arXiv subjects

Stéphane Kéna-Cohen

Publications and source records attributed to Stéphane Kéna-Cohen.

At least 19 recordsLinked to original sources

arXiv2026

Mid-infrared distributed-feedback lasing from black phosphorus under nanosecond excitation

Mid-infrared (MIR) light sources compatible with silicon photonics are highly desirable for environmental sensing and free-space optical communications. Conventional GaSb-based quantum-well and interband-cascade lasers, however, rely on complex epitaxial heterostructures, complicating their integration with silicon photonic platforms. Here, we demonstrate a room-temperature MIR surface-emitting distributed-feedback (DFB) laser using black phosphorus (b-P) as the active gain medium. By deterministically integrating exfoliated b-P flakes onto lithographically patterned SiO$_2$ gratings, we obtain narrowband emission with a full width at half maximum below 3 nm under 1064 nm optical excitation. The lasing wavelength is tunable from 3.79 to 4.05$~μ\text{m}$ through the b-P flake thickness, covering a technologically important region of the mid-infrared. Room-temperature thresholds as low as $(0.25 \pm 0.07)\ \text{mJ/cm}^2$ are achieved under nanosecond excitation. Upon cooling to 110 K, the threshold decreases tenfold to $(0.015 \pm 0.005)\ \text{mJ/cm}^2$. These results establish planar b-P DFB cavities as a promising platform for heterogeneously integrated MIR lasers based on van der Waals semiconductors.

physics.app-ph↗

arXiv2026

Planar Microcavities can Suppress Exciplex Formation and Increase the Emission Efficiency of Organic Semiconductors

Optical microcavities are widely used to control the emission of organic semiconductors, but their ability to reshape the molecular pathways that precede emission remains largely unexplored. Here we show that embedding a ZnPc:TPBi blend in a planar Fabry-Pérot microcavity suppresses the formation of non-radiative exciplexes and removes bimolecular annihilation at high excitation densities, increasing the photoluminescence quantum yield by more than forty-fold under continuous-wave excitation. This enhancement is far larger than expected from the weak Purcell effect. Instead, transient spectroscopy, power-dependent photoluminescence and kinetic modelling point to a cavity-induced rebalancing of excited-state populations: long-range Förster energy transfer from ZnPc monomers to emissive aggregates is enhanced, allowing it to outcompete charge transfer to dark exciplexes. Electromagnetic calculations predict FRET enhancements of up to ~400-fold at relevant distances, consistent with the observed suppression of exciplex-mediated losses. Our results show that optical cavities can control not only how molecules emit, but also which excited states they form, opening a route to improved efficiency and reduced roll-off in organic optoelectronic and photonic devices.

cond-mat.mtrl-sci↗

arXiv2026

Revealing full molecular orientation distributions in organic thin films by nonlinear polarimetry

The performance of organic optoelectronic devices is critically dependent on how molecules orient within organic thin films. Yet, standard characterization techniques only reveal the first and second moments of the molecular orientation distribution. This limitation obscures the true molecular arrangement, as diverse distributions can yield identical low-order averages while exhibiting distinct functional properties. Here, we bridge this gap by combining multi-harmonic nonlinear polarimetry (second, third, and fourth harmonic) with the Maximum Entropy Method to reconstruct the probability distribution without any \textit{a priori} assumptions. This allows us to resolve features in the distribution such as asymmetry and bimodality, that remain invisible to conventional probes. Furthermore, we use this method to benchmark molecular dynamics simulations, revealing that these simulations often fail to capture the complex distribution despite correctly predicting the first and second moments. This work transforms molecular orientation from an inferred average into a precise observable, establishing essential validation standards for predictive material design.

physics.optics↗

arXiv2026

Why Are Verdazyl Radicals Non-Emissive? An Experimental and Computational Study

Verdazyl radicals are a versatile class of air-stable organic radicals used in various applications, especially for their magnetic properties. Despite the development of a wide range of verdazyl derivatives, however, they are all non-emissive. To investigate the reasons behind this and to understand the excited-state dynamics of verdazyls, we combine steady-state and femtosecond pump-probe spectroscopy with quantum chemical calculations. In the carbazole-substituted 2,4,6-triphenylverdazyl (TPV-Cz) , we observe ultrafast internal conversion of the first excited state on a timescale of 0.5 $\pm$ 0.1 ps, followed by vibrational relaxation with a lifetime of 3.7 $\pm$ 0.4 ps. Spin-flip time-dependent density functional theory calculations reveal that the sub-picosecond non-radiative decay comes from a low-energy conical intersection between the D1 and D0 states, driven by an out-of-plane distortion of the verdazyl ring. This distortion is observed and remains energetically accessible in the isolated verdazyl ring in 2,4,6-triphenylverdazyl and in TPV-Cz. This shows that the conical intersection geometry is a recurring feature across different types of verdazyl derivatives and explains why all verdazyls are non-emissive despite different functionalization. Our results provide a mechanistic understanding of the photophysical properties of verdazyl radicals and offers a pathway for the future design of emissive verdazyl derivatives.

