arXiv subjects

Félix Thouin

Publications and source records attributed to Félix Thouin.

12 recordsLinked to original sources

arXiv2025

Field-enhancement and nonlocal effects in epsilon-near-zero photonic gap antennas

In recent years, the large electric field enhancement and tight spatial confinement supported by the so-called epsilon near-zero (ENZ) mode has attracted significant attention for the realization of efficient nonlinear optical devices. Here, we experimentally demonstrate ENZ photonic gap antennas (PGAs), which consist of a dielectric pillar within which a thin slab of indium tin oxide (ITO) material is embedded. In ENZ PGAs, hybrid dielectric-ENZ modes emerge from strong coupling between the dielectric antenna modes and the ENZ bulk plasmon resonance. These hybrid modes efficiently couple to free space and allow for large enhancements of the incident electric field over nearly an octave bandwidth, without the stringent lateral nanofabrication requirements of conventional plasmonic or dielectric nanoantennas. To understand the modal features, we probe the linear response of single ENZ PGAs with dark field scattering and interpret the results in terms of a simple coupled oscillator framework. Third harmonic generation (THG) is used to probe the ITO local fields and large enhancements are observed in the THG efficiency over a broad spectral range. Surprisingly, sharp peaks emerge on top of the nonlinear response, which were not predicted by full wave calculations. These peaks are attributed to the ENZ material's nonlocal response, which once included using a hydrodynamic model for the ITO permittivity improves the agreement of our calculations for both the linear and nonlinear response. This proof of concept demonstrates the potential of ENZ PGAs, which we have previously shown can support electric field enhancements of up to 100--200X, and the importance of including nonlocal effects when describing the response of thin ENZ layers. Importantly, inclusion of the ITO nonlocality leads to increases in the predicted field enhancement, as compared to the local calculation.

physics.optics↗

arXiv2024

Quantum dynamics of photophysical aggregates in conjugated polymers

Photophysical aggregates are ubiquitous in many solid-state microstructures adopted by conjugated polymers, in which $π$ electrons interact with those in other polymer chains or those in other chromophores along the chain. These interactions fundamentally define the electronic and optical properties of the polymer film. While valuable insight can be gained from linear excitation and photoluminescence spectra, nonlinear coherent excitation spectral lineshapes provide intricate understanding on the electronic couplings that define the aggregate and their fluctuations. Here, we discuss the coherent two-dimensional excitation lineshape of a model hairy-rod conjugated polymer. At zero population waiting time, we find a $π/2$ phase shift between the 0-0 and 0-1 vibronic peaks in the real and imaginary components of the complex coherent spectrum, as well as a dynamic phase rotation with population waiting time over timescales that are longer than the optical dephasing time. We conjecture that these are markers of relaxation of the photophysical aggregate down the tight manifold of the exciton band. These results highlight the potential for coherent spectroscopy via analysis of the complex spectral lineshape to become a key tool to develop structure-property relationships in complex functional materials.

cond-mat.soft↗

arXiv2022

Broadband field-enhancement in epsilon-near-zero photonic gap antennas

In recent years, the large electric field enhancement and tight spatial confinement supported by the so-called epsilon-near-zero (ENZ) mode have attracted significant attention for the realization of efficient nonlinear optical devices. Here, we experimentally demonstrate a new type of antenna, termed an ENZ photonic gap antenna (PGA), which consists of a dielectric pillar within which a thin slab of indium tin oxide (ITO) material is embedded. In ENZ PGAs, hybrid dielectric-ENZ modes emerge from strong coupling between the dielectric antenna modes and the ENZ bulk plasmon resonance. These hybrid modes efficiently couple to free space and allow for large enhancements of the incident electric field over nearly an octave bandwidth, without the stringent lateral nanofabrication requirements required by conventional plasmonic or dielectric nanoantennas. The linear response of single ENZ PGAs is probed using dark field scattering and interpreted using a simple coupled oscillator framework. Third harmonic generation is used to probe the field enhancement and large enhancements are observed in the THG efficiency over a broad spectral range. This proof of concept demonstrates the potential of ENZ PGAs, which we have previously shown can support electric field enhancements of up to 100--200X, which is comparable with those of the best plasmonic antennas.

