remarkably, polariton negative dispersion is found to be both robust and tunable through choice of membrane dielectric environment and thickness, and proposes a novel design for in-plane Veselago lensing harnessing this control. This work lays the foundation for tunable transformation optics at the nanoscale using polaritons in a wide range of freestanding complex oxide membranes.

freestanding oxide membranes

Modulation of the Electronic and Vibrational Landscape in Lead Organic Chalcogenides

Metal organic chalcogenides (MOCs) are an emerging class of two-dimensional (2D) materials featuring tunable band gaps and strong light-matter interactions with great potential for optical and polaritonic applications. Lead organic chalcogenides (LOCs) stand out among MOCs for sustaining long-lived coherent optical phonons despite their distorted lattices. However, the strong electron–phonon coupling also leads to rapid charge carrier self-trapping, hindering carrier transport. Herein, we demonstrate that charge carrier self-trapping is suppressed in Se- and Te-based LOCs. Specifically, the expansive Se and Te orbitals give rise to more dispersive conduction bands and reduced electron effective masses, thereby mitigating carrier self-trapping. As a result of reduced carrier self-trapping, the Se- and Te-based LOCs exhibit enhanced band-to-band photoluminescence and improved charge transport performance. Furthermore, our results provide a synthetic route to Se- and Te-based LOC single crystals and demonstrate the potential of orbital engineering to tune their electronic and phononic properties.

Chalcogenides

Emergent ferromagnetism and unusual irreversible magnetoresistance in an intercalated van der Waals antiferromagnet

Orthorhombic air-stable two-dimensional (2D) antiferromagnet (AFM) CrSBr has attracted much research interest lately thanks to its rich magnetic behaviors together with its remarkable electronic, excitonic, and polaritonic properties. Here, we report a reliable electrochemical intercalation method by inserting large tetrabutylammonium (TBA + ) ions into CrSBr layers. Magnetically, such intercalation efficiently suppresses the interlayer AFM and induces a ferromagnetic (FM) order with a much-enhanced transition temperature up to 200 K, nearly 70 K higher than the AFM onset of 132 K in pristine CrSBr. Electronically, the TBA + intercalation not only increases the electric conductivity of CrSBr, which is further enhanced by magnetic fields, but also introduces a giant negative irreversible magnetoresistance. This work demonstrates the tunable magnetic and electronic properties of CrSBr as well as their interplay, paving the way for advanced spintronic and magnetic memory devices.

36 MATERIALS SCIENCE

Plasmons Enable Ultralow Threshold Solid-State Triplet Fusion Upconversion with a 2D Sensitizer

Solid-state triplet−triplet annihilation (TTA) upconversion has significant potential for application in light harvesting, optoelectronic devices, and bioimaging. However, the high optical powers required to achieve efficient upconversion have inhibited its adoption. In this work, we demonstrate plasmon-enhanced near-infrared (NIR)-to-blue TTA upconversion in a monolayer WSe2/organic heterojunction. Under far-field excitation, the device reaches a threshold of 19 mW/cm 2 and an external quantum efficiency (EQE) of 0.17% with an anti-Stokes shift of 1.1 eV. Plasmon excitation lowers the threshold to 0.9 mW/cm 2 and improves the EQE to 3.6%. We attribute the plasmon enhancement to surface plasmon polariton (SPP) near-field enhancement and dark-exciton absorption. Optimization of the WSe 2 transfer process is identified as a key factor for the device performance. This work demonstrates that plasmon excitation overcomes the low far-field absorption of 2D transition-metal dichalcogenide (TMD) sensitizers. Consequently, monolayer TMDs can achieve solid-state upconversion with a performance among the best reported.

2D materials

Magnetic field driven emergent phenomena: Insights from magneto-optics and nanoscopy

This review explores magnetic field-driven emergent phenomena across various material systems, emphasizing the pivotal roles of magneto-optical and nanoscopy techniques. We examine fundamental aspects of Landau electrodynamics in both 2D and 3D systems, including quantum Hall and topological magnetoelectric effects in graphene and topological insulators. Particularly attention is given to magnetic excitations and magnetopolaritons, such as surface magnon polaritons, magnetoplasmons, and magnetoexcitons in novel quantum materials, including quantum magnets and hybrid heterostructures. Advanced imaging techniques, such as scattering-type scanning near-field optical microscopy (SNOM) and microwave impedance microscopy, are showcased for their capability to resolve these phenomena with microscopic and nanoscopic resolution. These insights are complemented by discussions of advanced experimental approaches, including cryogenic environments, ultrafast pump-probe techniques, and the integration of magnetic fields into near-field optical methodologies. We further investigate the potential of these imaging techniques for unraveling complex magnetic orders, quantum phases, and correlated electronic behaviors. Finally, we offer perspectives on future research directions and highlight emerging opportunities in the evolving field of optical magneto-nanoscopy.