physics.chem-ph↗

arXiv2025

Molecular Engineering for Enhanced Second-Order Nonlinear Response in Spontaneously-Oriented Evaporated Organic Films

Materials with large second-order nonlinearities are crucial for next-generation integrated photonics. Spontaneously oriented organic thin films prepared by physical vapor deposition offer a promising poling-free and scalable approach. This study investigates molecular engineering strategies to enhance the second-order nonlinear response of derivatives based on the donor-acceptor molecule 2-(4'-diphenylaminobiphenyl-4-yl)quinoxaline-6,7-dicarbonitrile (TPA-QCN). Four derivatives incorporating modifications designed to increase molecular hyperpolarizability ($β$) or promote favorable orientation were synthesized and characterized. The most successful modification, intramolecular bridge-locking, simultaneously increases hyperpolarizability and enhances spontaneous orientation by reducing detrimental electrostatic interactions during deposition. It leads to a significant enhancement of the second-order nonlinear response, achieving off-resonance $χ^{(2)}_{31} \approx 16$ pm V$^{-1}$ and $χ^{(2)}_{33} \approx 18$ pm V$^{-1}$ at 1550 nm, a twofold improvement over the parent TPA-QCN. Analysis combining nonlinear optical measurements, surface potential measurement, optical anisotropy, and density functional theory calculations indicates that improved molecular orientation, rather than increased $β$ alone, is the primary driver for the enhanced performance in the leading derivatives. These findings demonstrate the effectiveness of targeting molecular orientation via structural design and position spontaneously oriented organic films as compelling poling-free candidates for integrated nonlinear photonic applications where the increased electrode-induced optical losses, fabrication complexity and footprint are a critical limitation.

physics.optics↗

arXiv2025

Waveguide-Coupled Mid-Infrared GeSn Membrane Photodetectors on Silicon-on-Insulator

Silicon photonics has thrived in telecommunications over recent decades, and its extension to the mid-infrared range has the potential to unlock valuable opportunities for sensing, imaging, and free-space communications. With this perspective, germanium-tin (GeSn) alloy has been extensively investigated as a silicon-compatible semiconductor with bandgap tunability that covers this entire spectral range. Indeed, a variety of GeSn-based high-performance optoelectronic devices have been demonstrated, confirming the potential of this system for mid-infrared applications. However, the integration of these devices onto silicon photonic platforms remains underexplored. Herein, we demonstrate the fabrication and integration, through transfer-printing, of strain-relaxed GeSn membranes onto silicon-on-insulator waveguides to create integrated detectors operating up to 3.1 $μ$m at room temperature. Two different designs of waveguide structures are evaluated to study the coupling efficiency between the passive structures and the active membrane detector. A responsivity reaching 0.36 A/W at an operation wavelength of 2.33 $μ$m is measured under a bias of 1 V. Moreover, the fabrication resulted in multiple working devices exhibiting similar performance using a single transfer printing step, demonstrating the scalability of the proposed approach.

physics.app-ph↗

arXiv2025

Current Crowding in a High-Efficiency Black Phosphorus Light-Emitting Diode Using a Reflective Back Contact

We demonstrate a high-performance mid-infrared (MIR) light-emitting diode (LED) based on a black phosphorus (b-P)/n-MoS$_2$ heterojunction. A gold back contact combined with a rhenium-doped n-type MoS$_2$ layer is used to enhance light extraction. The device shows a MIR peak external quantum efficiency (EQE) of (1.6 $\pm$ 0.2) % at room temperature and a record (7.0 $\pm$ 0.5) % EQE at 77 K, with a maximum radiant power density of (108 $\pm$ 8) W/cm2. Finite-element simulations highlight the importance of phonon-assisted band-to-band tunneling under reverse bias and the influence of carrier velocity saturation under forward bias. The simulations also reveal that the high ideality factors extracted from the current-voltage characteristic are due to current crowding at the heterojunction and a consequence of the device geometry. These findings establish a new high-performance b-P LED architecture and provide crucial insights into the physics of MIR sources based on 2D materials.