physics.optics↗

arXiv2022

Highly nonlinear dipolar exciton-polaritons in bilayer MoS$_2$

Realizing nonlinear optical response in the low photon density limit in solid-state systems has been a long-standing challenge. Semiconductor microcavities in the strong coupling regime hosting exciton-polaritons have emerged as attractive candidates in this context. However, the weak interaction between these quasiparticles has been a hurdle in this quest. Dipolar excitons provide an attractive strategy to overcome this limitation but are often hindered by their weak oscillator strength. The interlayer dipolar excitons in naturally occurring homobilayer MoS$_2$ alleviates this issue owing to their hybridization of interlayer charge transfer exciton and intralayer B exciton. Here we demonstrate the formation of dipolar exciton polaritons in bilayer MoS$_2$ resulting in unprecedented nonlinear interaction strengths. A ten-fold increase in nonlinearity is observed for the interlayer dipolar excitons compared to the conventional A excitons. These highly nonlinear dipolar polaritons will likely be a frontrunner in the quest for solid-state quantum nonlinear devices.

cond-mat.mes-hall↗

arXiv2020

Stochastic scattering theory for excitation induced dephasing: Time-dependent nonlinear coherent exciton lineshapes

We develop a stochastic theory that treats time-dependent exciton-exciton s-wave scattering and that accounts for dynamic Coulomb screening, which we describe within a mean-field limit. With this theory, we model excitation-induced dephasing effects on time-resolved two-dimensional coherent optical lineshapes and we identify a number of features that can be attributed to the many-body dynamics occurring in the background of the exciton, including dynamic line narrowing, mixing of real and imaginary spectral components, and multi-quantum states. We test the model by means of multidimensional coherent spectroscopy on a two-dimensional metal-halide semiconductor that hosts tightly bound excitons and biexcitons that feature strong polaronic character. We find that the exciton nonlinear coherent lineshape reflects many-body correlations that give rise to excitation-induced dephasing. Furthermore, we observe that the exciton lineshape evolves with population time over time windows in which the population itself is static, in a manner that reveals the evolution of the multi-exciton many-body couplings. Specifically, the dephasing dynamics slow down with time, at a rate that is governed by the strength of exciton many-body interactions and on the dynamic Coulomb screening potential. The real part of the coherent optical lineshape displays strong dispersive character at zero time, which transforms to an absorptive lineshape on the dissipation timescale of excitation-induced dephasing effects, while the imaginary part displays converse behavior. Our microscopic theoretical approach is sufficiently flexible to allow for a wide exploration of how system-bath dynamics contribute to linear and non-linear time-resolved spectral behavior.

physics.chem-ph↗

arXiv2020

Exciton-polaron spectral structures in two dimensional hybrid lead-halide perovskites

Owing to both electronic and dielectric confinement effects, two-dimensional organic-inorganic hybrid perovskites sustain strongly bound excitons at room temperature. Here, we demonstrate that there are non-negligible contributions to the excitonic correlations that are specific to the lattice structure and its polar fluctuations, both of which are controlled via the chemical nature of the organic counter-cation. We present a phenomenological, yet quantitative framework to simulate excitonic absorption lineshapes in single-layer organic-inorganic hybrid perovskites, based on the two-dimensional Wannier formalism. We include four distinct excitonic states separated by $35\pm5$\,meV, and additional vibronic progressions. Intriguingly, the associated Huang-Rhys factors and the relevant phonon energies show substantial variation with temperature and the nature of the organic cation. This points to the hybrid nature of the lineshape, with a form well described by a Wannier formalism, but with signatures of strong coupling to localized vibrations, and polaronic effects perceived through excitonic correlations. Our work highlights the complexity of excitonic properties in this class of nanostructured materials.

cond-mat.mtrl-sci↗

arXiv2019

Electron-phonon couplings inherent in polarons drive exciton dynamics in two-dimensional metal-halide perovskites

We report on the exciton formation and relaxation dynamics following photocarrier injection in a single-layer two-dimensional lead-iodide perovskite. We probe the time evolution of four distinct exciton resonances by means of time-resolved photoluminescence and transient absorption spectroscopies, and find that at 5\,K a subset of excitons form on a $\lesssim$ 1-ps timescale, and that these relax subsequently to lower-energy excitons on $\sim$ 5--10\,ps with a marked temperature dependence over $<$ 100\,K. We implement a mode projection analysis that determines the relative contribution of all observed phonons with frequency $\leq$50\,cm$^{-1}$ to inter-exciton nonadiabatic coupling, which in turn determines the rate of exciton relaxation. This analysis ranks the relative contribution of the phonons that participate in polaronic lattice distortions to the exciton inter-conversion dynamics and thus establishes their role in the nonadiabatic mixing of exciton states, and this in the exciton relaxation rate.

cond-mat.mtrl-sci↗

arXiv2019

Phonon coherences reveal the polaronic character of excitons in two-dimensional lead-halide perovskites