36 MATERIALS SCIENCE

Low-Loss Charge Transfer Plasmons in Graphene/α-RuCl 3 Heterostructures Below 40 K

Charge transfer at material interfaces governs a wide range of physical properties, from electronic band structures to emergent collective excitations. In two-dimensional (2D) material heterostructures, charge transfer phenomena play important roles in enabling novel quantum phases, proximity effects, and tunable plasmonic responses. One representative charge transfer interface is formed between α-RuCl 3 , a van der Waals material with high electron affinity, and graphene. Significant charge transfer across this interface induces the formation of charge-transfer plasmon polaritons (CPPs), hybrid excitations between light and charge oscillations. However, previous studies found that as the charge transfer process takes place, α-RuCl 3 becomes lossy, which limits the quality factor of CPPs. Here, we investigate CPPs down to 10 K using a home-built scattering-type scanning near-field optical microscope (s-SNOM) optimized for low-temperature measurements. Our study reveals a dramatic suppression of plasmon loss channels below 40 K, contributing to a significant enhancement in the plasmonic quality factor. This reduction in loss is likely attributed to the blue shift of the correlation-induced Mott gap in α-RuCl 3 with decreasing temperature, along with the reduction of phonon scattering at low temperature. In conclusion, our results highlight the potential of using s-SNOM and CPPs to study complex 2D interfaces and reveal correlated electron dynamics in the underlying material.

36 MATERIALS SCIENCE

Sub-wavelength optical lattice in 2D materials

Recently, light-matter interaction has been vastly expanded as a control tool for inducing and enhancing many emergent nonequilibrium phenomena. However, conventional schemes for exploring such light-induced phenomena rely on uniform and diffraction-limited free-space optics, which limits the spatial resolution and the efficiency of light-matter interaction. Here, we overcome these challenges using metasurface plasmon polaritons (MPPs) to form a sub-wavelength optical lattice. Specifically, we report a “nonlocal” pump-probe scheme where MPPs are excited to induce a spatially modulated AC Stark shift for excitons in a monolayer of MoSe 2 , several microns away from the illumination spot. We identify nearly two orders of magnitude reduction for the required modulation power compared to the free-space optical illumination counterpart. Moreover, we demonstrate a broadening of the excitons’ linewidth as a robust signature of MPP-induced periodic sub-diffraction modulation. Our results will allow exploring power-efficient light-induced lattice phenomena below the diffraction limit in active chip-compatible MPP architectures.

36 MATERIALS SCIENCE

Applications of ultrafast nano-spectroscopy and nano-imaging with tip-based microscopy

Innovation in microscopy has often been critical in advancing both fundamental science and technological progress. Notably, the evolution of ultrafast near-field optical nano-spectroscopy and nano-imaging has unlocked the ability to image at spatial scales from nanometers to ångströms and temporal scales from nanoseconds to femtoseconds. This approach revealed a plethora of fascinating light-matter states and quantum phenomena, including various species of polaritons, quantum phases, and complex many-body effects. This review focuses on the working principles and state-of-the-art development of ultrafast tip-enhanced and near-field microscopy, integrating diverse optical pump-probe methods across the terahertz (THz) to ultraviolet (UV) spectral ranges. It highlights their utility in examining a broad range of materials, including two-dimensional (2D), organic molecular, and hybrid materials. The review concludes with a spatio-spectral-temporal comparison of ultrafast nano-imaging techniques, both within already well-defined domains, and offering an outlook on future developments of ultrafast tip-based microscopy and their potential to address a wider range of materials.

Zhao, Zhichen [Tongji University, Shanghai (China)

Observation of the axion quasiparticle in 2D MnBi 2 Te 4

The axion is a hypothetical fundamental particle that is conjectured to correspond to the coherent oscillation of the θ field in quantum chromodynamics. Its existence would solve multiple fundamental questions, including the strong CP problem of quantum chromodynamics and dark matter, but the axion has never been detected. Electrodynamics of condensed-matter systems can also give rise to a similar θ, so far studied as a static, quantized value to characterize the topology of materials. Coherent oscillation of θ in condensed matter has been proposed to lead to physics directly analogous to the high-energy axion particle—the dynamical axion quasiparticle (DAQ). Here we report the observation of the DAQ in MnBi 2 Te 4 . By combining a two-dimensional electronic device with ultrafast pump–probe optics, we observe a coherent oscillation of θ at about 44 gigahertz, which is uniquely induced by its out-of-phase antiferromagnetic magnon. This represents direct evidence for the presence of the DAQ, which in two-dimensional MnBi 2 Te 4 is found to arise from the magnon-induced coherent modulation of the Berry curvature. The DAQ also has implications in light–matter interaction and coherent antiferromagnetic spintronics, as it might lead to axion polaritons and electric control of ultrafast spin polarization. Finally, the DAQ could be used to detect axion particles. We estimate the detection frequency range and sensitivity in the millielectronvolt regime, which has so far been poorly explored.

topological matter