physics.app-ph↗

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

Transfer-printed multiple Ge$_{0.89}$Sn$_{0.11}$ membrane mid-infrared photodetectors

Due to their narrow band gap and compatibility with silicon processing, germanium-tin (Ge$_{1-x}$Sn$_x$) alloys are a versatile platform for scalable integrated mid-infrared photonics. These semiconductors are typically grown on silicon wafers using Ge as an interlayer. However, the large lattice mismatch in this heteroepitaxy protocol leads to the build-up of compressive strain in the grown layers. This compressive strain limits the material quality and its thermal stability besides expanding the band gap, thereby increasing the Sn content needed to cover a broader range in the mid-infrared. Released Ge$_{1-x}$Sn$_x$ membranes provide an effective way to mitigate these harmful effects of the epitaxial strain and control the band gap energy while enabling the hybrid integration onto different substrates. With this perspective, herein strain-relaxed Ge$_{0.89}$Sn$_{0.11}$ membranes are fabricated and subsequently transfer-printed with metal contacts to create multiple photodetectors in a single transfer step. The resulting photodetectors exhibit an extended photodetection cutoff reaching a wavelength of $3.1 \,μ$m, coupled with a significant reduction in the dark current of two orders of magnitude as compared to as-grown photoconductive devices. The latter yields a reduced cutoff of $2.8 \,μ$m due to the inherent compressive strain. Furthermore, the impact of chemical treatment and annealing on the device performance was also investigated showing a further reduction in the dark current. The demonstrated transfer printing, along with the use of an adhesive layer, would allow the transfer of multiple GeSn membranes onto virtually any substrate. This approach paves the way for scalable fabrication of hybrid optoelectronic devices leveraging the tunable band gap of Ge$_{1-x}$Sn$_x$ in the mid-wave infrared range.

physics.app-ph↗

arXiv2023

Structural Engineering of Colloidal Quantum Dots: Towards Realization of Highly Efficient, Aerobic-Stable, and Droop-Free QLEDs

Quantum dot light-emitting diodes (QLEDs) are promising building blocks for prospective lighting and display applications. Despite the significant advancements achieved towards increasing the efficiency and brightness levels of QLEDs, the unavoidable demand for an inert atmosphere during the fabrication process restrains their potential for large-scale manufacturing. Here, we demonstrate ZnCdSe/ZnSe/ZnSeS/ZnS core/multi-shell QDs with ultra-thick shell (14 monolayers), significantly suppressing the diffusion of moisture and oxidative species to realize efficient all solution-processed QLED devices fully fabricated under ambient air conditions. The lattice-mismatch-engineered shell growth in the synthesized QDs leads to the strong confinement of charge carriers inside the core and near-unity photoluminescence quantum yield (PLQY) in the amber-to-red wavelength region (595-625 nm). The best amber-emitting QLED devices exhibit an external quantum efficiency (EQE) of 14.8%, a current efficiency (CE) of 41.1 cd/A, and a luminance of 5.6 x 105 cd/m2 at 12 V. To the best of our knowledge, these are the highest efficiency levels achieved in air-fabricated QLEDs. Importantly, the demonstrated devices show significant suppression of non-radiative Auger recombination and optimal charge balance, leading to negligible EQE roll-off (i.e., droop-free behavior) at the maximum luminance level. Furthermore, employing a refractive-index-matched optical compound to enhance light out-coupling increases the EQE to 26.6%, which is comparable to the best devices fabricated in an inert atmosphere. Collectively, these advances will greatly facilitate the large-scale industrial fabrication of air-stable QLEDs.

physics.optics↗

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↗

arXiv2021

Hybrid Epsilon-Near-Zero Modes of Photonic Gap Antennas

We demonstrate that in photonic gap antennas composed of an epsilon-near-zero (ENZ) layer embedded within a high-index dielectric, hybrid modes emerge from the strong coupling between the ENZ thin film and the photonic modes of the dielectric antenna. These hybrid modes show giant electric field enhancements, large enhancements of the far-field spontaneous emission rate and a unidirectional radiation response. We analyze both parent and hybrid modes using quasinormal mode theory and find that the hybridization can be well understood using a coupled oscillator model. Under plane wave illumination, hybrid ENZ antennas can concentrate light with an electric field amplitude $\sim$100 times higher than that of the incident wave, which places them on par with the best plasmonic antennas. In addition, the far-field spontaneous emission rate of a dipole embedded at the antenna hotspot reaches up to $\sim$2300 that in free space, with nearly perfect unidirectional emission.