Hybrid organic-inorganic semiconductors feature complex lattice dynamics due to the ionic character of the crystal and the softness arising from non-covalent bonds between molecular moieties and the inorganic network. Here we establish that such dynamic structural complexity in a prototypical two-dimensional lead iodide perovskite gives rise to the coexistence of diverse excitonic resonances, each with a distinct degree of polaronic character. By means of high-resolution resonant impulsive stimulated Raman spectroscopy, we identify vibrational wavepacket dynamics that evolve along different configurational coordinates for distinct excitons and photocarriers. Employing density functional theory calculations, we assign the observed coherent vibrational modes to various low-frequency ($\lesssim 50$\,cm$^{-1}$) optical phonons involving motion in the lead-iodide layers. We thus conclude that different excitons induce specific lattice reorganizations, which are signatures of polaronic binding. This insight on the energetic/configurational landscape involving globally neutral primary photoexcitations may be relevant to a broader class of emerging hybrid semiconductor materials.

cond-mat.mtrl-sci↗

arXiv2019

Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites

In two-dimensional hybrid organic-inorganic metal-halide perovskites, the intrinsic optical lineshape reflects multiple excitons with distinct binding energies, each dressed differently by the hybrid lattice. Given this complexity, a fundamentally far-reaching issue is how Coulomb-mediated many-body interactions --- elastic scattering such as excitation-induced dephasing, inelastic exciton bimolecular scattering, and multi-exciton binding --- depend upon the specific exciton-lattice coupling. We report the intrinsic and density-dependent exciton pure dephasing rates and their dependence on temperature by means of a coherent nonlinear spectroscopy. We find exceptionally strong screening effects on multi-exciton scattering relative to other two-dimensional single-atomic-layer semiconductors. Importantly, the exciton-density dependence of the dephasing rates is markedly different for distinct excitons. These findings establish the consequences of particular lattice dressing on exciton many-body quantum dynamics, which critically define fundamental optical properties that underpin photonics and quantum optoelectronics in relevant exciton density regimes.

cond-mat.mtrl-sci↗

arXiv2018

End-to-end Deep Learning of Optical Fiber Communications

In this paper, we implement an optical fiber communication system as an end-to-end deep neural network, including the complete chain of transmitter, channel model, and receiver. This approach enables the optimization of the transceiver in a single end-to-end process. We illustrate the benefits of this method by applying it to intensity modulation/direct detection (IM/DD) systems and show that we can achieve bit error rates below the 6.7\% hard-decision forward error correction (HD-FEC) threshold. We model all componentry of the transmitter and receiver, as well as the fiber channel, and apply deep learning to find transmitter and receiver configurations minimizing the symbol error rate. We propose and verify in simulations a training method that yields robust and flexible transceivers that allow---without reconfiguration---reliable transmission over a large range of link dispersions. The results from end-to-end deep learning are successfully verified for the first time in an experiment. In particular, we achieve information rates of 42\,Gb/s below the HD-FEC threshold at distances beyond 40\,km. We find that our results outperform conventional IM/DD solutions based on 2 and 4 level pulse amplitude modulation (PAM2/PAM4) with feedforward equalization (FFE) at the receiver. Our study is the first step towards end-to-end deep learning-based optimization of optical fiber communication systems.

cs.IT↗

arXiv2018

Stable biexcitons in two-dimensional metal-halide perovskites with strong dynamic lattice disorder

With strongly bound and stable excitons at room temperature, single-layer, two-dimensional organic-inorganic hybrid perovskites are viable semiconductors for light-emitting quantum optoelectronics applications. In such a technological context, it is imperative to comprehensively explore all the factors --- chemical, electronic and structural --- that govern strong multi-exciton correlations. Here, by means of two-dimensional coherent spectroscopy, we examine excitonic many-body effects in pure, single-layer (PEA)$_2$PbI$_4$ (PEA = phenylethylammonium). We determine the binding energy of biexcitons --- correlated two-electron, two-hole quasiparticles --- to be $44 \pm 5$\,meV at room temperature. The extraordinarily high values are similar to those reported in other strongly excitonic two-dimensional materials such as transition-metal dichalchogenides. Importantly, we show that this binding energy increases by $\sim25$\% upon cooling to 5\,K. Our work highlights the importance of multi-exciton correlations in this class of technologically promising, solution-processable materials, in spite of the strong effects of lattice fluctuations and dynamic disorder.

cond-mat.mtrl-sci↗

arXiv2014

A Ballistic Monte Carlo Approximation of π

We compute a Monte Carlo approximation of π using importance sampling with shots coming out of a Mossberg 500 pump-action shotgun as the proposal distribution. An approximated value of 3.131 is obtained, corresponding to a 0.33% error on the exact value of π. To our knowledge, this represents the first attempt at estimating π using such method, thus opening up new perspectives towards computing mathematical constants using everyday tools.

physics.pop-ph↗