physics.optics↗

arXiv2021

Photonic Gap Antennas Based on High Index-Contrast Slot-Waveguides

Optical antennas made of low-loss dielectrics have several advantages over plasmonic antennas, including high radiative quantum efficiency, negligible heating and excellent photostability. However, due to weak spatial confinement, conventional dielectric antennas fail to offer light-matter interaction strengths on par with those of plasmonic antennas. We propose here an all-dielectric antenna configuration that can support strongly confined modes ($V\sim10^{-4}λ_{0}^3$) while maintaining unity antenna quantum efficiency. This configuration consists of a high-index pillar structure with a transverse gap that is filled with a low-index material, where the contrast of indices induces a strong enhancement of the electric field perpendicular to the gap. We provide a detailed explanation of the operation principle of such Photonic Gap Antennas (PGAs) based on the dispersion relation of symmetric and asymmetric horizontal slot-waveguides. To discuss the properties of PGAs, we consider silicon pillars with air or CYTOP as the gap-material. We show by full-wave simulations that PGAs with an emitter embedded in the gap can enhance the spontaneous emission rate by a factor of $\sim$1000 for air gaps and $\sim$400 for CYTOP gaps over a spectral bandwidth of $Δλ\approx300$ nm at $λ=1.25$ \textmu m. Furthermore, the PGAs can be designed to provide unidirectional out-of-plane radiation across a substantial portion of their spectral bandwidth. This is achieved by setting the position of the gap at an optimized off-centered position of the pillar so as to properly break the vertical symmetry of the structure. We also demonstrate that, when acting as receivers, PGAs can lead to a near-field intensity enhancement by a factor of $\sim$3000 for air gaps and $\sim$1200 for CYTOP gaps.

physics.optics↗

arXiv2019

Mid-infrared polarized emission from black phosphorus light-emitting diodes

The mid-infrared (MIR) spectral range is of immense use for civilian and military applications. The large number of vibrational absorption bands in this range can be used for gas sensing, process control and spectroscopy. In addition, there exists transparency windows in the atmosphere such as that between 3.6-3.8 $μ$m, which are ideal for free-space optical communication, range finding and thermal imaging. A number of different semiconductor platforms have been used for MIR light-emission. This includes InAsSb/InAs quantum wells, InSb/AlInSb, GaInAsSbP pentanary alloys, and intersubband transitions in group III-V compounds. These approaches, however, are costly and lack the potential for integration on silicon and silicon-on-insulator platforms. In this respect, two-dimensional (2D) materials are particularly attractive due to the ease with which they can be heterointegrated. Weak interactions between neighbouring atomic layers in these materials allows for deposition on arbitrary substrates and van der Waals heterostructures enable the design of devices with targeted optoelectronic properties. In this Letter, we demonstrate a light-emitting diode (LED) based on the 2D semiconductor black phosphorus (BP). The device, which is composed of a BP/molybdenum disulfide (MoS$_2$) heterojunction emits polarized light at $λ$ = 3.68 $μ$m with room-temperature internal and external quantum efficiencies (IQE and EQE) of ~1$\%$ and $\sim3\times10^{-2}\%$, respectively. The ability to tune the bandgap, and consequently emission wavelength of BP, with layer number, strain and electric field make it a particularly attractive platform for MIR emission.

physics.app-ph↗

arXiv2019

Spectral responsivity and photoconductive gain in thin film black phosphorus photodetectors

We have fabricated black phosphorus photodetectors and characterized their full spectral responsivity. These devices, which are effectively in the bulk thin film limit, show broadband responsivity ranging from <400 nm to the ~3.8 $μ$m bandgap. In the visible, an intrinsic responsivity >7 A/W can be obtained due to internal gain mechanisms. By examining the full spectral response, we identify a sharp contrast between the visible and infrared behavior. In particular, the visible responsivity shows a large photoconductive gain and gate-voltge dependence, while the infrared responsivity is nearly independent of gate voltage and incident light intensity under most conditions. This is attributed to a contribution from the surface oxide. In addition, we find that the polarization anisotropy in responsivity along armchair and zigzag directions can be as large as 103 and extends from the band edge to 500 nm. The devices were fabricated in an inert atmosphere and encapsulated by Al$_2$O$_3$ providing stable operation for more than 6 months.

physics.app-ph↗

arXiv2019

Time-resolved imaging of non-diffusive carrier transport in long-lifetime halide perovskite thin films

Owing to their exceptional semiconducting properties, hybrid inorganic-organic perovskites show great promise as photovoltaic absorbers. In these materials, long-range diffusion of charge carriers allows for most of the photogenerated carriers to contribute to the photovoltaic efficiency. Here, time-resolved photoluminescence (PL) microscopy is used to directly probe ambipolar carrier diffusion and recombination kinetics in hybrid perovskites. This technique is applied to thin films of methylammonium lead tri-iodide MAPbI$_3$ obtained with two different fabrication routes, methylammonium lead tribromide (MAPbBr$_3$), and an alloy of formamidinium lead tri-iodide (FAPbI$_3$) and methylammonium lead bromide FA$_{0.85}$MA$_{0.15}$Pb(I$_{0.85}$Br_${0.15}$)$_3$. Average diffusion coefficients in the films leading to the highest device efficiencies and longest lifetimes, i.e., in FA$_{0.85}$MA$_{0.15}$Pb(I$_{0.85}$Br$_{0.15}$)$_3$ and acetonitrile-processed MAPbI$_3$, are found to be several orders of magnitude lower than in the other films. Further examination of the time-dependence shows strong evidence for non-diffusive transport. In particular, acetonitrile-processed MAPbI$_3$ shows distinct diffusion regimes on short and long timescales with an effective diffusion constant varying over 2 orders of magnitude. Our results also highlight the fact that increases in carrier lifetime in this class of materials are not necessarily concomitant with increased diffusion lengths and that the PL quantum efficiency under solar cell operating conditions is a greater indication of material, and ultimately device, quality.

physics.app-ph↗

arXiv2019

Triplet harvesting in the polaritonic regime: a variational polaron approach

We explore the electroluminescence efficiency for a quantum mechanical model of a large number of molecular emitters embedded in an optical microcavity. We characterize the circumstances under which a microcavity enhances harvesting of triplet excitons via reverse intersystem-crossing (R-ISC) into singlet populations that can emit light. For that end, we develop a time-local master equation in a variationally optimized frame which allows for the exploration of the population dynamics of chemically relevant species in different regimes of emitter coupling to the condensed phase vibrational bath and to the microcavity photonic mode. For a vibrational bath that equilibrates faster than R-ISC (in emitters with weak singlet-triplet mixing), our results reveal that significant improvements in efficiencies with respect to the cavity-free counterpart can be obtained for strong coupling of the singlet exciton to a photonic mode, as long as the singlet to triplet exciton transition is within the inverted Marcus regime; under these circumstances, we show the possibility to overcome the detrimental delocalization of the polariton states across a macroscopic number of molecules. On the other hand, for a vibrational bath that equilibrates slower than R-ISC (i.e., emitters with strong singlet-triplet mixing), we find that while enhancemnents in photoluminiscence can be obtained via vibrational relaxation into polaritons, this only occurs for small number of emitters coupled to the photon mode, with delocalization of the polaritons across many emitters eventually being detrimental to electroluminescence efficiency. These findings provide insight on the tunability of optoelectronic processes in molecular materials due to weak and strong light-matter coupling.

cond-mat.mes-hall↗

arXiv2019

Inverting Singlet and Triplet Excited States using Strong Light-Matter Coupling

In organic microcavities, hybrid light-matter states can form with energies that differ from the bare molecular excitation energies by nearly 1 eV. A timely question, given recent advances in the development of thermally activated delayed fluorescence materials, is whether strong light-matter coupling can be used to invert the ordering of singlet and triplet states and, in addition, enhance reverse intersystem crossing (RISC) rates. Here, we demonstrate a complete inversion of the singlet lower polariton and triplet excited states. We also unambiguously measure the RISC rate in strongly-coupled organic microcavities and find that, regardless of the large energy level shifts, it is unchanged compared to films of the bare molecules. This observation is a consequence of slow RISC to the lower polariton due to the delocalized nature of the state across many molecules and an inability to compete with RISC to the dark exciton reservoir, which occurs at a rate comparable to that in bare molecules.

physics.app-ph↗